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Evaluation of the Specific Activity of MNCs and the Intrinsic Activity of Tetrapyrrolic FeN4 Sites for the Oxygen Reduction Reaction
- M−N−C electrocatalysts are considered pivotal to replace expensive precious group metal-based materials in electrocatalytic conversions. However, their development is hampered by the limited availability of methods for the evaluation of the intrinsic activity of different active sites, like pyrrolic FeN4 sites within Fe−N−Cs. Currently, new synthetic procedures based on active-site imprinting followed by an ion exchange reaction, e.g. Zn-to-Fe, are producing single-site M−N−Cs with outstanding activity. Based on the same replacement principle, we employed a conservative iron extraction to partially remove the Fe ions from the N4 cavities in Fe−N−Cs. Having catalysts with the same morphological properties and Fe ligation that differ solely in Fe content allows for the facile determination of the decrease in density of active sites and their turn-over frequency. In this way, insight into the specific activity of M−N−Cs is obtained and for single-site catalysts the intrinsic activity ofM−N−C electrocatalysts are considered pivotal to replace expensive precious group metal-based materials in electrocatalytic conversions. However, their development is hampered by the limited availability of methods for the evaluation of the intrinsic activity of different active sites, like pyrrolic FeN4 sites within Fe−N−Cs. Currently, new synthetic procedures based on active-site imprinting followed by an ion exchange reaction, e.g. Zn-to-Fe, are producing single-site M−N−Cs with outstanding activity. Based on the same replacement principle, we employed a conservative iron extraction to partially remove the Fe ions from the N4 cavities in Fe−N−Cs. Having catalysts with the same morphological properties and Fe ligation that differ solely in Fe content allows for the facile determination of the decrease in density of active sites and their turn-over frequency. In this way, insight into the specific activity of M−N−Cs is obtained and for single-site catalysts the intrinsic activity of the site is accessible. This new approach surpasses limitations of methods that rely on probe molecules and, together with those techniques, offers a novel tool to unfold the complexity of Fe−N−C catalyst and M−N−Cs in general.…
Autor*innen: | D. Menga, Ana de Oliveira Guilherme BuzanichORCiD, F. Wagner, Tim-Patrick FellingerORCiD |
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Dokumenttyp: | Zeitschriftenartikel |
Veröffentlichungsform: | Verlagsliteratur |
Sprache: | Englisch |
Titel des übergeordneten Werkes (Englisch): | Angewandte Chemie International Edition |
Jahr der Erstveröffentlichung: | 2022 |
Organisationseinheit der BAM: | 3 Gefahrgutumschließungen; Energiespeicher |
3 Gefahrgutumschließungen; Energiespeicher / 3.0 Abteilungsleitung und andere | |
Veröffentlichende Institution: | Bundesanstalt für Materialforschung und -prüfung (BAM) |
Verlag: | Wiley-VHC |
Jahrgang/Band: | 61 |
Ausgabe/Heft: | 50 |
Aufsatznummer: | e202207089 |
Erste Seite: | 1 |
Letzte Seite: | 6 |
DDC-Klassifikation: | Technik, Medizin, angewandte Wissenschaften / Ingenieurwissenschaften / Angewandte Physik |
Freie Schlagwörter: | Fe-N-C catalysts; Fuel Cells; M-N-C catalysts |
Themenfelder/Aktivitätsfelder der BAM: | Energie |
Energie / Elektrische Energiespeicher und -umwandlung | |
DOI: | 10.1002/anie.202207089 |
URN: | urn:nbn:de:kobv:b43-567406 |
ISSN: | 1433-7851 |
Verfügbarkeit des Dokuments: | Datei für die Öffentlichkeit verfügbar ("Open Access") |
Lizenz (Deutsch): | Creative Commons - CC BY - Namensnennung 4.0 International |
Datum der Freischaltung: | 02.01.2023 |
Referierte Publikation: | Ja |
Datum der Eintragung als referierte Publikation: | 02.01.2023 |
Schriftenreihen ohne Nummerierung: | Wissenschaftliche Artikel der BAM |