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On the effect of sulfite ions on the structural composition and ORR activity of Fe-N-C catalysts

Wagner, S. ; Martinaiou, I. ; Shahraei, A. ; Weidler, N. ; Kramm, Ulrike I. (2018)
On the effect of sulfite ions on the structural composition and ORR activity of Fe-N-C catalysts.
In: Hyperfine Interactions, 239 (1)
doi: 10.1007/s10751-017-1485-8
Artikel, Bibliographie

Kurzbeschreibung (Abstract)

Fe-N-C catalysts are the most promising group of non-precious metal catalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFC). This study focusses on two different porphyrin-based Fe-N-C catalysts and a Fe-N-C catalyst prepared from alternative precursors under S-addition. Catalysts are subjected to a wet-chemical poisoning treatment by sulfite ions . A mechanism for the deactivation process of the active sites is proposed. ORR activity is evaluated for the original catalysts (OC) and for the poisoned catalysts in 0.1 M H2SO4. In addition, the structural composition of the catalysts is identified by Mobauer spectroscopy. Our results show that the sulfite ions bound irreversible to the catalysts and the catalysts lose significant fractions of their ORR activity while in Mobauer spectroscopy a new doublet appears. Based on the results, possible models for the binding of the ambident sulfite ion to the FeN4 centers are discussed.

Typ des Eintrags: Artikel
Erschienen: 2018
Autor(en): Wagner, S. ; Martinaiou, I. ; Shahraei, A. ; Weidler, N. ; Kramm, Ulrike I.
Art des Eintrags: Bibliographie
Titel: On the effect of sulfite ions on the structural composition and ORR activity of Fe-N-C catalysts
Sprache: Englisch
Publikationsjahr: 15 Januar 2018
Verlag: Springer
Titel der Zeitschrift, Zeitung oder Schriftenreihe: Hyperfine Interactions
Jahrgang/Volume einer Zeitschrift: 239
(Heft-)Nummer: 1
DOI: 10.1007/s10751-017-1485-8
Kurzbeschreibung (Abstract):

Fe-N-C catalysts are the most promising group of non-precious metal catalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFC). This study focusses on two different porphyrin-based Fe-N-C catalysts and a Fe-N-C catalyst prepared from alternative precursors under S-addition. Catalysts are subjected to a wet-chemical poisoning treatment by sulfite ions . A mechanism for the deactivation process of the active sites is proposed. ORR activity is evaluated for the original catalysts (OC) and for the poisoned catalysts in 0.1 M H2SO4. In addition, the structural composition of the catalysts is identified by Mobauer spectroscopy. Our results show that the sulfite ions bound irreversible to the catalysts and the catalysts lose significant fractions of their ORR activity while in Mobauer spectroscopy a new doublet appears. Based on the results, possible models for the binding of the ambident sulfite ion to the FeN4 centers are discussed.

Freie Schlagworte: Fe-N-C catalyst, Mossbauer spectroscopy, PEMFC, oxygen reduction reaction
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: 11 Dez 2018 11:36
Letzte Änderung: 18 Aug 2021 07:38
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