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Title: Potentiostatic and Potential Cycling Dissolution of Polycrystalline Platinum and Platinum Nano-Particle Fuel Cell Catalysts

Abstract

The dissolution of Pt in aqueous electrolytes has been studied for over forty years, most recently in the context of understanding the observed loss in electrochemically-active surface area (ECA) of cathode electrocatalysts in polymer electrolyte fuel cells. Despite extensive research, there are many unresolved issues regarding the dissolution of nano-particle Pt, such as the source of the observed potential dependence of potentiostatic and potential cycling dissolution rates. To help resolve these issues, in this paper we present results of measurements of the concentration of dissolved Pt and Pt dissolution rates for carbon-supported platinum nano-particles (Pt/C) in dilute perchloric acid, as a mimic of the PEFC cathode environment, as a function of potential and upper potential limit of potential cycling. Also presented, for comparison, are results of similar studies on polycrystalline platinum. In situ Pt L III X-ray absorption spectroscopy was used to determine the extent of oxidation, the coordination environment, and loss of Pt from the Pt nano-particles to elucidate the mechanism of Pt dissolution. Finally, based on the correlation of these studies with those presented in the literature, mechanisms for Pt dissolution under potentiostatic and potential cycling conditions are proposed.

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [2]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technologies Office (EE-3F); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1460215
Alternate Identifier(s):
OSTI ID: 1461447
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 165; Journal Issue: 6; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Myers, Deborah, Wang, Xiaoping, Smith, Matt C., and More, Karren Leslie. Potentiostatic and Potential Cycling Dissolution of Polycrystalline Platinum and Platinum Nano-Particle Fuel Cell Catalysts. United States: N. p., 2018. Web. doi:10.1149/2.0211806jes.
Myers, Deborah, Wang, Xiaoping, Smith, Matt C., & More, Karren Leslie. Potentiostatic and Potential Cycling Dissolution of Polycrystalline Platinum and Platinum Nano-Particle Fuel Cell Catalysts. United States. doi:10.1149/2.0211806jes.
Myers, Deborah, Wang, Xiaoping, Smith, Matt C., and More, Karren Leslie. Tue . "Potentiostatic and Potential Cycling Dissolution of Polycrystalline Platinum and Platinum Nano-Particle Fuel Cell Catalysts". United States. doi:10.1149/2.0211806jes. https://www.osti.gov/servlets/purl/1460215.
@article{osti_1460215,
title = {Potentiostatic and Potential Cycling Dissolution of Polycrystalline Platinum and Platinum Nano-Particle Fuel Cell Catalysts},
author = {Myers, Deborah and Wang, Xiaoping and Smith, Matt C. and More, Karren Leslie},
abstractNote = {The dissolution of Pt in aqueous electrolytes has been studied for over forty years, most recently in the context of understanding the observed loss in electrochemically-active surface area (ECA) of cathode electrocatalysts in polymer electrolyte fuel cells. Despite extensive research, there are many unresolved issues regarding the dissolution of nano-particle Pt, such as the source of the observed potential dependence of potentiostatic and potential cycling dissolution rates. To help resolve these issues, in this paper we present results of measurements of the concentration of dissolved Pt and Pt dissolution rates for carbon-supported platinum nano-particles (Pt/C) in dilute perchloric acid, as a mimic of the PEFC cathode environment, as a function of potential and upper potential limit of potential cycling. Also presented, for comparison, are results of similar studies on polycrystalline platinum. In situ Pt LIII X-ray absorption spectroscopy was used to determine the extent of oxidation, the coordination environment, and loss of Pt from the Pt nano-particles to elucidate the mechanism of Pt dissolution. Finally, based on the correlation of these studies with those presented in the literature, mechanisms for Pt dissolution under potentiostatic and potential cycling conditions are proposed.},
doi = {10.1149/2.0211806jes},
journal = {Journal of the Electrochemical Society},
number = 6,
volume = 165,
place = {United States},
year = {2018},
month = {3}
}

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Works referenced in this record:

Characterization of High-Surface-Area Electrocatalysts Using a Rotating Disk Electrode Configuration
journal, January 1998

  • Schmidt, T. J.; Gasteiger, H. A.; Stäb, G. D.
  • Journal of The Electrochemical Society, Vol. 145, Issue 7, p. 2354-2358
  • DOI: 10.1149/1.1838642