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Stability of Fe–N–C Catalysts in Acidic Medium Studied by Operando Spectroscopy

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Choi,  Chang Hyuck
Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Baldizzone,  Claudio
Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Grote,  Jan-Philipp
Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Mayrhofer,  Karl Johann Jakob
Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Citation

Choi, C. H., Baldizzone, C., Grote, J.-P., Schuppert, A. K., Jaouen, F., & Mayrhofer, K. J. J. (2015). Stability of Fe–N–C Catalysts in Acidic Medium Studied by Operando Spectroscopy. Angewandte Chemie, International Edition, 54(43), 12753-12757. doi:10.1002/anie.201504903.


Cite as: https://hdl.handle.net/11858/00-001M-0000-0029-7820-E
Abstract
Fundamental understanding of non-precious metal catalysts for the oxygen reduction reaction (ORR) is the nub for the successful replacement of noble Pt in fuel cells and, therefore, of central importance for a technological breakthrough. Herein, the degradation mechanisms of a model high-performance Fe-N-C catalyst have been studied with online inductively coupled plasma mass spectrometry (ICP-MS) and differential electrochemical mass spectroscopy (DEMS) coupled to a modified scanning flow cell (SFC) system. We demonstrate that Fe leaching from iron particles occurs at low potential (< 0.7 V) without a direct adverse effect on the ORR activity, while carbon oxidation occurs at high potential (> 0.9 V) with a destruction of active sites such as FeNxCy species. Operando techniques combined with identical location-scanning transmission electron spectroscopy (IL-STEM) identify that the latter mechanism leads to a major ORR activity decay, depending on the upper potential limit and electrolyte temperature. Stable operando potential windows and operational strategies are suggested for avoiding degradation of Fe-N-C catalysts in acidic medium.