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- Title
Correlating activities and defects in (photo)electrocatalysts using in-situ multi-modal microscopic imaging.
- Authors
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
- 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. 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.
- Subjects
SCANNING electrochemical microscopy; MICROSCOPY; CHEMICAL reactions; CRYSTAL structure; HEMATITE; ELECTROCATALYSTS; PHOTOGRAPHS
- Publication
Nature Communications, 2024, Vol 15, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-024-47870-9