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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

Constructing Pr-doped CoOOH catalytic sites for efficient electrooxidation of 5-hydroxymethylfurfural

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Journal of Energy Chemistry 2025年第1期100卷 234-244页

作者： Botao Fan Hao Zhang Bang Gu Feng Qiu Qiue Cao Wenhao Fang school of Chemical science and technology Yunnan University National Center for International Research on Photoelectric and Energy materials School of Materials and Energy Yunnan University

Electrocatalytic conversion of renewable biomass is emerging as a promising route for sustainable chemical production;hence it urgently calls for developing efficient electrocatalysts with low potentials and high current ***,a Pr-doped Co（OH）2hexagonal sheet （Pr/Co=1/9,in mole） is synthesized by electrodeposition as highly performant catalyst for 5-hydroxymethylfurfural （HMF） oxidation reaction（HMFOR） to produce 2,5-furandicarboxylic acid （FDCA）.This novel and low-cost catalyst possesses a rather low onset potential of 1.05 V （***） and requires only 1.10 V （***） to reach a current density of 10 mA cm-2for HMFOR,significantly outperforming Co（OH）2benchmark (i.e.,210 mV higher to reach10 m A cm-2).The origin of Pr promotion effect as well as the evolution of CoOOH catalytic sites and HMFOR process has been deeply elucidated by physical characterizations,kinetic experiments,in situ electrochemical techniques,and theoretical *** unique Pr-ameliorated CoOOH active centers enable 100%conversion of HMF,99.6%selectivity of FDCA,and 99.7%Faraday efficiency,with a superior cycling durability toward *** can be one of the most outstanding results for Co-based HMFOR catalysts to date in the *** this work can help open up new horizons for constructing novel and efficient Co-based electrocatalysts by the utilization of lanthanide elements.

关键词： Bioconversion

Universal design of three-dimensional porous graphene-iron based promotors for kinetically rationalized lithium-sulfur chemistry

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Journal of Energy Chemistry 2025年第1期100卷 192-200页

作者： Hua Gao Yunfeng Zhang Menglei Wang Ruoxuan Yang Shuai Feng Xuan Cao Yaping Zhang Zhongyuan Lu Yingze Song State Key Laboratory of Environment-Friendly Energy materials School of Materials and Chemistry Southwest University of Science and Technology school of Material science and Engineering Henan University of Technology College of Chemistry and Chemical Engineering Taishan University

Lithium-sulfur （Li-S） batteries are widely deemed to be one of the most potential candidates for future secondary batteries because of their remarkable energy ***,notorious polysulfide shuttling and retarded sulfur reaction kinetics pose significant obstacles to the further application of Li-S *** rationally designed highly active electrocatalysts can facilitate polysulfide conversion,the universal and scalable synthesis strategies need to be ***,a universal synthetic strategy to construct a series of three-dimensional （3D） porous graphene-iron （3DGr-Fe） based electrocatalysts involving 3DGr-FeP,3DGr-Fe3C,and 3DGr-Fe3Se4is exploited for manipulating the Li-S redox *** has been observed that the implementation of a 3D porous Gr architecture leads to the well-designed conductive networks,while the uniformly dispersed iron nanoparticles introduce an abundance of active sites,fostering the lithium polysulfide conversion,thereby bolstering the overall electrochemical *** Li-S battery with the 3DGr-Fe based electrocatalyst exhibits remarkable capacity retention of 94.8%upon 100 times at 0.2 ***,the soft-packaged Li-S pouch cell based on such a 3DGr-Fe electrocatalyst delivers superior capacity of 1060.71 mA h g-1and guarantees for the continuous 30 min work of fan *** investigation gives comprehensive insights into the design,synthesis,and mechanism of 3DGr-Fe based electrocatalysts with high activity toward efficient and durable Li-S batteries.

关键词： Redox reactions

Preparation of silver nanoparticles through the reduction of straw-extracted lignin and its antibacterial hydrogel

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International Journal of Minerals,Metallurgy and materials 2025年第2期32卷 504-514页

作者： Lou Zhang Shuo Li Fu Tang Jingkai Zhang Yuetong Kang Hean Zhang Lidong Li State Key Laboratory for Advanced Metals and materials School of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China

Silver nanoparticles(Ag NPs)have attracted attention in the field of biomaterials due to their excellent antibacterial ***,the reducing and stabilizing agents used for the chemical reduction of Ag NPs are usually toxic and may cause water *** this work,Ag NPs(31.2 nm in diameter)were prepared using the extract of straw,an agricultural waste,as the reducing and stabilizing *** analysis revealed that the straw extract contained lignin,the structure of which possesses phenolic hydroxyl and methoxy groups that facilitate the reduction of silver salts into Ag *** surfaces of Ag NPs were negatively charged due to the encapsulation of a thin layer of lignin molecules that prevented their *** the prepared Ag NPs were added to the precursor solution of acrylamide,free radical polymerization was triggered without the need for extra heating or light irradiation,resulting in the rapid formation of an Ag NP-polyacrylamide composite *** inhibition zone test proved that the composite hydrogel possessed excellent antibacterial ability due to the presence of Ag *** prepared hydrogel may have potential applications in the fabrication of biomedical materials,such as antibacterial dressings.

关键词： silver nanoparticles hydrogel straw extraction antibacterial

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Conversion-type cathode materials for high energy density solid-state lithium batteries

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Journal of Energy Chemistry 2025年第1期100卷 409-425页

作者： Yuhao Ma Shihong Qing Hongyu Liu Chuntao Ma Yuan Yu Chuang Yu Liping Wang school of materials and Energy University of Electronic Science and Technology of China Zhejiang Provincial Key Laboratory of Fiber materials and Manufacturing technology Zhejiang Sci-Tech University State Key Laboratory of Advanced Electromagnetic Engineering and technology School of Electrical and Electronic Engineering Huazhong University of Science and Technology

Solid-state lithium batteries （SSLBs） are regarded as an essential growth path in energy storage systems due to their excellent safety and high energy *** particular,SSLBs using conversion-type cathode materials have received widespread attention because of their high theoretical energy densities,low cost,and *** the great progress in research and development of SSLBs based on conversiontype cathodes,their practical applications still face challenges such as blocked ionic-electronic migration pathways,huge volume change,interfacial incompatibility,and expensive processing *** review focuses on the advantages and critical issues of coupling conversion-type cathodes with solid-state electrolytes （SSEs）,as well as state-of-the-art progress in various promising cathodes （e.g.,FeS2,CuS,FeF3,FeF2,and S） in ***,representative research on conversion-type solid-state full cells is discussed to offer enlightenment for their practical ***,the energy density exhibited by the S cathode stands out impressively,while sulfide SSEs and halide SSEs have demonstrated immense potential for coupling with conversion-type ***,perspectives on conversion-type cathodes are provided at the material,interface,composite electrode,and battery levels,with a view to accelerating the development of conversion-type cathodes for high-energy–density SSLBs.

关键词： Sulfur compounds

Co/Co_(7)Fe_(3)heterostructures with controllable alloying degree on carbon spheres as bifunctional electrocatalyst forrechargeable zinc-air batteries

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International Journal of Minerals,Metallurgy and materials 2025年第2期32卷 476-487页

作者： Junkang Chen Yongyue Zhuang Yanxin Qiao Yu Zhang Aihua Yuan Hu Zhou school of materials science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China school of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China

Exploring efficient and nonprecious metal electrocatalysts of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is crucial for developing rechargeable zinc-air batteries(ZABs).Herein,an alloying-degree control strategy was employed to fabricate nitrogen-doped carbon sphere(NCS)decorated with dual-phase Co/Co_(7)Fe_(3)heterojunctions(CoFe@NCS).The phase composition of materials has been adjusted by controlling the alloying *** optimal CoFe_(0.08)@NCS electrocatalyst displays a half-wave potential of 0.80 V for ORR and an overpotential of 283 mV at 10 mA·cm^(-2)for OER in an alkaline *** intriguing bifunctional electrocatalytic activity and durability is attributed to the hierarchically porous structure and interfacial electron coupling of highly-active Co_(7)Fe_(3)alloy and metallic Co *** the CoFe_(0.08)@NCS material is used as air-cathode catalyst of rechargeable liquid-state zinc-air battery(ZAB),the device shows a high peak power-density(157 mW·cm^(-2))and maintains a stable voltage gap over 150 h,outperforming those of the benchmark(Pt/C+RuO_(2))-based *** particular,the as-fabricated solid-state flexible ZAB delivers a reliable compatibility under different bending *** work provides a promising strategy to develop metal/alloy-based electrocatalysts for the application in renewable energy conversion technologies.

关键词： bifunctional electrocatalysts oxygen reduction reaction oxygen evolution reaction zinc-air battery metal/alloy carbon sphere

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Fluorinated poly(p-triphenylene isatin) anion exchange membranes based on hydrophilic hydroxyl side chain modulation for fuel cells

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Journal of Energy Chemistry 2025年第1期100卷 702-709页

作者： Yiman Gu Yanchao Zhang Zhanyu Li Yijia Lei Baozeng Sun Xiaoyu Yu Zhe Wang College of Chemistry and Life science Changchun University of Technology College of Chemical Engineering Changchun University of Technology school of materials science and Engineering Changchun University of Technology Key Laboratory of Advanced Functional Polymer Membrane materials of Jilin Province

The development of alkaline fuel cells is moving forward at an accelerated pace,and the application of ether-free bonded polymers to anion exchange membranes （AEMs） has been widely ***,the question of the“trade-off”between AEM ionic conductivity and dimensional stability remains *** strategy of inducing microphase separation to improve the performance of AEM has attracted much attention recently,but the design of optimal molecular structures is still being ***,this work introduced different ratios of 3-bromo-1,1,1-trifluoroacetone （x=40,50,and 60） into the main chain of poly（p-terphenylene isatin）.Because fluorinated groups have excellent hydrophobicity,hydrophilic hydroxyl-containing side chains are introduced to jointly adjust the formation of phase separation *** results show that PTI-PTF50-NOH AEM with the appropriate fluorinated group ratio has the best ionic conductivity and alkali stability under the combined effect of *** has an ionic conductivity of 133.83 mS cm-1at 80°*** addition,the OH-conductivity remains at 89%of the initial value at 80°C and 3 M KOH for 1056 h of *** cell polarization curve based on PTI-PTF50-NOH shows a power density of 734.76 mW cm-2at a current density of 1807.7 mA cm-2.

关键词： Potassium hydroxide

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

Preparation of Low Ratio Magnesium Ccement by Acid Leaching Treatment of Boron Mud

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Journal of Wuhan University of technology(materials science) 2025年第1期40卷 120-129页

作者： YANG Mei ZHANG Mingzhe CHEN Hao school of materials science and Engineering Shenyang Jianzhu UniversityShenyang 110168China school of Physical science and technology Shenyang Normal UniversityShenyang 110168China

The effects of liquid-solid ratio and reaction time on the leaching rate of magnesium at room temperature were investigated,as well as the effects of the molar ratio of MgO/MgCl_(2),the amount of water added,and the amount of acid-impregnated slag dosed on the compressive strength and water resistance of *** results showed that the magnesium element in the boron mud could be maximally leached under the conditions of 1:1 concentration of hydrochloric acid at room temperature,liquid-solid ratio of 2.5 mL·g^(-1),and reaction time of 5 h,and the main products were amorphous SiO_(2) as well as a small amount of magnesium olivine which had not been completely *** LR-MOC prepared using the acid-soaked mixture could reach a softening coefficient of 0.85 for 28 d of water immersion when the molar ratio of MgO/MgCl_(2) was 2.2,the amount of water added was 0 g,and the acid-soaked slag dosing was 40 wt%,which also led to an appreciable late-strength,with an increase of 19.4%in compressive strength at 28 d compared to that at 7 *** previous studies,LR-MOC prepared in this way has a final strength phase that is not the more easily hydrolysed 3-phase but the lath-like *** this phenomenon,we analyzed the mechanism and found that,during the acid leaching process,a part of amorphous SiO_(2) dissolved in the acid leaching solution formed a silica sol,in which Mg^(2+)played a bridging role to make the silica sol more *** the addition and hydrolysis of MgO,the silica sol gel coagulation slows down,providing a capping layer to inhibit the hydrolysis of the 5-phase crystals and providing some strength after *** amorphous SiO_(2) in the other part of the acid-impregnated slag generated M-S-H gel with Mg^(2+)and OH-,which synergised with the dense structure composed of interlocking crystals to improve the water resistance of LR-MOC.

关键词： boron mud magnesium chloride-oxygen cement acid immersion water resistance silica sol

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