摘要
Electrocatalytic CO_(2)reduction reaction to low-carbon alcohol is a challenging task,especially high selectivity for ethanol,which is mainly limited by the regulation of reaction intermediates and subsequent C–C coupling.A Cu-Co bimetallic catalyst with CN vacancies is successfully developed by H_(2)cold plasma toward a high-efficiency CO_(2)RR into low-carbon alcohol.The Cu-Co PBA-V_(CN)(Prussian blue analogues with CN vacancies)electrocatalyst yields methanol and ethanol as major products with a total low-carbon alcohol FE of 83.8%(methanol:39.2%,ethanol:44.6%)at-0.9 V vs.RHE,excellent durability(100 h)and a small onset potential of-0.21 V.ATR-SEIRAS(attenuated total internal reflection surface enhanced infrared absorption spectroscopy)and DFT(density functional theory)reveal that the steric hindrance of V_(CN)can enhance the CO generation from*COOH,and the C–C coupling can also be increased by CO spillover on uniformly dispersed Cu atoms.This work provides a strategy for the design and preparation of electrocatalysts for CO_(2)RR into low-carbon alcohol products and highlights the impact of catalyst steric hindrance to catalytic performance.
基金
the National Natural Science Foundation of China(21902017)
the Project of Fundamental Research and Frontier Exploration of Chongqing(cstc2019jcyj-msxmX0052)
the Foundation of Technological Innovation and Application Development of Chongqing(cstc2021jscx-msxmX0308)
the Key Projects of Technology Innovation and Application Development of Chongqing(cstc2019jscx-gksbX0022)
the Banan Science and Technology Foundation of Chongqing(2018TJ03,2020QC374)
the Major Project of Science and Technology Research Program of Chongqing Education Commission of China(KJZD-M202101101)
the Youth Project of Science and Technology Research Program of Chongqing Education Commission of China(KJQN20211107)
the Scientific Research Foundation of Chongqing University of Technology(2020ZDZ022)。