Thermal synthesis of electron deficient oxygen species on crystalline IrO 2

Carbonio, E. A.; Sulzmann, F.; Teschner, D.; Velasco-Vélez, J. J.; Hävecker, M.; Gericke, A. Knop; Schlögl, R.; Jones, T.

doi:10.1039/D3CY01026K

Title: Thermal synthesis of electron deficient oxygen species on crystalline IrO ₂

Journal Article · Mon Feb 05 00:00:00 EST 2024 · Catalysis Science and Technology

DOI:https://doi.org/10.1039/D3CY01026K· OSTI ID:2280391

^[1]; Sulzmann, F. ^[2]; Teschner, D. ^[3]; Velasco-Vélez, J. J. ^[4]; Hävecker, M. ^[5]; Gericke, A. Knop ^[3]; Schlögl, R. ^[6]; Jones, T. ^[7]

Catalysts for Energy, Energy Materials In-situ Laboratory (EMIL), Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, BESSY II, Albert-Einstein-Straße 15, 12489 Berlin, Germany, Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany
Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany
Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany, Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, Stiftstraße 34-36, Mülheim an der Ruhr 45470, Germany
Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany, Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, Stiftstraße 34-36, Mülheim an der Ruhr 45470, Germany, ALBA Synchrotron Light Source, Cerdanyola del Vallés (Barcelona) 08290, Spain
Catalysts for Energy, Energy Materials In-situ Laboratory (EMIL), Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, BESSY II, Albert-Einstein-Straße 15, 12489 Berlin, Germany, Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, Stiftstraße 34-36, Mülheim an der Ruhr 45470, Germany
Catalysts for Energy, Energy Materials In-situ Laboratory (EMIL), Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, BESSY II, Albert-Einstein-Straße 15, 12489 Berlin, Germany, Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany, Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, Stiftstraße 34-36, Mülheim an der Ruhr 45470, Germany
Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany, Theoretical Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA

Water splitting is a promising technology in the path towards complete renewable energy within the hydrogen economy but overcoming the sluggishness of the oxygen evolution reaction (OER) is a major challenge. Iridium-based oxides remain the most attractive materials for the OER under acidic conditions since they offer the combination of activity and stability. Gaining knowledge about how these materials have such an ability is of great interest to develop improved electrocatalysts for the OER. Among the different iridium-based oxides the materials with high concentrations of electron deficient oxygen (O^I—) have been shown to have higher OER activity, however, they also have high dissolution rates, seemingly due to the presence or formation of Ir^III species. In contrast, rutile-type IrO₂, which does not contain Ir^III species, has high dissolution resistance but the OER activity remains comparatively low as only low coverages of O^I— species are formed under OER. The apparent link between O^I— and Ir^III species that comes from these observations has yet to be proven. In this work, using ab initio thermodynamics and in situ X-ray photoelectron and absorption spectroscopy we show that the same electrophilic O^I— species that appear on Ir-based oxides under OER can be formed on Ir^IV+δ by mild thermal oxidation of rutile-type IrO₂, without the presence Ir^III species.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 2280391

Alternate ID(s):: OSTI ID: 2323538

Report Number(s):: LA-UR-23-33448; CSTAGD

Journal Information:: Catalysis Science and Technology, Journal Name: Catalysis Science and Technology Vol. 14 Journal Issue: 3; ISSN 2044-4753

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United Kingdom

Language:: English

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