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Identification of active sites in nitrogen and sulfur co-doped carbon-based oxygen reduction catalysts
Li, Jin-Cheng1,2; Qin, Xueping3; Hou, Peng-Xiang1; Cheng, Min1; Shi, Chao1; Liu, Chang1; Cheng, Hui-Ming1; Shao, Minhua2,3
Corresponding AuthorLiu, Chang(cliu@imr.ac.cn) ; Shao, Minhua(kemshao@ust.hk)
2019-06-01
Source PublicationCARBON
ISSN0008-6223
Volume147Pages:303-311
AbstractDifferent heteroatoms co-doped carbons are a burgeoning class of metal-free catalysts to replace Pt for the oxygen reduction reaction (ORR), but the lack of understanding of active sites delays their further improvement. Here we combined experimental designs and theoretical simulations with attempts to understand the correlation between N and/or S doping configurations and their catalytic activities. The results indicated that there is no obvious synergistic effect between N and S co-doping, in contrast with previous observations. S doping followed by N doping contributes to a large pyridinic N content in the catalyst due to the low formation energy for N to substitute doped S, leading to greatly enhanced ORR activity. Inversely, N doping followed by S doping takes pyridinic N away, resulting in an obvious ORR performance loss. Therefore, the doping sequence of S and N is crucial for the ORR activity of the co-doped catalysts. Furthermore, the pyridinic N is determined as the active functional group in N, S co-doped carbons by first-principle density functional theory calculations. (C) 2019 Elsevier Ltd. All rights reserved.
KeywordCo-doped carbon Doping configuration Active site Oxygen reduction
Funding OrganizationNational Natural Science Foundation of China ; National Key R&D Program of China ; Ministry of Science and Technology of China ; Guangdong Special Fund for Science and Technology Development (Hong Kong Technology Cooperation Funding Scheme) ; Research Grant Council of the Hong Kong Special Administrative Region
DOI10.1016/j.carbon.2019.01.018
Indexed BySCI
Language英语
Funding ProjectNational Natural Science Foundation of China[51521091] ; National Natural Science Foundation of China[51532008] ; National Natural Science Foundation of China[51572264] ; National Natural Science Foundation of China[51625203] ; National Natural Science Foundation of China[51772303] ; National Key R&D Program of China[2017YFB0102900] ; Ministry of Science and Technology of China[2016YFA0200102] ; Guangdong Special Fund for Science and Technology Development (Hong Kong Technology Cooperation Funding Scheme)[201704030065] ; Guangdong Special Fund for Science and Technology Development (Hong Kong Technology Cooperation Funding Scheme)[201704030019] ; Guangdong Special Fund for Science and Technology Development (Hong Kong Technology Cooperation Funding Scheme)[201604030012] ; Research Grant Council of the Hong Kong Special Administrative Region[N_HKUST610/17]
WOS Research AreaChemistry ; Materials Science
WOS SubjectChemistry, Physical ; Materials Science, Multidisciplinary
WOS IDWOS:000468156500035
PublisherPERGAMON-ELSEVIER SCIENCE LTD
Citation statistics
Cited Times:26[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/133620
Collection中国科学院金属研究所
Corresponding AuthorLiu, Chang; Shao, Minhua
Affiliation1.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Liaoning, Peoples R China
2.Hong Kong Univ Sci & Technol, Fok Ying Tung Res Inst, Guangzhou 511458, Guangdong, Peoples R China
3.Hong Kong Univ Sci & Technol, Dept Chem & Biol Engn, Kowloon, Clear Water Bay, Hong Kong, Peoples R China
Recommended Citation
GB/T 7714
Li, Jin-Cheng,Qin, Xueping,Hou, Peng-Xiang,et al. Identification of active sites in nitrogen and sulfur co-doped carbon-based oxygen reduction catalysts[J]. CARBON,2019,147:303-311.
APA Li, Jin-Cheng.,Qin, Xueping.,Hou, Peng-Xiang.,Cheng, Min.,Shi, Chao.,...&Shao, Minhua.(2019).Identification of active sites in nitrogen and sulfur co-doped carbon-based oxygen reduction catalysts.CARBON,147,303-311.
MLA Li, Jin-Cheng,et al."Identification of active sites in nitrogen and sulfur co-doped carbon-based oxygen reduction catalysts".CARBON 147(2019):303-311.
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