The electrocatalytic carbon dioxide reduction reaction(CO_(2) RR)producing HCOOH and CO is one of the most promising approaches for storing renewable electricity as chemical energy in fuels.SnO_(2) is a good catalyst ...The electrocatalytic carbon dioxide reduction reaction(CO_(2) RR)producing HCOOH and CO is one of the most promising approaches for storing renewable electricity as chemical energy in fuels.SnO_(2) is a good catalyst for CO_(2)-to-HCOOH or CO_(2)-to-CO conversion,with different crystal planes participating the catalytic process.Among them,(110)surface SnO_(2) is very stable and easy to synthesisze.By changing the ratio of Sn:O for SnO_(2)(110),we have two typical SnO_(2) thin films:fully oxidized(stoichiometric)and partially reduced.In this work,we are concerned with different metals(Fe,Co,Ni,Cu,Ru,Rh,Pd,Ag,Os,Ir,Pt,and Au)-doped SnO_(2)(110)with different activity and selectivity for CO_(2) RR.All these changes are manipulated by adjusting the ratio of Sn:O in(110)surface.The results show that stochiometric and reduced Cu/Ag doped SnO_(2)(110)have different selectivity for CO_(2) RR.More specifically,stochiometric Cu/Ag-doped SnO_(2)(110)tends to generate CO(g).Meanwhile,the reduced surface tends to generate HCOOH(g).Moreover,we also considered the competitive hydrogen evolution reaction(HER).The catalysts SnO_(2)(110)doped by Ru,Rh,Pd,Os,Ir,and Pt have high activity for HER,and others are good catalysts for CO_(2) RR.展开更多
基金supported by the Ministry of Science and Technology(No.2017YFA0204904,No.2016YFA0400900,and No.2016YFA0200600)the National Natural Science Foundation of China(No.21973086 and No.21633006)。
文摘The electrocatalytic carbon dioxide reduction reaction(CO_(2) RR)producing HCOOH and CO is one of the most promising approaches for storing renewable electricity as chemical energy in fuels.SnO_(2) is a good catalyst for CO_(2)-to-HCOOH or CO_(2)-to-CO conversion,with different crystal planes participating the catalytic process.Among them,(110)surface SnO_(2) is very stable and easy to synthesisze.By changing the ratio of Sn:O for SnO_(2)(110),we have two typical SnO_(2) thin films:fully oxidized(stoichiometric)and partially reduced.In this work,we are concerned with different metals(Fe,Co,Ni,Cu,Ru,Rh,Pd,Ag,Os,Ir,Pt,and Au)-doped SnO_(2)(110)with different activity and selectivity for CO_(2) RR.All these changes are manipulated by adjusting the ratio of Sn:O in(110)surface.The results show that stochiometric and reduced Cu/Ag doped SnO_(2)(110)have different selectivity for CO_(2) RR.More specifically,stochiometric Cu/Ag-doped SnO_(2)(110)tends to generate CO(g).Meanwhile,the reduced surface tends to generate HCOOH(g).Moreover,we also considered the competitive hydrogen evolution reaction(HER).The catalysts SnO_(2)(110)doped by Ru,Rh,Pd,Os,Ir,and Pt have high activity for HER,and others are good catalysts for CO_(2) RR.
