Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 124, Issue 22, Pages 12016-12023Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.0c03951
Keywords
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Funding
- Department of Energy [DE-SC0010576]
- Welch Foundation [F-1841]
- U.S. Department of Energy (DOE) [DE-SC0010576] Funding Source: U.S. Department of Energy (DOE)
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Nitrogen-doped carbon materials are promising metal-free catalysts for the electrochemical oxygen reduction reaction (ORR). A better theoretical understanding on the nature of the active site(s) would help further optimization of their ORR activity. Although quantum mechanical calculations have been widely employed to elucidate the active sites over various catalysts, these calculations are typically done assuming constant-charge conditions rather than the experimentally relevant constant-potential conditions. In this study, we employ the double-reference method to simulate the energetics of the ORR over pure and N-doped carbon materials under constant-potential conditions. We demonstrate that constant-potential calculations enable more accurate theoretical predictions, comparing well with existing experiments. Our key findings are (1) the zigzag edge of pure graphite is highly active for ORR, (2) the pyridinic N-doped armchair edge is highly active for ORR in alkaline media but not in acid, and (3) graphitic N can donate electrons to pyridinic N to enhance the ORR activity. These fundamental insights provide guidelines for the design of better carbon- based ORR catalysts.
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