Operando XAS Study of the Surface Oxidation State on a Monolayer IrOx on RuOx and Ru Oxide Based Nanoparticles for Oxygen Evolution in Acidic Media

Pedersen, Anders F.; Escudero-Escribano, Maria; Sebok, Bela; Bodin, Anders; Paoli, Elisa; Frydendal, Rasmus; Friebel, Daniel; Stephens, Ifan E.  L.; Rossmeisl, Jan; Chorkendorff, Ib; Nilsson, Anders

doi:10.1021/acs.jpcb.7b06982

Title: Operando XAS Study of the Surface Oxidation State on a Monolayer IrO_x on RuO_x and Ru Oxide Based Nanoparticles for Oxygen Evolution in Acidic Media

Journal Article · Fri Oct 13 00:00:00 EDT 2017 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI:https://doi.org/10.1021/acs.jpcb.7b06982· OSTI ID:1471512

Pedersen, Anders F. ^[1]; Escudero-Escribano, Maria ^[2]; Sebok, Bela ^[1]; Bodin, Anders ^[1]; Paoli, Elisa ^[1]; Frydendal, Rasmus ^[1]; Friebel, Daniel ^[3]; Stephens, Ifan E. L. ^[4]; Rossmeisl, Jan ^[5];

^[1];

^[6]

Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics
Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics; Univ. of Copenhagen (Denmark). Dept. of Chemistry; Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis, Dept. of Chemical Engineering
Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis, Dept. of Chemical Engineering
Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics; Imperial College, London (United Kingdom). Dept. of Materials
Univ. of Copenhagen (Denmark). Dept. of Chemistry
Stockholm Univ. (Sweden). Fysikum

Here in this paper we present surface sensitive operando XAS L-edge measurements on IrO_x/RuO₂ thin films as well as mass-selected RuO_x and Ru nanoparticles. We observed shifts of the white line XAS peak toward higher energies with applied electrochemical potential. Apart from the case of the metallic Ru nanoparticles, the observed potential dependencies were purely core-level shifts caused by a change in oxidation state, which indicates no structural changes. These findings can be explained by different binding energies of oxygenated species on the surface of IrO_x and RuO_x. Simulated XAS spectra show that the average Ir oxidation state change is strongly affected by the coverage of atomic O. The observed shifts in oxidation state suggest that the surface has a high coverage of O at potentials just below the potential where oxygen evolution is exergonic in free energy. In conclusion, this observation is consistent with the notion that the metal–oxygen bond is stronger than ideal.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); European Union (EU); Villum Foundation; Danish Ministry of Higher Education and Science; Danish Council for Independent Research

Grant/Contract Number:: 9455; AC02-76SF00515; 607417

OSTI ID:: 1471512

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Vol. 122, Issue 2; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 52 works

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