AUTHOR=Sun Xiaoxu 

TITLE=Achieving Selective and Efficient Electrocatalytic Activity for CO2 Reduction on N-Doped Graphene

JOURNAL=Frontiers in Chemistry

VOLUME=Volume 9 - 2021

YEAR=2021

URL=https://www.frontiersin.org/journals/chemistry/articles/10.3389/fchem.2021.734460

DOI=10.3389/fchem.2021.734460

ISSN=2296-2646

ABSTRACT=The CO2 electrochemical reduction reaction (CO2RR) has been a promising conversion method for CO2 utilization. Currently, the lack of electrocatalysts with favorable stability and high efficiency hindered the development of CO2RR. Nitrogen doped graphene nanocarbons have great promise in replacing metal catalysts for catalyzing CO2RR. By using density functional theory (DFT) method, the catalytic mechanism and activity of CO2RR on 11 types of nitrogen doped graphene have been explored. The free energy analysis reveals that the zigzag pyridinic N and zigzag graphitic N doped graphene possess outstanding catalytic activity and selectivity for HCOOH production with energy barrier of 0.38 and 0.39 eV, respectively. CO is the competitive product since its free energy lies only about 0.20 eV above HCOOH. The minor product is CH3OH and CH4 for the zigzag pyridinic N doped graphene, HCHO for zigzag graphitic N doped graphene, respectively. However, for Z-pyN, CO2RR is passivated by too strong HER. Meanwhile, by modifying the pH value of electrolyte, Z-GN could be selected as a promising nonmetal electrocatalyst for CO2RR in generating HCOOH.