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Two-Orders-of-Magnitude Enhancement of Photoinitiation Activity via a Simple Surface Engineering of Metal Nanoclusters

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Angewandte Chemie 2024年第23期136卷

作者： Jin Tang Ning Xu An Ren Prof. Liang Ma Prof. Wenwu Xu Prof. Zhongkang Han Zijie Chen Prof. Qi Li Ministry of Education Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou 310058 China authors contributed equally to this work School of Materials Science and Engineering Zhejiang University Hangzhou 310058 China Department of Physics School of Physical Science and Technology Ningbo University Ningbo 315211 China The State Key Laboratory of Fluid Power and Mechatronic Systems. School of Mechanical Engineering Zhejiang University Hangzhou 310058 China

Development of high-performance photoinitiator is the key to enhance the printing speed, structure resolution and product quality in 3D laser printing. Here, to improve the printing efficiency of 3D laser nanoprinting, we investigate the underlying photochemistry of gold and silver nanocluster initiators under multiphoton laser excitation. Experimental results and DFT calculations reveal the high cleavage probability of the surface S−C bonds in gold and silver nanoclusters which generate multiple radicals. Based on this understanding, we design several alkyl-thiolated gold nanoclusters and achieve a more than two-orders-of-magnitude enhancement of photoinitiation activity, as well as a significant improvement in printing resolution and fabrication window. Overall, this work for the first time unveils the detailed radical formation pathways of gold and silver nanoclusters under multiphoton activation and substantially improves their photoinitiation sensitivity via surface engineering, which pushes the limit of the printing efficiency of 3D laser lithography.

关键词： Gold Nanocluster Silver Nanocluster 3D Nanoprinting Photoinitiator Photochemistry

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One-Pot Construction of Sulfur-Rich Thermoplastic Elastomers Enabled by Metal-Free Self-Switchable Catalysis and Air-Assisted Coupling

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Angewandte Chemie 2021年第7期134卷

作者： Xiao-Feng Zhu Guan-Wen Yang Rui Xie Guang-Peng Wu MOE Key Laboratory of Macromolecular Synthesis and Functionalization Key Laboratory of Adsorption and Separation Materials and Technologies of Zhejiang Province Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China

Construction of well-defined sulfur-rich macromolecules in a facile manner is an interesting but challenging topic. Herein, we disclose how to readily construct well-defined triblock sulfur-rich thermoplastic elastomers via a self-switchable isothiocyanate/episulfide copolymerization and air-assisted oxidative coupling strategy. During self-switchable polymerization, alternating copolymerization of isothiocyanate and episulfide occurs initially due to the lower energy barrier for isothiocyanate insertion with respect to successive episulfide ring-opening. After exhaustion of isothiocyanate, ring-opening polymerization of episulfide begins, providing diblock polymers. Subsequent exposure of the reaction to air leads to a transformation of diblock copolymers into triblock thermoplastic elastomers. This protocol can be extended to diverse isothiocyanates and episulfides, allowing fine-tuning of the performance of the produced sulfur-rich thermoplastic elastomers.

关键词： Block copolymers Ring-opening copolymerization Self-switchable polymerization Sulfur-rich polymers Thermoplastic elastomers

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Robust and Sensitive Sensing of Unsteady Flows Using a Hair-Like Macroscopic Graphene Fiber

Robust and Sensitive Sensing of Unsteady Flows Using a Hair-...

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IEEE International Conference on Micro Electro Mechanical Systems

作者： Binpeng Zhan Bo Fang Srikrishna C. Bodepudi Zhen Xu Jiahuan Cui Yang Xu Chao Gao Huan Hu School of Mechanical Engineering Zhejiang University MOE Key Laboratory of Macromolecular Synthesis and Functionalization Zhejiang University College of Information Science and Electronic Engineering Zhejiang University ZJUI Institute Zhejiang University International Campus Hangzhou China

ISBN: (数字)9781728135816

ISBN: (纸本)9781728135823

This paper reports a bio-inspired miniaturized hair-cell flow sensor using a novel material-graphene fiber (GF). We demonstrate that GF can be bent into an arc-shape and stick out of air flow boundary layer for velocity measurement. Air flow velocities ranging from 0.6 to 3.2m/s are generated to characterize the measurement sensitivity. It is found that flow velocity as low as 0.06m/s can be detected by the GF-based hair-cell sensor. Moreover, to measure the dynamic response of the GF-sensor, a periodic unsteady flow is generated by a single blade fan. The dominant frequency, i.e. the fan rotating frequency, has been clearly captured by the GF-based hair-cell sensor. This GF-based hair-cell sensor shows great promise in detecting small air flow and can be implemented in an array form on wings of small/micro flying vehicles for providing crucial aerodynamic flow field information on wings.

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Chemically Recyclable Polyethylene-like Sulfur-Containing Plastics from Sustainable Feedstocks

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Angewandte Chemie 2023年第13期135卷

作者： Yanni Xia Xinchen Yue Yue Sun Chengjian Zhang Xinghong Zhang MOE Key Laboratory of Macromolecular Synthesis and Functionalization International Research Center for X Polymers Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China Center of Chemistry for Frontier Technologies Zhejiang University Hangzhou 310027 China Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering Hangzhou 310027 China

The green revolution in plastics should be accelerated due to growing sustainability concerns. Here, we develop a series of chemically recyclable polymers from the first reported cascade polymerization of H 2 O, COS, and diacrylates. In addition to abundant feedstocks, the method is efficient and air-tolerant, uses common organic bases as catalysts, and yields polymers with high molecular weights under mild conditions. Such polymers, structurally like polyethylene with low-density in-chain polar groups, manifest impressive toughness and ductility comparable to high-density polyethylene. The in-chain ester group acts as a breaking point, enabling these polymers to undergo chemical recycling through two loops. The structures and properties of these polymers also have an immeasurably expanded range owing to the versatility of our method. The readily available raw materials, facile synthesis, and high performance make these polymers promising prospects as sustainable materials in practice.

关键词： Plastic Recycling Polyester Polymer synthesis Recyclable Polymers Sustainable Polymers

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A twin-track therapeutic strategy for massive rotator cuff tears based on robust and piezoelectric nanocomposite hydrogel films

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Chemical Engineering Journal 2025年 518卷

作者： Jiajie Wang Jiacheng Dai Dejin Jiao Jinghua Fang Kaiwang Xu Tengjing Xu Xinning Yu Kaijie Qiu Yuting Zhong Hongyun Song Sunan Zhu Siheng Wang Zongyou Pan Zi Liang Wu Xuesong Dai Department of Orthopedic Surgery Second Affiliated Hospital School of Medicine Zhejiang University Hangzhou 310009 China Orthopedics Research Institute of Zhejiang University Hangzhou 310009 China Zhejiang Key Laboratory of Motor System Disease Precision Research and Therapy Hangzhou 310009 China Clinical Research Center of Motor System Disease of Zhejiang Province Hangzhou 310009 China Ministry of Education Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou 310058 China

The high retear rate after massive rotator cuff tear (MRCT) repair is a significant roadblock that trouble both patients and doctors. Compared with traditional surgery, MRCT bridging repair with fascial autografts has great potential. However, the underlying risk of graft failure due to stretching and deformation during the postoperative stage is a grand challenge for its further use. In this study, we prepared robust, antimicrobial, and piezoelectric nanocomposite hydrogel films and used them for MRCT bridging repair with fascial autografts. The double-network structured nanocomposite hydrogel gel films consisting of ChNF and AA incorporate excellent mechanical properties (≈166 MPa) and remarkable antibacterial capacity. These properties ensure the gel films sustain long-term cyclic stretching and improve the anti-fatigue performance of fascial autografts. Besides, the composite gels with weakly-charged polyacrylic acid network exhibit appropriate piezoelectric behaviors, which generates electric stimulation and promotes tenogenic differentiation in vitro. Furthermore, compared to autografts alone, the combination of the nanocomposite gel films with fascial autografts shows more satisfactory results in a rabbit MRCT model, among which piezoelectric hyper-strong gels are superior to merely robust gels. This work demonstrates use of a robust, piezoelectric and antibacterial material to provide a twin-track therapeutic strategy to achieve mechanical reconstruction and biological regeneration synergistically, paving the new way to management for MRCT.

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Special topic on organic and perovskite photovoltaics

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Science China Chemistry 2019年第7期62卷 797-799页

作者： Hongzheng Chen Yongfang Li Alex K.-Y. Jen State Key Laboratory of Silicon Materials Key Laboratory of Macromolecular Synthesis and Functionalization (Ministry of Education) Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China Laboratory of Advanced Optoelectronic Materials College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China Department of Materials Science and Engineering University of Washington Seattle WA 98195 USA Department of Chemistry and Department of Materials Science & Engineering City University of Hong Kong Kowloon 999077 Hong Kong China

Photovoltaics, as a green technology for converting solar energy into electricity, have shown great promise to address the energy and environmental challenges for the sustainability of human society. In recent years, two types of photovoltaics, consisting of organic semiconductors or perovskites as light absorbers, have experienced a rapid development. The development of organic solar cells (OSC) can be dated back to 1986, since the discovery of a bi layer OSC by Di. C. W. Tang. Nowadays, OSCs made with polymer donors and small molecule acceptors have surpassed power conversion efficiencies (PCEs) of 16% for single-junction and 17% for tandem devices, through integrated innovative efforts on materials, interfaces, and device architectures.

关键词： perovskite photovoltaics electricity environmental challenges

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Insights into the Distinct Behaviors between Bifunctional and Binary Organoborane Catalysts through Terpolymerization of Epoxide, CO2, and Anhydride

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Angewandte Chemie 2024年第27期136卷

作者： Rui Xie Yuhui Wang Shuai Li Bo Li Jie Xu Jinqian Liu Yuchen He Guan-Wen Yang Guang-Peng Wu MOE Key Laboratory of Macromolecular Synthesis and Functionalization Key Laboratory of Adsorption and Separation Materials & Technologies of Zhejiang Province Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 Zhejiang P. R. China College of Material Chemistry and Chemical Engineering Key Laboratory of Organosilicon Chemistry and Material Technology Ministry of Education Hangzhou Normal University Hangzhou 311121 Zhejiang P. R. China Shaanxi Coal Chemical Industry Technology Research Institute Co. Ltd. Xi'an 710100 Shaanxi P. R. China

Alkyl borane compounds-mediated polymerizations have expanded to Lewis pair polymerization, free radical polymerization, ionic ring-opening polymerization, and polyhomologation. The bifunctional organoborane catalysts that contain the Lewis acid and ammonium or phosphonium salt in one molecule have demonstrated superior catalytic performance for ring-opening polymerization of epoxides and ring-opening copolymerization of epoxides and CO 2 than their two-component analogues, i.e., the blend of organoborane and ammonium or phosphonium salt. To explore the origin of the differences of the one-component and two-component organoborane catalysts, here we conducted a systematic investigation on the catalytic performances of these two kinds of organoborane catalysts via terpolymerization of epoxide, carbon dioxide and anhydride. The resultant terpolymers produced independently by bifunctional and binary organoborane catalyst exhibited distinct microstructures, where a series of gradient polyester-polycarbonate terpolymers with varying polyester content were afforded using the bifunctional catalyst, while tapering diblock terpolymers were obtained using the binary system. The bifunctional catalyst enhances the competitiveness of CO 2 insertion than anhydride, which leads to the premature incorporation of CO 2 into the polymer chains and ultimately results in the formation of gradient terpolymers. DFT calculations revealed the role of electrostatic interaction and charge distribution caused by intramolecular synergistic effect for bifunctional organoborane catalyst.

关键词： organoborane bifunctional catalysts ring-opening polymerization copolymerization block copolymer

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Graphene fiber based supercapacitors:Strategies and perspective toward high performances

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Journal of Energy Chemistry 2018年第1期27卷 6-11页

作者： Qiuyan Yang Zhen Xu Chao Gao MOE Key Laboratory of Macromolecular Synthesis and Functionalization.Department of Polymer Science and Engineering Key Laboratory of Adsorption and Separation Materials&Technologies of Zhejiang Province.Zhejiang UniversityHangzhou 310027Zhejiang.China

Modern wearable electronics are thirsty for flexible, lightweight energy storage and supply devices. Flexible fiber-shaped supercapacitors, possess good flexibility, high power density, fast charging capability and long cycle life, becoming a promising option for wearable devices. The past decade has witnessed the emergence of graphene fiber based supercapacitors（GFSCs） as one of the most active vicinity in fiber-supercapactiors, for their excellent properties including high surface area, chemical stability, excellent electrical conductivity, lightweight and mechanical properties. In this perspective, we introduced the basic energy storage mechanisms of GFSCs, followed by the analysis in improving their overall performances, recent advances, and a conclusive discussion on the challenges and opportunities.

关键词： Graphene Fiber Two-dimensional materials Supercapacitors Energy storage

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Long-acting glucose-responsive insulin with swift onset-of-action

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Journal of Controlled Release 2025年 383卷 113826页

作者： Liu, Wei Zhang, Juan Wang, Yanfang He, Yaqin Wang, Yuanwu Wei, Xiangqian Yao, Yuejun Xu, Jianchang Zhang, Wentao Sheng, Tao Dai, Haibin Wang, Jinqiang Gu, Zhen State Key Laboratory of Advanced Drug Delivery and Release Systems School of Pharmacy Zhejiang University Hangzhou310058 China Jinhua Institute of Zhejiang University Jinhua321299 China Department of Pharmacy Second Affiliated Hospital Zhejiang University School of Medicine Hangzhou310009 China Department of General Surgery Sir Run Run Shaw Hospital School of Medicine Zhejiang University Hangzhou310016 China Liangzhu Laboratory Hangzhou311121 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou310027 China

Long-acting glucose-responsive insulin is anticipated to reduce the frequency of injections via replacing both rapid-acting and long-acting insulin. Sequential rapid glucose-responsive insulin release and instant absorption are essential to the swift onset of action. Herein, we have developed injectable long-acting glucose-responsive insulin formulations (GRIF) prepared from glucosamine-modified insulin aspart (ASP-Gn) and phenylboronic acid-modified poly-ʟ-lysine (PLL-FPBA). The complex can form stable GRIF reservoir subcutaneously after injection. Upon food intake, the elevated blood glucose (BG) triggers the release of monomolecular insulin aspart (or ASP-Gn), which can be absorbed immediately to downregulate BG back to the normal range. Among the diverse formulations investigated, GRIF prepared from two-glucosamine-modified insulin aspart and twice weight of PLL-FPBA facilitates the best in vitro glucose-responsive insulin release performance. In type 1 diabetic mouse and minipig models, GRIF exhibit notably swift onset of action and achieve superior BG control. In addition, GRIF reveal no discernible signs of associated toxicity in the studied animals. © 2025 Elsevier B.V.

关键词： Glucose

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Investigation of anisotropic thermophysical properties of highly oriented carbon fiber composites: From one to three dimensions

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Carbon 2025年 243卷

作者： Yanhui Zhang Jie Yang Xiaoyu Zhang Rui Xu Minsu Liu Aoran Fan Yingjun Liu Jianli Wang Xing Zhang Jiangsu Key Laboratory for Design and Manufacturing of Precision Medicine Equipment Department of Mechanical Engineering Southeast University Nanjing 210096 China Key Laboratory for Thermal Science and Power Engineering of Ministry of Education Department of Engineering Mechanics Tsinghua University Beijing 100084 China Monash Suzhou Research Institute Monash University Suzhou 215000 China ARC Research Hub for Smart Process Design and Control School of Chemical and Biological Engineering Monash University Clayton VIC 3800 Australia MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Key Laboratory of Adsorption and Separation Materials & Technologies of Zhejiang Province Zhejiang University 38 Zheda Road Hangzhou 310027 China

Highly oriented carbon fiber composites exhibit three-dimensional anisotropic thermophysical properties, making them candidates for thermal management applications. In this study, the thermal properties of highly oriented carbon fiber/epoxy resin (CF/ER) composites and their components were systematically investigated. The T-type probe method was employed to measure the pitch CF, while the 2ω method and the laser-spot-periodic-heating method were combined to characterize the E51-ER film and the composites. The impact of local fiber bending on heat transfer in the composites was also analyzed through finite element simulations. The results show that these composites exhibit high thermal conductivity along the fiber orientation with an anisotropy ratio of about 294. At different temperatures, the thermal conductivity along the fiber orientation is lower than the value predicted by the parallel model, while the conductivity in the other two directions is significantly higher than that predicted by the series model. Simulation results suggest that the bending of certain pitch CF can be a key factor contributing to this discrepancy.

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