Applied Materials Today 39 (2024) 102331

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Applied Materials Today

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Passive daytime radiative cooling polymeric materials: Structure design,

fabrication, and applications
Ling Liu a, b , Jin Wang a, b, * , Qingwen Li a, b, *
a
Key Laboratory of Multifunctional Nanomaterials and Smart Systems, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, 215123,
PR China
b
School of Nano-Tech and Nano-Bionics, University of Science and Technology of China, Hefei, 230026, PR China

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

Keywords: Radiative cooling (RC) technology achieves passive cooling without consuming additional energy by reflecting
Passive radiative cooling sunlight and dissipating heat through the atmospheric transparent window via infrared radiation into the cold
Polymer radiative cooler outer space. It presents an excellent alternative to address the current challenges of energy shortage and envi­
Cooling principle
ronmental stress. While numerous materials and structures demonstrate robust RC performance, polymers, with
Preparation strategy
Application scenario
their inherent and strong infrared radiation characteristics, exhibit significant potential and possibilities in RC
due to their diverse structures with designable chemical bonds and groups, large-scale production capabilities,
and ease of manufacturing into RC devices. This review aims to provide a comprehensive summary of recent
advances in utilizing polymers for passive daytime radiative cooling. It will explore the relationship between
polymer structure and RC performance, discuss design principles for achieving high RC efficiency, examine the
production of polymeric materials for coolers, and systematically review and discuss the broad application
scenarios of RC polymers. Finally, this review will highlight future perspectives for the development of RC
polymers.

1. Introduction progress in this field.

In comparison to conventional heating, ventilation, and air condi­
In recent years, the consumption of fossil energy has been accom­ tioning systems (HVAC), PDRC technology offers several advantages,
panied by the emission of greenhouse gases, leading to the degradation including zero energy consumption, portability, easy integration with
of the Earth’s climate. This has prompted growing concerns regarding other technologies, and promising applications in the fields of con­
environmental challenges, including energy scarcity, global warming, struction, transportation, and personal thermal management (PTM)
depletion of the ozone layer, and air pollution [1–3]. Consequently, [13–18]. For instance, in the context of buildings, cooling demands
there is an increased interest in exploring renewable energy sources as alone account for approximately 20 % of total energy consumption [19,
alternatives to fossil fuels, as well as the development of cooling solu­ 20]. Moreover, the utilization of fossil fuels leads to the release of
tions that do not require additional energy consumption [4–7]. The greenhouse gases, such as carbon dioxide, contributing to a gradual rise
concept of passive daytime radiative cooling (PDRC) technology was in global temperatures. Consequently, extreme weather events often
initially proposed by Arago in 1828 [8]. This technology involves the result in numerous casualties and unnecessary property damage. It is
spontaneous reflection of sunlight and the radiative dissipation of excess anticipated that the demand for space cooling and heating will triple by
heat into the frigid outer space (3 K), resulting in lower surface tem­ 2050 [21].
peratures of radiative coolers than the ambient temperature under direct In 2014, Raman et al. pioneered the design of a multilayer photonic
sunlight. Importantly, PDRC technology operates without the need for structure that achieved PDRC [22]. This breakthrough sparked a surge
any additional energy input [8–11]. In the 1880s, the feasibility of of interest in radiative cooling technology, leading to extensive research
radiative cooling at night was experimentally verified [12]. However, in subsequent years. Many studies have focused on the development of
due to the intense solar radiation during the daytime, research on day­ multilayer photonic structures [23–27]. However, these designs often
time radiative cooling has faced significant challenges, impeding required intricate processing techniques and the incorporation of a

* Corresponding authors.
E-mail addresses: [email protected] (J. Wang), [email protected] (Q. Li).

https://doi.org/10.1016/j.apmt.2024.102331
Received 24 March 2024; Received in revised form 9 June 2024; Accepted 8 July 2024
Available online 13 July 2024
2352-9407/© 2024 Elsevier Ltd. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
L. Liu et al. Applied Materials Today 39 (2024) 102331

metal layer at the bottom to reflect sunlight. Consequently, adapting to achieve cooling in direct sunlight. This phenomenon occurs because
these structures to complex surfaces becomes challenging, while the Pa and Pnr are uncontrollable factors unrelated to the material’s intrinsic
preparation cost significantly escalates. To overcome these limitations, properties. Previous studies primarily focused on achieving high solar
researchers have explored the use of various materials for radiative reflectivity (Rsolar) and high long-wave infrared (LWIR) emissivity
cooling, with a particular emphasis on inorganic non-metallic materials (εLWIR) through intricate structural designs. However, it has been
and polymers. Among these materials, polymer-based PDRCs have discovered that various surfaces can achieve temperatures lower than
emerged as promising candidates for fabricating radiative coolers. They the ambient temperature under direct sunlight with the appropriate
offer advantages such as versatility, design flexibility, low preparation structural design. The subsequent analysis will delve into the surface
cost, and the potential for large-scale production. properties that exhibit radiative cooling characteristics.
Over the past decade, several review papers have been published on
the subject of radiative cooling [28–38]. These comprehensive reviews 2.1. High solar reflectivity and high infrared emissivity radiative cooling
have covered a range of topics, including the fundamental principles of
radiative cooling [29,30,32–34,36,38], the structure, classes, and In a typical clear outdoor environment, the sky-facing cooling
properties of photonic materials [31,37], the historical development of structure is exposed to short-wavelength solar radiation. After under­
passive radiative cooling [34], methods for evaluating the efficacy of going absorption, reflection, and scattering by the atmosphere, only a
radiative coolers, and the potential applications of radiative cooling [28, minuscule fraction of the solar radiation energy, approximately 2 bil­
29,32,35,38]. However, there is a relative scarcity of literature lionths of the total energy radiated, reaches the Earth’s surface. Never­
exploring the correlation between the cooling principle and the struc­ theless, this still amounts to around 1000 W m-2 [47]. If a radiative
ture, preparation methods, and challenges associated with cooler absorbs 5–10 % of the solar energy, the absorbed solar power
polymer-based radiative coolers. This review aims to bridge this gap in would fall within the range of 50–100 W m-2, which is comparable to the
the existing literature. Hence, Section 2 provides a comprehensive radiative cooling power of most current radiative coolers [48]. Conse­
overview of the principles of radiative cooling, accompanied by a brief quently, when designing radiative coolers, achieving high reflectivity in
discussion of the surface properties of radiative cooling materials. Sec­ the solar band becomes crucial, as illustrated in Fig. 1a. Furthermore, it
tion 3 summarizes the development timeline of polymer-based radiative is well-established that the diverse colors exhibited by objects result
coolers and their design principles. Section 4 outlines the preparation from their selective absorption of visible light at different wavelengths
methods employed by polymer-based radiative coolers and highlights [49]. Notably, the energy distribution in the visible light range
the technical challenges associated with their practical implementation. (390–780 nm) accounts for approximately 42 % of the total solar radi­
Section 5 examines various applications of radiative cooling and iden­ ation energy (AM 1.5), making it a significant portion of the entire solar
tifies potential future applications. Section 6 concludes this review by spectral range [50]. To achieve cooling in direct sunlight, the prepared
emphasizing the practical application potential of polymer-based radi­ radiative cooler is typically designed to appear white.
ative coolers. The specific contributions of this review include (1) To achieve optimal work efficiency, in addition to sunlight reflec­
summarizing and categorizing polymer-based radiative coolers reported tion, another crucial parameter of radiative coolers is IR emissivity.
in the literature based on their properties, and (2) analyzing the current Depending on the surface properties of radiative cooling materials, they
preparation methods for polymer-based radiative coolers. Finally, based can be categorized as either ideal broadband or selective [26]. The
on the literature review, conclusions and future research directions are emissivity of an ideal broadband radiative cooler surface in the 3–25 μm
proposed. wavelength range is 1, whereas the emissivity of an ideal selective
radiative cooler surface is 1 in the ATW wavelength range and 0 in other
2. The mechanism and types of passive radiative cooling ranges. Broadband materials can attain a greater net cooling power,
while selective materials can achieve a larger temperature differential
In general, objects on the Earth’s surface receive radiation from at­ between the radiative cooler surface and the surrounding environment.
mospheric components, solar radiation, and heat convection and con­ Calculations reveal that when the temperature of the radiative cooler is
duction from the surrounding environment. Simultaneously, any object lower than the ambient temperature and non-radiative influences are
with a temperature above absolute zero continuously exchanges energy eliminated, broadband radiative coolers can achieve a temperature
with the external environment through thermal radiation. During clear difference of 17 ◦ C, while ideal selective IR emitters can achieve a
weather conditions, the atmosphere exhibits a low radiation absorption temperature difference of 43 ◦ C [34]. However, in certain applications,
rate of radiation within the wavelength range of 8–13 μm, known as the radiative coolers can indeed lower the surface temperature of an object
atmospheric transparent window (ATW), which is a key pathway for but it is challenging to bring the temperature below ambient levels.
PDRC [39–41]. Typically, the relationship between the absorption (α), When the surface temperature of an object is relatively high,
reflectivity (β), and transmittance (τ) of electromagnetic waves is α +β + non-radiative heat transfer becomes dominant. For instance, when the
τ = 1 [42,43]. Furthermore, Kirchhoff’s law states that, under specific surface temperature of a radiative cooler exceeds the ambient temper­
conditions, the absorption and emissivity (ε) of an object at the same ature by 20 ◦ C, the cooling power of a broadband infrared emitter is
wavelength are equal. In the context of a radiative cooling device, the approximately 490 W m-2, whereas that of an ideal selective radiative
cooling capacity can be evaluated in terms of the net cooling power (Pc). cooler is 405 W m-2 [51]. Therefore, the design of radiative coolers can
The net radiative cooling power generated by a radiative cooler under be tailored according to the operational temperature of the equipment.
thermal equilibrium conditions is given by the Equation [44–46]:
2.2. High solar reflectivity and high infrared transparent radiative cooling
Pc = Pr − Ps − Pa − Pnr
Pr denotes the power radiated by the radiative cooler into outer space Radiative heat loss accounts for a significant proportion of the heat
through the atmospheric window, Ps represents the power radiated by dissipation from thermal radiators. For instance, the heat lost through
the sun, Pa is the power emitted by the atmosphere, and Pnr accounts for thermal radiation from the human body constitutes approximately 60 %
the exchange of other non-radiative energy. Therefore, the underlying of the total heat loss [52,53]. The human body serves as a typical heat
principle of PDRC operation is that the material’s surface does not radiator, exhibiting an emissivity of up to 0.98, and its thermal radiation
absorb sunlight (wavelength of 0.3–2.5 μm) while simultaneously spectrum ranges from 7 to 14 μm [54], which coincides with the ATW.
emitting heat through the ATW to the cold outer space, resulting in Therefore, for materials with high LWIR transparent (TLWIR), achieving a
spontaneous cooling. In summary, the mechanism of the radiative cooling effect under sunlight can be fulfilled by reflecting solar radiation
coolers is to minimize sunlight absorption and maximize heat radiation while simultaneously allowing the passage of thermal radiation emitted

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 1. Types of radiative coolers. Schematic heat transfer process of the radiative cooling emitter of (a) high Rsolar and high εLWIR. (b) high Rsolar and high TLWIR. (c)
high Tsolar and high εLWIR. The blue and orange boxes are the radiative-cooled emitter and the cooled substrate, respectively.

by the body, as depicted in Fig. 1b. Fabric was found to require a min­ Rayleigh scattering while maintaining visible opacity through strong
imum TLWIR of 0.644 and a maximum LWIR reflectance (RLWIR) of 0.2 to Michaelis scattering. The design of IR-transparent visible-opaque fabrics
ensure thermal comfort at ambient temperatures up to 26.1 ◦ C [55]. (ITVOF) was developed using synthetic polymer fibers with inherently
These fibers are then structured to minimize RLWIR through weak low IR absorption. Initially proposed for indoor environments, it was

Fig. 2. Roadmap of polymer for passive radiative cooling. NanoPE Film [63]. Copyright 2016, The American Association for the Advancement of Science. Nylon-6
Fiber [64]. Copyright 2017, The authors. Polymethylpentene (TPX) Film [65]. Copyright 2017, The American Association for the Advancement of Science. Poly­
tetrafluoroethylene (PTFE) Film [66]. Copyright 2018, Elsevier. P(VdF-HFP) Film [67]. Copyright 2018, The American Association for the Advancement of Science.
Cooling Wood [68]. Copyright 2019, The American Association for the Advancement of Science. PDMS Film [69]. Copyright 2019, Springer Nature. Poly(vinylidene
fluoride) (PVDF) Film [70]. Copyright 2020, The authors. Polyvinyl fluoride (PVF) Film [71]. Copyright 2020, Elsevier. Polyacrylonitrile (PAN) Film [72]. Copyright
2020, The authors. Polyethylene oxide (PEO) Film [73]. Copyright 2020, Springer Nature. Polymethyl methacrylate (PMMA) Film [74]. Copyright 2021, The authors.
Polystyrene (PS) Film [75]. Copyright 2021, John Wiley and Sons. Polylactic acid (PLA) Textile [76]. Copyright 2021, The American Association for the
Advancement of Science. Polypropylene (PP) Film [77]. Copyright 2021, The authors. Silk Textile [78]. Copyright 2021, Springer Nature. Polyethylene glycol
terephthalate (PET) Film [79]. Copyright 2022, Elsevier. TPU Coating [80]. Copyright 2022, John Wiley and Sons. Poly(vinyl alcohol) (PVA) Film [81]. Copyright
2022, Springer Nature. Polyethersulfone (PES) Textile [82]. Copyright 2023, John Wiley and Sons. Chitin Film [83]. Copyright 2023, The authors.
Styrene-ethylene-butylene-styrene (SEBS) Textile [84]. Copyright 2023, John Wiley and Sons. Polyoxymethylene (POM) Textile [85]. Copyright 2023,
Springer Nature.

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L. Liu et al. Applied Materials Today 39 (2024) 102331

later discovered that this structural design could reflect most of the be created into different forms, such as films, textiles, and coatings, to
direct sunlight while allowing the passage of thermal radiation emitted address various usage scenarios. For instance, nanoPE [63] developed
by the human body, enabling outdoor cooling. By embedding ZnO by Cui et al. can be fabricated into different forms, such as fibers, films,
nanoparticles in nanoporous polyethylene (nanoPE), Cui et al. devel­ and textiles, to meet various human wear requirements. Poly­
oped a novel spectrally nanocomposite textile that reflects 0.9 of solar dimethylsiloxane (PDMS) [69], polyvinylidene fluoride-co-hexafluor
irradiance and exhibits up to 0.8 transmittance in the range of 7–14 μm opropyleneP(VdF-HFP) [67], thermoplastic polyurethane (TPU) [80],
[56]. In actual outdoor tests, it has been shown to be 5–13 ◦ C cooler than and other materials can be formulated as paints for coating on diverse
ordinary textiles, demonstrating its energy-efficient outdoor thermal irregular surfaces. Moreover, biopolymers like silk and chitosan can also
management performance. be radiative cooling materials through structural design [78,83].
Modifying polymers through various approaches offers possibilities for
their application in various domains, including material innovation,
2.3. High solar transparent and high infrared emissivity radiative cooling
novel structural design, and advanced nanotechnology.
IR radiation represents the most extensive form of electromagnetic
Previous studies on PDRC structure design have primarily focused on
radiation arising from the irregular movement of molecules and atoms
the two aforementioned structures. However, it is worth noting that any
within objects in the conventional environment. This movement results
surface that does not absorb solar radiation will not experience solar
in the continuous emission of thermal IR energy, with radiation energy
heating. Selective absorption of solar radiation, similar to selective
directly proportional to the intensity of molecular and atomic motion
emission, finds practical applications in numerous fields despite the
[86]. The primary cause of IR radiation in polymers is the vibration of
potential for parasitic heat damage to the equipment [57–59]. As
functional groups, which can be broadly categorized as telescopic vi­
depicted in Fig. 1c, the transparent PDRC surface exhibits a high solar
bration and bending vibration. Fig. 3 illustrates the division of the IR
transmittance (Tsolar) and minimal absorption of solar energy. Simulta­
spectrum into two regions. In the range of 1300–4000 cm-1, there is a
neously, the top surface of the cooler demonstrates significantly high
relatively clear correspondence between the functional group and fre­
εLWIR, facilitating the outward radiation of heat through the ATW.
quency in polymers, allowing for the determination of substance type.
Consequently, when exposed to direct sunlight, the PDRC surface
This region is commonly referred to as the functional group area. In the
effectively reduces the operating temperature of the equipment while
range of 400–1300 cm-1, there are certain bands with irregular charac­
achieving selective solar transmission.
teristics that can still be used to distinguish congeners or compounds
Based on the above discussion, the cooling effect under direct sun­
with similar structures. This region is known as the fingerprint region.
light is not only related to the chemical composition of the radiative
Since IR radiation covers the entire ATW, it serves as a reference for
cooler but also to its micro-structure, and the effects of both on the
selecting radiative cooling polymers [87]. Notably, the bending vibra­
performance of the radiant cooler are discussed in detail below.
tions of chemical bonds such as C–O, C-F, C–Cl, and Si-O fall precisely
within this range, and polymers containing these bonds have been
3. Polymers for PDRC shown to be useful in the preparation of radiative coolers [88–92].
Based on the emissivity of functional groups of polymers, they can be
With the development of advanced design and manufacturing tech­ classified into three groups as illustrated in Fig. 4: high infrared emis­
nology, multilayer photonic structures have emerged as effective sivity polymers (e.g. P(VdF-HFP) [67], PVDF [70], PEO [73], PVF [71],
choices for current radiative coolers. These structures consist of alter­ PDMS [69], and PTFE [66]), medium infrared emissivity polymers (e.g.
nating layers of materials with different dielectric constants [60–62]. TPU [83], PS [75], cellulose [68], PVA [81], PET [79], PMMA [74], and
However, the complex manufacturing process limits their large-scale PLA [76]), and infrared transparency polymers (e.g. PE [63], PP [77],
use. Recent studies have shown that polymers can be structurally PAN [72], TPX [65], and PA6 [64]). This classification is based on the
designed to possess comparable optical properties to those of multilayer quantity and intensity of chemical bonds within the polymer. According
photonic structures. Fig. 2 depicts the development of polymer-based to the classification, PE (high LWIR transparent), PVDF (high LWIR
radiative coolers in recent years [63–85]. Furthermore, polymers can

Fig. 3. Functional group IR absorption peak and its corresponding wavelength.

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 4. Polymer structures and their emissivities that potentially for PDRC.

Fig. 5. (a) Schematics of comparison between nanoPE, normal PE, and cotton. (b) Simulated total and specular transmittance of infrared and visible light for nanoPE.
(c) Photo of commercial nanoPE [63]. Copyright 2016, The American Association for the Advancement of Science. (d) Image of a PEA sample (the inset shows an
SEM image). (e) Hemispherical transmittance and reflectance of a PEA sample [95]. Copyright 2019, The authors.

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L. Liu et al. Applied Materials Today 39 (2024) 102331

emissivity), cellulose (medium LWIR emissivity), and PDMS (chemical with a layer of PE film. Nonetheless, the thermal insulation performance
stability) will be selected as representative polymers for detailed dis­ of this approach remains suboptimal. Hence, Leroy et al. devised PE
cussion. Importantly, the emissivity of polymers can be increased aerogel (PEA) as a protective cover for existing radiative coolers [95].
through surface design in polymer-based radiative coolers. For instance, Fig. 5d illustrates an optical photo and SEM image of PEA, showcasing
surfaces with porous structures demonstrate higher emissivity compared its highly porous structure. This unique structure contributes to its low
to smooth surfaces. This is primarily attributed to the greater number of thermal conductivity (28 mW mK-1) and ability to scatter sunlight. The
polymer-air interfaces in porous structures, which enhances the poten­ optical properties of PEA were characterized in Fig. 5e, revealing its high
tial for infrared absorption through multiple diffuse reflections [93]. sunlight reflectivity (92.2 %) and infrared transparency (79.9 %).
Simulation results indicate that without PEA, a typical radiant cooler
3.1. Polyethylene would struggle to maintain a surface temperature lower than the
ambient temperature due to sunlight absorption and parasitic heat.
Given that the PE segments exclusively consist of C–C and C–H However, by applying PEA as a cover, the cooling effects can be ach­
bonds, PE demonstrates transparency in the mid-infrared spectra. It is ieved day and night, with a significant increase in cooling capacity.
worth noting that the thermal wavelength range of the human body’s Subsequent experiments confirmed these findings, with temperature
outward radiation falls within the 7–14 μm range, which overlaps with differences between the typical radiative cooler and the environment
the atmospheric transparency window ranging from 8 to 13 μm. As a without PEA coverage measuring 1.7 and 8.4 ◦ C, respectively. In
result, PE can be effectively incorporated into clothing to facilitate contrast, the temperature differences for the cooler with PEA coverage
thermal dissipation from the human body, thereby enabling passive were 13 and 18.3 ◦ C, respectively. This work greatly enhances the
cooling in the surrounding environment. However, a limitation of PE as cooling potential of existing radiative coolers [95]. Furthermore, Table 1
a textile material is its transparency in the visible light range. To address provides an overview of other PE-based radiative cooling studies.
this issue, Cui et al. developed a NanoPE film with a nanoporous
structure, as shown in Fig. 5a [63]. NanoPE reveals the presence of pores 3.2. Polyvinylidene fluoride and its derivatives
ranging from 50 to 1000 nm, as well as directional fibrous structures
measuring a few microns wide. These nanopores effectively scatter When compared to other polymers, fluorinated polymers exhibit
sunlight, resulting in visible opacity. Additionally, NanoPE retains its superior UV stability and corrosion resistance, making them highly
infrared transparency, allowing thermal radiation to pass through the versatile in various everyday applications. Additionally, polymers con­
cloth from the human body (Fig. 5b). The material has been engineered taining C-F bonds are commonly utilized in PDRC due to the absorption
to possess breathability, water absorption rate, and mechanical strength peak of C-F bonds falling within the 1250–1000 cm-1 range. For
comparable to ordinary textiles. Experimental results indicate that instance, Meng et al. developed a double-layer structure by applying a
NanoPE achieves lower temperatures than traditional textiles when silver (Ag) lining on the bottom surface of a PVF film, resulting in low
exposed to direct sunlight, indicating its superior cooling performance solar absorption and high infrared emission [71]. PVF possesses a
[63]. NanoPE with excellent cooling properties can be mass-produced refractive index of 1.425 within the 0.3–2.5 μm range and an extinction
(Fig. 5c). coefficient close to zero, indicating its negligible absorption in the solar
In the context of clothing, color represents a paramount attribute. spectral range. Moreover, the presence of multiple extinction peaks in
However, traditional textile dyes tend to strongly absorb light within the the infrared spectral range of PVF indicates its significant emission.
visible spectral range, thereby converting it into heat. Additionally, the Outdoor tests demonstrated a cooling reduction of 2 ◦ C for the
chemical bonds present in commonly used organic dyes exhibit pro­ double-layer structure.
nounced absorption of human thermal radiation, resulting in high Due to its simple preparation, applicability, and economic efficiency,
emissivity of textiles within the LWIR wavelength range. Consequently, the porous structure is commonly employed when polymers are utilized
identifying appropriate dyes that can adjust textile color while mini­ in PDRC. However, conventional preparation methods often require a
mizing visible light absorption holds immense promise for advancing significant number of organic solvents. To address this issue, Huang
the practical application of cooling fabrics. In their research, Cui et al. et al. introduced a "top-down" ball milling method for the fabrication of
selected non-toxic and cost-effective inorganic nanoparticles with sizes P(VdF-HFP) waterborne coatings (Fig. 6a) [101]. During the ball milling
ranging from 20 to 1000 nm, including Prussian blue (blue), iron oxide process, P(VdF-HFP) nanoparticles self-assemble to form secondary
(red), and silicon (yellow). These three colors served as primary colors, particles, resulting in the formation of numerous nanopores and mi­
while various other colors could be achieved by blending them in cropores between the primary and secondary particles, which effectively
different proportions [94]. By incorporating these nanoparticles into the scatter sunlight. As depicted in Fig. 6b, the P(VdF-HFP) waterborne
PE polymer, the resulting material maintained an infrared transmittance coatings exhibit favorable optical characteristics for PDRC, with a solar
of 80 %. Moreover, increasing the nanoparticle content did not
compromise its infrared transmittance properties. Subsequently, the
Table 1
nanoparticles were infused into the PE matrix using the same method,
PE radiative coolers, their optical properties, and cooling performance.
enabling the extrusion of mechanically robust and colored fibers that
Materials Solar IR emissivity (%) Temperature drop Refs.
were woven into RC textiles. Compared to commercial cotton fabrics,
reflectivity (%) (◦ C)a
this radiative cooling textile exhibited a cooling effect of 1.6–1.8 ◦ C,
thereby significantly expanding the potential applications of wearable Nano -PE/ 90 80 6 [56]
ZnO (Transmittance)
radiative coolers. NanoPE can now be mass-produced in all its forms, Nano-PE 90 70 2.3 (cotton) [96]
including films, fibers, fabrics, and colored nanoPE textiles, and this (Transmittance)
progress means that polymer-based radiative cooling materials can be PE/PEO 94 91 6.8 (Simulate [97]
expected to develop in the future. skin)
HDPE/h- 87 71 5 [98]
Theoretically, an ideal selective radiative infrared cooler has the
BN
potential to achieve a cooling effect of 43 ◦ C. However, the actual Nano-PE/ 96 90 6.1 [99]
cooling performance of a daytime radiative cooler is considerably lower SiO2
than this theoretical value due to the absorption of solar radiation and PE/ fabric 95 84 4.9 [100]
non-radiative heat exchange with the surrounding environment. Current (Transmittance)

experiments on daytime radiative cooling attempt to minimize the a

Unless otherwise specified, the temperature difference in the table is the
impact of the surrounding environment by covering the device’s surface temperature difference from the ambient temperature.

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 6. (a) The schematic illustrations, SEM images, and optical images of aqueous processing-based P(VdF-HFP) coatings. (b) The spectral reflectance of a porous P
(VdF-HFP) coating. (c) Rsolar and (d) εLWIR of a porous P(VdF-HFP) coating at different incident angles [101]. Copyright 2021, John Wiley and Sons. (e) Digital image
of FHPCM. (f) The spectral reflectance of FHPCM. (g) Rooftop measurement of the FHPCM films. (h) Temperature difference (ΔT) between the two cars’ front
windscreens or internal air [102]. Copyright 2021, John Wiley and Sons.

reflectivity of 0.94 and LWIR emissivity of 0.97, which remain relatively P(VdF-HFP) film prepared using the conventional phase separation
constant across different incidence angles (Fig. 6c and d). The coating method had a VOC content of approximately 758 g L-1.
demonstrated a cooling effect of 3.3 ◦ C and 1.7 ◦ C compared to com­ Wang et al. [102] devised a spray-phase-separation strategy to
mercial white paint and ambient temperature, respectively. Addition­ fabricate a flexible hierarchically porous complex membrane (FHPCM)
ally, the coating prepared using this method reduced the volatile organic by employing spray and high-speed airflow to regulate the phase evo­
compound (VOC) content to 71 g L-1, whereas the hierarchically porous lution kinetics during evaporation-induced phase separation. The

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method employed has successfully produced a product that is taking molecules within the range of 770–1250 cm-1, involving C–H, C–O,
shape, as shown in Fig. 6e, with the optical properties reaching an and C–O-C chemical bonds, results in strong emission within the ATW.
advanced level. The curve in Fig. 6f demonstrates that the FHPCM ex­ This characteristic suggests that cellulose-based materials hold immense
hibits a solar reflectivity of 0.97 and an LWIR emissivity of 0.94. potential for a wide range of applications in the field of radiative cool­
Furthermore, the FHPCM has demonstrated exceptional performance in ing. For instance, Li et al. produced cooled wood through a process
various practical tests. In roof measurements, the FHPCM achieved a involving complete delignification and densification of wood (Fig. 7a).
remarkable cooling performance of up to 14.9 ◦ C (Fig. 6g). Application This modified wood exhibited a distinct white appearance compared to
of the FHPCM to the car’s surface resulted in a cooling effect of 25.5 ◦ C natural wood [68]. The disordered mesoporous cellulose structure of
for the car’s interior (Fig. 6h). Additionally, when the FHPCM was cooling wood allows it to possess an impressive solar reflectivity of 0.96
applied to the building surfaces, it achieved a cooling effect of up to 30.7 (Fig. 7b) and an LWIR emissivity of 0.9, with negligible angular
◦
C. This study presents a simple and scalable approach for obtaining dependence (Fig. 7c). Moreover, practical outdoor testing confirmed the
PDRC products. remarkable cooling performance of the wood, both during the day and
Furthermore, the commonly used polymer PVDF encompasses four night. Additionally, modeling studies investigating the potential appli­
crystal phases. Among these, the β phase adopts an all-trans ortho­ cations of cooling wood in the construction sector have indicated po­
rhombic crystal system, where the dipoles within the unit cell align in tential energy savings of approximately 20–60 % for cooling buildings.
the same direction, resulting in strong polarity [103]. Consequently, Additionally, the incorporation of nanoparticles, such as silicon
PVDF and its copolymers with a dominant β-phase content exhibit oxide (SiO2), zinc oxide (ZnO), etc., into the precursor during the
exceptional piezoelectric properties. When subjected to an electrostatic preparation process or the surface treatment of cellulose can effectively
field, PVDF can be effectively polarized, leading to the transformation of enhance its solar and infrared emissivity. Tian et al. demonstrated this
the α phase into the β phase. Song et al. successfully prepared a P by applying a layer of PTFE particles with a size distribution of 1.4 ± 0.9
(VdF-HFP) film through electrospinning, demonstrating high solar μm onto the surface of a cellulose fiber membrane, resulting in the
reflectance and infrared absorptivity [104]. Moreover, owing to the formation of a white coating with embedded PTFE microparticles within
piezoelectric characteristics of P(VdF-HFP), the thin film can function as cellulose micropores (Fig. 7d) [118]. The rough surface structure
a sensor for monitoring cooler integrity during usage and as a nano­ created by the PTFE particles imparts superhydrophobic properties to
generator for harvesting energy from the environment, thereby the cellulose composite film, making it highly suitable for outdoor ap­
expanding the potential applications of PDRC. Subsequently, the authors plications and preventing a decrease in sunlight reflectivity due to sur­
redissolved the damaged polymer nanofiber membrane in a solvent for face dust adsorption. This successful modification significantly
recovery and re-electrospun, demonstrating the recyclability of increased the sunlight reflectivity of the cellulose fiber membrane from
polymer-based radiative coolers. Additionally, a considerable amount of 0.89 to 0.93 (Fig. 7e). Additionally, Gamage et al. investigated the
research has been conducted on PVDF-based radiative coolers, as sum­ manipulation of cellulose microstructure to modify its interaction with
marized in Table 2. sunlight [119]. They designed and synthesized cellulose membranes
with different microstructures, including homogeneous structural
3.3. Cellulose and its derivatives membranes and nanofiber structural membranes. Both materials
exhibited high LWIR emissivity (greater than 0.9) and minimal sunlight
Cellulose, as the world’s most abundant natural polymer, represents absorption (less than 0.1), enabling effective radiative cooling during
a remarkable and renewable resource. Through various modifications, the day. Experimental results demonstrated that these cellulose-based
such as methylcellulose, hydroxypropyl methylcellulose, hydroxyethyl membranes reduced the temperature of silicon samples by 15 ◦ C and 5
cellulose, and carboxymethyl cellulose, cellulose exhibits a diverse
◦
C under direct sunlight. Table 3 provides a comprehensive summary of
range of applications. Similarly, the telescopic vibration of cellulose the significant advancements in cellulose-based radiative cooling
research in recent years.

Table 2
PVDF and its derivatives for PDRC.
3.4. Polydimethylsiloxane

Materials Solar IR emissivity (%) Temperature Refs.

Moreover, PDMS, characterized by stable chemical properties and
reflectivity drop (◦ C)a
(%) negligible absorption in the solar spectrum range, is an excellent
candidate for fabricating radiation coolers due to its abundant Si-O-Si
PVDF 97 96 6 [105]
90 50 12 (Simulate [106]
bonds that exhibit significant absorption in the LWIR band. Zhai et al.
(Transmittance) skin) conducted a study where they utilized PDMS as the substrate to prepare
94 94 9 [107] a self-cleaning multilayer radiative cooler [128]. The top layer consisted
PVDF-HFP/ 96 96 7 [108] of PDMS and SiO2 particles, forming a thermal radiation layer, while the
Hydrogel
bottom layer comprised PDMS and an Al film, constituting a reflective
PVDF-HFP/ 90 83 10.8 [109]
fabric sunlight layer. Experimental results demonstrated that this multilayer
PVDF-HFP/ 94 97 10 [110] structure achieved a temperature reduction of up to 2.1 ◦ C during the
SiO2 day and 3.44 ◦ C at night. In their study, Zhang et al. incorporated ZrO2
PVDF-HFP/ 97 94 13.8 [111] as an additive, known for its high refractive index and wide bandgap
PDMS
PVDF-HFP/ 97 94 1.5 [112]
(5.4 eV), into the PDMS matrix [129]. Fig. 8a presents the refractive
BaSO4 index and extinction coefficient of PDMS, indicating a near-zero
PVDF-HFP 92 96 6.3 [113] extinction coefficient in the range of 0–2.5 μm and multiple extinction
PVDF-HFP/ 98 95 11.6 [114] peaks in the range of 8–13 μm. Through simulation, the authors selected
SiO2
ZrO2 with a particle size of 0.5 μm and a volume fraction of 10 % as an
PVDF /SiO2- 9.2 [115]
PTFE additive to achieve a coating thickness of 500 μm. A comparison be­
PVDF/ 96 96 3.8 [116] tween the prepared coating and commercial white paint revealed that
PNIPAm the average reflectance of the PDMS coating was 0.94 in the wavelength
PVDF/ZrO2 98 96 4 [117] range of 300–1350 nm, while the average reflectance of the commercial
a
Unless otherwise specified, the temperature difference in the table is the white paint was only 0.70 (Fig. 8b). Both coatings exhibited similar
temperature difference from the ambient temperature. emissivity in the LWIR wavelength range, indicating excellent thermal

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 7. (a) Photos of cooling wood. (b) Absorption of the natural and cooling wood in the solar spectrum. (c) Infrared emissivity spectra of the cooling wood at
different emission angles [68]. Copyright 2019, The American Association for the Advancement of Science. (d) Optical and SEM photos of PTFE-coated paper
composites. (e) Spectral reflectivity of the original and composite paper [118]. Copyright 2021, The authors.

infrared emission, Zhai et al. incorporated SiO2 microspheres into the

Table 3 TPX matrix and applied a silver film on the reverse side, as illustrated in
Cellulose derived PRC coolers and their cooling performance.
Fig. 9a [65]. By simulating the strong phonon polaron resonance of SiO2
Materials Solar IR emissivity Temperature Refs. microspheres at 9.7 μm, the authors calculated the normalized absor­
reflectivity (%) (%) drop (◦ C)
bance (σabs/a2), scattering (σsca/a2), and extinction (σext/a2)
Cellulose/TiO2 97 98 10 [120] cross-sections of individual SiO2 microspheres encapsulated in TPX. The
Cellulose/SiO2 94 90 6 [121] appropriate microsphere size was selected based on its size parameter
cellulose 96 95 6.2 [122]
acetate /SiO2
κ0a (Fig. 9b). Following the deposition of a 200 nm Ag layer on the
Cellulose/ZnO 81 93 5.6 [123] bottom. The sample exhibited a solar reflectivity of 0.96 and an LWIR
Cellulose/ 96 92 9.2 [124] emissivity of 0.93 (Fig. 9c). Experimental findings have confirmed the
MTMS PDRC performance. In addition to the C–C backbone, only C–H and
Cellulose 92 90 7.5 (nighttime) [125]
C–– N in the PAN polymer segment are considered typical LWIR trans­
–
Cellulose/ZnO 94 84 5 [126]
cellulose 95 94 4.6 [127] parent polymers capable of achieving high sunlight reflectivity through
acetate nanostructure design. Kim et al. employed electrospinning technology to
fabricate PAN nanofiber radiant coolers, which exhibit opacity in the
visible light region and transparency in the infrared region, allowing
radiation properties (Fig. 8c). In field tests, the PDMS coatings demon­ objects to radiate heat into outer space while scattering sunlight [72]. By
strated superior cooling performance compared to commercial white designing the structure of PAN nanofiber membranes, solar reflectivity
paints. exceeding 0.95 and high LWIR transmittance (0.7) can be achieved,
In contrast to the unidirectional cooling PDMS coating, Zhao et al. resulting in temperatures up to 3 ◦ C lower than the ambient temperature
devised a PDMS coating with switchable apertures to enable both in practical tests.
cooling and solar heating [130]. As depicted in Fig. 8d, the coating was Silk has been utilized as a textile since as early as 2700 BC. Its
designed as a bilayer structure comprising a porous PDMS film on top, popularity stems from its exceptional wearing comfort. The inherent
created using water droplets as a template and carbon black particles at self-assembly graded structure of silk grants it favorable reflectivity in
the bottom. The upper porous structure endowed the film with a solar the visible and near-IR ranges, while its inherent absorption in the mid-
reflectance of 0.93 and an LWIR emissivity of 0.94, without any stress IR region makes it an excellent material for radiative cooling. However,
(Fig. 8e). In its transparent state, the film could absorb 0.95 of sunlight its inherent absorption in the ultraviolet region hampers its cooling ef­
for heating purposes. Outdoor experiments demonstrated that the ficiency under direct sunlight. Zhu et al. addressed this issue by modi­
cooling state could achieve a temperature reduction of 5 ◦ C, while the fying the silk surface through molecular bonding design and a scalable
heating state could elevate the temperature from 10 ◦ C to 28 ◦ C. Table 4 coupling agent-assisted dipping method (Fig. 9d) [78]. The nano­
provides a summary of recent achievements in PDMS-based radiative processed silk exhibited an increased reflectivity in the solar spectral
coolers. range, rising from 0.86 to 0.95, thereby offering potential for passive
daytime radiative cooling (Fig. 9e).
3.5. Other polymers Additionally, certain polymers can be effectively utilized for radia­
tive cooling through appropriate structural design. Wang et al. devel­
TPX is a polymer renowned for its remarkable transparency to both oped a hierarchical structure of PMMA films by combining a
solar and infrared spectra. To achieve reflected sunlight and high microporous array with random nanopores [74]. Owing to the inherent

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 8. (a) Refractive index (n) and extinction coefficient (κ) of PDMS. (b) The reflectivity of the ZrO2/PDMS coating and commercial paint. (c) The emissivity of the
ZrO2/PDMS coating sample and commercial paint [129]. Copyright 2021, Elsevier. (d) Schematic of the bilayer structure and its cooling and heating mechanism. (e)
Typical spectral properties of the bilayer structure film in different wavelength ranges [130]. Copyright 2020, The authors.

functionalization, various micro-structures can be developed when

Table 4
using them as radiative coolers. In contrast to multilayer photonic
PDMS and its composite for PRC and their cooling performance.
structures, which usually require intricate structural designs involving
Materials Solar IR emissivity Temperature Refs. the inclusion of reflective metal layers at the bottom to reflect sunlight
reflectivity (%) (%) drop (◦ C)
and exploit material properties and interference effects [145–147],
PDMS 95 97 8 [131] polymer radiative coolers offer a broader range of morphology options,
PDMS 93 95 5.8 [132]
such as multilayer structure with a bottom reflective metal layer [148],
PDMS-NH2/ 92 93 2 [133]
Al2O3 nanoparticle composition structure [122], porous structure [74],
PDMS/ZnO 96 81 7.5 [134] nanofibers structure [73], and dynamic optical structure [149]. The
PDMS 97 96 4 [135] following sections detail polymer-based radiative coolers with different
PDMS/PS 93 94 4.8 [136] structural characteristics.
PDMS/PMMA/ 94 79 7.8 [137]
cotton
4.1. Multilayer structure
electromagnetic properties of PMMA, its extinction coefficient in the
Compared to photonic structures, it is relatively straightforward to
solar spectral range is negligible, and it exhibits multiple extinction
determine the mid-IR emissivity of a polymer with a specific structure.
peaks within the ATW. Furthermore, the substantial refractive index
As depicted in Fig. 3, if the polymer contains a significant number of
difference between PMMA and air enables efficient sunlight scattering.
fingerprint regions, its emissivity will be higher. Generally, the greater
The incorporation of graded holes in the PMMA film results in a solar
the proportion of these regions, the higher the emissivity. For instance, P
reflectivity of 0.95 and an LWIR emissivity of 0.98.
(VdF-HFP) exhibits a higher emissivity than PMMA [150]. To achieve
Shan et al. employed a straightforward phase separation method to
daytime radiative cooling, one can select a polymer with a high LWIR
fabricate a series of self-supporting composite films consisting of silica
emissivity and draw inspiration from the design principles of multilayer
aerogel functionalized TPU (AFTPU), as well as AFTPU-coated nylon
photonic structures. By incorporating a layer of reflective metal at the
fabrics (Fig. 9f) [80]. As depicted in Fig. 9g, the AFTPU films exhibit a
bottom of the polymer to reflect sunlight (Fig. 10a) [148].
remarkable solar reflectivity of up to 0.94 and LWIR emissivity of up to
Based on this design concept, Zhang et al. opted for PDMS with low
0.96. Practical experiments involving the attachment of the finished
solar reflectance and high IR emissivity as the top layer and Ag as the
fabric onto regular fabrics and wearing them on the human body have
bottom layer to construct a dual-layer radiative cooler [148]. Ag is
demonstrated the actual performance of AFTPU as a passive daytime
commonly employed as a reflective metal layer in designing multilayer
radiative cooler. Table 5 provides a summary of recent research on other
photonic structures, owing to its high reflectivity in the solar spectrum.
polymer-based radiative coolers.
This layer plays a crucial role in reflecting sunlight and minimizing the
heating effect caused by solar radiation. Fig. 11a presents an optical
4. Micro-structure design of polymer toward PDRC
image of the sample, revealing a white appearance at the top, where a
mixture of PDMS and SiO2 microspheres is located, and a metallic luster
As mentioned above, in addition to the chemical structure of the
at the bottom, resulting from the silver coating. Additionally, Fig. 11b
polymer itself, the morphology presented is also an essential consider­
and c display SEM photos, which indicate the presence of a cellulose
ation for its radiative cooling performance to achieve PDRC. Due to the
paper layer serving as integral support in addition to the aforementioned
excellent structural tunability of polymers and their ease of
sample. The structure, with Ag as the reflective layer, exhibits a solar

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 9. (a) Schematic of the hybrid metamaterial backed with a thin silver film. (b) Normalized absorption (blue), scattering (red), and extinction (black) cross
sections of individual microspheres as functions of size parameter (k0a). (c) The emissivity/absorptivity of measured and theoretical results [65]. Copyright 2017,
The American Association for the Advancement of Science. (d) Schematic of the net cooling performance of nanoprocessed silk. (e) The reflectivity spectrum of
nanoprocessed silk [78]. Copyright 2021, Springer Nature (f) Schematic of the AFTPU films and coatings. (g) Solar reflective and thermal emissive spectra of the TUP
and AFTPU films [80]. Copyright 2022, The authors.

radiative coolers utilizing SiO2-embedded perovskite nanocrystals

Table 5
(NC)/PMMA+ZnO/PET/Ag emitters [151]. By utilizing Ag as a reflec­
Other polymers for PRC and their cooling performance.
tive metal, the resulting radiative cooler demonstrated a temperature
Materials Solar reflectivity IR Temperature Refs. reduction of 4.2 ◦ C compared to the ambient temperature.
(%) emissivity drop (◦ C) a
(%)

PEO 0.96 0.78 5 [73]

4.2. Nanoparticle composite structure
EPDM/SiO2 0.96 0.95 12 [138]
PLA/TiO2/PTFE 0.92 0.95 4.8 [76] While the structure of using a reflective metal layer on the bottom
PMMA 0.96 (500–1500) 0.9 7.5 [139] can achieve high emissions in the solar spectral range, it often requires
Melamine/ 0.94 0.95 2.5 [140]
complex processing procedures. It increases production costs due to the
formaldehyde
PP/PDMS 0.95 0.82 4 [77] use of precious metals. Furthermore, this structure presents challenges
POE/SEBS/PW/ 0.8 5.5 (Electronic [15] in directly applying it to existing surfaces with specific complex shapes,
BN Equipment) thereby limiting its application in various domains. The incorporation of
Silk/Al2O3 0.95 0.9 3.5 [78]
nanoparticles into the polymer matrix has emerged as an alternative
PLA 0.91 0.92 6.7 [141]
PVA/SiO2 0.97 0.95 4.5–7.5 [81]
strategy to meet the current requirements for radiative cooling in in­
PA6/SiO2 0.99(0.3–0.76μm) 0.78 16.6 (Simulate [142] dustrial and daily life scenarios. By selecting nanoparticles with a high
0.89(0.76–2.5μm) skin) bandgap and optimizing the interface between the polymer and nano­
PU/Si3N4 0.91 0.93 15.9 (Simulate [143] particles, a high solar reflectance can be achieved [152]. Additionally,
skin)
nanoparticles exhibit a narrow absorption band within the ATW,
TPU/SiO2 0.96 0.95 10.6 [144]
enhancing thermal radiation within the ATW range (Fig. 10b) [121,
a
Unless otherwise specified, the temperature difference in the table is the 153]. This enables cooling effects without the presence of metals.
temperature difference from the ambient temperature. Several inorganic nanoparticles, such as SiO2 [154–158], TiO2
[159–161], CaCO3 [162,163], Si3N4 [164,165], BaSO4 [166,167], and
reflectivity of 0.91 and LWIR emissivity of 0.9, as depicted in Fig. 11d others, can be embedded in polymers by this method.
and e. Subsequent outdoor experiments further verified the material’s As illustrated in Fig. 12a and b, a radiative cooler was constructed,
effectiveness in achieving uninterrupted outdoor cooling for 24 h, comprising a 3D porous cellulose acetate (3DPCA) matrix with inter­
resulting in an average temperature difference of 5 ◦ C throughout the nally deposited resonant polar dielectric SiO2 microspheres. This
day (Fig. 11f). Son et al. conducted a study where they developed solution-based coating exhibits an impressive LWIR emissivity of up to

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 10. Schematic diagram of (a) Multilayer structure with a bottom reflective metal layer [148]. Copyright 2022, Elsevier. (b) Nanoparticle composition structure
[122]. Copyright. 2021 Elsevier. (c) Porous structure [74]. Copyright 2021, The authors. (d) Nanofibers structure [73]. Copyright. 2020 Springer Nature. (e) Dy­
namic optical structures [149]. Copyright 2024, Elsevier.

Fig. 11. (a) Digital photo of the radiative cooler (RC). (b) and (c) microstructure of RC. The curves of (d) reflectivity and (e) emissivity. (f) The 24-h measurement of
the ambient temperature and the temperature of RC [148]. Copyright 2022, Elsevier.

0.95 and solar reflectivity of 0.96 (Fig. 12c). Subsequently, the authors transfer coefficients (q). From Fig. 12d, it can be observed that the
performed calculations to establish the relationship between the theo­ maximum value of the temperature difference decreases as the q value
retical net cooling power (Pnet) and the temperature difference (Ta-Tr) increases. This indicates a significant impact of non-radiative heat
between the ambient temperature (Ta) and the surface temperature of transfer on the cooling efficiency of the radiative cooler. It is worth
the cooler (Tr) for 3DPCA/SiO2-B under different non-radiative heat noting that, in the absence of non-radiative heat, 3DPCA/SiO2-B can

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 12. (a) Photos of the 3DPCA/SiO2 films. (b) SEM images of the 3DPCA/SiO2 hybrid film. (c) The curves of reflectivity and emissivity. (d) Pnet of 3DPCA/SiO2 for
different q values, Ta =25 ◦ C. (e) Rooftop measurement of the 3DPCA/SiO2 films cooling performance [122]. Copyright 2021, Elsevier.

achieve a maximum temperature difference of approximately 18 ◦ C structure enables the application of coatings and templates on diverse
during the daytime. However, in actual outdoor experiments, the cool­ surfaces, thereby expanding the potential scenarios for radiative cooling
ing temperature of the radiative cooler is approximately 8.6 ◦ C at night applications.
and 6.2 ◦ C during the day (Fig. 12e). The PMMA radiative cooler with a hierarchically porous array
(PMMAHPA), was prepared using phase separation and template process
4.3. Porous structure to introduce hierarchical pores [74]. As shown in Fig. 13a and b,
PMMAHPA has a white appearance and exhibits superhydrophobicity.
Compared with multilayer structures with reflective metal layers at The micromorphology shows hierarchical porous arrays with ordered,
the bottom and nanoparticle composite structures, polymers with symmetrical micropores (about 4.6 μm diameter) and random nano­
porous structures have better material cost and scalability, which uti­ pores (about 250 nm average diameter). This hierarchical porous array
lizes air scattering sunlight within the hierarchical pore structure of the gives PMMAHPA excellent optical properties, with an LWIR emissivity of
polymer as a substitute for the conventional reflective metal layer and up to 0.98 and a solar reflectance of 0.95 (Fig. 13c). Compared with
nanoparticle/polymer structure (Fig. 10c). Notably, the optical perfor­ nanoporous PMMANP, monolayer micropore array PMMAMPA, and
mance of the polymer radiative cooler achieved through this structure original PMMA, the optical performance of PMMAHPA has been greatly
can match that of the multilayer photonic structure. Furthermore, this improved. The cooling power of PMMAHPA was then tested using a hot

Fig. 13. Photograph of the PMMAHPA (a) SEM micrographs. (b) Optical photographs. (c) Spectral reflectance of the PMMAHPA. (d) Real-time temperature data of the
outdoor experiment with the PMMAHPA. (e) Cooling powers of the PMMAHPA [74]. Copyright 2021, The authors.

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L. Liu et al. Applied Materials Today 39 (2024) 102331

box device with a feedback-controlled heating system, and it was found shown in Fig. 14e, where the surface temperature of es-PEO can be
that the average cooling power of the PMMAHPA film reached 85 W/m2 reduced by up to 5 ◦ C compared to the ambient temperature while
at a solar intensity of 900 W/m2, and the cooling capacity of PMMAHPA achieving a remarkable cooling power of up to 110 W m-2. In addition,
was demonstrated in experiments in different regions. polymer/inorganic hybrid nanofiber membranes can also be used to
Additionally, template-based fabrication for porous structures can be construct radiative coolers. Jing et al. [174] developed hybrid mem­
utilized to prepare polymer-based radiative coolers. Ni et al. incorpo­ branes by incorporating Al2O3 nanoparticles into the PVDF spinning
rated table salt as a pore-forming agent and alumina as a filler into P solution, resulting in membranes with a high solar reflectance of 0.97
(VdF-HFP), which was subsequently cured [168]. The resulting com­ and a high emissivity of 0.95 within the ATW range. Field tests
posite film featured a porous structure with a solar reflectance of 0.92 demonstrated a cooling effect below 4 ◦ C compared to the ambient
and an infrared emissivity of 0.94. Field tests demonstrated a cooling temperature, and the RC performance was observed under diverse
effect of 8.3 ◦ C. Fan et al. employed water, an environmentally friendly weather conditions.
template, to fabricate porous PDMS membranes [169]. These thin films
exhibited outstanding optical properties and were suitable for radiative
cooling under diverse conditions. 4.5. Dynamic optical structure

As a unidirectional cooling mechanism, PDRC continually dissipates

4.4. Nanofibers structure heat into outer space. While promising for curbing cooling expenses in
high-temperature environments, this approach poses the risk of poten­
Nanofiber membranes are important in practical applications pri­ tial overcooling. To address this concern, researchers have focused on
marily due to their inherent advantages of simplicity, versatility, and optimizing the cooling efficiency of radiative coolers by targeting the
ease of regulation [170–173]. Additionally, nanofibers possess the two crucial optical parameters in radiative cooling: solar reflectance and
ability to self-assemble into well-ordered arrays or diverse hierarchical LWIR emissivity. The transmittance of visible light undergoes significant
structures, resulting in the formation of self-supporting films. Through changes before and after phase transition, with control over sunlight
parameter adjustments during the spinning process, the fiber diameter transmittance achieved through a combination of phase change material
can be precisely controlled to align with its Michael’s resonance wave­ (PCM) with a suitable transition temperature and polymer [175].
length within the solar spectrum. Consequently, polymer nanofibers can Moreover, the regulation of sunlight transmittance [149] and LWIR
effectively scatter a considerable amount of sunlight, and the radiative emissivity can be accomplished by applying temperature-sensitive
cooling effect can be achieved. hydrogels [176].
The nanofiber structures employed in constructing a radiative cooler, Fig. 10e shows a model of a high critical dissolution temperature
as presented in Fig. 10d, were prepared using electrospinning technol­ (UCST) polymer hydrogel used as a smart window. The optical photo­
ogy [73]. The resulting film, composed of electrostatic spinning PEO graph of Fig. 15a shows that the visible light transmittance of this smart
(es-PEO) with randomly stacked nanofiber structures, displays a white window during the day provides good visibility and brightness, and the
appearance due to the pronounced scattering of visible light (Fig. 14a). transparency is reduced at night to protect privacy. The reason for this
This is also confirmed by SEM images and size distributions (Fig. 14b shift in optical properties is given from the SEM images in Fig. 15b,
and c), es-PEO with a widely distributed nanofiber structure (500–1100 where the hydrogel shows a porous sheet structure at 60 ◦ C, while
nm). The reflection of sunlight by es-PEO is substantiated by both shrinkage occurs at 20 ◦ C, resulting in the formation of rod and spherical
theoretical calculations and practical test results (Fig. 14d). Addition­ structures, and the shrinkage of the polymer chains creates polymer-rich
ally, the polymer chain structure of PEO imparts a high emissivity within regions resulting in a decrease in visible light transmittance. The optical
the ATW range, thereby conferring excellent PDRC performance to performance of Fig. 15c and d shows that smart windows have a high
es-PEO. This is further supported by the results of actual outdoor tests, as visible light transmittance during the day without affecting the lighting

Fig. 14. (a) A photo of an es-PEO film. (b) SEM images of the es-PEO film. (c) The statistical distribution of the diameters of es-PEO film. (d) Spectral reflectance/
emittance of es-PEO film. (e) Real-time temperature data of the outdoor experiment with the es-PEO film [73]. Copyright 2020, Springer Nature.

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 15. (a) Optical photographs for the UCST smart window. (b) SEM images of the UCST smart window. (c) Transmittance spectra for UCST smart window. (d)
Emissivity spectrum for the UCST smart window (e) Real-time temperature data of the outdoor experiment with the UCST smart window [149]. Copyright
2024, Elsevier.

of the windows, reduce solar heating as much as possible, and high LWIR and a polymer-poor phase. The polymer-rich phase solidifies into a
emissivity promotes radiative cooling with the outside space, and re­ robust framework within the membrane, while the remaining polymer-
duces transparency at night to protect privacy. The actual outdoor test poor phase contributes to pore formation [180,181]. During the prac­
results show that the UCST exhibits a temperature difference of 5.1 ◦ C tical preparation process, the pore morphology can be finely adjusted by
and 2.2 ◦ C compared to ordinary glass and low-E glass, which proves its manipulating the solution concentration and the proportion of the
excellent radiative cooling performance (Fig. 15e). The use of smart mixed solvents. Illustrated in Fig. 16c, P(VdF-HFP) is dissolved in a
polymers for dynamic radiative cooling has a promising application. solvent mixture of acetone and water. Upon evaporation, characterized
by acetone’s high volatility and water’s low volatility, a hierarchical
5. Preparation methods of polymeric PDRC pore structure emerges, facilitating high reflectivity across the solar
spectrum [67].
5.1. Spraying coating
5.4. Hot pressing
Spraying involves the atomization of paint using a spray gun, fol­
lowed by its application onto the surface of an object. Precise control Control over the morphology of polymer-based radiant coolers is
over the thickness of the coating is achieved through the manipulation of achieved by regulating the temperature distribution of the template and
spraying time and speed. This method boasts adaptability across a broad the duration of static heat treatment during the hot pressing process.
spectrum of profiled substrates and holds promise for large-scale pro­ Zheng et al. introduced an innovative method for fabricating a tunable
duction [177]. In their investigation, Fan et al. utilized coatings anisotropic porous PMMA film with highly efficient daytime radiative
composed of yttrium oxide, titanium dioxide, and PDMS. Applying the cooling capabilities using a hot-pressed melt assembly technique [182].
spray technique to the substrate yielded an RC coating endowed with By adjusting the hot plate temperature close to the melting point of
exceptional cooling properties (Fig. 16a) [178]. PMMA, localized melting and binding of PMMA particles occur, result­
ing in the formation of numerous disordered micro/nanopores within
5.2. Brushing the film, which effectively enhances the scattering of incident sunlight
(Fig. 16d). Furthermore, hot pressing enhances the mechanical strength
In contrast with spraying, brushing demands a flat and smooth sur­ of polymer-based radiant coolers, making them suitable for various
face for optimal application. Nevertheless, brushing offers the flexibility everyday life applications [121].
to either coat the substrate surface or produce a self-supporting film
[80]. Fine-tuning of the desired film thickness is attainable through 5.5. Electrospinning
adjustments in the distance between the scraper and the substrate sur­
face. When combined with phase separation techniques [110], brushing Electrospinning technology is a versatile approach for producing
facilitates the formation of porous structures while incorporating nanofibers with varied shapes and materials, and its utility spans
nanoparticles into the solution yields nanoparticle composite structures numerous disciplines (Fig. 16e). Fine-tuning the morphology of these
(Fig. 16b) [179]. The PVDF/PDMS coating prepared by Wang et al. still nanofibers is achievable by adjusting parameters such as voltage, dis­
exhibited excellent superhydrophobicity and PDRC properties after one tance, flow rate, and concentration of the spinning solution during the
year of outdoor weather resistance testing and also performed well in electrospinning process [72]. Moreover, different collector configura­
sandpaper abrasion and sand impact tests, which proved the long-term tions allow for the directional alignment of nanofibers. Presently, elec­
durability and efficiency of polymer-based radiative cooling materials trospinning technology has enabled the fabrication of diverse polymer
in practical use. nanofiber membrane radiant coolers encompassing PEO [73], PVDF
[105], cellulose [16], etc.
5.3. Phase inversion
5.6. Ball milling
The phase separation method offers notable advantages in the
domain of porous material fabrication, entailing the dissolution of The ball milling method relies on balls as the grinding medium,
polymers in a blend of highly volatile and low-volatile solvents, which employing impact, extrusion, and friction mechanisms to achieve ma­
subsequently evaporate in sequence. As the solvents evaporate, phase terial fragmentation. During the ball milling process, grinding balls
separation occurs, resulting in the segregation of a polymer-rich phase within a sealed container move at high velocities, colliding with the

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 16. Schematic diagram of (a) Spraying coating [178]. Copyright 2022, American Chemical Society. (b) Brushing [179]. Copyright 2023, Elsevier. (c) Phase
inversion [67]. Copyright 2018, The American Association for the Advancement of Science. (d) Hot pressing [182]. Copyright 2024, Elsevier (e) Electrospinning
[105]. Copyright 2019, Wiley. (f) Ball milling [183]. Copyright 2022, Elsevier.

material to crush and disintegrate it into smaller particles, thereby 6. Application scenarios of polymer coolers
facilitating sample fine grinding. These resulting particles can function
as additives when combined with polymer coatings (Fig. 16f) [183]. The choice of radiative cooling materials is dependent on the specific
Recently, a straightforward "bottom-up" ball milling strategy was pro­ application. For instance, cooling solar cells requires transparent ma­
posed to produce uniform microassemblies of poly(vinylidene terials within the solar spectrum. When used in the construction in­
fluoride-hexafluoropropylene) nanoparticles [101]. By adjusting the dustry, materials need to possess improved resistance to aging and
input energy, an exceptionally efficient radiative cooler can be fabri­ hydrophobic properties to prevent water infiltration. In the textile field,
cated, demonstrating outstanding cooling performance. in addition to the requirements for spectral performance, certain com­
fort properties should also be met. The use of atmospheric water har­
vesting has high requirements for the hydrophilicity of polymer-based
radiative cooling materials. When used in the field of medical

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L. Liu et al. Applied Materials Today 39 (2024) 102331

protection, it is necessary not only to meet a certain level of air Recent experimental and theoretical investigations have demonstrated
permeability but also to be able to resist bacteria. Although several the potential application of radiative cooling in the construction in­
polymer-based radiative cooling materials with excellent spectral dustry through the incorporation of room-temperature phase-change
properties have been developed, there are still other non-material- vanadium dioxide (VO2) in smart windows [190] and smart building
related challenges that limit the practical application of reliable radia­ coatings [191]. These studies provide comprehensive evidence that
tive cooling systems. This is mainly due to the relatively low radiative underscores the promising prospects of radiative cooling in the realm of
energy density of radiative cooling, making it difficult to meet the re­ building architecture. Comparing the smart windows with the current
quirements of large-scale energy-intensive applications. Therefore, one commercial low emissivity glass, it was found that more energy can be
of the major challenges faced by radiative cooling applications is the saved, up to 324 MJ m-2, which shows the important application of
large-scale implementation of this technology in engineering practice. PDRC in the field of energy conservation and emission reduction.
However, this technique holds significant potential in real-world sce­ The outstanding physicochemical stability of PDMS grants it a high
narios. The following section primarily discusses the current applica­ degree of versatility in numerous everyday applications. In a study
tions of existing radiative cooling technologies and ongoing explorations conducted by Zhou et al., porous PDMS sponges were manufactured
in various potential application areas, such as building cooling, human using sucrose as a template and subsequently utilized as roofing mate­
body cooling, solar cell cooling, atmospheric water harvesting, ther­ rials for buildings [184]. This innovative approach effectively main­
moelectric generators, and medical protection (Fig. 17). tained a comfortable indoor temperature for human occupants by
reflecting sunlight and dissipating heat, as illustrated in Fig. 18a. The
6.1. Building spectral properties of the porous PDMS sponge and the original PDMS
are depicted in Fig. 18b and c, respectively. It is worth noting that the
As previously discussed, temperature regulation in residential and porous PDMS sponge exhibited superior spectral properties when
commercial buildings constitutes a significant portion of global energy employed for radiative cooling applications compared to the original
consumption. This is primarily attributed to the substantial energy PDMS sample. The actual outdoor experimental results in Fig. 18d
wastage by conventional HVAC systems in unoccupied spaces, leading to provide empirical evidence that the porous PDMS sponge effectively
inefficient cooling [188]. It is worth emphasizing that a moderate in­ reduced the temperature below ambient levels, whereas the original
crease of 2 ◦ C in the indoor temperature setpoint can result in energy PDMS did not exhibit any cooling effect. Furthermore, the porous PDMS
savings exceeding 20 % [189]. Given that the roofs of buildings are sponge demonstrated hydrophobicity advantageous for its application
directly exposed to the open sky, using radiative cooling materials in as a building material (Fig. 18e). Subsequently, a comparison was made
roofs can effectively reduce energy consumption associated with between the temperature-regulating capabilities of the porous PDMS
building cooling. By comparing PDRC materials with traditional PCM, sponge and existing commercial building materials (Fig. 18f). The
foam, and HVAC systems for the CO2 emitted by the exterior walls of architectural model with the porous PDMS sponge as the roof achieved a
buildings, it is found that PDRC materials have obvious advantages [46]. temperature 2 ◦ C lower than the ambient temperature under simulated

Fig. 17. Application scenarios of polymer-based radiative coolers. Building [184] Copyright 2021, The authors. Clothing [76]. Copyright 2021, The American
Association for the Advancement of Science. Water harvesting [125]. Copyright 2022, The authors. Solar cell [185]. Copyright 2021, John Wiley and Sons. Ther­
moelectric generators [186]. Copyright 2021, Elsevier. Medical protective [187]. Copyright 2023, The authors.

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 18. (a) Schematic illustration of a radiative cooling roof integrated with a residential building. The curves of (b) reflectivity and (c) emissivity. (d) Real-time
temperature and solar intensity data of the outdoor experiment. (e) Photos to demonstrate the hydrophobicity of the PDMS sponge. (f) Photos and infrared images
[184]. Copyright 2021, The authors.

sunlight, surpassing commercial painted asphalt tiles. These findings is significant potential in developing clothing with intelligent tempera­
provide compelling evidence for the feasibility of employing polymer ture control. It is important to note that a microclimate, referred to as
radiative cooling materials as energy-saving building components. the space between the human skin and clothing, exists in the immediate
vicinity of the human body [194]. The temperature and humidity within
this microclimate have a significant influence on the comfort level
6.2. Clothing experienced by individuals. By employing materials with appropriate
structural designs, it is possible to provide individuals with an optimal
With the intensification of global warming, the probability of temperature [195,196]. The human body’s comfort range typically falls
extreme weather events also increases [192,193]. While most in­ within 33.4 ± 3.0 ◦ C, highlighting the importance of designing suitable
dividuals can seek shelter in buildings during such occurrences, there clothing to maintain the body within this temperature range, particu­
are numerous occupations that require prolonged outdoor work. In such larly in harsh environments [197,198]. Currently, commonly used
cases, the human body’s temperature regulation solely depends on strategies include textiles incorporating phase change materials,
clothing. However, traditional clothing exhibits limited thermal man­ liquid-cooled clothing, gas-cooled clothing, etc. However, these
agement capabilities, thereby exposing individuals to an increased risk methods have noticeable drawbacks, such as limited effectiveness over
of overheating from the surrounding environment. Consequently, there

Fig. 19. (a) Schematic of a metafabric for daytime radiative cooling. (b) Measured reflectivity and emissivity spectra of the metafabric. (c) Continuous temperature
measurement of the subambient cooling performance test. (d) Temperature tracking for skin under different fabrics in direct sunlight [76]. Copyright 2021, The
American Association for the Advancement of Science.

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L. Liu et al. Applied Materials Today 39 (2024) 102331

time, substantial weight, and unsuitability for prolonged wear. Radia­ Zhang et al. employed cellulose as a substrate to prepare a well-
tive cooling clothing with one-way cooling performance offers a prom­ structured cellulose network, which exhibited potential for atmo­
ising solution to address these challenges. spheric water collection [125]. Fig. 20a visually illustrates the funda­
Zeng et al. conducted a study in which they selected polylactic acid mental principle of atmospheric water collection, wherein the
(PLA) and high-refractive index TiO2 composite woven textiles hierarchical network structure effectively reflects sunlight, preventing
renowned for their excellent absorption properties in the mid-infrared excessive heating of the material. Furthermore, the transparent window
band. These materials were employed to fabricate a layered metafa­ of the atmosphere facilitates efficient heat dissipation through radiation,
bric with a distinctive layered structure (Fig. 19a) [76]. By simulating thereby reducing the material’s temperature. By lowering the surface
the scattering and absorption efficiency of particles of different sizes temperature of the material below the dew point, condensation occurs
within the wavelength range of 0.3–25 μm in the metafabric, it was on its surface. Additionally, the cellulose’s abundance of hydroxyl
observed that this layered structure provides metafabrics with high groups enables the attraction of atmospheric water through hydrogen
sunlight reflectivity and infrared emissivity. The fabrics, designed based bonding. Fig. 20b visually presents the sunlight absorption and emis­
on the simulation results, exhibited a broadband reflectivity of 0.92 in sivity properties of the material under wet and dry conditions. It is worth
the solar radiation region and an average emissivity of 0.95 (Fig. 19b). noting that the infrared emissivity is slightly higher in a humid envi­
Outdoor experiments, as depicted in Fig. 19c, demonstrated that the ronment, thereby ensuring the material’s ability to maintain its cooling
metafabric consistently maintained temperatures below ambient levels performance even after water absorption. Moreover, Fig. 20c displays
throughout the day. Actual test results revealed that the metafabric the actual testing results, clearly indicating that the material’s surface
provided a cooling effect of 4.8 ◦ C for the human body, surpassing that temperature can be lower than the ambient temperature. Notably,
of commercial cotton fabrics (Fig. 19d). This notable cooling effect offers despite the ambient temperature exceeding the dew point during the
valuable protection for individuals working in high-temperature day, the material’s radiative cooling capacity enables its surface tem­
environments. perature to remain below the dew point. During nighttime, the material
Moreover, various multifunctional passive radiative cooling fabrics exhibits a cooling power of 82.7 W m-2. The study highlights the po­
with diverse capabilities have been developed in recent years. Among tential of utilizing cellulose for atmospheric water collection, owing to
the essential features of clothing, breathability has also gained its cost-effectiveness and scalable preparation method, which can be
increasing attention. Miao et al. fabricated Janus wetting interlayer adapted to local climate variations. Notably, the simulation results
structured textiles with exceptional spectral properties and unidirec­ indicate that at higher relative humidity levels (60 % and 90 %), the cost
tional moisture transport performance [199]. Through practical trials of water collection using this material is remarkably low, amounting to
involving human subjects, it was empirically demonstrated that Janus only $5.2⋅L-1 and $0.01⋅L-1, as showcased in Fig. 20d and e.
fabrics achieved a cooling effect of 4.2 ◦ C compared to cotton fabrics. Gu
et al. incorporated carbon nanotubes into PAN and combined them with 6.4. Solar cell
graded nanofibers and aerogel membranes to create a composite
multilayer structure [200]. This structure not only achieved a cooling Solar energy, as an inexhaustible and environmentally friendly
effect of 7.2 ◦ C compared to white cotton fabrics in hot environments but renewable energy source, has attracted considerable attention in recent
also exhibited a warming effect of 12.2 ◦ C compared to black cotton years. Researchers have been actively exploring effective ways to
fabrics in cold conditions. These findings offer valuable insights for the harness solar energy, with particular emphasis on the application of
future development of intelligent clothing. solar cells for electricity generation. Theoretical analysis indicates that
the upper limit of power conversion for solar cells is 33.7 % [207].
6.3. Water harvesting However, by employing material substitutions and incorporating addi­
tional junctions, the current generation of solar cells has achieved an
In recent years, the issue of water scarcity has become increasingly impressive conversion efficiency of 47.1 % [208]. Nevertheless, it is
prominent as the climate continues to deteriorate. Despite water ac­ crucial to acknowledge that a significant proportion of solar energy is
counting for 70.8 % of the Earth’s total area, 96.5 % of it exists as still converted into heat energy [209,210]. This phenomenon poses
saltwater in the oceans. Consequently, the subject of desalination has substantial challenges to the service life and output power of solar cells.
gradually garnered attention [201]. However, traditional membrane Consequently, finding solutions to reduce the operating temperature of
filtration and thermal desalination technologies often demand sub­ solar cells without compromising sunlight absorption has become an
stantial energy inputs and deplete numerous non-renewable resources urgent and pressing issue [211].
[202,203]. Moreover, while using renewable solar energy for desalina­ Lee et al. conducted a study focusing on the thermal management of
tion may appear to be a favorable choice, it encounters the obstacle of solar cells by developing a metamaterial with specific optical properties
being constrained by weather conditions and geographical location [185]. This metamaterial exhibits high transmittance in the solar spec­
[204]. Hence, the quest for a low-carbon, consistently operational trum and high absorption in the ATW. The composition of the meta­
desalination method has become a challenging aspect of contemporary material, as depicted in Fig. 21a, involves PDMS as the matrix material,
research. Passive radiant cooling technology offers a potential solution with randomly distributed silica aerogel particles. Additionally, the
by facilitating the collection of dew during the night through the metamaterial incorporates a light modulator, namely n-hexadecane.
reduction of surface temperature below the dew point [205]. Previously, This choice is primarily motivated by the similar refractive index and
the collection of dew was limited to nighttime. However, recent ad­ low extinction coefficient of PDMS, silicon oxide, and n-hexadecane
vancements in passive radiant cooling technology have made it possible within the visible light range. Moreover, n-hexadecane effectively per­
to collect fresh water throughout the day. This is achieved by designing a meates the micropores of silica aerogels and can be homogeneously
thin film material that allows sunlight transmission through an ATW. In mixed with PDMS to achieve a visually transparent metamaterial. The
a study by Du et al., they successfully developed a transparent radiative data presented in Fig. 21b indicates that the metamaterials exhibit a
cooling film with a solar transmittance of 0.93 and a "skylight" emis­ transmittance exceeding 0.91 in the solar spectral range, while their
sivity of 0.96 [206]. This innovative device facilitates the collection of emissivity in the atmospheric transparency window is 0.98. This high
fresh water on the inner surface of the top by evaporating seawater emissivity can be attributed to the abundant presence of Si-O-Si bonds
during the day. Additionally, the surface temperature of the film de­ within the material. Subsequently, the device illustrated in Fig. 21c was
creases below the dew point at night, enabling the outer surface to employed to measure the temperature of silicon solar cells, both with
collect dew. Consequently, this technology enables the continuous and without the application of metamaterials, under direct sunlight. The
collection of fresh water throughout the day. corresponding results are depicted in Fig. 21d and e. Specifically, when

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 20. (a) Schematic of atmospheric water harvesting by radiative cooling fabric. (b) Measured transmittance and reflectance. (c) Profiles of the sample surface
temperatures and ambient temperature. (d) Cumulative annual water collection solely by cellulose-based AWH. (e) Spatially averaged monthly water production per
area [125]. Copyright 2022, The authors.

Fig. 21. (a) Schematic illustration and working principle. (b) Measured transmittance and reflectance (c) Photos of the field test. Data of the outdoor experiment (d)
real-time temperature and (e) solar intensity [185]. Copyright 2021, John Wiley and Sons.

the solar intensity is 920 W m-2 and the relative humidity ranges from 30 end to the cold end, resulting in the accumulation of charge carriers and
to 45 %, the temperature of the solar cell covered with metamaterials is the generation of a potential difference [213,214]. As the internal
observed to be 7.7 ◦ C lower than that of the uncovered solar cell. temperature of the semiconductor approaches equilibrium, a relatively
Furthermore, through the implementation of the template method, stable potential difference is established. When the thermoelectric unit
Wang et al. successfully fabricated a periodic pyramid-textured PDMS is connected to a load, a direct current (DC) is formed within the circuit.
film (PPPF) for the encapsulation of commercial silicon solar cells [212]. The thermoelectric conversion efficiency of thermoelectric generators is
Within the wavelength range of 0.3–1.1 μm (representing the absorption directly influenced by the temperature difference between the hot and
spectrum of commercial silicon solar cells) [145], PPPF demonstrated a cold ends, as well as the dimensionless figure of merit (ZT) [215,216].
transmittance exceeding 0.9. Subsequent outdoor testing substantiated Numerous strategies have been implemented to enhance the ZT value of
that PPPF effectively reduced the temperature of the solar cells by 2 ◦ C, thermoelectric materials. However, due to the intricate interplay be­
thereby holding substantial significance in terms of extending their tween the electron and phonon transport parameters, achieving further
operational lifespan. improvements in ZT has posed significant challenges. Therefore, one
effective avenue to enhance the thermoelectric conversion efficiency is
by increasing the temperature difference between the hot and cold ends.
6.5. Thermoelectric generators
Numerous active cooling technologies have been explored for thermo­
electric generators; however, they often entail additional weight and
Thermoelectric generators (TEGs) are semiconductor devices that
energy consumption [217–219]. In contrast, passive radiative cooling
operate based on the Seebeck effect, which was initially discovered by
technology introduces a novel concept. Polymer radiative cooling ma­
German physicist Thomas Johann Seebeck in 1821. The Seebeck effect
terials, characterized by their small mass and flexibility, provide a so­
arises from the principle that, in the presence of a temperature gradient,
lution that does not impose any extra burden on the TEGs.
charge carriers within the semiconductor material diffuse from the hot

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Simultaneously, these materials passively cool the cold end, thereby solution to improve human thermal comfort, and the capability to
amplifying the temperature difference between the cold and hot ends functionally customize polymers allows for tailored solutions to address
and ultimately improving the thermoelectric conversion efficiency [220, specific needs. To address this challenge, Xu et al. successfully synthe­
221]. For instance, Liu et al. conducted an experiment where they sized masks with excellent filtration performance by electrospinning
coated the surface of TEGs with a radiative cooling layer consisting of P PA-6 onto PE melt-blown nonwoven fabric [224]. Furthermore, the high
(VdF-HFP) and SiO2 microspheres [186]. The experimental findings mid-IR transmittance of these two polymers enables effective trans­
demonstrated that the radiative cooling layer significantly enhanced the mission of human body heat radiation, thereby ensuring thermal
performance of the TEGs. At an indoor temperature of 295 K, TEGs with comfort.
the radiative cooling coating exhibited twice the output power density Furthermore, Cai et al. conducted an electrospinning study to
compared to those without it. fabricate composite nanofiber membranes, as demonstrated in Fig. 23a
Khan et al. proposed an innovative combination of a porous P(VdF- [187]. These membranes comprised graded TPU/ZIF-8 nanoparticles
HFP) film with TEGs, enabling the utilization of the temperature dif­ with radiative cooling and antibacterial properties. The graded structure
ference between the human body and the material’s surface to power within the nanofiber membrane contributed to a solar reflectance of
wearable devices autonomously [186]. The integrated TEGs, as depicted 0.97, surpassing the value of 0.84 observed for pure TPU nanofiber
in Fig. 22a, comprise a flexible TEGs radiating radiator with 40 ther­ membranes. Additionally, the presence of abundant C–N and N–H
moelectric branches, along with a lithium-sulfur battery for storing chemical bonds in ZIF-8 nanoparticles resulted in a slightly lower IR
excess power. Additionally, Fig. 22b illustrates the emissivity and emissivity for the pure TPU membrane compared to the composite
reflectance curves of a radiant cooler, with the film exhibiting an membrane within the atmospheric transparency window, as illustrated
impressive sunlight reflectivity of 0.97 and a LWIR emissivity of 0.97, in Fig. 23b. Outdoor tests, as depicted in Fig. 23c and d, provided
owing to the nano-micron hierarchical pore structure of the cooler. The empirical evidence of the composite membrane’s potential for outdoor
results obtained from actual outdoor testing demonstrated that the cooling. The composite membrane demonstrates a significant cooling
surface temperature of the radiant radiator can be reduced by 5 ◦ C effect, achieving a temperature reduction of 7.2 ◦ C compared to the
compared to the ambient temperature, as shown in Fig. 22c. Subse­ ambient temperature when exposed to direct sunlight. When utilized in
quently, the device was worn on the wrist for testing purposes, and the a mask, the composite membrane exhibits a temperature difference of
findings are presented in Fig. 22d and e. Based on the current-to-voltage 4.9 ◦ C. The photocatalytic property of ZIF-8 contributes to the composite
(I-V) curve, the TEGs achieved a maximum power output of 98.67 W membrane’s effective antibacterial performance under sunlight expo­
with an open-circuit voltage (Voc) of 22.00 mV under load-matched sure. This is evident in Fig. 23e and f, where the bacterial death rate of
conditions. During the nighttime, the TEGs attained a peak power the composite membrane exceeds 0.96 after exposure to sunlight, using
output of 206.07 W at Voc = 30.46 mV. Notably, these integrated TEGs E. coli and S. aureus as representative examples. Additionally, the
exhibited a power density of 12.48 W cm-2 and a temperature difference composite membrane exhibits excellent waterproof and breathable
of 1.9 ◦ C under natural convection conditions, surpassing the perfor­ properties, rendering it suitable for potential use in the medical pro­
mance of previously reported wearable, flexible TEGs. tective field.

6.6. Medical protection 7. Summary and outlook

Since 2019, the coronavirus disease (COVID-19) has been wreaking Broadly speaking, the cooling of the Earth’s surface by utilizing outer
havoc worldwide. In order to minimize the risk of infection, healthcare space as a cold reservoir is a fundamental method for heat dissipation,
workers are obliged to wear masks and protective clothing while car­ and its mechanism has been thoroughly explored. The proposal of
rying out outdoor tasks [222,223]. However, protective clothing with various radiative cooling materials/structures, coupled with their
inadequate breathability and ventilation can subject workers to exces­ demonstrated cooling performance in practical tests, offers the potential
sive heat stress. Polymer-based radiative cooling materials offer a viable to achieve the large-scale implementation of PDRC. Simultaneously,

Fig. 22. (a) Schematic comparison of compactness and power output. (b) Measured transmittance and reflectance. (c) Real-time temperature data of the outdoor
experiment. Open circuit voltage and power output measurements for both devices during (d) daytime and (e) nighttime measurements [186]. Copyright
2021, Elsevier.

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Fig. 23. (a) Schematic illustration of a hierarchical TPU/MOF composite nanofiber-based antibacterial radiative cooling fabric. (b) Measured transmittance and
reflectance. (c) Real-time temperature data of the outdoor experiment. (d) IR images of a volunteer wearing a membrane partially covered mask exposed to the
sunlight. (e) The bacterial mortality rates of E. coli and S. Aureus. (f) Co-cultured with the TZM and protective suit in lysogeny broth (LB) liquid medium [187].
Copyright 2023, The authors.

pursuing low-carbon and zero-carbon cooling technologies will drive a Radiative cooling, as an energy-efficient and environmentally
new wave of research in line with the global carbon neutrality goal, friendly heat dissipation process, offers an alternative solution to the
thereby facilitating the extensive production of PDRC materials. recurring environmental problems that have become increasingly
The objective of this review is to present a comprehensive summary prevalent in recent years. By operating without energy consumption and
of the polymer radiative cooling materials documented in the existing pollution and with the ability to function anytime and anywhere, radi­
literature. These materials are categorized into three groups based on ative cooling presents a promising approach. Integrating radiative
their cooling mechanisms: high sunlight reflection and high infrared cooling into PTM can enhance the cooling set point of indoor air con­
transmission, high sunlight reflection and high infrared emission, and ditioners, thereby addressing the current challenges associated with CO2
high sunlight transmission and high infrared emission. Furthermore, we emissions. However, applying energy-intensive large-scale systems faces
provide an in-depth discussion of several commonly employed polymer challenges due to the relatively low cooling density of radiative cooling.
radiative cooling materials while also summarizing the common Furthermore, when employing radiative coolers to cool other systems,
methods for their preparation. Lastly, we analyze the current application factors such as weather conditions, geographic location, and durability
scenarios of radiative cooling according to the cooling mechanism. must be considered. The phenomenon of radiative cooling predates
Through a meticulous analysis of the aforementioned sections, we draw human understanding, much like the existence of nature itself. Although
the following conclusions and perspectives: human exploitation has caused harm to the environment, it is believed
that through human efforts, a way to live in harmony with nature will
(1) Polymer radiative coolers demonstrate strong IR radiation char­ eventually be discovered.
acteristics, and their IR radiation intensity and spectral range
have been comprehensively investigated in previous studies. This CRediT authorship contribution statement
information is an essential point of reference for future re­
searchers when selecting polymers for PDRC, constituting a Ling Liu: Writing – original draft, Visualization, Validation, Formal
pivotal factor in the decision-making process. analysis, Data curation. Jin Wang: Writing – review & editing, Writing –
(2) Polymer radiative coolers demonstrate outstanding cooling per­ original draft, Supervision, Project administration, Formal analysis,
formance, remarkable scalability, and effortless functionaliza­ Conceptualization. Qingwen Li: Writing – review & editing,
tion. These characteristics position them as highly promising Supervision.
candidates for mass production, which is an essential require­
ment for their practical utilization. Declaration of competing interest
(3) The present techniques utilized for preparing polymer radiant
coolers, including porous structures and nanoparticle-filled The authors declare that they have no known competing financial
structures, may adversely impact their mechanical strength, interests or personal relationships that could have appeared to influence
consequently diminishing their longevity when employed in the work reported in this paper.
practical settings.
(4) At present, the achievable radiant cooling power is approxi­ Data availability
mately 100 W m-2. This indicates that, in order to provide sub­
stantial cooling power in real-world applications, a large surface Data will be made available on request.
area is necessary. To overcome this challenge, researchers have
investigated the incorporation of evaporative cooling into radiant
cooling, leading to an increased cooling power of 240 W m-2
Acknowledgments
[225].
This work was financially supported by the National Natural Science

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L. Liu et al. Applied Materials Today 39 (2024) 102331

Foundation of China (91963124) and the Suzhou Municipal Science and [30] J. Liang, J. Wu, J. Guo, H. Li, X. Zhou, S. Liang, C.W. Qiu, G. Tao, Radiative
cooling for passive thermal management towards sustainable carbon neutrality,
Technology Bureau (SJC2021008).
Natl. Sci. Rev. 10 (2023) nwac208.
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