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  Reactive Electrophilic OI-Species Evidenced in High-Performance Iridium Oxohydroxide Water Oxidation Electrocatalysts

Massué, C., Pfeifer, V., Gastel, M. v., Noack, J., Algara-Siller, G., Cap, S., et al. (2017). Reactive Electrophilic OI-Species Evidenced in High-Performance Iridium Oxohydroxide Water Oxidation Electrocatalysts. ChemSusChem, 10(23), 4786-4798. doi:10.1002/cssc.201701291.

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Datensatz-Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-FCC9-C Versions-Permalink: http://hdl.handle.net/21.11116/0000-0000-75E8-7
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 Urheber:
Massué, Cyriac1, 2, Autor              
Pfeifer, Verena1, 3, Autor              
Gastel, Maurice van4, Autor
Noack, Johannes1, Autor              
Algara-Siller, Gerardo1, Autor              
Cap, Sébastien1, Autor              
Schlögl, Robert1, 2, Autor              
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, escidoc:24023              
2Department of Heterogenous Reactions Max Planck Institute for Chemical Energy Conversion , Mülheim an der Ruhr 45470, Germany, escidoc:persistent22              
3Helmholtz-Zentrum Berlin für Materialien und Energie GmbH Elektronenspeicherring BESSY II , Berlin 12489 , Germany, escidoc:persistent22              
4Department of Molecular Theory and Spectroscopy Max Planck Institute for Chemical Energy Conversion , Mülheim an der Ruhr 45470, Germany, escidoc:persistent22              

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 Zusammenfassung: Although quasi-amorphous Ir-oxohydroxides have repeatedly been identified as superior oxygen evolution reaction (OER) electrocatalysts, an exact description of the performancerelevant species has so far remained a challenge. In this context, we report on the characterization of hydrothermally prepared IrIII/IV-oxohydroxides exhibiting exceptional OER-performance. It was found that holes in the O2p states of IrIII/IV-oxohydroxides result in reactive OI--species identified by characteristic NEXAFS-features. A prototypical titration reaction based on CO as a probe molecule shows that these OI--species are highly susceptible to nucleophilic attack at room temperature. Similarly to pre-activated oxygen involved in the biological OER in Photosystem II, the electrophilic OI--species evidenced in IrIII/IV-oxohydroxides are suggested to be precursors to species involved in the O-O bond formation during electrocatalytic OER. CO-titration also highlights a link between OER-performance and the surface/sub-surface mobility of OI--species. The superior electrocatalytic properties of IrIII/IV-oxohydroxides are thus explained by their ability to accommodate pre-activated electrophilic OI--species able to migrate within the lattice.

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Sprache(n): eng - Englisch
 Datum: 2017-09-062017-07-172017-09-202017-12-08
 Publikationsstatus: Online publiziert
 Seiten: 13
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1002/cssc.201701291
 Art des Abschluß: -

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Titel: ChemSusChem
Genre der Quelle: Zeitschrift
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Ort, Verlag, Ausgabe: Weinheim : Wiley-VCH
Seiten: 13 Band / Heft: 10 (23) Artikelnummer: - Start- / Endseite: 4786 - 4798 Identifikator: ISSN: 1864-5631
CoNE: http://pubman.mpdl.mpg.de/cone/journals/resource/1864-5631