比较了甲醇对 Pt/C和炭载四羧基酞菁钴 (Co Pc Tc/C)催化氧还原性能的影响 .结果表明 ,甲醇使Pt/C催化氧还原的性能严重降低 ,而对经 80 0℃热处理的 Co Pc Tc/C(Co Pc Tc/C-80 0 )基本没有影响 ;并且Co Pc Tc/C-80 0催化氧还原的性能...比较了甲醇对 Pt/C和炭载四羧基酞菁钴 (Co Pc Tc/C)催化氧还原性能的影响 .结果表明 ,甲醇使Pt/C催化氧还原的性能严重降低 ,而对经 80 0℃热处理的 Co Pc Tc/C(Co Pc Tc/C-80 0 )基本没有影响 ;并且Co Pc Tc/C-80 0催化氧还原的性能优于经其它温度热处理的 Co Pc Tc/C,Co Pc Tc/C-80 0是一种较好的直接甲醇燃料电池的耐甲醇阴极电催化剂 .XPS结果表明 ,Co Pc Tc/C-80 0的活性位可能是含 Co N4结构的物质和零价 Co的混合物 .展开更多
Recently, the electrochemical N2 reduction reaction （NRR） in aqueous electrolytes at ambient temperature and pressure has demonstrated its unique advantages and potentials. The reactants are directly derived from ga...Recently, the electrochemical N2 reduction reaction （NRR） in aqueous electrolytes at ambient temperature and pressure has demonstrated its unique advantages and potentials. The reactants are directly derived from gaseous N2 and water, which are naturally abundant, and NH3 production is important for fertilizers and other industrial applications. To improve the conversion yield and selectivity （mainly competing with water reduction）, electrocatalysts must be rationally designed to optimize the mass transport, chemisorption, and transduction pathways of protons and electrons. In this review, we summarize recent progress in the electrochemical NRR. Studies of electrocatalyst designs are summarized for different categories, including metal-based catalysts, metal oxide-derived catalysts, and hybrid catalysts. Strategies for enhancing the NRR performance based on the facet orientation, metal oxide interface, crystallinity, and nitrogen vacancies are presented. Additional system designs, such as lithium-nitrogen batteries, and the solvent effect are introduced. Finally, existing challenges and prospects are discussed.展开更多
With the ever-pressing issues of global energy demand and environmental pollution,molecular hydrogen has been receiving increasing attention as a clean alternative energy carrier.For hydrogen production,the design and...With the ever-pressing issues of global energy demand and environmental pollution,molecular hydrogen has been receiving increasing attention as a clean alternative energy carrier.For hydrogen production,the design and development of high-performance catalysts remains rather challenging.As the compositions and structures of catalyst interfaces have paramount influences on the catalytic performances,the central topic here has always been to design and engineer the interface structures via rational routes so as to boost the activities and stabilities of electrocatalysts on hydrogen evolution reaction(HER).Here in this review,we focus on the design and preparation of multi-scale catalysts specifically catering to HER applications.We start from the design and structure-activity relationship of catalytic nanostructures,summarize the research progresses related to HER nanocatalysts,and interpret their high activities from the atomistic perspective;then,we review the studies regarding the design,preparation,HER applications and structure-activity relationship of single-atom site catalysts(SASCs),and thereupon discuss the future directions in designing HER-oriented SASCs.At the end of this review,we present an outlook on the development trends and faced challenges of catalysts for electrochemical HER.展开更多
Developing earth-abundant-electrocatalysts for hydrogen evolution reaction is one of the promising ways to achieve efficient water-splitting for hydrogen production(a clean chemical fuel).This paper reviews the activi...Developing earth-abundant-electrocatalysts for hydrogen evolution reaction is one of the promising ways to achieve efficient water-splitting for hydrogen production(a clean chemical fuel).This paper reviews the activity,stability and durability for hydrogen evolution reaction in alkaline medium of different types of recently reported potential electrocatalysts such as Ni,Co,NiCo,Fe,Cu,W,Mo,Se,Mn.Zn,V,and metal free based earth-abundant-electrocatalysts.Further,this paper reviews the strategies used to achieve the remarkably low overpotential(including r/i0:<35mV),high long term stability(including^:100 h)and high durability(including>5000 cycles)of potential earth-abundant-electrocatalysts for hydrogen evolution reaction in alkaline medium and those are better or well comparable with the state-of-the-art,noble,Pt/C electrocatalyst.Finally,this paper summarizes the efficient strategies such as preparing porous structured materials,preparing nanostructured materials with superaerophobic surface,preparing nanostructured materials,preparing carbon composites/integrating electrocatalysts with carbon,preparing amorphous materials,preparing materials w让h oxygen vacancies/defects,preparing metal chalcogenides,preparing bimetallic/multi-metallic materials,doping metals or heteroatoms,preparing electrocatalysts with core-shell structure,decorating electrocatalysts with amines,preparing homojunction/heterojunction structured materials,preparing hollow structured materials,and preparing boronrich surface to enhance the activity,stability,and durability for HER.展开更多
The development of efficient, low-cost, for water splitting, particularly those stable, non-noble-metal electrocatalysts that can catalyze both the hydrogen evolution reaction （HER） at the cathode and oxygen evoluti...The development of efficient, low-cost, for water splitting, particularly those stable, non-noble-metal electrocatalysts that can catalyze both the hydrogen evolution reaction （HER） at the cathode and oxygen evolution reaction （OER） at the anode, is a challenge. We have developed a facile method for synthesizing CoSe2 nanoparticles uniformly anchored on carbon fiber paper （CoSe2/CF） via pyrolysis and selenization of in situ grown zeolitic imidazolate framework-67 （ZIF-67）. CoSe2/CF shows high and stable catalytic activity in both the HER and OER in alkaline solution. At a low cell potential, i.e., 1.63 V, a water electrolyzer equipped with two CoSe2/CF electrodes gave a water-splitting current of 10 mA.cm-2. At a current of 20 mA-cm-2, it can operate without degradation for 30 h. This study not only offers a cost-effective solution for water splitting but also provides a new strategy for developing various catalytic nanostructures by changing the metal-organic framework precursors.展开更多
文摘比较了甲醇对 Pt/C和炭载四羧基酞菁钴 (Co Pc Tc/C)催化氧还原性能的影响 .结果表明 ,甲醇使Pt/C催化氧还原的性能严重降低 ,而对经 80 0℃热处理的 Co Pc Tc/C(Co Pc Tc/C-80 0 )基本没有影响 ;并且Co Pc Tc/C-80 0催化氧还原的性能优于经其它温度热处理的 Co Pc Tc/C,Co Pc Tc/C-80 0是一种较好的直接甲醇燃料电池的耐甲醇阴极电催化剂 .XPS结果表明 ,Co Pc Tc/C-80 0的活性位可能是含 Co N4结构的物质和零价 Co的混合物 .
文摘Recently, the electrochemical N2 reduction reaction （NRR） in aqueous electrolytes at ambient temperature and pressure has demonstrated its unique advantages and potentials. The reactants are directly derived from gaseous N2 and water, which are naturally abundant, and NH3 production is important for fertilizers and other industrial applications. To improve the conversion yield and selectivity （mainly competing with water reduction）, electrocatalysts must be rationally designed to optimize the mass transport, chemisorption, and transduction pathways of protons and electrons. In this review, we summarize recent progress in the electrochemical NRR. Studies of electrocatalyst designs are summarized for different categories, including metal-based catalysts, metal oxide-derived catalysts, and hybrid catalysts. Strategies for enhancing the NRR performance based on the facet orientation, metal oxide interface, crystallinity, and nitrogen vacancies are presented. Additional system designs, such as lithium-nitrogen batteries, and the solvent effect are introduced. Finally, existing challenges and prospects are discussed.
基金Acknowledgements This work was supported by the National Key R&D Program of China(2016YFA0202801,2017YFA0700101 and 2018YFA0702003)the National Natural Science Foundation of China(21925202,21872076 and 21890383)+4 种基金Beijing Natural Science Foundation(JQ18007)the Fundamental Research Funds for the Central Universities(19CX02008A)the Petro China Innovation Foundation(2019D-5007-0401)Taishan Scholars Program of Shandong Province(tsqn201909065)Tsinghua University Initiative Scientific Research Program.
文摘With the ever-pressing issues of global energy demand and environmental pollution,molecular hydrogen has been receiving increasing attention as a clean alternative energy carrier.For hydrogen production,the design and development of high-performance catalysts remains rather challenging.As the compositions and structures of catalyst interfaces have paramount influences on the catalytic performances,the central topic here has always been to design and engineer the interface structures via rational routes so as to boost the activities and stabilities of electrocatalysts on hydrogen evolution reaction(HER).Here in this review,we focus on the design and preparation of multi-scale catalysts specifically catering to HER applications.We start from the design and structure-activity relationship of catalytic nanostructures,summarize the research progresses related to HER nanocatalysts,and interpret their high activities from the atomistic perspective;then,we review the studies regarding the design,preparation,HER applications and structure-activity relationship of single-atom site catalysts(SASCs),and thereupon discuss the future directions in designing HER-oriented SASCs.At the end of this review,we present an outlook on the development trends and faced challenges of catalysts for electrochemical HER.
基金supported by the National Natural Science Foundation of Chinathe Innovative Research Team in the University+4 种基金the Program for Changjiang Scholarsthe Fundamental Research Funds for the Central Universitiesthe longterm subsidy mechanism from the Ministry of Financethe Ministry of Education of People’s Republic of China (PRC)the Science and Engineering Research Board (SERB), Department of Science and Technology, Government of India (Reference No. PDF/2017/000015)
文摘Developing earth-abundant-electrocatalysts for hydrogen evolution reaction is one of the promising ways to achieve efficient water-splitting for hydrogen production(a clean chemical fuel).This paper reviews the activity,stability and durability for hydrogen evolution reaction in alkaline medium of different types of recently reported potential electrocatalysts such as Ni,Co,NiCo,Fe,Cu,W,Mo,Se,Mn.Zn,V,and metal free based earth-abundant-electrocatalysts.Further,this paper reviews the strategies used to achieve the remarkably low overpotential(including r/i0:<35mV),high long term stability(including^:100 h)and high durability(including>5000 cycles)of potential earth-abundant-electrocatalysts for hydrogen evolution reaction in alkaline medium and those are better or well comparable with the state-of-the-art,noble,Pt/C electrocatalyst.Finally,this paper summarizes the efficient strategies such as preparing porous structured materials,preparing nanostructured materials with superaerophobic surface,preparing nanostructured materials,preparing carbon composites/integrating electrocatalysts with carbon,preparing amorphous materials,preparing materials w让h oxygen vacancies/defects,preparing metal chalcogenides,preparing bimetallic/multi-metallic materials,doping metals or heteroatoms,preparing electrocatalysts with core-shell structure,decorating electrocatalysts with amines,preparing homojunction/heterojunction structured materials,preparing hollow structured materials,and preparing boronrich surface to enhance the activity,stability,and durability for HER.
基金The project is supported by the National Natural Science Foundation of China （Nos. 21275076 and 61328401）, Jiangsu Provincial Founds for Distinguished Young Scholars （No. BK20130046）, Key University Science Research Project of Jiangsu Province （No. 15KJA430006）, Program for New Century Excellent Talents in University （No. NCET-13-0853）, QingLan Project, Nantong Key Laboratory of New Materials Industrial Technology, SERC Grant （#102170 0142） from A＇STAR Singapore, the scholarship from China Scholarships Council （No. 201508320304）.
文摘The development of efficient, low-cost, for water splitting, particularly those stable, non-noble-metal electrocatalysts that can catalyze both the hydrogen evolution reaction （HER） at the cathode and oxygen evolution reaction （OER） at the anode, is a challenge. We have developed a facile method for synthesizing CoSe2 nanoparticles uniformly anchored on carbon fiber paper （CoSe2/CF） via pyrolysis and selenization of in situ grown zeolitic imidazolate framework-67 （ZIF-67）. CoSe2/CF shows high and stable catalytic activity in both the HER and OER in alkaline solution. At a low cell potential, i.e., 1.63 V, a water electrolyzer equipped with two CoSe2/CF electrodes gave a water-splitting current of 10 mA.cm-2. At a current of 20 mA-cm-2, it can operate without degradation for 30 h. This study not only offers a cost-effective solution for water splitting but also provides a new strategy for developing various catalytic nanostructures by changing the metal-organic framework precursors.
