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Alfred Larsson. Portrait.

Alfred Larsson

Postdoctoral fellow

Alfred Larsson. Portrait.

Operando Stability Studies of Ultrathin Single-Crystalline IrO2(110) Films under Acidic Oxygen Evolution Reaction Conditions

Author

  • Tim Weber
  • Vedran Vonk
  • Daniel Escalera-López
  • Giuseppe Abbondanza
  • Alfred Larsson
  • Volkmar Koller
  • Marcel J.S. Abb
  • Zoltan Hegedüs
  • Thomas Bäcker
  • Ulrich Lienert
  • Gary S. Harlow
  • Andreas Stierle
  • Serhiy Cherevko
  • Edvin Lundgren
  • Herbert Over

Summary, in English

The anodic corrosion behavior of 50 Å thick single-crystalline IrO2(110) films supported on slightly bulk-reduced TiO2(110) single crystals is studied during acidic water splitting by a unique combination of operando techniques, namely, synchrotron-based high-energy X-ray reflectivity (XRR) and surface X-ray diffraction (SXRD) together with highly sensitive inductively coupled plasma mass spectrometry (ICP-MS). Corrosion-induced structural and morphological changes of the IrO2(110) model electrode can be followed on the atomic scale by operando XRR and SXRD that are supplemented with ex situ scanning tunneling microscopy (STM) and X-ray photoelectron spectroscopy (XPS), whereas with ICP-MS, the corrosion rate can be quantified down to 1 pg·cm-2·s-1 with a time resolution on the second scale. The operando synchrotron-based X-ray scattering techniques are surprisingly sensitive to Ir corrosion of about 0.10 monolayer of IrO2(110) in ∼26 h, i.e., 0.4 pg·cm-2·s-1. The present study demonstrates that single-crystalline IrO2(110) films are much more stable than hitherto expected. Although the dissolution rate is very small, ICP-MS experiments reveal a significantly higher dissolution rate than the operando high-energy XRR/SXRD experiments. These differences in dissolution rate are suggested to be due to the different modi operandi encountered in ICP-MS (dynamic) and operando XRR/SXRD experiments (steady state), a fact that may need to be considered when hydrogen production is coupled to intermittent energy sources such as renewables.

Department/s

  • Synchrotron Radiation Research
  • NanoLund: Centre for Nanoscience

Publishing year

2021-10-15

Language

English

Pages

12651-12660

Publication/Series

ACS Catalysis

Volume

11

Issue

20

Document type

Journal article

Publisher

The American Chemical Society (ACS)

Topic

  • Physical Chemistry (including Surface- and Colloid Chemistry)

Keywords

  • electrocatalyst stability
  • HESXRD
  • IrO
  • operando studies
  • oxygen evolution reaction (OER)
  • SFC-ICP-MS
  • single-crystalline model electrodes
  • XRR

Status

Published

ISBN/ISSN/Other

  • ISSN: 2155-5435