Activity of N-coordinated multi-metal-atom active site structures for Pt-free oxygen reduction reaction catalysis: Role of *OH ligands

Holby, Edward F.; Taylor, Christopher D.

doi:10.1038/srep09286

Title: Activity of N-coordinated multi-metal-atom active site structures for Pt-free oxygen reduction reaction catalysis: Role of *OH ligands

Journal Article · Thu Mar 19 00:00:00 EDT 2015 · Scientific Reports

DOI:https://doi.org/10.1038/srep09286· OSTI ID:1193434

Holby, Edward F. ^[1]; Taylor, Christopher D. ^[2]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
The Ohio State Univ., Columbus, OH (United States)

We report calculated oxygen reduction reaction energy pathways on multi-metal-atom structures that have previously been shown to be thermodynamically favorable. We predict that such sites have the ability to spontaneously cleave the O₂ bond and then will proceed to over-bind reaction intermediates. In particular, the *OH bound state has lower energy than the final 2 H₂O state at positive potentials. Contrary to traditional surface catalysts, this *OH binding does not poison the multi-metal-atom site but acts as a modifying ligand that will spontaneously form in aqueous environments leading to new active sites that have higher catalytic activities. These *OH bound structures have the highest calculated activity to date.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1193434

Report Number(s):: LA-UR-14-29207; srep09286

Journal Information:: Scientific Reports, Vol. 5, Issue 5; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 98 works

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Title: Activity of N-coordinated multi-metal-atom active site structures for Pt-free oxygen reduction reaction catalysis: Role of *OH ligands

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