First-principles investigation of electrochemical dissolution of Pt nanoparticles and kinetic simulation

Dissolution is the primary route of Pt nanoparticle degradation in electrochemical devices, e.g., fuel cells. Investigation of potential-dependent dissolution kinetics of Pt nanoparticles is crucial to optimize the nanoparticle size and operating conditions for better performance. A mean-field kinet...

Full description

Saved in:
Bibliographic Details
Published in:The Journal of chemical physics 2019-12, Vol.151 (23), p.234711-234711
Main Authors: Zhu, Jing, Hu, Sulei, Zeng, Zhenhua, Li, Wei-Xue
Format: Article
Language:English
Subjects:
Chemisorption
Dissolution
Electrode potentials
Electrodes
First principles
Fuel cells
Kinetic theory
Nanoparticles
Optimization
Organic chemistry
Oxygen
Particle size
Physics
Platinum
Surface energy
Water splitting
Citations: Items that this one cites
Items that cite this one
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:Dissolution is the primary route of Pt nanoparticle degradation in electrochemical devices, e.g., fuel cells. Investigation of potential-dependent dissolution kinetics of Pt nanoparticles is crucial to optimize the nanoparticle size and operating conditions for better performance. A mean-field kinetic theory under the steady-state approximation, combined with atomistic thermodynamics and Wulff construction, was developed to study the interplay between oxygen chemisorption, electrode potential, and particle size on the dissolution of Pt nanoparticles. We found that although oxygen chemisorption from electrode potential-induced water splitting can stabilize Pt nanoparticles through decreasing the surface energy and increasing the redox potential, the electrode potential plays a more decisive role in facilitating the dissolution of Pt nanoparticles. In comparison with the minor effect of oxygen chemisorption, an increase in the particle size, though reducing the dispersion, has a more significant effect on the suppression of the dissolution. These theoretical understandings on the effects of electrode potential and particle size on the dissolution are crucial for optimizing the nanoparticle size under oxidative operating conditions.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.5129631