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作 者:Junyi Peng Qiang Zhang Yang Zhou Xiaohui Yang Fang Guo Junqiang Xu
机构地区:[1]College of Chemistry and Chemical Engineering,Chongqing University of Technology,Chongqing 400054,China [2]College of Chemistry and Chemical Engineering,Chongqing University,Chongqing 400044,China [3]Chongqing Institute of Green and Intelligent Technology,Chinese Academy of Sciences,Chongqing 4000714,China
出 处:《Journal of Energy Chemistry》2023年第10期108-115,I0005,共9页能源化学(英文版)
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)。
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.
关 键 词:Cold plasma CN vacancies Steric hindrance Bimetallic catalyst Low-carbon alcohol
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