• 文献标题:   Free energy landscape of electrocatalytic CO2 reduction to CO on aqueous FeN4 center embedded graphene studied by ab initio molecular dynamics simulations
  • 文献类型:   Article
  • 作  者:   SHENG T, SUN SG
  • 作者关键词:  
  • 出版物名称:   CHEMICAL PHYSICS LETTERS
  • ISSN:   0009-2614 EI 1873-4448
  • 通讯作者地址:   Anhui Normal Univ
  • 被引频次:   3
  • DOI:   10.1016/j.cplett.2017.09.052
  • 出版年:   2017

▎ 摘  要

Experiments have found that the porphyrin-like FeN4 site in Fe-N-C materials is highly efficient for the electrochemical reduction of CO2 into CO. In this work, we investigated the reduction mechanisms on FeN4 embedded graphene layer catalyst with some explicit water molecules by combining the constrained ab initio molecular dynamics simulations and thermodynamic integrations. The reaction free energy and electron transfer in each elementary step were identified. The initial CO2 activation was identified to go through the first electron transfer to form adsorbed CO2 anion and the CO desorption was the rate limiting step in the overall catalytic cycle. (C) 2017 Elsevier B. V. All rights reserved.