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Edvin Lundgren. Portrait.

Edvin Lundgren

Professor

Edvin Lundgren. Portrait.

Probing the electrode-liquid interface using operando total-reflection X-ray absorption spectroscopy

Author

  • A. Grespi
  • A. Larsson
  • G. Abbondanza
  • J. Eidhagen
  • D. Gajdek
  • J. Manidi
  • A. Tayal
  • J. Pan
  • L. R. Merte
  • E. Lundgren

Summary, in English

Traditional methods to study electrochemical (EC) processes, although successful, are based on current/voltage measurements, providing information about performances rather than offering a direct observation of chemical and structural changes occurring at the electrode surface. These processes are localized at the electrode-electrolyte interface, the structure of which is the main determinant of their behavior, but most surface sensitive experimental techniques are limited to ex situ conditions, owing to the need for an ultra-high vacuum environment. In this contribution, we report operando X-ray absorption spectroscopy in total external reflection geometry (Refle-XAFS) at P64 beamline (DESY, Hamburg), using a simple and versatile EC flow cell designed for multimodal surface sensitive studies with hard X-ray scattering and spectroscopy techniques. We show that the Refle-XAFS method can be used to study chemical surface changes of industrial alloys and model electrodes in harsh electrochemical environments, without being limited to thin film samples. The surface passive film development and breakdown of a corrosion-resistant Ni-Cr-Mo alloy and the electro-oxidation of polycrystalline gold (poly-Au), relevant for fundamental studies on water electrolysis, were investigated. Despite the strong attenuation of the beam by the electrolyte and the PEEK walls of the EC cell, nanoscale surface oxide films were detected using beam energies down to 8 keV. The passivity breakdown region of Ni alloy 59 in 1 M NaCl at pH 7 and pH 12 was identified, showing differences in the composition of the surface oxides during anodic polarization. The electro-oxidation of poly-Au in 0.05 M H2SO4 was observed, showing a progression from two-dimensional Au1+/3+ to three-dimensional thick Au3+ surface oxide/hydroxide during OER.

Department/s

  • Synchrotron Radiation Research
  • LU Profile Area: Light and Materials
  • NanoLund: Centre for Nanoscience
  • LTH Profile Area: Nanoscience and Semiconductor Technology
  • LTH Profile Area: Photon Science and Technology

Publishing year

2024

Language

English

Publication/Series

Surface Science

Volume

748

Document type

Journal article

Publisher

Elsevier

Topic

  • Materials Chemistry

Keywords

  • Electrochemical refleXAFS
  • Operando X-ray spectroscopy
  • Oxygen evolution reaction
  • Passivity breakdown
  • Solid/liquid interface
  • Total reflection X-ray absorption spectroscopy

Status

Published

ISBN/ISSN/Other

  • ISSN: 0039-6028