Electrochemical conversion of CO_(2)(CO_(2)RR)into high-value fuel is identified as one of the promising approaches to achieve carbon neutrality.The synthesis of high-efficiency CO_(2)reduction electrocatalysts with h...Electrochemical conversion of CO_(2)(CO_(2)RR)into high-value fuel is identified as one of the promising approaches to achieve carbon neutrality.The synthesis of high-efficiency CO_(2)reduction electrocatalysts with high C_(2):C_(1) selectivity remains a field of intense interest.Previous studies have shown that the presence of Cu(I)is beneficial for the reduction of CO_(2)into C_(2)products.However,the stable presence of Cu(I)remains controversial,especially in the negative potential window.Here we report a simple and easily scalable catalyst precursor Cu_(2)(OH)_(3)Cl/C,which automatically forms in-situ chlorine-doped Cu/Cu_(2)O heterointerface during electrocatalysis.The catalyst not only exhibits a Faradaic efficiency of 33.03%but also provides a long-term stability of Cu^(+),gaining a stable electrolysis of 11 h,with an ethylene/methane ratio over 50.The experimental results and mechanistic studies confirm that the presence of Cl^(-)inhibits the reduction of Cu^(+),inducing the formation of Cu^(0)/Cu^(+),and reduces the reaction energy of the intermediate ^(*)CO dimerization,thereby facilitating the formation of C_(2)products.This work provides a feasible way to synthesize copper ions with long-term and stable positive charge in CO_(2)RR and expands a new way to synthesize ethylene industrial products in the future.展开更多
基金This work was financially supported by the Natural Science Foundation of Henan province(No.212300410281)the National Key Research and Development Program of China(No.2020YFA0406104)the National Natural Science Foundation of China(No.22001263).
文摘Electrochemical conversion of CO_(2)(CO_(2)RR)into high-value fuel is identified as one of the promising approaches to achieve carbon neutrality.The synthesis of high-efficiency CO_(2)reduction electrocatalysts with high C_(2):C_(1) selectivity remains a field of intense interest.Previous studies have shown that the presence of Cu(I)is beneficial for the reduction of CO_(2)into C_(2)products.However,the stable presence of Cu(I)remains controversial,especially in the negative potential window.Here we report a simple and easily scalable catalyst precursor Cu_(2)(OH)_(3)Cl/C,which automatically forms in-situ chlorine-doped Cu/Cu_(2)O heterointerface during electrocatalysis.The catalyst not only exhibits a Faradaic efficiency of 33.03%but also provides a long-term stability of Cu^(+),gaining a stable electrolysis of 11 h,with an ethylene/methane ratio over 50.The experimental results and mechanistic studies confirm that the presence of Cl^(-)inhibits the reduction of Cu^(+),inducing the formation of Cu^(0)/Cu^(+),and reduces the reaction energy of the intermediate ^(*)CO dimerization,thereby facilitating the formation of C_(2)products.This work provides a feasible way to synthesize copper ions with long-term and stable positive charge in CO_(2)RR and expands a new way to synthesize ethylene industrial products in the future.
