Applied Materials Today 44 (2025) 102694

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Applied Materials Today

journal homepage: www.elsevier.com/locate/apmt

Recent advancements in synthesis and applications of covalent

organic frameworks
Sapna Raghav a, Jyoti Raghav b, Ma’aruf Abdulmumin Muhammad c , Madhur Babu Singh d,
Pallavi Jain d,* , Dinesh Kumar e,*
a
Department of Chemistry, Shri Jagdishprasad Jhabarmal Tibrewala University (JJTU), Jhunjhunu 333010, Rajasthan, India
b
Department of Applied Sciences and Humanities, St. Andrews Institute of Technology and Management, Farukhnagarr, Gurugram 122506, Haryana, India
c
Department of Chemistry, Mewar University, Chittorgarh 312901, Rajasthan, India
d
Department of Chemistry, Faculty of Engineering and Tehnology, SRM Institute of Science and Technology, Delhi NCR, Campus, Modinagar 201204, Uttar Pradesh,
India
e
School of Chemical Sciences, Central University of Gujarat, Kundhela, Vadodara 391107, Gujarat, India

A R T I C L E I N F O A B S T R A C T

Keywords: Covalent Organic Frameworks (COFs) represent a groundbreaking class of porous, crystalline materials
COFs composed of light elements such as carbon, hydrogen, oxygen, nitrogen, and boron. These materials exhibit low
Synthesis density, high stability, a large specific surface area, and tunable pore structures, making them highly versatile for
Properties
various applications. This review provides a comprehensive overview of recent advancements in the synthesis,
Modification
Applications
properties, and applications of COFs. Innovative synthesis methods, including solvothermal, microwave-assisted,
Linkage type mechanochemical, and ionothermal techniques, enable precise control over the structural and functional
properties of COFs. The influence of different linkage types, such as imine, boronate ester, triazine, and carbonyl,
on the properties and functionalities of COFs is explored. Additionally, modification strategies, including func­
tional group introduction and metal incorporation, enhance the versatility and range of applications for COFs.
The diverse applications of COFs in gas storage, energy storage, water pollutant removal, drug delivery, food
safety analysis, sensing, catalysis, and optoelectronics are discussed. Challenges in COF synthesis, character­
ization, and application and future perspectives on developing COF-based materials for advanced technological
and environmental applications are addressed. This review serves as a valuable resource for researchers working
in the field of porous materials and their applications.

1. Introduction came with the creation of metal organic frameworks (MOFs), which
consist of polyatomic inorganic metal clusters connected by polytopic
Over the past ten years, the development of nanoporous materials organic linkers. The exceptional coordination versatility of metal ions
has surged, driven by their exceptional performance and vast potential and organic linkers’ diverse functionality unlocked extensive material
across various applications, including catalysis, energy conversion, gas design opportunities [1,2].
storage, gas separation, optoelectronics, superhydrophobic interfaces, In 2005, Yaghi and colleagues [3] revolutionized the field again by
and energy storage. These materials have captured the attention of re­ extending the principles of topological design to synthesizing porous
searchers and industries alike for their unique properties. Chemists have organic frameworks held together by covalent bonds. This milestone
made significant strides in developing a wide range of porous materials, marked the birth of covalent organic frameworks (COFs), a new class of
yet synthesizing organic polymer networks with well-defined, discrete crystalline porous materials. Yaghi and his team were pioneers in the
pores proved to be a considerable challenge for some time. This chal­ creation of two-dimensional (2D) COFs, specifically COF-1 and COF-5,
lenge was finally overcome with reticular chemistry, an innovative utilizing hydrothermal synthesis. These materials displayed highly or­
method that utilizes topologically engineered components to assemble dered porous architectures and exhibited remarkable specific surface
these materials accurately. The first major breakthrough in this field areas [3]. By 2007, they had significantly advanced the field by

* Corresponding authors.
E-mail addresses: [email protected] (P. Jain), [email protected] (D. Kumar).

https://doi.org/10.1016/j.apmt.2025.102694
Received 15 January 2025; Received in revised form 14 March 2025; Accepted 19 March 2025
Available online 12 April 2025
2352-9407/© 2025 Elsevier Ltd. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
S. Raghav et al. Applied Materials Today 44 (2025) 102694

developing 3D COFs, which featured even greater surface areas and Numerous reviews and research articles on the synthesis and appli­
more complex void structures [4]. Compared to their 2D counterparts, cations of COFs are published annually (yearly publication data shown
3D COFs are characterized by lower density, an extensive network of in Fig. 1). Recently, Guo et al. reported advancements in utilizing COFs
open channels, and the ability to facilitate direct interactions within the for the recovery of precious metals (PMs) [17], while Duo [18] and Li
framework. As a result, they hold immense promise for gas storage and et al. [19] demonstrated the effectiveness of COFs in wastewater treat­
separation applications [5]. In 2008, the remarkable thermal and ment. However, existing reviews primarily focus on specific applications
chemical stability of COFs, their efficient charge transport and separa­ of COFs.
tion properties, and the ability to integrate photoelectric functional In this review, we comprehensively compile recent advancements in
groups to enhance carrier movement positioned functional COF mate­ the synthesis of COFs and their derivatives, covering all potential ap­
rials as strong contenders for applications in photonics [6]. plications within the timeframe of 2021–2025. This review explores
Unlike MOFs, which rely on metal-ligand coordination, COFs are different types of linkages, synthesis strategies, and the increasing
formed by covalent interactions between first and second-period ele­ research interest in COFs based on publication trends. We discuss six key
ments such as H, B, C, N, and O. This unique bonding structure has synthesis techniques, such as solvothermal, microwave, and sono­
ignited tremendous interest in the scientific community over the past chemical methods, along with the influence of various linking units on
twelve years. The synthesis of COFs typically involves the condensation COF properties. Additionally, we highlight the diverse application areas
of two organic monomers, one serving as a linker and the other as a node enabled by COFs, including gas storage, energy storage, pollutant
that forms extended, periodic networks with well-ordered pores. In some removal from wastewater, food safety, sensors, optoelectronics, catal­
cases, a single monomer can undergo self-condensation to achieve a ysis, and drug delivery.
similar structure. The presence of only light elements in COFs, along Web of Science Core Collection, 2024, URL
with the precise selection of building blocks and the controllability of
the spatial structure and covalent bond connections, has made them 2. Types of linkages in COFs
highly attractive for a wide range of applications. This selectivity and
structural control enable researchers to fine-tune the properties of COFs, COFs can be categorized based on the types of linkages formed be­
opening new avenues for advancements in areas like catalysis, gas tween their organic building units. These include imine-based COFs,
storage, and separation technologies. They form a class of crystalline where imine (C=N) linkages are prevalent and formed through
materials characterized by highly ordered porous architectures and high condensation reactions involving aldehydes, ketones, and amines. Bor­
structural precision. COFs represent a novel class of porous materials onate ester-based COFs incorporate reversible boronate ester (B-O)
formed through the covalent bonding of organic building blocks, linkages, allowing for dynamic structural changes. Triazine-based COFs
resulting in durable, low-density structures with large specific surface feature triazine (C-N=C) linkages derived from nitrogen-containing ar­
areas. COFs occupy a niche among other porous materials, like MOFs omatic compounds, while carbonyl-based COFs utilize carbonyl (C=O)
and zeolites, due to the possibility of tuning their pore sizes with high linkages formed through condensation reactions with carbonyl-
flexibility in functionalization. These features have pushed COFs to the containing precursors. Each linkage type influences the COFs’ struc­
frontier of research, with the possibility of use ranging from environ­ tural properties, such as pore size and stability, which are crucial for
mental remediation to energy storage, optoelectronics, and advanced their applications in gas storage, separation, catalysis, and sensing
technological applications [7–10]. technologies (Table 1).
An in-depth grasp of building blocks is essential since they are the The choice of linkage in COFs significantly influences their structural
basis for developing COFs and deciding their additional qualities and stability, porosity, and functional properties. COFs are fundamentally
functionalities. From a structural perspective, organic building units can characterized by their covalent linkages, which determine their struc­
be categorized into two main groups based on their geometry and tural integrity, porosity, and functional properties. Key linkages include
connection kinds. COFs are acquired from the reticulation of organic boronate esters, imines, hydrazones, and triazines, each with distinct
units to 2D or 3D covalent-bond-based networks that confer great flex­ advantages and limitations. For instance, boronate ester-linked COFs
ibility and functionality. Due to their well-defined structures and mod­ such as COF-1 exhibit high crystallinity and surface area but are often
ulable functionality, COFs have now become promising candidates in prone to hydrolysis, limiting their stability in humid environments [3].
water pollutant removal [11] and energy storage applications [12], In contrast, imine-linked COFs like COF-300 show greater chemical
catalysis [13], and biomedicines [14]. The possibility of active site stability and versatility in post-synthetic modifications, making them
dispersion makes COFs outstanding in catalysis. The diversity in their suitable for applications in gas storage and catalysis [70]. Recent in­
biocompatibility and structures makes them equally useful for novations have introduced dynamic covalent linkages such as β-keto
drug-delivery systems in which what is mainly demanded is controlled enamines and sp2 carbon linkages, which combine robustness with
encapsulation and release of therapeutic agents. Despite the significant reversible bond formation, enabling self-healing and adaptive properties
progress, the major problems are still in synthesizing COFs, which would [71]. However, challenges such as hydrolytic stability and scalability
be mechanically strong and processable. Current investigations are remain, necessitating further research to optimize these linkages for
geared toward stabilizing COFs in aqueous and harsh environments and specific applications.
enhancing their functionality by incorporating various functional
groups and metals [15]. 2.1. Imine-based
In the 2023 work by Xiao et al., the author reports the successful
development of a 3D COF known as COF-904. This COF is constructed The imine-based COFs, first developed by Yaghi and his team [72],
through the interdigitation of 2D hcb nets, which involves creating an mark the third category of COFs. These COFs are characterized by
entangled network of inclined 2D layers [16]. Most of the development unique –C=N– bonds synthesized by the Schiff base reaction via
of COFs has involved solvothermal and microwave-assisted approaches co-condensation of amines and aldehydes. In 2009, Yaghi’s group syn­
and the more recent mechanochemical method in controlling the thesized the first imine-based COF, COF-300 (Fig. 2(I)), via the dehy­
reversible polymerization of light elements to achieve well-defined dration of an aldehyde and an amine. COF-300 has a 3D diamond-like
frameworks with targeted properties. More importantly, due to such structure with a BET surface area of 1360 m²/g and a pore size of 7.8 Å.
inefficiencies in low processability and poor mechanical strength, In 2011, COF-LZU1 was synthesized by co-condensing 1,4-diaminoben­
research has now oriented itself to stabilize these COFs for practical zene and 1,3,5-triformylbenzene for catalytic applications. COF-LZU1
applications and expand functionality through diverse synthetic exhibits a 2D eclipsed structure of a 3.7 Å interlayer gap, enabling
techniques. metal ion inclusion [73]. More recently, COF-366, which incorporates

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

Fig. 1. Number of publications on COFs from 2010–2024.

porphyrin, was synthesized and used for optoelectronic applications. with controllable morphologies. They achieved morphology control by
COF-42 and COF-43 were also synthesized via a solvothermal method varying solvent and catalyst conditions, providing a novel approach for
using aldehyde and hydrazide precursors, resulting in 2D eclipsed tuning COF structures for specific applications [78].
structures with BET surface areas of 710 m²/g and 620 m²/g, respec­ Li et al. reported that while solvothermal synthesis remains a com­
tively. The numerous hydrogen bonds in the hydrazone units contribute mon approach for preparing spherical COFs, controlling the uniformity
to the stability of these eclipsed structures, while the hydrazone-linked of COF microspheres remains challenging due to uncontrollable kinetics.
COFs exhibited exceptional chemical and thermal stability [74]. They introduced 2,4,6-trimethylbenzaldehyde (TBA) as a molecular
Achieving precise control over the quantity and placement of catalytic regulator to control the size and uniformity of COFs via imine exchange,
metal ions in heterogeneous catalysts is a significant challenge. Recent dependent on TBA concentration, molecular structure, and synthesis
studies highlight significant advancements in applying COFs for selec­ temperature. The method’s versatility was demonstrated with different
tive adsorption and sensing. Wei (2023) developed two imine-linked structural units, and imine linkages served as active sites for Pd atom
COFs, TFPPy-CB and TFPPy-ODH, designed for isolating and enriching coordination, enhancing electrocatalytic oxygen reduction. This
flavonoids from natural extracts. These COFs exhibited high crystal­ approach addresses previous challenges in achieving uniform COF mi­
linity, thermal stability, and strong hydrophobicity, with impressive crospheres in solvothermal methods. Fig. 2(III) illustrates the sche­
luteolin, quercetin, and rutin adsorption capacities. They demonstrated matic synthesis of imine-based COF microspheres using dynamic imine
selective flavonoid adsorption in the presence of alkaloids and main­ exchange between the TBA regulator and BPDA building [76].
tained their performance over multiple cycles, making them promising Liu et al. demonstrated that COFs are often synthesized through the
for rapid enrichment in complex systems [75]. Xiao et al. reported the Schiff base reaction, which typically requires acetic acid, high temper­
successful synthesis of a three-dimensional covalent organic framework atures, reduced pressure, and extended reaction times. They introduced
(3D COF) named COF-904 (Fig. 2(II)). The framework was created group 14 and 15 metal halides as cost-effective and versatile catalysts for
through [3+2] imine condensation reactions using 1,3,5-triformylben­ synthesizing imine-linked COFs. The catalytic performance of lead,
zene and 2,3,5,6-tetramethyl-1,4-phenylenediamine. The structure of antimony, and bismuth halides was confirmed through the successful
COF-904 was determined via 3D electron diffraction, achieving a reso­ production of various imine COFs with various pore sizes and strong
lution of 0.8 Å, which allowed for the precise identification of all structural stability. This process yielded crystalline COFs having high
non-hydrogen atom positions. This research broadens the techniques for surface areas such as 2522 m²/g. The research broadens the scope of
creating 3D COF through interdigitation and demonstrates how intricate catalysts available for imine-based COFs and establishes a foundation for
structures can be formed from basic molecular components [16]. designing composites (perovskite@COF) for various applications [45].
In 2022, Afshari et al. synthesized a novel imine-linked conjugated They also synthesized a sturdy organic cage, Cage-6-NH2, containing six
COF called IC-COF through a water-based reaction. This material amine groups arranged in a trigonal prismatic configuration. By reacting
demonstrated outstanding sensitivity and selectivity for phosphate ions Cage-6-NH2 with 2,5-dihydroxyterephthalaldehyde (DHTPA), they
(PO₄³⁻), achieving a low detection limit of 0.61 μM. The COF’s high created a 3D COF, 3D-CageCOF-1 (Fig. 2(IV)), which adopts an acs to­
recyclability and the theoretical analysis revealed the fluorescence pology. This structure contains two interpenetrating acs networks.
quenching mechanism due to the selective binding of PO₄³⁻ ions [77]. Notably, 3D-CageCOF-1 undergoes reversible transformations between
Additionally, Guo et al. (2023) explored the synthesis of small-pore and large-pore forms when exposed to dimethylformamide
Pyridyl-Functionalized Dodecyl-Triazine-Linked COFs (PD-TPA COFs) (DMF). Furthermore, its hydrophilic nature allows for a high water

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Table 1
Application of different linkage in COF.
COF Linkage Application Remark Ref.

TFPPy-TPh-COF (Fig. 5(I)) Imine electro chemiluminescent sensor for detection range of 0.01–1000 ng/mL [20]
malathion detection
2
USCOFs and USCOPs Imine trypsin immobilization and drug delivery SSA of USCOFs 658 m /g, pore size of 3 nm; SSA of USCOPs 16 [4]
m2/g with 19 nm pores.
TADM COF Imine sensing of DNA purine bases. Range of detection for guanine (G) and adenine (A) 0.6–180 μM; [21]
LODs for G and A 0.020 μM and 0.024 μM, respectively
TBBT-COF Imine Pb removal %R is 99% in 90 min [5]
CMCOFs (Fig. 5(II)) Imine analysis of chlorine-containing herbicides. LOD range for chlorine 0.35–5.5 ng/mL [22]
BPA-TAPA COF Imine MG, JGB, CR, and AO dye adsorption Qe of MG 1070 mg/g [23]
Qe of CR 2016 mg/g
COF-LZU1 Imine H2O2 production autooxidation of COF-LZU1 to Wurster’s salt promotes H2O2 [24]
production
ESM-COF-1 and ESM-COF-2 Imine Uptake of CO2 ESM-COF-2 show better CO2 uptake, which was 4.64 m mol/g [25]
TFPPy-CB-COF and TFPPy-ODH- Imine Flavonoid adsorption of luteolin, quercetin, Qe TFPPy-CB TFPPy-ODH [18]
COF rutin Luteolin 66.32 73.20
Quercetin 67.85 70.83
Rutin 10.69 9.76
COF Imine analysis of PAHs in contaminated soil LOD is 0.01–0.05 ng/g [26]
samples.
COF@silica Imine chromatographic separation materials COF-based HPLC stationary phases [27]
TAPT-TFPB COF@SiO2; TAPT- Imine chromatographic separation more favorable separation ability [28]
TFPB COF@SiO2/SiO2–CHO
(80/20, mass ratio)
COF-LZU1 PVP/PVDF membrane Imine EBT, AR, CR, MB, (CBT), dye removal 19.37 L/m2/h/bar permeance in the case of CR and NaCl solution [29]
TAT-COF and Co@TAT-COF Imine Asymmetric supercapacitor SC of Co@TAT-COF and TAT-COF was 637 F/g and 315 F/g, [8]
respectively.
Pd/COF-BASU1 Imine Utilized in synthesis of axially chiral biaryls Stereoselective catalytic role [9]
β-ketoenamine-based COFs (2N- Imine photocatalytic oxidation activity 0N-TP-COF (99%, 16 h) < 1N-TP-COF (99%, 3.5 h) < 2N-TP-COF [30]
TP-COF) (99%, 1.5 h)
RT-COF-1 Imine Ibuprofen drug delivery 33% of drug was release after 105 min [31]
TA-P COFs Imine photoelectrochemical biosensor mercury ion (Hg2+) and aflatoxin B1 detection [32]
​ ​ ​ ​ ​
COF/CN (gC3N4) (Fig. 5(III)) Triazine photocatalytic activity The COF/CN composite achieved a 4.9-fold and 6.6-fold increase [33]
in photocatalytic efficiency for sulfamethazine removal
compared to COF and g-C₃N₄, respectively
F-CTFs Triazine solid-phase extraction (PT-SPE) of Maximum of 109.1 mg/g adsorption capacity was achived by F- [34]
amphiphilic fluoroquinolones (FQs) CTFs
Fe3O4@TAPT-OH-COF Triazine Extraction of extract AFTs (aflatoxins), and Low quantification limits (0.05–0.50 μg/kg), recoveries of [35]
ZORs (zearalenone) from food samples and 75.8–110.9%, and precise RSDs under 12.2% were achieve
biological samples
Fe@Tr-COF and Ni@Tr-COF Triazine Photocatalyst N2 reduction via the electron “acceptance–donation” process [36]
COF-Tys Triazine selective extraction of TcO–4/ReO–4 Over 99% of TcO–4 was removed within 5 min, with less than a [37]
1.5% reduction in ReO–4 removal after five adsorption/desorption
cycles, indicating excellent recyclability
CTF-1/AgI Triazine Degradation of POPs A type II charge transfer pathway of the heterojunction [38]
photocatalysts was proposed.
D-A COF Triazine photoelectrochemical sensing specific sensing of trace dopamine in serum. [39]
CTF Triazine heterogeneous photocatalyst photocatalyst can be recycled without significant loss of [40]
selectivity, and also some mechanistic tests suggested the
preferred oxidation pathway.
COTF-P Triazine photocatalytic degradation of photocatalyst under visible light. [41]
phenanthrene
TzDva Triazine C3H6/C2H4 separation selective adsorption toward C3H6 was theoretically and [42]
experimentally verified.
TFP-TAB, TFP-TTA, and TTA- Triazine CO2 photoreduction exhibits a superior visible-light-induced photocatalytic activity [43]
TTB that yields 121.7 μmol HCOOH g− 1 h− 1.
MIL-101-NH2@COF Triazine removal of dye from textile water 90% with maximum adsorption capacity of 256 mg g− 1 after 45 [44]
min
FT-COF Triazine fire resistant with enhanced mechanical Adding 3.0 wt% FT-COF reduced the peak heat release rate and [45]
performance total heat release of the TPU composite by 51.6% and 47.3%,
respectively
COF-Tr-BA Triazine battery cathode materials Achieved a discharge capacity of 1349 mA h/g and retained 627 [46]
mA h/g after 200 cycles at 0.5C
DA-CTF Triazine photocatalysts for RhB and MB degradation. Within 60 min, 92.3% of RhB and 99.2% of MB (30 mg/L) were [47]
degraded, with rate constants of 0.04096 min− 1 and 0.04843
min− 1, respectively
ART-COF/S Triazine Li-S battery It started with a high specific capacity of 1270 mA h/g, retaining [48]
1220 mA h/g after 100 charge-discharge cycles at 0.2 C
AuNPs@TS-COF/RGOs Triazine sensing of uric Acid, Dopamine and The detection limits for UA, DA, and AA were 0.07 μM, 0.03 μM, [49]
Ascorbic acid and 4.30 μM (S/N = 3), respectively.
TAPA− Tp@MGO Triazine extraction and separation of triazine The method’s LODs ranged from 0.01 to 0.05 μg kg− 1, LOQs from [50]
herbicides 0.05 to 0.2 μg kg− 1, and recoveries varied between 72.3% and
112.8%.
(continued on next page)

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Table 1 (continued )
COF Linkage Application Remark Ref.

FeIII-TA@TTB-TTA Triazine photocatalyst degradation rate for methyl orange dye was 372 times higher [51]
under >600 nm light illumination
DCB-COF Triazine organic electrode in LIB initial capacity of 2100 mA h/g [52]
Keto-CTF Triazine photocatalytic degradation of tetracycline ​ [53]
riazineB2 COF Triazine anticancer Tegafur drug delivery ​ [54]
Nb@COF Triazine Capacitors Specific capacitance retention capacity is good even after 5000 [55]
cycles
TDADE, TBAPB, and TBPDA Triazine iodine adsorption and sensing of iodine and COFs possess substantial surface areas (1490, 1596, and 1657 m² [56]
p-nitrophenol g− 1), excellent crystallinity, and remarkable adsorption
capacities for volatile iodine (4.10, 4.13, and 3.40 g/g), in
addition to outstanding recyclability
TPTP-COF and TPDA-COF Triazine supercapacitor electrode The electrodes based on TPTP-COF and TPDA-COF demonstrated [57]
good specific capacitances of 577.4 F g− 1 and 640.4 F/g, with a
scan rate of 5 mVs-1.
TD-COF β-Ketoenamine removal of p-phenylenediamine. hydrogen bonds and π-π interaction between p- [58]
phenylenediamine and TD-COF.
CCOF Triazine removal of mb dye removal efficiency (95%) for methyl orange and dsorption [59]
capacity (196.08 mg/g)
NMF/TT) Triazine removal of antibiotic NMF/TT-90 achieved the highest tetracycline adsorption at [60]
118.48 mg/g and also adsorbed 55.93 mg/g of ciprofloxacin
TzCOF, (b) CTzCOF, and (c) Triazine anticancer drug loading Efficacy of doxorubicin-loaded COF in killing cancer cells [61]
NTzCOF
Fe3O4@BB-COF benzodiimidazole extraction of aflatoxins from cereals Detection limit 0.01–0.45 μg/L [62]
2D-COF phenothiazines organic electrode in LIBs capacity of 220–773 mA h/g at high rates ranging from 100 to [63]
(PTZs) 3200 mA h/g with a good cycle life,
CTF Azo organic electrode in LIBs The Azo-CTF electrode delivers a substantial reversible capacity [64]
of 205.6 mA h/g, exceptional cycle life with 89.1% retention of
the capacity after 5000 cycles, and a significant power density of
4253 W/kg with an energy density of 258 Wh/kg
BUCT-COF-7 Imidazole electrochemical H2O2 production BUCT-COF-7, as a metal-free catalyst, [65]
TZ-COF Thiazole photocatalytic Generation of H2O2 The thiazole linkage is more effective in facilitating the [66]
formation of the *O2 intermediate in H2O2 production than the
oxazole and imidazole linkages
Tp-PTO-COF@CNTs Pyrene-4,5,9,10- cathode material in SIBs Specific capacity of 223.2 mA h/g at 0.1 A/g. [67]
tetraone
CN-COF Ethylene fluorescence sensing for Al3+ detection limit was 1.815 μM and detection in drinking water [68]
and fish samples
TFTH-COF Hydrazone detection of ClO− in real samples low detection limit of 0.417 μM [69]

Note: acid red = AR; congo red = CR; and methylene blue = MB; limit of detection = LOD; Qe = adsorption capacity; %R = removal capacity; malachite green = MG,
Janus green B = JGB, Congo red = CR; acid orange = AO; specific capacitance = SC; dye adsorption = DA

uptake of 22 wt.% at 40% relative humidity, and it also exhibits a sig­ shielding, allowing these materials to tolerate substantial amounts of
nificant carbon dioxide uptake of 204 mg/g at 273 K and 1 bar [57]. water and alcohol. These cages showed promise in encapsulating dyes
The synthesis of PD-TPA COFs with controlled morphology. PD- and catalysts for heterogeneous water oxidation [82].
(NH2)6 and TPA were used in the Schiff-base condensation method to Molecular imprinted polymers with rod-shaped COFs (RCOFs-
create PD-TPA COFs. A combination of polar and nonpolar solvents was SH@BA-MIPs) with a high concentration of hydrophilic boronate af­
typically used to synthesize COFs. To create PD-TPA COFs, a mixture of finity imprinted recognition sites were synthesized for the first time by
toluene and dioxane was chosen based on TPA and PD-(NH2)6 charac­ Shucheng Liu et al. in 2024. After stabilizing Pickering HIPEs, the
teristics. By varying the volume ratio of the two compounds, various resulting rod-shaped COFs-MIPs (Fig. 3(III)) significantly improved the
morphologies could be achieved for PD-TPA COF [79]. transport of flavoniod molecules in hierarchically porous polymers. In
the meantime, adding a hydrophilic boronic acid imprinted recognition
site allowed HPs@RCOFs-SH@BA-MIPs to display a significant contact
2.2. Boronate Ester-Based COFs angle (112.52◦ ). In phosphate acetic acid/water solution (9/1 v/v) at
303 K and 8.0 pH, the resultant HPs@RCOFs-SH@BA-MIPs demon­
The synthesis of boron-containing COFs using boronate anhydride or strated significant value for adsorption (49.0 µmol/g) and better selec­
boronate ester methods has garnered significant attention from re­ tivity as well (better than 1.19). HPs@RCOFs-SH@BA-MIPs
searchers. Boron-containing COFs are the most synthesized and can be simultaneously demonstrated decent adsorption kinetics for NRG (180
categorized into two groups based on their production techniques. One min). Furthermore, after six cycles, the HPs@RCOFs-SH@BA-MIPs sor­
group consists of COFs formed through the self-condensation of single- bents demonstrated outstanding stability (94.9%). Up to 91.0% was the
building units. For example, 1,4-benzene boronic acid self-condensed extraction efficiency of commercial NRG using HPs@RCOFs-SH@BA-
to form 2D COF-1 [80]. The other group involves COFs synthesized by MIPs. The adsorption of NRG was aided by the presence of several
the co-condensation of two or more building units. Recent research has boronate affinity imprinted recognition sites, and the use of an interfa­
showcased the advancements of COFs in a variety of applications. Li cial emulsion polymerization method stopped the leaking of imprinted
et al. (2024) developed borate-ester-based COFs (COF-5 and COF-10, adsorbents (HPs@RCOFs-SH@BA-MIPs). In conclusion, the encouraging
Fig. 3(I)) with high specific surface areas and rapid response times for outcomes of the experiments and the easy synthesis method suggest that
detecting water content in food, crucial for maintaining food quality and HPs@RCOFs-SH@BA-MIPs have a lot of promise for use in chemical
safety. These COFs demonstrated excellent sensitivity with low detec­ engineering, specialized separation, and other fields [83].
tion limits and effective performance in quantifying water content in
various food products [81]. Kirchner et al. (2024) introduced cubic
boronate ester cages (Fig. 3(II)) with enhanced stability due to steric

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

Fig. 2. (I) COF based on an imine with a 3.5 mm pore size. Reproduced with permission from Ref. 73. Copyright. (II) Constructing 3D COF from 2hcb nets through
inclined interpretation. Reproduced with permission from 16. Copyright 2023 ACS [16], (III) the formation of an imine-linked COF microsphere. Reproduced with
permission from 76. Copyright from ACS 2023 [76], (IV) Synthesis of the model compound and its single-crystal structure. Single-crystal atom colors: C, gray; N, blue;
O, red. H atoms are omitted for clarity. Reproduced with permission from 57. Copyright 2020 ACS [57].

2.3. Triazine based COFS precursor molecules, TFPT, DETH, and BETH, in a reaction medium of
Dioxane/Mesitylene/6 M HOAc (5/15/2) at 120 ◦ C for three days (Fig. 4
Triazine-based COFs came into the limelight owing to their robust (I)). The resulting product is TDB-COF, which features a
structural stability and versatile applications. The constructed COFs two-dimensional lattice structure with triazine rings and thioether
with triazine units in the framework using Schiff base condensations groups, forming a porous framework [86].
provide highly crystalline products with substantial surface areas and Developing highly efficient organic photoelectrodes remains a
exceptionally high thermal stability. For instance, triazine-based COFs considerable challenge. The study by Dai et al. (2021) demonstrated that
have been proven to greatly enhance thermoplastic polyurethane’s fire two COFs (TPT-COF-1 and TPT-COF-2), incorporating 2,4,6-triphenyl-
retardancy and mechanical properties, such as promoting char residue 1,3,5-triazine, function effectively as cathodes for hydrogen genera­
and reducing heat and smoke release. In addition, these COFs also tion photo-catalytically [88]. The incorporation of 2,4,6-triphenylben­
exhibited excellent energy storage performance, especially in super­ zene in these COFs forms donor-acceptor pairs, leading to a significant
capacitors, where they showed high capacitance and long-time stability increase in visible-light photocurrent (110 µA/cm2) as compared to
during many charge-discharge cycles. TTA-TTB COF having a photocurrent of 35 µA/cm2 at 0 V against
Recent studies have explored the potential of COFs in enhancing reversible hydrogen electrode (RHE) in the absence of any metal co­
material properties and performance. Ashari (2021) developed a flame- catalysts or organic sacrificial agents. This increased photocurrent is due
retardant COF based on triazine (FT-COF) for the betterment of fire to the reduced bandgap and increased charge transfer via intramolecular
safety and to enhance the mechanical characteristics of thermoplastic donor-acceptor interactions. Xu et al. (2016) highlighted the potential of
polyurethane (TPU) [84]. Adding 3.0 wt% FT-COF significantly crystalline COFs as highly efficient organic photoelectrodes for water
increased TPU’s tensile strength and elongation, enhanced its thermal splitting, focusing on their enhanced donor-acceptor characteristics
stability, and notably reduced heat release and smoke production, [89].
making TPU more fire-resistant. Yang et al. (2023) developed 2D COFs Wang et al. (2024) designed and synthesized a triazine-carbazole-
based on triazine (TPDA-COF and TPTP-COF) [85] and combined them based COF (COF-TCZ) using Schiff condensation. The COF exhibited
with carbon nanotube fibers (f-CNFs) to create high-performance high crystallinity, thermal and chemical stability, and excellent photo­
supercapacitor electrodes. The COFs demonstrated high surface areas active properties. The imine-linked COF-TCZ was further oxidized to an
and capacitance, with TPDA-COF showing superior energy and power amide-linked COF (COF-TCZ-O). Both frameworks showed enhanced
densities. Although incorporating f-CNFs reduced specific capacitance, light-harvesting and charge separation efficiencies, making them effec­
the COF-based devices maintained excellent stability over 10,000 cycles. tive photocatalysts for N-aryl tetrahydroisoquinoline oxidation. The
Zhou et al. synthesized a thioether-decorated triazine-based covalent study demonstrated their high conversion rates, photostability, and
organic framework (TDB-COF). The process involved combining three recyclability and provided insights into their photocatalysis

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

Fig. 3. (1) COF-5 and COF-10. Reproduced with permission from 81. Copyright 2024 Elsevier. (II) SC-XRD structure of 6a with views of one layer along the c-axis
(left) and stacked layers along the b-axis (right). (b) PXRD data for crystalline 6a (blue) and simulation from SC-XRD structure (black). (c) Thin section cut of the pore
system indicating the cage windows (orange) and intrinsic pores (purple). The occupied area after 360◦ rotation along the channel axis is indicated in gray.
Reproduced with permission from 82. Copyright 2024 ACS. (III) TEM images of RCOFs-DDS (a), RCOFs-SH (b), RCOFs-SH-Br (c), RCOFs-SH@BA-NIPs (d), and
RCOFs-SH@BA-MIPs. Reproduced with permission from 83. Copyright 2024 Elsevier.

mechanisms, highlighting their potential for organic conversion appli­ catalytic processes and environmental applications [91]. Additionally,
cations [90]. carbonyl-based COFs have shown promising results in the field of pho­
A simple and economical reaction involving catalyst-free cyclo­ tocatalysis. Wang et al. (2024) developed a novel COF featuring
trimerization and a single-pot reaction of alkynes at room temperature carbonyl linkages that demonstrated increased catalytic activity for the
on a gram scale is used to create triazine COF (Fig. 4(II)a). By running photodegradation of organic molecules in the presence of visible light.
the reaction at three distinct time intervals, the development of the The carbonyl groups contributed to efficient charge separation and
sheets was tracked. AFM pictures of the products of the 2 h, 6 h, and 18 h transfer within the framework, producing high photocatalytic perfor­
reactions—named PTrz2, PTrz6, and PTrz18, respectively—are dis­ mance. The study highlights the potential of carbonyl-based COFs in
played in Fig. 1c. The two-hour reaction produced inhomogeneous flat environmental remediation, where their high stability and activity make
materials that were laterally joined with larger sheets. Sheet-like them effective in degrading harmful substances [90].
structures having distinct edges were formed after 6 h. The lateral A recent investigation focused on the COF Tp-PTO-COF as a potential
growth of small particles connecting the margins of large sheets was electrode material for water-based secondary rechargeable zinc-ion
counted. The product had sheet-like structures with distinct borders and batteries (ZIBs). This framework, notable for its numerous carbonyl
lateral sizes of several micrometers after 18 h. Concurrent lateral and active sites, achieved impressive specific capacities of 301.4 mA h/g
vertical growth was shown by the material’s thickness and basal plane along with 0.2 A/g current density and 192.8 mA h/g at 5 A/g current
rising as the reaction time increased. The vertical development and density. It exhibited remarkable stability and consistent charge-
lateral crosslinking of the materials are indicative of the π-π stacking of discharge cycles for the long term. The improved electrochemical
their backbone and the cyclotrimerization of ethynyl groups (Fig. 4(II) characteristics are linked to the plentiful carbonyl sites (nucleophilic
b) [87] sites), their proper porous structure, and their chemical stability. The
study also investigates the structural changes and the intercalation
mechanism of Zn²⁺ ions through both experimental methods and density
2.4. Carbonyl-based COFs
functional theory (DFT) calculations [92].
Carbonyl-based COFs are materials characterized by carbonyl groups
in the framework structure, significantly influencing their properties 2.5. β-Ketoenamine-based COFs
and functionalities. Recent studies have highlighted the versatility and
advantages of these COFs in various applications. Zhao et al. (2023) Although imine-based COFs exhibit significantly improved stability
synthesized a new carbonyl-based COF series demonstrating their high compared to boron-based COFs, the intrinsic reversibility and strong
surface areas and tunable pore sizes. These COFs could have potential polarization of imine bonds can still influence the overall stability of
for gas storage and separation applications as they exhibited excellent these frameworks. Kandambeth et al. [93] described the synthesis of
stability and high adsorption capacities for various gases, including CO2 chemically robust COFs using a two-step approach. This process first
and CH4. The incorporation of carbonyl groups improves the structural employed a reversible Schiff base reaction to construct a crystalline
integrity of these frameworks. It enhances their chemical reactivity and framework, which was then stabilized through irreversible enol-keto
interaction with guest molecules, leading to superior performance in tautomerism. The synthesized COFs, designated as TpPa-1 and TpPa-2,

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

Fig. 4. (I) A diagrammatic illustration of the synthesis process for TDB-COF. (II) (a) Schematic representation of the synthesis of porous heteroaromatic frameworks.
Reproduced with permission from 86. Copyright 2023 Elsevier, (b) Lateral growing and vertical stacking of PTrz sheets. Reproduced with permission from 87.
Copyright 2024 Elsevier.

exhibited exceptional resistance to boiling water and acidic conditions. enriching the growing collection of COFs with varied functionalities and
Additionally, TpPa-2 displayed outstanding stability even in a highly potential applications. COF-42 and COF-43 are building units linked by
alkaline environment (9 mol/L NaOH). Fang et al. [94] demonstrated hydrazone bonds, which impart high crystallinity, permanent porosity,
that β-Ketoenamine-based COFs possessed a rich array of active catalytic and remarkable chemical and thermal stability. Their successful syn­
sites under alkaline conditions, which could catalyze organic reactions thesis and outstanding properties highlight the practical potential of
in an alkaline environment. This discovery is significant as it expands hydrazone-based COFs for real-world applications.
the scope of applications for COFs in catalysis, particularly in reactions
that require a basic medium.
2.7. Imide COFs

2.6. Hydrazone COFs COFs containing -C-N- bonds, formed through the condensation of
anhydrides with aniline derivatives, represent a significant class of
Hydrazone-linked COFs represent another category of COFs con­ COFs. While imide and amide bonds offer exceptional thermal and
taining -C-N- bonds, typically synthesized via the condensation of hy­ chemical stability, their irreversible formation poses challenges for
drazines and aldehydes. Unlike imine bonds, hydrazone bonds synthesizing imide- and amide-based COFs in a single step. Fang et al.
incorporate a highly electronegative element attached to the C=N bond. [96] were the first to utilize imide reactions for synthesizing
The nitrogen lone pair, along with the p-π conjugation formed with the two-dimensional polyimide COFs, leading to the development of three
C=O bond, greatly enhances the overall stability of the linkage. More­ hexagonal, crystalline COFs: PI-COF-1, PI-COF-2, and PI-COF-3. In
over, the presence of hydrazone components facilitates hydrogen bond comparison to amorphous porous polyimides, Polyimide COFs
formation within the pores, further improving the hydrolytic and (PI-COFs), including polyarylether-based covalent organic frameworks
oxidative stability of the COFs. Uribe-Romo et al. [95] synthesized two (PAE-COFs), offer notable advantages in thermal stability, specific sur­
novel COFs, COF-42 and COF-43, through the condensation of 2,5-dieth­ face area, and pore size. The superior thermal stability of PI-COFs is due
oxyterephthalic hydrazide (DETH) with either 1,3,5-tri(4-formylphenyl) to the strong covalent bonds within their structure, which prevent
benzene (TFB) or 1,3,5-tri(4-carboxyphenyl)benzene (TFPB). These degradation at high temperatures, making them well-suited for appli­
COFs exhibit unique structural characteristics and properties, further cations in extreme thermal conditions.

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COFs constructed with imide bonds exhibit outstanding crystallinity, valuable insights. This section will provide an overview of the various
stability, and porosity. Their robust aromatic frameworks make them synthesis approaches, highlighting their benefits and limitations
ideal for various applications, including chemical sensors [97], ion through Figures and Tables 2 and 3. The aim is to broaden the appli­
probes, energy storage [98], photocatalysis [99], and other advanced cability of COFs and offer a thorough reference for researchers and
fields. For instance, Jarju et al. synthesized MPc-COFs by combining professionals in the field.
metalized phthalocyanine (MPc) with benzidine (BZ), where imide Recent advancements in COF synthesis have expanded the toolkit for
bonds link the macromolecular building blocks, while the phthalocya­ creating highly crystalline and functional frameworks. Solvothermal
nine cavities serve as active sites, enhancing photocatalytic performance methods remain the most widely used due to their simplicity and ability
[100]. Imide bond-based COFs typically possess an extended π-conju­ to produce high-quality COFs; however, they often require long reaction
gated structure, broadening their visible light absorption range. Addi­ times and harsh conditions. Microwave-assisted synthesis offers rapid
tionally, they exhibit high charge carrier density and mobility, which and efficient production, while ionothermal methods provide enhanced
contribute to improved photocatalytic efficiency [101]. crystallinity and stability. Mechanochemical approaches are emerging
as environmentally friendly alternatives, but challenges in scalability
3. Synthesis methods and reproducibility persist. The hydrogen bonding preassembly strategy
enables the synthesis of soluble and highly crystalline COFs under mild,
This section covers traditional and recent advances in COF synthesis catalyst-free conditions. This approach addresses the limitations of
techniques. Fig. 6 illustrates the various methods employed in COF traditional solvent-thermal methods, such as long reaction times and
synthesis. Achieving highly structured covalent networks necessitates high temperatures, while also offering control over particle size and
precise control over the thermodynamic equilibrium during bond for­ solubility [139]. This section mainly discusses the various methods of
mation. The creation of thermodynamically stable polymeric crystalline COF synthesis: microwave synthesis, solvothermal, ionothermal, room
architectures depends on carefully managing reaction conditions, such temperature synthesis, and mechanochemical grinding (Table 2).
as temperature, pressure, and the presence of templates. For COFs to
achieve ordered and pre-designed covalent connections between
organic units, it is crucial to follow a topology diagram that guides the 3.1. Solvothermal synthesis
assembly of extended polygonal structures with multiple reactive sites
for optimal growth [102,103]. The synthesis of COFs was conducted using the solvothermal method
COFs have drawn considerable interest due to their exceptional for the first time [136]. Most COFs synthesized to date primarily utilize
properties and wide-ranging applications. However, their synthesis re­ the solvothermal method. The raw material is dispersed in a mixed
mains a significant challenge. The choice of preparation methods and solvent in this synthesis approach. A common method for synthesizing
reaction conditions plays a crucial role in determining the crystallinity COFs involves a solvothermal approach wherein monomers and solvents
of the resulting COFs, directly affecting their overall properties. Re­ are degassed in a Pyrex glass tube through repeated freeze-pump-thaw
searchers have made notable advancements in this area, contributing cycles. After sealing the Pyrex tube, it is heated to a specific tempera­
ture for a predetermined duration. Once the reaction is complete, COFs

Fig. 5. (I) Schematic diagram of the TFPPy-TPh-COF synthesis, (B) ECL mechanism of the TFPPy-TPh-COF/TPrA. Reproduced with permission from 20. Copyright
2024 Elsevier. (II) Schematic of synthesis and MSPE application of CMCOFs materials. Reproduced with permission from 22. Copyright 2024 Elsevier. (III) Schematic
representation of the preparation of COF/CN-x. Reproduced with permission from 33. Copyright 2025 Elsevier.

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

Fig. 6. Schematic representation of the properties and advantages of various conventional methods for the preparation of COFs. Reproduced with permission from
102. Copyright 2023 Elsevier.

are isolated as a solid powder by collecting the precipitate, washing it 3.2. Microwave synthesis
with suitable solvents, and drying it under a vacuum. Important con­
siderations for selecting the reaction medium and conditions include Microwave synthesis is increasingly used to prepare small-molecule
various factors such as crystal nucleation, solubility, growth rates, re­ organic compounds, offering faster reaction rates and higher yields. This
action kinetics, and self-healing properties. An adequate temperature is method enhances efficiency and reproducibility compared to traditional
vital to ensure that the reaction can be reversed. Typically, COFs are heating. Recent studies indicate that it can also be applied to synthesize
synthesized in the temperature range of 85–120 ◦ C, depending on the crystalline COFs, which have potential applications in gas storage,
reactivity of the components. Maintaining a closed reaction system is separation technologies, and catalysis. Microwave synthesis presents
essential to prevent moisture from initiating a reverse reaction. advantages over solvothermal techniques. It generates COFs quickly,
To synthesize COFs, suitable monomers to be placed at the vertices does not require a sealed vessel, and effectively removes residues and
and edges are mixed with a catalyst and solvents in a Pyrex tube. After contaminants from frameworks, thereby increasing porosity. In 2008,
brief sonication and degassing via freeze-pump-thaw cycles, the tube is Cooper’s research team utilized microwave-assisted synthesis to suc­
sealed and held at a controlled temperature for a specified time. Once cessfully produce COF-5, marking a significant advancement in the field
cooled, the precipitate is collected through centrifugation or filtration, of covalent organic frameworks. This innovative approach enabled the
washed with a suitable solvent, or treated with Soxhlet extraction to formation of COF-5 within a remarkably short reaction time of just 20
eliminate oligomers or high-boiling-point solvents. The residue is minutes, showcasing the efficiency and effectiveness of microwave
vacuum-dried at 80–120 ◦ C and stored in a dark environment under synthesis in creating complex materials. The ability to rapidly synthesize
nitrogen or argon. This method effectively produces various COFs, such COF-5 emphasizes the potential of microwave-assisted techniques in
as TPT-COF-1, synthesized using 2,4,6-tris(4-aminophenoxy)-1,3,5- organic chemistry and contributes to a broader understanding of COFs
triazine (TPT-NH2) along with 2,4,6-tris(4-formylphenoxy)-1,3,5- and their applications in various fields [142].
triazine (TPT-CHO), scalable to gram-level production [137]. Alsudairy et al. pioneered the integration of microwave-assisted
Recent studies highlight advancements in synthesizing and applying synthesis (as shown in Fig. 7(I)) with a mixed-linker approach to
COFs. A triphenylamine-based COF, TPA-COF, was synthesized through create multivariate COF adsorbents (denoted as X% OMe-TFB-BD COFs,
Schiff base coupling, which demonstrated a high specific capacitance of where X represents 0, 33, 50, 67, and 100 mol%) by utilizing different
263.1 F/g and excellent cycle stability, showing a capacitance retention proportions of benzidine (BD) and 3,3′-dimethoxylbenzidine (BD-OMe)
rate of 111% after 5000 cycles [140]. Also, Shanxin Xiong reported linkers. This method enabled the rapid and efficient fabrication of the
triphenyl-based COF named TABT-COF and TABH-COF, which had COFs. By varying the mole ratios of BD-OMe to BD, the researchers
higher optical properties. Additionally, uniform spherical COFs were achieved significant differences in the porosity, density, thermal sta­
synthesized using 2,4,6-trimethylbenzaldehyde as a molecular regu­ bility and chemical stability crystallinity, and morphology of the COFs,
lator, resolving issues with sphere uniformity and size and improving facilitating precise optimization of their adsorption capabilities for static
electrocatalytic performance for oxygen reduction reactions by coordi­ iodine vapor [143]. A study presents a novel method for synthesizing
nating imine linkages with Pd atoms and clusters [141]. functionalized ultra-microporous carbons using segregated microwave
irradiation with COFs as carbon and nitrogen sources. This method re­
sults in carbons with high nitrogen content (>30 wt%), narrow pore size

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Table 2
Application of synthesis method of COFs.
COF Synthesis method Application Remark Ref.

TABP-COF/C-Rgo solvothermal electrochromic properties Demonstrated outstanding stability, retaining 80.1% of the initial contrast after 5000 [104]
seconds of cycling
ICOFs solvothermal adsorption of ReO−4 High adsorption capacity for ReO−4 (714 mg/g for TABD-COF, 633 mg/g for TAPB- [105]
COF) with fast ion exchange, capturing 98% within 3 to 5 minutes
TABT-COFs and TATH- solvothermal Electrochromic The coloring and bleaching times for TABT-COFs are 5.2 seconds and 5.6 seconds, [106]
COFs while for TATH-COFs they are 3.9 seconds and 3.5 seconds, respectively
COF-ETTA-2,3-Dha and solvothermal large scale synthesis scalable synthesis of high-quality COFs [107]
(b) COF-DHTA
COFDAAQ-TFP solvothermal electrochromic properties in various areas like smart windows and smartphone back covers [108]
​ solvothermal photocatalytic degradation 90% of RhB molecules were broken down within 10 minutes of UV light exposure [109]
RhB
COTTT solvothermal photoelectric materials retention rate of the electrochromic device is 90.6% after 1600 s switching [110]
TFP-PPDA COFs solvothermal adsorption of RhB dye SSA = 705 m2/g and Qe = 704.3 mg/g [111]
TAPB-PDA COF solvothermal ​ these results provide a new approach for recrystallizing or solvent-annealing 2D COFs, [112]
potentially guiding the crystallization of large-area imine-linked 2D polymers from
solution
3D COF-320 solvothermal ​ the first successfully fabricated 3D COF functional membrane on a standard porous [113]
α-Al2O3 ceramic support
COF-1 solvothermal pesticide removal 99.5% removal efficiency [114]
COF-30 Solvothermal DDT removal 92.3% removal efficiency [115]
COF-90 Solvothermal parathion removal 93.99% removal efficiency [116]
COF-100 Solvothermal malaoxon removal 95.7% removal efficiency [117]
COF-120 Solvothermal chlorfenapyr removal 94.3% removal efficiency [118]
iCOF@cotton mechanochemical detection domoic acid (DA) in Trace amounts of DA were detected at a concentration of 18.6 pg/mL, demonstrating a [119]
marine samples satisfactory recovery rate that ranged from 85.7% to 107.2%. This indicates the
method’s reliability and effectiveness in accurately measuring low levels of DA,
confirming its potential for sensitive detection in various applications
LZU1-NH2IL-NTf2 mechanochemical anti-wear and friction the lubrication performance primarily results from the physical adsorption film [120]
reduction (lubricant additive) facilitated by the ionic liquid and the strong protective layer formed through
tribochemical reactions
TpBD-(SO3Na)2 mechanochemical adsorption of Fluoroquinolone the adsorption capacities (Qe) for norfloxacin, enoxacin, and ciprofloxacin were [121]
antibiotics (FQs) 1709.6, 1661.5, and 1362.8 mg/g, respectively
TpBD mechanochemical U6+ adsorption specific area (139 m2/g) [122]
high adsorption capacity (167 mg/g) and good re-usability (no significant difference
after five cycles)
CdS/COF sonochemical photocatalytic degradation of n-p heterojunction of CdS/COF is beneficial to the separation of photogenerated [123]
Bisphenol-A electron-hole pairs
LZU1-PEIS mechanochemical water lubricant additives the average friction coefficients were reduced from 0.67 to 0.31 (LZU1-PEIS-TC) and [124]
0.23 (LZU1-PEIS-BM), respectively.
2D-COF mechanochemical EP/TpPa-1 composite coating anticorrosion performance [125]
Fe3O4@TpMA mechanochemical Degradation of methyl orange 88.1% of methyl orange (MO) was degraded within 40 min. [126]
COF-145 mechanochemical Dimethoate removal 99.1% removal efficiency [127]
TH-COF Microwave solid-phase micro-extraction SSA = 1254 m2/g; LOD = 0.0020–0.0045 ng/L [128]
OMe-TFB-BD COF microwave Iodine capture adsorption capacity 8.2 mg/g [59]
TFPPy-AD sonochemical Flavonoid adsorption rapidly synthesized at room temperature within just 60 min [129]
BDT@Co-COF Microwave electrochemical performance Asymmetric supercapacitor device showed specific capacitance of 220 F/g at 2 mV/s. [130]
in supercapacitors.
COF-AP-IL@HA Microwave Tumor therapy the loading rate of AP in COF hollow spheres (with a shell thickness of approximately [131]
30 nm) was around 40.3%, attributed to the interactions between hydrogen bonds and
π-π bonds between AP and the COF shell
Pz-CTFs Ionothermal CO2 adsorption with a specific surface area of 1009 m²/g, the highly crosslinked, electron-rich [132]
phosphazene core contributed to the significant structural and thermal stability of the
synthesized CTFs, enduring temperatures up to 500 ◦ C, while also enhancing their CO₂
philicity
COF-95 ionothermal carbofuran removal 98.1% removal efficiency [133]
TABP-COF Solvothermal electrochromic film - [134]
2D-COF mechanochemical ​ this study presents the first experimental evidence of solvent-based COF templating, [135]
marking a significant step forward in the mechanistic understanding of
mechanochemistry as an eco-friendly method for COF synthesis

distribution, and significant surface areas (507 and 243 m²/g at 0.4 and these COFs improve oil adsorption efficiency over time and demonstrate
0.6 nm pore sizes, respectively). These carbons exhibit superior chemi­ exceptional water-in-oil emulsion separation, achieving at least 99.5%
cal, irradiation, and thermal stability while maintaining the precursor’s efficiency. This study highlights the potential of microwave sol­
bulk morphology and introducing a unique cyano group for further vothermal synthesis of superhydrophobic COFs as a viable alternative to
modification. The carbons demonstrated an impressive uranium traditional methods for industrial-scale production. Additionally, these
adsorption capacity of 50 mg/g at pH 1.0, with 80% of uranium findings present a novel approach for addressing oil spill remediation
adsorbed, showing potential for applications in heavy metal removal, and the separation of water-in-oil emulsions using advanced 2D COFs
gas storage, and carbon super-capacitors. [144]. Dey et al. demonstrated in 2024 a microwave-assisted method for
Wei et al. detailed the building blocks for COFs, which include 1,3,5- the fast and efficient synthesis of COFs, specifically of the
tris(4-aminophenyl) benzene and either 2,3,5,6-tetrafluoroterephthalal­ donor-acceptor TzPm-COF type, within seconds to minutes. This method
dehyde or 1,4-phthalaldehyde. The incorporation of fluorine groups could thus solve standard solvothermal methods’ time and scalability
enhances the hydrophobicity and stability of the COFs. As adsorbents, limitations, usually requiring days. TzPm-COF showed excellent

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Table 3 exceptional stability and porosity for environmental applications, such

Advantages and Disadvantages of synthesis method. as pollutant removal and water purification, are achieved through ion­
Method Advantages Disadvantages Ref. othermal synthesis. Song et al. (2023) described the creation of
metallophthalocyanine-based COFs through a mixed-metal salt ion­
Solvothermal Simplicity insoluble products, [136,
high crystalline product long reaction time, 137] othermal technique. The resulting COFs, M-pPPCs and M-anPPCs, were
variety of solvents can be complex process, produced from 1,2,4,5-tetracyanobenzene and 2,3,6,7-tetracyanoan­
used limited to few types of thracene, demonstrating remarkable stability, crystallinity, and sur­
well-established method COF structure only face area. These frameworks exhibited impressive CO2 adsorption
Microwave generate fast and clean For small size COFs [130]
products. only,
capacities, reaching as high as 7.6 mmol/g at 273 K and 1.1 bar. When
ability to monitor the Reaction conditions integrated with carbon nanofibers, the Co-pPPC and Co-anPPC COFs
phase behaviour are difficult to control, showed significant catalytic efficiency in electrochemical CO2 reduc­
simultaneous control of Potential issue in tion, achieving Faradaic efficiencies of up to 74% at − 0.64 V versus RHE
pressure and temperature uniform heating
[148]. Guan et al. reported a simple and direct strategy to produce a
fast and cheap
Sonochemical green chemistry required higher [129] series of 3D ionic liquid-containing COFs (3D-IL-COFs) using green
approach temperature, solvents (ionic liquids) (Fig. 8(I)). The syntheses were conducted at
minimum waste reaction conditions ambient temperature and pressure with high reaction speed, and the
generation are difficult to control ionic liquid could be reused without any loss of activity [149]. Maschita
short reaction time
Ionothermal yield highly crystalline side reactions [130]
et al. employed ionothermal synthesis (Fig. 8(II)) to produce crystalline
product and porous PI-COFs utilizing zinc chloride and eutectic salt mixtures in a
Mechanochemical manual grinding, issue of uniformity [121, separate study. This innovative approach eliminated the need for soluble
environmentally friendly, and reproducibility 138] precursors and considerably shortened the reaction time compared to
RT synthesis,
traditional solvothermal methods. They applied this technique to pre­
provide exfoliated
structure viously established imide COFs and succeeded in synthesizing a novel
perylene-based COF, which was unattainable through conventional
solvothermal synthesis [150].
photocatalytic properties: visible light absorption, appropriate band According to Maschita et al., the study presents an innovative ion­
alignment, and low exciton binding energy. It efficiently generates su­ othermal method for synthesizing polyimide-linked COFs (PI-COFs)
peroxide radical anions and promotes aerobic photo-oxidative amida­ using zinc chloride and eutectic salt mixtures. This approach effectively
tion reactions between various aromatic aldehydes and amines, addresses traditional solvothermal synthesis challenges, such as long
realizing moderate to high yields. Meanwhile, the work has applied in reaction times and the need for soluble precursors. The ionothermal
situ diffuse reflectance FTIR to make clear the catalytic mechanism of technique accelerates the synthesis and facilitates the formation of new
the microwave-assisted approach as a robust and scalable alternative in PI-COFs, including a unique perylene-based COF that cannot be pro­
producing COFs and catalytic applications Dey et al. demonstrated that duced using conventional methods. High-temperature XRPD analysis
traditional solvothermal methods for synthesizing COFs are limited by reveals that the reaction involves crystalline precursor-salt adducts,
low scalability and long reaction times. They developed a which subsequently interact to form the COF, thereby improving syn­
microwave-assisted synthesis for the donor-acceptor COF, TzPm-COF (, thesis efficiency and expanding the scope of COF development [150,
significantly reducing synthesis time to 10 min. TzPm-COF, which ex­ 151].
hibits high crystallinity, porosity, and morphological stability, effi­
ciently generates superoxide radicals under visible light. This capability 3.4. The formation of monolayers on a HOPG surface
enables effective aerobic photooxidative amidation reactions with high
recyclability. The method works well with various substituted aromatic The formation of monolayers on the surface of the highly ordered
aldehydes and amines, and the catalytic process was studied by in-situ pyrolytic graphite (HOPG) surface plays a crucial role in synthesizing
diffused reflectance infrared Fourier transform spectroscopy (DRIFTS) COFs. When COFs are synthesized on a HOPG surface, the high flatness
[145]. A study developed multivariate COFs using a microwave-assisted and stability of HOPG provide an ideal substrate for forming well-
synthesis and mixed-linker strategy to capture hazardous radioiodine. ordered monolayers. This process often involves the deposition of pre­
By varying BD and BD-OMe linkers, different COFs were produced, with cursor molecules onto the HOPG surface, followed by polymerization or
the 50% OMe-TFB-BD COF (Fig. 7(II)) showing the highest 8.2 g/g condensation reactions that form a covalent network. Their uniformity
iodine adsorption capacity. This COF also demonstrated excellent and high crystallinity typically characterize the resulting monolayers,
recyclability over seven cycles, highlighting the effectiveness of the thanks to the smooth surface of HOPG, which minimizes defects and
synthesis method for creating high-performance COFs tailored for irregularities in the COF structure. This method is advantageous for
environmental remediation [146]. studying the growth and properties of COFs at the monolayer level, of­
fering insights into their electronic, optical, and mechanical properties.
3.3. Ionothermal synthesis Additionally, the well-defined nature of monolayers on HOPG facilitates
the development of advanced COF-based materials with tailored prop­
Triazine-based COFs were first synthesized by Thomas’s group using erties for various applications.
ionothermal method [147]. Ionothermal synthesis of COFs involves In this experiment, a monolayer of COFs was created on a HOPG
using ionic liquids as the reaction medium to facilitate COF formation, surface using BPDA and 9,9-dihexylfluorene-2,7-diboronic acid in THF.
exploiting their wide liquid range, low vapor pressure, and high thermal The samples were heated in an autoclave at 150.1 ◦ C for 1 h. Adding
stability. This method creates highly crystalline and porous COFs with CuSO4⋅5H2O was crucial, as it provided a water reservoir that main­
enhanced stability and porosity by adjusting ionic liquid composition, tained chemical equilibrium, improving surface coverage from 7 to 98%.
temperature, and reaction time. Recent studies have highlighted its The water released by CuSO4⋅5H2O during heating helped repair defects
advantages: Wang et al. (2023) demonstrated that ionothermal synthesis and form a well-ordered COF network, while cooling allowed CuSO4 to
leads to COFs with superior crystallinity and stability, surpassing con­ reabsorb water, stabilizing the structure [142].
ventional methods [18]. Triazine-based COFs show that varying ionic Niu et al. (2022) reviewed 2D polymers, highlighting their unique
liquids allow for precise control over porosity and surface area, opti­ properties, exotic band structures, and synthesis strategies. It empha­
mizing them for gas storage and separation. Additionally, COFs with sizes recent advances in photopolymerization and monomer design for

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

Fig. 7. (I) Microwave-assisted synthesis of mixed-linker X% OMe-TFB-BD COFs (where X % = 0, 33, 50, 67, and 100 mol%) was achieved quickly and easily. The
inset features digital images of the resulting COFs exhibiting varying densities. Reproduced with permission from 143. Copyright 2024 Elsevier. (II) (A) Simple
microwave-assisted synthesis of Mw-TFB-BD-X COFs (where X represents -CH3 and –OCH3) conducted in the air within one hour, (B) Models of Mw-TFB-BD-CH3 and
(C) Mw-TFB-BD–OCH3, featuring layers organized in an eclipsed stacking configuration. Reproduced with permission 146. Copyright 2023 ACS.

creating mesoscale-ordered 2D polymers [152]. A related study by Lu mortar to achieve this. The resulting COFs, TpPa-1(MC) and TpPa-2
et al. (2020) explores the synthesis of single-layered homochiral 2D COF (MC), exhibited low BET surface areas and moderate crystallinity.
[153]. These COFs demonstrated excellent chemical stability in boiling water,
3M NaOH (aq), and 9M HCl (aq). Additionally, mechanochemical syn­
3.5. Mechanochemical Synthesis thesis enables the conversion of COFs into two-dimensional nanosheets
through spontaneous delamination. In 2016, the same research group
Solvothermal and microwave synthesis methods often require intri­ introduced a liquid-assisted grinding (LAG) technique to enhance the
cate conditions, including sealed Pyrex tubes, inert atmospheres, and synthesis rate of COFs. This method involved adding catalytic liquids to
specific solvents and temperatures for crystallization. In contrast, help aggregate the reactants, thereby improving crystallinity and yield.
mechanochemical synthesis offers a straightforward, cost-effective, and Zhang et al. employed a simple ball milling process to prepare a func­
environmentally friendly alternative to these complex solvothermal tionalized COF. Fig. 9(I) depicts the synthesis of a compound called
techniques. This method has successfully produced various sponge-like COF-F, formed through the reaction of two molecular compounds, TIA
porous materials such as porous carbon, MOFs, metal oxides, and gra­ and TFT, under specific conditions (120 ◦ C for 72 h). The aldehyde-
phene derivatives. The synthesis of COF through mechanochemical terminated COF-F then reacted with amino thiadiazole in the ball mill­
methods is still in the developmental stage. For instance, researchers ing jar, resulting in the thiadiazole-functionalized COF-F (Thdz@COF-F)
manually ground COF precursors at room temperature for 40 min in a [138].

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

Fig. 8. (I) Approach for the synthesis of three-dimensional COFs that incorporate ionic liquids (3D-IL-COFs). Reproduced with permission from 149. Copyright 2018
ACS. (II) Synthesis of TAPB-PTCDA COF and TAPB-PMDA COF in ZnCl2 under ionothermal conditions. Reproduced with permission from 150. Copyright 2020 Wiley.

Fig. 9. (I) Mechanochemical Synthesis of Thiadiazole Functionalized COF. Reproduced with permission from 138. Copyright 2024 ACS. (II) The process for creating
TpPa/PSF membranes through interfacial polymerization (IP) involves the following steps: (a) a diagrammatic representation outlining the steps to prepare the
TpPa/PSF composite membranes and (b) an image showcasing the physical characteristics of the synthesized TpPa/PSF composite membrane. Reproduced with
permission from 154. Copyright 2018 Elsevier.

Brown et al. (2023) introduced a green and efficient method for The COFs, Tp-Azo and Tp-Azo-BD(Me)2, were produced in 45 g batches
synthesizing COF using liquid-assisted mechanochemical techniques. with BET surface areas of 3345 m²/g and 2342 m²/g, and methane
This approach, which replaces hazardous solvents and high tempera­ storage capacities of 174.10 cc/cc and 151 cc/cc, respectively. The
tures with ball milling at ambient temperature, rapidly produces six method achieved consistent CH4 sorption with minimal variation and
imine-linked COFs with varying pore sizes and functionalities in just one stable adsorption-desorption cycles, showcasing the potential of COFs
hour. One COF achieved a surface area of 1387 m²/g in only 1 min of for efficient methane storage at room temperature and pressure and
milling. The COFs showed high iodine vapor adsorption capacities advancing sustainable energy storage solutions [156].
(6.4–7.1 g/g) and confirmed charge transfer interactions between iodine
and the COFs. This sustainable method offers a scalable solution for COF
3.6. Interfacial synthesis
production with potential environmental application [155].
Asokan et al. (2022) demonstrated the scalable synthesis of highly
Interfacial synthesis is a method used to create COFs by reacting
porous COFs for methane storage using a mechanochemical approach.
precursors at the interface of two immiscible phases, such as organic

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

solvents and aqueous solutions. This technique takes advantage of the method using ionic liquids (IL) as green solvents enables the synthesis of
unique environment at the interface, where reactants are concentrated, 3D-IL-COFs at suitable temperature and pressure with better reaction
to facilitate the formation of well-ordered COF structures. By controlling speed (e.g., 3 min for 3D-IL-COF-1). This approach allows the IL to be
factors such as the concentration of reactants, temperature, and the reused without activity loss [64].
nature of the interface, researchers can achieve high crystallinity and
precise control over the framework’s properties. Interfacial synthesis is 3.8. Synthesis on substrates
particularly useful for producing COFs with large surface areas, high
porosity, and tailored functionalities, making it an effective approach Creating free-standing thin films poses a considerable challenge
for developing advanced materials for various applications. Tp-Bpy, Tp- compared to the bulk synthesis of microsized crystals. These thin films
Azo, Tp-Ttba, and Tp-Tta are COF with distinctive structures. Tp-Bpy can be fabricated on various substrates, including single-layer graphene
uses pyridyl linkages, Tp-Azo features azobenzene groups, Tp-Ttba in­ (SLG) and 2D COF. Covalent organic frameworks are advanced polymer
corporates bulky tert-butyl groups, and Tp-Tta includes anthracene networks that assemble molecular building blocks into highly porous,
groups. Each framework has specific linkers and precursors to achieve layered structures. Their significant surface area and tunable porosity
unique properties for various applications. Tp-Bpy, Tp-Azo, Tp-Ttba, make them ideal for various applications, including organic optoelec­
and Tp-Tta were produced at the junction of two solvents, where TFP tronics, such as OLEDs and solar cells, and energy storage in batteries
was dissolved in dichloromethane. An aqueous solution containing and supercapacitors. COFs thus represent a promising avenue for
diamine or triamine and p-toluenesulfonic acid (PTSA) in a 7:3 water/ developing innovative materials in electronic and energy technologies
acetonitrile blend was layered over dichloromethane [157,158]. Wang [161]. Current synthetic methods produce COFs as either insoluble
et al. tackled the issues of COF particle agglomeration and extreme microcrystalline powders or oriented thin films on substrates like SLG.
synthetic conditions in the creation of COF-based separation mem­ In these processes, COF films form on graphene-coated and exposed
branes. They introduced a method utilizing interfacial polymerization areas, suggesting uncontrolled nucleation. However, improved poly­
(IP) directly on polymer substrates, akin to the conventional IP tech­ merization conditions have been found that selectively create COF films
nique used for polyamide (PA) membranes (Fig. 9 (II)). By achieving a on SLG. This advancement enables the growth of COF films on litho­
moderate reaction rate between monomers in both aqueous and organic graphically patterned SLG substrates, offering insights into the unifor­
phases, they facilitated the conformation-specific growth of COF crys­ mity of film growth and the factors affecting nucleation and growth. The
tallites onto polysulfone (PSF) ultrafiltration substrates in just one selective fabrication of COF films on patterned substrates enables their
minute. The synthesis parameters, such as reaction time and precursor integration into devices and non-selective application on various sur­
concentrations, were carefully optimized [154]. faces, including highly oriented pyrolytic graphite (HOPG), metal sub­
In contrast, the COF TTA-DHTA film was created by dissolving the strates like Ag(111) and Au(111), copper foil, glass, 3D graphene,
monomer 4,4,4-(1,3,5-triazine-2,4,6-triyl)trianiline (TTA), the Sc(OTf)3 porous ceramic α-Al2O3, and amine-modified reduced graphene oxide
catalyst, and aqueous acetic acid solution. This solution was then spread (NH2− rGO). COFs are a new class of porous polymers featuring distinct
over a hydrogel that had been immersed in the oil phase of 2,5-dihydrox­ two or three-dimensional channels. Wang et al. highlighted that despite
yterethaldehyde (DHTA) [158]. This process produces films ranging in significant progress in COF powder synthesis, the development of
thickness from 4 to 150 nm. The Suzuki coupling reaction recently COF-based separation membranes is hindered by particle agglomeration
synthesized 2DCCOF1 and 2DCCOF2 containing C-C links [75]. and strict synthesis conditions. This research employed interfacial
Synthesis under Ambient Conditions: Synthesis under ambient polymerization (IP) directly on polymer substrates, enabling rapid,
conditions involves the formation of COF without the need for extreme controlled growth of COF crystallites alongside PSF ultrafiltration sub­
temperatures or pressures, using standard laboratory environments. strates within just one minute due to moderate reaction rates between
Recent work has demonstrated significant advancements, such as monomer pairs in both aqueous and organic solutions. The optimized
developing ambient-condition synthesis methods that enable rapid and synthesis parameters, including reaction time and precursor concen­
efficient COF formation. Liu et al. (2023) reported a new approach for trations, led to a COF/PSF membrane achieving an impressive Congo red
synthesizing imine-linked COFs at room temperature using simple sol­ dye rejection rate of 99.5% and a water permeance of 50 L/m²/h/ bar,
vents and catalysts, drastically reducing the reaction time and surpassing other membranes with similar rejection capabilities by 2 to
improving scalability [18]. Similarly, Zhang et al. (2022) synthesized 10 times. This simple interfacial polymerization method aims to support
robust COFs using aqueous solutions and mild conditions, facilitating the scaling up and practical use of COF-based membranes in real-world
the incorporation of various functional groups without requiring applications [162].
specialized equipment. These advancements in ambient-condition syn­
thesis are expanding the practical applications of COFs by making the 4. Synthetic strategies for functional COFs
production process more accessible and environmentally friendly [31].
COFs are typically synthesized under solvothermal conditions, but Chemically, COFs are entirely designable. Bottom-up and post-
ambient temperature synthesis benefits fragile or sensitive substrates modification strategies can effectively tailor their skeletal and physi­
[88]. Room-temperature vapor-assisted synthesis can effectively pro­ cochemical properties, facilitating functional design to address specific
duce boroxine-based COF films. For instance, BDT-COF and COF-5 thin environmental needs.
films can be created by drop-casting a combination of acetone and
ethanol (150–200 μL) of COF precursors onto a clean glass substrate, 4.1. Bottom-Up technique
then placing the substrate in a desiccator with mesitylene and dioxane
(1/1 v/v) for 72 h [159]. Metal triflates, such as Sc(OTf)3, are efficient COFs have emerged as a promising class of porous materials due to
catalysts for rapidly synthesizing imine-linked 2D COFs at ambient their tunable structures, high surface areas, and potential applications in
temperature. For example, the TAPB-PDA COF can be synthesized in just catalysis, gas storage, and separation. The bottom-up synthesis tech­
10 minutes using a mixture of 1,4-dioxane and mesitylene (4:1 v/v), nique plays a crucial role in their development by facilitating the as­
avoiding the high temperatures (>70 ◦ C) and long reaction times (>24 sembly of molecular building blocks into extended frameworks. This
h) required by traditional methods. Similarly, imine-linked COF-LZU1 method offers significant advantages, including structural diversity and
can be prepared at room temperature by polycondensing 1,3,5-trifor­ tunability, as demonstrated by Côté et al. (2005), who synthesized
mylbenzene (TFB) and p-phenylenediamine (PPDA) in a CO2/water highly crystalline COFs using boronate ester linkages, paving the way for
solvent at 4.5 MPa for 24 h [160]. While the synthesis of 3D COFs has further advancements with imine, hydrazone, and triazine linkages [3,
been limited to high-temperature solvothermal techniques, a new 163]. The bottom-up approach has been instrumental in achieving high

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surface areas, as illustrated by COF-LZU1, which exhibited a surface area directions include developing milder and scalable chemical conversion
of over 2000 m2/g and exceptional gas storage properties while also methods and exploring new types of chemical conversions, such as
allowing for functionalization and post-synthetic modifications. For introducing redox-active groups for enhanced electrochemical
example, stable keto-enol-linked COFs developed by Kandambeth et al. properties.
(2012) enhance their applicability in catalysis and sensing [70]. Despite
these contributions, challenges exist, including issues with crystallinity 4.2.4. Host-guest modifications
and stability, as some COFs suffer from poor order and susceptibility to Host-guest modifications involve incorporating guest molecules into
hydrolysis. Additionally, there are scalability and reproducibility con­ the pores of COFs to enhance their functionality for specific applications
cerns due to complex synthesis conditions involving high temperatures such as drug delivery, gas storage, and sensing [180]. This approach has
and toxic solvents, along[164] with limited control over macroscopic been employed to create COF-based drug delivery systems with high
morphology, which restricts their use in applications requiring specific drug-loading capacities and controlled release profiles. Huo et al.
structural forms [165]. Addressing these limitations necessitates novel developed hollow COF nanospheres that encapsulated doxorubicin and
synthetic strategies that integrate the bottom-up approach with exhibited pH-sensitive release, making them effective for cancer therapy
improved crystallization methods, enhanced stability, and better [181]. However, the stability of host-guest systems under real condi­
morphology control, potentially through hybrid strategies that combine tions, such as exposure to moisture or mechanical stress, remains a
bottom-up synthesis with top-down processing techniques to unlock concern. COF-MOF composites show high CO2 adsorption, but their
COFs’ full potential for real-world applications [166]. performance decreases over time due to the leaching of MOF particles
[182]. Therefore, developing more robust host-guest systems and
4.2. Post-synthetic method (PSM) exploring new types of guest molecules, such as biomolecules or nano­
particles, is essential to create multifunctional COFs with enhanced
PSM is a good method to enhance the functionality and tailor the properties for biomedical and environmental applications.
properties of COFs for specific applications. PSM strategies are catego­ Post-synthetic methods have significantly advanced the functionality
rized into four groups: post-functionalization, post-metalation, chemical and application range of COFs. However, challenges such as stability,
conversion, and host guest modifications [167]. scalability, and precise control over modifications remain. Addressing
these limitations through new synthesis methods will be crucial for the
4.2.1. Metalation future development of COF-based materials.
Metalation involves the coordination of metal ions to ligand sites
within COFs that can significantly enhance their catalytic, sensing, and 4.3. Blending method
gas storage properties. For example, nitrogen atoms in imine-linked
COFs can donate lone-pair electrons to bind with metal ions such as The blending method, which combines COFs with metals, CNTs,
Pd2+, Fe2+, Co3+
, and Ni2+, which are effective catalysts in various re­ MOFs, and graphene, provides a versatile approach to enhancing the
actions [168]. Metalation has been successfully used to create properties of COFs for various applications. Blending COFs with metals
COF-based heterogeneous catalysts with high stability, and recyclability like Fe3O4 improves magnetic properties, enabling easier recovery in
challenges such as metal leaching and harsh synthesis conditions remain environmental remediation, but some challenges, such as nanoparticle
[169]. Pd NPs supported TpBpy COFs show exceptional catalytic per­ aggregation and stability under harsh conditions, remain unresolved
formance in hydrogenation reactions, but the gradual loss of Co2+ ions [183,184]. Integrating COFs with CNTs enhances electrical conductivity
over multiple cycles limited their practical application [170–172]. and mechanical strength, making them suitable for energy storage, yet
Future directions include developing more robust coordination strate­ achieving uniform dispersion of CNTs within the COF matrix is difficult,
gies and exploring new metal ions to enhance stability and performance. and the high cost of CNTs limits scalability [185,186]. Blending COFs
with MOFs creates hybrid materials with superior porosity and gas
4.2.2. Functionalization adsorption capabilities, but these composites often suffer from structural
Functionalization involves adding extra functional groups to COFs degradation in humid environments, raising concerns about their
through post-synthetic modifications, increasing their physical and long-term stability [187]. Graphene, another promising blending part­
chemical properties. Common methods include addition reactions and ner, improves electrochemical performance in energy storage applica­
substitution reactions [173]. Functionalization has significantly tions, but the use of toxic reducing agents and issues with graphene
increased the application range of COFs, such as improving proton restacking hinder its practical application [188]. While the blending
conductivity for fuel cells or enabling high sensitivity in sensing appli­ method holds great promise, challenges such as uniform dispersion of
cations [174,175]. However, introducing bulky functional groups can blending materials, long-term stability, and environmentally friendly
disrupt crystallinity and porosity, reducing surface area and adsorption synthesis need to be addressed. Optimizing synthesis strategies to
capacity [176]. For example, while carboxyl groups enhanced CO2 overcome these limitations and fully realize the potential of COF-based
adsorption, they also decreased the BET surface area of the COF [177]. composites in advanced materials development is needed.
There should be a focus on milder functionalization methods and
exploring the synergistic effects of multiple functional groups to create 5. Applications of COFs
multifunctional materials.
COFs are an innovative class of crystalline materials characterized by
4.2.3. Chemical conversion their highly ordered, porous structures composed of light elements such
Chemical conversion involves transforming one type of linkage as carbon, hydrogen, oxygen, nitrogen, and boron. Due to their modular
within COFs into another to improve stability or introduce new func­ and tunable architecture, COFs offer exceptional versatility and per­
tionalities [178]. Imine-linked COFs can be converted into more stable formance in various applications. They are particularly valuable in
amide-linked COFs through post-synthetic treatment [179]. This environmental applications, such as water purification, where they can
approach yields good results in enhancing stability, as shown by Waller efficiently adsorb and degrade organic pollutants due to their high
et al., which improved the stability of 2D COFs in acidic and basic en­ surface area and customizable pore sizes. In addition to environmental
vironments. However, the conversion process often requires harsh remediation, COFs are used in gas storage and separation, catalysis, and
conditions that can degrade the COFs’ structure and reduce crystallinity. sensing, leveraging their chemical stability and functional diversity. The
For instance, converting imine-linked COFs to thiazole-linked COFs ability to tailor the chemical functionality and pore environment of
improved stability but reduced porosity and surface area. Future COFs makes them promising candidates for advanced materials in

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energy storage and drug delivery, underscoring their broad potential H2 can be stably absorbed on both sides of a Li-decorated COF-1 unit
across various scientific and industrial fields. The development of cell, resulting in a storage capacity of 5.26 wt.% [199]. Another study
functional COF materials is presented in this section (Table 4). examined five boron-phosphorus (BP) cube-based COFs, revealing that
BP-COF-4 and BP-COF-5 have superior hydrogen adsorption capacities
5.1. Gas storage compared to BP-COF-1, BP-COF-2, and BP-COF-3 at temperatures of 77
K and 298 K. Numerical Monte Carlo and grand canonical Monte Carlo
COF are highly effective for gas storage due to their porous, crys­ simulations were used to evaluate structural parameters and hydrogen
talline structures and tunable properties. They demonstrate exceptional adsorption properties, suggesting further enhancements for
hydrogen storage capabilities, making them vital for hydrogen fuel high-performance hydrogen storage materials [200]. Additionally, a
systems. COFs’ high surface area and customizable pore sizes optimize comprehensive review noted that while current hydrogen storage
gas uptake and stability. Additionally, COFs are advantageous for methods face high costs and safety risks, advanced sorbents such as
methane storage, enhancing natural gas applications by selectively MOFs, COFs, porous carbon-based adsorbents, zeolites, and composites
adsorbing methane over other gases. They also improve carbon dioxide show promise. MOFs can achieve up to 10 wt.% hydrogen storage, COFs
storage, aiding in carbon capture and sequestration efforts. COFs’ up to 6 wt.%, and porous carbon-based adsorbents between 3 and 5 wt.
versatility, high storage capacities, recyclability, and stability make %, with high-entropy alloys and machine-learning techniques
them sustainable and cost-effective for long-term gas storage [197]. enhancing stability and optimization [201].
Alharbi et al. (2023) examined the effectiveness of COFs in mitigating
hazardous gases like ozone (O₃) and nitric oxide (NO), which have 5.1.2. Methane storage
increased due to industrial growth. Traditional methods, such as cata­ COF exhibits good methane storage properties because of their high
lytic decomposition and zeolites, are insufficient, prompting the need for surface areas and tunable pore structures. The ability of these materials
new materials. The study employed first-principle calculations and DFT to be functionalized with given functional groups further enhances the
to analyze these gases’ binding energies and interactions with nitrogen selective adsorption of methane, and thus, it works efficiently for natural
and π-bond-containing COFs. The findings revealed that COFs bind more gas applications. COFs can afford very good capacities for methane
strongly with O₃ than with NO, suggesting their potential for effectively storage at relatively low pressures, increasing efficiency and safety in
sensing and removing specific gases in mixed environments [198]. methane storage and transport. Therefore, it underscores their practi­
Table 4 outlines various applications of COFs in gas storage. cality in sustainable storage solutions for methane concerning stability
and recyclability. Do et al. demonstrated a design strategy (Fig. 10) for a
5.1.1. Hydrogen storage new COF by replacing silicon in zeolites with carbon through thiophene,
COF are highly promising for hydrogen storage due to their high furan, and pyrrole linkers, resulting in 300 ZCOF structures with 100
surface areas, tunable pore sizes, and robust covalent bonds. Their or­ zeolite topologies. Key porous parameters, including accessible surface
dered and porous structures allow efficient hydrogen adsorption and area, pore size, and pore volume, were analyzed using Zeo++ software
storage, essential for hydrogen fuel systems. The customizable nature of to assess the quality of the ZCOF materials. The results revealed that
COFs enables the incorporation of functional groups that enhance ZCOFs have a larger surface area than zeolites, which is advantageous
hydrogen binding, improving adsorption at low pressures and temper­ for methane storage [202]. Recent studies highlight advances in
atures. COFs also exhibit excellent stability and recyclability, making methane storage using COFs. Zhang et al. (2021) utilized computational
them sustainable and cost-effective for long-term hydrogen storage. materials screening combined with machine learning to evaluate the
Recent studies highlight the potential of COFs for hydrogen storage. methane storage capacities of 404 and 460 COFs at 298 K.
One study focused on 2D COF-1, finding that lithium (Li) decoration High-throughput simulations and various ML algorithms identified the
significantly enhances hydrogen storage capacity to 7.69 wt percent (wt. random forest model as the most accurate for predicting storage per­
%). Ab initio molecular dynamics simulations at 300 K showed that 12 formance. This model highlighted key features influencing storage

Table 4
Various applications of COF in gas storage.
Gas COF Type Features Ref.
storage

H2 Sc-COF 108 H2 molecules were adsorbed and [189]

8.43% storage capacity
H2 Cu(I)–COF- ​ [190]
301
H2 CTFs 4.02 wt.% storage [191]
H2 COF-320 Li-doped COF-320 can reach 0.725 wt.% at [192]
298 K and 100 bar
H2, CH4, COF-102 72 mg/g at 77 K, 187 mg/g at 298 K, and [193]
CO2 1180 mg/g at 298 K for H2, CH4, CO2
COF-1 15 mg/g at 77 K, 40 mg/g at 298 K, and 210
mg/g at 298 K for H2, CH4, CO2
COF-5 36 mg/g at 77 K, 89 mg/g at 298 K, and 779
mg/g at 298 K for H2, CH4, CO2
COF-6 23 mg/g at 77 K, 65 mg/g at 298 K, and 298
mg/g at 298 K for H2, CH4, CO2
COF-8 35 mg/g at 77 K, 87 mg/g at 298 K, and 598
mg/g at 298 K for H2, CH4, CO2
H2 3D-COF-320 H2 selective with high permeance of 5.67 × [194]
107 mol/(m2 s Pa)
I2 COF up to 481 wt.% [193]
H2 Li-doped Pc- 24 H2 molecules can be adsorbed in one [195]
PBBA COF formula unit
CO2 TpPa-COF 5.1 mmol/g at 273 K under 1bar pressure [196]
Fig. 10. Zeolite-COFs for methane storage. Reproduced with permission from
​ ​ ​ ​
202. Copyright 2023 MDPI.

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

capacity and identified top-performing COFs with deliverable capacities Ahmed et al. synthesized three novel β-ketoenamine-linked COFs
surpassing existing adsorbents [203]. Mercado et al. (2018) developed a through Schiff-base [3 + 3] polycondensations of 1,3,5-triformylphloro­
database of 69,840 novel COFs, evaluating their methane storage po­ glucinol (TFP-3OHCHO) with three derivatives featuring tris(amino­
tential through simulations. The top COF showed a deliverable capacity phenyl) units—specifically, amino, carbazole, and pyridine units
of 216 v(STP)/v at 65 bar, exceeding the current best materials [204]. (Fig. 12(I)). The resulting TFP-COFs exhibited impressive properties,
Do et al. (2020) designed zeolite-based COFs (ZCOFs) by substituting including high electrochemical specific capacitances of up to 291.1 F/g,
silicon with carbon in linkers, resulting in 300 structures with varying CO2 absorption efficiency reaching 200 mg/g at 273 K, a large BET
surface areas and pore sizes. Simulations identified two ZCOFs—JST-S specific surface area of up to 686 m²/g, and remarkable crystallinity.
183 and NPT-S 177—as promising candidates for methane storage due Stronger quadrupolar contact with the incorporated CO2 molecules was
to their high adsorption performance [202]. caused by the hexagonal structures of the resulting COFs having more
strongly planar monomer units [206].
5.1.3. Carbon dioxide storage Chao Liang added the tentacle-like COF to the Pebax matrix as a filler
In addition to the high surface area and tunable porosity due to to separate CO2 from CH4. The COF forms effective CO2 capture nano­
organic linking, the COFs offer a vital extension in functionality traps in the MMMs because it has a lot of Lewis base sites (O and N
regarding carbon dioxide storage. These engineered, discrete COF ma­ atoms) and porous pores. DFT calculations and the Grand Canonical
terials have desired functional groups on the pore walls, making them Monte Carlo (GCMC) simulation both support the idea that CO2 capture
chemically stable and enhancing their adsorption capacity and selec­ nanotraps aid in CO2 transport in MMMs. Concurrently, the surface of
tivity toward carbon dioxide. COFs have the potential for large CO₂ the tentacle-like COF is covered in CO2 capture nanotraps, enhancing
adsorption across various pressures and temperatures, making them the CO2 capture capability. As a result, Pebax/COF MMMs, (Fig. 12(II)),
very promising for carbon capture and sequestration. Their singular performed better at CO2 gas separation than the pure Pebax membrane.
structural versatility allows for optimizing the pore environment to The MMM, including 3 wt.% COF loading outperformed the pure Pebax
maximize CO₂ storage efficiency, which is potentially useful in light of membrane regarding selectivity and permeability, measuring 73.4% and
the rising challenges of climate change and environmental sustainabil­ 32.9% higher, respectively, for CO2 gas separation. Therefore, the
ity. To enhance the effectiveness of CO2 adsorbents, Hansheng Chen tentacle-like COF used to produce the CO2 capture nanotraps in the
employed a linkage engineering technique to transform imine-bonded MMMs demonstrated a promising potential for CO2 separation [207].
COFs into amide-bonded COFs (Fig. 11). This conversion led to a sig­ Aqi Riaz showed that using a porous COF-TpPa-1 improved CO2
nificant increase in CO2 uptake capacity, rising from approximately 55 permeability and selectivity. To create COF-TpPa-1/PIM-1 MMMs
mg/g to around 235 mg/g, while the N2 uptake capacity remained (Fig. 12), they described a new PIM-1 mixed with COF-TpPa-1 in a range
largely unchanged. Also, breakthrough experiments significantly of 0–10 wt.%. The PIM-1 matrix and COF-TpPa-1 particles were
improve the CO2/N2 separation performance. According to Monte Carlo compatible, producing perfect interfacial morphology. The MMMs with
simulations and density-functional theory calculations, the key to the 7 wt.% COF-TpPa-1 have an optimal CO2/N2 selectivity of 20.1 among
enhanced performance is the interaction between the carbonyl group in the five investigated compositions and a CO2 permeability of 6336
the amide segment and the CO2 molecule. this work offers a simple and Barrer, an improvement of 104% over the pristine sample. After 30 days
effective method for designing COFs’ structural elements for carbon of age, the CO2/N2 selectivity of the COF-TpPa-1 7 wt.% doped mem­
capture applications [205]. brane was 88% higher than that of pristine PIM-1, and it also exhibited

Fig. 11. Conversion from imine to amide linkage in COFs. Reproduced with permission from 205. Copyright 2025 Elsevier.

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

Fig. 12. (I) Synthesis of three β-ketoenamine-linked COFs—the TFP-TPA, TFP-Car, and TFP-TPP COFs—from TFP-3OHCHO and tris(aminophenyl) derivatives with
different degrees of planarity. Reproduced with permission from 206. Copyright 2018 Elsevier. (II) The synthesis diagram of TPDH-COF. Reproduced with permission
from 200. Copyright 2024 Elsevier.

good mixed-gas separation and anti-plasticization qualities [208]. environmentally sustainable management [209].
Recent studies highlight advancements in ammonia (NH₃) storage
5.1.4. Ammonia storage using COF. Tian et al. (2021) demonstrated that COFs can effectively
COF are such materials that, owing to their features of high surface store ammonium ions (NH₄⁺) with a good capacity of 220.4 mA h/g with
area, tunable pore sizes, and chemical stability, make them quite 0.5 A/g current density. The study identified a universal mechanism
effective in storing ammonia. Their porous and crystalline nature en­ involving hydrogen bonds between nitrogen and oxygen, which en­
ables the effective adsorption of ammonia. This can be important in hances NH₄⁺ ion storage and guides the design of COFs for better elec­
applications such as energy storage or other industrial processes. trochemical energy storage [210]. Fu et al. (2023) introduced
Customizing the chemical functionality of COFs can increase their ca­ zwitterionic COFs for ammonia storage and separation, achieving a
pacity to adsorb and retain ammonia by a huge margin. This would record-high adsorption capacity of 44.98 mmol/g at 25 ◦ C and 1 bar.
involve the optimization of pore environments, as well as the inclusion The COFs’ cationic and anionic groups enable efficient NH₃ storage and
of those functional groups that can improve ammonia binding and separation from NH₃/CO₂/N₂ mixtures with fully reversible adsorption.
storage capacities. In this context, COFs offer a highly workable solution The work advances COF-based adsorbents for effective ammonia man­
for ammonia storage, facilitating advanced energy systems and agement in industrial applications [211].

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

COFs have demonstrated exceptional potential for gas storage ap­ various functional groups to optimize properties such as ionic conduc­
plications, particularly for hydrogen, methane, and carbon dioxide tivity and energy density, positioning them as promising materials for
(Table 4). Their high surface area, tunable pore sizes, and chemical advanced energy storage solutions (Table 5). Various innovative design
stability make them ideal candidates for energy storage and environ­ strategies have emerged to further enhance their electrochemical
mental remediation. COFs have shown exceptional gas storage and properties, as emphasized by the scientific community [217].
separation promise due to their high surface areas, tunable pore struc­ COFs have emerged as promising materials for energy storage,
tures, and functionalization capabilities. For example, 3D COFs like particularly in supercapacitors and rechargeable batteries. High
COF-102 and COF-103 exhibit superior methane (25 wt%) and hydrogen porosity, redox-active sites, and tuneable functionalities enable efficient
(72.4 mg/g) storage capacities. In contrast, COF-based membranes such charge storage and ion transport. Imine-linked π-conjugated COFs such
as the 3D COF-320 membrane demonstrate high H2 selectivity with a as TFPh-NDA and Phos-COF-1 as advanced electrode materials for
5.67 × 107 mol/(m2s Pa) [212–214] permeance. Mixed-matrix mem­ supercapacitors. TFPh-NDA IC-COF exhibited a high specific capaci­
branes like those developed by Shan et al. further highlight COF’s po­ tance of 583 F/g and energy density (280.58 Wh/kg with 98% capaci­
tential for selective CO2/CH4 separation [215]. However challenges tance retention after 10,000 cycles highlighting its stability and
such as low adsorption capacities at ambient conditions and long-term efficiency [243]. Phos-COF-1 demonstrated a specific capacitance of 100
stability under real-world conditions need to be addressed. Future F/g and excellent rate capability (75% retention at higher current den­
research should focus on optimizing COF structures for enhanced gas sities) attributed to its porous structure and strong π-π interactions.
uptake and developing scalable synthesis methods for industrial appli­ These results underscore the advantages of COFs including high surface
cations [216]. area and efficient charge transport for energy storage [244]. However,
challenges such as low electrical conductivity and cycling stability
remain. Future research should focus on integrating COFs with
5.2. Energy storage conductive materials and optimizing their electrochemical performance
for practical energy storage devices. Given the growing need for
Recent advances in COF for energy storage demonstrate their high-performance energy storage technologies, COFs have the potential
applicability across a variety of applications. COFs have attracted sig­ to completely transform the energy sector and captivate researchers and
nificant attention due to their unique characteristics and diverse uses. enthusiasts.
These frameworks showcase uniform porosity, multifaceted function­
ality, and intricate design possibilities. However, their true significance 5.2.1. Supercapacitors
lies in their porous architecture, which facilitates efficient charge and As COFs become more commonplace, there is excitement about their
mass transport while displaying notable reversible redox activity. COFs potential to revolutionize supercapacitor technology, leading to greener
have gained considerable interest for their potential in electrochemical and more efficient energy storage solutions than ever before. Zhang
energy storage devices, including supercapacitors and rechargeable et al.’s [245] ground-breaking method is a proof of method for using
batteries. Their porous structure and large surface area enhance charge COF structures demonstrating a significant breakthrough in energy
storage capabilities, enabling rapid ion transport and improved capac­ storage. The main focus of their investigation was synthesizing two
itance in supercapacitors. Additionally, COFs can be tailored with

Table 5
Energy storage application of COF.
Electrode Material Application Specific Capacitance Energy Density (W Redox Sites Capacitance Retention Ref.
(F/g) h/kg) (%)

COF/rGO Supercapacitor 321 10.3 Oxygen functional group on rGO ​ [218]

Hex-Aza-COF-2 Supercapacitor 663 23.3 quinone and phenazine redox moieties 89 [219]
N-doped carbon/g-C3N4 Supercapacitor 835.2 45.97 ​ 86.5 [220]
DBT-MA-COF Supercapacitor 407 ​ quionine ​ [221]
COF@rGO Supercapacitor 451.96 44.22 Oxygen functional group on rGO ​ [222]
Boron based COF Supercapacitor 15.3 μF/cm2 ​ Electron deficient boron atom ​ [223]
2D COF (TAPA- TPT) Supercapacitor 205 ​ ​ 95 [224]
TTT-DHTD COF Supercapacitor 273.3 ​ quinone groups, sulfur-containing 50 [225]
thiophene moieties
Pent-TRUX-DAB Supercapacitor 634 ​ - 92 [226]
Triazine based2D polyimide Supercapacitor 130 32.55 - 88 [227]
COF
2
CNT@COF Supercapacitor 376.2 30.7 μWh cm− anthraquinone ​ [228]
COF@rGO Supercapacitor 451.96 44.22 ​ 94.02 [229]
Phos-COF-1 Supercapacitor 100 ​ phosphine ​ [230]
PP/rGO Supercapacitor 360.4 ​ Phosphine group and oxygen group of rGO ​ [230]
ILCOF-1 Supercapacitor 321 ​ oxygen group of rGO ​ [231]
​ ​ Capacity (mAh/g) ​ ​ Capacity Retention ​
(%)
3D-flu-COF Batteries 1249 ​ ​ ​ [232]
COF-PDA/SWCNT/PP Batteries 1031 75.87 Polysulphide, quinone 72.3 [233]
COF extended π conjugate Batteries 1617 ​ ​ 55 [234]
TpPa-SO3Li Batteries 822.9 ​ Sulfonate sites 78 [235]
P-COF@SWCNT Batteries 438 ​ ​ ​ [236]
COF@graphene Batteries 188 ​ Oxygen functional group on rGO ​ [237]
truxenone-based COF Batteries 268 ​ Truxenone, 99 [238]
β-ketoenamine moietie and carbonyl
groups
BQ1-COF Batteries 502.4 1033 C=O and C=N 81 [239]
Tp-Azo-COF Batteries 529.5 ​ N=N and C=O ​ [240]
TQBQ-COF Batteries 452 ​ C=O and C=N ​ [241]
TB-COF Batteries 1390 ​ polysulfides 68 [242]

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

different COF films with distinctive structures and properties. The for the fabricated COF/carbon composite foam. Furthermore, it dem­
A-COF film was the first to show mesoporous properties with imine bond onstrates exceptional long-term stability, retaining nearly 100% capac­
connections, whereas the B-COF film showed microporous properties itance after 20,000 charge-discharge cycles at 10 A/g, highlighting its
with β-ketoenamine linkages. This study is unique in that it cleverly strong cycling performance and mechanical durability. The composite’s
assembles superlattices employing these COF films as self-supported robustness, elasticity, electrical conductivity, and redox activity stem
electrodes, utilizing the complementary interactions between two from the conductive carbon skeleton and the redox-active properties of
pseudo-capacitance energy storage mechanisms and electrochemical the 2D COF [247].
double-layer capacitance. The design idea was twofold: (1) long-range Using these foam features in flexible supercapacitors can achieve
periodic superlattices with uniform nano-thickness could be created excellent electrochemical performance. Thanks to the controlled growth
because of the bending and stacking capabilities of the covalent bonds of COF on the carbon framework and the use of melamine foam as a
inside the COF structures. This arrangement enables excellent ion access template, new options for creating mechanically robust and electrically
to the inner surfaces of the active sites. Additionally, superlattices allow conductive composite materials are available. The synergistic combi­
for the unrestricted assembly of COF films, leveraging the cumulative nation of carbon and energy harvesting components could advance
effect of each layer to enhance electrochemical properties. The resulting supercapacitor technology, developing flexible energy storage devices
interdigital supercapacitor device revealed a noteworthy characteristic: with excellent performance.
the superlattices were arranged in a distinctive "nano-hourglass" ABA Alumina has recently been investigated by Xu et al. [248] as a base
steric structure. This configuration promotes fast charge transport and substrate for COF-based materials development for electrodes used in
accumulation at the heterojunction interface by utilizing supercapacitors. They started by altering the surface of β-Al2O3, then
geometry-induced phenomena. The overall development of energy grafted a two-dimensional highly conjugated DHTA-COF material onto
storage is aided by the interaction between faradaic redox processes and the altered alumina substrate (Fig. 13c). 50% Al2O3@DHTA-COF, the
the electrochemical double-layer. resultant electrode material, showed remarkable characteristics, such as
Moreover, at a scan rate of 10 mV/s, the resultant micro- a large specific surface area along with strong conductivity. The COF’s
supercapacitor (MSC–ABA–COF) showed remarkable inherent volu­ electrochemical energy storage performance was improved by this
metric capacitance, reaching 927.9 F/cm3. It also demonstrated excep­ combination. Tested at 0.5 A/g, the 50% Al2O3@DHTA-COF composite
tional bending resistance, with a performance value of 63.2 mWh/cm3. showed an impressive specific capacitance 9.6 times higher than that of
With exceptionally high activity, the superlattice demonstrated θ-Al2O3–CHO and DHTA-COF, respectively. This demonstrates the
remarkable performance as flexible electrodes for in-plane super­ considerable enhancement made possible by the COF structure’s inte­
capacitors. These COF-based superlattices’ exceptional qualities and gration of alumina hybridization.
cooperative effects signify a major advancement in the creation of Even after 6000 charge-discharge cycles, the electrodes coated with
cutting-edge energy storage technologies. In a similar spirit, Dong et al. alumina demonstrated significant capacitance and exceptional long-
[246] described a novel method for producing a hierarchically porous term cycling stability. The authors observed that after this extended
three-dimensional carbon framework using melamine foam as a tem­ cycling, the capacitance retention rate remained at approximately 92%,
plate. This scaffolding supports the homogeneous growth of indicating that the hybridization with θ-Al2O3 has enhanced the elec­
well-defined porous 2D COFs, forming an elastic and mechanically trochemical energy storage in the COF. The development of superior
strong composite foam for compressive and bending supercapacitors. supercapacitor electrode materials has advanced considerably through
Melamine foam was first used to load graphene oxide efficiently. After the effective integration of COFs into composite materials and the use of
that, the foam was carbonized to create a carbon framework wrapped alumina as a substrate. This study improves the design of high-
with graphene. performance energy storage devices by optimizing capacitance and
This process results in a composite foam featuring a hierarchical long-term stability. Its findings highlight innovative strategies for
porous structure composed of carbon and 2D COF, which forms spon­ enhancing energy density and cycling stability, which are crucial for
taneously and uniformly along the carbon skeleton’s surface. The carbon applications in electric vehicles and renewable energy systems.
fiber/CF/carbon composite foam exhibits impressive characteristics. Khayum et al. [251] advanced the field of flexible solid-state
The authors reported a significant capacitance of 129.2 F/g at 0.5 A/g supercapacitors by introducing a novel synthetic technique for

Fig. 13. (I). Schematic illustration of the endogenous Tf corona-mediated DOX@COF-PEG-T10 for a cascade-targeting glioma drug delivery across the BBB.
Reproduced with permission from 249. Copyright 2020 Elsevier. (II) Diagrammatic representation of the process used to prepare MGPPCLP and the associated
method of controlled drug delivery to get past the reflux and matrix barriers in the treatment of pancreatic cancer. Reproduced with permission from 250. Copyright
2022 Wiley.

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

producing structurally resilient and redox-active 2D COFs, known as confined ILs inside the COF pores exhibited superior transport charac­
CT–Dq1Da1Tp COF. This innovative method is based on a simple and teristics compared to the pure PIL system. Both ion mobility and total
scalable mechano-chemical mixing approach, eliminating the need for conductivity improve by confining ILs within COFs. Furthermore, dur­
binders or additives. ing charge-discharge testing, the IGE-COF composite displayed
The resulting convergent COF thin sheets are redox-active due to the outstanding rate performance and long-term stability, maintaining
Dq linker and are mechanically resilient because of the π-electron-rich performance for up to 800 cycles at a rate of 1C (Fig. 15d).
Da moieties. Convergent COFs are significant because they attain the According to these results, COFs have the potential to serve as
necessary mechanical strength and flexibility while preserving high effective fillers in PIL/IL-based IGEs, enhancing the longevity and con­
crystallinity and porosity, both of which are essential for solid-state ductivity of lithium metal batteries (Fig. 15e). This work also illustrates
supercapacitors. With a capacitance retention of 90% even after 2500 how COFs can help address the limitations of conventional electrolyte
cycles, the CT–Dq1Da1Tp COF demonstrated exceptional long-term systems by significantly improving conductivity and stability.
cyclic stability, according to the researchers. Remarkably, the device Su et al. [257] developed a multilayer COF structure featuring two
maintained 78% of its initial capacitance value even after 7000 charge- functional groups to serve as an anode material in potassium-ion bat­
discharge cycles, showcasing its strong performance over prolonged use. teries (PIBs). The COF was synthesized through the reaction of aldehyde
By employing this innovative synthetic approach, Khayum et al. groups with amino groups to create imine bonds, and the reaction of
expanded the possibilities for the logical design of redox-active mate­ carboxyl groups with amino groups resulted in amidogen linkages. Their
rials in flexible supercapacitor devices and successfully demonstrated findings revealed that amidogen bonds generated more redox-active
the synthesis and fabrication of mechanically resilient 2D COFs. This sites, enhancing the diffusion of K+ ions and increasing the specific ca­
cutting-edge strategy could fundamentally alter the development of pacity; however, imine bonds exhibited lower solubility in electrolytes.
high-performance energy storage systems, producing more adaptable Overall, the multilayer COF structure improved both charge and ion
and efficient supercapacitors for future applications. transport. According to experimental results, the dual functional groups
Li et al. surveyed a crystalline COF with dithiophenedione moieties, produced superior electrochemical performance than the single func­
TTT-DHTD. Further, they demonstrated that it exhibited superior per­ tional group. The COF demonstrated exceptional cycle stability and a
formance in supercapacitors than a COF with dimethoxybenzene- high charge-specific capacity of 229.5 mA h/g when used as an anode in
dithiophene (TTT-DMTD) due to its high capacitance, reaching up to photoion batteries.
273.3 F/g at 0.5 A/g and 163.7 F/g at 10 mV/s. Ding et al. (2022) Sun et al. summarized the research progress of COFs in stabilizing
reviewed prospects in 2D COFs about their tunable porosity, huge sur­ metal anodes. Special attention has been given to the application of
face area, and stability. They indicated that redox-active and π-electron- COFs in the design of metal anode hosts, artificial solid electrolyte in­
rich 2D COFs readily facilitate charge carrier hopping and ion migration, terfaces, electrolyte additives, solid-state electrolytes, and separator
rendering them very efficient in supercapacitors, fuel cells, and various modifications [258,259].
metal-ion batteries (H. Ding et al., 2022). Kim et al. [260] presented a fluorine-rich F-COF as a possible elec­
trode material for PIBs. The kinetics of K+ ion intercalation were
5.2.2. Rechargeable secondary batteries improved by adding fluorine atoms to the structured framework, which
The quest for alternatives to conventional organic battery electrodes also increased redox activity and K+ ion interactions. As a result, the
is driven by limitations like slow ion diffusion, low electrical conduc­ ionic character of the CF bond underwent a reversible shift from
tivity, and poor cycling stability. Consequently, researchers are semi-ionic to fully ionic. Consequently, the F–COF electrode showed fast
exploring redox-active COFs for energy storage, harnessing their po­ charge ability, reaching a high reversible capacity of 95 mA h/g at a 5 C
tential for reversible redox charge storage mechanisms in metal-ion rate in 12 min. It maintained stable performance, maintaining approx­
battery systems. This promising research direction draws inspiration imately 100% of its capacity after 5000 cycles. Conversely, after 4000
from supercapacitor design principles, encouraging scientists to create cycles, there was a noticeable decrease in the coulombic efficiency of
COF-based battery electrodes that can address the shortcomings of COF-based electrodes devoid of fluorine. The fluorine atom was shown
traditional organic battery systems [252–254]. Because of their strong, to be crucial in increasing electrode conductivity and electron affinity,
well-organized layers, flexible redox-active elements, and modifiable both of which enhanced the stability of K+ ion binding, according to
porosity, COFs are useful electrode materials for various rechargeable computational analysis. The development of organic electrode materials
metal-ion batteries. Using the special properties of COFs, He et al. [255] is greatly aided by this research, which opens the door for PIB
suggested a solution to the conductivity problems in host-guest elec­ commercialization (Table 5).
trolyte systems. These characteristics made it possible to create porous
host materials that effectively carry lithium ions (Fig. 15b). Their 5.3. Water pollutant removal
research aimed to leverage COFs as host materials due to their excellent
stability in liquid lithium electrolytes, positioning them as promising COFs are emerging as a ground-breaking class of crystalline porous
candidates for efficient lithium-ion transport. They demonstrated that materials, defined by their strong covalent bonds that connect the in­
the host-guest system could function effectively, surpassing traditional dividual structural units. What sets COFs apart is their exceptional
conductivity issues limits. combination of large surface areas, high porosity, and uniform pore size
To enhance the ionic conductivity and overall performance of PIL/IL- distribution, along with their remarkable hydrothermal stability and
based ion gel electrolytes (IGEs) for lithium metal batteries, Wang et al. easily tunable framework structures. Compared to traditional organic
[256] explored incorporating 2D COFs, specifically TPB-DMTP-COF, as polymers, COFs offer distinct advantages, including well-defined crystal
fillers. They utilized DFT and molecular dynamics simulations to structures, organized channel architectures, significant surface areas,
investigate the structure and ion transport behavior of confined ILs and excellent chemical stability. These features enhance their physico­
within the COF, as well as the impact of COFs when used as fillers. The chemical properties and expand their applications, making them highly
addition of COFs significantly improved ionic conductivity limits in the versatile. The ease with which COFs can be functionalized further adds
PIL/IL-based IGE composite. At 30 ◦ C, ionic conductivity in the to their appeal, allowing them to be tailored for specific purposes. As
COF-enhanced IGE composite was approximately 2.2 times higher than living standards continue to improve, the need for effective pollution
in the PIL/IL-based IGE without COFs. This enhancement is attributed to detection and treatment has become more urgent. Among various
the presence of COFs, which facilitate effective lithium ion transport methods, adsorption stands out due to its simplicity and efficiency in
within the electrolyte. Corresponding to the increased ionic conductivity removing many pollutants. COFs, with their unique properties, show
observed in the composite, simulations (Fig. 15c) demonstrated that the great promise in this area and have garnered growing interest in recent

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years for environmental applications, especially in pollution control methods such as filtration, centrifugation, magnetic separation, solvent
[261–263]. washing, and thermal treatment [306]. Studies confirm that COFs retain
Elewa and colleagues synthesized a hydroxyl-functionalized COF, their crystallinity and adsorption capacity under harsh conditions,
known as DHTP-TPB COF, specifically for the removal of Pb²⁺ ions from supporting their long-term usability [307]. Advancing practical appli­
water [264]. At a pH of 4, this COF exhibited impressive adsorption cations necessitates eco-friendly recovery techniques, long-term per­
capabilities, achieving a Pb²⁺ adsorption capacity of 154.3 mg/g. Their formance assessments, and integration with complementary
study also investigated the material’s selectivity in the presence of other technologies for scalable, sustainable solutions. COFs with high surface
metal ions, including Co²⁺, Ni²⁺, Fe²⁺, Cu²⁺, and Zn²⁺, revealing a Pb²⁺ area, tuneable porosity, and chemical stability offer promise for sus­
removal rate exceeding 96%. XPS analysis indicated that this high tainable water treatment and pollutant removal. Their efficiency de­
removal efficiency was due to strong coordination bond interactions pends on effective recovery and reuse without performance loss.
between the COF’s hydroxyl groups and Pb²⁺ ions. In a related study, Ma Techniques such as filtration and solvent extraction enable COF sepa­
et al. (2023) synthesized two novel carboxymethylated ration from treated water, maintaining adsorption efficiency over mul­
triazine-functionalized COFs specifically for Pb²⁺ adsorption. These tiple cycles. Characterization methods like SEM and XRD confirm
COFs exhibited π-π conjugated structures, one-dimensional pore chan­ structural integrity post-recycling. COFs also exhibit high selectivity for
nels, and a high density of nitrogen and oxygen functional groups, all contaminants in complex matrices, reinforcing their suitability for
contributing to efficient Pb²⁺ capture [265]. The mechanism of adsorp­ environmental applications. Future efforts should optimize recovery
tion was primarily driven by electrostatic interactions and coordination. methods, enhance chemical stability, and functionalize COFs for
In a different study, Wang and colleagues developed a β-ketoenamine improved recyclability [308,309]. Studies show COF potential in se­
COF through a simple solvothermal method [266]. This COF’s lective pollutant adsorption and resource recovery. Cao et al. reported
one-dimensional ordered pore structure and the presence of hydrazide COF-based adsorptive membranes (AMs) maintaining high adsorption
groups facilitated Hg²⁺ adsorption, achieving a maximum capacity of efficiency over multiple cycles, with thiourea successfully eluting
909 mg/g. Ma and his team also took an alternative approach by syn­ palladium. XPS and TEM confirmed structural integrity, and COF-AMs
thesizing a sulfhydryl-functionalized COF via a Schiff base reaction, exhibited strong Pd2+ selectivity, which is crucial for electronic waste
resulting in an impressive adsorption capacity of 1283 mg/g for Hg2+ at management and sustainable resource utilization [310]. Zhou et al.
a pH of 7 [267]. highlighted MoS2-COF composites for selective gold recovery, achieving
Remarkably, the COF maintained its selectivity for Hg2+ even in the >99% Au(III) desorption via a thiourea-hydrochloric acid solution with
presence of other metal ions and demonstrated exceptional stability in preserved structural stability [311]. This integration enhances resource
regeneration and reuse tests. In addition, Fu et al. synthesized a recovery while minimizing environmental impact. Beyond metal re­
pyridine-based COF through Schiff base condensation, resulting in covery, COFs improve water treatment efficiency. Li et al. showed
nitrogen-rich pore channels that exhibited high selectivity and variable COF-doped membranes with excellent recyclability in desalination and
adsorption capacities for Hg2+, which ranged from 719.4 mg/g at 293 K wastewater treatment [312]. Wang et al. used liquid-liquid interfacial
to 1000 mg/g at 313 K [268]. Theoretical calculations indicated that this polymerization to prepare ABC-structured COF membranes for dye
COF and Hg2+ binding was primarily driven by chelation rather than separation, achieving a stable interception rate of 97.57%.
covalent interactions. Furthermore, two nitrogen-rich COFs synthesized Solvent-assisted desorption preserved membrane integrity, while high
via a Schiff base reaction displayed extraordinary iodine adsorption selectivity for ions and organic molecules ensured efficacy in real-world
capacities, with TFBT-1 achieving 3150 mg/g and TFBT-2 reaching applications [313,314]. Integrating COFs into membrane technologies
2600 mg/g [269]. offers a sustainable approach to water resource management. COF
The interaction mechanisms, analyzed through spectroscopy, recyclability, selectivity, and stability underscore their role in sustain­
pointed to the role of nitrogen adsorption sites within the COFs’ pores. able environmental applications. Future research should refine recovery
Another study by Liu et al. reported the synthesis of an imide-linked, 3D techniques, enhance long-term stability, and explore novel functionali­
microporous COF using a template-assisted modulation strategy, which zation aligning COFs with green chemistry principles for broader prac­
achieved an iodine adsorption capacity of 3150 mg/g and exhibited a tical adoption.
notable average adsorption rate [270]. This COF’s micropores played a
crucial role in capturing iodine, as confirmed by detailed characteriza­ 5.3. COFs for drug delivery
tion studies. Together, these studies underscore the vast potential of
COFs in environmental remediation, particularly for the adsorption of Besides, COFs have recently emerged as versatile drug delivery ma­
heavy metals and other pollutants, highlighting their unique structural terials owing to their larger surface area, tailorable pore sizes, and sta­
advantages and adaptability for a wide range of applications (Table 6). bility. Some of the latest advances in this regard include COF-based
COFs have shown remarkable potential for water pollutant removal, systems with large drug-loading capacities and controlled release pro­
particularly for heavy metals and organic contaminants. Their high files. COFs are gaining attention for their use in drug delivery due to
surface area, tuneable pore sizes, and functional groups enable efficient their lightweight organic scaffolds, tunable properties, and robust
adsorption and degradation of pollutants. Functionalized COFs, such as structures. Their ability to encapsulate and release drugs efficiently in
thioether- and thiourea-based frameworks, exhibit ultrahigh adsorption biological media is a significant advantage. COFs’ high drug adsorption
capacities (>4200 mg/g for Hg2+) and exceptional selectivity due to capacity, biocompatibility, and modifiability address stability issues
strong soft-soft interactions between sulfur-containing groups and target drug molecules face in biological environments, making them effective
metal ions. Additionally, magnetic COF composites (e.g., Fe3O4/TpPa-1) vectors for targeted delivery and minimizing cytotoxicity [315]. Recent
and photocatalytic COF catalysts (e.g., Ag/AgBr/TzDa) enable efficient advancements in COFs include the development of 3D COFs with novel
Cr6+ reduction to less toxic Cr3+ addressing both adsorption and network topologies. For instance, TUS-84, a 3D COF with a two-fold
detoxification challenges [301–305]. However, challenges such as interpenetrated structure and a BET surface area of 679 m²/g, has
regeneration, selectivity, and long-term stability in aqueous environ­ demonstrated impressive drug loading and sustained release profiles.
ments must be addressed. Future research should focus on developing These innovations highlight COFs’ potential for enhancing drug delivery
cost-effective and scalable COF-based materials for large-scale water systems through their versatile structures and high performance [316].
treatment applications Bhaumik et al. [317] loaded cisplatin into the empty spaces of stiff 2D
The recyclability of COFs is important for their environmental ap­ crystalline COF nanomaterials, effectively delivering medication against
plications, including pollutant adsorption, water purification, and cat­ metastatic breast cancer cells. This nano-DDS showed a good thera­
alytic degradation. Ensuring sustainability requires efficient recovery peutic effect on triple-negative breast cancer cells and demonstrated

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Table 6
Applications of COF in the removal of pollutants.
COF Pollutant Adsorption capacity Adsorption parameters Mechanism Remarks Ref.
(mg/g)/% Removal

OM-COF-300 and Iodine 3.15 g/g ​ adsorption Reusability up to 5 cycles with [270]
NM-COF-300 90% efficiency
2+
Amino-sulphonic- Hg 99.98% pH = 7 adsorption excellent selectivity and [271]
COF sensitivity
Ag NPs@COF Hg2+ 99% ​ adsorption COF as electron donor in the [272]
adsorption process.
COF2 Cr6+ 649.35 mg/g pH = 9 ​ ​ [273]
Fe3O4@COF(TpPa- Cr6+ & bisphenol 245.45 & 1220.97 ​ hydrogen N SSA = 485.2 m2/g [274]
1) mg/g -bonding
(hydrothermal (NH…O…HO) and
method) π-π interaction
BiOBr/TzDa COF RhB dye & Cr6+ total (97% Dye removal in 20 min ​ 2D Z-scheme heterostructure [275]
(BTDC) and Cr6+ removal in 40 photocatalyst
mins
COF TzDa/Ag/ TC & Cr6+ 78% (both) & 98% dose =20 mg; Ci = 10 Photocatalytic SSA = 1456.9 m2/g [276]
AgBr Cr6+ ppm; V = 50 ml; t= 30 (visible light)
min
Fe0/TpPa- Cr6+ 516 mg/g dose =220 mg; Ci = 30 Adsorption SSA = 734.13 m2/g [277]
1@DOPA ppm; t= 120 min
COF-SH Pb2+ 239 mg/g Cycles =5; time = 48 h; Adsorption SSA = 167.3 m²/g [278]
(hydrothermal)
2+
DHMR@COF Pb 359.94 mg/g / 81.42% pH = 4; dose = 10 mg; Adsorption Monolayer adsorption with [279]
V = 5 mL; cycle =4; exothermic process
2+
COFDBD-BTA Hg 687.38 mg/g Ci = 10 mg/30 mL; dose Adsorption SSA = 41.10 m2/g [280]
= 30 μg t = 10 min, pH
6.5 ± 0.25
DHTA-Pa/CS Pb2+ 1268 mg/g Ci = 1000 ppm; pH = 5; Adsorption SSA = 337 m2/g [281]
t = 15 min
2+ 2
MCOFV1 and Pb 52.1 and 31.1 mg/g Dose = 10 mg; V = 120 ​ SSA = 204.9 & 587.5 m /g [282]
MCOFV2 mg/L;
2+ 2+ 2+ 2
TB-HCOF Pb , Cu and Hg 766.28, 759.32, and pH = 5, t = 12 min homogeneous SSA = 139.9 m /g [283]
640.83 mg/g monolayer
chemisorption
adsorption
TFBT-1 & TFBT-2 I2 3150 & 2600 mg/g t = 3min & 3 min Electrostatic ​ [284]
attraction
TTA-DMTP-COF I2 2590 mg/g t = 36 h coordination ​ [285]
interaction
COF-R5 UO2+
2
253.7 mg/g t = 4; cycle =6 hydrogen bonding ​ [286]
NDA-TN-AO UO2+
2
6.07 mg/g T = 648 h; cycle = 6 electrostatic ​ [287]
attraction
2+
Ni0.6Fe2.4O4-HT- Pb 411.80 mg/g / 95.64 T = 10min; cycle = 4; Ci electrostatic ​ [288]
COF % = 600 mg/L; V = 10 interaction and
mL; chelation
Fe0/TAPB-PDA As3+ 135.78 mg/g Dose = 10 mg; V = 50 Chemical SSA = 131.49 m2/g [289]
COFs mL; adsorption
COF EB-COF:Br H3PO4 6980 mg/g pH = 0.86 to − 0.65; Electrostatic SSA = 1326 m2/g [290]
dose =2g/L; t = 10 min adsorption and
isoenthalpic
process.
EB-COF:Br PO3−
4
35.3 mg/g & 53.1 mg/ pH = 7; t = 4–5h; PO3−
4 adsorption is
1326 m2/g [291]
and AsO3− g exothermic while
4
removal AsO3−
4 is
endothermic
pristine CN-COF- Detction OF roxarsone (ROX) 732 and 787 mg/g by Cycle = 5; ​ LOD for ROX was found 6.5 and [292]
ben and CN- and adsorption of organic CN-COF-ben and CN- 12.3 Nm by CN-COF-ben and CN-
COF-tri arsenic COF-tri, respectively COF-tri, respectively
COFBTLP-1 Detection of heavy metal ions LOD for Cd2+, Pb2+, Sensitivity for LOD for ​ Each COFBTLP-1 unit contains a [293]
Cu2+ and Hg2+ was Cd2+, Pb2+, Cu2+ and total of 12 adsorption sites,
12.3, 11.8, 18.6 and Hg2+ 1337.4, 1389.0 comprising 6 sulfur atoms and 6
21.4 nM, respectively and 886.2, 770.0 μA/ nitrogen atoms
μM cm2, respectively
COF-ETTA-2,3- Cd2+ removal 39.6 mg/g at 1 min pH = 7, t = 20 min; adsorption SSA = 1476.5 m2/g [294]
Dha and 95.6 mg/g in cycle = 4
20 min
TpPa-1 COF@CDs Hg2+ removal 235 mg/g; fast t = 30 min; cycle = 5 ​ LOD is 0.75 μg/L, demonstrating [295]
adsorption rate (58.2 that the metal-free raw material
mg/g/min) used to create TpPa− 1 COF@CDs
is reliable, cost-effective, and
environmentally friendly
COF@SO3H Cd2+, Co2+ and Cr3+ 81.97, 77.52, and Dose = 20 mg; pH 5.5 adsorption SSA = 62.5 m2/g; pore width = [296]
105.26 mg/g for Cd, 7.0 for Co and 1.3 nm and pore volume = 0.17
5.3 for Cr cm3/g
(continued on next page)

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

Table 6 (continued )
COF Pollutant Adsorption capacity Adsorption parameters Mechanism Remarks Ref.
(mg/g)/% Removal

TH-COF, dp-TH, p- MB and MO dye removal The dp-TH COF 50 mg were added into adsorption For the MB dye, the order of [297]
TH captured 5.5 mg/g of a 100 mL of 25 ppm dye effectiveness was dp-TH > TH >
MB dye, whereas the p- solution and stirred at p-TH COFs, while for the MO dye,
TH COF captured 25.9 500 rpm mixing rate the sequence was p-TH > TH >
mg/g of MO dye dp-TH COFs
COF-DL229 Th4+ 513 mg/g T = 1 min adsorption SSA = 569.30 m2/g [298]
Magnetic COF Organothiophosphate 163.9 to 178.6 mg/g Cycle = >10 electrostatic SSA = 1543 m2/g, mesopores = [299]
pesticides (OPPs) interaction (π-π, 3.1 nm
CH⋯π, and CH⋯S)
CFO@COF) Catalytic property for 99.8% removal of SMX ​ Radical mechanism Risk assessment in CFO@COF/ [300]
(hydrothermal degredation of (10 mg/L) within 30 PMS/SMX system were estimated
method) peroxymonosulfate (PMS) for min and 90.8% TOC via ECOSAR
sulfamethoxazole (SMX) removal

great drug-loading efficiency, as in vitro tests indicated. effect between PTT, chemotherapy, and CDT. Tumor therapy and
In 2022, flexible hollow COF nanospheres were easily created by effective precision medication delivery are made possible by a range of
Huang et al. [249] using heterogeneous nucleation growth. Because of mechanical characteristics that can satiate tumor-specific responses.
their large specific surface area and porosity, the resulting hollow COF In 2022, Zhou et al. developed a novel drug carrier—a pH/GSH/
nanoparticles effectively encapsulated doxorubicin (DOX). Additionally, photo triple-responsive 2D-flexible COF—designed for a combined
the nanoparticles exhibited a pH-sensitive release profile due to their approach to chemotherapy, photothermal therapy, and chemodynamic
acid-labile breakdown. Furthermore, adding DOX may improve their therapy, enabling highly effective passive targeting of tumors [320].
mechanical characteristics and stability, providing them with strong in Under typical physiological conditions, this nano-DDS was stable and
vivo anticancer efficacy (Fig. 13(I)). COFs are useful drug carriers could efficiently accumulate in tumor locations. Once within the tumor
because of their customizable mechanical properties, which open up the cells, the acidic pH and over-expressed GSH created a unique microen­
possibility of developing nano-delivery systems with superior stability vironment that weakened the ultrasensitive nanosystem and encouraged
and targeted delivery degradation. the release of DOX, which kills cancer cells exclusively. Concurrently,
Tang et al. (2021) proposed the rational design of a smart nucleic there was a notable rise in the generation of ROS, which disrupted the
acid-gated COF nanosystem for microenvironment-responsive drug redox balance of tumor cells. The outstanding photothermal perfor­
release and cancer-specific imaging [318]. On the surface of COF NPs mance of the drug delivery system was made possible by the substan­
loaded with DOX, single-stranded DNA (ssDNA) tagged with Cy5 dye for tially extended flexible 2D structure. The breakdown and release of the
mRNA recognition was adsorbed. While the densely coated ssDNA could medication were further augmented by the photothermal action of
stop DOX from leaking out of COF NPs and provide flexible properties, external 808 nm laser irradiation.
the DOX loaded in the pores of COF NPs could strengthen the interaction In 2021, Jiang et al. synthesized a nanoscale, hypoxia-responsive
force and improve its mechanical stability. Additionally, in vitro studies flexible COF containing azo bonds to bind the hypoxia-activated drug
demonstrated a delivery impact specific to tumor cells. This work pro­ tirapazamine (TPZ) and the photosensitizer chlorin e6 (Ce6). When
vided a potential method for controlling the mechanical force between exposed to a hypoxic environment, such as that found in tumor tissues,
COFs and biomolecules and a universal nanoplatform for cancer the COF ruptured and released the loaded drugs. Additionally, upon
theranostics. exposure to near-infrared (NIR) light, Ce6 consumed oxygen, generating
In 2022, Huang et al. developed a space-time conversion carrier that harmful reactive oxygen species and further exacerbating hypoxia. To
incorporated interlayered polyethyleneimine (PEI) layers with different produce large amounts of biotoxic oxyradicals, the two-step hypoxic
mechanical properties to accommodate various cargos. This design stimulation successively triggered the flexible COF disintegration,
featured COF-coated mesoporous silica nanospheres (MSNs) (Fig. 13 released medicines, and activated TPZ. To control a cell’s behavior and
(II)). Therefore, the extracellular matrix could be pulled, drug efflux functions, the cytoskeleton, which is physically attached to the nucleus,
could be inhibited, the sequential release of different medications could can transfer mechanical signals regulated by the microenvironment to
be successfully mediated, and variations in nanoparticle surface charge the nucleus. The strongest form of cytoskeleton is microtubules, and the
could be used in concert with programmed drug delivery to enhance the viability of tumor cells is directly impacted by their structural degra­
chemotherapeutic effect on pancreatic cancer. This study introduced a dation [321].
space-time conversion technique to overcome barriers created by the In 2022 [322], Herrero et al. synthesized a novel
extracellular matrix and drug reflux, enabling programmed multi-drug microtubule-destabilizing agent of PILA9 to disrupt the microtubule
delivery. This approach presents a new therapeutic option for pancre­ network and provide beneficial cytotoxic effects. This agent can bind to
atic cancer [250]. the tubulin colchicine site. Nevertheless, COF is a new biomaterial with
In 2023, Li and colleagues developed a multifunctional nanoplatform a lot of promise that hasn’t been documented in this field yet.
(CuS@COFs-BSA-FA/DOX) that integrates copper sulfide nanoparticles In 2020, Pang et al. [323] reported on a flexible COF nanosystem
with COFs to facilitate photothermal therapy (PTT), chemotherapy, and loaded with ICG and chicken ovalbumin (OVA) (COF@ICG@OVA),
chemodynamic therapy (CDT). The application of flexible poly­ which demonstrated significant photothermal conversion efficiency
ethyleneimine (PEI) and BSA-FA coatings on the surface of CuS@COFs (35.75%) and ROS production ability when primary tumors were
improved cancer targeting and reduced the nonspecific release of exposed to laser irradiation at 650 nm and 808 nm. Tum-associated
doxorubicin (DOX) from the particles [319]. The near-infrared light-­ antigens were also generated following a combination of PTT/PDT
mediated photothermal effect and the acidic tumor microenvironment therapy. By generating robust immune responses, it could be used in
initiated the release of DOX for chemotherapy. Simultaneously, this conjunction with anti-programmed cell death one ligand (PD-L1)
boosted the CDT efficiency of CuS@COFs, strengthening the synergistic checkpoint blockade therapy to efficiently eradicate initial tumors and

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

prevent cancer cells from metastasizing. The post-modified 2D stiff COFs nanoscale COFs capable of loading drugs like 5-FU, captopril, and
showed enhanced in vivo circulation, delivery efficiency, and good ibuprofen with low cytotoxicity, highlighting their therapeutic potential
flexibility features (Fig. 14). In 2021, Sun et al. synthesized a serrated [327]. Covalent triazine polymers demonstrated pH-controlled doxo­
packing COF, designated COF-606, which exhibits remarkable photo­ rubicin release and bioimaging capabilities, emphasizing their role in
stability and two-photon absorption (2PA) characteristics. Its rigid cancer theranostics [328]. However, challenges such as scalability,
framework effectively minimizes aggregation-induced quenching, stability in biological environments, and long-term biocompatibility
resulting in high efficiency for ROS generation. Consequently, COF-606 need to be addressed. Future research should focus on developing
was utilized as a 2PA photosensitizer for photodynamic therapy (PDT) in multifunctional COF-based nanocarriers for personalized medicine and
deep tumor tissues [324]. It was demonstrated that COF-606-induced cancer therapy
PDT effectively elicited an immunological response, immunogenic cell
death, and the initial restoration of immunosuppressive status. 5.4. Food safety analysis
Combining immune checkpoint blockade therapy with programmed cell
death protein one and two PA-induced PDT using COF allowed this. COFs are utilized in a variety of sample pretreatment techniques,
Strong abscopal tumor-inhibiting efficacy and long-lasting immunolog­ including dispersive solid-phase extraction (DSPE) and solid-phase
ical memory effects were the results of this combination, making it a extraction (SPE). Ionic covalent organic frameworks (iCOFs) have
viable combinatorial therapeutic approach for cancer treatment. proven particularly effective when used in conjunction with cutting-
COFs have gained significant attention as drug delivery systems due edge analytical techniques such as mass spectrometry (MS) and high-
to their high loading capacity, biocompatibility, and controlled release performance liquid chromatography (HPLC) for analyzing a wide
profiles. Their tunable pore sizes and surface functionalities enable range of food contaminants, including pesticides, veterinary medica­
targeted delivery and reduced cytotoxicity. Yan et al. developed 3D tions, contaminants found in food packaging, and perfluoroalkyl sub­
polyimide COFs (PI-COF-4 and PI-COF-5) with high ibuprofen loading stances (PFAS). Table 7 lists and summarizes the pollutants in different
and controlled release, setting a foundation for COF-based pharmaceu­ foods using various COF materials.
tical applications [325]. Photo-responsive COFs with azobenzene groups Imidazoline-linked cationic covalent triazine framework (IM-iCTF)
further enabled light-triggered drug release, showing their potential for was created by Cai et al. IM-iCTF offers excellent adsorption capabilities
stimuli-responsive systems [326]. Zhao et al. advanced this by creating for EEs because of the combined effects of hydrogen bonding,

Fig. 14. (a) Fabrication and (b) Mechanism of antitumor immune responses induced by CIO nanoparticle-based phototherapy combined with checkpoint blockade
therapy. Reproduced with permission from 325. Copyright 2023 Wiley.

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

Table 7
Application of COF in the detection of analytes from food samples.
COF extraction material Analyte Method Sample Recovery (%) Ref.

IM-iCTF Ees HPLC-DD water, fish 44–77 [329]

C-H-COF PFASs UHPLC-MS/MS dairy product 12.6–80.1 [330]
TPB-BFBIm-iCOF PFASs UHPLC-MS/MS Seafood 85.3–109.4 [331]
CD-F-CTF PFASs HPLC-MS/MS Food 76.7–107 [332]
Fe3O4@COF-SO3Na Basic orange-II HPLC-DAD dried bean curd 90.1–98.8 [333]
C-COFs PFASs MALDI-TOF/MS Water 81–112 [334]
BT-TDC–COF (COF1), BT-BDB-COF (COF2) GenX HPLC-MS/MS Water ​ [335]
Cotton @iCOF PFASs UHPLC-MS/MS Water 77.9–117.6 [336]
COF-FIN5 PFASs HPLC-CDD Water ​ [337]
CN-iHCP EDCs HPLC-UV Milk 85.5–116 [338]
TFPB-DgCl-COF IBP HPLC Water ​ [339]
CACP Neonicotinoids HPLC Fruits 93.3–121.3 [340]
Fe3O4@iCOF Phosphopeptides MALDI-TOF MS non-fat milk ​ [341]
Fe3O4@EBTFB-iCOF Polar organic acids HPLC-UV Water 73.3–101.0 [342]
Fe3O4@EB-iCOF PFCs HPLC-MS/ MS Water 73.9–108.3 [343]
NKCOFs AAI UPLC-Q-TOF-MS/MS Water ​ [344]

electrostatic interaction, and π-π conjugation (Fig. 15(I)). The EEs in developing novel materials and offers a reliable method for enriching
water, fish, and shrimp were determined using SPE-HPLC-DAD and the and identifying trace-level organic pollutants.
IM-iCTF, with detection limits of 0.008–0.05 ng/mL, 0.015–0.11 μg/g, Chen’s team successfully identified eight long-chain PFASs in food
and 0.012–0.10 μg/g, respectively [345]. This work contributes to products by employing a post-modified CF-COF (Fig. 15(II)) as the

Fig. 15. (I) Reproduced with permission from 345. Copyright 2024 Elsevier. (II) A diagram of the preparation of Fe3O4@CF-COF and MSPE procedure. Reproduced
with permission from 346. Copyright 2024 Elsevier.

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

adsorbent for magnetic solid-phase extraction (MSPE), followed by LC- applications. Additionally, the stability and reversibility of COF-based
MS/MS analysis. Their molecular simulation studies revealed that sensors contribute to their practical use in environmental monitoring,
both electrostatic attraction and fluorine affinity enhanced the adsorp­ industrial safety, and healthcare diagnostics, showcasing their potential
tion of PFASs onto CF-COF. This approach stands out for its high in various fields.
sensitivity and straightforward sample preparation compared to other The vinylene-linked COF, TMT-BPDA-COF, is synthesized from
methods, offering a novel strategy for developing adsorbents specifically 2,4,6-trimethyl-1,3,5-triazine (TMT) and 4,4′-biphenyl dimethyl form­
targeting PFASs [346]. aldehyde (BPDA), exhibiting exceptional crystallinity, thermal stability,
and chemical durability. This COF produces strong yellow fluorescence
5.5. COF in sensing with a quantum yield of 14.9% and displays a broad response to pH
changes due to intramolecular charge transfer. Additionally, portable
Modifying their structure and composition can optimize the perfor­ fluorescent sensors incorporating TMT-BPDA-COF in agarose gel and
mance of COFs in sensing applications, which has great potential for a cellulose acetate butyrate (CAB) films demonstrate high sensitivity to
variety of analytical and detection applications. COFs are particularly NH3 gas and effective pH detection, making them ideal for environ­
attractive as viable sensor materials because of the special qualities that mental and industrial applications. COFs, with their customizable
allow them to incorporate sensitive functional groups. This offers the structures and excellent material properties, are promising for gas
opportunity to create sophisticated and specialized sensor technologies. storage, pollutant removal, catalysis, adsorption, optoelectronics, and
Compared to other reported sensors for analyte detection, COFs have sensing (Table 8).
shown encouraging results. These frameworks are ideal for sensing ap­
plications because of their special qualities. For instance, their large
surface area promotes analyte adsorption and raises the detection 5.6. Catalysis
sensitivity. Furthermore, selective analyte detection is made possible by
COFs’ variable pore diameters, which improve the sensor’s specificity COFs are considered promising next-generation catalysts due to their
[347]. large surface areas, accessible nano-pores, and the ability to incorporate
The analyte-COF structural interaction is the basis for COFs’ lumi­ active ingredients such as ligands, complexes, and metal nanoparticles.
nous characteristics. As the analyte interacts with the COF structure, the COFs are emerging as a versatile platform for creating heterogeneous
parameters of the material’s luminescence are altered. Different analytes catalysts for various chemical reactions (Table 9). Their unique prop­
can be detected and sensed depending on the ensuing changes in lumi­ erties allow them to catalyze various organic reactions, including
nescence, which can be caused by changes in emission wavelength, in­ important C-C bond formations. Furthermore, advanced pore-
tensity, or lifetime [348,349]. engineering in COFs enables enantioselective asymmetric C-C bond
Identifying and quantifying this modification can ascertain the formations, achieving high yield and enantiomeric excess in shorter
presence and concentration of the analyte. Fluorescence quenching is an reaction times than their monomer and oligomer counterparts [365].
example of a luminous COF sensing mechanism. The concentration of Fig. 16 illustrates the concept of COFs as a new generation of catalyst
the analytes present determines how much quenching occurs [350]. materials [366].
This MOF@COF-B(OH)2 platform was created by Hu et al. as a novel Younas et al. [371] proposed that non-precious metal atoms sup­
material with easily detectable fluorescence properties. The researchers ported on a covalent organic framework (TM@COF SACs) could serve as
found that excited-state intramolecular proton transfer (ESIPT) effective electrocatalysts for the hydrogen evolution reaction (HER).
improved fluorescence emission from MOFs when MOF and COF were They assessed the catalytic performance of single atoms of Co, Ni, Cu,
combined. After further research, the scientists discovered that and Zn on the COF substrate using various parameters, including ther­
MOF@COF-B(OH)2′s affinity for boron allowed it to effectively capture modynamic stability, HOMO and LUMO energies, HOMO-LUMO energy
Trf. By incorporating Trf into MOF@COF-B(OH)2 and allowing it to bind gaps, and the change in Gibbs free energy of adsorbed atomic hydrogen
only on the surface, an imprinted version of the material known as (ΔGH*). Among these complexes, Zn@COF emerged as the most
MOF@COFB(OH)2@MIP was produced. By monitoring the fluorescence promising catalyst, exhibiting an interaction energy (Eint) value of
quenching of MOFCOF-B(OH)2@MIP following incubation with Trf at approximately 0.11 eV (Fig. 17(I)). Density functional theory (DFT)
430 nm, photoinduced electron transfer (PET) can be used to identify results indicated that the HER performance was significantly influenced
Trf. The results showed that this COF material has high sensitivity and by the presence of a single Zn atom doped onto the COF surface, with a
specificity for detecting Trf [351]. ΔGH* value of about 0.88 eV.
This cutting-edge method effectively constructs pyridinium motifs He et al. developed an efficient catalytic system by integrating Co
into a carbon-conjugated COF, allowing for quick and precise detection
of the target analyte. With its online and visibly monitored design, the Table 8
system provides a user-friendly solution for various applications in Application COF in sensing.
chemical sensing technology [352,353]. COF sensor Analyte Mechanism LOD Ref.
The fluorescence mechanisms are ICT, RET, PET, and AIE [354]. 3D-LCOF nitro pesticide PET 0.056 ppm [355]
These sensors form a charge transfer complex between an electron donor F-Csp2 -TT cartap PET 0.5 µg/L [356]
and acceptor by employing fluorescence techniques to facilitate signal TAPB-DMTP- Amine vapor PET 1.2 ppb [357]
changes. When an excited state relaxes to a ground state, photons are COFs
SH-COF Cu2+ and Hg2+ PET 0.244 μM and [358]
emitted. Fluorescence signals indicate the return of the additional 0.239 μM
electron from the acceptor to the donor. Py-An-COF Cr3+
PET 8.17 × 10–5 M [359]
COFs have emerged as highly effective chemical sensors due to their TAPB-BTDD triethylamine PET 27 nM and 170 nM [360]
inherent porosity, high surface area, and tunable chemical functional­ DSE-COF aliphatic PET & ICT 0.23 µM [354]
amines
ities. These characteristics allow COFs to interact selectively with
TpTt-COF tetracycline PET & ICT 0.014 μmol/L [361]
various analytes, enabling the detection of gases, pH changes, and TpTt-COF tetracycline PET & ICT 7.4 nmol/L [362]
chemical vapors with high sensitivity and specificity. COFs have been (UNT)
developed to detect NH3 gas at extremely low concentrations and to TMT-BPDA-COF ammonia ICT 1.6 ppb [363]
function as robust pH sensors across a broad range. Integrating func­ UiO@COF ATP ESIPT 0.038 μM [364]

tional groups into COFs enhances their ability to capture and respond to Note: photoinduced electron transfer = PET; Intramolecular charge transfer =
specific molecules, making them versatile platforms for sensing ICT; excited-state intramolecular proton transfer = ESIPT

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

Table 9
Applications of COF in catalysis.
Application COF Type Catalytic Activity Features Ref.

Dehydrogenation Pd5Au3Ir2/NH2- Formic acid dehydrogenation The initial turnover of frequency (TOF) value for FA dehydrogenation without [367]
TAP-TPA-COFs rate and Cr(VI) reduction additives was 9970 h− 1 at 298 K, the apparent activation energy (Ea) was 30.3 kJ/
mol and the rate constant (k) for Cr6+ reduction was 0.742 min− 1
Dehydrogenation Cp*Ir@CTF Formic acid dehydrogenation Complete dehydrogenation occurs in 24 min at 80 C [368]
Photocatalytic activity CdSe/CTF carbon dioxide reduction with a HER 19.0 mmol/g/h under visible-light irradiation; evolution rate of 1.48 mmol/g/ [369]
carbon monoxide h
photocatalytic COF-Sr2Fe1 benzylamine oxidative coupling yield of 97% [370]
oxidative coupling reaction

Fig. 16. COF as heterogeneous catalysts. Reproduced with permission from 366. Copyright 2018 Elsevier.

Fig. 17. (I) Gibbs free energy change of OER intermediates for designed complexes. Reproduced with permission from 371. Copyright 2024 Elsevier. (II)(a) A
possible mechanism for the [Cu(bpy)2]2+ catalyst in photo-assisted syngas production, along with the HOMO-LUMO orbitals of (b) CTF-TPN and (c) CTF-HUST-1, and
the electrostatic potential maps of (d) CTF-TPN and (e) CTF-HUST-1. Reproduced with permission from 372. Copyright 2024 Elsevier.

single sites as active centers into CTFs, which serve as photoabsorbers complex, achieved a syngas yield of 3303 μmol/g (CO = 1.4:1) in 10 h
for photocatalytic syngas production from CO2 in an aqueous solution. three times higher than CTFs without heterojunctions. Theoretical cal­
The CTFs, containing intramolecular heterojunctions, exhibited culations revealed that the heterojunctions facilitated charge separation,
enhanced light absorption and, combined with 0.8 mmol/L of the Co further boosting the photocatalytic performance. Fig. 17(II) illustrates

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

the fabrication of TpPa/PSF composite membranes via interfacial heat, and chemicals. Additionally, optimizing their integration into de­
polymerization (IP). Part (a) shows a schematic of the preparation steps, vices involves addressing compatibility issues and ensuring efficient
starting with a PSF substrate coated with an orange solution, followed by functionality, which demands a multidisciplinary approach that com­
heat treatment, transforming the membrane. The molecular structure of bines advanced materials science, engineering, and device technology.
TpPa is depicted alongside, and part (b) presents the membrane’s Despite significant progress in COF research, several challenges
physical appearance, highlighting its rough surface texture and crys­ remain, including scalability, stability, and processability. The synthesis
talline structures. This visual summary is essential for research detailing of COFs often requires precise conditions, and their characterization can
novel materials or methods [372]. be complex due to intricate structures. In practical applications,
ensuring stability under real-world conditions and optimizing their
integration into devices are critical. Future research should focus on
5.7. Optoelectronics
developing scalable synthesis methods, improving characterization
techniques, and exploring new applications in areas such as catalysis,
Given their highly tailored structure and excellent optical properties,
sensing, and optoelectronics. Collaborative efforts between academia
COFs represent huge strides in optoelectronics. Their potential appli­
and industry will be essential to overcome these challenges and unlock
cations in photodetectors, light-emitting devices, and photovoltaic cells
the full potential of COFs.
have recently been explored. COF-based photodetectors exhibit high
sensitivity and fast response times, enabled by excellent charge carrier
mobility and a well-defined electronic structure of COFs. 7.1. Synthesis Challenges
Moreover, the fluorescent features of COFs are attracting massive
interest. Yao et al. examined the inclusion of functional groups into 7.1.1. Scalability
COFs, which might modulate charge transport properties to suit various Transitioning the synthesis of COFs from laboratory settings to an
optoelectronic devices, including sensors and transistors. Hence, this industrial scale presents significant challenges. Laboratory-scale
progress represents the versatility of COFs in developing next- methods often yield COFs in limited quantities, complicating the
generation electronic and optoelectronic technologies [373]. scaling-up process. Issues such as reproducibility, cost, and process
Alihosseini et al. (2023) examined the optoelectronic characteristics optimization become prominent when moving to larger scales. Recent
of bilayers and heterostructures composed of C₆N₆ and B₆O₆ COFs using studies have highlighted these challenges, particularly with sol­
first-principles methods. Their research, which integrates excitonic ef­ vothermal synthesis methods, where minor deviations in reaction con­
fects through the G₀W₀-BSE approach along with van der Waals cor­ ditions can lead to substantial variations in product quality. This
rections, reveals that AC-stacking is the energetically favorable variability in large-scale production can impact the consistency and
configuration. In this configuration, the alignment of C-N or B-O rings economic feasibility of COF synthesis. Effective scaling-up requires the
with the pores of the lower layer causes a surface buckling of 0.55 Å and development of robust synthesis protocols that preserve high-quality
results in an intrinsic type II band alignment. These attributes lead to a COFs while optimizing cost-efficiency, necessitating advancements in
redshift in optical absorption, and the computed band edge alignments reactor design and process control [375,376].
indicate promising applications in photocatalytic water splitting [374].
7.1.2. Complexity and Reproducibility
6. Challenges in COFs’ synthesis, characterization, and The synthesis of COFs involves precise control over numerous reac­
application tion conditions, including temperature, solvent, and time, making
reproducibility a critical issue. Research has shown that even slight
Challenges in synthesizing, characterizing, and applying, as shown in variations in these parameters can result in significant differences in the
Fig. 18, include managing their complex synthesis processes, which COF’s structural properties, such as crystallinity and porosity. This
often require precise conditions and result in variable product quality. sensitivity highlights the need for stringent control and standardization
All the synthesis methods have their own advantages and disadvantages, during synthesis to achieve consistent results. Moreover, the complexity
which are tabulated in Table 8. Characterization can be difficult due to of COF synthesis often involves multiple reaction steps and the use of
the frameworks’ intricate structures and potential sensitivity to envi­ sensitive reagents, which can further exacerbate issues with reproduc­
ronmental conditions, making accurate analysis and validation chal­ ibility. Developing standardized synthesis protocols and advanced
lenging. In practical applications, ensuring COFs’ stability and monitoring techniques is essential for ensuring consistent product
performance under real-world conditions, such as exposure to moisture, quality and performance across different environments batches.

Fig. 18. Challenges in COFs’ synthesis.

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

7.1.3. Functionalization dynamic light scattering, to monitor structural changes in real time.
Functionalizing COFs to tailor their properties for specific applica­ These methods hold promise for providing a more comprehensive un­
tions is a complex process that requires careful optimization. Incorpo­ derstanding of COF behavior but require further development and
rating functional groups into COFs can significantly enhance their refinement validation.
performance, such as improving selectivity or catalytic activity; how­
ever, it also presents challenges in maintaining the framework’s stability 7.2.3. Structural Analysis
and structural integrity. Recent studies have demonstrated that the Accurate determination of COF structures, including pore size, con­
success of functionalization strategies depends on the chemical nectivity, and overall framework integrity, is a complex task due to the
compatibility of the functional groups with the COF framework and the intricate nature of COF architectures. The complexity of COF structures
precision of the reaction conditions. Balancing these factors is crucial to often necessitates advanced analytical methods and sophisticated
achieving the desired functionality while preserving the COF’s inherent interpretation skills. XRD and gas adsorption studies are commonly
properties. Effective functionalization strategies involve carefully used. However, interpreting the data can be challenging due to the often
selecting functional groups and optimizing synthesis conditions to ambiguous or overlapping signals. Furthermore, multiple types of pores
ensure that the modifications do not adversely affect the COF’s overall and functional groups within a COF framework add to the difficulty of
performance effectiveness. achieving precise structural characterization. Developing and refining
analytical methods to accurately resolve these complexities is essential
7.2. Characterization Challenges for advancing COF research and applications. Yong Cui et al. reported
the successful synthesis of 14 MOCOF single crystals within 1 to 2 days,
Characterizing COFs presents significant challenges due to their with sizes ranging from 50 to 500 μm. Their structures were determined
complex structures and sensitivity to environmental conditions. Accu­ using single-crystal X-ray diffraction (SCXRD) at resolutions as high as
rately determining COFs’ structural integrity and crystallinity can be 0.79 Å. The SCXRD analysis revealed that both MOCOFs crystallized in
difficult, with conventional methods like X-ray diffraction and scanning the C2/m space group, with all non-hydrogen atoms refined aniso­
electron microscopy sometimes falling short, especially if the frame­ tropically [378].
works degrade under ambient conditions. Nitrogen adsorption/desorp­ Fig. 19(k) presents the XRD patterns of MOF-5, MOF-5-NH2, and
tion and infrared spectroscopy are necessary to elucidate pore structures MOF@COF, all of which confirm the well-defined cubic structure of
and functional groups. However, these methods can be complicated by MOF-5. The XRD pattern of MOF-5 displays characteristic peaks at 2θ =
the COFs’ susceptibility to moisture, heat, and chemical exposure. 6.8, 10.0, 13.6, 15.7, 19.2, 20.6, 22.6, and 25.1, consistent with previ­
Advanced techniques, including synchrotron X-ray methods and high- ously reported diffraction patterns for MOF-5. The distinct peaks cor­
resolution NMR spectroscopy, are often required to obtain detailed responding to the [143,207,244], and [312] planes further validate its
and reliable characterization data. cubic lattice structure. In the case of MOF@COF, the XRD pattern in
Fig. 18(k) reveals variations in peak width and sharpness, suggesting a
7.2.1. Advanced Techniques reduction in crystallinity while preserving the material’s crystalline
Detailed characterization of COFs often necessitates using sophisti­ characteristics. This change is attributed to the successful surface
cated and expensive techniques, such as high-resolution electron mi­ growth of COF. Additionally, as highlighted by the dashed line, the
croscopy, synchrotron radiation, and nuclear magnetic resonance observed peak fluctuation serves as supporting evidence for COF for­
(NMR) spectroscopy. These advanced methods provide crucial insights mation [377].
into the structural and chemical properties of COFs, but their high cost
and technical complexity can limit accessibility for many researchers. 7.3. Application Challenges
For instance, high-resolution electron microscopy is essential for visu­
alizing COF structures at the atomic level but requires specialized Integrating COFs into practical applications requires addressing
equipment and expertise. Similarly, synchrotron radiation techniques several key challenges. These challenges include ensuring stability
offer detailed structural information but are typically available only at under various environmental conditions, such as moisture, heat, and
large-scale facilities. The technical demands and high costs associated chemical exposure. Optimizing performance is also essential, necessi­
with these techniques pose significant barriers to the widespread and tating precise control over parameters like pore size and surface area to
routine characterization of COFs. fit specific applications. Furthermore, effective integration into devices
Shaoxiang Li et al. MOF-5 and MOF@COF exhibit distinct structural involves resolving issues of compatibility and efficiency, which demands
features observable through scanning electron microscopy (SEM). As a multidisciplinary approach that combines materials science, engi­
shown in Figs. 2(a) and (b), MOF-5 possesses a well-defined cubic neering, and device fabrication expertise.
structure. In Fig. 2(c) and (d), it is evident that spherical COF structures
uniformly coat the surface of the MOF-5 cube, forming in situ. MOF@­ 7.3.1. Stability
COF composite retains its cubic morphology, though the surface appears The stability of COFs is a significant concern due to their sensitivity
rougher. Additionally, Fig. 2(g) and (h) confirm the presence of zinc and to environmental factors such as moisture, heat, and chemical exposure.
nitrogen in the elemental mapping, verifying the successful synthesis of COFs can undergo hydrolysis when exposed to moisture, resulting in a
the MOF@COF shell material [377]. loss of crystallinity and functionality. Researchers have been exploring
various strategies to enhance the moisture resistance of COFs, including
7.2.2. Dynamic Behavior developing more robust structures and applying protective coatings.
Studying the dynamic behavior of COFs under varying conditions is High temperatures can also affect the thermal stability of COFs, leading
crucial for understanding their real-world performance, but this requires to structural degradation. Recent studies have focused on designing
advanced in situ characterization methods. It is challenging to develop COFs with improved thermal stability by incorporating heat-resistant
techniques that can accurately capture real-time changes in COF struc­ building blocks and optimizing synthesis conditions. Chemical expo­
tures as they interact with different environmental conditions. Tradi­ sure presents another challenge; COFs may react with aggressive
tional characterization methods often provide static snapshots of COF chemicals, impacting their performance. Strategies to address this
structures, which may not fully capture their dynamic responses to include functionalizing COFs with protective groups or integrating
environmental stimuli such as temperature, pressure, or chemical chemical-resistant materials into their structure. Ensuring that COFs
exposure. To address this, researchers are exploring new in situ tech­ maintain consistent performance under diverse environmental condi­
niques, such as environmental scanning electron microscopy and tions is crucial for their practical applications.

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

Fig. 19. SEM images of (a) (b) MOF-5(c–i) MOF@COF; Elemental mapping images of (g) (h)MOF@COF; EDS of (j) MOF@COF; XRD of (k) MOF-5, MOF-5-NH2 and
MOF@COF; FT-IR of (l)MOF-5 and MOF@COF. Reproduced with permission from 372. Copyright 2025 Elsevier.

The stability of COFs is highly dependent on the type of linkages used improved catalytic efficiency. Chemical functionality is also critical, as
in their construction. Different linkage modes exhibit varying degrees of functional groups can influence the performance of COFs in specific
resistance to environmental factors such as moisture, heat, and chemical applications such as sensing. Tailoring these functionalities requires a
exposure. For example, imine-linked COFs are generally less stable in detailed understanding of their interaction with the COF framework and
acidic or humid conditions due to the reversible nature of the imine the target analytes. Advances in computational modeling and synthetic
bond, which can hydrolyze under these circumstances. However, recent techniques aid in designing and optimizing COFs to achieve desired
advancements have shown that β-ketoenamine-linked COFs exhibit performance outcomes.
enhanced stability, particularly in acidic and alkaline environments, due
to the irreversible enol-keto tautomerism that occurs after the initial 7.3.3. Integration into devices
imine formation. This makes β-ketoenamine-linked COFs more suitable Integrating COFs into practical devices such as sensors, filtration
for applications requiring long-term stability in harsh conditions units, and energy storage systems poses several challenges, particularly
(Table 10). regarding their solubility and device processing properties. COFs are
typically synthesized as insoluble microcrystalline powders, which can
7.3.2. Optimization of COF properties for specific applications limit their processability in device fabrication. Addressing these chal­
Performance optimization of COFs involves balancing factors such as lenges demands a multidisciplinary approach, combining materials
pore size, surface area, and chemical functionality. In gas storage ap­ science, engineering, and device fabrication insights.
plications, optimizing pore size is crucial for achieving maximum stor­
age capacity. Research has shown that precise control over pore size 7.3.3.1. Solubility of COFs. The inherent insolubility of COFs in com­
during synthesis can significantly impact the performance of COFs in gas mon solvents is a significant barrier to their application in device
adsorption applications. Similarly, enhancing the surface area of COFs is fabrication. This insolubility arises from the strong covalent bonds that
vital for applications like catalysis, where increased surface area leads to

Table 10
Differences in the stability of COFs based on different linkage modes.
Linkage Type Stability Characteristics Strengths Weaknesses Strategies to Enhance Stability

Imine-linked COFs Susceptible to hydrolysis in acidic or Easy synthesis, Tuneable Degrades in moisture, Limited Introduce bulky groups or electron
aqueous environments due to reversible pore size and functionality stability in acidic conditions donating substituents, Use hydrophobic
imine bonds. monomers
Boronate ester- Prone to hydrolysis in water due to Self-healing properties, Hydrolyzes in aqueous Steric shielding of boronate groups, Use
linked COFs dynamic covalent chemistry. reversible bond formation environments, limited long term hydrophobic linkers or protective
stability in water coatings
Triazine-linked Highly resistant to thermal and Exceptional thermal Limited flexibility in Optimize synthesis conditions, Use rigid
COFs chemical degradation due to strong stability, robust framework functionalization and stable monomers
covalent bonds.
β-Ketoenamine Enhanced stability due to irreversible Resistant to hydrolysis, Requires two-step synthesis process Optimize tautomerization conditions,
linked COFs enol-keto tautomerism after Schiff base stable in acidic and basic Use stable precursors for irreversible
reaction. conditions bond formation

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S. Raghav et al. Applied Materials Today 44 (2025) 102694

form the framework, making it difficult to dissolve COFs without and behaviours. Future research should focus on developing high-
degrading their structure. Researchers have explored various strategies throughput screening methods to identify the most promising COF
to address this issue, including introducing solubilizing functional structures for specific applications. Additionally, 3D printing techniques
groups into the COF structure. For instance, the incorporation of flexible could be explored to fabricate COFs with complex architectures and
side chains or polar functional groups can enhance the solubility of COFs tailored functionalities.
in organic solvents, allowing for solution-based processing techniques
such as spin-coating, inkjet printing, and drop-casting. Additionally, the 8.5. Integration with other materials
use of exfoliation techniques to produce COF nanosheets or thin films
has shown promise in improving solubility and processability. Integrating COFs with other materials, such as MOFs, CNTs, and
graphene, could develop hybrid materials with enhanced properties. For
7.3.3.2. Device processing properties. The processing of COFs into de­ instance, COF-MOF composites could merge the high surface area and
vices often requires the formation of thin films or coatings on substrates. tunable porosity of COFs with the catalytic activity of MOFs, resulting in
Techniques such as interfacial polymerization, layer-by-layer assembly, materials with superior performance in gas storage, separation, and
and vapor-assisted conversion have been employed to fabricate COF- catalysis.
based thin films with controlled thickness and uniformity. These
methods enable the deposition of COFs onto various substrates, 8.6. Scalability and processability
including metals, polymers, and ceramics, which is essential for device
integration. Moreover, the mechanical properties of COFs, such as One major challenge in applying COFs is their scalability and pro­
flexibility and durability, play a critical role in their performance in cessability. Future research should focus on developing scalable syn­
devices. For example, in flexible electronics or wearable sensors, COFs thesis methods that can produce COFs in large quantities without
must withstand mechanical stress without cracking or delaminating. compromising quality. Additionally, interfacial polymerization and
Recent studies have demonstrated that blending COFs with polymers or mechanochemical synthesis techniques should be further explored to
other flexible materials can enhance their mechanical stability, making enable the fabrication of COF-based membranes, films, and coatings for
them more suitable for flexible device applications. industrial applications.

8. Future perspective 8.7. Environmental and energy applications

The immense structural diversity and modular design of COFs offer COFs are promising for environmental and energy-related applica­
vast opportunities for developing functional materials tailored for spe­ tions, such as water purification, carbon capture, and energy storage.
cific applications. To fully realize the potential of COFs, future research Future research should focus on optimizing the pore size, surface area,
should focus on the following key areas: and chemical functionality of COFs to enhance their performance in
these areas. For instance, developing COFs with highly selective
8.1. Linkage engineering adsorption sites for heavy metals or organic pollutants could lead to
more efficient water treatment technologies.
Linkage choice is critical in determining the properties and stability
of COFs. Future research should explore the development of new linkage 9. Conclusion
types, such as amide, imide, and thiazole linkages, which offer enhanced
stability and functionality. Additionally, incorporating dynamic cova­ COFs represent an impressive and versatile category of crystalline
lent bonds could enable the creation of COFs with self-healing proper­ porous materials, distinguished by the flexible covalent connections
ties, making them more durable in practical applications. between their organic building blocks. These building blocks mainly
comprise light elements such as carbon, silicon, oxygen, boron, and
nitrogen. COFs possess a unique structural composition that provides
8.2. Functionalization strategies
several advantages compared to other crystalline porous materials,
including inorganic zeolites and hybrid MOFs. Key advantages include
Post-synthetic modification (PSM) offers a powerful tool for intro­
low density, large surface areas, and customizable properties and
ducing functional groups into COFs without disrupting their structural
functionalities. The well-defined pore structures of COFs enhance their
integrity. Future work should focus on developing site-specific func­
potential for advanced applications in fields such as catalysis, adsorp­
tionalization techniques that allow for precisely placing functional
tion, gas storage, and optoelectronics. The growing interest from re­
groups within the COF framework. This could include the use of click
searchers in diverse disciplines highlights COF research’s rapid progress
chemistry, metalation, and host-guest interactions to introduce cata­
and dynamic nature. This review provides a comprehensive summary of
lytic, sensing, or adsorption functionalities.
the latest developments in the design, synthesis, characterization, and
application of COFs, covering a wide range of documented work. The
8.3. Stability enhancement review highlights COFs’ significant potential to address real-world
challenges, particularly in materials science, energy, and catalysis. As
While significant progress has been made in improving the stability the field continues to evolve, there is a growing need to explore new
of COFs, further research is needed to develop COFs that can withstand synthesis techniques, develop innovative linkage types, and identify
harsh environmental conditions, such as high temperatures, acidic or novel applications. Additionally, scaling up COF production will be
alkaline environments, and prolonged exposure to moisture. Strategies crucial for fully realizing the potential of these extraordinary materials.
such as chemical locking (e.g., converting imine linkages to more stable Ongoing research and development are anticipated to pave the way for
amide or thiazole linkages) and incorporating protective coatings could groundbreaking discoveries and applications in both scientific and in­
enhance the long-term stability of COFs. dustrial domains.
Despite significant progress in COF research, several challenges
8.4. Computational Design and Machine Learning remain, including scalability, stability, and processability. The synthesis
of COFs often requires precise conditions, and their characterization can
Using computational modeling and machine learning can accelerate be complex due to intricate structures. In practical applications,
the discovery and optimization of COFs by predicting their properties ensuring stability under real-world conditions and optimizing their

33
S. Raghav et al. Applied Materials Today 44 (2025) 102694

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