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Molecular engineering binuclear copper catalysts for selective CO_(2) reduction to C_(2) products

Journal of Energy Chemistry 2024年第6期93卷 166-173,I0005页

作者： Qi Zhao Kai Lei bao yu xia Rachel Crespo-Otero Devis Di Tommaso Department of Chemistry School of Physical and Chemical SciencesQueen Mary University of LondonLondonE14NSUK Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureState Key Laboratory of Materials Processing and Die&Mould TechnologySchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan 430074HubeiChina Department of Chemistry University College LondonLondonWC1H 0AJUK Digital Environment Research Institute Queen Mary University of LondonEmpire HouseLondon E11HHUK

Molecular copper catalysts serve as exemplary models for correlating the structure-reaction-mechanism relationship in the electrochemical CO_(2) reduction(eCO_(2)R),owing to their adaptable environments surrounding the copper metal *** investigation,employing density functional theory calculations,focuses on a novel family of binuclear Cu molecular *** modulation of their coordination configuration through the introduction of organic groups aims to assess their efficacy in converting CO_(2) to C_(2)*** findings highlight the crucial role of chemical valence state in shaping the characteristics of binuclear Cu catalysts,consequently influencing the eCO_(2)R behaviour,Notably,the Cu(Ⅱ)Cu(Ⅱ)macrocycle catalyst exhibits enhanced suppression of the hydrogen evolution reaction(HER),facilitating proton trans fer and the eCO_(2)R *** rthermore,we explo re the impact of diverse electro n-withdrawing and electron-donating groups coordinated to the macrocycle(R=-F,-H,and-OCH_3)on the electron distribution in the molecular *** placement of-OCH_3 groups in the macrocycles leads to a favourable oxidation state of the Cu centres and subsequent C-C coupling to form C_(2) *** research provides fundamental insights into the design and optimization of binuclear Cu molecular catalysts for the electrochemical conversion of CO_(2) to value-added C_(2) products.

关键词： Molecular catalyst design Selective CO_(2)reduction C_(2)products Density functional theory calculations

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一种用于肼氧化-复合海水电解制氢的富吡啶氮碳纸

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Science China Materials 2024年第3期67卷 752-761页

作者：马闪闪喻博夏宝玉游波 Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

丰富的中性海水有望替代高纯淡水用于绿氢制备,然而基于过渡金属材料催化的直接海水电解会因析氯反应(ClER)引发严重的腐蚀问题并造成二次重金属污染,且析氧反应(OER)的动力学缓慢.本工作中,我们报道了一种稳定的富吡啶氮的碳纸(N-CP-80... 详细信息

丰富的中性海水有望替代高纯淡水用于绿氢制备,然而基于过渡金属材料催化的直接海水电解会因析氯反应(ClER)引发严重的腐蚀问题并造成二次重金属污染,且析氧反应(OER)的动力学缓慢.本工作中,我们报道了一种稳定的富吡啶氮的碳纸(N-CP-800),可以有效地催化肼氧化反应(HzOR),以取代中性海水中的OER用于节能制氢.结合电化学实验、原位衰减全反射-表面增强傅里叶变换红外光谱表征和密度泛函理论计算,我们发现:相较于吡咯氮和石墨氮,zig和arm构型的吡啶氮更有利于决速步(^(*)H+N_(2)H_(1))的质子脱附,以促进肼氧化反应.因此,N-CP-800在中性介质中进行HzOR时,仅需0.78 V(相对于可逆氢电势)便可达到10 mA cm^(-2),低于其OER/ClER竞争反应.当N-CP-800与非贵金属析氢催化剂CoP耦合进行HzOR-复合海水电解时,仅需1.56 V的电压即可达到10 mA cm^(-2),并能稳定运行200 h,优于Pt/C和RuO_(2)标准电极对催化的海水电解.

关键词： seawater electrolysis hydrazine oxidation hydrogen evolution nitrogen doping metal-free carbon

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Periodic Defect Boundary-Mediated Activity of Electrocatalytic Oxygen Reduction Reactions of Fe-N-C Catalysts

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Renewables 2024年第3期2卷 213-221页

作者： Ziwei Wang Huiting Niu Tiantian Wu Shujiang Ding bao yu xia Yaqiong Su School of Chemistry Engineering Research Center of Energy Storage Materials and Devices of Ministry of EducationNational Innovation Platform(Center)for Industry-Education Integration of Energy Storage TechnologyXi’an Jiaotong UniversityXi’an 710049 School of Chemistry and Chemical Engineering Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education)Hubei Key Laboratory of Material Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsWuhan National Laboratory for OptoelectronicsHuazhong University of Science and Technology(HUST)Wuhan 430074

The introduction of defects can adjust the activity of graphene-based single-atom catalysts for oxygen reduction reactions(ORR).Herein,we for the first time investigate the ORR catalytic activity of FeN_(4)sites embedded on graphene with four types of line-defective boundary via density functional theory *** results show that periodic line defects consisting of pentagon-pentagon-octagon(C_(585))or quad-octagon chains(C_(484))can significantly enhance ORR activity,owing to the optimized electronic structures of FeN_(4)*** spin magnetic moment and the valence state of the Fe atom are both well correlated with the ORR *** investigations further corroborate that FeN_(4)with a high degree of defects exhibits better ORR activity and stability compared to FeN_(4)sites of pristine graphene and commercial Pt/*** work unravels the influence of the periodic defect boundary on the ORR performance of Fe-N-C catalysts and paves the way towards the rational design of highly effective single-atom electrocatalysts.

关键词： density functional theory Fe-N-C catalysts oxygen reduction reaction periodic defect electrocatalyst

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Progress in MXene-based catalysts for oxygen evolution reaction

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Electron 2024年第1期2卷 48-67页

作者： Jieli Chen xiaohong Gao Jing Li Zhenye Kang Juan Bai Tianjiao Wang yuliang yuan Chenghang You yu Chen bao yu xia Xinlong Tian School of Marine Science and Engineering Hainan Provincial Key Lab of Fine ChemistrySchool of Chemistry and Chemical EngineeringHainan UniversityHaikouChina School of Chemistry and Physics Queensland University of TechnologyBrisbaneQueenslandAustralia Key Laboratory of Macromolecular Science of Shaanxi Province School of Materials Science and EngineeringShaanxi Normal UniversityXi'anChina School of Chemistry and Chemical Engineering State Key Laboratory of Materials Processing and Die&Mould TechnologyKey Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education)Hubei Key Laboratory of Material Chemistry and Service FailureWuhan National Laboratory for OptoelectronicsHuazhong University of Science and Technology(HUST)WuhanChina

Electrochemical water splitting for hydrogen generation is considered one of the most promising strategies for reducing the use of fossil fuels and storing renewable electricity in hydrogen ***,the anodic oxygen evolution process remains a bottleneck due to the remarkably high overpotential of about 300 mV to achieve a current density of 10 mA cm^(−2).The key to solving this dilemma is the development of highly efficient catalysts with minimized overpotential,long-term stability,and low *** a new 2D material,MXene has emerged as an intriguing material for future energy conversion technology due to its benefits,including superior conductivity,excellent hydrophilic properties,high surface area,versatile chemical composition,and ease of processing,which make it a potential constituent of the oxygen evolution catalyst *** review aims to summarize and discuss the recent development of oxygen evolution catalysts using MXene as a component,emphasizing the synthesis and synergistic effect of MXene-based composite *** on the discussions summarized in this review,we also provide future research directions regarding electronic interaction,stability,and structural evolution of MXene-based oxygen evolution *** believe that a broader and deeper research in this area could accelerate the discovery of efficient catalysts for electrochemical oxygen evolution.

关键词： MXene-based catalysts oxygen evolution reaction water splitting

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调节铜催化剂表面分子亲电性以调控电催化二氧化碳还原选择性

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Science China Materials 2024年第6期67卷 1858-1865页

作者：周贤龙单洁琼郑敏李欢夏宝玉郑尧 School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureNational Laboratory for OptoelectronicsSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China Jiangsu Co-Innovation Centre of Efficient Processing and Utilization of Forest Resources College of Chemical EngineeringNanjing Forestry UniversityNanjing 210037China

Cu是唯一能选择性将二氧化碳电还原(CRR)为多碳产物的过渡金属.然而,调控Cu的CRR选择性获得多种产物仍非常具有挑战性.本文选择了一系列具有不同亲电性的分子来修饰Cu催化剂以调控其CRR选择性,从而产生CH_(4)或C_(2)H_(4).理论计算表明... 详细信息

Cu是唯一能选择性将二氧化碳电还原(CRR)为多碳产物的过渡金属.然而,调控Cu的CRR选择性获得多种产物仍非常具有挑战性.本文选择了一系列具有不同亲电性的分子来修饰Cu催化剂以调控其CRR选择性,从而产生CH_(4)或C_(2)H_(4).理论计算表明,分子的亲电性决定催化反应中的质子活度,进而能促进或抑制CRR中的质子耦合电子转移(PCET)过程.实验发现,低亲电性分子(如1,2-双(4-吡啶基)乙烷)可以促进质子转移,加快^(*)CO中间体氢化过程而生成CH_(4),实现58.2%的法拉第效率;而高亲电性分子(如顺-1,2-双(4-吡啶基)乙烯)能构建强的氢键以稳定^(*)CO中间体,促进其偶联生成C_(2)H_(4),实现65.9%的法拉第效率.理论计算结合原位光谱表征揭示,分子亲电性可调节催化剂质子活度,影响CRR反应中^(*)CO氢化或偶联,进而调控CRR选择性.不同于常规的催化剂结构工程,本策略通过调节CRR中的PCET过程来调控选择性,为CRR的发展提供了新的认识.

关键词： molecular electrophilicity Cu catalysts proton transfer CO_(2)electroreduction C1/C2 selectivity

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Emerging two-dimensional nanocatalysts for electrocatalytic hydrogen production

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Chinese Chemical Letters 2022年第4期33卷 1831-1840页

作者： Hong Chen Yansong Zhou Wei Guo bao yu xia Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsWuhan National Laboratory for OptoelectronicsSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan 430074China

Hydrogen energy could be a economic and powerful technology for sustainable future. Producing hydrogen fuel by electrochemical water splitting has attracted intense interest. Due to their physical and chemical properties, two-dimensional(2 D) nanomaterials have sparked immense interest in water electrocatalysis for hydrogen production. This review focuses on the emerging nanocatalysts in 2 D nanoarchitectures for electrocatalytic hydrogen production. The fundamentals of HER are firstly depicted, following the discussion of recent advances in typical 2 D electrocatalysts for HER. The insights into the relationship among the synthetic protocols, structure, catalytic performance and thermodynamics will be discussed in details. Finally, the outlooks regarding further development of 2 D nanocatalysts for HER are *** hope this review will offer a comprehensive understanding in 2 D nanocatalysts to promote electrochemical hydrogen production.

关键词： Hydrogen evolution Electrocatalyst Two-dimensional Active sites Modification

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Progress on nanostructured gel catalysts for oxygen electrocatalysis

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Nano Research 2022年第12期15卷 10343-10356页

作者： Huan Yang Huilin Hu Chenfeng xia Feng You Junlong Yao Xueliang Jiang bao yu xia Wuhan Institute of Technology Hubei Key Laboratory of Plasma Chemistry and Advanced MaterialsSchool of Materials Science and EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationWuhan430205China Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureWuhan National Laboratory for OptoelectronicsSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan430074China

Driven by the serious ecological problems,it is urgent to explore high-efficiency sustainable energy *** electrocatalysis acts as important half-reactions in the emerging electrochemical energy techniques including electrolysis and *** composites exhibit the merits of rich porous,superior hydrophilic,and large specific surface area,which can significantly improve the electrolyte penetration and boost the kinetics process of oxygen *** this invited contribution,the advances and challenges of a novel gel materials for oxygen electrocatalysis are *** from the structure-activity-performance relationship of gel materials,synthetic routes of nanostructured gel materials,namely,radical polymerization,sol-gel method,hydrothermal/solvothermal reactions,and ligand-substitution method,are ***,the gel composites are divided into polymer-based,metal-based,and carbon-based materials in turn,and their applications in oxygen electrocatalysis are discussed *** the end,the perspective and challenges for advanced gel oxygen electrocatalysts are proposed.

关键词： oxygen electrocatalysis gel materials polymer metal carbon

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Trimetallic PtRhNi alloy nanoassemblies as highly active electrocatalyst for ethanol electrooxidation

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Nano Research 2017年第10期10卷 3324-3332页

作者： Huimin Liu Jiahui Li Lijuan Wang Yawen Tang bao yu xia yu Chen Key Laboratory of Macromolecular Science of Shaanxi Province Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology School of Materials Science and Engineering Shaanxi Normal University 620 Changan Road Xi'an 710062 China Jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Center of Biomedical Functional Materials School of Chemistry and Materials Science Nanjing Normal University 1 Wenyuan Road Nanjing 210023 China A key laboratory of Material Chemistry for Energy Conversion and Storage Ministry of Education Hubei Key Laboratory of Material Chemistry and Service Failure School of Chemistry and Chemical Engineering Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology (HUST) 1037 Luoyu Road Wuhan 430074 China Shenzhen Institute of Huazhong University of Science and Technology 9 Yuexing Road Shenzhen 518000 China

Although nanostructures based on noble metal alloys are widely utilized in （electro）catalysis, their low-temperature synthesis remains an enormous challenge due to the different Nernst equilibrium potentials of metal precursors. Herein, we describe the successful synthesis of trimetallic PtRhNi alloy nanoassemblies （PtRhNi-ANAs） with tunable Pt/Rh ratios using a simple mixed cyanogel reduction method and provide a detailed characterization of their chemical composition, morphology, and structure. Additionally, the electrochemical properties of PtRhNi-ANAs are examined by cyclic voltammetry, revealing composition- dependent electrocatalytic activity in the ethanol oxidation reaction （EOR）. Compared to a commercial Pt black electrocatalyst, optimized Pt3Rh1Ni2-ANAs display remarkably enhanced EOR electrocatalytic performance in alkaline media.

关键词： cyanogel trimetallic alloy electrocatalysis activity ethanol oxidation reaction

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Exfoliation and dispersion of graphene in ethanol-water mixtures

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Frontiers of Materials Science 2012年第2期6卷 176-182页

作者： Wei-Wei LIU bao-yu xia xiao-xia WANG Jian-Nong WANG Shanghai Key Laboratory for Laser Processing and Materials Modification School of Materials Science and EngineeringShanghai Jiao Tong University800 Dong Chuan RoadShanghai 200240China School of Materials Science and Engineering Tongji University1239 Siping RoadShanghai 200092China Key Laboratory of Safety Science of Pressurized System(Ministry of Education) ScHool of Mechanical and Power EngineeringEast China University of Science and Technology130 Meilong RoadShanghai 200237China

Graphene has attracted much attention as a new nano-carbon for its unique structure and properties. However, production and dispersion of unfunctionalized graphene are still big challenges. Herein, we demonstrate a simple method for preparation and dispersion of such graphene with low cost and non toxicum. This approach is achieved by exfoliating graphite in an ethanol/water mixture and forming stable dispersion of mono- and few-layer graphenes. The ratio of ethanol/water in the mixture is found to be crucial to both the exfoliation and dispersion processes. Exfoliation in pure water or pure ethanol produces no graphene. This method avoids the conventional use of harsh oxidants and surfactants; therefore, the graphitic structure is well maintained without destruction. Benefiting from the use of ethanol and water, it can be easy to prepare transparent and conductive graphene films by vacuum filtering or spray method, and does not need special post-treatment to remove the impurity, which could be beneficial for potential applications in electronic, optic and energy areas.

关键词： graphene liquid-phase exfoliation transparent conductive film solubilityparameter

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Continuous nitrogen-doped carbon nanotube matrix for boosting oxygen electrocatalysis in rechargeable Zn-air batteries

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Journal of Energy Chemistry 2021年第4期30卷 183-189页

作者： Guangda Chen Yangyang Xu Lei Huang Aboulkader Ibro Douka bao yu xia Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureWuhan National Laboratory for OptoelectronicsSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan 430074HubeiChina

Developing robust oxygen electrocatalyst with high-performance is very significant for practical rechargeable Zn-air *** report herein the preparation of three-dimensional continuous nanocarbon network composed of interconnected nitrogen-doped carbon nanotubes and its application as oxygen electrocatalysis in rechargeable Zn-air *** the excellent electrochemical bifunctionality,this carbon nanotube matrix also delivers an impressive battery ***,an opencircuit voltage of 1.50 V as well as a high power density of 220 m W cm^(-2) with remarkable cycling stability for 1600 h is achieved in the rechargeable Zn-air *** study not only provides an efficient bifunctional oxygen electrocatalyst but more importantly may pave significant concepts in designing robust electrode for long-life rechargeable Zn-air battery and other energy technologies.

关键词： Zeolitic-imidazolate framework Carbon nanotube Bifunctionality Electrocatalyst Zn-air battery

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