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 

机构地区：[1]School of Physical Science and Technology,ShanghaiTech University,Shanghai 201210,China [2]CAS Key Laboratory of Low-Carbon Conversion Science&Engineering,Shanghai Advanced Research Institute,Chinese Academy of Sciences,Shanghai 201210,China [3]University of Chinese Academy of Sciences,Bejing 100049,China

出　　处：《Journal of Energy Chemistry》2021年第2期20-25,I0002,共7页能源化学（英文版）

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)。

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.

关 键 词：Single atom catalyst Electroreduction of CO_(2) Adsorption CO Ab initio molecular dynamics 

分 类 号：O643.36[理学—物理化学]