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Deconvolution of Utilization, Site Density, and Turnover Frequency of Fe–Nitrogen–Carbon Oxygen Reduction Reaction Catalysts Prepared with Secondary N-Precursors

Leonard, Nathaniel D. ; Wagner, Stephan ; Luo, Fang ; Steinberg, Julian ; Ju, Wen ; Weidler, Natascha ; Wang, Huan ; Kramm, Ulrike I. ; Strasser, Peter (2018)
Deconvolution of Utilization, Site Density, and Turnover Frequency of Fe–Nitrogen–Carbon Oxygen Reduction Reaction Catalysts Prepared with Secondary N-Precursors.
In: ACS Catalysis, 8 (3)
doi: 10.1021/acscatal.7b02897
Artikel, Bibliographie

Kurzbeschreibung (Abstract)

Metal nitrogen carbon (MNC) catalysts represent a potential means of reducing cathode catalyst costs in low temperature fuel cell cathodes. Knowledge-based improvements have been hampered by the difficulty to deconvolute active site density and intrinsic turnover frequency. In the present work, MNC catalysts with a variety of secondary nitrogen precursors are addressed. CO chemisorption in combination with Mossbauer spectroscopy are utilized in order to unravel previously inaccessible relations between active site density, turnover frequency, and active site utilization. This analysis provides a more fundamental description and understanding of the origin of the catalytic reactivity; it also provides guidelines for further improvements. Secondary nitrogen precursors impact quantity, quality, dispersion, and utilization of active sites in distinct ways. Secondary nitrogen precursors with high nitrogen content and micropore etching capabilities are most effective in improving catalysts performance.

Typ des Eintrags: Artikel
Erschienen: 2018
Autor(en): Leonard, Nathaniel D. ; Wagner, Stephan ; Luo, Fang ; Steinberg, Julian ; Ju, Wen ; Weidler, Natascha ; Wang, Huan ; Kramm, Ulrike I. ; Strasser, Peter
Art des Eintrags: Bibliographie
Titel: Deconvolution of Utilization, Site Density, and Turnover Frequency of Fe–Nitrogen–Carbon Oxygen Reduction Reaction Catalysts Prepared with Secondary N-Precursors
Sprache: Englisch
Publikationsjahr: März 2018
Verlag: ACS Publications
Titel der Zeitschrift, Zeitung oder Schriftenreihe: ACS Catalysis
Jahrgang/Volume einer Zeitschrift: 8
(Heft-)Nummer: 3
DOI: 10.1021/acscatal.7b02897
URL / URN: https://doi.org/10.1021/acscatal.7b02897
Kurzbeschreibung (Abstract):

Metal nitrogen carbon (MNC) catalysts represent a potential means of reducing cathode catalyst costs in low temperature fuel cell cathodes. Knowledge-based improvements have been hampered by the difficulty to deconvolute active site density and intrinsic turnover frequency. In the present work, MNC catalysts with a variety of secondary nitrogen precursors are addressed. CO chemisorption in combination with Mossbauer spectroscopy are utilized in order to unravel previously inaccessible relations between active site density, turnover frequency, and active site utilization. This analysis provides a more fundamental description and understanding of the origin of the catalytic reactivity; it also provides guidelines for further improvements. Secondary nitrogen precursors impact quantity, quality, dispersion, and utilization of active sites in distinct ways. Secondary nitrogen precursors with high nitrogen content and micropore etching capabilities are most effective in improving catalysts performance.

Freie Schlagworte: Oxygen reduction reaction, nonprecious metal catalysts, fuel cells, Mossbauer spectroscopy,electrocatalysis
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 11:20
Letzte Änderung: 18 Aug 2021 08:17
PPN:
Sponsoren: U.I.K and S.W. acknowledge financial support by the BMBF via contract 05K16RD1 and by the Graduate School of Excellence Energy Science and Engineering (GRC1070)., P.S. acknowledges support by the European Commission and the Horizon 2020 framework funding under the FCH JU 2 program via the "CRECENDO" project.
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