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Effect of metal species on the stability of Me-N-C catalysts during accelerated stress tests mimicking the start-up and shut-down conditions

Martinaiou, Ioanna and Shahraei, Ali and Grimm, Fabian and Zhang, Hongbin and Wittich, Carolin and Klemenz, Sebastian and Dolique, Stephanie J. and Kleebe, Hans-Joachim and Stark, Robert W. and Kramm, Ulrike I. (2017):
Effect of metal species on the stability of Me-N-C catalysts during accelerated stress tests mimicking the start-up and shut-down conditions.
In: Electrochimica Acta, Elsevier Science Publishing, pp. 183-196, 243, ISSN 00134686, DOI: 10.1016/j.electacta.2017.04.134, [Online-Edition: https://doi.org/10.1016/j.electacta.2017.04.134],
[Article]

Abstract

Currently, Me-N-C catalysts are the most prominent alternative to Pt/C catalysts for the oxygen reduction reaction in acidic media. It is well known that the achievable activity and selectivity strongly correlates with the nature of metal species. However, so far the effect of the metal species on the stability of these catalysts was not investigated systematically. In this work, a group of 13 different Me-N-C catalysts were investigated with respect to their activity and stability in accelerated stress tests mimicking the start-up and shut-down conditions (AST_SSC). A strong correlation between the nitrogen content assigned to different MeN4 sites and the D3 band from Raman spectroscopy is found. Moreover, we were able to correlate changes in the D3 band and variations in the displacement of the metal atoms out of the N4 plane with the losses in ORR activity. Based on these findings, we propose a model for the degradation of Me-N-C catalysts during accelerated stress tests mimicking the start-up and shut-down conditions.

Item Type: Article
Erschienen: 2017
Creators: Martinaiou, Ioanna and Shahraei, Ali and Grimm, Fabian and Zhang, Hongbin and Wittich, Carolin and Klemenz, Sebastian and Dolique, Stephanie J. and Kleebe, Hans-Joachim and Stark, Robert W. and Kramm, Ulrike I.
Title: Effect of metal species on the stability of Me-N-C catalysts during accelerated stress tests mimicking the start-up and shut-down conditions
Language: English
Abstract:

Currently, Me-N-C catalysts are the most prominent alternative to Pt/C catalysts for the oxygen reduction reaction in acidic media. It is well known that the achievable activity and selectivity strongly correlates with the nature of metal species. However, so far the effect of the metal species on the stability of these catalysts was not investigated systematically. In this work, a group of 13 different Me-N-C catalysts were investigated with respect to their activity and stability in accelerated stress tests mimicking the start-up and shut-down conditions (AST_SSC). A strong correlation between the nitrogen content assigned to different MeN4 sites and the D3 band from Raman spectroscopy is found. Moreover, we were able to correlate changes in the D3 band and variations in the displacement of the metal atoms out of the N4 plane with the losses in ORR activity. Based on these findings, we propose a model for the degradation of Me-N-C catalysts during accelerated stress tests mimicking the start-up and shut-down conditions.

Journal or Publication Title: Electrochimica Acta
Volume: 243
Publisher: Elsevier Science Publishing
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Earth Science
11 Department of Materials and Earth Sciences > Earth Science > Geo-Material-Science
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Catalysts and Electrocatalysts
11 Department of Materials and Earth Sciences > Material Science > Physics of Surfaces
11 Department of Materials and Earth Sciences > Material Science > Theory of Magnetic Materials
07 Department of Chemistry
07 Department of Chemistry > Fachgebiet Anorganische Chemie
07 Department of Chemistry > Physical Chemistry
Date Deposited: 06 Jul 2018 12:28
DOI: 10.1016/j.electacta.2017.04.134
Official URL: https://doi.org/10.1016/j.electacta.2017.04.134
Funders: Financial Support by the German Research Foundation (DFG) via the Excellence initiative TU Darmstadt Graduate School of Excellence Energy Science and Engineering (ESE) (GSC1070) is gratefully acknowledged.
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