Journal
SCIENCE
Volume 351, Issue 6271, Pages 361-365Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aad0832
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Funding
- New Energy and Industrial Technology Development Organization
- Japan Science and Technology Agency-Precursory Research for Embryonic Science and Technology (JST-PRESTO) program
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Nitrogen (N)-doped carbon materials exhibit high electrocatalytic activity for the oxygen reduction reaction (ORR), which is essential for several renewable energy systems. However, the ORR active site (or sites) is unclear, which retards further developments of high-performance catalysts. Here, we characterized the ORR active site by using newly designed graphite (highly oriented pyrolitic graphite) model catalysts with well-defined p conjugation and well-controlled doping of N species. The ORR active site is created by pyridinic N. Carbon dioxide adsorption experiments indicated that pyridinic N also creates Lewis basic sites. The specific activities per pyridinic N in the HOPG model catalysts are comparable with those of N-doped graphene powder catalysts. Thus, the ORR active sites in N-doped carbon materials are carbon atoms with Lewis basicity next to pyridinic N.
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