Cited 18 time in webofscience Cited 18 time in scopus

First principles study of oxygen reduction reaction mechanisms on N-doped graphene with a transition metal support

Title
First principles study of oxygen reduction reaction mechanisms on N-doped graphene with a transition metal support
Authors
Noh, SH[Noh, Seung Hyo]Kwak, DH[Kwak, Do Hyun]Seo, MH[Seo, Min Ho]Ohsaka, T[Ohsaka, Takeo]Han, B[Han, Byungchan]
DGIST Authors
Kwak, DH[Kwak, Do Hyun]; Han, B[Han, Byungchan]
Issue Date
2014-09-10
Citation
Electrochimica Acta, 140, 225-231
Type
Article
Article Type
Article
Keywords
3D MetalsChemical InteractionsDensity Functional TheoryDoping (Additives)Electrolytic ReductionElectronic StructureFirst-PrinciplesFirst-Principles Density Functional TheoryFirst-Principles StudyFree-Energy DiagramsGrapheneMetallic SupportMoleculesN-DopedN-Doped Graphene on 3D MetalOxygenOxygen Reduction ReactionPolymer Electrolyte Membrane Fuel Cell (PEMFC)Proton-Exchange Membrane Fuel Cells (PEMFC)Transition-Metalss
ISSN
0013-4686
Abstract
Using first principles density functional theory calculations, we systematically studied oxygen reduction reactions (ORRs) on N-doped graphene (N-Gr) with and without a Cu metallic support (N-Gr/Cu(111) surface). Our ab-initio calculated free energy diagrams surprisingly show that oxygen molecules are dissociated into two oxygen atoms on the N-Gr/Cu(111) surface, which alters the well-known associative ORR mechanisms on pure graphene and N-Gr. Our results, however, indicate that the mechanistic shift does not directly lead to enhancement of ORR activity once water molecules solvate the N-Gr/Cu(111) surface via substantially stabilized intermediates such as O, OH, and OOH. Our results suggest that transition metal supports can be a promising way to control the ORR mechanism on doped graphene and that the evaluation of ORR activity requires understandings of not only the electronic structures of doped graphene but also the chemical interactions between the intermediates and solvating water molecules. © 2014 Elsevier Ltd.
URI
http://hdl.handle.net/20.500.11750/3037
DOI
10.1016/j.electacta.2014.03.076
Publisher
Elsevier Ltd
Files:
There are no files associated with this item.
Collection:
Energy Science and EngineeringETC1. Journal Articles
Energy Science and EngineeringEnergy Systems Engineering1. Journal Articles


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