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

MPG-Autoren
http://pubman.mpdl.mpg.de/cone/persons/resource/persons85190

Massué,  Cyriac
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Department of Heterogenous Reactions Max Planck Institute for Chemical Energy Conversion ;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons104550

Pfeifer,  Verena
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH Elektronenspeicherring BESSY II ;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons71845

Noack,  Johannes
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons144491

Algara-Siller,  Gerardo
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons104326

Cap,  Sébastien
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons22071

Schlögl,  Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Department of Heterogenous Reactions Max Planck Institute for Chemical Energy Conversion ;

Externe Ressourcen
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Volltexte (frei zugänglich)

Massu-_et_al-2017-ChemSusChem.pdf
(Verlagsversion), 2MB

Ergänzendes Material (frei zugänglich)

SI_2483126.pdf
(Ergänzendes Material), 2MB

Zitation

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.


Zitierlink: http://hdl.handle.net/11858/00-001M-0000-002D-FCC9-C
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.