Electrocatalysis is becoming more and more important in energy conversion and storage due to rising energy demands,increasing carbon dioxide emissions,and impending climate change.The design and synthesis of high-perf...Electrocatalysis is becoming more and more important in energy conversion and storage due to rising energy demands,increasing carbon dioxide emissions,and impending climate change.The design and synthesis of high-performance electrocatalysts are the spotlights of electrocatalysis.Among many design methodologies reported,strain engineering has gained growing attention because it can change the atomic arrangement and lattice structure of electrocatalysts.However,strain engineering remains to be problematic in regulating the properties of electrocatalysts.This review discusses the strain effect tactics to regulate metal and non-metal electrocatalysts,including three sections focusing on strain categorization,strain regulation mechanism,and applications in electrocatalysis,respectively.Finally,the current challenges and an outlook of strain engineering are discussed.展开更多
Electrochemical reduction of CO_(2)(CO_(2)RR)coupled with renewable electrical energy is an attractive way of upgrading CO_(2)to value-added chemicals and closing the carbon cycle.However,CO_(2)RR electrocatalysts sti...Electrochemical reduction of CO_(2)(CO_(2)RR)coupled with renewable electrical energy is an attractive way of upgrading CO_(2)to value-added chemicals and closing the carbon cycle.However,CO_(2)RR electrocatalysts still suffer from high overpotential,and the complex reaction pathways of CO_(2)RR often lead to mixed products.Early research focuses on tuning the binding of reaction intermediates on electrocatalysts,and recent efforts have revealed that the design of electrolysis reactors is equally important for efficient and selective CO_(2)RR.In this review,we present an overview of recent advances and challenges toward achieving high activity and high selectivity in CO_(2)RR at ambient conditions,with a particular focus on the progress of CO_(2)RR electrocatalyst engineering and reactor design.Our discussion begins with three types of electrocatalysts for CO_(2)RR(noble metalbased,none-noble metal-based,and metal-free electrocatalysts),and then we examine systems-level strategies toward engineering specific components of the electrolyzer,including gas diffusion electrodes,electrolytes,and polymer electrolyte membranes.We close with future perspectives on catalyst development,in-situ/operando characterization,and electrolyzer performance evaluation in CO_(2)RR studies.展开更多
Electrocatalytic CO2 reduction (ECR) into value-added chemicals offers potential solution for renewable energy as well as global carbon footprint concerns. In this review we introduce the general methods and metrics t...Electrocatalytic CO2 reduction (ECR) into value-added chemicals offers potential solution for renewable energy as well as global carbon footprint concerns. In this review we introduce the general methods and metrics that are commonly applied in ECR, followed by a discussion of current reaction mechanisms and different pathways. We highlight how size and structure of electrocatalysts affect ECR performance and review recent advances in metalfree and single-atom catalysts. The challenges of ECR are also discussed and optimistic perspectives are made for future work.展开更多
As a model reaction for the electrooxidation of many small organic molecules,formic acid electrooxidation(FAEO)has aroused wide concern.The promises of direct formic acid fuel cells(DFAFC)in application further streng...As a model reaction for the electrooxidation of many small organic molecules,formic acid electrooxidation(FAEO)has aroused wide concern.The promises of direct formic acid fuel cells(DFAFC)in application further strengthen people’s attention to the related research.However,despite decades of study,the FAEO mechanism is still under debate due to the multi-electron and multi-pathway nature of the catalytic process.In this review,the progresses towards understanding the FAEO mechanism along with the developed methodology(electrochemistry,in-situ spectroscopy,and theoretical calculation and simulation)are summarized.We especially focused on the construction of anti-poisoning catalysts system based on understanding of the catalytic mechanism,with anti-poisoning catalyst design being systemically summarized.Finally,we provide a brief summarization for current challenges and future prospects towards FAEO study.展开更多
制备低成本的高效电催化剂是缓解目前面临的环境能源危机的重要方式.通过无定型化和构建异质结构可以有效地改变催化剂的电子结构,从而实现电催化性能的稳步提升.但是对于两者之间协同作用的研究则相对较少.在本文中,我们构建了富含异...制备低成本的高效电催化剂是缓解目前面临的环境能源危机的重要方式.通过无定型化和构建异质结构可以有效地改变催化剂的电子结构,从而实现电催化性能的稳步提升.但是对于两者之间协同作用的研究则相对较少.在本文中,我们构建了富含异质结构的无定型FeMo基(a-FeMo)电催化剂,并系统评估了该催化剂的氮气还原和析氧反应性能.得益于无定型结构引起的活性位点数目的增多和异质结构引发的电子的重新分布,a-FeMo催化剂表现出优异的电化学催化性能.在-0.1 V vs.RHE的电势下,a-FeMo催化剂表现出29.15%的法拉第效率和71.78μg_(NH_(3)) mg_(cat.)^(-1) h^(-1)的氨气产率.这为合理设计具有低成本优势、高活性和长时间稳定性的优异催化剂提供了有益的参考.展开更多
基金This research was supported by the National Natural Science Foundation of China(Nos.T2222002,21973079,22032004,and 21991130)the Natural Science Foundation of Fujian Province(No.2021J06008).
文摘Electrocatalysis is becoming more and more important in energy conversion and storage due to rising energy demands,increasing carbon dioxide emissions,and impending climate change.The design and synthesis of high-performance electrocatalysts are the spotlights of electrocatalysis.Among many design methodologies reported,strain engineering has gained growing attention because it can change the atomic arrangement and lattice structure of electrocatalysts.However,strain engineering remains to be problematic in regulating the properties of electrocatalysts.This review discusses the strain effect tactics to regulate metal and non-metal electrocatalysts,including three sections focusing on strain categorization,strain regulation mechanism,and applications in electrocatalysis,respectively.Finally,the current challenges and an outlook of strain engineering are discussed.
基金We acknowledge the support from the National Natural Science Foundation of China(21991153,21991150).
文摘Electrochemical reduction of CO_(2)(CO_(2)RR)coupled with renewable electrical energy is an attractive way of upgrading CO_(2)to value-added chemicals and closing the carbon cycle.However,CO_(2)RR electrocatalysts still suffer from high overpotential,and the complex reaction pathways of CO_(2)RR often lead to mixed products.Early research focuses on tuning the binding of reaction intermediates on electrocatalysts,and recent efforts have revealed that the design of electrolysis reactors is equally important for efficient and selective CO_(2)RR.In this review,we present an overview of recent advances and challenges toward achieving high activity and high selectivity in CO_(2)RR at ambient conditions,with a particular focus on the progress of CO_(2)RR electrocatalyst engineering and reactor design.Our discussion begins with three types of electrocatalysts for CO_(2)RR(noble metalbased,none-noble metal-based,and metal-free electrocatalysts),and then we examine systems-level strategies toward engineering specific components of the electrolyzer,including gas diffusion electrodes,electrolytes,and polymer electrolyte membranes.We close with future perspectives on catalyst development,in-situ/operando characterization,and electrolyzer performance evaluation in CO_(2)RR studies.
基金National Natural Science Foundation of China (Grant No. 51773092)National Natural Science Foundation of China (21825202, 21575135, 21733012, 21633008, 21605136)+3 种基金Research Fundation of State Key Lab (ZK201717)the support from Department of Education of Jilin Province (JJKH20190767KJ)Department of Education of Guangdong Province (2017KCXTD031)Science Foundation for High-level Talents of Wuyi University (2017RC23)
文摘Electrocatalytic CO2 reduction (ECR) into value-added chemicals offers potential solution for renewable energy as well as global carbon footprint concerns. In this review we introduce the general methods and metrics that are commonly applied in ECR, followed by a discussion of current reaction mechanisms and different pathways. We highlight how size and structure of electrocatalysts affect ECR performance and review recent advances in metalfree and single-atom catalysts. The challenges of ECR are also discussed and optimistic perspectives are made for future work.
基金the National Natural Science Foundation of China(No.21905267,)the National Key R&D Program of China(No.2018YFB1502400)+2 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA21090400)the Department of Science and Technology of Shandong province(No.2019JZZY010905)the Jilin Province Science and Technology Development Program(Nos.20190201300JC,20170520150JH,and 20200201001JC)for financial support.
文摘As a model reaction for the electrooxidation of many small organic molecules,formic acid electrooxidation(FAEO)has aroused wide concern.The promises of direct formic acid fuel cells(DFAFC)in application further strengthen people’s attention to the related research.However,despite decades of study,the FAEO mechanism is still under debate due to the multi-electron and multi-pathway nature of the catalytic process.In this review,the progresses towards understanding the FAEO mechanism along with the developed methodology(electrochemistry,in-situ spectroscopy,and theoretical calculation and simulation)are summarized.We especially focused on the construction of anti-poisoning catalysts system based on understanding of the catalytic mechanism,with anti-poisoning catalyst design being systemically summarized.Finally,we provide a brief summarization for current challenges and future prospects towards FAEO study.
基金supported by National Natural Science Fund of China (Grant Nos. 51677182, 51472238 and 51721005)Beijing Municipal Science and Technology Project (Grant No. Z171100000917007)
基金supported by the National Key Project on Basic Research (No.2015CB932302)National Natural Science Foundation of China (No.21773263 and No.91645123)the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB12020100)
基金supported by the Natural Science Foundation of China (NSFC) (21733004, 21327901)the National Basic Research Program of China (973 Program, 2015CB932303)+1 种基金the International Cooperation Program of Shanghai Science and Technology Committee (STCSM) (17520711200)partially supported by American University
基金supported by the National Natural Science Foundation of China(U2032149)Shenzhen Science and Technology Project(JCYJ20180507182246321)+3 种基金Hunan Provincial Natural Science Foundation of China(2020JJ2001)Hefei National Laboratory for Physical Sciences at the Microscale(KF2020108)the Fundamental Research Funds for the Central UniversitiesChina Postdoctoral Science Foundation(2019M663058 and 2019M652749).
文摘制备低成本的高效电催化剂是缓解目前面临的环境能源危机的重要方式.通过无定型化和构建异质结构可以有效地改变催化剂的电子结构,从而实现电催化性能的稳步提升.但是对于两者之间协同作用的研究则相对较少.在本文中,我们构建了富含异质结构的无定型FeMo基(a-FeMo)电催化剂,并系统评估了该催化剂的氮气还原和析氧反应性能.得益于无定型结构引起的活性位点数目的增多和异质结构引发的电子的重新分布,a-FeMo催化剂表现出优异的电化学催化性能.在-0.1 V vs.RHE的电势下,a-FeMo催化剂表现出29.15%的法拉第效率和71.78μg_(NH_(3)) mg_(cat.)^(-1) h^(-1)的氨气产率.这为合理设计具有低成本优势、高活性和长时间稳定性的优异催化剂提供了有益的参考.
