Brüller, Sebastian ; Liang, Hai-Wei ; Kramm, Ulrike I. ; Krumpfer, Joseph W. ; Feng, Xinliang ; Müllen, Klaus (2015)
Bimetallic porous porphyrin polymer-derived non-precious metal electrocatalysts for oxygen reduction reactions.
In: Journal of Materials Chemistry A, 3 (47)
doi: 10.1039/C5TA06309D
Artikel, Bibliographie
Kurzbeschreibung (Abstract)
The development of efficient and stable electrocatalysts on the basis of non-precious metals (Co, Fe) is considered as one of the most promising routes to replace expensive and susceptible platinum as the oxygen reduction reaction (ORR) catalyst. Here we report a synthetic strategy for the precursor controlled, template-free preparation of novel mono- (Fe; Co) and bimetallic (Fe/Co) nitrogen-doped porous carbons and their electrocatalytic performance towards the ORR. The precursors are composed of metal–porphyrin based conjugated microporous polymers (M-CMPs with M = Fe; Co; Fe/Co) derived from polymerization of metalloporphyrins by the Suzuki polycondensation reaction, which enables the synthesis of bimetallic polymers with alternating metal–porphyrin units for the preparation of carbon-based catalysts with homogenously distributed CoN4 and FeN4 centres. Subsequent pyrolysis of the networks reveals the key role of pre-morphology and network composition on the active sites. 57Fe-Mössbauer spectroscopy was conducted on iron catalysts (Fe; Fe/Co) to determine the coordination of Fe within the N-doped carbon matrix and the catalytic activity-enhancing shift in electron density. In acidic media the bimetallic catalyst demonstrates a synergetic effect for cobalt and iron active sites, mainly through a 4-electron transfer process, achieving an onset potential of 0.88 V (versus a reversible hydrogen electrode) and a half-wave potential of 0.78 V, which is only 0.06 V less than that of the state-of-the-art Pt/C catalyst.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2015 |
| Autor(en): | Brüller, Sebastian ; Liang, Hai-Wei ; Kramm, Ulrike I. ; Krumpfer, Joseph W. ; Feng, Xinliang ; Müllen, Klaus |
| Art des Eintrags: | Bibliographie |
| Titel: | Bimetallic porous porphyrin polymer-derived non-precious metal electrocatalysts for oxygen reduction reactions |
| Sprache: | Englisch |
| Publikationsjahr: | 21 Dezember 2015 |
| Verlag: | The Royal Society of Chemistry |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Journal of Materials Chemistry A |
| Jahrgang/Volume einer Zeitschrift: | 3 |
| (Heft-)Nummer: | 47 |
| DOI: | 10.1039/C5TA06309D |
| Kurzbeschreibung (Abstract): | The development of efficient and stable electrocatalysts on the basis of non-precious metals (Co, Fe) is considered as one of the most promising routes to replace expensive and susceptible platinum as the oxygen reduction reaction (ORR) catalyst. Here we report a synthetic strategy for the precursor controlled, template-free preparation of novel mono- (Fe; Co) and bimetallic (Fe/Co) nitrogen-doped porous carbons and their electrocatalytic performance towards the ORR. The precursors are composed of metal–porphyrin based conjugated microporous polymers (M-CMPs with M = Fe; Co; Fe/Co) derived from polymerization of metalloporphyrins by the Suzuki polycondensation reaction, which enables the synthesis of bimetallic polymers with alternating metal–porphyrin units for the preparation of carbon-based catalysts with homogenously distributed CoN4 and FeN4 centres. Subsequent pyrolysis of the networks reveals the key role of pre-morphology and network composition on the active sites. 57Fe-Mössbauer spectroscopy was conducted on iron catalysts (Fe; Fe/Co) to determine the coordination of Fe within the N-doped carbon matrix and the catalytic activity-enhancing shift in electron density. In acidic media the bimetallic catalyst demonstrates a synergetic effect for cobalt and iron active sites, mainly through a 4-electron transfer process, achieving an onset potential of 0.88 V (versus a reversible hydrogen electrode) and a half-wave potential of 0.78 V, which is only 0.06 V less than that of the state-of-the-art Pt/C catalyst. |
| Fachbereich(e)/-gebiet(e): | 11 Fachbereich Material- und Geowissenschaften 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft 07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Anorganische Chemie > Fachgruppe Katalysatoren und Elektrokatalysatoren 07 Fachbereich Chemie 07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Anorganische Chemie |
| Hinterlegungsdatum: | 01 Mär 2016 09:34 |
| Letzte Änderung: | 18 Aug 2021 08:26 |
| PPN: | |
| Sponsoren: | This work was financially supported by the Max Planck Society through the program MaxNet Energy, ERC grant on NANOGRAPH, the project INSOLCELL and EC Graphene Flagship (CNECT-ICT-604391)., Financial support by the DFG funding of the Excellence Initiative, Darmstadt Graduate School of Excellence Energy Science and Engineering (GSC 1070) is gratefully acknowledged by UIK. |
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