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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

Abstract

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.

Authors:
 [1];  [2]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. The Ohio State Univ., Columbus, OH (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1193434
Report Number(s):
LA-UR-14-29207
Journal ID: ISSN 2045-2322; srep09286
Grant/Contract Number:
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 5; Journal Issue: 5; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION

Citation Formats

Holby, Edward F., and Taylor, Christopher D.. Activity of N-coordinated multi-metal-atom active site structures for Pt-free oxygen reduction reaction catalysis: Role of *OH ligands. United States: N. p., 2015. Web. doi:10.1038/srep09286.
Holby, Edward F., & Taylor, Christopher D.. Activity of N-coordinated multi-metal-atom active site structures for Pt-free oxygen reduction reaction catalysis: Role of *OH ligands. United States. doi:10.1038/srep09286.
Holby, Edward F., and Taylor, Christopher D.. Thu . "Activity of N-coordinated multi-metal-atom active site structures for Pt-free oxygen reduction reaction catalysis: Role of *OH ligands". United States. doi:10.1038/srep09286. https://www.osti.gov/servlets/purl/1193434.
@article{osti_1193434,
title = {Activity of N-coordinated multi-metal-atom active site structures for Pt-free oxygen reduction reaction catalysis: Role of *OH ligands},
author = {Holby, Edward F. and Taylor, Christopher D.},
abstractNote = {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.},
doi = {10.1038/srep09286},
journal = {Scientific Reports},
number = 5,
volume = 5,
place = {United States},
year = {Thu Mar 19 00:00:00 EDT 2015},
month = {Thu Mar 19 00:00:00 EDT 2015}
}

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Free Publicly Available Full Text
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Cited by: 15 works
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