Insights into the adsorption/desorption of CO_(2) and CO on single-atom Fe-nitrogen-graphene catalyst under electrochemical environment

作     者：Jiejie Li Jian Liu Bo Yang Jiejie Li;Jian Liu;Bo Yang

作者机构：School of Physical Science and TechnologyShanghaiTech UniversityShanghai 201210China CAS Key Laboratory of Low-Carbon Conversion Science&EngineeringShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China University of Chinese Academy of SciencesBejing 100049China 

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

年 卷 期：2021年第30卷第2期

页      面：20-25,I0002页

核心收录：

学科分类：081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基　　金：financially supported by the National Natural Science Foundation for Young Scientists of China (21902102) the Shanghai Yangfan Youth Talent Program from STCSM (17YF1428900) the Major Program of National Natural Science Foundation of China (21991152) 

主　　题：Single atom catalyst Electroreduction of CO_(2) Adsorption CO Ab initio molecular dynamics 

摘      要：Single-atom metal-nitrogen-graphene(M-N-Gra) catalysts are promising materials for electrocatalytic CO_(2) reduction reaction(CO_(2) RR). However, theoretical explorations on such systems were greatly hindered because of the complexity in modeling solid/liquid interface and electrochemical environment. In the current work, we investigated two crucial processes in CO_(2) RR, i.e. adsorption and desorption of CO_(2) and CO at Fe-N_(4) center, with an explicit aqueous model. We used the ab initio molecular dynamics simulations associated with free energy sampling methods and electrode potential analysis to estimate the energetics under electrochemical environment, and found significant difference in aqueous solution compared with the same process in vacuum. The effect of applied electrode potential on the adsorption structures,charge transfer and free energies of both CO_(2) and CO on Fe-N-Gra was thoroughly discussed. These findings bring insights in fundamental understandings of the CO_(2) RR process under realistic conditions, and facilitate future design of efficient M-N-Gra-based CO_2 RR catalysts.