摘要
Regulating the electronic structure of Bi-based materials by alloying engineering is promising to promote the electrocatalytic activity,but it remains some challenges to be solved.In this study,a facile electrochemical co-deposition strategy is developed to synthesize the bimetallic Bi_(9)Cu_(1) alloy nanosheet on carbon cloth(Bi_(9)Cu_(1)/CC),which represents a novel self-supporting electrode for the electrocatalytic carbon dioxide(CO_(2))reduction reaction(CO_(2)RR).The Bi_(9)Cu_(1)/CC catalyst has achieved a remarkable catalytic performance with high Faradaic efficiencies(FE)of over 90%for formate at wide potentials from-0.7 to-1.2 V vs.reversible hydrogen electrode(RHE).Moreover,the reversible Zn-CO_(2) battery can be driven by Bi_(9)Cu_(1)/CC cathode with a largest power density of 1.4 mW·cm^(-2),and superior operating stability.The systematic characterizations and electrochemical results confirm that the improved catalytic active sites,the enhanced mass/charge transport and the optimal reaction kinetics of Bi nanosheet are realized for CO_(2)RR by Cu alloying.In situ attenuated total reflection infrared(ATR-IR)result confirms the bimetallic Bi-Cu active sites prefer to follow the^(*)OCHO conversion pathway.The density functional theory(DFT)calculations suggest that the Cu alloying contributes to the increased density of states near the Fermi surface of Bi and the optimized adsorption of^(*)OCHO intermediates on the Bi sites,resulting in the excellent catalytic performance.
基金
supported by the National Natural Science Foundation of China(22205205)
Zhejiang Provincial Natural Science Foundation of China(No.LQ22B030008)
the Science Foundation of Zhejiang Sci-Tech University(ZSTU)under Grant(Nos.21062337-Y,22062312-Y).
