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

Seung Hyo Noh, Do Hyun Kwak, Min Ho Seo, Takeo Ohsaka, Byungchan Han

Research output: Contribution to journalArticle

33 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)225-231
Number of pages7
JournalElectrochimica Acta
Volume140
DOIs
Publication statusPublished - 2014 Sep 10

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Graphite
Graphene
Transition metals
Oxygen
Molecules
Water
Free energy
Electronic structure
Density functional theory
Atoms

All Science Journal Classification (ASJC) codes

  • Chemical Engineering(all)
  • Electrochemistry

Cite this

Noh, Seung Hyo ; Kwak, Do Hyun ; Seo, Min Ho ; Ohsaka, Takeo ; Han, Byungchan. / First principles study of oxygen reduction reaction mechanisms on N-doped graphene with a transition metal support. In: Electrochimica Acta. 2014 ; Vol. 140. pp. 225-231.
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First principles study of oxygen reduction reaction mechanisms on N-doped graphene with a transition metal support. / Noh, Seung Hyo; Kwak, Do Hyun; Seo, Min Ho; Ohsaka, Takeo; Han, Byungchan.

In: Electrochimica Acta, Vol. 140, 10.09.2014, p. 225-231.

Research output: Contribution to journalArticle

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