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Catalysts 2019, 9(2), 144; https://doi.org/10.3390/catal9020144

The Challenge of Achieving a High Density of Fe-Based Active Sites in a Highly Graphitic Carbon Matrix

1
Institut Charles Gerhardt Montpellier, UMR 5253, CNRS, Université Montpellier, ENSCM, Place Eugène Bataillon, CEDEX 5, 34095 Montpellier, France
2
Department of Chemistry and Chemical Biology, Northeastern University, Boston, MA 02115, USA
3
Department of Materials Chemistry, National Institute of Chemistry, 1000 Ljubljana, Slovenia
4
Synchrotron SOLEIL, L’orme des Merisiers, BP 48 Saint Aubin, 91192 Gif-sur-Yvette, France
*
Authors to whom correspondence should be addressed.
Received: 11 December 2018 / Revised: 10 January 2019 / Accepted: 11 January 2019 / Published: 2 February 2019
(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)
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Abstract

As one of the most promising platinum group metal-free (PGM-free) catalysts for oxygen reduction reaction (ORR), Fe–N–C catalysts with a high density of FeNx moieties integrated in a highly graphitic carbon matrix with a proper porous structure have attracted extensive attention to combine the high activity, high stability and high accessibility of active sites. Herein, we investigated a ZnCl2/NaCl eutectic salts-assisted ionothermal carbonization method (ICM) to synthesize Fe–N–C catalysts with tailored porous structure, high specific surface area and a high degree of graphitization. However, it was found to be challenging to anchor a high density of FeNx sites onto highly graphitized carbon. Iron precursors with preexisting Fe–N coordination were required to form FeNx sites in the nitrogen-doped carbon with a high degree of graphitization, while individual Fe and N precursors led to a Fe–N–C catalyst with poor-ORR activity. This provides valuable insights into the synthesis-structure relationship. Moreover, the FeNx moieties were identified as the major active sites in acidic conditions, while both FeNx sites and Fe2O3 were found to be active in alkaline medium. View Full-Text
Keywords: oxygen reduction reaction; Fe–N–C; active site; graphitic carbon oxygen reduction reaction; Fe–N–C; active site; graphitic carbon
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Li, J.; Jia, Q.; Mukerjee, S.; Sougrati, M.-T.; Drazic, G.; Zitolo, A.; Jaouen, F. The Challenge of Achieving a High Density of Fe-Based Active Sites in a Highly Graphitic Carbon Matrix. Catalysts 2019, 9, 144.

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