Mo_(2)B_(2)O_(2) MBene for Efficient Electrochemical CO Reduction to C_(2) Chemicals:Computational Exploration  

作　　者：Bikun Zhang Jianwen Jiang 

机构地区：[1]Department of Chemical and Biomolecular Engineering,National University of Singapore,Singapore 117576,Singapore

出　　处：《Energy & Environmental Materials》2024年第6期342-350,共9页能源与环境材料（英文）

基　　金：the A*STAR LCER-FI project(LCERFI01-0033 U2102d2006);the Ministry of Education of Singapore and the National University of Singapore(C-261-000-207-532/C-261-000-777-532 and R-279-000-574-114)for financial support.

摘　　要：Emerging as a new class of two-dimensional materials with atomically thin layers,MBenes have great potential for many important applications such as energy storage and electrocatalysis.Toward mitigating carbon footprint,there has been increasing interest in CO_(2)/CO conversion on MBenes,but mostly focused on C_(1) products.C^(2+) chemicals generally possess higher energy densities and wider applications than C_(1) counterparts.However,C–C coupling is technically challenging because of high energy requirement and currently few catalysts are suited for this process.Here,we explore electrochemical CO reduction reaction to C_(2) chemicals on Mo_(2)B_(2)O_(2) MBene via density-functional theory calculations.Remarkably,the most favorable CO–COH coupling is revealed to be a spontaneous and barrierless process,making Mo_(2)B_(2)O_(2) an efficient catalyst for C–C coupling.Among C_(1) and C_(2) chemicals,ethanol is predicted to be the primary product.Furthermore,by charge and bond analysis,it is unraveled that there exist significantly more unbonded electrons in the C atom of intermediate*COH than other C_(1) intermediates,which is responsible for the facile C–C coupling.From an atomic scale,this work provides microscopic insight into C–C coupling process and suggests Mo_(2)B_(2)O_(2) a promising catalyst for electrochemical CO reduction to C_(2) chemicals.

关 键 词：C_(2) chemicals C-C coupling density-functional theory MBene Mo2B2O2 

分 类 号：O646[理学—物理化学]