Modeling the effect of surface CO coverage on the electrocatalytic reduction of CO2 to CO on Pd surfaces

doi:10.1039/c8cp07427e

	Modeling the effect of surface CO coverage on the electrocatalytic reduction of CO2 to CO on Pd surfaces
	Liu, Hong1,2 ; Liu, Jian1 ; Yang, Bo1
	2019-05-21
发表期刊	PHYSICAL CHEMISTRY CHEMICAL PHYSICS (IF:2.9[JCR-2023],3.0[5-Year])
ISSN	1463-9076
卷号	21 期号:19 页码:9876-9882
发表状态	已发表
DOI	10.1039/c8cp07427e
摘要	Electrocatalytic reduction of CO2 has attracted considerable attention recently, and it was found experimentally that Pd could show activity for the electroreduction of CO2 to CO. However, theoretical studies showed that the adsorption of CO on Pd surfaces is strong and the coverage of CO is high, indicating that the interactions between the neighboring adsorbed CO and other reaction intermediates on the Pd surfaces cannot be neglected. Here, with density functional theory calculations and utilizing the Sabatier analysis method, we find that an adsorbate-adsorbate interaction is playing a crucial role in the modeling of the electrocatalytic reduction of CO2 to CO on Pd surfaces, whilst the reaction rates obtained by neglecting the interactions between the surface adsorbates are substantially lower than those reported in the experiments. Upon analyzing the interactions quantitatively and using a self-consistent iterative microkinetic modeling method, we find that the active site for CO2 electroreduction is Pd(111) at different potentials applied. Our modeling results provide a reasonable computational interpretation for the electroreduction of CO2 to CO on Pd.
收录类别	SCI ; SCIE ; EI
语种	英语
资助项目	Shanghai Young Eastern Scholar Program[QD2016049]
WOS研究方向	Chemistry ; Physics
WOS类目	Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS记录号	WOS:000473071200021
出版者	ROYAL SOC CHEMISTRY
EI入藏号	20201708550769
EI主题词	Carbon dioxide ; Computation theory ; Density functional theory ; Electrolytic reduction ; Iterative methods ; Reaction intermediates ; Reaction rates ; Surface reactions
EI分类号	Precious Metals:547.1 ; Computer Theory, Includes Formal Logic, Automata Theory, Switching Theory, Programming Theory:721.1 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Numerical Methods:921.6 ; Probability Theory:922.1
WOS关键词	ADSORBATE-ADSORBATE INTERACTIONS ; TOTAL-ENERGY CALCULATIONS ; ELECTROCHEMICAL REDUCTION ; CARBON-DIOXIDE ; UNDERSTANDING TRENDS ; COPPER ; HYDROGENATION ; HYDROCARBONS ; MORPHOLOGY ; EFFICIENCY
原始文献类型	Article
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/61123
专题	物质科学与技术学院_硕士生物质科学与技术学院_PI研究组_杨波组
通讯作者	Yang, Bo
作者单位	1.ShanghaiTech Univ, Sch Phys Sci & Technol, 393 Middle Huaxia Rd, Shanghai 201210, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
第一作者单位	物质科学与技术学院
通讯作者单位	物质科学与技术学院
第一作者的第一单位	物质科学与技术学院
推荐引用方式 GB/T 7714	Liu, Hong,Liu, Jian,Yang, Bo. Modeling the effect of surface CO coverage on the electrocatalytic reduction of CO2 to CO on Pd surfaces[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2019,21(19):9876-9882.
APA	Liu, Hong,Liu, Jian,&Yang, Bo.(2019).Modeling the effect of surface CO coverage on the electrocatalytic reduction of CO2 to CO on Pd surfaces.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,21(19),9876-9882.
MLA	Liu, Hong,et al."Modeling the effect of surface CO coverage on the electrocatalytic reduction of CO2 to CO on Pd surfaces".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 21.19(2019):9876-9882.