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

Janßen, A. ; Martinaiou, I. ; Wagner, S. ; Weidler, N. ; Shahraei, A. ; Kramm, U. I. (2018)
Influence of sulfur in the precursor mixture on the structural composition of Fe-N-C catalysts.
In: Hyperfine Interactions, 239 (1)
doi: 10.1007/s10751-017-1481-z
Artikel, Bibliographie

Kurzbeschreibung (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.

Typ des Eintrags: Artikel
Erschienen: 2018
Autor(en): Janßen, A. ; Martinaiou, I. ; Wagner, S. ; Weidler, N. ; Shahraei, A. ; Kramm, U. I.
Art des Eintrags: Bibliographie
Titel: Influence of sulfur in the precursor mixture on the structural composition of Fe-N-C catalysts
Sprache: Englisch
Publikationsjahr: 2018
Verlag: Springer International Publishing AG, part of Springer Nature
Titel der Zeitschrift, Zeitung oder Schriftenreihe: Hyperfine Interactions
Jahrgang/Volume einer Zeitschrift: 239
(Heft-)Nummer: 1
DOI: 10.1007/s10751-017-1481-z
Kurzbeschreibung (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.

Freie Schlagworte: Fe-N-C catalysts, Electrocatalysis, Mößbauer spectroscopy, Oxygen reduction reaction (ORR)
Fachbereich(e)/-gebiet(e): 11 Fachbereich Material- und Geowissenschaften
11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft
07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Anorganische Chemie > Fachgruppe Katalysatoren und Elektrokatalysatoren
07 Fachbereich Chemie
07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Anorganische Chemie
Hinterlegungsdatum: 06 Jul 2018 12:13
Letzte Änderung: 18 Aug 2021 07:39
PPN:
Sponsoren: 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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