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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

Title
First Principles Study of Morphology, Doping Level, and Water Solvation Effects on the Catalytic Mechanism of Nitrogen-Doped Graphene in the Oxygen Reduction Reaction
Authors
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
2014-09
Citation
ChemCatChem, 6(9), 2662-2670
Type
Article
Article Type
Article
Keywords
CalculationsDensity Functional CalculationsDensity Functional TheoryDoping (Additives)Edge EffectEdge EffectsElectrolytic ReductionFirst-Principles Dft CalculationsFirst-Principles StudyFree EnergyGibbs Free EnergyGrapheneGround-StateGround-State StructuresHeterogeneous CatalystMorphologyNitrogen Doped GrapheneOxygenOxygen ReductionOxygen Reduction ReactionSolvation
ISSN
1867-3880
Abstract
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.
URI
http://hdl.handle.net/20.500.11750/3052
DOI
10.1002/cctc.201402248
Publisher
Wiley-VCH Verlag
Files:
There are no files associated with this item.
Collection:
Department of Energy Science and EngineeringEnergy Systems Engineering1. Journal Articles


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