4.8 Article

Developing micro-kinetic model for electrocatalytic reduction of carbon dioxide on copper electrode

期刊

JOURNAL OF CATALYSIS
卷 393, 期 -, 页码 11-19

出版社

ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2020.11.014

关键词

CO2 reduction reaction; Reaction kinetics; Reaction mechanism; Product selectivity; Density functional theory

资金

  1. National Natural Science Foundation of China [21603176]
  2. Chongqing Talents Program [CQYC201905041]
  3. Fundamental Research Funds for the Central Universities [XDJK2019C032]
  4. Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University) [201929]
  5. Chongqing Graduate Scientific Research Innovation Project [CYS18115]

向作者/读者索取更多资源

A micro-kinetic model was developed to study the influences of solution pH and electrode potential on the reaction rate, pathways, and product distribution of electrocatalytic CO2 conversion. The study investigated competing proton-electron transfer pathways and pathways controlled by thermodynamics and kinetics, showing that different mechanisms occur at different pH levels and electrode potentials. Manipulating solution pH and electrode potential can effectively modulate the electrocatalytic activity and selectivity.
A micro-kinetic model combining electrochemical rate theory and first-principles simulation is devel-oped to study the influences of solution pH and electrode potential on reaction rate, reaction pathways, and product distribution of electrocatalytic CO2 conversion. Two critical issues involved in electrochem-ical reaction mechanism are investigated: 1) competing concerted and sequential proton-electron trans-fer pathways, 2) competing thermodynamics-controlled and kinetics-controlled pathways. Our results show that the electrochemical reduction of CO2 to CO and HCOOH adopts a thermodynamics-controlled CPET mechanism at low pH, while follows a kinetics-controlled SPET mechanism at high pH. The electrocatalytic activity and selectivity can be effectively modulated by manipulating of solution pH and electrode potential. It is demonstrated that HCOOH is the main product at low overpotential while CO becomes the main product at high overpotential. In addition, increasing pH is conducive to improving the Faradic efficiency of HCOOH production and suppressing the hydrogen evolution reaction. (C) 2020 Elsevier Inc. All rights reserved.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.8
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

暂无数据
暂无数据