Journal
CARBON
Volume 147, Issue -, Pages 303-311Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.carbon.2019.01.018
Keywords
Co-doped carbon; Doping configuration; Active site; Oxygen reduction
Funding
- National Natural Science Foundation of China [51521091, 51532008, 51572264, 51625203, 51772303]
- National Key RAMP
- 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, 201704030019, 201604030012]
- Research Grant Council of the Hong Kong Special Administrative Region [N_HKUST610/17]
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Different 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.
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