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Resolving the Dilemma of Fe-N-C Catalysts by the Selective Synthesis of Tetrapyrrolic Active Sites via an Imprinting Strategy

  • Combining the abundance and inexpensiveness of their constituent elements with their atomic dispersion, atomically dispersed Fe−N−C catalysts represent the most promising alternative to precious-metal-based materials in proton Exchange membrane (PEM) fuel cells. Due to the high temperatures involved in their synthesis and the sensitivity of Fe ions toward carbothermal reduction, current synthetic methods are intrinsically limited in type and amount of the desired, catalytically active Fe−N4 sites, and high active site densities have been out of reach (dilemma of Fe−N−C catalysts). We herein identify a paradigm change in the synthesis of Fe−N−C catalysts arising from the developments of other M−N−C single-atom catalysts. Supported by DFT calculations we propose fundamental principles for the synthesis of M−N−C materials. We further exploit the proposed principles in a novel synthetic strategy to surpass the dilemma of Fe−N−C catalysts. The selective formation of tetrapyrrolic Zn−N4Combining the abundance and inexpensiveness of their constituent elements with their atomic dispersion, atomically dispersed Fe−N−C catalysts represent the most promising alternative to precious-metal-based materials in proton Exchange membrane (PEM) fuel cells. Due to the high temperatures involved in their synthesis and the sensitivity of Fe ions toward carbothermal reduction, current synthetic methods are intrinsically limited in type and amount of the desired, catalytically active Fe−N4 sites, and high active site densities have been out of reach (dilemma of Fe−N−C catalysts). We herein identify a paradigm change in the synthesis of Fe−N−C catalysts arising from the developments of other M−N−C single-atom catalysts. Supported by DFT calculations we propose fundamental principles for the synthesis of M−N−C materials. We further exploit the proposed principles in a novel synthetic strategy to surpass the dilemma of Fe−N−C catalysts. The selective formation of tetrapyrrolic Zn−N4 sites in a tailor-made Zn−N−C material is utilized as an active-site imprint for the preparation of a corresponding Fe−N−C catalyst. By successive low- and high-temperature ion exchange reactions, we obtain a phase-pure Fe−N−C catalyst, with a high loading of atomically dispersed Fe (>3 wt %). Moreover, the catalyst is entirely composed of tetrapyrrolic Fe−N4 sites. The density of tetrapyrrolic Fe−N4 sites is more than six times as high as for previously reported tetrapyrrolic single-site Fe−N−C fuel cell catalysts.zeige mehrzeige weniger

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Autor*innen:D. Menga, J. L. Low, Y.-S. Li, I. Arcon, B. Koyutürk, F. Wagner, F. Ruiz-Zepeda, M. Gaberscek, B. Paulus, Tim-Patrick FellingerORCiD
Dokumenttyp:Zeitschriftenartikel
Veröffentlichungsform:Verlagsliteratur
Sprache:Englisch
Titel des übergeordneten Werkes (Englisch):Journal of the American Chemical Society
Jahr der Erstveröffentlichung:2021
Organisationseinheit der BAM:3 Gefahrgutumschließungen; Energiespeicher
3 Gefahrgutumschließungen; Energiespeicher / 3.1 Sicherheit von Gefahrgutverpackungen und Batterien
Verlag:American Chemical Society
Jahrgang/Band:143
Ausgabe/Heft:43
Erste Seite:18010
Letzte Seite:18019
DDC-Klassifikation:Technik, Medizin, angewandte Wissenschaften / Ingenieurwissenschaften / Angewandte Physik
Freie Schlagwörter:Carbon materials; Fe-N-C catalyst; Fuel cell; Precious-group metal-free catalyst; Single-site catalyst; Tetrapyrrolic active-site
Themenfelder/Aktivitätsfelder der BAM:Energie
DOI:10.1021/jacs.1c04884
ISSN:1520-5126
Verfügbarkeit des Dokuments:Datei im Netzwerk der BAM verfügbar ("Closed Access")
Datum der Freischaltung:04.11.2021
Referierte Publikation:Ja
Datum der Eintragung als referierte Publikation:01.11.2021
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