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

Mesa, CA; Sachs, M; Pastor, E; Gauriot, N; Merryweather, AJ; Gomez-Gonzalez, MA; Ignatyev, K; Giménez, S; Rao, A; Durrant, JR; Pandya, R

Journal article

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

Abstract:: International audiencePhoto(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 (alpha-Fe2O3) photoelectrodes. We demonstrate that regions of alpha-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. Physicochemical heterogeneity poses a significant constraint in photocatalyst advancement. Here the authors introduce a multimodal optical microscopy platform to assess activity and defects concurrently in photoelectrocatalysts, revealing that disorder can unexpectedly enhance local photoelectrocatalytic performance in certain instances

Publication status:: Published

Peer review status:: Peer reviewed

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APA Style

Mesa, C. A., Sachs, M., Pastor, E., Gauriot, N., Merryweather, A. J., Gomez-Gonzalez, M. A., Ignatyev, K., Giménez, S., Rao, A., Durrant, J. R., & Pandya, R. (2024). Correlating activities and defects in (photo)electrocatalysts using in-situ multi-modal microscopic imaging. Nature Communications, 15(1), 3908–3908.

MLA Style

Mesa, CA, et al. “Correlating Activities and Defects in (Photo)Electrocatalysts Using in-Situ Multi-Modal Microscopic Imaging.” Nature Communications, vol. 15, no. 1, 2024, pp. 3908–08.

Chicago Style

Mesa, CA, M Sachs, E Pastor, et al. 2024. “Correlating Activities and Defects in (Photo)Electrocatalysts Using in-Situ Multi-Modal Microscopic Imaging.” Nature Communications 15 (1): 3908–.
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