The electrochemical CO_(2)reduction reaction(CO_(2)RR)to yield high-value added fuels and chemicals provides a promising approach towards global carbon neutrality.Constant endeavors have been devoted to the exploratio...The electrochemical CO_(2)reduction reaction(CO_(2)RR)to yield high-value added fuels and chemicals provides a promising approach towards global carbon neutrality.Constant endeavors have been devoted to the exploration of high-efficiency catalyst with rapid reaction kinetics,low energy input,and high selectivity.In addition to the maximum metal atomic utilization and unique catalytic performance of single-atom catalyst(SAC),dual-atomic-site catalysts(DASCs)offer more sophisticated and tunable atomic structure through the modulations of another adjacent metal atom,which can bring new opportunities for CO_(2)RR as a deeper extension of SACs and have recently aroused surging interest.In this review,we highlight the recent advances on DASCs for enhancing CO_(2)RR.First,the classification,synthesis,and identification of DASCs are provided according to the geometric structure and electronic configuration of dual-atomic active sites.Then,the catalytic applications of DASCs in CO_(2)RR are categorized based on marriage-type,hetero-nuclear,and homo-nuclear dual-atomic sites.Particularly,the structure-activity relationship of DASCs in CO_(2)RR is elaborately summarized through systematically analyzing the reaction pathways and the atom structures.Finally,the opportunities and challenges are proposed for inspiring the design of future DASCs with high structural accuracy and high CO_(2)RR activity and selectivity.展开更多
Electrochemical CO2 reduction(ECR)represents a promising strategy for utilizing CO2,an industrial waste,as an abundant and cheap carbon source for organic synthesis as well as storing intermittent renewable electricit...Electrochemical CO2 reduction(ECR)represents a promising strategy for utilizing CO2,an industrial waste,as an abundant and cheap carbon source for organic synthesis as well as storing intermittent renewable electricity from renewable sources.Efficient electrocatalysts allowing CO2 to be reduced selectively and actively are crucial since the ECR is a complex and sluggish process producing a variety of products.Metal-organic frameworks(MOFs)and covalentorganic frameworks(COFs)have emerged as versatile materials applicable in many fields due to their unique properties including high surface areas and tunable pore channels.Besides,the emerging reticular chemistry makes tuning their features on the atomic/molecular levels possible,thereby lending credence to the prospect of their utilizations.Herein,an overview of recent progress in employing framework material-based catalysts,including MOFs,COFs and their derivatives,for ECR is provided.The pertinent challenges,future trends,and opportunities associated with those systems are also discussed.展开更多
基金supported by Shandong Provincial Natural Science Foundation (ZR2019BB025)the Project of “20 items of University” of Jinan (2018GXRC031)the National Natural Science Foundation of China (22071172)
文摘The electrochemical CO_(2)reduction reaction(CO_(2)RR)to yield high-value added fuels and chemicals provides a promising approach towards global carbon neutrality.Constant endeavors have been devoted to the exploration of high-efficiency catalyst with rapid reaction kinetics,low energy input,and high selectivity.In addition to the maximum metal atomic utilization and unique catalytic performance of single-atom catalyst(SAC),dual-atomic-site catalysts(DASCs)offer more sophisticated and tunable atomic structure through the modulations of another adjacent metal atom,which can bring new opportunities for CO_(2)RR as a deeper extension of SACs and have recently aroused surging interest.In this review,we highlight the recent advances on DASCs for enhancing CO_(2)RR.First,the classification,synthesis,and identification of DASCs are provided according to the geometric structure and electronic configuration of dual-atomic active sites.Then,the catalytic applications of DASCs in CO_(2)RR are categorized based on marriage-type,hetero-nuclear,and homo-nuclear dual-atomic sites.Particularly,the structure-activity relationship of DASCs in CO_(2)RR is elaborately summarized through systematically analyzing the reaction pathways and the atom structures.Finally,the opportunities and challenges are proposed for inspiring the design of future DASCs with high structural accuracy and high CO_(2)RR activity and selectivity.
基金financially supported by the National Natural Science Foundation of China(21671096 and 11775105)Shenzhen Peacock Plan(KQTD2016022620054656)。
文摘Electrochemical CO2 reduction(ECR)represents a promising strategy for utilizing CO2,an industrial waste,as an abundant and cheap carbon source for organic synthesis as well as storing intermittent renewable electricity from renewable sources.Efficient electrocatalysts allowing CO2 to be reduced selectively and actively are crucial since the ECR is a complex and sluggish process producing a variety of products.Metal-organic frameworks(MOFs)and covalentorganic frameworks(COFs)have emerged as versatile materials applicable in many fields due to their unique properties including high surface areas and tunable pore channels.Besides,the emerging reticular chemistry makes tuning their features on the atomic/molecular levels possible,thereby lending credence to the prospect of their utilizations.Herein,an overview of recent progress in employing framework material-based catalysts,including MOFs,COFs and their derivatives,for ECR is provided.The pertinent challenges,future trends,and opportunities associated with those systems are also discussed.
