Predicting the oxygen-binding properties of platinum nanoparticle ensembles by combining high-precision electron microscopy and density functional theory
Predicting the oxygen-binding properties of platinum nanoparticle ensembles by combining high-precision electron microscopy and density functional theory
Many studies of heterogeneous catalysis, both experimental and computational, make use of idealized structures such as extended surfaces or regular polyhedral nanoparticles. This simplification neglects the morphological
diversity in real commercial oxygen reduction reaction (ORR) catalysts used in
fuel-cell cathodes. Here we introduce an approach that combines 3D
nanoparticle structures obtained from high-throughput high-precision electron
microscopy with density functional theory. Discrepancies between experimental
observations and cuboctahedral/truncated-octahedral particles are revealed and
discussed using a range of widely used descriptors, such as electron-density, d-band centers, and generalized coordination numbers. We use this new approach to determine the optimum particle size for which both detrimental surface roughness and particle shape effects are minimized.
Heterogeneous catalysis, fuel cells, ADF STEM, Density functional theory
4003-4012
Aarons, Jolyon
93e68133-73b0-43e0-8c91-464920f4a503
Jones, Lewys
9befb123-3e38-4c64-a92b-adc935b50737
Varambhia, Aakash
78a03233-af29-4426-a25e-188e51099fe9
MacArthur, Katherine E.
5b0027e8-6145-4e64-b3d2-7c16fe4450cc
Ozkaya, Dogan
d6b30e54-3986-41af-a129-d20c42ff94d7
Sarwar, Misbah
ae93ef8f-8a84-4a46-95ac-cd9352c44e56
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61
Nellist, Peter D.
f237015c-a26a-473c-960e-de99f2ef5a2d
12 July 2017
Aarons, Jolyon
93e68133-73b0-43e0-8c91-464920f4a503
Jones, Lewys
9befb123-3e38-4c64-a92b-adc935b50737
Varambhia, Aakash
78a03233-af29-4426-a25e-188e51099fe9
MacArthur, Katherine E.
5b0027e8-6145-4e64-b3d2-7c16fe4450cc
Ozkaya, Dogan
d6b30e54-3986-41af-a129-d20c42ff94d7
Sarwar, Misbah
ae93ef8f-8a84-4a46-95ac-cd9352c44e56
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61
Nellist, Peter D.
f237015c-a26a-473c-960e-de99f2ef5a2d
Aarons, Jolyon, Jones, Lewys, Varambhia, Aakash, MacArthur, Katherine E., Ozkaya, Dogan, Sarwar, Misbah, Skylaris, Chris-Kriton and Nellist, Peter D.
(2017)
Predicting the oxygen-binding properties of platinum nanoparticle ensembles by combining high-precision electron microscopy and density functional theory.
Nano Letters, 17 (7), .
(doi:10.1021/acs.nanolett.6b04799).
Abstract
Many studies of heterogeneous catalysis, both experimental and computational, make use of idealized structures such as extended surfaces or regular polyhedral nanoparticles. This simplification neglects the morphological
diversity in real commercial oxygen reduction reaction (ORR) catalysts used in
fuel-cell cathodes. Here we introduce an approach that combines 3D
nanoparticle structures obtained from high-throughput high-precision electron
microscopy with density functional theory. Discrepancies between experimental
observations and cuboctahedral/truncated-octahedral particles are revealed and
discussed using a range of widely used descriptors, such as electron-density, d-band centers, and generalized coordination numbers. We use this new approach to determine the optimum particle size for which both detrimental surface roughness and particle shape effects are minimized.
Text
Revised Submitted Version 4
- Accepted Manuscript
More information
Accepted/In Press date: 20 June 2017
e-pub ahead of print date: 28 June 2017
Published date: 12 July 2017
Keywords:
Heterogeneous catalysis, fuel cells, ADF STEM, Density functional theory
Organisations:
Chemistry, Computational Systems Chemistry
Identifiers
Local EPrints ID: 411963
URI: http://eprints.soton.ac.uk/id/eprint/411963
ISSN: 1530-6984
PURE UUID: e73a6251-dfa5-4e67-a950-cf7430f0a30f
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Date deposited: 03 Jul 2017 16:31
Last modified: 16 Mar 2024 05:29
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Contributors
Author:
Jolyon Aarons
Author:
Lewys Jones
Author:
Aakash Varambhia
Author:
Katherine E. MacArthur
Author:
Dogan Ozkaya
Author:
Misbah Sarwar
Author:
Peter D. Nellist
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