Probing the Electronic Structure of Oxide Electrocatalysts and the Formation of Reaction Intermediates
Kelsey Stoerzinger a b
a Oregon State University, 105 SW 26th St, Corvallis, United States
b Pacific Northwest National Laboratory, Battelle Boulevard, 902, Richland, United States
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting 2021 (NFM21)
#SolFuel21. Solar Fuel: In-situ and operando characterization of electrified interfaces
Online, Spain, 2021 October 18th - 22nd
Organizers: Bastian Mei, Jan Philipp Hofmann and María Escudero-Escribano
Invited Speaker, Kelsey Stoerzinger, presentation 004
DOI: https://doi.org/10.29363/nanoge.nfm.2021.004
Publication date: 23rd September 2021

Perovskite oxides (ABO3) are highly active for the oxygen evolution reaction (OER). Activity is observed to correlate with changes in bulk electronic structure parameters, such as metal-oxygen covalency and transition metal oxidation state. We employ spectroscopic approaches to consider such descriptors at the surface of perovskite oxides in situ, as well as their implications on the formation of surface adsorbates proposed to act as reaction intermediates during the OER.

Many surface science techniques, such as X-ray photoelectron spectroscopy (XPS), collect information from inherently surface-sensitive low-energy processes, requiring operation in ultrahigh vacuum. This constraint is lifted for ambient pressure XPS, which can probe the surface in equilibrium with the gas phase at pressures up to ~a few Torr, or with thin liquid layers using a higher incident photon energy. This presentation will discuss the insights obtained with this technique regarding the electronic structure of oxide electrocatalysts in an oxidizing or humid environment, as well as the reaction intermediates of relevance to electrocatalysis.1 We will then extend the technique to probe electrocatalysts in operando,2 driving current through a thin layer of liquid electrolyte and employing a tender X-ray source.

This research used resources of the Advanced Light Source, a U.S. DOE Office of Science User Facility under contract no. DE-AC02-05CH11231.

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