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π-conjugated chromophore functionalized high-nuclearity titanium-oxo clusters containing structural unit of anatase for photocatalytic selective oxidation of sulfides

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Rare Metals 2024年第4期43卷 1736-1746页

作者： Ling-Rong Liao Dong-Chun Zheng Pin-Xi Ou Qi-Xin Zhao Wei-Min Xuan Qi Zheng state key laboratory for modification of chemical fibers and polymer materials & College of materials Science and Engineering Donghua University state key laboratory for modification of chemical fibers and polymer materials and College of Chemistry and chemical Engineering Donghua University

N-doping has significant influence in manipulating the properties of TiO2,and this has stimulated the development of N-donor-functionalized titanium-oxo clusters（TOCs） as molecular models to study the structure-property relationship.However,the structural type and photoresponsive application are still limited for such TOCs,especially regarding the high-nuclearity TOCs that contain structure unit of TiO2for photocatalysis.Herein,we showed the synthesis of a series of high-nuclearity TOCs 1-3 compounds using π-conjugated 1,10-phenanthroline（phen） as chromophore and N-donor functional ligand.Compound 1 features cocrystal structure composed of one [Ti26]2+and half [Ti22]2+,which renders it as the first cocrystallized TOC containing two positively charged species and phen-functionalized TOC showing the highest nuclearity up to 37 Ti centers.By adjusting the synthetic conditions,the individual {Ti22} and {Ti26} clusters can also be isolated as Compounds 2 and 3,respectively.The core structure of {Ti22} is mainly constructed from four lacunary {Ti4} derived from pentagonal {Ti（Ti）5} unit,while {Ti26} is built from four complete {Ti（Ti）5} unit.Notably,a {Ti8O14} structure unit of anatase TiO2can be identified in {Ti26}.Based on the unique structural features and proper photophysical and photochemical properties of Compounds 1-3,they are applied for photocatalytic sulfoxidation.Owing to the presence of anatase structure unit in {Ti26} and the synergistic effect from {Ti22} and {Ti26},the catalytic performance presents in the order of Compound 1> Compound 3> Compound 2.This work provides excellent models to understand the structureproperty relationship from the perspective of cocrystallization and Ti-O binding model and will further promote the application of TOCs as functional catalysts for organic transformation.

关键词： Titanium-oxo cluster Molecular model of anatase TiO 2 High nuclearity π-conjugated chromophore Photocatalytic sulfoxidation

A Skin-Inspired Self-Adaptive System for Temperature Control During Dynamic Wound Healing

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Nano-Micro Letters 2024年第8期16卷 211-224页

作者： Yaqi Geng Guoyin Chen Ran Cao Hongmei Dai Zexu Hu Senlong Yu Le Wang Liping Zhu Hengxue Xiang Meifang Zhu state key laboratory for modification of chemical fibers and polymer materials College of Materials Science and EngineeringDonghua University2999 North Renmin RoadShanghai 201620People’s Republic of China

The thermoregulating function of skin that is capable of maintaining body temperature within a thermostatic state is critical.However,patients suffering from skin damage are struggling with the surrounding scene and situational awareness.Here,we report an interactive self-regulation electronic system by mimicking the human thermos-reception system.The skin-inspired self-adaptive system is composed of two highly sensitive thermistors(thermal-response composite materials),and a low-power temperature control unit(Laserinduced graphene array).The biomimetic skin can realize self-adjusting in the range of 35–42℃,which is around physiological temperature.This thermoregulation system also contributed to skin barrier formation and wound healing.Across wound models,the treatment group healed~10%more rapidly compared with the control group,and showed reduced inflammation,thus enhancing skin tissue regeneration.The skin-inspired self-adaptive system holds substantial promise for nextgeneration robotic and medical devices.

关键词： Thermo-reception Self-regulation Flexible electronic system Wound healing

A Low Cost, Green Sustainable and Biodegradable Biomass-based Fluorine-free Water and Oil Repellent

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Chinese Journal of polymer Science 2024年第4期42卷 480-491页

作者： Zhi-Wei Shen Shu-Feng Hu Chen Zeng Wei-Qing Kong Mei-Fang Zhu state key laboratory for modification of chemical fibers&polymer materials College of Materials Science and EngineeringDonghua UniversityShanghai201620China state key laboratory of Pulp and Paper Engineering School of Light Industry and EngineeringSouth China University of TechnologyGuangzhou510630China

With the global ban on plastics intensifying, the substitution of plastic with paper has garnered increasing attention. However, the inadequate water and oil repellency of pulp molding hinders its practical applications. Currently, the common method to enhance the oil and water repellency of pulp molding is by adding fluorinated water and oil repellents. Nevertheless, fluorinated compounds are environmentally and physiologically harmful. Therefore, the development of fluorine-free, water and oil repellent alternatives is crucial. In this study, chitosan and stearic acid were utilized as the first and second layers of the oil and water repellent coatings, respectively. The coated samples exhibited favorable water repellency, with a water contact angle of 116.4°, and excellent oil repellency, achieving a 12/12 rating on the kit scale. Importantly, the samples did not exhibit any leakage after being soaked in hot water and hot oil at 95±5℃ for 30 min, demonstrating remarkable performance as a barrier against hot water and oil. Moreover, the coated samples displayed outstanding mechanical properties, thermal stability, biodegradability, and recyclability. The approach presented in this study is simple, cost-effective, environmentally friendly, and represents a promising technique for producing fluoride-free, oil-and water-resistant pulp molding products.

关键词： Biomass Fluoride-free Oil-andwater-resistant Plasticfree

Constructing on-demand single/multi-color transitioning fabrics with photocatalysis/photothermal-armed deficient semiconductors

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Nano Research 2024年第5期17卷 3633-3643页

作者： Daniel K.Macharia Shamima Sarker Meng Liu Zeyulong Wen Nuo Yu Meifang Zhu Zhigang Chen state key laboratory for modification of chemical fibers and polymer materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620China

On-demand color switching systems that utilize synchronized semiconductor-catalyzed reduction and photothermal-accelerated oxidation in liquid/solid are highly appealing.Herein,on-demand single/multi-color switching fabrics have been constructed by using defective SnO_(2):Sb-based color switching systems.SnO_(2):Sb nanocrystals with the suitable doping concentration accord lattices with abundant free electrons,conferring high photocatalytic and photothermal performances.A well-crafted set of dual light-responsive semiconductor-catalyzed systems with rapid color change can be attained via the homogenous mixture of SnO_(2):Sb with suitable redox dyes to produce single-color(RGB(red,green,blue))and multi-color transitioning(purple and green)systems.The illumination of these systems by 450 nm light triggers rapid photocatalytic discoloration,while irradiation by 980 nm light confers the photothermal effect that accelerates recoloration in air.Besides,the inks can be extended to rewritable fabrics by embedding the nanocrystals and redox dyes into hydroxyethyl cellulose(as the polymer matrix)and then coating on hydrophobic cotton fabrics to produce photo-switchable fabrics with excellent single/multi-color response.By exploiting the dual light interactions with the semiconductor-mediated systems,various images/letters can be remotely printed and erased on the rewritable fabrics which show promise for potential applications as information storage media and visual sensors.Importantly,the present rewritable fabric shows good stability and reversibility.The present work provides insights into the development of novel color-switching materials.

关键词： color switching defective semiconductor photocatalysis photothermal rewritable fabrics

Investigating the Absorption and Desorption Behavior of Methylene Chloride in the Poly(aryl ether ketone) Film with Different Crystallinities

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Chinese Journal of polymer Science 2024年第2期42卷 239-246,I0009页

作者： Hong-Ru Yang Jin-Dong Zhang Dong-Ting Gao Gang Liu Chun-Hai Chen Jia-Nan Yao Center for Advanced Low-Dimension materials State Key Laboratory for Modification of Chemical Fibers and Polymer MaterialsCollege of Materials Science and EngineeringDonghua UniversityShanghai201620China

Poly(aryl ether keton e)(PAEK) films with different crystallinities were obtained by controlling the cooling rate,which were subjected to the absorption and desorption of methylene chloride(CH_(2)Cl_(2)).We employed attenuated total reflection Fourier transform infrared(ATR-FTIR)spectroscopy analyses to investigate the diffusion behavior of CH_(2)Cl_(2) in PAEK films with different crystallinities.According to the Fickian diffusion model,the calculated diffu sion coefficients of CH_(2)Cl_(2) in PAEK films were observed to decrease with increasing crystallinity.The effect of CH_(2)Cl_(2)absorption and desorption on the mechanical properties of PAEK films with different crystallinity was further analyzed using tensile tests.The tensile tests exhibited that CH_(2)Cl_(2) has two concurrent effects:plasticization and solvent-induced crystallization.Differential scanning calorimetry(DSC) and wide-angle X-ray diffraction(WXRD) techniques further confirmed solvent-induced crystallization behavior.The results would be beneficial to understand the solvent resistance of PAEK materials and consequently provide the practical application conditions of PAEK with a theoretical basis.

关键词： Poly(aryl ether ketone) Diffusion behavior Infrared spectra Solvent-induced crystallization Mechanical properties

A breakthrough in fabric cleaning: coating-at-will concept for stainproof fabrics

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Science China Chemistry 2024年第3期67卷 744-745页

作者： Zhouyue Lei Peiyi Wu state key laboratory for modification of chemical fibers and polymer materials College of Chemistry and Chemical EngineeringDonghua UniversityShanghai 201620China

Surfactants are extensively used in daily life and industrial production, posing significant challenges to global sustainability. Household detergents, including dishwashing detergents and laundry, alone account for o... 详细信息

关键词： breakthrough proof coating

Highly Porous Yet Transparent Mechanically Flexible Aerogels Realizing Solar-Thermal Regulatory Cooling

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Nano-Micro Letters 2024年第7期16卷 231-243页

作者： Meng Lian Wei Ding Song Liu Yufeng Wang Tianyi Zhu Yue-EMiao Chao Zhang Tianxi Liu state key laboratory for modification of chemical fibers and polymer materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620People’s Republic of China key laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122People’s Republic of China

The demand for highly porous yet transparent aerogels with mechanical flexibility and solar-thermal dual-regulation for energy-saving windows is significant but challenging.Herein,a delaminated aerogel film(DAF)is fabricated through filtration-induced delaminated gelation and ambient drying.The delaminated gelation process involves the assembly of fluorinated cellulose nanofiber(FCNF)at the solid-liquid interface between the filter and the filtrate during filtration,resulting in the formation of lamellar FCNF hydrogels with strong intra-plane and weak interlayer hydrogen bonding.By exchanging the solvents from water to hexane,the hydrogen bonding in the FCNF hydrogel is further enhanced,enabling the formation of the DAF with intra-layer mesopores upon ambient drying.The resulting aerogel film is lightweight and ultra-flexible,which pos-sesses desirable properties of high visible-light transmittance(91.0%),low thermal conductivity(33 mW m^(-1) K^(-1)),and high atmospheric-window emissivity(90.1%).Furthermore,the DAF exhibits reduced surface energy and exceptional hydrophobicity due to the presence of fluorine-containing groups,enhancing its durability and UV resistance.Consequently,the DAF has demonstrated its potential as solar-thermal regulatory cooling window materials capable of simultaneously providing indoor lighting,thermal insulation,and daytime radiative cooling under direct sunlight.Significantly,the enclosed space protected by the DAF exhibits a temperature reduction of 2.6℃ compared to that shielded by conventional architectural glass.

关键词： Transparent aerogel Cellulose nanofiber aerogel Delaminated gelation Thermal insulation Passive daytime radiative cooling

Poly(3-hexylthio) thiophene Field-effect Transistor Device Performance: Impact of the Content of Hexylthio Side Chain on Backbone

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Chinese Journal of polymer Science 2024年第1期42卷 14-23,I0005页

作者： Hao-Yu Liu Lian-He Han Ling-Wei Kong Li-Ping Zhu Xiao-Lan Qiao Mei-Fang Zhu state key laboratory for modification of chemical fibers and polymer materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620China School of Electronic Information and Electrical Engineering Shanghai Jiao Tong UniversityShanghai 200240China

Regioregular poly(3-hexylthio)thiopene(P3HTT) has emerged tremendous potential in organic electronic applications due to the strong noncovalent interactions from the sulfur atom linked to thiophene. However, P3HTT generally exhibits low charge mobility mostly due to poor solution processability attributed to dense arrangement of hexylthio side chain in polymer, which led to strong noncovalent interactions among sulfur atoms. To balance the nonvalent interaction and aggregation for P3HTT, herein, we systematically study the effect of hexylthio side chain content in polymer backbone on the structure and properties. A series of regioregular P3HTT-based homopolymers(P3HTT, P3HTT-50,P3HTT-33 and P3HTT-25) were prepared via Kumada catalyst transfer polycondensation method from a set of mono-, bi-, ter-and quarterthiophenes containing different contents of hexylthio side chain. The DFT calculation shows the planarity of polymers backbone could be improved through reducing the density of hexylthio side chain in polymer mainchain. And significant changes in their crystallinity, aggregation and optical properties were observed with the content of hexylthio side chain reducing. The P3HTT-33 displayed the highest field-effect transistor hole mobility of 2.83×10^(-2) cm^(2)·V^(-1)·s^(-1) resulting from a balance between the crystallinity and planarity. This study demonstrates modulating the content of hexylthio side chain in P3HTT is an effective strategy to optimize the opto-electronic properties of polymer obtaining excellent semiconductor device performance.

关键词： Conjugated polymer Polythiophene Noncovalent interaction Molecular aggregation Organic field-effect transistor

A Radiative-Cooling Hierarchical Aligned Porous Poly(vinylidene fluoride)Film by Freeze-Thaw-Promoted Nonsolvent-Induced Phase Separation

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Chinese Journal of polymer Science 2024年第7期42卷 976-983,I0009页

作者： Yiting Zhang Jiahui Sun Yufeng Wang Yunchen Wu Chun Huang Chao Zhang Tianxi Liu key laboratory of Synthetic and Biological Colloids Ministry of Education School of Chemical and Material EngineeringJiangnan UniversityWuxi214122China state key laboratory for modification of chemical fibers and polymer materials College of Materials Science and EngineeringDonghua UniversityShanghai201620China

Passive daytime radiative cooling(PDRC)is an innovative and sustainable cooling technology that holds immense potential for addressing the energy crisis.Despite the numerous reports on radiative coolers,the design of a straightforward,efficient,and readily producible system remains a challenge.Herein,we present the development of a hierarchical aligned porous poly(vinylidene fluoride)(HAP-PVDF)film through a freeze-thaw-promoted nonsolvent-induced phase separation strategy.This film features oriented microporous arrays in conjunction with random nanopores,enabling efficient radiative cooling performance under direct sunlight conditions.The incorporation of both micro-and nano-pores in the HAP-PVDF film results in a remarkable solar reflectance of 97%and a sufficiently high infrared thermal emissivity of 96%,facilitating sub-environmental cooling at 18.3℃ on sunny days and 13.1℃ on cloudy days.Additionally,the HAP-PVDF film also exhibits exceptional flexibility and hydrophobicity.Theoretical calculations further confirm a radiative cooling power of 94.8 W·m^(-2)under a solar intensity of 1000W·m^(-2),demonstrating a performance comparable to the majority of reported radiative coolers.

关键词： Daytime radiative cooling Hierarchical porosity PVDF porous film Thermal insulation Nonsolvent-induced phase separation