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Hyperfine Interactions

, 239:7 | Cite as

Influence of sulfur in the precursor mixture on the structural composition of Fe-N-C catalysts

  • A. Janßen
  • I. Martinaiou
  • S. Wagner
  • N. Weidler
  • A. Shahraei
  • U. I. KrammEmail author
Article
Part of the following topical collections:
  1. Proceedings of the International Conference on the Applications of the Mössbauer Effect (ICAME 2017), Saint-Petersburg, Russia, 3-8 September 2017

Abstract

Fe-N-C catalysts were prepared by a new synthesis protocol at 800 C with subsequent acid leaching. The effect of sulfur was investigated by a systematic study in which the molar S/Fe ratio in the precursor was varied from 0.0 to 2.45. The obtained catalysts were evaluated for their ORR activity in 0.1 M H2 SO 4. In addition, the specific BET surface area was determined from N2 sorption measurements and structural characterization was made by Mößbauer spectroscopy. Catalysts contain FeN4 moieties and inorganic iron species. Structure activity correlation indicate a dominance of the ferrous low-spin FeN4 site for the ORR activity. This is in agreement with previous findings. In addition, the optimum in terms of ORR activity is in the same S/Me range as found for porphyrin-based catalysts. However, in contrast to previous conclusions of an avoidance of iron carbide formation by sulfur addition, a very high S/Fe ratio is required to obtain a catalyst free of iron carbide. Further work is required to identify the parameter that indeed enables inhibition of iron carbide formation.

Keywords

Fe-N-C catalysts Electrocatalysis Mößbauer spectroscopy Oxygen reduction reaction (ORR) 

Notes

Acknowledgements

Financial support by the German Research Foundation (DFG) for the Graduate School of Excellence Energy Science and Engineering (GSC1070), the Federal Ministry of Education and Research (BMBF) via the projects NUKFER (05K16RD1) and StRedO (03XP0092) is gratefully acknowledged.

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Copyright information

© Springer International Publishing AG, part of Springer Nature 2017

Authors and Affiliations

  1. 1.Graduate School of Excellence Energy Science and EngineeringTechnische Universität DarmstadtDarmstadtGermany
  2. 2.Department of Materials- and Earth SciencesTechnische Universität DarmstadtDarmstadtGermany
  3. 3.Department of ChemistryTechnische Universität DarmstadtDarmstadtGermany

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