摘要
Electrochemical CO_(2) reduction reaction(CO_(2)RR)offers a promising strategy for CO_(2) conversion into value-added C2+products and facilitates the storage of renewable resources under comparatively mild conditions,but still remains a challenge.Herein,we propose the strategy of surface reconstruction and interface integration engineering to construct tuneable Cu^(0)-Cu^(+)-Cu^(2+)sites and oxygen vacancy oxide derived from CeO_(2)/CuO nanosheets(OD-CeO_(2)/CuO NSs)heterojunction catalysts and promote the activity and selectivity of CO_(2)RR.The optimized OD-CeO_(2)/CuO electrocatalyst shows the maximum Faradic efficiencies for C2+products in the H-type cell,which reaches 69.8%at−1.25 V versus a reversible hydrogen electrode(RHE).Advanced characterization analysis and density functional theory(DFT)calculations further confirm the fact that the existence of oxygen vacancies and Cu^(0)-Cu^(+)-Cu^(2+)sites modified with CeO_(2) is conducive to CO_(2) adsorption and activation,enhances the hydrogenation of^(*)CO to^(*)CHO,and further promotes the dimerization of^(*)CHO,thus promoting the selectivity of C2+generation.This facile interface integration and surface reconstruction strategy provides an ideal strategy to guide the design of CO_(2)RR electrocatalysts.
基金
Key Specialized Research and Development-International Science and Technology Cooperation Program in Henan Province,Grant/Award Number:231111520500
Program for Science&Technology Innovation Talents in Universities of Henan Province,Grant/Award Number:24HASTIT009
The 111 Project,Grant/Award Number:D17007
National Natural Science Foundation of China,Grant/Award Numbers:52072114,52271176
Henan Center for Outstanding Overseas Scientists,Grant/Award Number:GZS2022017。
