The local coordination environment of catalysts has been investigated ftor an extended period to obtain enhanced catalytic performance.Especially with the advancement of single-atom catalysts(SACs),research on the coo...The local coordination environment of catalysts has been investigated ftor an extended period to obtain enhanced catalytic performance.Especially with the advancement of single-atom catalysts(SACs),research on the coordination environment has been advanced to the atomic level.The surrounding coordination atoms of central metal atoms play important roles in their catalytic activity,selectivity and stability.In recent years,remarkable improvements of the catalytic performance of SACs have been achieved by the tailoring of coordination atoms,coordination numbers and second-or higher-coordination shells,which provided new opportunities for the further development of SACs.In this review,the characterization of coordination environment,tailoring of the local coordination environment,and their related adjustable catalytic performance will be discussed.We hope this review will provide new insights on further research of SACs.展开更多
The development of efficient and cost-effective catalysts to catalyze a wide variety of electrochemical reactions is key to realize the large-scale applicati on of ren ewable and clean en ergy tech no logies.Owing to ...The development of efficient and cost-effective catalysts to catalyze a wide variety of electrochemical reactions is key to realize the large-scale applicati on of ren ewable and clean en ergy tech no logies.Owing to the maximum atom-utilization efficie ncy and unique electronic and geometric structures,single atom catalysts(SACs)have exhibited superior performance in various catalytic systems.Recently,assembled from the function alized orga nic lin kers and metal no des,metal-organic frameworks(MOFs)with ultrafi ne porosity have received treme ndous attention as precursors or self-sacrificing templates for preparing porous SACs.Here,the recent advances toward the synthesis strategies for using MOF precursors/templates to con struct SACs are systematically summarized with special emphasis on the types of central metal sites.The electrochemical applications of these recently emerged MOF-derived SACs for various energy-conversion processes,such as oxygen reduction/evolution reaction(ORR/OER),hydrogen evolution reaction(HER),and CO2 reduction reaction(CO2RR),are also discussed and reviewed.Fin ally,the curre nt challe nges and prospects regardi ng the developme nt of MOF-derived SACs are proposed.展开更多
In recent decades,the environmental protection and long-term sustainability have become the focus of attention due to the increasing pollution generated by the intense industrialization.To overcome these issues,enviro...In recent decades,the environmental protection and long-term sustainability have become the focus of attention due to the increasing pollution generated by the intense industrialization.To overcome these issues,environmental catalysis has increasingly been used to solve the negative impact of pollutants emission on the global environment and human health.Supported platinum-metal-group(PGM)materials are commonly utilized as the state-of-the-art catalysts to eliminate gaseous pollutants but large quantities of PGMs are required.By comparison,single-atom site catalysts(SACs)have attracted much attention in catalysis owing to their 100%atom efficiency and unique catalytic performances towards various reactions.Over the past decade,we have witnessed burgeoning interests of SACs in heterogeneous catalysis.However,to the best of our knowledge,the systematic summary and analysis of SACs in catalytic elimination of environmental pollutants has not yet been reported.In this paper,we summarize and discuss the environmental catalysis applications of SACs.Particular focus was paid to automotive and stationary emission control,including model reaction(CO oxidation,NO reduction and hydrocarbon oxidation),overall reaction(three-way catalytic and diesel oxidation reaction),elimination of volatile organic compounds(formaldehyde,benzene,and toluene),and removal/decomposition of other pollutants(Hg0 and SO3).Perspectives related to further challenges,directions and design strategies of single-atom site catalysts in environmental catalysis were also provided.展开更多
基金the National Key R&D Program of China(Nos.2018YFA0702003 and 2016YFA0202801)the National Natural Science Foundation of China(Nos.51631001,51872030,21890383,21671117,21871159,21901135,51702016,and 51501010)+1 种基金Beijing Institute of Technology Research Fund Program for Young ScholarsBeijing Municipal Science&Technology Commission(No.Z191100007219003).
文摘The local coordination environment of catalysts has been investigated ftor an extended period to obtain enhanced catalytic performance.Especially with the advancement of single-atom catalysts(SACs),research on the coordination environment has been advanced to the atomic level.The surrounding coordination atoms of central metal atoms play important roles in their catalytic activity,selectivity and stability.In recent years,remarkable improvements of the catalytic performance of SACs have been achieved by the tailoring of coordination atoms,coordination numbers and second-or higher-coordination shells,which provided new opportunities for the further development of SACs.In this review,the characterization of coordination environment,tailoring of the local coordination environment,and their related adjustable catalytic performance will be discussed.We hope this review will provide new insights on further research of SACs.
基金This work was supported by the National Key R&D Program of China(No.2016YFA0202801)the National Natural Science Foundation of China(Nos.21671117,21871159,21890383,and 21676018)and the China Postdoctoral Science Foundation(No.2017M610864).
文摘The development of efficient and cost-effective catalysts to catalyze a wide variety of electrochemical reactions is key to realize the large-scale applicati on of ren ewable and clean en ergy tech no logies.Owing to the maximum atom-utilization efficie ncy and unique electronic and geometric structures,single atom catalysts(SACs)have exhibited superior performance in various catalytic systems.Recently,assembled from the function alized orga nic lin kers and metal no des,metal-organic frameworks(MOFs)with ultrafi ne porosity have received treme ndous attention as precursors or self-sacrificing templates for preparing porous SACs.Here,the recent advances toward the synthesis strategies for using MOF precursors/templates to con struct SACs are systematically summarized with special emphasis on the types of central metal sites.The electrochemical applications of these recently emerged MOF-derived SACs for various energy-conversion processes,such as oxygen reduction/evolution reaction(ORR/OER),hydrogen evolution reaction(HER),and CO2 reduction reaction(CO2RR),are also discussed and reviewed.Fin ally,the curre nt challe nges and prospects regardi ng the developme nt of MOF-derived SACs are proposed.
基金This work was supported by the China Postdoctoral Science Foundation(No.2020M670355)the National Key R&D Program of China(No.2018YFA0702003)+2 种基金the National Natural Science Foundation of China(Nos.21890383,21671117,and 21871159)the Science and Technology Key Project of Guangdong Province of China(No.2020B010188002)Beijing Municipal Science&Technology Commission(No.Z191100007219003).
文摘In recent decades,the environmental protection and long-term sustainability have become the focus of attention due to the increasing pollution generated by the intense industrialization.To overcome these issues,environmental catalysis has increasingly been used to solve the negative impact of pollutants emission on the global environment and human health.Supported platinum-metal-group(PGM)materials are commonly utilized as the state-of-the-art catalysts to eliminate gaseous pollutants but large quantities of PGMs are required.By comparison,single-atom site catalysts(SACs)have attracted much attention in catalysis owing to their 100%atom efficiency and unique catalytic performances towards various reactions.Over the past decade,we have witnessed burgeoning interests of SACs in heterogeneous catalysis.However,to the best of our knowledge,the systematic summary and analysis of SACs in catalytic elimination of environmental pollutants has not yet been reported.In this paper,we summarize and discuss the environmental catalysis applications of SACs.Particular focus was paid to automotive and stationary emission control,including model reaction(CO oxidation,NO reduction and hydrocarbon oxidation),overall reaction(three-way catalytic and diesel oxidation reaction),elimination of volatile organic compounds(formaldehyde,benzene,and toluene),and removal/decomposition of other pollutants(Hg0 and SO3).Perspectives related to further challenges,directions and design strategies of single-atom site catalysts in environmental catalysis were also provided.
