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Journal Articles Angewandte Chemie Year : 2020

On the Influence of Oxygen on the Degradation of Fe‐N‐C Catalysts


Precious metal-free catalysts for oxygen reduction reaction (ORR) in proton exchange membrane fuel cells are gaining momentum, with Fe-N-C catalysts comprising atomic FeN x sites the most promising candidate. Research and development is shifting from activity targets to improved stability of Fe-N-C catalysts in fuel cells. Their durability has hitherto been extensively studied using accelerated stress tests (AST) performed at room temperature and in inert-gas saturated acidic pH electrolyte. Here, 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 point towards strong carbon corrosion after AST in O2 , even when cycling at low potentials of 0.3-0.7 V vs. the reversible hydrogen electrode, while no corrosion occurred after any load cycling AST in Ar. The load cycling AST in O2 leads to the loss of a significant fraction of FeN x 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 H 2 O 2 and Fe sites via Fenton reactions.
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hal-02464078 , version 1 (02-02-2020)



Kavita Kumar, Laetitia Dubau, Michel Mermoux, Jingkun Li, Andrea Zitolo, et al.. On the Influence of Oxygen on the Degradation of Fe‐N‐C Catalysts. Angewandte Chemie, 2020, 59, pp.3235-3243. ⟨10.1002/ange.201912451⟩. ⟨hal-02464078⟩
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