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Operando Observation of Chemical Transformations of Iridium Oxide During Photoelectrochemical Water Oxidation
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. SLAC Natl Accelerator Lab, SUNCAT Ctr Interface Sci & Catalysis, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA.
Lawrence Berkeley Natl Lab, Joint Ctr Artificial Photosynth, 1 Cyclotron Rd, Berkeley, CA 94720 USA.
SLAC Natl Accelerator Lab, SUNCAT Ctr Interface Sci & Catalysis, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA;Tampere Univ Technol, Surface Sci Lab, Optoelect Res Ctr, FI-33101 Tampere, Finland.
SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Light Source, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA.
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2019 (English)In: ACS APPLIED ENERGY MATERIALS, ISSN 2574-0962, Vol. 2, no 2, p. 1371-1379Article in journal (Refereed) Published
Abstract [en]

Iridium oxide is one of the few catalysts capable of catalyzing the oxygen evolution reaction (OER) in both acidic and basic conditions. Understanding the mechanism of IrOx under realistic photoelectrochemical conditions is important for the development of integrated water-splitting systems. Herein, we have developed a highly efficient OER photoanode in pH 1 aqueous solutions based on a sputtered IrOx film and a p(+)n-Si light absorber, interfaced with a sputtered Au layer. Operando high-energy-resolution fluorescence detection X-ray absorption spectroscopy (HERFD XAS) was employed to monitor the oxidation state changes of IrOx during both electrochemical and photoelectrochemical (PEC) water oxidation reactions in pH 1 aqueous solutions. We observed a gradual increase of the average oxidation state of Ir with increasing anodic potential in the precatalytic region, followed by a reduction of Ir under O-2 evolution conditions. Consistent results were obtained on dark anodes and illuminated photoanodes. However, when the thickness of IrO2 was increased to 2 and 3 nm, the spectral changes became much less pronounced, and the reduction of Ir oxidation state after the OER onset was not observed. This is due to the lower surface-to-bulk ratio, where lattice oxygen sites in the bulk are not accessible for the formation of hydroxide. More generally, the operando method developed here can be extended to other materials, thereby providing a powerful tool for mechanism discovery and an enabling capability for catalyst design.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2019. Vol. 2, no 2, p. 1371-1379
Keywords [en]
operando method, high energy resolution fluorescence detection X-ray absorption spectroscopy (HERFD XAS), iridium oxide, electrochemical and photoelectrochemical (PEC), oxygen evolution reaction (OER)
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-379265DOI: 10.1021/acsaem.8b01945ISI: 000459948900051OAI: oai:DiVA.org:uu-379265DiVA, id: diva2:1296571
Funder
Knut and Alice Wallenberg Foundation, KAW 2012.0359Available from: 2019-03-15 Created: 2019-03-15 Last updated: 2019-03-15Bibliographically approved

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