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Why do CuAl catalysts outperform in CO_(2) electro-reduction to C_(2)H_(4)?

Science China Chemistry 2025年第2期68卷 763-771页

作者： Dongfang Cheng Gong Zhang Lulu Li Xiangcheng Shi Wenjin Zhu Xintong Yuan Lyudmila Moskaleva Peng Zhang Zhi-Jian Zhao Jinlong Gong Key Laboratory for Green chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin University Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin 300072China Joint School of National university of Singapore and tianjin university International Campus of Tianjin UniversityFuzhou 350207China department of Chemistry University of the Free StateBloemfontein 9301South Africa Haihe Laboratory of Sustainable chemical Transformations Tianjin 300192China National Industry-Education Platform of Energy Storage Tianjin UniversityTianjin 300350China International Joint Laboratory of Low-carbon chemical engineering Tianjin 300192China tianjin Normal university Tianjin 300387China

Highly efficient CO_(2) electroreduction(CO_(2)RR)holds the promise of closing the carbon ***,the strategies for enhancing activity and selectivity for single C2+ products are still *** paper describes the oxophilicity of doped metals on copper(Cu)as a key descriptor for predicting the selectivity in the production of ethylene and ethanol in CO_(2)*** findings reveal a volcano-like relationship between the*O binding energy and catalytic activity,with aluminum(Al)-doped Cu alloys situated at the *** strong Al–O bond facilitates C–O bond cleavage,thereby promoting C_(2)H_(4) *** grand canonical density functional theory(GCDFT)calculations,we elucidate the significance of strong oxygen affinity in enhancing*CO_(2) adsorption,leading to its activation into a bidentate-adsorbed ***,our results demonstrate that Al doping promotes C–C coupling by altering the adsorption mode of the key intermediate *OCCO,shifting it from a less favorable boattype to a more stable chair-type *** modification significantly contributes to the improved catalytic activity for C2+products on CuAl *** research provides a detailed mechanistic insight into the high activity and selectivity observed in CO_(2)RR to ethylene on CuAl catalysts,underscoring the critical role of metal oxophilicity in enhancing CO_(2)RR performance.

关键词： CO_(2)RR dilute alloy descriptor surface oxophilicity

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Methyl Groups Pendant on Triphenylmethane Toward Modulating Thermal Stability and Dielectric Properties of the Crosslinkable Fluorinated Polyimide Films with High Transparency

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Chinese Journal of Polymer Science 2025年第2期43卷 316-327页

作者： Wen Yang Liang Yuan Kai Gong Ruo-Han Zhang Lan Lei Hui Li School of Chemistry and chemical engineering Shandong Key Laboratory of Fluorine Chemistry and Chemical Engineering MaterialsUniversity of JinanJinan250022China School of Materials Science and engineering Tianjin Key Laboratory of Composite and Functional MaterialsTianjin UniversityTianjin300350China

It is urgent to develop high-performance polyimide(PI)films that simultaneously exhibit high transparency,exceptional thermal stability,mechanical robustness,and low dielectric to fulfil the requirements of flexible display ***,a series of fluorinated polyimide films(FPIs)were fabricated by the condensation of 5,5′-(perfluoropropane-2,2-diyl)bis(isobenzofuran-1,3-dione)(6FDA)and the fluorinated triphenylmethane diamine monomer(EDA,MEDA and DMEDA)with heat-crosslinkable tetrafluorostyrene side groups,which was incorporated by different numbers of methyl groups pendant in the ortho position of amino ***,the FPI films underwent heating to produce crosslinking FPIs(C-FPIs)through the self-crosslinking of double bonds in the *** transparency,solvent resistance,thermal stability,mechanical robustness and dielectric properties of FPI and C-FPI films can be tuned by the number of methyl groups and crosslinking,which were deeply investigated by virtue of molecular dynamics(MD)simulations and density functional theory(DFT).As a result,all the films exhibited exceptional optically colorless and transparent,with transmittance in the visible region of 450-700 nm exceeding 79.9%,and the cut-off wavelengths(λ_(off))were nearly 350 *** thermal decomposition temperatures at 5% weight loss(T_(d5%))for all samples exceeded 504℃.These films exhibited a wide range of tunable tensile strength(46.5-75.1 MPa).Significantly,they showed exceptional dielectric properties with the dielectric constant of 2.3-2.5 at full frequency(10^(7)-20 Hz).This study not only highlights the relationship between the polymer molecular structure and properties,but offer insights for balancing optical transparency,heat resistance and low dielectric constant in PI films.

关键词： Crosslinkable fluorinated polyimide Methyl group Triphenylmethane Transparency Thermal stability Low dielectric constant

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Cross-section design of the flow channels in membrane electrode assembly electrolyzer for CO_(2) reduction reaction through numerical simulations

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Chinese chemical Letters 2025年第1期36卷 332-337页

作者： Lili Zhang Hui Gao Gong Zhang Yuning Dong Kai Huang Zifan Pang Tuo Wang Chunlei Pei Peng Zhang Jinlong Gong Key Laboratory for Green chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovation Center of chemical Science and engineering(tianjin) Tianjin 300072China Haihe Laboratory of Sustainable chemical Transformations Tianjin 300192China National Industry-Education Platform of Energy Storage Tianjin UniversityTianjin 300350China Joint School of National university of Singapore and tianjin university International Campus of Tianjin UniversityFuzhou 350207China

Membrane electrode assembly(MEA)is widely considered to be the most promising type of electrolyzer for the practical application of electrochemical CO_(2) reduction reaction(CO_(2)RR).In MEAs,a square-shaped cross-section in the flow channel is normally adopted,the configuration optimization of which could potentially enhance the performance of the *** paper describes the numerical simulation study on the impact of the flow-channel cross-section shapes in the MEA electrolyzer for CO_(2)*** results show that wide flow channels with low heights are beneficial to the CO_(2)RR by providing a uniform flow field of CO_(2),especially at high current ***,the larger the electrolyzer,the more significant the effect *** study provides a theoretical basis for the design of high-performance MEA electrolyzers for CO_(2)RR.

关键词： Electrochemical reduction of CO_(2) Membrane electrode assembly Mass transfer Gas diffusion electrode Computational fluid dynamics

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High-temperature-tolerant flexible supercapacitors: Gel polymer electrolytes and electrode materials

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Journal of Energy Chemistry 2025年第1期100卷 426-457页

作者： Chong Peng Xinyi Huang Mingwei Zhao Shuling Liao Quanhong Yang Nianjun Yang Siyu Yu School of Chemistry&chemical engineering Southwest UniversityChongqing 400715 China Nanoyang Group Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy StorageSchool of Chemical Engineering and Technologyand Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin UniversityTianjin 300072 China department of Chemistry&IMO–IMOMEC Hasselt UniversityDiepenbeek 3590Belgium Received 26 July 2024Revised 19 Aug

The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and electrode materials stand as two key components that significantly impact the efficacy of hightemperature-tolerant FSCs(HT-FSCs). They should not only exhibit high electrochemical performance and excellent flexibility, but also withstand intense thermal stress. Considerable efforts have been devoted to enhancing their thermal stability while maintaining high electrochemical and mechanical performance. In this review, the fundamentals of HT-FSCs are outlined. A comprehensive overview of state-of-the-art progress and achievements in HT-FSCs, with a focus on thermally stable gel polymer electrolytes and electrode materials is provided. Finally, challenges and future perspectives regarding HT-FSCs are discussed, alongside strategies for elevating operational temperatures and *** review offers both theoretical foundations and practical guidelines for designing and manufacturing HT-FSCs, further promoting their widespread adoption across diverse fields.

关键词： Flexible supercapacitors High-temperature tolerance Gel polymer electrolytes Electrode materials

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Metal nanoparticles decorated CoFe-(oxy)hydroxysulfides nanosheets fabricated by a general strategy for electrocatalytic water splitting

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Journal of Energy Chemistry 2025年第1期100卷 26-38页

作者： Xiaodong Yang Haochen Shen Xiaoming Xiao Zhichao Li Qi Zhou Wei Yang Bin Jiang Yongli Sun Luhong Zhang Zhenhua Yan School of chemical engineering and Technology Tianjin UniversityTianjin 300072China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization *** developed Ag/SLDH and Pt/SLDH catalysts with abundant heterogeneous interfaces and hierarchical nanostructures demonstrated outstanding oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)performance,achieving low overpotentials of 212 and 35 mV at 10 mA cm^(-2)in 1 M KOH,*** both anode and cathode in water splitting,they required only 1.47 V to reach 10 mA cm^(-2)and exhibited high structural robustness,maintaining stability at 1000 mA cm^(-2)for 300 ***-situ Raman analysis revealed that the synergistic effects of metal nanoparticles and S doping significantly promote the transformation into the S-Co1-xFexOOH layer,which serves as the active phase for water ***,ultraviolet photoelectron spectroscopy(UPS)and density functional theory(DFT)analyses indicated that incorporating metal nanoparticles and S doping increase electron density near the Fermi level and reduce reaction energy barriers,thus enhancing intrinsic OER and HER *** study provides a scalable strategy for synthesizing high-performance electrocatalysts for water splitting,with promising potential for broader applications.

关键词： LDH Spontaneous reaction Metal nanoparticles Water splitting

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Atomically precise M-N-C electrocatalysts for oxygen reduction:Effects of inter-site distance,metal-metal interaction,coordination environment,and spin states

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Journal of Energy Chemistry 2025年第2期101卷 132-155页

作者： Junfeng Huang Saira Ajmal Anuj Kumar Jianwen Guo Mohammed Mujahid Alam Abdullah G.Al-Sehemi Ghulam Yasin School of Mechanical engineering Dongguan University of Technology Nano-Technology Research Laboratory Department of Chemistry GLA University department of Chemistry College of Science King Khalid University School of Environmental Science and engineering Tianjin University State Key Laboratory of chemical Resource engineering College of Materials Science and Engineering Beijing University of Chemical Technology

Inspired by molecular catalysts,researchers developed atomically precise nitrogen-coordinated single or dual metal sites imbedded in graphitized carbon（M-N-C） to fully utilize metallic sites for *** catalysts performed remarkably well in the electrocatalytic oxygen reduction reaction（ORR） due to their distinct coordination and electrical structures,Nonetheless,their maximum efficacy in practical applications has yet to be *** agenda identifies tailoring the coordination environment,spin states,intersite distance,and metal-metal interaction as innovative approaches to regulate the ORR performance of these ***,it is necessary to undertake a precise assessment of these methodologies and the knowledge obtained to be implemented in the design of future M-N-C catalysts for ***,this review aims to analyze recent progress in M-N-C ORR catalysts,emphasizing their innovative engineering with aspects such as alteration in intersite distance,metal-metal interaction,coordination environment,and spin ***,we critically discuss how to logically monitor the atomic structure,local coordination,spin,and electronic states of M-N-C catalysts to modulate their ORR *** have also highlighted the challenges associated with M-N-C catalysts and proposed suggestions for their future design and fabrication.

关键词： Activity descriptors Electrocatalysis M-N-C electrocatalysts ORR Spin states

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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

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A review of over-discharge protection through prelithiation in working lithium-ion batteries

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Journal of Energy Chemistry 2025年第2期101卷 437-452页

作者： Hanchen Wang Yingtian Liu Mingze Jiang Qiang Zhang School of Aerospace engineering National Engineering Research Center of Neuromodulation Tsinghua University Tsinghua Center for Green chemical engineering Electrification Department of Chemical Engineering Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Tsinghua University

The demand for high safety and high reliability lithium-ion batteries(LIBs) is strongly considered for practical ***,due to their inherent self-discharge properties or abuse,LIBs face the threat of over-discharge,which induces premature end of life and increased risk of thermal *** addition,a strong demand for batteries with zero-volt storage is strongly considered for aerospace and implantable medical *** this review,we firstly introduce the necessity and the importance of over-discharge and zero-volt protection for *** mechanism of damage to the Cu current collectors and SEI induced by potential changes during over-discharge is *** current over-discharge protection strategies based on whether the zero-crossing potential of the electrodes is ***,the fresh insights into the material design of cathode prelithiation additives are presented from the perspective of over-discharge protection.

关键词： Electrode potential regulation Electrode prelithiation Li-ion batteries Over-discharge protection Zero-volt storage

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Multilevel analysis of the central-peripheral-target organ pathway:contributing to recovery after peripheral nerve injury

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Neural Regeneration Research 2025年第10期20卷 2807-2822页

作者： Xizi Song Ruixin Li Xiaolei Chu Qi Li Ruihua Li Qingwen Li Kai-Yu Tong Xiaosong Gu Dong Ming Academy of Medical engineering and Translational Medicine Tianjin UniversityTianjinChina Haihe Laboratory of Brain-Machine Interface and Human-Machine Fusion TianjinChina department of Rehabilitation Tianjin University Tianjin HospitalTianjinChina department of Hand Microsurgery Tianjin University Tianjin HospitalTianjinChina School of Exercise and Health Tianjin University of SportTianjinChina department of Biomedical engineering the Chinese University of Hong KongHong Kong Special Administrative RegionChina

Peripheral nerve injury is a common neurological condition that often leads to severe functional limitations and *** on the pathogenesis of peripheral nerve injury has focused on pathological changes at individual injury sites,neglecting multilevel pathological analysis of the overall nervous system and target *** has led to restrictions on current therapeutic *** this paper,we first summarize the potential mechanisms of peripheral nerve injury from a holistic perspective,covering the central nervous system,peripheral nervous system,and target *** peripheral nerve injury,the cortical plasticity of the brain is altered due to damage to and regeneration of peripheral nerves;changes such as neuronal apoptosis and axonal demyelination occur in the spinal *** nerve will undergo axonal regeneration,activation of Schwann cells,inflammatory response,and vascular system regeneration at the injury *** damage to target organs can occur,including skeletal muscle atrophy and sensory receptor *** then provide a brief review of the research advances in therapeutic approaches to peripheral nerve *** main current treatments are conducted passively and include physical factor rehabilitation,pharmacological treatments,cell-based therapies,and physical ***,most treatments only partially address the problem and cannot complete the systematic recovery of the entire central nervous system-peripheral nervous system-target organ ***,we should further explore multilevel treatment options that produce effective,long-lasting results,perhaps requiring a combination of passive(traditional)and active(novel)treatment methods to stimulate rehabilitation at the central-peripheral-target organ levels to achieve better functional recovery.

关键词： central nervous system central peripheral target organ multilevel pathological analysis nerve regeneration peripheral nerve injury peripheral nervous system target organs therapeutic approach

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Flexible molecules dedicate to release strain of inverted inorganic perovskite solar cell

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Journal of Energy Chemistry 2025年第1期100卷 87-93页

作者： Hongrui Sun Sanlong Wang Pengyang Wang Yali Liu Shanshan Qi Biao Shi Ying Zhao Xiaodan Zhang Institute of Photoelectronic Thin Film Devices and Technology Renewable Energy Conversion and Storage CenterState Key Laboratory of Photovoltaic Materials and CellsNankai UniversityTianjin 300350China Key Laboratory of Photoelectronic Thin Film Devices and Technology of tianjin Tianjin 300350China Haihe Laboratory of Sustainable chemical Transformations Tianjin 300192China engineering Research Center of Thin Film Photoelectronic Technology of Ministry of Education Tianjin 300350China Collaborative Innovation Center of chemical Science and engineering(tianjin) Tianjin 300072China

The tensile strain in inorganic perovskite films induced by thermal annealing is one of the primary factors contributing to the inefficiency and instability of inorganic perovskite solar cells(IPSCs),which reduces the defect formation ***,a flexible molecule 5-maleimidovaleric acid(5-MVA)was introduced as a strain buffer to release the residual strain of CsPbI_(2.85)Br_(0.15)*** anhydride and carboxyl groups in 5-MVA interact strongly with the uncoordinated Pb^(2+)through Lewis acid-base reaction,thus tightly“pull”the perovskite *** in-between soft carbon chain increased the structural flexibility of CsPbI_(2.85)Br_(0.15)perovskite materials,which effectively relieved the intrinsic internal strain of CsPbI_(2.85)Br_(0.15),resisted the corrosion of external strain,and also reduced the formation of defects such as VIand *** addition,the introduction of 5-MVA improved crystal quality,passivated residual defects,and narrowed energy level ***,power conversion efficiency(PCE)of NiOxbased inverted IPSCs increased from 19.25%to 20.82%with the open-circuit voltage enhanced from 1.164 V to 1.230 *** release of strain also improved the stability of CsPbI_(2.85)Br_(0.15)perovskite films and devices.

关键词： Inverted inorganic perovskite solar cells Flexible molecules Strain release Crystallization Energy barrier High PCE

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