Unravelling the Stability Stressors of Atomically Dispersed Fe-N-C Oxygen Reduction Catalysts

Xiaohong Xie; Boyang Li; Pan Xu; Moulay Tahar Sougrati; Ricardo Garcia-Serres; David A. Cullen; A. Jeremy Kropf; Fan Xia; Miao Song; Sulay Saha; Yachao Zeng; Mark H. Engelhard; Mark E. Bowden; Hanguang Zhang; Litao Yan; Teresa Lemmon; Xiaohong S. Li; Ulises Martinez; Yingwen Cheng; Gang Wu; Piotr Zelenay; Vijay Ramani; Deborah J. Myers; Frederic Jaouen; Lijun Yang; Guofeng Wang; Yuyan Shao

doi:10.1021/jacs.5c15451

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Unravelling the Stability Stressors of Atomically Dispersed Fe-N-C Oxygen Reduction Catalysts

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Unravelling the Stability Stressors of Atomically Dispersed Fe-N-C Oxygen Reduction Catalysts

Xiaohong Xie, Boyang Li, Pan Xu, Moulay Tahar Sougrati, Ricardo Garcia-Serres, David A. Cullen, A. Jeremy Kropf, Fan Xia, Miao Song, Sulay Saha, …

Journal of the American Chemical Society, Vol.147(52), pp.48117-48126

31/12/2025

DOI: https://doi.org/10.1021/jacs.5c15451

PMID: 41400425

Résumé

Chemistry

Chemistry, Multidisciplinary

Physical Sciences

Science & Technology

Enhancing the catalytic stability of Fe-N-C catalysts for cathodic oxygen reduction in proton-exchange membrane fuel cells (PEMFCs) necessitates an in-depth understanding of their degradation mechanisms. This study identifies key stressors affecting the stability of Fe-N-C catalysts, specifically acidic environment, oxygen (O2), and reactive oxygen species (ROS). Through ex situ/operando experiments, we show that the oxidation of local carbon by acidic environment + O2 + ROS, along with the demetalation of catalytic FeN x C y sites by O2 or O2 + ROS, is the primary factor responsible for the initial fast degradation of Fe-N-C catalysts. The demetalation of FeN x C y sites, influenced by O2, in particular by O2 + ROS, leads to the subsequent gradual degradation of Fe-N-C. Notably, FeN4C12-type active sites are more susceptible to demetalation than FeN4C10-type sites in O2 or O2 + ROS. Our findings indicate that, besides constructing more stable FeN x C y sites, preventing local carbon oxidation and scavenging of ROS are all critical for maintaining the stability of Fe-N-C catalysts.

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Détails

Titre: Unravelling the Stability Stressors of Atomically Dispersed Fe-N-C Oxygen Reduction Catalysts
Créateurs - sans rôle: Xiaohong Xie - Pacific Northwest Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA
Boyang Li - Univ Pittsburgh, Dept Mech Engn & Mat Sci, Pittsburgh, PA 15260 USA
Pan Xu - Ballard Power Syst Inc, Burnaby, BC V5J 5J8, Canada
Moulay Tahar Sougrati - Univ Montpellier, ICGM, CNRS, ENSCM, F-34293 Montpellier, France
Ricardo Garcia-Serres - Univ Grenoble Alpes, CNRS, Lab Chim & Biol Metaux, CEA,IRIG, F-38000 Grenoble, France
David A. Cullen - Ctr Nanophase Mat Sci, Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA
A. Jeremy Kropf - Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Fan Xia - Northern Illinois Univ, Dept Chem & Biochem, De Kalb, IL 60115 USA
Miao Song - Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99354 USA
Sulay Saha - Washington Univ St Louis, Dept Energy Environm & Chem Engn, St Louis, MO 63130 USA
Yachao Zeng - Univ Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USA
Mark H. Engelhard - Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99354 USA
Mark E. Bowden - Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99354 USA
Hanguang Zhang - Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA
Litao Yan - Pacific Northwest Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA
Teresa Lemmon - Pacific Northwest Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA
Xiaohong S. Li - Pacific Northwest Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA
Ulises Martinez - Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA
Yingwen Cheng - Northern Illinois Univ, Dept Chem & Biochem, De Kalb, IL 60115 USA
Gang Wu - Washington Univ St Louis, Dept Energy Environm & Chem Engn, St Louis, MO 63130 USA
Piotr Zelenay - Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA
Vijay Ramani - Washington Univ St Louis, Dept Energy Environm & Chem Engn, St Louis, MO 63130 USA
Deborah J. Myers - Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Frederic Jaouen - Univ Montpellier, ICGM, CNRS, ENSCM, F-34293 Montpellier, France
Lijun Yang - Ballard Power Syst Inc, Burnaby, BC V5J 5J8, Canada
Guofeng Wang - Univ Pittsburgh, Dept Mech Engn & Mat Sci, Pittsburgh, PA 15260 USA
Yuyan Shao - Pacific Northwest Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA
Détails de publication: Journal of the American Chemical Society, Vol.147(52), pp.48117-48126
Éditeur: Amer Chemical Soc
Nombre de pages: 10
Note de subvention: NA / Hydrogen and Fuel Cell Technologies Office
Identifiants: 99158450509311
Unité académique: Institut Charles Gerhardt Montpellier - ICGM
Langue: English
Type de ressource: Journal article