Validation of H2O2-mediated pathway model for elucidating oxygen reduction mechanism: Experimental evidences and theoretical simulations | |
Yin, Fengjun1,3; Liu, Yuan1; Wang, Sha1; Wang, Chuan2; Liu, Hong1 | |
刊名 | ELECTROCHIMICA ACTA |
2019-08-01 | |
卷号 | 313页码:378-388 |
关键词 | Oxygen reduction reaction H2O2-Mediated strategy Pathway model Tendency Electrochemical kinetics |
ISSN号 | 0013-4686 |
DOI | 10.1016/j.electacta.2019.04.155 |
通讯作者 | Liu, Hong(liuhong@cigit.ac.cn) |
英文摘要 | Oxygen reduction reaction (ORR) on an electrode is a multi-step process that involves both H2O and H2O2 as final products, and the mechanism focusing on the productions of them has yet to be elucidated. In this study, simplifying the multi-step process of ORR by means of rate-limiting step (RLS) led to a H2O2-mediated pathway model. This model accounts for the productions of H2O and H2O2 by the H2O2-mediated strategy existing in 2 x 2e pathway. The model links the overall reaction with RLS and serves to establish the electrochemical kinetic equations of sub-processes. A tending degree (R-H2O2) quantifying the "tendency" toward H2O and H2O2 was proposed. Finally, a mathematic approach based on the H(2)O(2-)mediated strategy are formed and well account for two common ORR behaviors: i) H2O2 is inevitably produced on most of the ORR catalysts, including Pt-based catalysts, and ii) the tendency is regulable from external factors rather than merely determined by the intrinsic properties of catalysts. Furthermore, this model is fully validated by the kinetic simulations of the ORR behaviors in the rotating ring-disk electrode (RRDE) system. This study opens a way to advance the ORR applications by regulating the tendency, and may facilitate the comprehensive understanding of ORR mechanism. (C) 2019 Published by Elsevier Ltd. |
资助项目 | National Natural Science Foundation of China[51525805] ; National Natural Science Foundation of China[51727812] ; National Natural Science Foundation of China[51808526] |
WOS研究方向 | Electrochemistry |
语种 | 英语 |
出版者 | PERGAMON-ELSEVIER SCIENCE LTD |
WOS记录号 | WOS:000470236500040 |
内容类型 | 期刊论文 |
源URL | [http://119.78.100.138/handle/2HOD01W0/8121] |
专题 | 中国科学院重庆绿色智能技术研究院 |
通讯作者 | Liu, Hong |
作者单位 | 1.Chinese Acad Sci, Chongqing Inst Green & Intelligent Technol, Key Lab Reservoir Aquat Environm, Chongqing 400714, Peoples R China 2.Guangzhou Univ, Inst Environm Res Greater Bay, Minist Educ, Key Lab Water Qual & Conservat Pearl River Delta, Guangzhou 510006, Guangdong, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China |
推荐引用方式 GB/T 7714 | Yin, Fengjun,Liu, Yuan,Wang, Sha,et al. Validation of H2O2-mediated pathway model for elucidating oxygen reduction mechanism: Experimental evidences and theoretical simulations[J]. ELECTROCHIMICA ACTA,2019,313:378-388. |
APA | Yin, Fengjun,Liu, Yuan,Wang, Sha,Wang, Chuan,&Liu, Hong.(2019).Validation of H2O2-mediated pathway model for elucidating oxygen reduction mechanism: Experimental evidences and theoretical simulations.ELECTROCHIMICA ACTA,313,378-388. |
MLA | Yin, Fengjun,et al."Validation of H2O2-mediated pathway model for elucidating oxygen reduction mechanism: Experimental evidences and theoretical simulations".ELECTROCHIMICA ACTA 313(2019):378-388. |
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