Correlating activities and defects in (photo)electrocatalysts using in-situ multi-modal microscopic imaging

Camilo A. Mesa, Michael Sachs, Ernest Pastor, Nicolas Gauriot, Alice J. Merryweather, Miguel A. Gomez-Gonzalez, Konstantin Ignatyev, Sixto Giménez, Akshay Rao, James R. Durrant and Raj Pandya ()
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Camilo A. Mesa: Imperial College London
Michael Sachs: Imperial College London
Ernest Pastor: Institute of Advanced Materials (INAM) Universitat Jaume I
Nicolas Gauriot: J.J. Thomson Avenue
Alice J. Merryweather: J.J. Thomson Avenue
Miguel A. Gomez-Gonzalez: Harwell Science and Innovation Campus
Konstantin Ignatyev: Harwell Science and Innovation Campus
Sixto Giménez: Institute of Advanced Materials (INAM) Universitat Jaume I
Akshay Rao: J.J. Thomson Avenue
James R. Durrant: Imperial College London
Raj Pandya: J.J. Thomson Avenue

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Photo(electro)catalysts use sunlight to drive chemical reactions such as water splitting. A major factor limiting photocatalyst development is physicochemical heterogeneity which leads to spatially dependent reactivity. To link structure and function in such systems, simultaneous probing of the electrochemical environment at microscopic length scales and a broad range of timescales (ns to s) is required. Here, we address this challenge by developing and applying in-situ (optical) microscopies to map and correlate local electrochemical activity, with hole lifetimes, oxygen vacancy concentrations and photoelectrode crystal structure. Using this multi-modal approach, we study prototypical hematite (α-Fe2O3) photoelectrodes. We demonstrate that regions of α-Fe2O3, adjacent to microstructural cracks have a better photoelectrochemical response and reduced back electron recombination due to an optimal oxygen vacancy concentration, with the film thickness and extended light exposure also influencing local activity. Our work highlights the importance of microscopic mapping to understand activity, in even seemingly homogeneous photoelectrodes.

Date: 2024
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DOI: 10.1038/s41467-024-47870-9

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