4.8 Article

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

期刊

ACS CATALYSIS
卷 11, 期 20, 页码 12651-12660

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c03599

关键词

IrO2; single-crystalline model electrodes; operando studies; oxygen evolution reaction (OER); electrocatalyst stability; HESXRD; XRR; SFC-ICP-MS

资金

  1. BMBF [05 K2016-HEXCHEM]
  2. Swedish Research Council [201605234]
  3. DFG [SPP2080: Ov21-16, CH1763/3-1, CH1763/4-1]

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The anodic corrosion behavior of 50 angstrom thick single-crystalline IrO2 (110) films supported on slightly bulk-reduced TiO2 (110) single crystals during acidic water splitting was studied using a combination of synchrotron-based high-energy X-ray reflectivity (XRR) and surface X-ray diffraction (SXRD) with inductively coupled plasma mass spectrometry (ICP-MS). The operando synchrotron-based X-ray scattering techniques proved to be surprisingly sensitive to Ir corrosion, revealing differences in dissolution rate compared to ICP-MS experiments, which may have implications for hydrogen production coupled to intermittent energy sources.
The anodic corrosion behavior of 50 angstrom 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 similar to 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.

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