期刊
CHEMCATCHEM
卷 6, 期 9, 页码 2662-2670出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201402248
关键词
heterogeneous catalyst; density functional calculations; edge effects; graphene; oxygen reduction
资金
- Global Frontier R&D Program on Center for Hybrid Interface Materials - Ministry of Science, ICT and Future Planning [2013-073298]
- Ministry of Education, Science and Technology [2012K1A4A3053565]
- New and Renewable Energy R&D Program under the Ministry of Knowledge Economy, Republic of Korea [20113020030020]
- Deutsche Forschungsgemeinschaft (DFG)
By using first principles DFT calculations, we reveal oxygen reduction reaction mechanisms in N-doped graphene (N-Gr). Considering both the morphology and the concentration of dopant N atoms in bulk and edge N-Gr forms, we calculate the energies of a large number of N-Gr model systems to cover a wide range of possible N-Gr structures and determine the most stable N-Gr forms. In agreement with experiments, our DFT calculations suggest that doping levels in stable N-Gr forms are limited to less than approximately 30at.% N, above which the hexagonal graphene framework is broken. The ground state structures of bulk and edge N-Gr forms are found to differ depending on the doping level and poisoning of the edge bonds. Oxygen reduction reaction mechanisms are evaluated by using Gibbs free-energy diagrams with and without water solvation. Our results indicate that N doping significantly alters the catalytic properties of pure graphene and that dilutely doped bulk N-Gr forms are the most active.
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