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Metal-organic frameworks with dinuclear metal centers for synergistically boosting CO_(2) 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 UniversityYangzhou 225002China Institute for new energy materials and Low Carbon Technologies School of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China

Dinuclear metal synergistic catalysis(DMSC)has been proved powerful in boosting CO_(2)reduction,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 CO_(2)reduction 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^(-1)h^(-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 CO_(2)reduction,which provides new insights into the DMSC and paves a new way to design highly active catalysts for photochemical CO_(2)reduction.

关键词： metal-organic frameworks dinuclear metal centers synergistic catalysis CO_(2)reduction photocatalysis

An improved method to evaluate trap depth from thermoluminescence

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Journal of Rare Earths 2025年第2期43卷 262-269,I0002页

作者： Shiyou Zhang Fangyi Zhao Shengqiang Liu Zhen Song Quanlin Liu The Beijing Municipal Key Laboratory of new energy materials and Technologies School of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing100083China

Rare earth-doped inorganic compounds contribute mostly to the family of persistent luminescent materials due to the versatile energy levels of rare earth *** of the key research aims is to match the trap level stemming from the doped rare earth ion or intrinsic defects to the electronic structure of the host,and therefore thermoluminescence measurement becomes a radical technology in studying trap depth,which is one of the significant parameters that determine the properties of persistent luminescence and photostimulated ***,the results of trap depth obtained by different thermoluminescence methods are quite different so that they are not ***,we analyzed different thermoluminescence methods,selected and improved the traditional peak position method of T_(m)/500 to be E=(-0.94Inβ+30.09)kT_(m).Only the experimental heating rate(β)is needed additionally,but the accuracy is improved greatly in most *** convenient and accurate method will accelerate the discovery of novel rare earth-doped materials.

关键词： Thermoluminescence Persistent luminescence Photostimulated luminescence Rare earths Trap depth

Constructing electrochemically stable single crystal Ni-rich cathode material via modification with high valence metal oxides

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Journal of energy Chemistry 2025年第02期101卷 392-401页

作者： Hancheng Shi Jiongzhi Zheng Tao Wan Hongqiang Wang Zeping Wen Fenghua Zheng Mingru Su Aichun Dou Yu Zhou Ahmad Naveed Panpan Zhang Hailong Wang Ruiqiang Guo Yunjian Liu Dewei Chu school of Material Science and Engineering Jiangsu University Thayer school of Engineering Dartmouth College school of materials Science and Engineering The University of New South Wales school of Chemistry and Pharmaceutical Sciences Guangxi Normal University school of materials and new energy Ningxia University Thermal Science Research Center Shandong Institute of Advanced Technology

Single crystal Ni-rich cathode materials（SCNCM） are a good supplement in the market of nickel-based materials due to their safety and excellent electrochemical ***,the challenges of cation mixing,phase change during charge/discharge,and low thermal stability remain unresolved in single crystal *** address these issues,SCNCM are rationally modified by incorporating transition metal（TM） oxides,and the influence of metal ions with different valence states on the electrochemical properties of SCNCM is methodically explored through experimental results and theoretical *** structural stability is demonstrated in SCNCM after the modifications,and the degree of improvement in the matrix materials varies depending on the valence state of doped TM *** highest structural stability is found in WO3-modified SCNCM,due to the smaller effective ion radii,higher electro-negativity,stronger W-O bond,and efficient suppression of oxygen vacancy *** a result,WO3-modified SCNCM have outstanding cycle performance,with a capacity retention rate of90.2% after 200 *** study provides an insight into the design of advanced SCNCM with enhanced reversibility and cyclability.

关键词： In-situ coating Ion doping Lithium-ion battery Single crystal Ni-rich material Strengthening mechanism analysis

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 UniversityKunming 650091YunnanChina National Center for International Research on Photoelectric and energy materials School of Materials and EnergyYunnan UniversityKunming 650091YunnanChina

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)_(2)hexagonal 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^(-2)for HMFOR,significantly outperforming Co(OH)_(2)benchmark(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： Biomass conversion Electrocatalysis 2,5-Furandicarboxylic acid Doped Co catalyst Co3+active sites Charge transfer rate

Revisit the Gibbs-Thomson Equation Fitting of Poly(butylene succinate)Based on Oligomer Extended-Chain Crystals

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Chinese Journal of Polymer Science 2025年第2期43卷 392-398页

作者： Na Li Yu-Pei Tian Tian-Yu Wu Qiong Zhou Hai-Mu Ye College of new energy and materials China University of PetroleumBejing 102249China

The equilibrium melting point(T_(m)^(0))is a crucial thermodynamic parameter for characterizing the crystallization and melting behavior of semi-crystalline ***,the direct measurement of T_(m)^(0) poses a significant challenge because of the difficulty in physically fabricating fully-extended chain crystals of high-molecular-weight ***,various extrapolation equations for T_(m)^(0) have been proposed that utilize the thermal properties of ordinary folded-chain *** these,the Gibbs-Thomson equation is one of the most commonly employed for *** its widespread use,there are notable variations in the T_(m)^(0) values obtained by different research groups,even when based on similar *** raises questions about the validity and accuracy of using the Gibbs-Thomson equation to linearly extrapolate T_(m)^(0).In this study,we prepared a series of oligomer extended-chain crystals(ECCs)of poly(butylene succinate)(PBS)and used their properties for Gibbs-Thomson *** results reveal a perfect linear relationship,with an extrapolated T_(m)^(0) value of 136.08℃.The basal surface free energy of the oligomer ECCs was calculated as 0.084 J/m^(2),which is approximately twice that of folded-chain *** difference is attributed to the aggregation of highly mobile free tails on the crystal *** two structural features of oligomer ECCs—large thickness and fixed surface—better fulfill the conditions for applying the Gibbs-Thomson equation,ensuring its validity and ***,we believe that the Gibbs-Thomson fit can produce reliable results when sufficient high-quality data are used.

关键词： Equilibrium melting point Extended-chain crystal Gibbs-Thomson equation Inclusion complex

In situ construction of Cu(Ⅰ)-Cu(Ⅱ) pairs for efficient electrocatalytic nitrate reduction reaction to ammonia

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Journal of energy Chemistry 2025年第1期100卷 106-113页

作者： Muyun Zheng Yuchi Wan Leping Yang Shen Ao Wangyang Fu Zhengjun Zhang Zheng-Hong Huang Tao Ling Feiyu Kang Ruitao Lv State Key Laboratory of new Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China Institute of new energy materials and Engineering School of Materials Science and EngineeringFuzhou UniversityFuzhou 350108FujianChina Key Laboratory of Advanced materials(MOE) School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education Tianjin Key Laboratory of Composite and Functional MaterialsSchool of Materials Science and EngineeringTianjin UniversityTianjin 300072China

Electrocatalytic nitrate reduction reaction (NO_(3)-RR) to ammonia under ambient conditions is expected to be a green process for ammonia synthesis and alleviate water pollution *** report a CuO nanoparticles incorporated on nitrogen-doped porous carbon (CuO@NC) catalyst for NO_(3)-*** of Cu(Ⅱ) is reduced to Cu(Ⅰ) during the NO_(3)-RR process to construct Cu(Ⅰ)-Cu(Ⅱ) pairs,confirmed by in situ X-ray photoelectron spectroscopy (XPS) and Raman *** functional theory (DFT) calculations indicated that the formation of Cu(Ⅰ) could provide a reaction path with smaller energy barrier for NO_(3)-RR,while Cu(Ⅱ) effectively suppressed the competition of hydrogen evolution reaction (HER).As a result,CuO@NC catalyst achieved a Faradaic efficiency of 84.2% at -0.49 V versus reversible hydrogen electrode (RHE),and a NH_(3)yield rate of 17.2 mg h^(-1)mg^(-1)*** -0.79 V ***,higher than the HaberBosch process (new avenue for effective NO_(3)-RR by modulating oxidation states.

关键词： Ammonia synthesis Cu oxidation state Electrochemistry Nitrate reduction In situ XPS

A low-cost wide bandgap polymer based on carboxylate substituted thiazole enables efficient organic solar cells with remarkable batch-to-batch reproducibility

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Science China Chemistry 2025年第2期68卷 733-744页

作者： Xiaodong Zhu Yuchen Lei Jianhong Gao Yanjun He Jinsicheng Liu Qian Guo Xiang Gao Liwei Xiong Xunchang Wang Renqiang Yang Zhitian Liu Hubei Engineering Technology Research Center of Optoelectronic and new energy materials Hubei Key Laboratory of Plasma Chemistry and Advanced MaterialsSchool of Materials Science and EngineeringWuhan Institute of TechnologyWuhan 430205China Key Laboratory of Optoelectronic Chemical materials and Devices(Ministry of Education) School of Optoelectronic Materials&TechnologyJianghan UniversityWuhan 430056China

Constructing the low-cost,high-efficiency,and good batch-to-batch reproducibility polymer donor is vitally important for the application of organic solar ***,we develop a structurally simple carboxylate-substituted thiazole as an electronwithdrawing building block to construct a low-cost polymer,PBTTzE,containing a facilely prepared chlorinated benzo[1,2-b:4,5-b′]dithiophene(BDTCl)donor *** from synergistic electron deficient effects of chlorination and ester group and C=N,as well as the noncovalent interaction of S…O and S…N,PBTTzE exhibits a deep HOMO energy level(−5.59 eV),and a planar skeleton *** combined with the IT-4F acceptor,the polymer(54 kDa)demonstrated a champion PCE of 15.87%,which is the highest value in the IT-4F-based binary devices to ***,PBTTzE exhibits excellent batch-tobatch reproducibility due to its very similar PCEs within a range of 43–76 *** addition,an alloyed state and complementary absorption can be formed between PM6 and ***,in a ternary device with PBTTzE added to the PM6:BTP-eC9 blend,a top PCE of 18.76%is achieved due to the suppressed energy loss,prolonged exciton diffusion distance,and improved charge *** work demonstrates that the carboxylate-substituted thiazole is a highly promising acceptor unit for constructing low-cost and high-performance polymers.

关键词： carboxylate substituted thiazole polymer donor low-cost batch-to-batch reproducibility organic solar cells

Morphology engineering of ZnO micro/nanostructures under mild conditions for optoelectronic application

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International Journal of Minerals,Metallurgy and materials 2025年第2期32卷 498-503页

作者： Liang Chu Haoyu Shen Hudie Wei Hongyu Chen Guoqiang Ma Wensheng Yan Institute of Carbon Neutrality and new energy&school of Electronics and Information Hangzhou Dianzi UniversityHangzhou 310018China school of Applied Physics and materials Wuyi UniversityJiangmen 529020China

Zinc oxide(ZnO)serves as a crucial functional semiconductor with a wide direct bandgap of approximately 3.37 *** reaction is commonly used in the synthesis of ZnO micro/nanostructures,given its low cost,simplicity,and easy ***,ZnO morphology engineering has become desirable through the alteration of minor conditions in the reaction process,particularly at room *** this work,ZnO micro/nanostructures were synthesized in a solution by varying the amounts of the ammonia added at low temperatures(including room temperature).The formation of Zn^(2+)complexes by ammonia in the precursor regulated the reaction rate of the morphology engineering of ZnO,which resulted in various structures,such as nanoparticles,nanosheets,microflowers,and single ***,the obtained ZnO was used in the optoelectronic application of ultraviolet detectors.

关键词： morphology engineering low temperature ZnO nanosheets microflowers ultraviolet detector

Improving structure stability of single-crystalline Ni-rich cathode at high voltage by element gradient doping and interfacial modifcation

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Journal of energy Chemistry 2025年第2期101卷 630-640页

作者： Ruijuan Wang Yixu Zhang Zhi Li Lei Wu Jiarui Chen Xiaolin Liu Hui Hu Hao Ding Shuang Cao Qiliang Wei Xianyou Wang National Base for International Science & Technology Cooperation of new energy Equipment Energy Storage Materials and Devices National Local Joint Engineering Laboratory for Key Materials of New Energy Storage Battery Hunan Province Key Laboratory of Electrochemical Energy Storage & Conversion School of Chemistry Xiangtan University Institute of Micro/Nano materials and Devices Ningbo University of Technology

Single-crystalline Ni-rich cathodes can provide high energy density and capacity retention rates for lithium-ion batteries（LIBs）.However,single-crystalline Ni-rich cathodes experience severe transition metal dissolution,irreversible phase transitions,and reduced structural stability during prolonged cycling at high voltage,which will significantly hinder their practical ***,a Li4TeO5surface coating along with bulk Te-gradient doping strategy is proposed and developed to solve these issues for single-crystalline Ni-rich LiNi0.90Co0.05Mn0.05O2cathode（LTeO-1.0）.It has been found that the bulk Te6+gradient doping can lead to the formation of robust Te-O bonds that effectively inhibit H2-H3 phase transformations and reinforce the lattice framework,and the in-situ Li4TeO5coating layer can act as a protective layer that suppresses the parasitic reactions and grain ***,the modified material exhibits a higher Young's modulus,which will be conducive to maintaining significant structural and electrochemical stability under high-voltage conditions,Especially,the LTeO-1.0 electrode shows the improved Li+diffusion kinetics and thermodynamic stability as well as high capacity retention of 95.83%and 82.12% after 200 cycles at the cut-off voltage of 4.3 and 4,5 ***,the efficacious dualmodification strategy will definitely contribute to enhancing the structural and electrochemical stability of single-crystalline Ni-rich cathodes and developing their application in LIBs.

关键词： High cut-off voltage Li4TeO5 coating layer Material fragmentation Single-crystalline Ni-rich cathode Te6+ doping