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On the Influence of Oxygen on the Degradation of Fe-N-C Catalysts
Authors:Dr. Kavita Kumar  Dr. Laetitia Dubau  Dr. Michel Mermoux  Dr. Jingkun Li  Dr. Andrea Zitolo  Dr. Jaysen Nelayah  Dr. Frédéric Jaouen  Dr. Frédéric Maillard
Affiliation:1. Univ. Grenoble Alpes, Univ. Savoie Mont Blanc, CNRS, Grenoble INP, LEPMI, 38000 Grenoble, France;2. CNRS, Université de Montpellier, ENSCM, Institut Charles Gerhardt Montpellier UMR 5253, 2 Place Eugène Bataillon, 34095 Montpellier, France;3. Synchrotron SOLEIL, L'orme des Merisiers, BP 48 Saint Aubin, 91192 Gif-sur-Yvette, France;4. Université de Paris, Laboratoire Matériaux et Phénomènes Quantiques, CNRS, 75013 Paris, France
Abstract:Fe-N-C catalysts containing atomic FeNx sites are promising candidates as precious-metal-free catalysts for oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. The durability of Fe-N-C catalysts in fuel cells has been extensively studied using accelerated stress tests (AST). Herein we reveal stronger degradation of the Fe-N-C structure and four-times higher ORR activity loss when performing load cycling AST in O2- vs. Ar-saturated pH 1 electrolyte. Raman spectroscopy results show carbon corrosion after AST in O2, even when cycling at low potentials, while no corrosion occurred after any load cycling AST in Ar. The load-cycling AST in O2 leads to loss of a significant fraction of FeNx sites, as shown by energy dispersive X-ray spectroscopy analyses, and to the formation of Fe oxides. The results support that the unexpected carbon corrosion occurring at such low potential in the presence of O2 is due to reactive oxygen species produced between H2O2 and Fe sites via Fenton reactions.
Keywords:Kohlenstoffkorrosion  Fe-N-C-Katalysatoren  Sauerstoffreduktion  Polymerelektrolytbrennstoffzellen  Reaktive Sauerstoffspezies (ROS)
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