Abstract
Electrocatalysis of CO2 reduction reaction is an effective way to convert CO2 into high value-added prod-ucts,but the selectivity of Cu-based catalysts for C2+products needs to be improved due to the high energy barrier of C-C coupling.Therefore,a viable catalyst design strategy to decrease energy barrier of C-C coupling should be put forward.Here,a nanocavity-enriched CuPd single atom alloy(CuPd SAA)catalyst is designed to promote C-C coupling process.The faradaic efficiency of CuPd SAA for ethylene and C2+reaches 75.6％and 85.7％at-0.7 V versus reversible hydrogen electrode(RHE),respectively.Based on the results given by in situ characterization,the porous hollow structure dramatically increases the ratio of the linear-bond*CO,thus enhancing the faradaic efficiency for ethylene.Density functional theory(DFT)calculation reveals that the Pd doping can regulate the electronic structure of neighboring Cu atoms to decrease the energy barrier of C-C coupling,further improving the faradaic efficiency.This work provides a new idea for designing catalyst with high selectivity for ethylene.
基金项目
National Natural Science Foundation of China(50835002)
National Natural Science Foundation of China(51105102)
NETL
NSTL
万方数据