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High-Yield Synthesis of Fe-NC Electrocatalysts Using Mg2+ Templating and Schiff-Base Porous Organic Polymers
- The decoupled synthesis of Fe-NC single-site electrocatalysts mediated by Lewis acids enables high active site density and utilization. However, current approaches often rely on small organic molecules and suffer from low synthesis yields due to the high Lewis acid-to-precursor ratios required to achieve highly porous carbons. Here, a porous organic polymer (POP) based on 2,4,6-Triaminopyrimidine (TAP) is utilized as a carbon-nitrogen-based scaffold for the synthesis of Fe─NC electrocatalysts. By tuning the amounts of MgCl2 ·6H2O used both as porogen and active site templating agent, synthetic yields exceeding 45% are achieved, a significant improvement compared to the 6% yield from the molecular analogue and the highest reported forMg2+ templated systems. Subsequent low-temperature exchange with Fe leads to atomically dispersed FeNx, minimizing Fe aggregation. The resulting materials exhibit high specific surface areas (>1000 m2 g−1) with micro-, meso-, and macropores, which promoteThe decoupled synthesis of Fe-NC single-site electrocatalysts mediated by Lewis acids enables high active site density and utilization. However, current approaches often rely on small organic molecules and suffer from low synthesis yields due to the high Lewis acid-to-precursor ratios required to achieve highly porous carbons. Here, a porous organic polymer (POP) based on 2,4,6-Triaminopyrimidine (TAP) is utilized as a carbon-nitrogen-based scaffold for the synthesis of Fe─NC electrocatalysts. By tuning the amounts of MgCl2 ·6H2O used both as porogen and active site templating agent, synthetic yields exceeding 45% are achieved, a significant improvement compared to the 6% yield from the molecular analogue and the highest reported forMg2+ templated systems. Subsequent low-temperature exchange with Fe leads to atomically dispersed FeNx, minimizing Fe aggregation. The resulting materials exhibit high specific surface areas (>1000 m2 g−1) with micro-, meso-, and macropores, which promote mass transport and active site accessibility. Compared to Fe─NC synthesized via direct pyrolysis of Fe-coordinated POP, the decoupled method enables significantly higher catalytic activity in both alkaline and acidic media, and delivers 1 A cm−2 at 0.687 ± 0.004 VRHE in an alkaline gas diffusion electrode, highlighting its potential for practical oxygen reduction devices.…


| Autor*innen: | Eliot Petitdemange, Jinjie Zhu, Angus PedersenORCiD, Joseph Parker, Esmael Balaghi, Shaohua Li, Silvia Favero, José Ignacio Martínez, Sarah Haigh, Maria-Magdalena Titirici, Anna Fischer, Jesús Barrio |
|---|---|
| Dokumenttyp: | Zeitschriftenartikel |
| Veröffentlichungsform: | Verlagsliteratur |
| Sprache: | Englisch |
| Titel des übergeordneten Werkes (Englisch): | Advanced Functional Materials |
| Jahr der Erstveröffentlichung: | 2025 |
| Organisationseinheit der BAM: | 3 Gefahrgutumschließungen; Energiespeicher |
| 3 Gefahrgutumschließungen; Energiespeicher / 3.6 Elektrochemische Energiematerialien | |
| Veröffentlichende Institution: | Bundesanstalt für Materialforschung und -prüfung (BAM) |
| Verlag: | Wiley-VCH GmbH |
| Aufsatznummer: | e18944 |
| Erste Seite: | 1 |
| Letzte Seite: | 15 |
| DDC-Klassifikation: | Technik, Medizin, angewandte Wissenschaften / Ingenieurwissenschaften / Angewandte Physik |
| Freie Schlagwörter: | Oxygen reduction; Porous Organic Polymers; Single Atom |
| Themenfelder/Aktivitätsfelder der BAM: | Energie |
| Energie / Elektrische Energiespeicher und -umwandlung | |
| DOI: | 10.1002/adfm.202518944 |
| URN: | urn:nbn:de:kobv:b43-652618 |
| ISSN: | 1616-3028 |
| Verfügbarkeit des Dokuments: | Datei für die Öffentlichkeit verfügbar ("Open Access") |
| Lizenz (Deutsch): | Creative Commons - CC BY - Namensnennung 4.0 International |
| Datum der Freischaltung: | 29.12.2025 |
| Referierte Publikation: | Ja |
| Datum der Eintragung als referierte Publikation: | 23.03.2026 |
| Schriftenreihen ohne Nummerierung: | Wissenschaftliche Artikel der BAM |


