First principles computational study on the electrochemical stability of Pt–Co nanocatalysts
Abstract
Using density functional theory (DFT) calculations, we identify the thermodynamically stable configurations of Pt-Co alloy nanoparticles of varying Co compositions and particle sizes. Our results indicate that the most thermodynamically stable structure is a shell-by-shell configuration where the Pt atom only shell and the Co only shell alternately stack and the outermost shell consists of a Pt skin layer. DFT calculations show that the structure has substantially higher dissolution potential of the outermost Pt shell compared with pure Pt nanoparticles of approximately the same size. Furthermore, our DFT calculations also propose that the shell-by-shell structure shows much better oxygen reduction reaction (ORR) activity than conventional bulk or nanoparticles of pure Pt. These novel catalyst properties can be changed when the surfaces are adsorbed with oxygen atoms via selective segregation followed by the electrochemical dissolution of the alloyed Co atoms. However, these phenomena are thermodynamically not plausible if the chemical potentials of oxygen are controlled below a certain level. Therefore, we propose that the shell-by-shell structures are promising candidates for highly functional catalysts in fuel cell applications.
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Areas of ordered arrangement or/and disordered arrangement in composition of a Pt alloy play an important role in determining catalytic activity of fuel cell electrocatalysts.
“Furthermore, the areas of ordered arrangement or/and disordered arrangement in the composition of a Pt alloy play an important role in determining the catalytic activity of fuel cell electrocatalysts.263,376,401,402”
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Self-citation
- Authors
- Noh, S. H., Seo, M. H., Seo, J. K., Fischer, P., & Han, B.
- Affiliations
- Daegu Gyeongbuk Institute of Science and Technology (KR)
- Lawrence Berkeley National Laboratory (US)
- Corresponding author
- Han, Byungchan
- Venue
- Nanoscale
- Publisher
- Royal Society of Chemistry (RSC)
- Published
- 2013
- Volume
- 5
- Issue
- 18
- Pages
- 8625
- ISSN
- 2040-3364 (ISSN-L)
- 2040-3372
- OpenAlex
- W2160946810
- Cited by
- 78
- References
- 46
- Citations by year
- 2026: 4 · 2025: 5 · 2024: 2 · 2023: 3 · 2022: 7 · 2021: 3 · 2020: 8 · 2019: 3 · 2018: 6 · 2017: 6 · 2016: 9 · 2015: 10 · 2014: 11 · 2013: 1
- FWCI
- 3.76
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Nanoscale (publishedVersion)
- PubMed (publishedVersion)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Keywords
- electrochemical stability, oxygen reduction reaction, dissolution potential, oxygen adsorption, thermodynamic stability, fuel cell catalysts, particle size effects
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