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On the chemical state of Co oxide electrocatalysts during alkaline water splitting.

  • Author(s): Friebel, Daniel;
  • Bajdich, Michal;
  • Yeo, Boon Siang;
  • Louie, Mary W;
  • Miller, Daniel J;
  • Sanchez Casalongue, Hernan;
  • Mbuga, Felix;
  • Weng, Tsu-Chien;
  • Nordlund, Dennis;
  • Sokaras, Dimosthenis;
  • Alonso-Mori, Roberto;
  • Bell, Alexis T;
  • Nilsson, Anders
  • et al.
Abstract

Resonant inelastic X-ray scattering and high-resolution X-ray absorption spectroscopy were used to identify the chemical state of a Co electrocatalyst in situ during the oxygen evolution reaction. After anodic electrodeposition onto Au(111) from a Co(2+)-containing electrolyte, the chemical environment of Co can be identified to be almost identical to CoOOH. With increasing potentials, a subtle increase of the Co oxidation state is observed, indicating a non-stoichiometric composition of the working OER catalyst containing a small fraction of Co(4+) sites. In order to confirm this interpretation, we used density functional theory with a Hubbard-U correction approach to compute X-ray absorption spectra of model compounds, which agree well with the experimental spectra. In situ monitoring of catalyst local structure and bonding is essential in the development of structure-activity relationships that can guide the discovery of efficient and earth abundant water splitting catalysts.

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