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First Principles Study of Morphology, Doping Level, and Water Solvation Effects on the Catalytic Mechanism of Nitrogen-Doped Graphene in the Oxygen Reduction Reaction
- First Principles Study of Morphology, Doping Level, and Water Solvation Effects on the Catalytic Mechanism of Nitrogen-Doped Graphene in the Oxygen Reduction Reaction
- Kwak, D[Kwak, Dohyun]; Khetan, A[Khetan, Abhishek]; Noh, S[Noh, Seunghyo]; Pitsch, H[Pitsch, Heinz]; Han, B[Han, Byungchan]
- DGIST Authors
- Kwak, D[Kwak, Dohyun]; Han, B[Han, Byungchan]
- Issue Date
- ChemCatChem, 6(9), 2662-2670
- Article Type
- Calculations; Density Functional Calculations; Density Functional Theory; Doping (Additives); Edge Effect; Edge Effects; Electrolytic Reduction; First-Principles Dft Calculations; First-Principles Study; Free Energy; Gibbs Free Energy; Graphene; Ground-State; Ground-State Structures; Heterogeneous Catalyst; Morphology; Nitrogen Doped Graphene; Oxygen; Oxygen Reduction; Oxygen Reduction Reaction; Solvation
- 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 30 at.% 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. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
- Wiley-VCH Verlag
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