Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 54, Issue 43, Pages 12753-12757Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201504903
Keywords
corrosion; degradation mechanisms; demetalation; electrochemistry; fuel cells
Categories
Funding
- Alexander von Humboldt Foundation
- IMPRS-SurMat doctoral program
- French Embassy by Campus France
- MAXNET Energy
- ANR [2011CHEX00401]
- Basic Science Research Program through National Research Foundation of Korea (NRF) - Ministry of Education, Science and Technology [NRF-2014R1A6A3A03056182]
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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.
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