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Heteroatom Substitution Strategy Modulates Thermodynamics Towards Chemically Recyclable Polyesters and Monomeric Unit Sequence by Temperature Switching

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Angewandte Chemie 2024年第24期136卷

作者： Da Zhang Xin Wang Zhengbiao Zhang Nikos Hadjichristidis State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China State Key Laboratory of Radiation Medicine and Protection Soochow University Suzhou 215123 China Polymer Synthesis Laboratory KAUST Catalysis Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology (KAUST) Thuwal 23955 Saudi Arabia Note: Prof. Nikos Hadjichristidis is an Honorary Visiting Professor at Soochow University.

In this paper, we proposed a heteroatom substitution strategy (HSS) in the δ -valerolactone (VL) system to modulate thermodynamics toward chemically recyclable polyesters. Three VL-based monomers containing different heteroatoms (M 1 (N), M 2 (S), and M 3 (O)), instead of C-5 carbon, were designed and synthesized to verify our proposed HSS. All three monomers undergo organocatalytic living/controlled ROP and controllable depolymerization. Impressively, the resulting P(M 1 ) achieved over 99 % monomer recovery under both mild solution depolymerization and high vacuum pyrolysis conditions without any side reactions, and the recycled monomers can be polymerized again forming new polymers. The systematic study of the relationship between heteroatom substitution and recyclability shows that introducing heteroatoms does change the thermodynamics of the monomers (Δ H p o , Δ S p o and T c values), thereby adjusting the polymerizability and depolymerizability. DFT calculations found that the introduction of heteroatoms adjusts the ring strain by changing the angular strain of the monomers, and the order of their angular strain (M 2 >M 1 >M 3 ) is consistent with the order of the experimentally obtained enthalpy change. Notably, the one-pot/one-step copolymerization of two of each of the three monomers enables the synthesis of sequence-controlled copolymers from gradient to random to block structures, by simply switching the copolymerization temperature.

关键词： heteroatom ring-opening polymerization chemically recyclable sequence-control polyesters

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Plasmonic metallic Bi-modified defective Bi 4 Ti 3 O 12 nanosheets with upward migrating electrons for efficient photocatalytic NO removal and NO 2 inhibition

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Chinese Chemical Letters 2025年

作者： Wenjie He Lin Jing Wendong Zhang Xing'an Dong Yan Zou Xin Liu Xin Lv Peng Chen Jiazhen Liao Xiao Zhang Rong Xiao Yuechang Wei Chongqing Polytechnic University of Electronic Technology Chongqing 401331 China Engineering Research Center for Waste Oil Recovery Technology and Equipment Ministry of Education Chongqing Technology and Business University Chongqing 400067 China Chongqing Key Laboratory of Green Synthesis and Application College of Chemistry Chongqing Normal University Chongqing 401331 China College of Physics and Electronic Engineering Chongqing Normal University Chongqing 401331 China State Key Laboratory of Heavy Oil Processing Key Laboratory of Optical Detection Technology for Oil and Gas China University of Petroleum Beijing 102249 China

The limited redox capability of photocatalysts often leads to harmful NO 2 byproduct formation during photocatalytic NO oxidation. Herein, Bi 4 Ti 3 O 12 nanosheets modified with plasmonic metallic bismuth and abundant oxygen vacancies were synthesized via an in-situ reduction method. The optimized catalyst (BTOR2, with a molar ratio of 40% NaBH 4 to Bi 4 Ti 3 O 12 ) achieved a maximum NO removal efficiency of 62.3%, significantly higher than pristine Bi 4 Ti 3 O 12 (40.5%) while minimizing NO 2 production. The results reveal that the synergistic effects of Bi's plasmonic resonance and oxygen vacancies enhanced visible light absorption and charge separation. The density functional theory (DFT) analysis showed electrons can transfer from Bi 4 Ti 3 O 12 to Bi, promoting O 2 activation to • O 2 - radicals. In-situ diffuse reflectance infrared fourier transform spectroscopy (DRIFTS) confirmed that light-induced H 2 O adsorption was strengthened, improving • OH radical generation. These radicals promoted the selective conversion of activated NO - to NO 3 - , rather than NO 2 . This work provides valuable insights for advancing research into efficient photocatalysts for air pollution control.

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Effects of Ni content on the cast and solid-solution microstructures of Cu-0.4wt% Be alloys

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International Journal of Minerals,Metallurgy and materials 2018年第6期25卷 641-651页

作者： Shuang-jiang He Yan-bin Jiang Jian-xin Xie Yong-hua Li Li-juan Yue Key Laboratory for Advanced Materials Processing of Ministry of Education Institute of Advanced Materials and Technology University of Science and Technology Beijing Beijing 100083 China Beijing Laboratory of Metallic Materials and Processing for Modern Transportation University of Science and Technology Beijing Beijing 100083 China CNMC Ningxia Orient Group Co. Ltd. Shizuishan 753000 China

The effects of Ni content（0–2.1wt%）on the cast and solid-solution microstructures of Cu-0.4wt%Be alloys were investigated,and the corresponding mechanisms of influence were *** results show that the amount of precipitated phase increases in the cast alloys with increasing Ni *** the Ni content is 0.45wt%or 0.98wt%,needle-like Be_（21）Ni_5 phases form in the grains and are mainly distributed in the interdendritic *** the Ni content is 1.5wt%or greater,a large number of needle-like precipitates form in the grains and chain-like Be_（21）Ni_5 and Be Ni precipitates form along the grain *** addition of Ni can substantially refine the cast and solid-solution microstructures of Cu-0.4wt%Be *** hindering effects of both the dissolution of Ni into the matrix and the formation of Be–Ni precipitates on grain-boundary migration are mainly responsible for refining the cast and solid-solution microstructures of Cu-0.4wt%Be *** Ni contents result in finer microstructures;however,given the precipitation characteristics of Be–Ni phases and their dissolution into the matrix during the solid-solution treatment,the upper limit of the Ni content is 1.5wt%–2.1wt%.

关键词： beryllium-copper alloys alloying Ni content microstJ-ucture solid-solution treatment

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Ultrathin nanobelts-assembled Chinese knot-like 3D TiO2 for fast and stable lithium storage

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Nano Research 2018年第4期11卷 2116-2128页

作者： Qili Wu Shiman He Xianfeng Yang Jingling Yang Gaoren Li Yuying Meng Shengfu Tong Liqiang Mai Mingmei Wu MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of Chemistry Sun Yat-Sen University Guangzhou 510275 China Analytical and Testing Center South China University of Technology Guangzhou 510640 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China

Nanostructured TiO2 has applications in solar cells, photocatalysts, and fast- charging, safe lithium ion batteries （LIBs）. To meet the demand of high-capacity and high-rate LIBs with TiO2-based anodes, it is important to fine-tune the nanoarchitecture using a well-controlled synthesis approach. Herein, we report a new approach that involves epitaxial growth combined with topotactic conversion to synthesize a unique type of three-dimensional （3D） TiO2 nano- architecture that is assembled by well-oriented ultrathin nanobelts. The whole nanoarchitecture displays a 3D Chinese knot-like morphology; the core consists of robust perpendicular interwoven nanobelts and the shell is made of extended nanobelts. The nanobelts oriented in three perpendicular [001]A directions facilitate Li＋ penetration and diffusion. Abundant anatase/TiO2-B interfaces provide a large amount of interfacial pseudocapacitance. A high and stable capacity of 130 mA.h.g-1 was obtained after 3,000 cycles at 10 A·g-1 （50 C）, and the high-rate property of our material was greater than that of many recently reported high-rate TiO2 anodes. Our result provides, not only a novel synthesis strategy, but also a new type of 3D anatase TiO2 anode that may be useful in developing long-lasting and fast-charging batteries.

关键词： three-dimensional （3D） nanoarchitectures ultrathin nanobelts TiO2 lithium ion storage ultrahigh rate battery

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Research on additive manufacturing and properties of Ni-Al-Cr medium-entropy alloy

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materials Today Communications 2025年 46卷

作者： Wang, Wei Wu, Dongting Yin, Haidong Zhu, Zihao Gao, Zhenhuan Nie, Liping Liu, Ying Zou, Yong Key Laboratory of Liquid-Solid Structural Evolution and Processing of Materials Ministry of Education Shandong University Shandong Jinan250061 China School of Materials Science and Engineering Shandong University Shandong Jinan250061 China State Key Laboratory of Clean and Efficient Turbomachinery Power Equipment Deyang618000 China School of Materials Science and Engineering Sichuan University Chengdu610065 China Shandong Engineering & Technology Research Center for Modern Welding Shandong University Jinan250061 China

This study utilized Cold Metal Transfer (CMT) technology to prepare manufactured Ni-Al-Cr medium-entropy alloy (MEA) samples through Wire Arc Additive Manufacturing (WAAM) in combination with self-made nickel-based flux-cored wire. The specimens in the manufactured condition were fabricated by cold metal transfer (CMT) deposition onto IN939 nickel-based superalloy substrates, followed by post-deposition annealing at 1273 K for 96 h. The wire arc additively manufactured Ni-Al-Cr MEA in the as-deposited condition exhibited a microstructure comprising γ phase, γ'-Ni₃Al phase, β-NiAl phase, α-Cr phase, and 14M phase, with a hardness of 431.0–455.2 HV0.2. However, it demonstrated brittle fracture behavior at 700 °C (tensile strength ∼ 400 MPa, elongation 1 %). After annealing at 1273 K for 96 h, the 14M phase disappeared while γ' and α-Cr phases coarsened, accompanied by recrystallization. The hardness decreased to 200–400 HV0.2, with the fracture mode transitioning to ductile fracture. Notably, the tensile strength significantly increased to 721.69–782.13 MPa, accompanied by enhanced elongation reaching 10.53–12.82 %. High-temperature wear tests revealed a transition from abrasive wear in the as-deposited state to adhesive wear after annealing, with both conditions exhibiting excellent wear resistance. © 2025

关键词： Brittle fracture

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Design of Ligand-Nonbridging Sites in Metal–Organic Frameworks for Boosting Lithium Storage Capacity

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Angewandte Chemie 2024年第6期137卷

作者： Lanju Sun Chongzhi Zhu Lukun Li Rumeng Zheng Jian Yuan Zhiliang Li Jikai Sun Guan Sheng Hao Wu Qingdao Engineering Research Center of Agricultural Recycling Economy Materials College of Chemistry and Pharmaceutical Sciences Qingdao Agricultural University 266109 Qingdao China Institute of Frontier Chemistry School of Chemistry and Chemical Engineering Shandong University 266237 Qingdao China Center for Electron Microscopy Institute for Frontier and Interdisciplinary Sciences State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology College of Materials Science and Engineering and College of Chemical Engineering Zhejiang University of Technology 310014 Hangzhou China School of Materials Science and Engineering State Key Laboratory of Heavy Oil Processing China University of Petroleum (East China) 266580 Qingdao China

Metal–organic frameworks (MOFs) are lagging in the use of lithium-ion batteries (LIBs), ascribing to full coordination between metal nodes and organic ligands, to a large extent. By integrating a modulator into a ligand with missing bridging functionality, this study elucidates the role of non-bridging defect sites in MOFs in tailoring lithium storage performance. A fully bridged pristine MOF (p-MOF) utilizing the meso-tetra(4-carboxylphenyl) porphyrin ligand is compared with a modified MOF containing non-bridging defects (d-MOF) introduced by a homologous ligand, tris(4-carboxyphenyl) porphyrin. Spectroscopic and cryogenic low-dose electron microscopy techniques verify the presence of non-bridging defect sites in the d-MOF and reveal their explicit local structure. Density functional theory calculations show significantly enhanced Li + adsorption energies and reduced Li + migration barriers at the non-bridging sites in the d-MOF compared to the fully bridging sites in the p-MOF. As a result, the d-MOF exhibits exceptional lithium storage performance, achieving a high capacity of 761 mAh g −1 at 0.05 A g −1 and superior rate performance of 203 mAh g −1 at 5 A g −1 , which substantially outperform the p-MOF. This study highlights the potential of modulating MOFs with non-bridging defects to develop high-performance LIBs.

关键词： Lithium storage Ligand engineering Defects Metal–organic frameworks Adsorption energy

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Electrospinning and electrospun nanofibers: From academic research to industrial production

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Progress in materials Science 2025年 154卷

作者： Wang, Ce Wang, Wei Qi, Hongxu Dai, Yunqian Jiang, Shaohua Ding, Bin Wang, Xianfeng Li, Congju Zeng, Jinfeng Wu, Tong Li, Haoyi Wang, Yuanfei Zhao, Yong Wang, Wenli Li, Zhenyu Mo, Xiumei Hou, Haoqing Dong, Lijie Ma, Hongyang Liu, Yong Su, Chunlei Bai, Jie Wu, Weiwei Guo, Gang Nie, Guangdi Wang, Nü Zhu, Han Bai, Jing Fang, Jian Liang, Daxin Ba, Zhichen Han, Guangping Lu, Xiaofeng Wang, Kaizhong Zhang, Xiaoyong Kang, Weimin Deng, Nanping Hu, Wei Chen, Weihua Zhang, Xiuling Yang, Dongzhi Wang, Fengyun Bian, Ye Liu, Zi'ang Zhang, Liang Li, Xiang Li, Lei Li, Yongxin Huang, Hui Jia, Xiaoteng Li, Xiaofeng Yang, Daxiang Jin, Xianchang Li, Shiyang Zhang, Xindan Tang, Nan Hao, Ruinan Tian, Feng Mai, Liqiang Wei, Yen Xue, Jiajia Alan G. MacDiarmid Institute Jilin University Changchun130012 China Harbin Institute of Technology Harbin150001 China Tsinghua University Beijing100084 China Southeast University Nanjing211189 China Nanjing Forestry University Nanjing210037 China Donghua University Shanghai201620 China Qingdao University Qingdao266071 China State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing100029 China Qingdao Stomatological Hospital Affiliated to Qingdao University Qingdao260001 China School of Chemistry Beihang University Beijing100191 China College of Textile and Clothing Engineering Jiangsu Engineering Research Center of Textile Dyeing and Finishing for Energy Conservation Discharge Reduction and Cleaner Production National Engineering Laboratory for Morden Silk Soochow University Suzhou215123 China Southwest Petroleum University Chegdu610500 China Jiangxi Normal University Nanchang330022 China Wuhan University of Technology Wuhan430070 China Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Inner Mongolia University of Technology Hohhot010051 China Xidian University Xian710071 China Sichuan University Chengdu610065 China Beihang University Beijing100191 China Jiangnan University Wuxi214122 China Northeast Forestry University Harbin150040 China Jilin University Changchun130012 China First Hospital of Jilin University Changchun130031 China Nanchang University Nanchang330031 China Tiangong University Tianjin300387 China Northeast Normal University Changchun130024 China Zhengzhou University Zhengzhou450001 China University of Science and Technology Beijing Beijing100083 China Co. Ltd. Chongqing404617 China Beijing Guo Wei Na Research Center for Fiber Materials Beijing China Shanghai University Shanghai200444 China South China University of Technology Guangzhou510006 China State Key Laboratory of Advanced Technology for Materials Synthesis and Pr

Electrospinning is a versatile and rapidly evolving technique that has gained significant attention for its ability to produce nanofibers with unique structures and properties. Over the past few decades, the scope of electrospun nanofibers has expanded from simple polymer fibers to more complex composites and ceramics, enabling a wide range of applications across fields such as environmental protection, biomedical engineering, energy storage, and smart materials. This review provides a comprehensive overview of recent advancements, covering material selection, process optimization, and innovative applications. We discuss the unique structural features of electrospun nanofibers, including their tunable diameters, porous architectures, and diverse compositions, which underpin their multifunctionality. key applications are highlighted in areas including environmental protection and safety, biomedical engineering, energy storage and conversion, and catalysis, as well as emerging uses in flexible electronics, advanced engineering materials, and textiles. Additionally, we review state-of-the-art characterization techniques and discuss the challenges and opportunities involved in scaling up industrial production. Finally, we offer a forward-looking perspective on the future of electrospun nanofibers, emphasizing the need for continued innovation in both academic research and commercial applications. © 2025 Elsevier Ltd

关键词： Medical applications

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Bifunctional o-CoSe 2 /c-CoSe 2 /MoSe 2 heterostructures for enhanced electrocatalytic and photoelectrochemical hydrogen evolution reaction

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materials Today Chemistry 2022年 23卷

作者： Y. Ji W. Luo Y. Liu Z. He N. Cheng Z. Zhang X. Qi J. Zhong L. Ren Hunan Key Laboratory of Micro-Nano Energy Materials and Devices Laboratory for Quantum Engineering and Micro-Nano Energy Technology Faculty of Materials and Optoelectronic Physics Xiangtan University Hunan 411105 PR China Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education Institutes of Physical Science and Information Technology Anhui University Hefei 230601 PR China Department of Materials Science and Engineering and Shenzhen Key Laboratory of Hydrogen Energy Southern University of Science and Technology Shenzhen 518055 PR China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 PR China

The bottleneck of alkaline hydrogen evolution reaction lies in the kinetically sluggish brought from multistep reaction processes involving water adsorption and dissociation, as well as hydrogen adsorption. In this work, we successfully synthesized o-CoSe 2 /c-CoSe 2 heterostructures anchored on MoSe 2 nanosheets to powerfully promote reaction processes. As an electrocatalyst, it exhibits a low overpotential of 112 mV at 10 mA/cm 2 and a Tafel slope of 96.9 mV/dec for an alkaline hydrogen evolution reaction. Moreover, the as-prepared catalyst can behave as both cathode and anode for overall water splitting, which only requires 1.61 V cell voltage at 10 mA/cm 2 . Significantly, the cell voltage can be further reduced to 1.53 V at 10 mA/cm 2 for water electrolysis under the simulated solar irradiation owing to such a semiconductor-based heterostructure that facilitates the separation of photogenerated charges. Here, the improving overall performance of this ternary electrocatalyst is attributed to the multifunctionality and synergistic interaction of different components in this heterogeneous material. The work provides a novel strategy to design active catalysts simultaneously using electric energy and solar energy for effective water splitting.

关键词： Transition-metal dichalcogenides Ternary hybrids Alkaline hydrogen evolution Photoelectrochemical water splitting

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On the Origin of Capacity Increase in Rechargeable Magnesium Batteries with Manganese Oxide Cathodes and Copper Metal Current Collectors

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Angewandte Chemie 2024年第5期137卷

作者： Zhao Li Yi Li Yang Zhan Xiaodong Lin Yingying Yao Tianshuo Zhao Fengzhan Sun Hao Xu Zhewen Ma Wei Zhang Yanling Xue Xiaolong Li Alexandru Vlad Jianxin Zou National Engineering Research Center of Light Alloy Net Forming State Key Laboratory of Metal Matrix Composite Center of Hydrogen Science School of Materials Science and Engineering Shanghai Jiao Tong University 200240 Shanghai China Institute of Condensed Matter and Nanosciences Université Catholique de Louvain B-1348 Louvain-la-Neuve Belgium Institute for Clean Energy & Advanced Materials School of Materials and Energy Southwest University 400715 Chongqing China State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals School of Materials Science and Engineering Lanzhou University of Technology 730050 Lanzhou China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences 201204 Shanghai China

Rechargeable magnesium batteries (RMBs), with Cu as positive electrode current collector (CC), typically display a gradual capacity increase with cycling. Whereas the origin of this was suggested in gradual active material electro-activation, the fact that this is prevalent in many positive electrode material systems remains unexplained. Herein, we elucidate the underlying mechanism through a series of multiscale joint operando X-ray characterizations, including operando synchrotron X-ray diffraction and imaging technology. We select a series of manganese oxides as benchmark positive electrodes and find that no magnesium ions are stored within the lattices of these materials, despite an apparent cell capacity increase with cycling. The origin of capacity increase is rooted in the gradual electrochemical corrosion of metallic Cu, release of Cu(I, II) species in electrolyte, and their subsequent redox activity, resulting in apparent electrode capacity gains. Furthermore, the shuttle and redox speciation of Cu ions trigger the irreversible depletion of both the Cu CC (or any other source) and the magnesium metal, ultimately leading to cell failure. Our work suggests the need to reconsider the appropriateness of using Cu as a positive electrode CC for RMBs.

关键词： Magnesium metal batteries synchrotron X-ray characterizations X-ray imaging operando X-ray characterizations copper current collector

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Regulating Crystallinity Mismatch Between Donor and Acceptor to Improve Exciton/Charge Transport in Efficient Organic Solar Cells

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Angewandte Chemie 2024年第11期136卷

作者： Prof. Dr. Xunfan Liao Mingtao Liu Hongqiao Pei Dr. Peipei Zhu Xinxin Xia Zeng Chen Yihan Zhang Zhongyuan Wu Dr. Yongjie Cui Dr. Guodong Xu Mengyuan Gao Prof. Dr. Long Ye Dr. Ruijie Ma Prof. Dr. Tao Liu Prof. Dr. Xinhui Lu Prof. Dr. Haiming Zhu Prof. Dr. Yiwang Chen Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education College of Chemistry and Chemical Engineering Jiangxi Normal University 99 Ziyang Avenue Nanchang 330022 China Department of Physics Chinese University of Hong Kong New Territories Kowloon Hong Kong 999077 China State Key Laboratory of Modern Optical Instrumentation Key Laboratory of Excited State Materials of Zhejiang Province Department of Chemistry Zhejiang University Hangzhou Zhejiang 310027 China School of Materials Science & Engineering Tianjin Key Laboratory of Molecular Optoelectronic Sciences Tianjin University Tianjin 300350 China Department of Electronic and Information Engineering Research Institute for Smart Energy (RISE) The Hong Kong Polytechnic University Hung Hom Kowloon Hong Kong China Guangxi Key Lab of Processing for Nonferrous Metals and Featured Materials Key Lab of New Processing Technology for Nonferrous Metals and Materials Ministry of Education School of Resources Environments and Materials Guangxi University Nanning 530004 China

Achieving a more balanced charge transport by morphological control is crucial in reducing bimolecular and trap-assisted recombination and enhancing the critical parameters for efficient organic solar cells (OSCs). Hence, a facile strategy is proposed to reduce the crystallinity difference between donor and acceptor by incorporating a novel multifunctional liquid crystal small molecule (LCSM) BDTPF4-C6 into the binary blend. BDTPF4-C6 is the first LCSM based on a tetrafluorobenzene unit and features a low liquid crystal phase transition temperature and strong self-assembly ability, conducive to regulating the active layer morphology. When BDTPF4-C6 is introduced as a guest molecule into the PM6 : Y6 binary, it exhibits better compatibility with the donor PM6 and primarily resides within the PM6 phase because of the similarity-intermiscibility principle. Moreover, systematic studies revealed that BDTPF4-C6 could be used as a seeding agent for PM6 to enhance its crystallinity, thereby forming a more balanced and favourable charge transport with suppressed charge recombination. Intriguingly, dual Förster resonance energy transfer was observed between the guest molecule and the host donor and acceptor, resulting in an improved current density. This study demonstrates a facile approach to balance the charge mobilities and offers new insights into boosting the efficiency of single-junction OSCs beyond 20 %.

关键词： organic solar cells crystallinity difference liquid crystal small molecule energy transfer tetrafluorobenzene

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