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Metal-organic frameworks with dinuclear metal centers for synergistically boosting CO2 photoreduction

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science China Chemistry 2025年第1期68卷 201-208页

作者： Hui-Feng Wang Wen-Jie Shi Yu-Xin Yang Bao-Xia Dong Tong-Bu Lu Di-Chang Zhong school of Chemistry and Chemical engineering Yangzhou University institute for New Energy materials and Low Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology

Dinuclear metal synergistic catalysis （DMSC） has been proved powerful in boosting CO2reduction,while this has not been achieved in heterogeneous catalysts with long-range order *** this study,we,by introduction of metal catalytic centers into an indium-based metal-organic framework （MOF）,obtained a series of isostructural In-MOFs,including three MOFs with mononuclear metal catalytic center （M-In）,three MOFs with dinuclear homometallic catalytic centers （MM-In）,and three MOFs with dinuclear heterometallic catalytic centers (MM’-In,M/M’=Co（II）,Ni（II）,Zn（II）).It was found that all these MOFs can serve as catalysts for photochemical CO2reduction to *** with M-In,the catalytic activities of MM-In were obviously enhanced,and that of MM’-In was further significantly *** example,the CO yield of Co Zn-In reaches a record value of 12,700μmol g-1h-1,which is 4.0,8.1,9.4,and 18.6-fold higher than that of Co Co-In,Zn Zn-In,Co-In,and Zn-In,***,the catalytic activities of Co Ni-In and Ni Zn-In also show different fold increase than those of corresponding dinuclear homometallic and mononuclear metallic *** results of control experiments and theoretical calculation reveal that the higher catalytic activities of MM-In over M-In can be ascribed to the DMSC effect,and the higher catalytic activity of MM’-In over MM-In can be ascribed to the strengthened DMSC *** work reveals the relationship between DMSC effect and bimetal centers in CO2reduction,which provides new insights into the DMSC and paves a new way to design highly active catalysts for photochemical CO2reduction.

关键词： metal-organic frameworks dinuclear metal centers synergistic catalysis CO2 reduction photocatalysis

Controlled cationic ring-opening polymerization of L-lactide by organic ion pair: novel approach to isotactic-rich and crystalline polylactide

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science China Chemistry 2025年第1期68卷 394-402页

作者： Zhiqiang Ding Mingqian Wang Zijing Zhou Bin Wang Yuesheng Li Tianjin Key Laboratory of Composite & Functional materials School of Materials Science and Engineering Tianjin University

Living/controlled cationic ring-opening polymerization （ROP） of L-lactide is a promising approach to isotactic-rich and crystalline poly（L-lactide）.In contrast with the unsubstituted lactones,L-LA can not be polymerized by organic Lewis acids or carbenium ions,and the state of the art in this field is the cationic ROP of L-LA catalyzed by Br?nsted acid/alcohol system via activated monomer ***,we reported the first example of controlled cationic ROP of L-LA by using Meerweintype ion pair[Me3O]+[B（C6F5）4]-as the catalyst.[Me3O]+[B（C6F5）4]-promoted rapid L-LA cationic polymerization in the absence of alcohol,producing isotactic-rich and crystalline PLLA without transesterification and epimerization side *** activated chain end mechanism,involving twice SN2 substitution and configuration-inversion （S→R→S） with the assistance of released Me2O,was proposed and further verified by density functional theory and control *** work expands the catalytic toolbox of isotactic-rich and crystalline polylactide *** represents a unique example of cationic-controlled polymerization of L-LA catalyzed by an organic ion pair.

关键词： organic ion pair controlled cationic ring-opening polymerization activated chain end mechanism isotactic-rich polylactide

“One stone, two birds”: Salt template enabling porosity engineering and single metal atom coordinating toward high-performance zinc-ion capacitors

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Journal of Energy Chemistry 2025年第1期100卷 637-645页

作者： Chunliu Zhu Huanyu Liang Ping Li Chenglong Qiu Jingyi Wu Jingwei Chen Weiqian Tian Yue Zhu Zhi Li Huanlei Wang school of materials science and engineering Ocean University of China Department of Chemical and materials engineering University of Alberta

Zinc-ion hybrid capacitors （ZIHCs） have received increasing attention as energy storage devices owing to their low cost,high safety,and environmental ***,their progress has been hampered by low energy and power density,as well as unsatisfactory long-cycle stability,mainly due to the lack of suitable electrode *** this context,we have developed manganese single atoms implanted in nitrogen-doped porous carbon nanosheets （MnSAs/NCNs） using a metal salt template method as cathodes for *** metal salt serves a dual purpose in the synthesis process:It facilitates the uniform dispersion of Mn atoms within the carbon matrix and acts as an activating agent to create the porous *** applied in ZIHCs,the MnSAs/NCNs electrode demonstrates exceptional performance,including a high capacity of 203 m Ah g-1,an energy density of 138 Wh kg-1at 68 W kg-1,and excellent cycle stability with 91%retention over 10,000 *** calculations indicate that the introduced Mn atoms modulate the local charge distribution of carbon materials,thereby improving the electrochemical *** work demonstrates the significant potential of carbon materials with metal atoms in zinc-ion hybrid capacitors,not only in enhancing electrochemical performance but also in providing new insights and methods for developing high-performance energy storage devices.

关键词： Zinc ion hybrid capacitors Cathodes Carbon materials Heteroatoms Single atoms

Electrocatalytic nitrite reduction to ammonia on isolated bismuth alloyed ruthenium

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Journal of Energy Chemistry 2025年第1期100卷 369-376页

作者： Shiyao Shang Fuzhou Wang Zeyi Sun Chaofan Qiang Ke Chu school of materials science and engineering Lanzhou Jiaotong University

Electrochemical reduction of NO2-to NH3（NO2-RR） is recognized as an appealing approach for achieving renewable NH3synthesis and waste ***,we report isolated Bi alloyed Ru （Bi1Ru） as an efficient NO2-RR *** calculations and in situ electrochemical measurements reveal the creation of Bi1-Ru dual sites which can remarkably promote NO2-activation and suppress proton adsorption,while accelerating the NO2-RR protonation energetics to render a high NO2--to-NH3conversion ***,Bi1Ru assembled in a flow cell delivers an NH3yield rate of 1901.4μmol h-1cm-2and an NH3-Faradaic efficiency of 94.3%at an industrial-level current density of 324.3 mA *** study offers new perspectives for designing and constructing p-block single-atom alloys as robust and high-current-density NO2-RR catalysts toward the ammonia electrosynthesis.

关键词： Ammonia

Thickness and sp3 bond modulation of（Ti/tetrahedral amorphous carbon）_n multilayer coatings

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Tungsten 2025年第1期7卷 152-160页

作者： Zhi-Jun Xie Jia-Lin Li Ling Gong Xiang-Li Zhong Hong-Jia Song Jin-Bin Wang National-Provincial Laboratory of Special Function Thin Film materials School of Materials Science and Engineering Xiangtan University

The durability of wear-resistant tetrahedral amorphous carbon（ta-C） coatings is intimately linked to their thickness and the concentration of *** enhance the lifespan of the coatings,we have prepared a multilayer coating consisting of alternating layers of Ti and ta-C,denoted as（Ti/ta-C）_n,using arc ion plating.A multi-layer structure in conjunction with stage cooling is employed to enhance the thickness and promote *** results indicate that the ID/IGvalue,representing the ratio of the intensity of the D peak to that of the G peak in Raman spectroscopy,decreases from 0.85 when no stage cooling is applied to 0.35 when stage cooling is employed,suggesting an enhancement in the fraction of sp3bonds within the *** obtained（Ti/ta-C）_n multilayer coating without peeling off has a maximum thickness of 1.14 μm,which is almost double that of the ta-C coating single layer *** the same time,the coating has a low coefficient of friction,down to 0.069,and maintains excellent friction properties with a wear rate of 3.4×10-6mm3·N-1·*** results conclusively show that the preparation technology can enhance both thickness and sp3bonding in ta-C coatings,significantly expanding their utility across tools,molds,and precision engineering components.

关键词： Arc ion plating Multilayer structure sp3 bond Ta-C coating Wear resistance

Highly conductive and stable iodine doped argyrodite electrolyte for all-solid-state lithium batteries

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Journal of Energy Chemistry 2025年第1期100卷 50-58页

作者： Gaozhan Liu Jing Zhang Jing Yang Jinghui Chen Xingyue Xiao Xiayin Yao Ningbo institute of materials Technology and engineering Chinese Academy of Sciences Center of materials science and Optoelectronics engineering University of Chinese Academy of Sciences

Lithium argyrodites with high ionic conductivity and low cost are considered as one of the most prospective solid electrolytes for all-solid-state lithium ***,the poor chemical stability and compatibility with lithium metal limit their ***,Li5.4PS4.4Cl1.4I0.2solid electrolyte with high ionic conductivity of 11.49 m S cm-1and improved chemical stability is synthesized by iodine *** ultra-thin Li5.4PS4.4Cl1.4I0.2membrane with thickness of 10μm can be obtained by wet coating process,exhibiting a high ionic conductivity of 2.09 mS cm-1and low areal resistance of 1.17Ω***,iodine doping could in-situ form LiI at the lithium/electrolyte interface and improve the critical current density of Li5.4PS4.4Cl1.6from 0.8 to 1.35 mA *** resultant LiCoO2/Li5.4PS4.4Cl1.4I0.2/Li battery shows excellent cycling stability at 1 C,with a reversible specific capacity of 110.1 mA h g-1and a retention of 80.5% after 1000 *** addition,the assembled LiCoO2/Li5.4PS4.4Cl1.4I0.2membrane/Li pouch cell delivers an initial discharge capacity of 110.4 mA h g-1and 80.5% capacity retention after 100 cycles.

关键词： Solid-State Batteries

Dielectric-ion-conductive ZnNb2O6 layer enabling rapid desolvation and diffusion for dendrite-free Zn metal batteries

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Journal of Energy Chemistry 2025年第1期100卷 693-701页

作者： Haifeng Yang Jian Wang Panpan Zhang Xiaomin Cheng Qinghua Guan Jing Dong Bixian Chen Lujie Jia Jing Zhang Yongzheng Zhang Yunjian Liu Hongzhen Lin school of materials science and engineering Jiangsu University i-Lab & CAS Key Laboratory of Nanophotonic materials and Devices Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences Helmholtz institute Ulm (HIU) Karlsruhe institute of Technology (KIT) school of materials science and engineering Xi'an University of Technology State Key Laboratory of Chemical engineering East China University of Science and Technology

Rechargeable aqueous zinc-metal batteries （AZMBs） are promising candidates for large-scale energy storage systems due to their low cost and high ***,their performance and sustainability are significantly hindered by the sluggish desolvation kinetics at the electrode/electrolyte interface and the corresponding hydrogen evolution reaction where active water molecules tightly participate in the Zn（H2O）62+solvation ***,learnt from self-generated solid electrolyte interphase （SEI） in anodes,the dielectric but ion-conductive zinc niobate nanoparticles artificial layer is constructed on metallic Zn surface （ZNB@Zn）,acting as a rapid desolvation *** zincophilic and dielectric-conductive properties of ZNB layer accelerate interfacial desolvation/diffusion and suppress surface corrosion or dendrite formation,achieving uniform Zn plating/stripping behavior,as confirmed by electronic/optical microscopies and interface spectroscopical measurements together with theoretical ***,the as-prepared ZNB@Zn electrode exhibits excellent cycling stability of over 2000 h and robust reversibility （99.54%） even under high current density and depth of discharge ***,the assembled ZNB@Zn-based full cell displays high capacity-retention rate of 80.21%after 3000 cycles at 5 A g-1and outstanding rate performance up to 10 A *** large-areal pouch cell is stabilized for hundreds of cycles,highlighting the bright prospects of the dielectric but ion-conductive layer in further application of AZMBs.

关键词： Zn metal battery Dielectric artificial layer Rapid ion diffusion Zincophilic diffusion Active water inhibition

Preparation of Modified Composite Nanofiltration Membrane Synergistically Using Carboxylic Multi- walled Carbon Nanotube and β-cyclodextrin

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Journal of Wuhan University of Technology(materials science) 2025年第1期40卷 232-239页

作者： LIU Peng MAO Junpeng FANG Yanfeng YU Yunwu CHEN Changxiu TANG Ning WAN Ye GU Yaxin LIU Yunxue WANG Lihua school of materials science and engineering Shenyang Jianzhu UniversityShenyang 110168China

A new modified blend ultrafiltration(UF)membrane with good hydrophilicity,high porosity and excellent anti-fouling performance was developed by using carboxylic multi-walled carbon nanotube(CMWCNT)as casting solution ***,a composite nanofiltration(NF)membrane with large water flux and good retention rate was fabricated by using the PVDF/CMWCNT blend UF membrane as the substrate,and polyvinyl alcohol(PVA),β-cyclodextrin(β-CD)and polyethylenimine(PEI)as the coating *** results show that with the appropriate addition of CMWCNT in the casting solution,the surface roughness,porosity and recovery rate of the PVDF/CMWCNT blend UF membrane is obviously *** water flux of blend UF membrane is significantly improved when the CMWCNT content increases from 0 wt%to 0.2 wt%.The water flux of blend UF membrane with 0.2 wt%CMWCNT is 162.7 L/(m^(2)·h),which is 44.3%higher than that of the pure PVDF ***β-CD content is 0.8 wt%,the retention rate of Congo red by PVDF/CMWCNT/β-CD composite NF membrane reaches 98.7%,which is 28.3%higher than that of single PVA/PEI modified *** research will provide a new idea and simple method for developing novel high-performance composite NF membranes.

关键词： CMWCNT cyclodextrin nanofiltration membrane

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Mainchain conformation ordering self-assembly tailored room temperature phosphorescence emission

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science China Chemistry 2025年第1期68卷 329-336页

作者： Yuzhu Li Yumeng Gao Feng Tian Yu Wang Yuan Yao Shaoliang Lin Xiang Ma Binbin Xu Shanghai Key Laboratory of Advanced Polymeric materials Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Key Laboratory for Advance materials and Feringa Noble Prize Scientist Joint Research Centre Frontiers Science for Materiobiology and Dynamic Chemistry School of Chemistry and Molecular Engineering East China University of Science & Technology

Developing organic room-temperature phosphorescence （RTP） materials with a wide range of tunable-emission is significant in expanding the applications of RTP ***,we rationally designed amphiphilic alternating copolymers poly(1,2-bis（4-alkoxyphenyl）ethane-1,2-dione-alt-（ethylene glycol）x)(P（Bz-alt-EGx）) that combined the advantage of alternating benzil and EGxskeleton,and tunable mainchain *** a mainchain conformation ordering assembly （COA） process,P（Bz-alt-EGx） self-assembled into well-defined platelets,and such assemblies emitted blue RTP at ca.425 nm due to the ordered folded-chain conformation and confined *** contrast,traditional self-assembly （TA） of P（Bz-alt-EGx） obtained less ordered aggregates,such as asymmetric worms,vesicles,and rod-like *** resultant less ordered aggregates exhibited yellow-green RTP at ca.550 *** wide-tuning RTP emission in solution （between blue and yellow-green,over125 nm） is realized using the P（Bz-alt-EGx） alternating copolymers under the treatment of different self-assembly *** study uncovers a new strategy to tailor the RTP emission through different self-assembly pathways and holds great promise for the fabrication of advanced optical materials.

关键词： self-assembly conformation ordering alternating copolymer phosphorescence emission