Fe-Sn-N-C Catalysts

Advancing Oxygen Reduction Reaction Performance

verfasst von: Julia G. Buschermöhle, Julia Müller-Hülstede, Henrike Schmies, Dana Schonvogel, Tanja Zierdt, Rene Lucka, Franz Renz, Peter Wagner, Michael Wark
Abstract: High-temperature proton exchange membrane fuel cells (HT-PEMFCs) typically rely on platinum-based catalysts, which require high loadings due to Pt deactivation by phosphates from the phosphoric acid-doped membrane. As alternative catalysts for the oxygen reduction reaction, metal-nitrogen-carbons (M-N-Cs) are promising due to their high intrinsic activity and tolerance to phosphates. However, low volumetric activity compared to Pt nanoparticles on carbon blacks (Pt/C) and insufficient stability limit their applicability. In order to enhance the stability and activity of Fe-N-Cs, this study investigates the incorporation of tin as a second metal, resulting in Fe-Sn-N-Cs, prepared by a metal-organic framework (MOF)-based approach. Stable and highly active catalysts with total mass activities of 8.2 A g^-1 (Fe-Sn-N-C (1:1)) and 19.3 A g^-1 (Fe-Sn-N-C (1:0.3)) in 0.5 mol L^-1 H₃PO₄, drastically exceeding those of the commercial Fe-N-C catalyst PMF-014401 (Pajarito-Powder, 4.8 A g^-1), are obtained by a synthesis without the need for subsequent purification steps. A stress test under harsh conditions (0.6-1.0 V_RHE, 10,000 cycles, O₂-saturated electrolyte) ascertains stability-enhancing effects of tin, highlighting an increase in stability in conjunction with the tin content. These results provide a valuable contribution to the development of cost-effective HT-PEMFCs by significantly enhancing the catalytic activity of platinum group metal-free catalysts.
Organisationseinheit(en): Institut für Anorganische Chemie
Externe Organisation(en): Deutsches Zentrum für Luft- und Raumfahrt e.V. (DLR)
Carl von Ossietzky Universität Oldenburg
Typ: Artikel
Journal: ACS catalysis
Band: 15
Seiten: 4477-4488
Anzahl der Seiten: 12
ISSN: 2155-5435
Publikationsdatum: 21.03.2025
Publikationsstatus: Veröffentlicht
Peer-reviewed: Ja
ASJC Scopus Sachgebiete: Katalyse, Allgemeine Chemie
Elektronische Version(en): https://doi.org/10.1021/acscatal.4c06338 (Zugang: Offen)

BibTeX

@article{fbe48ce0d7544bada81daf869eb2f44b,
title = "Fe-Sn-N-C Catalysts: Advancing Oxygen Reduction Reaction Performance",
abstract = "High-temperature proton exchange membrane fuel cells (HT-PEMFCs) typically rely on platinum-based catalysts, which require high loadings due to Pt deactivation by phosphates from the phosphoric acid-doped membrane. As alternative catalysts for the oxygen reduction reaction, metal-nitrogen-carbons (M-N-Cs) are promising due to their high intrinsic activity and tolerance to phosphates. However, low volumetric activity compared to Pt nanoparticles on carbon blacks (Pt/C) and insufficient stability limit their applicability. In order to enhance the stability and activity of Fe-N-Cs, this study investigates the incorporation of tin as a second metal, resulting in Fe-Sn-N-Cs, prepared by a metal-organic framework (MOF)-based approach. Stable and highly active catalysts with total mass activities of 8.2 A g-1 (Fe-Sn-N-C (1:1)) and 19.3 A g-1 (Fe-Sn-N-C (1:0.3)) in 0.5 mol L-1 H3PO4, drastically exceeding those of the commercial Fe-N-C catalyst PMF-014401 (Pajarito-Powder, 4.8 A g-1), are obtained by a synthesis without the need for subsequent purification steps. A stress test under harsh conditions (0.6-1.0 VRHE, 10,000 cycles, O2-saturated electrolyte) ascertains stability-enhancing effects of tin, highlighting an increase in stability in conjunction with the tin content. These results provide a valuable contribution to the development of cost-effective HT-PEMFCs by significantly enhancing the catalytic activity of platinum group metal-free catalysts.",
keywords = "M-N-C, metal organic frameworks, multimetallic catalysts, non-PGM catalysts, oxygen reduction reaction, PEM fuel cells, rotating ring disc electrode",
author = "Buscherm{\"o}hle, {Julia G.} and Julia M{\"u}ller-H{\"u}lstede and Henrike Schmies and Dana Schonvogel and Tanja Zierdt and Rene Lucka and Franz Renz and Peter Wagner and Michael Wark",
note = "Publisher Copyright: {\textcopyright} 2025 The Authors. Published by American Chemical Society.",
year = "2025",
month = mar,
day = "21",
doi = "10.1021/acscatal.4c06338",
language = "English",
volume = "15",
pages = "4477--4488",
journal = "ACS catalysis",
issn = "2155-5435",
publisher = "American Chemical Society",
number = "6",
}