Electrocatalytic Reduction of CO_(2)to CO with Almost 100%Faradaic Efficiency Using Oxygen-Vacancy Enriched Two-Dimensional MgO  

作　　者：Yu Han Sunggi An Xinyu Zhan Leiduan Hao Liang Xu Song Hong Dongmin Park Yuxin Chen Yiwen Xu Jiwen Zhao Xinyi Tan Alex W.Robertson Yousung Jung Zhenyu Sun 

机构地区：[1]State Key Laboratory of Organic-Inorganic Composites,College of Chemical Engineering,Beijing University of Chemical Technology,Beijing 100029 [2]Department of Chemical and Biomolecular Engineering(BK21four),Korea Advanced Institute of Science and Technology(KAIST),Daejeon 34141 [3]Beijing Key Laboratory of Environmental Science and Engineering,School of Materials Science and Engineering,Beijing Institute of Technology,Beijing 100081 [4]Department of Physics,University of Warwick,Coventry

出　　处：《CCS Chemistry》2024年第6期1477-1486,共10页中国化学会会刊（英文）

基　　金：supported by the National Natural Science Foundation of China(grant no.21972010);the National Key Research and Development Program of China(grant no.2022YFC2105900);the Beijing Natural Science Foundation(grant no.2192039);Fundamental Research Funds for the Central Universities(grant nos.JD2310,ZY2317,and buctrc202226);the NRF Korea(grant no.NRF-2019M3D3A1A01069099).

摘　　要：The design and development of cheap,abundant,and efficient electrocatalysts for selective CO_(2)electroreduction is highly desirable yet remains an ongoing challenge.Herein,we report on our discovery of the use of two-dimensional MgO rich in oxygen vacancies(VO)as an electrocatalyst for the efficient reduction of CO_(2)to yield CO in 1-butyl-3-methylimidazolium hexafluorophosphate dissolved in acetonitrile.The faradaic efficiency toward CO reaches as high as 99.6±0.24%with a current density of up to 40.8 mA cm−2.Density functional theory calculations illustrate that the introduction of VO in MgO substantially lowers the reaction-free energy for the transformation of ^(*)COO^(−) to ^(*)COOH,the potential determining step,which greatly boosts CO_(2)conversion efficiency.This work opens the way to realizing economic and efficient CO_(2)electrolysis of group II metals.

关 键 词：CO_(2)reduction electrocatalysis CO MGO ionic liquid oxygen-vacancy 

分 类 号：O64[理学—物理化学]