南方科技大学知识苑(SUSTech KC): Reconciling the experimental and computational methanol electro-oxidation activity via potential-dependent kinetic mechanism analysis

题名	Reconciling the experimental and computational methanol electro-oxidation activity via potential-dependent kinetic mechanism analysis
作者	Liu，Haijun 1,2,3; Sun，Fengman1,2,3 ; Chen，Ming2,3 ; Wang，Haijiang2,3
通讯作者	Chen，Ming; Wang，Haijiang
发表日期	2022
DOI	10.1039/d2ta07190h
发表期刊	Journal of Materials Chemistry A 影响因子和分区
ISSN	2050-7488
EISSN	2050-7496
摘要	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.
相关链接	[Scopus记录]
收录类别	SCI
语种	英语
学校署名	通讯
资助项目	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研究方向	Chemistry ; Energy & Fuels ; Materials Science
WOS类目	Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
WOS记录号	WOS:000874878700001
出版者	ROYAL SOC CHEMISTRY
Scopus记录号	2-s2.0-85141812912
来源库	Scopus
引用统计	被引频次[WOS]：5
成果类型	期刊论文
条目标识符	http://sustech.caswiz.com/handle/2SGJ60CL/411864
专题	工学院_机械与能源工程系
作者单位	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
第一作者单位	机械与能源工程系; 南方科技大学
通讯作者单位	机械与能源工程系; 南方科技大学
推荐引用方式 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).