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Title: Effects of surface charge and cluster size on the electrochemical dissolution of platinum nanoparticles using COMB3 and continuum electrolyte models

Abstract

We study the site-dependent dissolution of platinum nanoparticles under electrochemical conditions to assess their thermodynamic stability as a function of shape and size using empirical molecular dynamics and electronic-structure models. The third-generation charge optimized many-body potential is employed to determine the validity of uniform spherical representations of the nanoparticles in predicting dissolution potentials (the Kelvin model). To understand the early stages of catalyst dissolution, implicit solvation techniques based on the self-consistent continuum solvation method are applied. It is demonstrated that interfacial charge and polarization can shift the dissolution energies by amounts on the order of 0.74 eV depending on the surface site and nanoparticle shape, leading to the unexpected preferential removal of platinum cations from highly coordinated sites in some cases.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]
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  1. Pennsylvania State Univ., University Park, PA (United States)
Publication Date:
Research Org.:
Pennsylvania State Univ., University Park, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1803446
Alternate Identifier(s):
OSTI ID: 1598733
Grant/Contract Number:  
SC0018646
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 152; Journal Issue: 6; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Physics

Citation Formats

Goff, James M., Sinnott, Susan B., and Dabo, Ismaila. Effects of surface charge and cluster size on the electrochemical dissolution of platinum nanoparticles using COMB3 and continuum electrolyte models. United States: N. p., 2020. Web. doi:10.1063/1.5131720.
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Goff, James M., Sinnott, Susan B., & Dabo, Ismaila. Effects of surface charge and cluster size on the electrochemical dissolution of platinum nanoparticles using COMB3 and continuum electrolyte models. United States. https://doi.org/10.1063/1.5131720
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Goff, James M., Sinnott, Susan B., and Dabo, Ismaila. Mon . "Effects of surface charge and cluster size on the electrochemical dissolution of platinum nanoparticles using COMB3 and continuum electrolyte models". United States. https://doi.org/10.1063/1.5131720. https://www.osti.gov/servlets/purl/1803446.
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@article{osti_1803446,
title = {Effects of surface charge and cluster size on the electrochemical dissolution of platinum nanoparticles using COMB3 and continuum electrolyte models},
author = {Goff, James M. and Sinnott, Susan B. and Dabo, Ismaila},
abstractNote = {We study the site-dependent dissolution of platinum nanoparticles under electrochemical conditions to assess their thermodynamic stability as a function of shape and size using empirical molecular dynamics and electronic-structure models. The third-generation charge optimized many-body potential is employed to determine the validity of uniform spherical representations of the nanoparticles in predicting dissolution potentials (the Kelvin model). To understand the early stages of catalyst dissolution, implicit solvation techniques based on the self-consistent continuum solvation method are applied. It is demonstrated that interfacial charge and polarization can shift the dissolution energies by amounts on the order of 0.74 eV depending on the surface site and nanoparticle shape, leading to the unexpected preferential removal of platinum cations from highly coordinated sites in some cases.},
doi = {10.1063/1.5131720},
journal = {Journal of Chemical Physics},
number = 6,
volume = 152,
place = {United States},
year = {Mon Feb 10 00:00:00 EST 2020},
month = {Mon Feb 10 00:00:00 EST 2020}
}
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https://doi.org/10.1063/1.5131720
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