Water Research 251 (2024) 121111

Contents lists available at ScienceDirect

Water Research
journal homepage: www.elsevier.com/locate/watres

New directions on membranes for removal and degradation of emerging

pollutants in aqueous systems
Die Ling Zhao a, Wangyi Zhou a, Liguo Shen a, Bowen Li a, Hongyu Sun a, Qianqian Zeng a,
Chuyang Y. Tang b, Hongjun Lin a, *, Tai-Shung Chung c, d, **
a
College of Geography and Environmental Sciences, Zhejiang Normal University, Jinhua 321004, China
b
Department of Civil Engineering, University of Hong Kong, Pokfulam, Hong Kong 999077, China
c
Graduate Institute of Applied Science and Technology, National Taiwan University of Science and Technology, 10607, Taiwan
d
Department of Chemical and Biomolecular Engineering, National University of Singapore, 117585, Singapore

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

Keywords: Emerging pollutants (EPs) refer to a group of non-regulated chemical or biological substances that have been
Emerging pollutants recently introduced or detected in the environment. These pollutants tend to exhibit resistance to conventional
Wastewater treatment treatment methods and can persist in the environment for prolonged periods, posing potential adverse effects on
Membrane-based technology
ecosystems and human health. As we enter a new era of managing these pollutants, membrane-based technol­
Degradation
ogies hold significant promise in mitigating impact of EPs on the environment and safeguarding human health
due to their high selectivity, efficiency, cost-effectiveness and capability for simultaneous separation and
degradation. Moreover, these technologies continue to evolve rapidly with the development of new membrane
materials and functionalities, advanced treatment strategies, and analyses for effectively treating EPs of more
recent concerns. The objective of this review is to present the latest directions and advancements in membrane-
based technologies for addressing EPs. By highlighting the progress in this field, we aim to share valuable
perspectives with researchers and contribute to the development of future directions in sustainable treatments
for EPs.

awareness of the potential risks they pose to human health, particularly

1. Introduction through the contamination of drinking water and food sources
(Noguera-Oviedo and Aga, 2016). As these concerns gain prominence,
In recent years, the unprecedented growth of industrialization and researchers and authorities are paying more attention to understand the
urbanization has led to the introduction of numerous non-regulated implications of EPs and identify implementable measures to mitigate
chemical and biological substances into the environment, collectively their potential harm.
known as emerging pollutants (EPs) (Petrie et al., 2015). They can Currently, the management of EPs presents a significant challenge
originate from industrial, agricultural, pharmaceutical, and urban because conventional wastewater treatment methods (e.g. filtration,
sources and there are over 20 classes of compounds considered as EPs, coagulation, and sedimentation) and their hybrids have been repeatedly
including persistent organic pollutants (POPs), pharmaceuticals and shown to be inefficient or ineffective in removing even trace amounts of
personal care products (PPCPs), veterinary medicines such as antibi­ EPs (Rathi et al., 2021; Rodriguez-Narvaez et al., 2017). In response to
otics, endocrine-disrupting chemicals (EDCs), and nanomaterials like the escalating challenges posed by EPs, membrane-based technologies
micro/nano plastics which little is known regarding their environmental have emerged as a promising and efficient approach for their removal
fate or effects (Noguera-Oviedo and Aga, 2016; Taheran et al., 2018). (Dharupaneedi et al., 2019). Membrane separation processes offer
Although the complete extent of their impacts on the environment and distinct advantages, such as high selectivity, scalability, small footprint,
human health remains uncertain, there is a mounting apprehension that and cost-effectiveness, making them an attractive solution for tackling
they could be exerting severe adverse effects on aquatic ecosystems and the diverse array of EPs (Kim et al., 2018). Membranes can be designed
wildlife (Taheran et al., 2018). Additionally, there is a growing to selectively remove specific pollutants based on their size, charge, and

* Corresponding author.
** Corresponding author at: Department of Chemical and Biomolecular Engineering, National University of Singapore, 117585, Singapore.
E-mail addresses: [email protected] (H. Lin), [email protected] (T.-S. Chung).

https://doi.org/10.1016/j.watres.2024.121111
Received 31 August 2023; Received in revised form 6 December 2023; Accepted 5 January 2024
Available online 6 January 2024
0043-1354/© 2024 Elsevier Ltd. All rights reserved.
D.L. Zhao et al. Water Research 251 (2024) 121111

Nomenclatures PAA-PVP polyacrylic acid (PAA) and polyvinylpyrrolidone (PVP)

composite membranes
AC activated carbon PDA polydopamine
ARB antibiotic-resistant bacteria PEM polyelectrolyte multilayer
ARGs antibiotic-resistant genes PIMs polymers of intrinsic microporosity
BP benzylparaben PNF photocatalytic NF membranes
BPA bisphenol A POPs persistent organic pollutants
CFs carbon nanofibers PP propylparaben
CNTs carbon nanotubes PPCPs pharmaceuticals and personal care products
COFs covalent-organic frameworks PPy polypyrrole
CQDs carbon quantum dots PVP polyvinylpyrrolidone
eARGs extracellular ARGs PWP pure water permeance
EAOPs electrochemical advanced oxidation processes R&D research and development
EDCs endocrine-disrupting chemicals RO reverse osmosis
EPs emerging pollutants ROS reactive oxygen species
EPS extracellular polymeric substance SMP soluble microbial product
Fe-POMs Fe-containing polyoxometalates SMX sulfamethoxazole
GO graphene oxide SS-M stainless steel-metal-organic framework
HOFs hydrogen-bonded organic frameworks St stevioside
HWPSs home water purification systems TA tannic acid
MBRs membrane bioreactors TC tetracycline hydrochloride
MF microfiltration TFC thin film composite
MOFs metal-organic frameworks TFN thin film nanocomposite
MP methylparaben TMP trimethoprim
MWCO molecular weight cut-off TPs transformation products
NF nanofiltration WWTPs wastewater treatment plants
OEP oxygen evolution potential UF ultrafiltration
ORR oxygen reduction reaction UV ultraviolet
PAA polyacrylic acid

chemical properties, and therefore, they can achieve high removal ef­ of membrane-based technologies, promising more efficient and sus­
ficiencies for a wide range of pollutants, including those that are difficult tainable solutions for the removal and degradation of EPs. Thus, in this
to remove by conventional treatment methods. In addition, membrane review, we first provide a bibliometric analysis of research trend on EC
processes can be operated at a relatively low cost, especially when being treatment by membrane technologies based on publication records
compared to other advanced treatment methods since they often require dated from 2000 to 2022. Then we aim to disseminate a snapshot of the
a minimal use of chemicals, which reduces the risk of producing harmful new R&D directions on membranes for EPs, covering recent advance­
byproducts and simplifies the overall treatment process. The common ments, breakthroughs, applications in real-world scenarios, limitations,
membranes applied in wastewater treatment plants (WWTPs) constitute and prospects.
nanofiltration (NF), reverse osmosis (RO), ultrafiltration (UF), micro­
filtration (MF) membranes, and membrane bioreactors (MBRs). They 2. Bibliometric analysis of research trend
have been applied successfully to remove a wide range of EPs from
domestic and industrial wastewater (Dharupaneedi et al., 2019; Kim We conducted a simple bibliometric analysis based on publications
et al., 2018). on membrane-based EP treatment in the past 2 decades to reveal the
The separation efficiency of a membrane is heavily influenced by its thematic networks and knowledge frame as well as illustrate the evo­
specific characteristics, including porosity, surface charge, and hydro­ lution of hotspots and research trends. The dataset was sourced from the
phobicity, in addition to the properties of the treated EPs. In the last Web of Science Core Collection’s online database. Topics, encompassing
decade, extensive research has been devoted to developing highly titles, abstracts, and keywords were set to include terms like "mem­
advanced membrane materials that aim to overcome the inherent trade- branes for emerging pollutant*" or "membranes for emerging contami­
off relationship between water permeability and selectivity for water- nant*". The time frame was established from January 1, 2001, to
solute or solute-solute interactions. Moreover, recent advancements December 31, 2022. From the statistics depicted in Fig. 1a, it is evident
have transformed membranes from simple separation barriers for EPs that together with the research on EPs, research on membranes for EPs
into multifunctional platforms for additional functions such as catalytic has become increasingly important, experiencing a remarkable surge
degradation of EPs, enhancing their overall effectiveness in water over the past 20 years. Moreover, this upward trend is expected to
treatment (Urtiaga, 2021; Subramaniam et al., 2022; Matei et al., 2022; persist in the years ahead, highlighting the growing significance of
Pekgenc et al., 2022). Furthermore, ongoing intensive research is membrane studies in conjunction with research on EPs.
focused on evaluating the removal efficiency of membrane technologies To accurately analyze the content of each publication, keywords
for other EPs, including micro/nano plastics and antibiotic-resistant were extracted using VOSviewer (Version 1.6.17) for analysis (van Eck
genes (ARGs) (Ren et al., 2018; Yang et al., 2023, 2022). These rising and Waltman, 2010). Only keywords appearing more than 30 times
environmental concerns are driving researchers to explore and optimize were considered for further studies. During the term extraction process,
membrane-based approaches to tackle the diverse array of contempo­ two categories of irrelevant words were excluded. First, non-technical
rary pollutants. terms such as “all,” “min,” and “limit,” and units of measurements
Overall, the continuous evolution of membrane materials and the were disregarded, as they held no significance for the research topic.
incorporation of novel functionalities are revolutionizing the landscape Second, broadly used technical terms like “emerging pollutants,”

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D.L. Zhao et al. Water Research 251 (2024) 121111

Fig. 1. (a) Numbers of publications related to EPs (blue columns for the left Y axis) and membranes for EPs (orange line for the right Y axis) since 2000 (data
obtained from Web of Science). The publications on membranes for EPs are further categorized into more specific catalogues in the pie chart; (b) A co-occurrence
network map of frequent terms like titles, keywords, and abstracts and their average emerging times.

“emerging contaminants,” and “pollution,” despite their high frequency, 3. New membranes for EP separation
were eliminated to enhance clarity and precision in the results. From the
titles, keywords, and abstracts of the publications, a total of 52 pertinent To overcome critical deficits of commercially available membranes,
terms were identified and used to create the co-occurrence networks, as such as insufficient rejection and low efficiency for large treatment
depicted in Fig. 1b. In this figure, the frequency of a term is represented amounts, tailoring membrane chemistry and structure (e.g. surface
by the size of its bubble, while the color signifies the average time of modification, morphology control, and nanoarchitecture construction)
emergence of the terms. It’s important to note that the study period has risen as an important topic in the design of new membranes for EP
ranged from 2000 to 2022, but publications before 2017 were too sparse separation (Wang et al., 2022a). For instance, thin film composite (TFC)
and the keywords were unfocused to contribute significantly to the term NF and RO membranes have proven effective in removing various pol­
generation. lutants from wastewater, including inorganic salts. However, these
In the initial phase (indicated by blue in the figure), the research membranes often exhibit limited rejection rates for neutral and hydro­
predominantly concentrated on identifying and understanding the phobic organic micropollutants, such as EDCs. For example, the NF200
toxicity of EPs, with terms like “pharmaceutical,” “determination,” membrane exhibited a rejection <50 % for bisphenol A (BPA) (Yanga­
“occurrence,” “source,” and “health” being more frequent. The research li-Quintanilla et al., 2009), while Jin et al. (2010) reported low rejection
focus then evolved towards evaluating EP treatment using membranes rates ranging from 10 to 50 % for estrone using both NF and RO
and developing new membranes, as indicated by frequently used terms membranes.
such as “performance,” “challenges,” “material,” “efficient removal,”
and “kinetics.” In the most recent phase, represented by red circles in 3.1. Manipulation of membranes’ surface and pore structure
Fig. 1b, the research emphasis has shifted to the simultaneous separation
and degradation of EPs and their transformation products (TPs) using A hydrophilic surface coating on the membrane surface has been
membranes. This phase highlights the growing interest in photocatalysis applied to address this limitation. For example, coating NF90 mem­
and advanced oxidation as key integrated technologies, as suggested by branes with polydopamine (PDA) resulted in a significant reduction of
terms like “degradation,” “mechanism,” “photocatalyst,” “nano­ BPA passage, up to 75 % compared to the uncoated NF90 ones (Guo
material,” “activation,” and “visible light.” et al., 2016). Sorption experiments demonstrated that the hydrophilic
PDA coating effectively weakened the hydrophobic interactions

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D.L. Zhao et al. Water Research 251 (2024) 121111

Fig. 2. (a) Interfacial polymerization reaction between St in an aqueous NaOH solution and trimesoyl chloride (TMC) in hexane; (b) PWP and Na2SO4 rejection of the
St/TMC TFC membrane with different St concentrations; (c) Rejections of various antibiotic molecules using St0.1/TMC0.1–3; Reprinted with permission from Bai
et al. (2023). Copyright 2023 American Association for the Advancement of Science; (d) Schematic illustration of the preparation of MP30 nanosheet and MP30
membrane; (e) d-spacing and (f) separation performance of the Ti3C2Tx, MP10, MP20, and MP30 membranes using an aqueous feed solution of bacitracin with a
concentration of 200 ppm; Reprinted with permission from Sun et al. (2022). Copyright 2022 Wiley-VCH GmbH.

between EDC and the membrane, thereby reducing EDC sorption. In c). By employing a combined theoretical-experimental approach, they
another study (Guo et al., 2017a), researchers immobilized silver optimized the structure of St-derived membranes, underscoring the
nanoparticles on PDA-coated polyamide-based commercial TFC mem­ significance of an ultrathin selective layer and a microporous structure
branes (i.e., NF90). A resistance-in-series analysis indicated that this with an enhanced free volume. In addition, thy highlighted the specific
coating displayed a high water permeability while being highly resistant monomer requirements for achieving such membrane features,
to EDCs, resulting in an EDC selectivity an order of magnitude greater including low diffusion rates, moderate reactivity, and a rigid contorted
than the pristine and bare PDA-coated NF90 NF membranes. Further­ structure.
more, Tang’s group developed a green and efficient coating method
using a tannic acid (TA) and ferric ion (Fe3+) complex on a commercial 3.2. Membranes based on new porous materials
NF270 membrane, resulting in a smaller effective pore size and signif­
icantly higher rejections of both NaCl and EDCs (Guo et al., 2017b). In the last decade, a wide range of alterative membrane materials,
Comparing to the more time-consuming PDA coating, the TA-Fe coating especially porous ones with relatively rigid and highly tuneable pore
produced membranes with a lower EDC permeability. structure and rich surface functionality, spring up and show great po­
The pore structure of selective layers in NF and RO membranes can tentials to surpass polymeric membranes with breaking the “trade-off”
also be finely manipulated through a judicious choice of monomers for relationship between permeability and selectivity in polymeric mem­
interfacial polymerization. Bai et al. (2023) developed ultrathin poly­ branes for EP separation (Dou et al., 2021; Jiang et al., 2022; Sun et al.,
ester NF membranes with enhanced structural rigidity and micropo­ 2023; Yu et al., 2023a). These materials, such as polymers of intrinsic
rosity using stevioside (St), a contorted molecule derived from plants, as microporosity (PIMs), metal-organic frameworks (MOFs),
a key building block for interfacial polymerization (Fig. 2a). These covalent-organic frameworks (COFs), hydrogen-bonded organic frame­
membranes exhibited outstanding antibiotic desalination performance works (HOFs), graphene oxide (GO), graphitic carbon nitride (g-C3N4),
with an unprecedented pure water permeance (PWP) of 81.2 l m− 2 h− 1 and MXenes, exhibit remarkable characteristics including ultra-fast
bar− 1 (LMH/bar) and a salt/antibiotic separation factor of 11.4 (Fig. 2b, water permeation and exceptional selectivity (Huang et al., 2024; Dai

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D.L. Zhao et al. Water Research 251 (2024) 121111

Fig. 3. (a) Schematic illustration of pH-responsive nanochannels in GO-PEI; (b) Rejections of methylene blue (MnB, positively charged) and methyl orange (MO,
negatively charged) of GOM and 5p-nGOM at pH 2, 7, and 12; Reprinted with permission from Zhang et al. (2021a). Copyright 2021 American Chemical Society; (c)
Illustration of the voltage-gated membrane (BABD-CB) in an electric field; (d) Gating performance for methyl green (50 ppm, 4 bar) of the BABD-CB membrane
(inserted is the SEM surface morphologies of the BABD-CB membrane; e) Comparisons in response performance of the BABD-CB membrane with state-of-the-art
nanofiltration membranes; Reprinted with permission from Wang et al. (2022b). Copyright 2022 American Chemical Society.

et al., 2024; Lin et al., 2022a; Zhao et al., 2021a; Wang et al., 2023; You excellent performance. Additionally, the water flux exhibited a linear
et al., 2023). Most of them can also be designed at the atomic level with increase with increasing pressure while maintaining a constant rejection
precise window sizes according to the separation requirements for rate, indicating the sufficient rigidity and mechanical properties of the
different EPs (Halliwell et al., 2023; Lu et al., 2021; Sun et al., 2022). In nanochannels within g-C3N4.
addition, their features of high porosity and surface area also impart the To further enhance the water permeance of these membranes, re­
membranes with a high adsorption capacity for EPs (Qalyoubi et al., searchers have explored various strategies involving the manipulation of
2021; Song et al., 2021; Zhao et al., 2021b). pore/interlayer structure and surface chemistry (Shi et al., 2022; Wu
Incorporating these novel materials into traditional membranes, et al., 2022, Zhang et al., 2021d). For instance, Ran et al. (2019)
either as thin film nanocomposite (TFN) or mixed matrix membranes, introduced molecules with -SO3H and benzene moieties between the
has proven to be a viable approach because the resultant membranes layers of g-C3N4 to disrupt the tightly stacked structure and enlarge the
have notable enhancements in separation performance (Zhao et al., interlayer channels. This modification resulted in a remarkably
2023a, 2023b, 2023c, 2022, 2020a, 2020b; Dai et al., 2019; Liu et al., improved water permeance of 8867 LMH/bar, two orders of magnitude
2022a; Pan et al., 2023; Yu et al., 2023b). Dai et al. (2019) fabricated higher than the pristine membrane, while maintaining a rejection of
TFN NF membranes that contained MIL-101(Cr) with pentagonal (1.2 100 % toward methyl blue. Additionally, the introduction of -SO3H sites
nm) and hexagonal (1.6 nm) structures to filter out EDCs. The optimal facilitated the firm anchoring of N atoms within g-C3N4 through
TFN membranes had a water flux of 39.5 LMH, which was 1.3 times acid-base interactions, enhancing the stability of nanochannels in harsh
higher than the TFC membranes (i.e., 17.5 LMH). They were able to environments. In another study, Sun et al. (2022) prepared
reject methylparaben (MP), propylparaben (PP), benzylparaben (BP), inorganic-organic hybrid MXene-pillararene nanosheets with a large
and BPA at rates of 47.4 %, 45.9 %, 51.1 %, and 79.8 %, respectively, lateral size of 5–8 μm and an interlayer spacing of 1.36 nm (Fig. 2d, e),
which were significantly higher than the control values of 27.7 %, 25.2 which were utilized for purifying antibiotic-containing water. The per­
%, 31.3 %, and 64.9 %, respectively. In a subsequent study (Dai et al., meance of their membrane increased 100-fold compared to most poly­
2020), they created dually charged MOFs by adding ethylenediamine to meric and other two-dimensional (2D) NF membranes, while
MIL-101(Cr) and integrated them into the selective layer to remove maintaining promising rejections towards a wide range of antibiotics,
pharmaceuticals from wastewater. The resulting membranes exhibited a from ampicillin (349.4 g mol− 1, 88.9 % rejection) to bacitracin (1422.7
higher water permeance of 17.3–24.6 LMH/bar and greatly improved g mol− 1, 95.8 % rejection) (Fig. 2f). The enhanced separation perfor­
rejections of positively charged pharmaceutical active compounds while mance arose from the large lateral size of nanosheets, regular interlayer
maintaining high rejections of negatively charged ones. spacing, and electrostatic interactions between the membrane and
Microporous framework membranes composed solely of these antibiotics.
porous materials hold immense promise as the next-generation mem­
branes and have spurred significant interests, leading to a flourishing
research domain. Caro et al. (Wang et al., 2017a) successfully developed 3.3. Stimuli-responsive membranes
a g-C3N4 membrane by assembling partially exfoliated g-C3N4 nano­
sheets. Their optimal 160-nm-thick g-C3N4 membrane exhibited an In addition, inspired by stimuli-responsive cell membranes, func­
impressive water permeance of 29 LMH/bar. Moreover, it displayed tional membranes possessing smart gating properties (i.e., controllable
rejections of 75.5 %, 87.2 %, 93.1 %, and 99.5 % for rhodamine B, Evans and reversible pore structures) have been developed in order to meet the
blue, cytochrome c, and 5 nm-diameter Au nanoparticles, respectively. separation requirements for different EPs (Han et al., 2022; Liu et al.,
The presence of transport pathways, including artificial nanopores 2023). Their inherent characteristics, including surface charge, pore
(ranging from 1.5 to 3 nm) and interlayer passages between nanosheets size, porosity, and surface morphology, can be distinctly controlled by
(created by unstripped fragments), contributed to the membrane’s environmental stimuli such as light (Liu et al., 2020), electricity (Wang
et al., 2022b), pH (Zhang et al., 2021a), temperature (Zhang et al.,

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D.L. Zhao et al. Water Research 251 (2024) 121111

Fig. 4. (a) The microscopic images of the PAA-PVP membranes before and after self-repairing in water for 2, 12, and 48 h, respectively; (b) The recovery of sep­
aration performance of the damaged membrane as a function of self-repairing duration; (c) The mechanism behind the self-repairing process of the damaged
membrane within water; Reproduced with permission from Han et al. (2021). Copyright 2021 Wiley-VCH GmbH; (d) The targeted repair of the SS-M membrane
mimicking the broken foot repair of an octopus; (e) The flux and rejection of SS-M membrane before and after the repair process; (f) SEM images of the damage repair
of SS-M after exposure for 15, 30, 60, and 120 s; Reproduced with permission from Zhang et al. (2023). Copyright 2023 Wiley-VCH GmbH.

2022), and specific molecules (Shu et al., 2023). Bioinspired by the voltage but also enabled to cycle the voltage eight times, showing its
filtration function of the renal glomerulus, Zhang et al. (2021a) con­ superiority to most state-of-the-art membranes (Fig. 3e).
structed a smart GO membrane by introducing positively charged
polyethylenimine-grafted GO (GO-PEI) to negatively charged GO 3.4. Self-healing membranes
nanosheets (Fig. 3a). It was found that the additional GO-PEI component
changed the surface charge, improved the hydrophilicity, and enlarged Self-healing, a natural function in biology, has inspired many studies
the nanochannels, with a water permeance up to 88.57 LMH/bar, which to explore artificial materials with self-repairing ability as membranes to
corresponded to 4-time higher than a conventional GO membrane due to sustain their long-term continuous processes for EP treatment. It is
the enlarged nanochannels. Meanwhile, owing to the electrostatic usually realized by strong noncovalent interactions including electro­
interaction, the membrane could selectively remove positively charged static interactions, dipole–dipole interactions, host–guest interactions,
methylene blue at pH 12 and negatively charged methyl orange at pH 2, metal coordination, π-π stacking interactions, and hydrogen bond in­
with a removal rate of over 96 % (Fig. 3b). These impressive separation teractions (Han et al., 2021; Zhang et al., 2023). Han et al. (2021)
performances (i.e., high water permeance and organic removal) resulted designed polyacrylic acid (PAA) and polyvinylpyrrolidone (PVP) com­
from the synergic effect of the precisely controlled nanochannels and posite membranes (PAA-PVP). The membrane could entirely restore
tuneable electrostatic interactions in responding to the environmental separation performance after self-repairing by a simply immersion in
pH. Sun et al. (Wang et al., 2022b) also demonstrated a novel water at 45 ◦ C for 48 h due to the reconstruction of hydrogen bonds
voltage-gated membrane by employing the host− guest interaction be­ between PAA and PVP chains (Fig. 4a–c). Zhang et al. (2023) presented
tween viologen and cucurbit [7]uril molecular containers (Fig. 3c). a novel approach that combined dry-wet spinning and electrosynthesis
Under simple external voltage stimulation, the voltage-gated membrane to create composite membranes comprising stainless-steel metal-organic
exhibited an adjustable ion selectivity and high separation performance framework (SS-M). By taking inspiration from the self-healing mecha­
for molecules with similar sizes. The membrane rejection for charged nism observed in an octopus with a broken foot, they repaired the
organic species could be tuned from 20 to 95 % by applying an electric damaged surface of the SS-M membrane. This was because the damaged
field (Fig. 3d). It not only displayed a high responsiveness to the applied surface had a high electrochemical activity which enabled the

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D.L. Zhao et al. Water Research 251 (2024) 121111

Fig. 5. (a) The separation performance of the GO/M88A membrane for different dyes with and without photo-Fenton; (b) Flux changes with and without the photo-
Fenton process for methylene blue; Reprinted with permission from Xie et al. (2020). Copyright 2019 Elsevier; (c) Schematic illustration of Co-N-C/CF for appli­
cations in solar-driven generation of vapor and persulfate mediating water purification; (d) Evaporation rates and the solar-vapor efficiencies of PE, CF and
Co-N-C/CF; (e) photodegradation constants (k) of CF and Co-N-C/CF with and without persulfate (2 mM) under non-circulating water condition; Reprinted with
permission from Cui et al. (2023). Copyright 2023 Elsevier.

preferential deprotonation of organic ligands and subsequent deposition 4.1. Photocatalytic membranes
of MOFs, thus effectively repairing the damage (Fig. 4d). As the depo­
sition time was prolonged to 120 s, the intercrystalline voids were A promising and increasingly popular approach in the field of water
gradually filled by the newly deposited MOFs, resulting in the formation treatment is the use of photocatalytic membranes. These membranes
of an intact MOF membrane and the restoration of dextran rejection combine sub-nanoscale physical separation with chemical decontami­
capabilities (Fig. 4e, f). nation, effectively harnessing the complementary advantages of both
techniques within a single unit (Gokulakrishnan et al., 2021). In addi­
4. Functional membranes for separation and degradation of EPs tion, immobilization of photocatalysts on the membranes facilitates
their convenient recovery from the wastewater, significantly enhancing
With significant advancements in the development of new mem­ process sustainability and minimizing the treatment unit’s environ­
brane materials and fabrication methods, high levels of EP removal can mental footprint. The process of photocatalysis begins with the ab­
be achieved through various membrane filtration processes. However, a sorption of a photon possessing energy greater than the band-gap energy
persistent challenge arises as EPs and other pollutants gradually accu­ of the photocatalysts (Ren et al., 2018; Chen et al., 2022). This results in
mulate on the membrane surface or within the pores, leading to mem­ the generation of electron-hole pairs, which subsequently react with
brane fouling and a lower productivity (Yangali-Quintanilla et al., 2009; H2O, OH− , and O2, leading to the formation of highly oxidizing species.
Song et al., 2021; Hu et al., 2014). Particularly, WWTPs are recognized These species are capable of initiating a cascade of redox reactions,
as major sources of various EPs, as these pollutants tend to concentrate enabling the degradation of organic materials, including certain EPs
or remain isolated rather than being fully detoxified in these facilities (Song et al., 2023; Zhao et al., 2016).
(Olasupo and Suah, 2021; Zhang et al., 2018; Ziajahromi et al., 2017). The efficiency of photocatalytic membranes heavily relies on the
Consequently, researchers are increasingly mindful of preventing sec­ photocatalytic activity of the employed photocatalysts, which have
ondary pollution caused by EPs discharged as effluents from WWTPs. To continuously evolved with the development of photocatalyst technol­
address this issue, ongoing efforts focus on developing advanced treat­ ogy. Among various photocatalysts, titanium dioxide (TiO2) stands out
ment strategies for EP decontamination. These strategies often entail as the most widely used additive in membranes due to its excellent
integrating physical separation techniques with photocatalytic, elec­ photocatalytic activity under ultraviolet (UV) light, good chemical sta­
trochemical, or biocatalytic processes to effectively degrade a wide bility, low toxicity, and cost-effectiveness (Hatat-Fraile et al., 2017;
range of EPs, including benzene-derived pollutants, heavy metals, an­ Ramasundaram et al., 2013). However, since its absorption edge of is in
tibiotics, chlorinated organics, azo dyes, and more (Urtiaga, 2021; the UV region, only 3–5 % of the total solar energy in the form of UV
Subramaniam et al., 2022; Barbhuiya et al., 2022; Chin et al., 2023). light can be utilized. Additional UV light sources are required which
These processes typically involve reductive and/or oxidative reactions greatly limits its large-scale application. Moreover, single photocatalysts
to achieve successful EP removal and environmental remediation. often suffer from the recombination of photogenerated electrons and
holes, leading to a lower catalytic performance. One should broaden
spectrum of light absorption by combining TiO2 with narrow-bandgap

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D.L. Zhao et al. Water Research 251 (2024) 121111

Fig. 6. (a) Schematic illustration of the mechanisms for membrane electrode-based electro-advanced oxidation processes; (b) Schematic illustration of novel bio­
catalytic membranes with enhanced enzyme activity and stability, developed by precisely adjusting the confinement strength of the enzyme within the membrane
through the modification of the support layer of a polymeric NF membrane, followed by reverse filtration of the enzyme; (c) analyses of storage stability by assessing
the relative activity of Pristine-E, PEI-E, and Zn-E immersed in an acetic buffer (10 mM, pH = 5) for a duration of 7 days; Reprinted with permission from Zhang et al.
(2021c). Copyright 2020 Elsevier.

semiconductors to form heterojunctions. As a result, the efficiency of promises for practical applications. These synergistic processes work
photogenerated charge separation can also be enhanced. together to generate oxidative radicals, significantly enhancing the
Meanwhile, R&D are currently active in the field of other visible degradation of EPs over functional membranes (Lan et al., 2019a;
light-driven photocatalysts, such as g-C3N4, MoS2, BiOCl, MOFs and Liangdy et al., 2023; Xue et al., 2023; Xie et al., 2020). For example, Lan
their heterojunctions (Zhao et al., 2023c; Arefi-Oskoui et al., 2022; et al. (2019a) developed a photo-Fenton-like membrane by vacuum
Cheng et al., 2022; Lin et al., 2022b). Song et al. (2023) fabricated novel filtration of a mixed solution of g-C3N4 sol and Fe-containing poly­
photocatalytic NF membranes (PNF-4) with carbon quantum dots oxometalates (Fe-POMs). Their novel membrane demonstrated syner­
(CQDs) embedded PEI-based polyamide as a carrier and N-doped CQDs gistic pollutant retention and degradation capabilities. Similarly, Xie
modified g-C3N4 surface anchored, and explored their feasibility for et al. (2020) integrated photo-Fenton catalytic MIL-88A(Fe) into GO
separation and degradation of antibiotics in sewage effluents using a nanosheets to create a GO/M88A membrane, which exhibited enhanced
dynamic process. Due to the synergetic photocatalytic activity of CQDs flux of 26.3–30.6 LMH/bar and high separation efficiencies of
and g-C3N4 under visible light, the bifunctional PNF-4 membranes 97.57–99.95 % for various contaminants under visible light (Fig. 5a, b).
effectively decreased the concentrations of trimethoprim (TMP) (rejec­ Moreover, the membrane displayed high photo-Fenton catalytic degra­
tion rate: 99.9 %) and sulfamethoxazole (SMX) (rejection rate: 99.8 %) dation efficiencies, which achieved removal rates of 98.81 % for meth­
by more than two orders of magnitude for both simulated and actual ylene blue within 40 min and 97.27 % for BPA within 80 min.
sewage effluents. Additionally, the fouled membranes showed the In another interesting study, Cui et al. developed a novel bifunctional
lowest fouling coverage after the irradiation of visible light, confirming photothermal membrane (Co-N-C/CF) by modifying N-doped carbon
its superior ability in terms of environmental friendliness and nanosheets with Co nanoparticles. Their membrane offered the dual
cost-effectiveness for fouling removal (Zhang et al., 2021b). benefits of water evaporation and persulfate-mediated water purifica­
The combination of photocatalysis with other advanced oxidation tion simultaneously (Fig. 5c) (Cui et al., 2023). The unique properties of
processes, such as photo-assisted Fenton reaction and photo-assisted carbon-based materials, including molecular thermal vibrations, com­
persulfate oxidation in composite membranes, holds immense bined with the plasmonic effect of Co nanoparticles, contributed to the

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D.L. Zhao et al. Water Research 251 (2024) 121111

remarkable water evaporation rate of 1.88 kg m− 2 h− 1 under 1 sun carbon-CNT hollow fiber membrane could serve as the cathode in an
irradiation which was about 1.8 times as that of a pure carbon fiber cloth electro-Fenton process, generating approximately 38.0 μM of H2O2 at a
(CF) system (Fig. 5d). Additionally, Co-N-C/CF effectively activated potential of -0.8 V without the addition of Fe2+ (Yang et al., 2019). If 0.4
persulfate for phenol removal through a non-radical reaction process, mM Fe2+ was incorporated, the removal efficiencies of the doped
resulting in a significantly enhanced reaction constant of 0.0314 min− 1 membrane to glucose and phenol were approximately 6.2 and 9.7 times
(Fig. 5e). This innovative membrane design not only holds great higher, respectively, compared to membrane filtration alone.
promises for energy-efficient water evaporation but also efficient The limitation of traditional photocatalytic technologies is the quick
pollutant removal, offering potential applications in sustainable systems recombination of photogenerated electron-holes. However, this issue
for water treatment. can be effectively addressed by applying an electric field, which leads to
efficient separation of photogenerated electron-holes and significantly
4.2. Electrochemical reactive membranes enhances photocatalytic efficiency. Studies have shown that both pho­
tocatalysis and electro-oxidation occur simultaneously in the photo­
Electrochemical advanced oxidation processes (EAOPs) have flour­ electrocatalytic process and result in a high synergistic effect on
ished in wastewater treatment due to the efficient utilization of a very pollutant removal. For instance, when using a g-C3N4/CNTs/Al2O3
clean reagent (i.e., the electron) to generate reactive hydroxyl radicals membrane anode in a photoelectrocatalysis system under visible light,
(•OH) in situ (Su et al., 2022; An et al., 2020). The combination of EAOPs the removal efficiency of 5 mg/L phenol was 71.0 %. In comparison, the
and membrane technologies can potentially overcome their own ob­ corresponding removal efficiencies were only 26.0 % in the photo­
stacles. First, the flow-through membrane acts as a barrier to concen­ catalytic system and 36 % in the electrooxidation system (Wang et al.,
trate the EP molecules and provides a more electroactive area than the 2017b). Similarly, the combination of membrane filtration and elec­
plate electrode in traditional EAOPs to remarkably increase the oxida­ troactive persulfate can be achieved by employing membrane cathodes
tion chance of EPs (An et al., 2020; Ren et al., 2023). In addition, the in the electrocatalytic persulfate process, showing a synergistic effect on
combination of these two technologies has been demonstrated to pollutant degradation. Xu et al. (2022) developed an electrocatalytic
effectively mitigate membrane fouling, which would otherwise signifi­ persulfate system using a CNT- polypyrrole (PPy)/PVDF membrane
cantly reduce the separation efficiency. The improvement is achieved cathode. It had removal rate of over 90 % for small molecule organic
through various mechanisms, including electrostatic repulsion, in-situ pollutants, including carbamazepine, sulfamethoxazole, phenol, and
degradation of EPs and other foulants, hydrodynamic shear, and the diclofenac because of higher reaction kinetics constants. Comparing to
formation of a protective air shield on membrane surfaces by bubbles the simple membrane filtration system, the new system exhibited
(Du et al., 2021, 2022a). These mechanisms work together to prevent significantly better removal efficiency for all pollutants. In addition, its
the accumulation of foulants and ensure a more efficient and sustainable performance remained relatively stable during 20 operating cycles.
operation of membrane systems. Electro-peroxone is another process that involves the generation of
Novel membrane electrodes (e.g., carbon-, metal/metal oxide-, H2O2 through a two-electron oxygen reduction reaction (ORR) on the
ceramic-, and polymer-based conductive membranes) have been cathode surface, followed by the reaction of H2O2 with ozone to produce
designed and fabricated to ameliorate their electrochemical activity, •OH. A flow-through CNT membrane cathode in the electro-peroxone
conductivity, porosity, corrosion resistance, and long-term stability (Su system has been demonstrated to effectively remove 95.75 ± 1.12 %
et al., 2022; Du et al., 2022b; Li et al., 2022a; Xu et al., 2022; Yang et al., of ibuprofen, a typical ozone-resistant pharmaceutical and personal care
2022b). In electro-oxidation processes, the choice of anodes signifi­ product. This value surpassed the removal rates achieved by means of
cantly affects the performance of the systems. Non-active membrane electrochemical filtration, ozonation- and peroxone-coupled filtration
anodes, which possess a higher oxygen evolution potential (OEP), are by 3.72, 1.97, and 1.60 folds, respectively (Yang et al., 2022c). These
preferred over active anodes. Among them, sub-stoichiometric titanium advanced combinations of electro-oxidation processes with membrane
oxide membranes and modified carbon or titanium membranes coated technologies truly offer promising and efficient solutions for pollutant
with non-active anode materials such as PbO2, SnO2, and boron-doped removal in wastewater treatment.
diamond, hold great promise for practical applications (Liu et al.,
2017; Ma et al., 2023; Xu et al., 2019; Yu et al., 2020). Yu et al. (2020) 4.3. Biocatalytic membranes
successfully designed a novel membrane for electrochemical degrada­
tion. They integrated graphene/tin dioxide (G/SnO2) into carbon Biocatalytic membranes, which harness the synergistic effect of
nanofibers (CFs) to create a flow-through MF membrane based on membranes and enzymes, have emerged as an attractive method for
polyacrylonitrile (PAN). The PAN-based G/SnO2/CFs MF membrane treating EPs. Immobilizing enzymes on membranes offers several ad­
exhibited an 85 % higher electrochemical degradation rate for SMX than vantages, including enzyme reusability and higher operational stability
the pure CFs due to the synergistic effect of graphene and SnO2. It (Vitola et al., 2021; Zhao et al., 2023d). Unlike other catalytic mem­
effectively degraded SMX into nine non-toxic smaller intermediates, as branes, biocatalytic membranes do not require additional external fac­
confirmed by LC-MS/MS analyses. Remarkably, the CFs membrane did tors like UV visible light for photocatalytic membranes or power supply
not interfere with the electrocatalytic degradation process, underscoring for electrocatalytic membranes, making them more self-sufficient.
the efficiency and compatibility of the PAN-based G/SnO2/CFs MF Moreover, biocatalytic membranes outperform photocatalytic mem­
membrane. branes in terms of membrane lifespan, as the latter may experience
In the pursuit of higher degradation efficiency and shorter retention degradation due to hydroxyl radicals or UV radiation, while the enzymes
time, membrane electrode-based EAOPs have evolved beyond simple anchored on biocatalytic membranes do not compromise the polymer’s
electro-oxidation to encompass various innovative approaches, such as longevity. As a result, biocatalytic membranes represent a promising
electro-Fenton (Li et al., 2020a; Jiang et al., 2018), and sustainable approach for EP treatment.
photo/thermo-electrocatalysis (Li et al., 2022b; Liu et al., 2019), elec­ Enzymes play a crucial role in wastewater treatment, and several
trocatalytic persulfate (Xu et al., 2022), and electro-peroxone (Yang types have proven effective for this purpose: oxidoreductases (such as
et al., 2022c). Their differences and characteristics are depicted in peroxidases, polyphenol oxidases, and laccases), hydrolases (including
Fig. 6a (Ren et al., 2023; Wang et al., 2021). In electro-Fenton processes, lipases, proteases, esterases, and cellulases), and lyases (Pekgenc et al.,
membranes are primarily investigated as cathodes and are often based 2022). Among these, laccases and horseradish peroxidase have garnered
on carbonaceous materials such as carbon nanotubes (CNT), graphene, special attention due to their ability to oxidize a wide range of sub­
and porous carbon, which have demonstrated high efficiency in H2O2 strates, their environmental friendliness, and their low energy con­
production (Jiang et al., 2018; Yang et al., 2019). For instance, a porous sumption. Laccase, in particular, stands out as a commonly used enzyme

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D.L. Zhao et al. Water Research 251 (2024) 121111

Fig. 7. (a) Free DNA removal by membranes with different MWCOs and surface charges; (b) Retention of supercoiled pure plasmid, mixture of plasmid and linear
DNA fragments, and mixture of only linear fragments in distilled water by UF2 and RO1 membranes; (c) The effect of free DNA concentration in the feed on free DNA
concentration in the permeate after filtration of spiked distilled water with the RO1 membrane; Reprinted with permission from Slipko et al. (2019). Copyright 2019
Elsevier; (d) Swine wastewater treatment process including pretreatment and a hybrid membrane filtration system; (e) Absolute abundances of the 5 types of ARGs
and total ARGs in each stage of treatment; Reprinted with permission from Liang et al. (2021). Copyright 2020 Elsevier; (f) DNA concentrations in the influent and
effluent of membranes with different MWCOs; (g) Concentration of undamaged target plasmid segment DNA during the UV-LED concentrate post-treatment with UV
fluences between 0 and 300 mJ/cm2; Reprinted with permission from Krzeminski et al. (2020). Copyright 2019 Elsevier.

in wastewater treatment because it does not require additional chem­ application to bioremediate EPs. A commercial laccase (EC 1.10.3.2)
icals like H2O2 to initiate the degradation process (Zhao et al., 2023d; Li was utilized as the model biocatalyst, while different strategies were
et al., 2020b; Masjoudi et al., 2021). Phosphodiesterase is a recently employed to improve the catalytic properties of the membranes in terms
explored enzyme in the context of EP investigations (Pekgenc et al., of enzyme loading and apparent activity per membrane weight. Through
2022). the co-deposition of PDA and PEI, the team achieved the best yield of
To enhance the enzyme’s performance and stability, a mussel- enzyme immobilization with an impressive 57.9 ± 0.5 % and a high
inspired coating was utilized by Zhang et al. (2021c) to modify the apparent activity of 6.4 ± 1.1 U per gram of membrane. Comparing with
interior support of an NF membrane. The modification improved charge the free enzyme, the newly fabricated bio-catalytic membranes main­
and steric effects on the enzyme and effectively stabilized it within the tained 80 % of the residual activity even after undergoing five cycles,
membrane, while causing only a minimal increase in mass transfer indicating their robustness and reusability. Additionally, they demon­
resistance for substrates and products (Fig. 6b). The resultant bio­ strated exceptional pollutant removal capabilities. More than 95 %
catalytic membrane exhibited excellent enzyme retention, and showed depletion was observed for five different EPs including diclofenac,
negligible declines in BPA removal efficiency even after 7 reuse cycles mefenamic acid, benzefabrite, bicalutamide, and clarithromycin.
(<3.5 %) or 36 h continuous operation (<1 %) under a flow-through
mode (Fig. 6c). Clearly, to design biocatalytic membranes effectively 5. EPs of more recent concerns to be treated by membranes
for sustainable wastewater treatment, the membranes must (1) have an
appropriately confinement strength to retain the enzyme and (2) pro­ The list of EPs is continually evolving as new substances are intro­
vide the enzyme with necessary mobility for efficient reactions. duced into the environment, and their potential impacts are studied and
Zhao et al. (2023d) proposed a novel approach to fabricate highly understood. Researchers and environmental authorities have been
flexible SiO2 biocatalytic nanofiber membranes and explored their continuously monitoring and assessing the presence and effects of these

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D.L. Zhao et al. Water Research 251 (2024) 121111

pollutants to develop effective strategies for their mitigation and con­ filters, with Proteobacteria, Acidobacteria, Chloroflexi, and Bacter­
trol. Meanwhile, their treatment by membrane-based technologies has oidetes being the dominant phyla, and Alphaproteobacteria and Gam­
also been progressively studied. maproteobacteria being the predominant classes. The abundances of
Cyanobacteria, Patescibacteria, Bacteroidetes, and Proteobacteria
5.1. Antibiotic-resistant genes (ARGs) showed significant positive correlations with the abundances of ARGs.
The biofilm formation facilitated the adsorption of antibiotics, microbial
The widespread production and usage of antibiotics have accelerated proliferation, and ARG proliferation, leading to an increase in the
the prevalence of antibiotic-resistant bacteria (ARB) and ARGs. Both of presence of antibiotics and ARGs in the effluents of HWPSs.
them pose potential threats to human and ecology because they can As antibiotics are also intensively used in livestock farming, the
result in failures in medical treatment (Calderón-Franco et al., 2021). In resulting swine wastewater becomes the main emission source of ARGs
2006, ARGs were identified as EPs (Pruden et al., 2006), which have (Lan et al., 2019b). Liang et al. (2021) quantified the abundance of 16
been detected widely in environmental reservoirs, such as surface water, target ARGs, which accounted for around 72.6 % of the total ARGs, in
soil, and agriculture wastes. One important distinction between each stage of the swine wastewater filtration process including UF
ARB/ARGs and other EPs is that the former can multiply and spread in (membrane pore size: ~50 nm) and 2-stage RO, as shown in Fig. 7d. The
the environment. WWTPs are recognized as important reservoirs and pore size of UF membranes is 50 nm, much larger than those of bacteria,
sources for various ARB and ARGs (Zhang et al., 2018). Although the but the pressure-driven process could deform bacterial and cause the
disinfection step can inactivate ARB, the release of their cell-free ARG leakage of ARGs from the cells. In the next filtration step, RO rejected
into natural environments might lead to the horizontal transfer of these most of eARGs in the forms of supercoiled plasmid molecules and linear
genes to non-resistant bacteria (Zhang et al., 2018; Li et al., 2018; fragments. However, due to their flexibility, partial eARGs could still
Pepper et al., 2018). Therefore, it necessitates the control of discharging penetrate the RO membranes with pore sizes much smaller than theirs.
these extracellular ARGs (eARGs) from WWTPs to the receiving aquatic The integrated membrane filtration systems totally reduced the ARG
systems. So far, the removal of ARB by membranes is well investigated in concentration from 3.02 × 108 to 6.45 × 105 copy numbers/mL with a
an analogous mechanism of removing bacteria, but the study on rejection rate of 99.79 % (Fig. 7e).
membrane-based eARG removal is still in its infant stage. Zheng and Wang (2022) fabricated polyelectrolyte multilayer (PEM)
Slipko et al. (2019) studied the potential and mechanisms to remove NF membranes with a tailored selectivity for eAGRs by the
eAGRs from different water matrices (i.e., pure water and effluent of a layer-by-layer assembly of poly (diallyl dimethylammonium chloride)
WWTP) by membranes ranging from MF to RO. Several key findings and poly (sodium styrenesulfonate). The loose NF membranes with more
were reported: (1) As illustrated in Fig. 7a, UF membranes with a mo­ than 4 polyelectrolyte bilayers could retain more than 99.9 % eARGs
lecular weight cut-off (MWCO) below 5000 Da were found to retain over from a wastewater effluent under 100 psi (~6.9 bar). However, contrary
99.80 % of free DNA (including pure plasmid containing ARGs and to the Slipko’s finding on the effect of membrane surface charge on
linear fragments) under 12 bar mainly by the size exclusion mechanism. eARG retention, the membrane terminated with polyanionic electrolytes
(2) Membrane surface charge also played a key role owing to the showed enhanced eARG rejections through electrostatic repulsion. The
adsorption of free DNA molecules on the membrane surface that could disparity in the effects of membrane charge on eARG retention may arise
prevent their passage across the membrane. Generally, negatively from the different applied pressures on the membranes. Because a higher
charged membranes showed a lower retention rate due to the weak applied pressure can overcome the electrostatic repulsion as well as drag
adsorption of the same charged ARGs (Fig. 7a). (3) The retention of free the stretchable eARGs through the membranes rather than being
DNA molecules by membranes was influenced by their size, shape, and adsorbed on the membrane surface, a reduced retention efficiency might
concentration. Because linear and small DNA fragments had a higher be observed for negatively charged membranes at a high operating
elongational flexibility, they could permeate through the membranes pressure than neutral ones (Liu et al., 2022b).
more easily than supercoiled plasmid molecules (Fig. 7b). When the feed To prevent functional activities of genes and avoid the secondary
concentration of free DNA molecules increased, more molecules would pollution by ARGs, Krzeminski et al. (2020) further treated the
be adsorbed on the membrane, resulting in higher retention rates concentrated retentate in UF or NF filtration processes by UV irradiation
(Fig. 7c). (4) Pre-mixing the feed with a WWTP effluent led to a higher at 265 nm (Fig. 7f). They found that UF and NF membranes with a
removal rate of free DNA than pre-mixing it with distilled water. The nominal MWCO of <1 kDa could almost completely remove two
hydrophobic interactions between free DNA and various molecules cell-free DNA plasmids (i.e., Ampicillin resistance genes and Kanamycin
present in the wastewater might increase EP sizes for easier removal Ampicillin resistance genes with respective sizes of 267 bp and 601 bp)
(Breazeal et al., 2013). by a removal value of >5 log (Fig. 7f). Afterwards, UV illumination
Gu et al. (2021) investigated the occurrences of ARGs in tap water, showed effectiveness in inactivating plasmid DNA in the concentrate
effluents, and filters before and after utilizing home water purification retentate. The inactivation rate per segment length for the larger DNA
systems (HWPSs), which sequentially consisting of polypropylene cotton segment (i.e., Kanamycin Ampicillin resistance genes) was higher than
filter (PP), a granular AC filter (GAC), a compressed AC filter (CAC), a that of the smaller one, in accordance with its higher pyrimidine and TT
UF cartridge, and a post granular AC filter (PGAC). In tap waters, the content (Fig. 7g). The fluences necessary to achieve a 1 log inactivation
detected levels of ARGs ranged from below the limit of detection to 3.45 via UV at 265 nm in ultrapure water differed between 267 bp (for
× 105 copies/L. HWPSs equipped with fresh filters effectively removed Ampicillin resistance genes) and 601 bp (for Kanamycin Ampicillin
ARGs, achieving removal rates between 0.46 and 2.43 log. In short, the resistance genes) target segment, with the former requiring 73 mJ/cm2
performance of each unit was analyzed individually. Over the course of a and the latter requiring 23 mJ/cm2. The results indicated that by inte­
week, the units PP, GAC, CAC, UF, and PGAC demonstrated ARG grating membrane filtration with UV, it is possible to remove and
removal efficiencies ranging between 0.07–0.47 log, 0.01–1.37 log, damage eARGs simultaneously.
0.03–0.20 log, 0.07–1.63 log, and 0.04–1.75 log, respectively. However, Zhu et al. (2018) elucidated the fate of ARGs during the MBR process
following operations lasting 3 or 6 months without changing the filters, and paid special attention to the role of membrane fouling in ARG
it was observed that the ARG levels in the treated water were higher than removal. They found that although the addition of SMX and tetracycline
those in the incoming water. Each unit played a role in this increase, hydrochloride (TC) increased ARG abundance by 0.5–1.4 orders of
where UF also showed a significant contribution. The filters in HWPSs magnitude in the activated sludge and membrane fouling layer, the
contained ARGs with relative abundances (i.e., the ratio of the abun­ membrane module displayed robust performance to remove ARGs with
dance of ARGs to the abundance of 16S rRNA) ranging from 2.56 × 10− 8 the abundance of removed ARGs in the range of 0.6–5.6 orders of
to 2.89 × 10− 2. Biofilms were observed to form within many HWPS magnitude. Additionally, antibiotic residues could potentially promote

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D.L. Zhao et al. Water Research 251 (2024) 121111

Fig. 8. (a) Potential discharge amounts of microplastics in the primary, secondary, and tertiary treatments of a WWTP; (b) Number of microplastic particles of
different shapes per liter in the effluent of each treatment step; Reprinted with permission from Ziajahromi et al. (2017). Copyright 2017 Elsevier; (c) Schematic
illustration of microplastic removal by holey Ti3C2Tx nanosheet-based membranes; Reprinted with permission from Yang et al. (2022). Copyright 2022 Elsevier.

the horizontal gene transfer because the antibiotic stress on the bacterial 5.2. Micro/nano plastics
community in the MBR system could increase the resistant proportion of
the bacterial community through environmental selection in wastewater Micro/nano plastics refer to fragments of plastics smaller than 5 mm.
treatment processes. Furthermore, the distribution of ARGs in mem­ Production of plastics has risen over 20 fold over the last half century
brane foulants accounted for 13 %− 25 % of the total absolute abun­ (Kahane-Rapport et al., 2022). Their widespread applications and
dance of all tested samples in the MBR process under the antibiotic improper disposal have contributed to the ubiquitous existence of
stress. Interestingly, both the contents and components of the soluble microplastics debris in diverse aquatic systems (e.g. wastewater, marine
microbial product (SMP) and extracellular polymeric substance (EPS) in water, and freshwater) (Yang et al., 2023; Ziajahromi et al., 2017;
membrane foulants were well correlated with the ARG abundance in Malankowska et al., 2021; Mukherjee et al., 2022). More seriously, as
foulants. Specifically, protein and polysaccharide in both EPS and SMP plastic materials are difficult to break down naturally, these micro­
showed more significant correlations with ARG absolute abundance plastics tend to accumulate in the environment overtime, posing po­
than with that of humic acid. These solid evidences strongly suggested tential dangers to the health of human beings and ecosystems
that membrane foulants indeed played an important role in ARG (Kahane-Rapport et al., 2022; Murphy et al., 2016; de Souza Machado
removals. et al., 2019; Novotna et al., 2019).
Photocatalytic UF membranes consisting of TiO2 nanoparticle were Yang et al. (2023) studied the distribution of microplastics in
also developed for the removal of ARB and ARGs from wastewater ef­ different water sources (i.e., seawater, municipal wastewater, pharma­
fluents, (Ren et al., 2018) which exhibited complete retention of ARB ceutical factory wastewater and drinking water) in France and their fate
and effectively facilitated the photocatalytic degradation of ARGs and in treatment plants. It was found that the concentration of microplastics
integrons. Specifically, the total removal efficiency of ARGs, including was the highest in wastewater (4203–42,000 microplastics/L), followed
plasmid-mediated chloramphenicol resistance gene (floR) and sulfon­ by surface water/ground water (153–19,836 microplastics/L) and
amides resistance genes (sul1 and sul2) could reach approximately 98 % seawater (420 microplastics/L). In addition, polyethylene was the most
after exposing the TiO2-modified PVDF membrane under UV irradiation. common material of microplastics in all water sources, followed by
It was observed that the photocatalytic degradation of ARGs located in polypropylene (PP), polystyrene, and polyethylene terephthalate. The
the genome was more efficient than those located in plasmids. More­ study by Krishnan et al. (2023) revealed that the removal efficiency of
over, the TiO2 photocatalytic reaction demonstrated excellent removal microplastics in WWTPs was 65 % after the primary treatment, and it
of integrons (i.e., intI1, intI2, and intI3) after UV treatment. This finding decreased to 0.2–14 % and 0.2–2 % after the secondary and tertiary
suggested that the potential of horizontal transfer of ARGs could be treatments, respectively. This highlights the need for significant im­
effectively controlled by the TiO2 photocatalytic process. provements in WWTPs to enhance the containment of microplastics.
However, only a few advancements have been reported regarding pri­
mary and secondary treatments, while most advancements have been

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D.L. Zhao et al. Water Research 251 (2024) 121111

focused on advanced treatment methods, including membrane tech­ the membranes (Pellegrin et al., 2015). This variation in pore size would
nologies. Membrane processes hold great promise as an effective strat­ decrease the mechanical strength of membrane’s, which may ultimately
egy for removing microplastics from aquatic systems due to their result in breaches or even degradation of the membranes to release a
multiple advantages, such as ease of management, scalability, and great amount of microplastics.
operational efficiency.
So far, membranes ranging from MF to RO as well as MBR have been 6. Future works and outlook
applied for removing micro/nano plastics (Mukherjee et al., 2022). In
addition to the assessment of microplastics in different water sources in In this review, a state-of-the-art review on membrane-based sepa­
France and their fate in their treatment plants, Yang et al. (2023) also ration and degradation for EPs is provided to facilitate knowledge
studied the feasibility of using UF for the removal of microplastics. UF sharing and technology transfer. Numerous recent studies have high­
membranes with MWCO of 200 kDa retained 70–100 % of microplastics lighted the presence of aggressive EPs in aqueous systems, resulting in
in quantity in both lab- and field-scale experiments. Ziajahromi et al. potential adverse effects on human health, hygiene, and ecology.
(2017) investigated the effectiveness of RO membranes to remove Membrane-based technology, as one of the advanced water treatment
microplastics as part of the tertiary treatment in WWTPs (Fig. 8a). technologies, shows immense potential to remove a wide range of EPs
Although RO membranes should eliminate all particles present in the which are not sufficiently achieved by natural attenuation and con­
feed due to their very dense polymeric barrier, a few plastic particles ventional treatment methodologies. Especially, the integration of
(~0.21 microplastics/L) were unexpectedly detected in the permeate advanced oxidation processes with membranes presents an exciting
stream (Fig. 8b). The authors attributed this to the presence of pores on opportunity for synergistic removal and degradation of recalcitrant EPs.
the membrane surface, other imperfections, or simply small gaps be­ However, improvements and future research must be conducted to
tween pipework. Despite these inevitable imperfections inherent in any further enhance the efficiency and applicability of these technologies.
process, RO remains the most efficient membrane type for removing First, continuous studies on the monitoring and identification of EPs
microplastics from water. are essential to address environmental challenges effectively. Future
Besides employing commercially available membranes for the research should prioritize the development of advanced analytical
removal of microplastics, researchers also explored novel membranes techniques and sensors for early detection and tracking of EPs. Addi­
for this purpose. Yang et al. (2022a) prepared 2D holey Ti3C2Tx tionally, EPs can transform into various by-products during biological,
nanosheet-based membranes by vacuum-assisted filtration (Fig. 8c). The environmental, or treatment processes. These TPs sometimes pose
membranes had an average pore size of 25 nm. They not only showed greater risks than the parent compounds due to their increased toxicity,
effectiveness to capture and remove 99.3 % of polystyrene microspheres persistence, or mobility. Assessing the health and environmental im­
with a size range of 80–1000 nm from wastewater but also displayed a pacts of EPs and their TPs is of paramount importance, necessitating
water flux as high as 1.97 × 104 LMH/bar. The performance of MBR for studies on their toxicological effects on humans, wildlife, and their long-
the removal of microplastics was also evaluated against other waste­ term ecological consequences.
water treatment technologies including disc-filter, rapid sand filtration, To optimize membrane performance for specific EPs, further explo­
and dissolved air flotation (Talvitie et al., 2017). The MBR system ration of membrane material and fabrication should be undertaken to
consisted of a submerged membrane unit (membrane area: 8 m2, pore tailor the membrane morphology and pore structure. Breakthroughs in
size: 0.4 µm) in a UF process. Comparing to other advanced treatment membrane materials, surface engineering, and functionalization can
processes, the MBR system showed a significant higher microplastic lead to highly efficient separation and degradation capabilities. For
removal rate of 99.0 % and a higher quality of the final effluent, indi­ instance, incorporating antifouling functionalities in membranes is
cating its potential to reduce the number of process stages by replacing crucial for their effectiveness to remove eARGs. The adsorption of eARGs
the conventional secondary clarifiers (i.e., conventional activated on membrane surface may facilitate the formation of biofouling as they
sludge). However, their study only considered plastics particles with are crucial to the stability and viability of biofilms. Thus, one must
sizes above 20 µm which might be out of the size range of microplastics. develop membranes accompanied with antifouling functionalities for
Lares et al. (2018) also compared the performance to remove micro/­ the treatment of eARGs.
nano plastics between a conventional activated sludge process and a More importantly, future works should emphasize the implementa­
pilot-scale MBR in a WWTP. During the 3-month test, the researchers tion of membrane technologies in real-world settings. For example, the
observed that the MBR process exhibited a slightly better removal effi­ chemical multiformity and structural designability of microporous
ciency than the overall conventional activated sludge process (i.e., framework membranes have made them promise to become the most
99.4% vs. 98.3 %). Moreover, they discovered that microplastic fibers popular next-generation membranes in environment related fields, and
accounted for 82 % of the microplastic contamination, indicating that great advances have been achieved so far. However, most of them have
they pose a more significant concern than microplastic particles, not been commercialized for industrial applications due to the diffi­
Therefore, future research should also include the occurrence and fate of culties of fabricating them with features of defect-free, large scale, and
microplastic fibers. cost-effective. Conducting pilot studies and scale-up experiments will
Although membrane filtration systems are designed to intercept help assess the feasibility, cost-effectiveness, and environmental impact
microplastics, it is also possible for them to release or produce micro­ of these technologies. In addition, most studies have performed exper­
plastics from the polymeric materials of membranes. It is worth noting iments using synthetic wastewater containing a single pollutant. More
that microplastics have been detected in the effluents of some drinking research is needed using real wastewater or other real case scenarios to
water treatment plants while none of them were present in the influents address the problem for better commercial exploration. The influence of
(Novotna et al., 2019). The most used membrane materials for water coexisting ions and pollutants in actual wastewater on EP removal,
treatment are polyethersulfone (PES), polyvinylchloride (PVC), PP, and membrane fouling, and stability must be studied and understood.
PVDF. It is important to note that microplastic particles made of PES, There will be an upsurge trend on membrane research for simulta­
PVC, and PP have been commonly identified in drinking water treat­ neous filtration and degradation of EPs. However, there are many issues
ment plants (Sun et al., 2019). Physical cleaning, chemical agents, me­ to concern before these membranes can be really deployed for practical
chanical stress, aging, and wear of membranes affect the likelihood of use. For photocatalytic membranes, the high energy consumption from
their breach during prolonged usage (Ding et al., 2021). Research artificial light sources raises concerns. Exploring the use of natural
indicated that when being subjected to 350 ppm NaClO at pH 8 for 144 sunlight to drive photocatalytic reactions holds promise as a sustainable
h, the water permeability of PES membranes was roughly double approach. Additionally, the long-term stability of photocatalytic mem­
compared to the original state, resulting from the increase in pore size of branes under illumination and the presence of reactive oxygen species

13
D.L. Zhao et al. Water Research 251 (2024) 121111

Fig. 9. Trend of research focus on membrane-based treatment of EPs.

(ROS) requires thorough investigations. For biocatalytic membranes, of selectivity, durability, or efficiency, the long-term benefits could
the protection of enzyme activity and stability during membrane fabri­ outweigh the initial costs. Membranes with enhanced fouling resistance
cation and continuous operation is the most challenging task. Effective and durability may have higher manufacturing costs but could result in
strategies for enzyme immobilization need to be developed to ensure lower operational and maintenance costs over the membrane’s lifespan.
long-term stability and sustainable enzymatic activity. The cost of en­ Market dynamics, including demand and competition, also exert an in­
zymes also remains a significant obstacle for scaling up biocatalytic fluence on manufacturing costs. With the increasing prevalence of
membranes. Novel approaches to reduce enzyme costs or identification membrane technologies and rising demand for EP treatment, economies
of alternative enzyme sources should be explored to enable practical of large-scale processes may contribute to cost reductions. Ongoing in­
implementation. novations and advancements in membrane technologies hold the po­
In addition, while integration of membrane separation with photo­ tential to refine manufacturing processes, optimize costs, and improve
catalytic, electrocatalytic or biocatalytic processes are effective in the overall economic feasibility of these technologies.
degrading EPs during separating, the formation of TPs is inevitable and In conclusion, this review has highlighted the promise of membranes
may raise environmental and health concerns. However, the current for the removal and degradation of EPs. We speculate that the research
studies in this area usually tried to ignore this issue and only evaluated on this topic has originated from and is likely to continue along the
the effectiveness of membranes in treating their parent pollutants. In the trajectory illustrated in Fig. 9. Moving forward, it will be imperative to
future, addressing this challenge requires a combination of advanced engage in coordinated efforts and cross-disciplinary partnerships to
analytical techniques, toxicological research, process optimization, and pioneer novel membrane materials, optimize or develop new processes,
regulatory measures to ensure that water treatment technologies are and refine practicality and sustainability for applications in real-world
both effective and safe. scenarios. Through such collaborative endeavors, we will progres­
Some membrane materials or their cleaning processes, as mentioned sively advance toward securing cleaner water resources and protecting
above, may lead to secondary contamination (i.e., micro/nano plastics) the environment against the complexities posed by EPs.
in the treated water. Although their toxicity to the human body and
environment needs further study, this concern should not be ignored Declaration of competing interest
because effluents from the membrane filtration processes usually
directly enter the water distribution systems. To meet this challenge, it is The authors declare that they have no known competing financial
first necessary to have in-depth research on toxicity of micro/nano interests or personal relationships that could have appeared to influence
plastics of various types and sizes to human health and environment as a the work reported in this paper.
reference to establish their concentration limits in drinking water pro­
duction and wastewater treatment. Meanwhile, the potential release of Data availability
these macro/nano plastics from membrane filtration systems must be
thoroughly examined under different operating conditions, including No data was used for the research described in the article.
the underlying mechanisms. The life cycle of the membranes should be
evaluated with this factor in mind. Furthermore, preventive actions to
minimize membrane degradation and follow-up treatment options to Acknowledgments
capture the released microplastics must be explored.
Last but not the least, the perceived manufacturing costs associated This work research was supported by National Natural Science
with treatment of EPs by membrane-based technologies are multifac­ Foundation of China (Grant No. 52300112), Zhejiang Provincial Natural
eted. They depend on the type, materials used, manufacturing processes, Science Foundation of China under Grant No. LQ23E080008, Key Pro­
scalability, and the specific characteristics and performance re­ jects of Jinhua Science and Technology Bureau (Grant No. 2023-3-078)
quirements of the membranes. The complexity of the membrane struc­ and Key Research and Development Projects of Zhejiang Province
ture and the materials significantly influence the overall cost. For (Grant No. 2023C03147). Prof. Chung also likes to thank the Yushan
example, the use of innovative materials (e.g. GO, COFs, MOFs and Scholar Program supported by the Ministry of Education, Taiwan.
HOFs) or advanced fabrication processes (like electrospinning and 3D
printing) may initially have higher manufacturing costs. However, if
these materials or processes provide significant improvements in terms

14
D.L. Zhao et al. Water Research 251 (2024) 121111

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