中文版 | English
Title

Reconciling the experimental and computational methanol electro-oxidation activity via potential-dependent kinetic mechanism analysis

Author
Corresponding AuthorChen,Ming; Wang,Haijiang
Publication Years
2022
DOI
Source Title
ISSN
2050-7488
EISSN
2050-7496
Abstract
The kinetic mechanism of the methanol oxidation reaction (MOR) has been controversial due to the lack of accurate monitoring technology and static calculation of the kinetic process, as well as the failure to consider the relationship between the free energy barriers and electrode potential. This work focused on Pt and PtRu catalysts and assessed the potential-dependent MOR kinetic process via metal-electrolyte models to reconcile the experimental and computational MOR activity. The obtained results demonstrate that the potential-dependent rate-determining steps (RDSs) change with the increase of electrode potential in the orders of (R3: CHO* → CHO* + H + e) → (R5: CHO* → CO* + H + e) → (R14: CO* + OH* → CO* + H + e), and (R4: CHO* → CHO* + H + e) → (R5: CHO* → CO* + H + e) → (R14: CO* + OH* → CO* + H + e), respectively, which is attributed to the variation in the adsorption of intermediates and strength of the electrochemical double layer (E). Furthermore, the potential-dependent coverage of intermediates and degree of rate control (DRC) in the MOR kinetic process draw support from microkinetic modeling. The experimental cyclic voltammograms and theoretical computation are reconciled with max absolute differences (Δ) of 0.020 and 0.023 mA cm for Pt and PtRu, respectively, giving evidence for the nature of higher MOR activity for PtRu. Importantly, our explicitly dynamic approach elucidates the potential-dependent MOR kinetic process at both the molecular and atomic levels and paves the way for the complex multi-electron reaction kinetic simulation.
URL[Source Record]
Indexed By
Language
English
SUSTech Authorship
Corresponding
Funding Project
Ministry of Education Key Laboratory of Energy Conversion and Storage Technologies[Y01406010] ; Guangdong Innovative and Entrepreneurial Research Team Program[2016ZT06N500] ; Guangdong Provincial Key Laboratory of Energy Materials for Electric Power[2018B030322001]
WOS Research Area
Chemistry ; Energy & Fuels ; Materials Science
WOS Subject
Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
WOS Accession No
WOS:000874878700001
Publisher
Scopus EID
2-s2.0-85141812912
Data Source
Scopus
Citation statistics
Cited Times [WOS]:0
Document TypeJournal Article
Identifierhttp://kc.sustech.edu.cn/handle/2SGJ60CL/411864
DepartmentDepartment of Mechanical and Energy Engineering
Affiliation
1.Harbin Institute of Technology,Harbin,150001,China
2.Department of Mechanical and Energy Engineering,Southern University of Science and Technology,Shenzhen,518055,China
3.Key Laboratory of Energy Conversion and Storage Technologies (Southern University of Science and Technology),Ministry of Education,Shenzhen,518055,China
First Author AffilicationDepartment of Mechanical and Energy Engineering;  Southern University of Science and Technology
Corresponding Author AffilicationDepartment of Mechanical and Energy Engineering;  Southern University of Science and Technology;  
Recommended Citation
GB/T 7714
Liu,Haijun,Sun,Fengman,Chen,Ming,et al. Reconciling the experimental and computational methanol electro-oxidation activity via potential-dependent kinetic mechanism analysis[J]. Journal of Materials Chemistry A,2022.
APA
Liu,Haijun,Sun,Fengman,Chen,Ming,&Wang,Haijiang.(2022).Reconciling the experimental and computational methanol electro-oxidation activity via potential-dependent kinetic mechanism analysis.Journal of Materials Chemistry A.
MLA
Liu,Haijun,et al."Reconciling the experimental and computational methanol electro-oxidation activity via potential-dependent kinetic mechanism analysis".Journal of Materials Chemistry A (2022).
Files in This Item:
There are no files associated with this item.
Related Services
Fulltext link
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Export to Excel
Export to Csv
Altmetrics Score
Google Scholar
Similar articles in Google Scholar
[Liu,Haijun]'s Articles
[Sun,Fengman]'s Articles
[Chen,Ming]'s Articles
Baidu Scholar
Similar articles in Baidu Scholar
[Liu,Haijun]'s Articles
[Sun,Fengman]'s Articles
[Chen,Ming]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[Liu,Haijun]'s Articles
[Sun,Fengman]'s Articles
[Chen,Ming]'s Articles
Terms of Use
No data!
Social Bookmark/Share
No comment.

Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.