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Towards understanding ORR activity and electron-transfer pathway of M-Nx/C electro-catalyst in acidic media
Zhang, Xiaohua1,2; Lu, Ping1,3; Zhang, Chen1,2; Cui, Xiangzhi1; Xu, Yingfeng1,2; Qu, Haiyun1,3; Shi, Jianlin1
2017
发表期刊Journal of Catalysis
ISSN00219517
卷号356页码:229-236
摘要M-Nx/C (M = Fe, Co) type electro-catalyst as a promising alternative to Pt-based electro-catalyst for oxygen reduction reaction (ORR) in fuel cells has been studied for years. However, the mechanism of this four-electron process involving several successive steps and the dynamic intermediate (hydrogen peroxide) participation still remains obscure. In this study, a series of Co-Nx/C with varied densities of Co-Nxsites have been obtained for probing the ORR activity and pathway in acid media via adopting zinc ions as a size-comparable template to disperse and regulate Co-Nxsites. Importantly, it has been found that the half-wave potential can be positively correlated with the weight percentage of ionic cobalt species, which suggests the decisive role of the density of Co-Nxsites on ORR activity. More importantly, our results suggest that both Co-Nx/C and 20 wt% Pt/C catalyze ORR via two successive steps: ORR begins at the onset potential accompanying the generation of H2O2intermediate, which is more easily to be adsorbed on platinum than on Co-Nx/C surface as detected by ring electrode; Subsequently at the half-wave potential and more negative, H2O2is further reduced immediately and efficiently on platinum, but unfortunately at much lower rate on Co-Nx/C. Thus in addition to improving the initial ORR activity by maximizing the M-Nxcoordination, it will be of great significance to endow the non-platinum catalysts with surface active sites capable of adsorbing and efficiently reducing the H2O2intermediate for the complete oxygen reduction to water. © 2017 Elsevier Inc.
DOI10.1016/j.jcat.2017.10.020
EI入藏号20174504373359
EI主题词Cobalt compounds
EI分类号547.1 Precious Metals - 702.2 Fuel Cells - 802.2 Chemical Reactions - 804 Chemical Products Generally - 804.2 Inorganic Compounds
引用统计
文献类型期刊论文
条目标识符http://ir.sic.ac.cn/handle/331005/25781
专题中国科学院上海硅酸盐研究所
作者单位1.The State Key Laboratory of High Performance Ceramics and Superfine Microstructures, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai; 200050, China;
2.University of Chinese Academy of Sciences, Beijing; 100049, China;
3.Analysis and Testing Center for Inorganic Materials, Shanghai Institute of Ceramics, Chinese Academy of Sciences, China
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GB/T 7714
Zhang, Xiaohua,Lu, Ping,Zhang, Chen,et al. Towards understanding ORR activity and electron-transfer pathway of M-Nx/C electro-catalyst in acidic media[J]. Journal of Catalysis,2017,356:229-236.
APA Zhang, Xiaohua.,Lu, Ping.,Zhang, Chen.,Cui, Xiangzhi.,Xu, Yingfeng.,...&Shi, Jianlin.(2017).Towards understanding ORR activity and electron-transfer pathway of M-Nx/C electro-catalyst in acidic media.Journal of Catalysis,356,229-236.
MLA Zhang, Xiaohua,et al."Towards understanding ORR activity and electron-transfer pathway of M-Nx/C electro-catalyst in acidic media".Journal of Catalysis 356(2017):229-236.
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