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

Mesa, Camilo A.; Sachs, Michael; Pastor, Ernest; Gauriot, Nicolas; Merryweather, Alice J.; Gomez-Gonzalez, Miguel A.; Ignatyev, Konstantin; Giménez, Sixto; Rao, Akshay; Durrant, James R.; Pandya, Raj

doi:10.1038/s41467-024-47870-9

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

Journal Article · 08 May 2024 · Nature Communications

DOI: https://doi.org/10.1038/s41467-024-47870-9 · OSTI ID:2405175

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^[4]; Gomez-Gonzalez, Miguel A. ^[5];

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Barcelona Institute of Science and Technology (BIST) (Spain); Consejo Superior de Investigaciones Cientificas (CSIC), Barcelona (Spain); Imperial College, London (United Kingdom); Universitat Jaume I, Castelló (Spain); BioGRID, Bogotá (Colombia); SLAC
Imperial College, London (United Kingdom); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE)
Universitat Jaume I, Castelló (Spain); Centre National de la Recherche Scientifique (CNRS) (France); Univ. of Rennes (France)
Univ. of Cambridge (United Kingdom). Cavendish Lab.
Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Diamond Light Source, Ltd.
Universitat Jaume I, Castelló (Spain)
Imperial College, London (United Kingdom); Swansea University (United Kingdom)
Univ. of Cambridge (United Kingdom). Cavendish Lab.; Sorbonne Univ., Paris (France); Centre National de la Recherche Scientifique (CNRS) (France); Univ. of Warwick, Coventry (United Kingdom)

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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 2405175

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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