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Journal article
Unveiling the Origin of Morphological Instability in Topologically Complex Electrocatalytic Nanostructures
Journal of the American Chemical Society, v 147(37), pp 33482-33494
06 Sep 2025
PMID: 40913561
Featured in Collection : Research Supported by Drexel Libraries' OA Programs
Abstract
Coarsening and degradation phenomena in metals have largely focused on thermally driven processes, such as bulk and surface diffusion. However, dramatic coarsening has been reported in high-surface-area, nanometer-sized Pt-based catalysts during potential cycling in an electrolyte at room temperature─a temperature too low for the process to be explained purely by surface mobility values measured in both vacuum and electrolytes (∼10–22 and ∼10–18 cm2/s, respectively). This morphological evolution must be due to a different mechanism for mass transport that is sensitive to electrochemical conditions (e.g., electrolyte composition, potential limits, and scan rate). However, there have been no notable studies of electrochemically induced coarsening in nanometer-sized electrocatalysts. Here, we unveil the origins of coarsening in an electrolyte through coupled in situ experiments and atomistic kinetic Monte Carlo (kMC) simulations. Our work demonstrates electrochemical coarsening is driven by two concurrent mechanisms that can be explained at the atomistic level: (i) dissolution/redeposition during the reduction of an oxidized species and (ii) rapid surface diffusion of undercoordinated atoms.
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Details
- Title
- Unveiling the Origin of Morphological Instability in Topologically Complex Electrocatalytic Nanostructures
- Creators
- Yawei Li - Drexel UniversityJames L Hart - Drexel UniversityRamchandra Babali Gawas - Drexel University, Chemical and Biological EngineeringZhiyong Xia - Johns Hopkins University Applied Physics LaboratoryPietro P. Lopes - Argonne National LaboratoryJieyu Zhang - Shanxi UniversitySiming Li - Shanxi UniversityYucheng Wang - Xiamen UniversityMitra L Taheri - Johns Hopkins UniversityIan McCue - Northwestern UniversityJoshua D Snyder (Corresponding Author) - Drexel University
- Publication Details
- Journal of the American Chemical Society, v 147(37), pp 33482-33494
- Publisher
- ACS Publications
- Number of pages
- 13
- Grant note
- U.S. Department of Energy: 1904571, 1904578 NSF DMR program: DE-AC02-06CH11357 U.S. Department of Energy Office of Science laboratoryU.S Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division via the Early Career Research Project Award
This work was supported by the NSF DMR program under Grants #1904571 and #1904578. Thin film deposition and in situ ICP-MS experiments were conducted at Argonne National Laboratory, a U.S. Department of Energy Office of Science laboratory operated by UChicago Argonne, LLC under Contract no. DE-AC02-06CH11357. P.P.L. acknowledges the support from the U.S Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division via the Early Career Research Project Award.
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Chemical and Biological Engineering
- Web of Science ID
- WOS:001565593300001
- Scopus ID
- 2-s2.0-105016513078
- Other Identifier
- 991022085455704721
InCites Highlights
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- Collaboration types
- Domestic collaboration
- International collaboration
- Web of Science research areas
- Chemistry, Multidisciplinary