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Title: (Invited) Kinetic Models for the Degradation Mechanisms of PGM-Free ORR Catalysts

Abstract

Platinum group metal-free (PGM-free) catalysts, based on earth-abundant elements such as carbon, nitrogen, and transition metals, have shown promising oxygen reduction reaction (ORR) activity in fuel cells. Intensive research activities have focused on the improvement of activity and understanding of active sites in PGM-free catalysts. However, the durability of PGM-free catalysts in fuel cell cathode under realistic operating conditions has been addressed to a much lesser degree than the initial ORR activity, with only qualitative degradation mechanisms proposed to account for the generally fast activity loss in the fuel cell. Herein, we introduce to PGM-free ORR electrocatalysis a quantitative logistic decay model, based on a two-step autocatalytic degradation mechanism to portray catalyst degradation behavior. This model describes well the current-time data measured in the kinetic range of the fuel cell (fuel cell cathode) operation. Here, the results further suggest that the formation of deactivation species during the ORR is responsible for the loss of catalytic active sites and ensuing cell performance loss.

Authors:
ORCiD logo [1]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office
OSTI Identifier:
1471365
Report Number(s):
LA-UR-18-24640
Journal ID: ISSN 1938-6737
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ECS Transactions (Online)
Additional Journal Information:
Journal Volume: 85; Journal Issue: 13; Journal ID: ISSN 1938-6737
Publisher:
Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; PGM-free ORR Catalyst; non-PGM ORR Catalyst; Oxygen reduction reaction; Fe-C-N catalyst; Durability; Fuel cell; Kinetic models; Logistic decay; Exponential decay; Double exponential decay

Citation Formats

Yin, Xi, and Zelenay, Piotr. (Invited) Kinetic Models for the Degradation Mechanisms of PGM-Free ORR Catalysts. United States: N. p., 2018. Web. doi:10.1149/08513.1239ecst.
Yin, Xi, & Zelenay, Piotr. (Invited) Kinetic Models for the Degradation Mechanisms of PGM-Free ORR Catalysts. United States. https://doi.org/10.1149/08513.1239ecst
Yin, Xi, and Zelenay, Piotr. 2018. "(Invited) Kinetic Models for the Degradation Mechanisms of PGM-Free ORR Catalysts". United States. https://doi.org/10.1149/08513.1239ecst. https://www.osti.gov/servlets/purl/1471365.
@article{osti_1471365,
title = {(Invited) Kinetic Models for the Degradation Mechanisms of PGM-Free ORR Catalysts},
author = {Yin, Xi and Zelenay, Piotr},
abstractNote = {Platinum group metal-free (PGM-free) catalysts, based on earth-abundant elements such as carbon, nitrogen, and transition metals, have shown promising oxygen reduction reaction (ORR) activity in fuel cells. Intensive research activities have focused on the improvement of activity and understanding of active sites in PGM-free catalysts. However, the durability of PGM-free catalysts in fuel cell cathode under realistic operating conditions has been addressed to a much lesser degree than the initial ORR activity, with only qualitative degradation mechanisms proposed to account for the generally fast activity loss in the fuel cell. Herein, we introduce to PGM-free ORR electrocatalysis a quantitative logistic decay model, based on a two-step autocatalytic degradation mechanism to portray catalyst degradation behavior. This model describes well the current-time data measured in the kinetic range of the fuel cell (fuel cell cathode) operation. Here, the results further suggest that the formation of deactivation species during the ORR is responsible for the loss of catalytic active sites and ensuing cell performance loss.},
doi = {10.1149/08513.1239ecst},
url = {https://www.osti.gov/biblio/1471365}, journal = {ECS Transactions (Online)},
issn = {1938-6737},
number = 13,
volume = 85,
place = {United States},
year = {Tue Jun 19 00:00:00 EDT 2018},
month = {Tue Jun 19 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 33 works
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Figures / Tables:

Figure 1 Figure 1: Schematics of proposed two degradation mechanisms of PGM-free catalysts.

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Works referencing / citing this record:

Progress in the Development of Fe‐Based PGM‐Free Electrocatalysts for the Oxygen Reduction Reaction
journal, December 2018


PGM‐Free Cathode Catalysts for PEM Fuel Cells: A Mini‐Review on Stability Challenges
journal, December 2018


On the Influence of Oxygen on the Degradation of Fe‐N‐C Catalysts
journal, January 2020


On the Influence of Oxygen on the Degradation of Fe‐N‐C Catalysts
journal, February 2020


Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.