Although many catalysts have been reported for the CO_(2)electroreduction to C_(1)or C_(2)chemicals,the insufficient understanding of fundamental correlations among different products still hinders the development of ...Although many catalysts have been reported for the CO_(2)electroreduction to C_(1)or C_(2)chemicals,the insufficient understanding of fundamental correlations among different products still hinders the development of universal catalyst design strategies.Herein,we first discover that the surface*CO coverage is stable over a wide potential range and reveal a linear correlation between the partial current densities of CH_(4)and C_(2)products in this potential range,also supported by the theoretical kinetic analysis.Based on the mechanism that*CHO is the common intermediate in the formation of both CH_(4)(*CHO→CH4)and C_(1)(*CHO+*CO→C_(2)),we then unravel that this linear correlation is universal and the slope can be varied by tuning the surface*H or*CO coverage to promote the selectivity of CH_(4)or C_(2)products,respectively.As proofs-of-concept,using carbon-coated Cu particles,the surface*H coverage can be increased to enhance CH_(4)production,presenting a high CO_(2)-to-CH_(4)Faradaic efficiency(FE_(CH_(4))~52%)and an outstanding CH_(4)partial current density of-337 m A cm;.On the other hand,using an Agdoped Cu catalyst,the CO_(2)RR selectivity is switched to the C_(2)pathway,with a substantially promoted FE;of 79%and a high partial current density of-421 m A cm;.Our discovery of tuning intermediate coverages suggests a powerful catalyst design strategy for different CO_(2)electroreduction pathways.展开更多
基金supported by the National Key Research and Development Program of China(2018YFA0209401 and 2017YFA0206901)the National Natural Science Foundation of China(22025502 and 21975051)+1 种基金the Science and Technology Commission of Shanghai Municipality(21DZ1206800,19XD1420400)the Shanghai Municipal Education Commission(2019-01-07-00-07-E00045)。
文摘Although many catalysts have been reported for the CO_(2)electroreduction to C_(1)or C_(2)chemicals,the insufficient understanding of fundamental correlations among different products still hinders the development of universal catalyst design strategies.Herein,we first discover that the surface*CO coverage is stable over a wide potential range and reveal a linear correlation between the partial current densities of CH_(4)and C_(2)products in this potential range,also supported by the theoretical kinetic analysis.Based on the mechanism that*CHO is the common intermediate in the formation of both CH_(4)(*CHO→CH4)and C_(1)(*CHO+*CO→C_(2)),we then unravel that this linear correlation is universal and the slope can be varied by tuning the surface*H or*CO coverage to promote the selectivity of CH_(4)or C_(2)products,respectively.As proofs-of-concept,using carbon-coated Cu particles,the surface*H coverage can be increased to enhance CH_(4)production,presenting a high CO_(2)-to-CH_(4)Faradaic efficiency(FE_(CH_(4))~52%)and an outstanding CH_(4)partial current density of-337 m A cm;.On the other hand,using an Agdoped Cu catalyst,the CO_(2)RR selectivity is switched to the C_(2)pathway,with a substantially promoted FE;of 79%and a high partial current density of-421 m A cm;.Our discovery of tuning intermediate coverages suggests a powerful catalyst design strategy for different CO_(2)electroreduction pathways.
