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Extraction uranium (VI) (U(VI)) from wastewater and seawater is highly important for environmental protection and life safety, but it remains a great challenge. In this work, the growth of the zeolitic imidazolate framework-8 (ZIF-8) nanoparticles on the tannic acid (TA)-3-aminopropyltriethoxysilane (APTES) modified PVDF (TAP) membrane was designed to obtain an excellent U(VI) adsorbent. The zeolite imidazolate framework composite membrane (TAPP-ZIF-60) was prepared through polyethyleneimine (PEI) bridging strategy and temperature regulation strategy in solvothermal method. The coordination bond between PEI and ZIF-8 and the covalent bond between PEI and TAP are essential in forming stable composite membrane. TAPP-ZIF with different properties was synthesized through a temperature regulation process and the TAPP-ZIF prepared at 60 °C has the uniform morphology and good performance. The adsorption capacity of TAPP-ZIF-60 is 153.68 mg/g (C0 = 95.01 mg/L and pH = 8.0) and water permeability is 5459 L m-2 h-1 bar-1. After ten adsorption-desorption cycles, it is proved that TAPP-ZIF-60 has good repeatability and stability. In addition, the TAPP-ZIF-60 composites membrane has a good inhibitory effect on Staphylococcus aureus and Escherichia coli. X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) analysis reveal that the coordination between TAPP-ZIF-60 and uranyl ions is the primary factor contributing to the high adsorption capacity.
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It is a significant challenge to develop a fast carbon fiber (CF) surface modification method, especially for the high strength electromagnetic wave (EMW) absorption materials. Herein, magnetic CoOx nanoparticles are successfully synthesized and uniformly assembled on CF surface with high oxygen-containing groups by rapid ambient microwave carbon thermal shock (MCTS). The presence of oxygen defect sites on CF surface promotes CoOx nanoparticles nucleation. The number of oxygen defects and the types of magnetic nanoparticles on the CF surface effectively adjust the surface chemical activity and the electromagnetic properties of CF, which is conducive to improving the EMW absorption performance and interface compatibility of the CoOx nanoparticles modified CF reinforced polyamide 6 (CO@CF/PA6) composites. Compared with CO@CF-0 s/PA6, the tensile strength and modulus of CO@CF-3.5 s/PA6 composite are increased by 18.1 % and 18.6 %, respectively. It also displays a minimum reflection loss value (-59.9 dB) at a thinner thickness of 1.9 mm while the maximum effective absorption bandwidth reaches 5.02 GHz with a thickness of 1.8 mm. Its radar cross-section values exhibit less than -10 dBm2 at all tested detection angles. This rapid MCTS shows great potential for large-scale production of CF modification with low-cost, efficient and environmentally friendly process.
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Diglycidyl ether of bisphenol A crosslinking with glutaric anhydride is used to form the conventional "covalent adaptive network", polyether sulfone (PES) by coiling and aggregating on the adaptive network is used to significantly increase the uncured resin viscosity for improving the processability of epoxy resin, but inevitably affecting the curing reaction and dynamic transesterification reaction. This study investigates the crucial roles of PES in curing dynamics and stress relaxation behavior. The results indicate that although PES does not directly participate in the crosslinking reaction of polyester-based epoxy vitrimers. Moreover, the isothermal curing studies reveal that the addition of PES can greatly bring forward the reaction rate peak from conversion α = 0.6 to α = 0.2, meaning that the curing mechanism transfers from chemical control to diffusion control. Dynamic property analysis shows that the addition of PES significantly accelerates stress relaxation, especially at lower temperatures, leading to low viscous flow activation energy Eτ and relatively insensitive stress relaxation behavior to temperature. Introducing PES into vitrimer resin greatly improves crosslinking density (2.31 × 104 mol m- 3), enhancing glass transition temperature (82.68 °C), tensile strength (68.66 MPa), and fracture toughness (6.25%). Additionally, the modified vitrimer resin exhibits satisfying shape memory performance and reprocessing capability.
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The design and development of high-quality electromagnetic waves (EMW) absorbing materials play a vital role in combating the escalating negative effects of microwave radiation and interference. Herein, MoS2@Co/NC@CF fibrous membranes are successfully fabricated by electrospinning technology and carbonization, and a molybdenum disulfide (MoS2) layer is synthesized on the surface of these fibers via hydrothermal method. The seed-assisted growth method not only effectively avoids the accumulation and improves the loading of ZIF-67 particles, so as to ensure that the magnetic components in the fibers are evenly distributed in a wider range, rather than only intermittently present in some sites. Meanwhile, the introduction of semiconductor MoS2 as the shell further optimizes the impedance matching and improves the EMW absorption performance of the carbon fibrous membranes: the minimum reflection loss (RLmin) is -67.56 dB, and the maximum effective absorption bandwidth (EABmax) is further expanded to 6.56 GHz (2.1 mm, 11.44-18 GHz). This work provides a feasible method for developing high-efficient EMW-absorbing materials.
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It is a significant challenge to obtain hydrogels simultaneously with low tensile energy dissipation, high compressive resilience and long durability. Herein, the uniform dynamic nanospheres (Sil-4H0.75) derived from 4-Hydroxybutyl acrylate glycidyl ether grafted silk fibroin is designed to overcome this issue. Due to its uniform and dynamic characteristic, Sil-4H0.75 could endow hydrogel with homogeneous multiscale structure and produce unique framework effect. Thus, transparent Sil-4H0.75 crosslinked acrylamide hydrogel doped with Ag nanowires APS3.75%/AgNW0.1 exhibits a high stretchability (1260 %) and outstanding elastic resilience. The tensile energy dissipation ratio maintains a low value of 9 % across a wide 800 % strain range. A high compression resilience ratio of 92.2 % is kept after ten compression cycles under 90 % compressive strain. The orderly AgNWs motion guided by framework effect also make it be used as both tensile and compressive sensors and exhibits high gauge factor of 7.35, outstanding compression sensitivity of 30.379 kPa-1 and excellent durability (up to 2000 cycles). The detection or other applications based on both two sensing modes are also demonstrated. In a word, this work affords a general strategy to achieve high-performance hydrogel based on uniform dynamic nanospheres which exhibits great potential in the applications of flexible wearable strain sensors.
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Transparent electromagnetic interference (EMI) shielding is highly desired in specific visual scenes, but the challenge remains in balancing their EMI shielding effectiveness (SE) and optical transmittance. Herein, this study proposed a directionally aligned silver nanowire (AgNW) network construction strategy to address the requirement of high EMI SE and satisfactory light transmittance using a rotation spraying technique. The orientation distribution of AgNW is induced by centrifugal inertia force generated by a high-speed rotating roller, which overcomes the issue of high contact resistance in random networks and achieves high conductivity even at low AgNW network density. Thus, the obtained transparent conductive film achieved a high light transmittance of 72.9% combined with a low sheet resistance of 4.5 Ω sq-1 and a desirable EMI SE value of 35.2 dB at X band, 38.9 dB in the K-band, with the highest SE of 43.4 dB at 20.4 GHz. Simultaneously, the excellent conductivity endowed the film with outstanding Joule heating performance and defogging/deicing ability, ensuring the visual transparency of windows when shielding electromagnetic waves. Hence, this research presents a highly effective strategy for constructing an aligned AgNW network, offering a promising solution for enhancing the performance of optical-electronic devices.
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Liquid crystal elastomers (LCEs), consisting of polymer networks and liquid crystal mesogens, show a reversible phase change under thermal stimuli. However, the kinetic performance is limited by the inherently low thermal conductivity of the polymers. Transforming amorphous bulk into a fiber enhances thermal conductivity through the alignment of polymer chains. Challenges are present due to their rigid networks, while cross-links are crucial for deformation. Here, we employ hydrodynamic alignment to orient the LCE domains assisted by controlled in situ cross-linking and to remarkably reduce the diameter to submicrons. We report that the intrinsic thermal conductivity of LCE fibers at room temperature reaches 1.44 ± 0.32 W/m-K with the sub-100 nm diameter close to the upper limit determined in the quasi-1D regime. Combining the outstanding thermal conductivity and thin diameters, we anticipate these fibers to exhibit a rapid response and high force output in thermomechanical systems. The fabrication method is expected to apply to other cross-linked polymers.
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The efficient capture of uranium from wastewater is crucial for environmental remediation and the sustainable development of nuclear energy, yet it poses considerable challenges. In this study, amphiphilic ionic covalent organic framework intercalated into graphene oxide (GO) nanosheets functionalized with polyethyleneimine (PEI) were used to construct hybrid membranes with ultrafast uranium adsorption. These hybrid membranes achieved equilibrium in just 10 min and the adsorption capacity was as high as 358.8 mg g-1 at pH = 6. X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) analyses revealed that the strong interaction between sulfonic acid groups and uranyl ions was the primary reason for the high adsorption capacity and selectivity. The extended transition state and natural orbitals for chemical valence (ETS-NOCV) analysis revealed that the interaction between the 7 s and 5f orbitals of uranyl and the 2p orbitals of S and O in the sulfonate was the primary reason for the strong interaction between the sulfonate and the uranyl ion. This research presents an effective method for the rapid extraction of uranium from wastewater.
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Grafito , Uranio , Aguas Residuales , Uranio/química , Grafito/química , Aguas Residuales/química , Adsorción , Espectroscopía de Fotoelectrones , Membranas Artificiales , Estructuras Metalorgánicas/química , Contaminantes Radiactivos del Agua/químicaRESUMEN
Conductive hydrogels (CHs) are emerging materials for next generation sensing systems in flexible electronics. However, the fabrication of competent CHs with excellent stretchability, adhesion, self-healing, photothermal conversion, multisensing, and environmental stability remains a huge challenge. Herein, a nanocomposite organohydrogel with the above features is constructed by in situ copolymerization of zwitterionic monomer and acrylamide in the existence of carboxylic cellulose nanofiber-carrying reduced graphene oxide (rGO) plus a solvent displacement strategy. The synergy of abundant dipole-dipole interactions and intermolecular hydrogen bonds enables the organohydrogel to exhibit high stretchability, strong adhesion, and good self-healing. The presence of glycerol weakens the formation of hydrogen bonds between water molecules, endowing the organohydrogel with excellent environmental stability (-40 to 60 °C) to adapt to different application scenarios. Importantly, the multimodal organohydrogel presents excellent sensing behavior, including a high gauge factor of 16.3 at strains of 400-1440% and a reliable thermal coefficient of resistance (-4.2 °C-1) over a wide temperature widow (-40 to 60 °C). Moreover, the organohydrogel displays a highly efficient and reliable photothermal conversion ability due to the favorable optical absorbing behavior of rGO. Notably, the organohydrogel can detect accurate human activities at ambient temperature, demonstrating potential applications in flexible intelligent electronics.
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Polymers are often used as adhesives to improve the mechanical properties of flexible electromagnetic interference (EMI) shielding layered films, but the introduction of these insulating adhesives inevitably reduces the EMI performance. Herein, ultrafine aramid nanofibers (UANF) with a diameter of only 2.44 nm were used as the binder to effectively infiltrate and minimize the insulating gaps in MXene films, for balancing the EMI shielding and mechanical properties. Combining the evaporation-induced scalable assembly assisted by blade coating, flexible large-scale MXene/UANF films with highly aligned and compact MXene stacking are successfully fabricated. Compared with the conventional ANF with a larger diameter of 7.05 nm, the UANF-reinforced MXene film exhibits a "brick-mortar" structure with higher orientation and compacter stacking MXene nanosheets, thus showing the higher mechanical properties, electrical conductivity, and EMI shielding performance. By optimizing MXene content, the MXene/UANF film can achieve the optimal tensile strength of 156.9 MPa, a toughness of 2.9 MJ m-3, satisfactory EMI shielding effectiveness (EMI SE) of 40.7 dB, and specific EMI SE (SSE/t) of 22782.4 dB cm2/g). Moreover, the composite film exhibits multisource thermal conversion functions including Joule heating and photothermal conversion. Therefore, the multifunctional MXene/UANF EMI shielding film with flexibility, foldability, and robust mechanical properties shows the practical potential in complex application environments.
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A lightweight flexible thermally stable composite is fabricated by combining silica nanofiber membranes (SNM) with MXene@c-MWCNT hybrid film. The flexible SNM with outstanding thermal insulation are prepared from tetraethyl orthosilicate hydrolysis and condensation by electrospinning and high-temperature calcination; the MXene@c-MWCNTx:y films are prepared by vacuum filtration technology. In particular, the SNM and MXene@c-MWCNT6:4 as one unit layer (SMC1) are bonded together with 5 wt% polyvinyl alcohol (PVA) solution, which exhibits low thermal conductivity (0.066 W m-1 K-1) and good electromagnetic interference (EMI) shielding performance (average EMI SET, 37.8 dB). With the increase in functional unit layer, the overall thermal insulation performance of the whole composite film (SMCx) remains stable, and EMI shielding performance is greatly improved, especially for SMC3 with three unit layers, the average EMI SET is as high as 55.4 dB. In addition, the organic combination of rigid SNM and tough MXene@c-MWCNT6:4 makes SMCx exhibit good mechanical tensile strength. Importantly, SMCx exhibit stable EMI shielding and excellent thermal insulation even in extreme heat and cold environment. Therefore, this work provides a novel design idea and important reference value for EMI shielding and thermal insulation components used in extreme environmental protection equipment in the future.
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Endoscopic surgery is an effective and common clinical practice for chronic sinusitis. Nasal packing materials are applied in nasal surgery to prevent hemorrhage and promote wound healing. In this study, a degradable polyurethane foam dressing is successfully developed as a promising nasal packing material with good biocompatibility and antibacterial capability. Specifically, quaternized chitosan (QCS) serves as the crosslinker instead of polyols to offer polyurethane foam (PUF-QCS) antibacterial capability. The PUF-QCS2.0 % (with 2.0 wt% QCS) exhibits satisfactory liquid absorption capacity (19.4 g/g), high compressive strengths at both wet (14.5 kPa) and dry states (7.7 kPa), and a good degradation rate (8.3 %) within 7 days. Meanwhile, PUF-QCS2.0 % retains long-term antibacterial activity for 7 days and kills 97.3 % of S. aureus and 91.8 % of E. coli within 6 hours in antibacterial testing. Furthermore, PUF-QCS2.0 % demonstrates a positive hemostatic response in the rabbit nasal septum mucosa trauma model by reducing hemostatic time over 50.0 % and decreasing blood loss up to 76.1 % compared to the commercial PVA nasal packing sponge. Importantly, PUF-QCS also exhibits a significant antibacterial activity in nasal cavity. This nasal packing material has advantages in post-surgery bleeding control and infection prevention. STATEMENT OF SIGNIFICANCE: The performance of a nasal packing sponge requires good mechanical properties, fast and high liquid absorption rate, effective degradability and strong antibacterial activity. These features are helpful for improving the postoperative recovery and patient healing. However, integrating these into a single polyurethane foam is a challenge. In this study, quaternized chitosan (QCS) is synthesized and used as a chain extender and antibacterial agent in preparing a degradable polyurethane foam (PUF-QCS) dressing. PUF-QCS undergoes partial degradation and exhibits effective broad-spectrum antibacterial activity in 7 days. The reduction of postoperative bleeding and infection observed in the animal experiment further demonstrates that the PUF-QCS developed here outperforms the existing commercial nasal packing materials.
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Antibacterianos , Quitosano , Poliuretanos , Poliuretanos/química , Poliuretanos/farmacología , Quitosano/química , Quitosano/farmacología , Conejos , Animales , Antibacterianos/farmacología , Antibacterianos/química , Hemostasis/efectos de los fármacos , Staphylococcus aureus/efectos de los fármacos , Hemostáticos/química , Hemostáticos/farmacología , Vendajes , Escherichia coli/efectos de los fármacos , MasculinoRESUMEN
Poor interfacial quality and low refractive index contrast (Δn) are critical challenges for the development of high-performance one-dimensional photonic crystals (1DPhCs) via solution methods that impede their optical efficiency. Herein, we introduce an innovative approach by hybridizing hollow SiO2 with poly(vinyl alcohol), referred to as PHS, followed by alternate assembly with TiO2 via spin-coating, achieving a 1DPhC with Δn = 0.76 at the wavelength of 550 nm. This method circumvents the need for high-temperature treatment and complex curing conditions, resulting in a 1DPhC with superior interfacial and optical characteristics. By adjusting the thickness of the PHS layers, we can finely tune the reflectance spectrum, attaining over 99% reflectance at the photonic band gap. Furthermore, 1DPhC demonstrates excellent adhesion to polycarbonate substrates and retains its optimal optical performance even after rigorous environmental testing, including hygrothermal cycles, exposure to hot water, friction, and solvent sonication. This research paves the way for the facile fabrication of high-performance 1DPhCs under mild conditions, offering new perspectives for photonic material processing.
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Plasmonic photocatalysis demonstrates great potential for efficiently harnessing light energy. However, the underlying mechanisms remain enigmatic due to the transient nature of the reaction processes. Typically, plasmonic photocatalysis relies on the excitation of surface plasmon resonance (SPR) in plasmonic materials, such as metal nanoparticles, leading to the generation of high-energy or "hot electrons", albeit accompanied by photothermal heating or Joule effect. The ability of hot electrons to participate in chemical reactions is one of the key mechanisms, underlying the enhanced photocatalytic activity observed in plasmonic photocatalysis. Interestingly, surface-enhanced Raman scattering (SERS) spectroscopy allows the analysis of chemical reactions driven by hot electrons, as both SERS and hot electrons stem from the decay of SPR and occur at the hot spots. Herein, we propose a highly efficient SERS substrate based on cellulose paper loaded with either Ag nanoplates (Ag NPs) or AgPd hollow nanoplates (AgPd HNPs) for the in situ monitoring of C-C homocoupling reactions. The data analysis allowed us to disentangle the impact of hot electrons and the Joule effect on plasmon-enhanced photocatalysis. Computational simulations revealed an increase in the rate of excitation of hot carriers from single/isolated AgPd HNPs to an in-plane with a vertical stacking assembly, suggesting its promise as a photocatalyst under broadband light. In addition, the results suggest that the incorporation of Pd into an alloy with plasmonic properties may enhance its catalytic performance under light irradiation due to the collection of plasmon-excitation-induced hot electrons. This work has demonstrated the performance-oriented synthesis of hybrid nanostructures, providing a unique route to uncover the mechanism of plasmon-enhanced photocatalysis.
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Developing novel absorbent materials targeting high-efficiency, low-energy-consumption, and environmental-friendly oil spill cleanup is still a global issue. Porous absorbents endowed with self-heating function are an attractive option because of that they are able to in-situ heat crude oil and dramatically reduce oil viscosity for efficient remediation. Herein, we facilely prepared an eco-friendly multifunctional bacterial cellulose/MXene aerogel (P-SBC/MXene aerogel) for rapid oil recovery. Thanks to excellent full solar spectrum absorption (average absorbance = 96.6 %), efficient photo-thermal conversion, and superior electrical conductivity (electrical resistance = 36 Ω), P-SBC/MXene aerogel exhibited outstanding photothermal and electrothermal capabilities. Its surface temperature could quickly reach 93 °C under 1.0 kW/m2 solar irradiation and 124 °C under 3.0 V voltage respectively, enabling effective heat transfer toward spilled oil. The produced heat significantly decreased crude oil viscosity, allowing P-SBC/MXene aerogel to rapidly absorb oil. By combining solar heating and Joule heating, P-SBC/MXene aerogel connected to a pump-assisted absorption device was capable of achieving all-weather crude oil removal from seawater (crude oil flux = 630 kg m-2 h-1). More notably, P-SBC/MXene aerogel showed splendid outdoor crude oil separation performance. Based on remarkable crude oil/seawater separation ability, the versatile aerogel provides a promising way to deal with large-area oil spills.
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The rational use and conversion of energy are the primary means for achieving the goal of carbon neutrality. MXenes can be used for photothermal conversion, but their opaque appearance limits wider applications. Herein, we successfully develop visible-light transparent and UV-absorbing polymer composite film by solution blending the MXene with polyethylene and then vacuum pressing. The resulting film could be quickly heated to 65 °C under 400 mW cm-2 light irradiation and maintained over 85% visible-light transmittance as well as low haze (<12%). The findings of the indoor heat insulation test demonstrate that the temperature of the glass house model covered by this film was 6-7 °C lower than that of the uncovered model, revealing the potential of transparent film in energy-saving applications. In order to mimic the energy-saving condition of the building in various climates, a typical building model with this film as the outer layer of the window was created using the EnergyPlus building energy consumption software. According to predictions, they could reduce yearly refrigeration energy used by 31-61 MJ m-2, and 3%-12% of the total energy used for refrigeration in such structures. This work imply that the film has wide potential for use as transparent devices in energy-related applications.
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Metal-organic frameworks (MOF)-polymer hybrid hydrogel solves the processable forming of MOF powder and energy consumption of uranium extraction. However, the hybrid hydrogel by conventional synthesis methods inevitably lead to MOF agglomeration, poor filler-polymer interfacial compatibility and slowly adsorption. Herein, we designed that ZIF-67 was implanted into the carboxymethyl cellulose/polyacrylamide (CMC/PAM) by network-repairing strategy. The carboxyl and amino groups on the surface of CMC/PAM drive the uniform growth of ZIF-67 inside the CMC/PAM, which form an array of oriented and penetrating microchannels through coordination bonds. Our strategy eliminate the ZIF-67 agglomeration, increase the interfacial compatibility between MOF and polymer. The method also improve the free and fast diffusion of uranium in CMC/PAM/ZIF-67 hydrogel. According to the experimental, these enhancements synergistically enabled the CMC/PAM/ZIF-67 have a maximum adsorption capacity of 952â¯mgâ¯g-1. The adsorption process of CMC/PAM/ZIF-67 fits well with pseudo-second-order model and Langmuir isotherm. Meanwhile, the CMC/PAM/ZIF-67 maintain a high removal rate (87.3â¯%) and chemical stability even during ten adsorption-desorption cycles. It is worth noting that the adsorption amount of CMC/PAM/ZIF-67 in real seawater is 9.95â¯mgâ¯g-1 after 20â¯days, which is an ideal candidate adsorbent for uranium extraction from seawater.
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Resinas Acrílicas , Carboximetilcelulosa de Sodio , Estructuras Metalorgánicas , Agua de Mar , Uranio , Uranio/química , Uranio/aislamiento & purificación , Adsorción , Resinas Acrílicas/química , Carboximetilcelulosa de Sodio/química , Estructuras Metalorgánicas/química , Agua de Mar/química , Hidrogeles/química , Cinética , Purificación del Agua/métodos , Contaminantes Radiactivos del Agua/aislamiento & purificación , Contaminantes Radiactivos del Agua/químicaRESUMEN
Passive radiative cooling (PRC) that realizes thermal management without consuming any energy has attracted increasing attention. Unfortunately, polymer fibers with radiative cooling function fabricated via a facile, continuous, large-scale and eco-friendly method have been scarcely reported. Herein, polyethylene fibers containing directional microchannels (PFCDM) are facilely fabricated via melt extrusion and water leaching. Interestingly, fabric based on such hydrophobic PFCDM shows high sunlight reflectivity (93.6%), and mid-infrared emissivity (93.9%), endowing it with remarkable PRC performance. Compared with other reported examples, the as-prepared PFDCM fabric has the highest cooling power (i.e., 104.285 W m-2) and temperature drop (i.e., 27.71 °C). Furthermore, decent self-cleaning performance can keep the PFCDM fabric away from contamination and enable it to retain an excellent radiative cooling effect. The method proposed to fabricate PFCDM in this paper will widen the potential application of thermoplastic polyolefins in the field of radiative cooling.