Electrochemical CO2 reduction over nitrogen-doped SnO2 crystal surfaces

作     者：Yuefeng Zhang Jianjun Liu Zengxi Wei Quanhui Liu Caiyun Wang Jianmin Ma Yuefeng Zhang;Jianjun Liu;Zengxi Wei;Quanhui Liu;Caiyun Wang;Jianmin Ma

作者机构：School of Physics and ElectronicsHunan UniversityChangsha 410082HunanChina ARC Centre of Excellence for Electromaterials Science. Intelligent Polymer Research InstituteAIIM FacilityUniversity of WollongongNorth WollongongNSW 2500Australia 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2019年第28卷第6期

页      面：22-30页

核心收录：

学科分类：0820[工学-石油与天然气工程] 0808[工学-电气工程] 07[理学] 0817[工学-化学工程与技术] 0807[工学-动力工程及工程热物理] 0827[工学-核科学与技术] 0703[理学-化学] 0702[理学-物理学] 

基　　金：supported by the National Natural Science Foundation of China (51302079) the Natural Science Foundation of Hunan Province (Grant No. 2017JJ1008) 

主　　题：CO2 reduction reaction SnO2 Crystal surface Electrocatalysis First principles 

摘      要：Crystal planes of a catalyst play crucial role in determining the electrocatalytic performance for CO2 reduction.The catalyst SnO2 can convert CO2 molecules into valuable formic acid(HCOOH).Incorporating heteroatom N into SnO2 further improves its catalytic activity.To understand the mechanism and realize a highly efficient CO2-to-HCOOH conversion,we used density functional theory(DFT)to calculate the free energy of CO2 reduction reactions(CO2RR)on different crystal planes of N-doped SnO2(N-SnO2).The results indicate that N-SnO2 lowered the activation energy of intermediates leading to a better catalytic performance than pure SnO2.We also discovered that the N-Sn O2 (211)plane possesses the most suitable free energy during the reduction process,exhibiting the best catalytic ability for the CO2-to-HCOOH conversion.The intermediate of CO2RR on N-SnO2 is HCOO*or COOH* instead of OCHO*.These results may provide useful insights into the mechanism of CO2RR,and promote the development of heteroatomdoped catalyst for efficient CO2RR.