Journal
ACS ENERGY LETTERS
Volume 3, Issue 4, Pages 986-991Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.8b00258
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Funding
- National Key Research and Development Program of China [2017YFA0206500]
- Natural Science Foundation of China [91645121, 21573107, 21703184, 21621091]
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N-doped carbon materials are promising electro-catalysts for oxygen reduction reaction (ORR). However, the lack of knowledge in the nature of active sites limits the rational design of this type of catalysts. Although pyridinic N species are proposed to be active for ORR, little experimental evidence is provided to reveal the reactive sites. Herein, we developed a surface modification method to identify the ortho-carbon atom of the pyridinic ring as the reactive site for ORR on N-doped graphene. The pyridinic ring of N-doped graphene was selectively grafted by an acetyl group at pyridinic N and ortho-C atoms by electrophilic and radical substitution, respectively. The former remained most of ORR catalytic activity, while the latter lost its activity completely. DFT calculations confirm that O-2 can get adsorbed and reduced favorably on the ortho-C atom of the pyridinic ring. This study provides new insight into the nature of active sites and the ORR mechanism for N-doped carbon materials.
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