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Mechanistic Insights Into H2O Dissociation in Overall Photo-/Electro-Catalytic CO2Reduction

Angewandte Chemie 2025年

作者： Minzhi Ma Yuanxing Fang Zeai Huang Sixin Wu Weiwei He Suxiang Ge Zhi Zheng Ying Zhou Wenjun Fa Xinchen Wang Key Laboratory of Micro-Nano Materials for Energy Storage and Conversion of Henan Province Institute of Surface Micro and Nano Materials College of Chemical and Materials Engineering Xuchang University Xuchang Henan 461000 China Department Key Lab for Special Functional Materials Ministry of Education National & Local Joint Engineering Research Center for High-Efficiency Display and Lighting Technology School of Materials Science and Engineering Collaborative Innovation Center of Nano Functional Materials and Applications Henan University Kaifeng Henan 475004 China State Key Laboratory of Photocatalysis on Energy and Environment College of Chemistry Fuzhou University Fuzhou Fujian 350116 China State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation School of New Energy and Materials Southwest Petroleum University Chengdu Sichuan 610500 China

Photo-/electro-catalytic CO 2 reduction with H 2 O to produce fuels and chemicals offers a dual solution to address both environmental and energy challenges. For a long time, catalyst design in this reaction system has primarily focused on optimizing reduction sites to improve the efficiency or guide the reaction pathway of the CO 2 reduction half-reaction. However, less attention has been paid to designing activation sites for H 2 O to modulate the H 2 O dissociation half-reaction. Impressively, the rate-determining step in overall CO 2 reduction is the latter, and it influences the evolution direction and formation energy of carbon-containing intermediates through the proton-coupled electron transfer process. Herein, we summarize the mechanism of the H 2 O dissociation half-reaction in modulating CO 2 reduction performance based on cutting-edge research. These analyses aim to uncover the potential regulatory mechanisms by which H 2 O activation influences CO 2 reduction pathways and conversion efficiency, and to establish a mechanism-structure-performance relationship that can guide the design and development of high-efficiency catalytic materials. A summary of advanced characterization techniques for investigating the dissociation mechanism of H 2 O is presented. We also discuss the challenges and offer perspectives on the future design of activation sites to improve the performance of photo-/electro-catalytic CO 2 reduction.

关键词： H2O oxidation/activation Proton/electron-feeding Rate-determining step Reduction of CO2 Reverse reaction Water hydrogen bond network

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highly Stable 3d Li Metal Anodes Enabled by a Shielding/Rectifying Polymer Layer

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SSRN 2022年

作者： Ye, Fangjun Gao, Jiafei Yan, Xiaolin Zheng, Hongfei He, Wei Lin, Liang Liu, Fang Qu, Shasha Luo, Qing Wang, Laisen Lin, Jie Xie, Qingshui Peng, Dong-Liang State Key Lab of Physical Chemistry of Solid Surface Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Xiamen36105 China

The practical application of Li metal anode is hindered by the uncontrollable dendrites growth, severe side reactions and huge volume fluctuation, which would result in low coulombic efficiency (CE) and poor cycling performance. Herein, a 3D Li host is functionalized by a low-cost and environment-friendly polyvinyl alcohol (PVA) layer via a facile solution immersion method to solve the above issues. On one hand, the polymer layer can act as a stable artificial SEI with high ionic conductivity during cycling, so as to isolate the direct contact between Li metal and electrolyte and then avoid interfacial side reaction. On the other hand, the abundant hydroxyl (−OH) polar groups in PVA, which own a strong binding energy with Li atoms, can effectively regulate Li plating/stripping behaviors on the 3D framework. As a result, the symmetric cell using PVA-Cu mesh-Li electrode delivers a superior long-term stability over 1000 h with a low average voltage hysteresis of 17 mV at 1 mA cm −2 . And the PVA-Cu mesh-Li || LiFePO 4 full cell can remain a high discharge capacity of 104.4 mAh g −1 and a high CE of 99.1% after 350 cycles at 5 C. © 2022, The Authors. All rights reserved.

关键词： Electrolytes

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Enhanced anticorrosion and wear resistance of epoxy coatings via surface amphiphilic functionalization of silica fillers

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Colloids and surfaces A: Physicochemical and engineering Aspects 2025年 722卷

作者： Guan, Jintao Lan, Jianfeng Huang, Ting Xiao, Jingyao Wang, Junwei Wei, Fuan Zhang, Xian-Hui Salt Lake Chemical Engineering Research Complex Qinghai Provincial Key Laboratory of New Light Alloys Qinghai Provincial Engineering Research Center of High Performance Light Metal Alloys and Forming Qinghai University Xining 810016 China Fujian Province Key Laboratory of Naval Architecture and Marine Engineering School of Marine Engineering Jimei University Xiamen 361021 China Luoyang Ship Materials Research Institute Xiamen Branch China Shipbuilding Industry Corporation Xiamen 361021 China

In this study, we develop a novel anticorrosive and wear-resistant epoxy resin coating through the synergistic modification of silica nanoparticles using phenyltriethoxysilane (PTES) and aminopropyltriethoxysilane (APTES). This amphiphilic dual-functionalization strategy improves the dispersion of nanoparticles and enhances interfacial bonding with the epoxy matrix. Characterization using FTIR, SEM, and EIS reveals that the resulting hybrid coating exhibited exceptional corrosion resistance, maintaining high low-frequency impedance (|Z|0.01 Hz) of 2.29 × 109 Ω·cm2 after 21 days of immersion in 3.5 wt.% NaCl solution. Friction and wear tests demonstrate remarkable wear resistance, with the coating preserving its integrity and hydrophobicity (contact angle decreasing only slightly from 116.8° to 93.1°) even after the control group fails. Compared to conventional anticorrosive coatings employing single-silane functionalization or unmodified nanoparticle systems, the dual-silane modified coating exhibits superior interfacial compatibility and sustained protective performance under prolonged exposure to corrosive environments. These results underscore the effectiveness and promise of synergistic multi-group functionalization strategies in advancing the performance of protective coatings. © 2025

关键词： Coating performance Epoxy resin Modified fillers Silica nanoparticles Synergistic effect

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Efficient photocatalytic biomass-alcohol conversion with simultaneous hydrogen evolution over ultrathin 2D NiS/Ni-CdS photocatalyst

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Chinese Chemical Letters 2024年第7期35卷 422-427页

作者： Zongyi Huang Cheng Guo Quanxing Zheng Hongliang Lu Pengfei Ma Zhengzhong Fang Pengfei Sun Xiaodong Yi Zhou Chen State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China College of Materials Key Laboratory of High Performance Ceramic Fibers(Xiamen University)Ministry of EducationXiamen UniversityXiamen 361005China Technology Center China Tobacco Fujian Industrial Co.Ltd.Xiamen 361021 China

The photocatalytic conversion of biomass into high-value chemicals,coupled with simultaneous hydrogen(H_(2))evolution,leveraging the electrons and holes generated by solar energy,holds great promise for addressing energy *** this study,we constructed a dual functional photocatalytic system formed by NiS loaded on Ni doped two-dimensional(2D)CdS nanosheet(NiS/Ni-CdSNS)heterostructure for visible-light-driven H_(2)evolution and ethanol oxidation to ***,the 2D NiS/NiCdSNS exhibited significant activity and selectivity in both photocatalytic H_(2)evolution and ethanol oxidation,achieving yields of 7.98 mmol g^(-1)h^(-1)for H_(2)and 7.33 mmol g^(-1)h^(-1)for *** heterogeneous interface of the composite facilitated efficient charge separation,while NiS provided abundant sites for proton reduction,thereby promoting the overall dual-functional photocatalytic *** functional theory calculations further reveal that both Ni doping and NiS loading can reduce the reaction energy barrier of ethanol oxidation of free radicals,and NiS/Ni-CdSNS composite materials exhibit stronger ethanol C-H activation ability to generate key intermediate·CH(OH)CH_(3)on the *** work serves as a valuable guide for the rational design of efficient dual functional photocatalytic systems that combine H_(2)evolution with the selective conversion of organic compounds into high-value chemicals.

关键词： Photocatalysis Biomass-alcohol oxidation H_(2)evolution Dual-functional catalysis

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Effects of H3po4 on Synthesis and Luminescence of Metal Halide Perovskites

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SSRN 2023年

作者： Wang, Xiao-Jun Zhang, Xuehu Chen, Fan Hao, Wen Zhang, Changhua Xuan, Tongtong Jiangsu Key Laboratory of Advanced Laser Materials and Devices School of Physics and Electronic Engineering Jiangsu Normal University Jiangsu Xuzhou221116 China Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Fujian Xiamen361005 China

Metal halide perovskites are attractive light-emitting materials due to their excellent optoelectronic properties. However, the traditional preparation methods are mostly complicated. Recently, we introduced a near room temperature synthesis strategy, named H3PO4-assisted precipitation method, which has advantages of thermal- and pressure-free, eco-friendly, as well as short reaction time. Here, we taken Cs2InBr5·H2O as an example to study the impacts of H3PO4 on synthesis and luminescence of metal halide perovskites. Upon adding H3PO4, Cs2InBr5·H2O gives a bright red emission peaked at 630 nm. Various analytic techniques, including X-ray diffraction, FTIR spectra, X-ray photoelectron spectroscopy, Scanning electron microscope, Absorption spectra, and Photoluminescence spectra were employed to investigate the structure and luminescent properties of the prepared Cs2InBr5·H2O perovskites. The results indicate that H3PO4 significantly affects the crystallinity, morphology and STEs emission of Cs2InBr5·H2O. Additionally, various ions doping (such as Sb3+: Cs2InBr5·H2O) and other metal halide microcrystals (such as CsPbBr3 and CsPb2Br5) can also be obtained with the assistance of H3PO4, indicating H3PO4 is a significant additive for synthesizing and enhancing the luminescence of metal halide perovskites. © 2023, The Authors. All rights reserved.

关键词： Bromine compounds

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engineering nanointerface of molybdenum-based heterostructures to boost the electrocatalytic hydrogen evolution reaction

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Journal of Energy Chemistry 2021年第7期30卷 370-376页

作者： Tong Liu Shuqing Zhou Jing Qi Kaiwen Wang Lirong Zheng Qingming Huang Tianhua Zhou Jian Zhang State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China Key Laboratory of Applied Surface and Colloid Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an 710000ShaanxiChina Beijing Key Laboratory and Institute of Microstructure and Property of Advanced Materials Beijing University of TechnologyBeijing 100124China Beijing Synchrotron Radiation Facility(BSRF) Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Testing Center Fuzhou UniversityFuzhou 350116FujianChina

Rational heterostructure-design in electrocatalysts represents a promising approach toward high performance in the electrocatalytic hydrogen evolution reaction(HER).In specific,optimizing the H adsorption behavior at the surface/interface of heterostructure is of key importance to improve the catalytic ***,we demonstrate the construction of a heterostructure from a well-defined oxygenbridged Co/Mo heterometallic zeolitic imidazolate framework(MOZ) as an efficient electrocatalyst for *** optimized hybrid exhibits high catalytic activity and stability in electrolytes with a wide pH *** XPS,XAS and theoretical studies reveal that the regulation of metal species can tailor the lattice of Mo_(2)C within the hybrid and induce the formation of defect sites,which could not only induce surface charge transfer between the atoms and provide an additional active site,but also affect the H adsorption behavior at the interface of a *** work provides an effective strategy to design a heterostructure with tailored active sites for energy conversion.

关键词： Electrocatalysis Metal-organic framework Water splitting Heterostructure

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Experimental Investigation and Thermodynamic Assessment of Phase Equilibria in the Al-Ta-V Ternary System

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SSRN 2023年

作者： Lu, Yong Wang, Cuiping Zheng, Debin Zheng, Zhangcan Wu, Lianzhang Le, Jianping Guo, Yihui Huang, Yixiong Zhang, Jinbin Liu, Xingjun College of Materials Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials Xiamen University Xiamen361005 China Xiamen Key Laboratory of High Performance Metals and Materials Xiamen University Xiamen361005 China School of Materials Science and Engineering Institute of Materials Genome & Big Data Harbin Institute of Technology Shenzhen518055 China

The phase equilibria in the Al-Ta-V ternary system at 1000 °C and 1200 °C have been studied by using electron probe microanalysis and X-ray diffraction. τ-Al2.9Ta2.7V1.4 phase was found in the Al-Ta-V ternary system in both two isothermal sections. The addition of V makes the Al69Ta39 phase be stable at 1000 °C. The linear compound Al3(V,Ta) phase (D022-type) forms a continuous solution from the Al-V side to the Al-Ta side at both temperatures. Based on our experimental results, reported liquidus projection of the ternary Al-Ta-V system and thermodynamic data of the binary systems of Al-V, Al-Ta and V-Ta, a thermodynamic evaluation of Al-Ta-V system was carried out by CALPHAD technique. A set of reliable thermodynamic parameters for the Al-Ta-V system was obtained. The current calculation results agree well with the available experimental data. The invariant reaction scheme of Al-Ta-V ternary system was presented. The present study could provide essential experimental and thermodynamic data for establishing a comprehensive Co-based alloy database. © 2023, The Authors. All rights reserved.

关键词： Ternary systems

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Modulating Structural Stability and Properties in the Co-Based Alloy Via Anti-Site Defects

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SSRN 2023年

作者： Yang, Chen Yu, Xiang Chen, Youheng Han, Jiajia Wang, Cuiping Liu, Xingjun College of Materials Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials Xiamen University Xiamen361005 China Xiamen Key Laboratory of High Performance Metals and Materials Xiamen University Xiamen361005 China School of Materials Science and Engineering Institute of Materials Genome & Big Data Harbin Institute of Technology Shenzhen518055 China

The design of the composition for two-phase superalloys of γ/γ' has always been key to achieving a breakthrough in their mechanical performance. However, the underlying mechanism of the anti-site defects in γ' precipitates that severely affect stability and performance have rarely been explored. The present work therefore specifically investigated the structural stability and mechanical properties of strictly stoichiometric and off-stoichiometric γ'-Co3(Al, Nb) phases by using the first-principles calculations. The results show that the change in the Al/Nb ratios in the compounds could induce the instability of the L12 structure, while an increase of Nb atoms leads to compounds with predominantly covalent bonds exhibiting stronger mechanical properties. After evaluating the Gibbs free energy of these γ'-Co3(Al, Nb) phases at finite temperature, it is found that Co29Al2Nb1 and Co29Al1Nb2 compounds with anti-site defects can be thermodynamically stable at greater than 710 and 905 K, respectively. Accordingly, Co-10Al-2Nb and Co-2.5Al-3Nb alloys were successfully prepared experimentally, further confirming that the γ'-Co3(Al, Nb) phase with anti-site defects can precipitate preferentially and remain stable during the 168 h annealing treatment. © 2023, The Authors. All rights reserved.

关键词： Aluminum alloys

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Achieving ultrahigh anodic-efficiency and energy-density Mg–air battery via the discharge product film design of bulk Mg anode

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Journal of Magnesium and Alloys 2024年

作者： Huang, Jialuo Sun, Zuxiang Tan, Jianxin Sun, Can Liao, Xingpeng Ying, Tao Cao, Fuyong Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Xiamen361005 China National Engineering Research Center of Light Alloy Net Forming School of Materials Science and Engineering Shanghai Jiao Tong University Shanghai 200240 China

This study exhibits a design of the discharge product film of a bulk AZ63-Ce-La-Ca (AZ63X) anode for Mg-air battery. An ideal discharge product film for Mg anode is that it could inhibit the anodic hydrogen evolution but does not hinder the transfer of the electrons at the interface. Fortunately, the addition of Ce, La, and Ca into AZ63 alloy achieves this goal. The Mg-air battery with AZ63X anode in 3.5 % NaCl has an ultrahigh anodic efficiency of 85.7 ± 1.7 % and energy-density of 2431 ± 53 mWh g-1 with the unique discharge product film, surpassing the values of most reported Mg-air batteries. Furthermore, the alloying elements reduce the anode delamination effect significantly by transforming the block Mg17Al12 phase into the connected Mg17Al12 structure and fine rod Al2RE and Al2Ca. © 2024

关键词： Anodes

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A library of carbon-supported ultrasmall bimetallic nanoparticles

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Nano Research 2020年第10期13卷 2735-2740页

作者： Shi-Long Xu Shan-Cheng Shen Ze-Yue Wei Shuai Zhao Lu-Jie Zuo Ming-Xi Chen Lei Wang Yan-Wei Ding Ping Chen Sheng-Qi Chu Yue Lin Kun Qian Hai-Wei Liang Hefei National Laboratory for Physical Sciences at the Microscale Departm ent of ChemistryUniversity of Science and Technology of ChinaHefei 230026China Hefei National Laboratory for Physical Sciences at the Microscale Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesCAS Key Laboratory of Materials for Energy Conversion and Department of Chemical PhysicsUniversity of Science and Technology of ChinaHefei 230026China School of Chemistry and Chemical Engineering Anhui UniversityHefei 230601China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China

Small-sized bimetallic nanoparticles that possess numerous accessible metal sites and optimal geometric/electronic structures show great promise for advanced synergetic catalysis but remain synthetic challenge so ***,an universial synthetic method is developed for building a library of bimetallic nanoparticles on mesoporous sulfur-doped carbon supports,consisting of 24 combinations of 3 noble metals(that is,Pt,Rh,Ir)and 7 other metals,with average particle sizes ranging from 0.7 to 1.4 *** synthetic strategy is based on the strong metal-support interaction arising from the metal-sulfur bonding,which suppresses the metal aggregation during the H2-reduction at 700℃ and ensure the formation of small-sized and alloyed bimetallic *** enhanced catalytic properties of the ultrasmall bimetallic nanoparticles are demonstrated in the dehydrogenation of propane at high temperature and oxidative dehydrogenations of N-heterocycles.

关键词： bimeallic nanoparticles sulfur doped carbon catalysis ultrasmall metal-support interaction

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