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

doi:10.1016/j.jcat.2020.11.014

	Developing micro-kinetic model for electrocatalytic reduction of carbon dioxide on copper electrode
	Xiang, Shi-Qin 1; Gao, Shu-Ting 1; Shi, Jun-Lin 1; Zhang, Wei 2; Zhao, Liu-Bin 1
刊名	JOURNAL OF CATALYSIS
	2021
卷号	393 页码:11-19
关键词	CO2 reduction reaction Reaction kinetics Reaction mechanism Product selectivity Density functional theory
ISSN号	0021-9517
DOI	10.1016/j.jcat.2020.11.014
通讯作者	Zhang, Wei(andyzhangwei@163.com) ; Zhao, Liu-Bin(lbzhao@swu.edu.cn)
英文摘要	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.
资助项目	National Natural Science Foundation of China[21603176] ; Chongqing Talents Program[CQYC201905041] ; Fundamental Research Funds for the Central Universities[XDJK2019C032] ; Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University)[201929] ; Chongqing Graduate Scientific Research Innovation Project[CYS18115]
WOS研究方向	Chemistry ; Engineering
语种	英语
出版者	ACADEMIC PRESS INC ELSEVIER SCIENCE
WOS记录号	WOS:000640936700002
内容类型	期刊论文
源URL	[http://119.78.100.138/handle/2HOD01W0/13341]
专题	中国科学院重庆绿色智能技术研究院
通讯作者	Zhang, Wei; Zhao, Liu-Bin
作者单位	1.Southwest Univ, Sch Chem & Chem Engn, Dept Chem, Chongqing 400715, Peoples R China 2.Chinese Acad Sci, Chongqing Inst Green & Intelligent Technol, Chongqing 400714, Peoples R China
推荐引用方式 GB/T 7714	Xiang, Shi-Qin,Gao, Shu-Ting,Shi, Jun-Lin,et al. Developing micro-kinetic model for electrocatalytic reduction of carbon dioxide on copper electrode[J]. JOURNAL OF CATALYSIS,2021,393:11-19.
APA	Xiang, Shi-Qin,Gao, Shu-Ting,Shi, Jun-Lin,Zhang, Wei,&Zhao, Liu-Bin.(2021).Developing micro-kinetic model for electrocatalytic reduction of carbon dioxide on copper electrode.JOURNAL OF CATALYSIS,393,11-19.
MLA	Xiang, Shi-Qin,et al."Developing micro-kinetic model for electrocatalytic reduction of carbon dioxide on copper electrode".JOURNAL OF CATALYSIS 393(2021):11-19.