Electrochemical reduction of CO_(2) to value-added chemicals holds promise for carbon utilization and renewable electricity storage.However,selective CO_(2) reduction to multi-carbon fuels remains a significant challe...Electrochemical reduction of CO_(2) to value-added chemicals holds promise for carbon utilization and renewable electricity storage.However,selective CO_(2) reduction to multi-carbon fuels remains a significant challenge.Here,we report that B/N-doped sp^(3)/sp^(2) hybridized nanocarbon(BNHC),consisting of ultra-small nanoparticles with a sp^(3) carbon core covered by a sp^(2) carbon shell,is an efficient electrocatalyst for electrochemical reduction of CO_(2) to ethanol at relatively low overpotentials.CO_(2) reduction occurs with a Faradaic efficiency of 58.8%-69.1% for ethanol and acetate production at -0.5∼-0.6 V(vs.RHE),among which 51.6%-56.0% is for ethanol.The high selectivity for ethanol is due to the integrated effect of sp^(3)/sp^(2) carbon and B/N doping.Both sp^(3) carbon and B/N doping contribute to enhanced ethanol production with sp^(2) carbon reducing the overpotential for CO_(2) reduction to ethanol.展开更多
基金supported by National Natural Science Foundation of China(Nos.22076019 and 21707016)The Youth Talent Support Program of Liaoning Province(No.XLYC2007069)U.S.Department of Energy(DOE),Office of Basic Energy Sciences under Award(No.DE-SCO015739).
文摘Electrochemical reduction of CO_(2) to value-added chemicals holds promise for carbon utilization and renewable electricity storage.However,selective CO_(2) reduction to multi-carbon fuels remains a significant challenge.Here,we report that B/N-doped sp^(3)/sp^(2) hybridized nanocarbon(BNHC),consisting of ultra-small nanoparticles with a sp^(3) carbon core covered by a sp^(2) carbon shell,is an efficient electrocatalyst for electrochemical reduction of CO_(2) to ethanol at relatively low overpotentials.CO_(2) reduction occurs with a Faradaic efficiency of 58.8%-69.1% for ethanol and acetate production at -0.5∼-0.6 V(vs.RHE),among which 51.6%-56.0% is for ethanol.The high selectivity for ethanol is due to the integrated effect of sp^(3)/sp^(2) carbon and B/N doping.Both sp^(3) carbon and B/N doping contribute to enhanced ethanol production with sp^(2) carbon reducing the overpotential for CO_(2) reduction to ethanol.