Electroreduction of carbon dioxide into fuels and feedstocks with renewable energy is an attractive route to mitigate carbon emission and solve energy crisis.However,how to improve the selectivity of high‐value multi...Electroreduction of carbon dioxide into fuels and feedstocks with renewable energy is an attractive route to mitigate carbon emission and solve energy crisis.However,how to improve the selectivity of high‐value multicarbon products is still challenging.Here,we demonstrate that the high‐index crystalline surface of copper could be designed and obtained through a simple square‐wave potential treatment on copper nanowires,which is beneficial to improve the selectivity of multi‐carbon products,especially the reaction route towards ethylene.The Faradaic efficiency of C_(2+)products can reach nearly 60%,and hydrogen can be suppressed to below 20%.Density functional theory(DFT)calculations reveal that(311)high‐index facet can activate CO_(2) effectively and promote adsorption of the*COCOH intermediate on copper for ethylene formation,therefore improves the selectivity of ethylene and inhibits the competing hydrogen evolution reaction.This method can be extended to the design of other catalytic systems and has inspirations for other electrochemical catalytic reactions.展开更多
基金supported by the National Key Research and Development Project(2018YFB1502401 and 2018YFA0702002)the Program for Changjiang Scholars and Innovation Research Team in the University(IRT1205)+1 种基金the Fundamental Research Funds for the Central Universitiesthe long-term subsidy mechanism from the Ministry of Finance and the Ministry of Education of China。
基金National Natural Science Foundation of China,Grant/Award Number:21902009National Key Research and Development Project,Grant/Award Numbers:2018YFB1502401,2018YFA0702002+2 种基金Royal Society and the Newton Fund through the Newton Advanced Fellowship Award,Grant/Award Number:NAF\R1\191294Program for Changjiang Scholars and Innovation Research Team in the University,Grant/Award Number:IRT1205Fundamental Research Funds for the Central Universities,and the longterm subsidy mechanism from the Ministry of Finance and the Ministry of Education of PRC。
文摘Electroreduction of carbon dioxide into fuels and feedstocks with renewable energy is an attractive route to mitigate carbon emission and solve energy crisis.However,how to improve the selectivity of high‐value multicarbon products is still challenging.Here,we demonstrate that the high‐index crystalline surface of copper could be designed and obtained through a simple square‐wave potential treatment on copper nanowires,which is beneficial to improve the selectivity of multi‐carbon products,especially the reaction route towards ethylene.The Faradaic efficiency of C_(2+)products can reach nearly 60%,and hydrogen can be suppressed to below 20%.Density functional theory(DFT)calculations reveal that(311)high‐index facet can activate CO_(2) effectively and promote adsorption of the*COCOH intermediate on copper for ethylene formation,therefore improves the selectivity of ethylene and inhibits the competing hydrogen evolution reaction.This method can be extended to the design of other catalytic systems and has inspirations for other electrochemical catalytic reactions.
