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:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- The Ohio State Univ., Columbus, OH (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (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:
- 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. https://doi.org/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. https://doi.org/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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