Importance of Pd monomer pairs in enhancing the oxygen reduction reaction activity of the AuPd(1 0 0) surface: A first principles study

Hyung Chul Ham, Gyeong S. Hwang, Jonghee Han, Sung Pil Yoon, SukWoo Nam, Tae Hoon Lim

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

Based on density functional theory calculations, we present that pairs of 1st nearest Pd monomers play an important role in significantly enhancing the oxygen reduction reaction (ORR) on the AuPd(1 0 0) surface. While the catalytic ORR activity tends to be sensitive to the surface atomic ordering, we find that the Pd monomer pairs lead to a substantial reduction in the activation barrier for O/OH hydrogenation with no significant suppression of O-O bond scission, thereby considerably lowering the overall activation energy for the ORR as compared to the case of pure Pd(1 0 0). On the other hand, an isolated Pd monomer tends to greatly suppress the O-O bond cleavage reaction, which in turn slows down the ORR kinetics. Unlike the monodentate adsorption of O2 on an isolated Pd monomer, the pairing of Pd monomers allows O2 adsorption in a bidentate configuration and consequently facilitating O-O bond scission. However, the barrier for OH hydrogenation at each Pd site shows no significant change between the isolated and paired cases, while it is noticeably lower than the pure Pd case.

Original languageEnglish
Pages (from-to)11-15
Number of pages5
JournalCatalysis Today
Volume263
DOIs
Publication statusPublished - 2016 Apr 1
Externally publishedYes

Fingerprint

Monomers
Oxygen
Hydrogenation
Adsorption
Reaction kinetics
Density functional theory
Activation energy
Chemical activation

Keywords

  • AuPd(1 0 0)
  • Ensembles
  • First-principles
  • ORR

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

Cite this

Importance of Pd monomer pairs in enhancing the oxygen reduction reaction activity of the AuPd(1 0 0) surface : A first principles study. / Ham, Hyung Chul; Hwang, Gyeong S.; Han, Jonghee; Yoon, Sung Pil; Nam, SukWoo; Lim, Tae Hoon.

In: Catalysis Today, Vol. 263, 01.04.2016, p. 11-15.

Research output: Contribution to journalArticle

Ham, Hyung Chul ; Hwang, Gyeong S. ; Han, Jonghee ; Yoon, Sung Pil ; Nam, SukWoo ; Lim, Tae Hoon. / Importance of Pd monomer pairs in enhancing the oxygen reduction reaction activity of the AuPd(1 0 0) surface : A first principles study. In: Catalysis Today. 2016 ; Vol. 263. pp. 11-15.
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