期刊
JOURNAL OF CATALYSIS
卷 396, 期 -, 页码 215-223出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2021.02.016
关键词
Electrocatalysis; Transition-metal-nitrogen-carbon catalyst; Oxygen reduction reaction; Potential-dependent kinetics; Reaction mechanism
资金
- National Key Research and Development Program of China [2017YFA0206500]
- National Natural Science Foundation of China [21673040, 21973013, 21573107]
- National Natural Science Foundation of Fujian Province, China [2020J02025]
By systematically investigating the oxygen reduction reaction process on dual-metal-nitrogen-carbon catalysts through first-principle calculations, it is found that the high activity of dual-metal sites can be attributed to facilitating O-O bond cleavage and mitigating *OH removal issue. The introduction of a descriptor called antibonding center simplifies the evaluation of kinetics.
In this work, the oxygen reduction reaction (ORR) process on dual-metal-nitrogen-carbon (DM-N-C) catalysts by including two important factors (potential of zero charge and potential-dependent kinetics of O-O bond cleavage) from first-principle calculations is systematically investigated. Our results reveal that the origin for the high activity of dual-metal sites can be attributed to the fact that introducing a second metal site can facilitate the O-O bond cleavage in the key OOH* intermediate during ORR and meanwhile mitigate the *OH removal issue. Importantly, we define a descriptor called antibonding center that simplifies the evaluation of the kinetics. Based on the advanced approach used in this work, we demonstrate that several DM-N-C electrocatalysts including FeFeN6, FeCoN6, and CoZnN6 have high ORR activity consistent with previous experiments, and also predict MnCoN6 can be more highly stable and active for acidic ORR. This study demonstrates the advantage of the dual metal sites for the ORR in acidic electrolyte and highlights the significance of kinetics in the theoretical study of ORR electrocatalysts. (C) 2021 Elsevier Inc. All rights reserved.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据