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A simple decagram-scale synthesis of an atomically dispersed, hierarchically porous Fe–N–C catalyst for acidic ORR

  • Carbons doped with iron and nitrogen (Fe–N–Cs) are highly promising electrocatalysts for energy conversion reactions in the oxygen, nitrogen and carbon cycles. Containing no platinum group metals, they nevertheless compete with platinum-based catalysts in crucial fuel cell reactions, such as oxygen reduction in acid. Yet deployment of Fe–N–Cs in fuel cells requires also a flow-enhancing pore structure, and a scalable synthesis procedure – a rarely-met combination of requirements. We now report such a simple synthesis of over 10 g of an Fe–N–C catalyst with high activity towards oxygen reduction in acid. Atomically-dispersed Fe–N4 active sites were designed orthogonally and simultaneously with hierarchical micro-, meso- and macroporosity, by exploiting a dual role of magnesium ions during pyrolysis. Combining the “active site imprinting” and “self-templating” strategies in a single novel magnesium iminodiacetate precursor yielded a catalyst with high specific surface area (SSA > 1600 m2Carbons doped with iron and nitrogen (Fe–N–Cs) are highly promising electrocatalysts for energy conversion reactions in the oxygen, nitrogen and carbon cycles. Containing no platinum group metals, they nevertheless compete with platinum-based catalysts in crucial fuel cell reactions, such as oxygen reduction in acid. Yet deployment of Fe–N–Cs in fuel cells requires also a flow-enhancing pore structure, and a scalable synthesis procedure – a rarely-met combination of requirements. We now report such a simple synthesis of over 10 g of an Fe–N–C catalyst with high activity towards oxygen reduction in acid. Atomically-dispersed Fe–N4 active sites were designed orthogonally and simultaneously with hierarchical micro-, meso- and macroporosity, by exploiting a dual role of magnesium ions during pyrolysis. Combining the “active site imprinting” and “self-templating” strategies in a single novel magnesium iminodiacetate precursor yielded a catalyst with high specific surface area (SSA > 1600 m2 g−1), a flow-enhancing hierarchical porosity, and high relative abundance of the most desirable D1-type Fe–N4 sites (43%, by Mössbauer spectroscopy at 4.2 K). Despite the relatively low iron contents, the catalysts feature halfwave potentials up to 0.70 V vs. RHE at pH 1 and a mass activity of 1.22 A g−1 at 0.8 V vs. RHE in RDE experiments. Thanks to the simple and scalable synthesis, this active and stable catalyst may serve as a workhorse in academic and industrial research into atomically-dispersed ORR electrocatalysis.zeige mehrzeige weniger

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Metadaten
Autor*innen:B. Koyutürk, E. Farber, F. Wagner, Tim-Patrick FellingerORCiD, D. Eisenberg
Dokumenttyp:Zeitschriftenartikel
Veröffentlichungsform:Verlagsliteratur
Sprache:Englisch
Titel des übergeordneten Werkes (Englisch):Journal of Materials Chemistry A
Jahr der Erstveröffentlichung:2022
Organisationseinheit der BAM:3 Gefahrgutumschließungen; Energiespeicher
3 Gefahrgutumschließungen; Energiespeicher / 3.1 Sicherheit von Gefahrgutverpackungen und Batterien
Veröffentlichende Institution:Bundesanstalt für Materialforschung und -prüfung (BAM)
Verlag:Royal Society of Chemistry
Erste Seite:1
Letzte Seite:10
DDC-Klassifikation:Technik, Medizin, angewandte Wissenschaften / Ingenieurwissenschaften / Angewandte Physik
Freie Schlagwörter:Catalysis; Electrochemistry; Fe-N-C catalysts; Fuel Cells
Themenfelder/Aktivitätsfelder der BAM:Energie
Energie / Elektrische Energiespeicher und -umwandlung
DOI:10.1039/d2ta00925k
URN:urn:nbn:de:kobv:b43-550113
ISSN:2050-7488
Verfügbarkeit des Dokuments:Datei im Netzwerk der BAM verfügbar ("Closed Access")
Datum der Freischaltung:15.06.2022
Referierte Publikation:Ja
Datum der Eintragung als referierte Publikation:15.06.2022
Schriftenreihen ohne Nummerierung:Wissenschaftliche Artikel der BAM
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