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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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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-FCC9-C Version Permalink: http://hdl.handle.net/21.11116/0000-0000-75E8-7
Genre: Journal Article

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 Creators:
Massué, Cyriac1, 2, Author              
Pfeifer, Verena1, 3, Author              
Gastel, Maurice van4, Author
Noack, Johannes1, Author              
Algara-Siller, Gerardo1, Author              
Cap, Sébastien1, Author              
Schlögl, Robert1, 2, Author              
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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 Abstract: 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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Language(s): eng - English
 Dates: 2017-09-062017-07-172017-09-202017-12-08
 Publication Status: Published online
 Pages: 13
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1002/cssc.201701291
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Title: ChemSusChem
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: 13 Volume / Issue: 10 (23) Sequence Number: - Start / End Page: 4786 - 4798 Identifier: ISSN: 1864-5631
CoNE: http://pubman.mpdl.mpg.de/cone/journals/resource/1864-5631