Correlating activities and defects in (photo)electrocatalysts using in-situ multi-modal microscopic imaging
Mesa, Camilo A. (Imperial College London)
Sachs, Michael (Stanford University)
Pastor, Ernest (Université Rennes)
Gauriot, Nicolas (University of Cambridge)
Merryweather, Alice J. (University of Cambridge)
Gomez-Gonzalez, Miguel A. (Harwell Science and Innovation Campus)
Ignatyev, Konstantin (Harwell Science and Innovation Campus)
Giménez, Sixto (Universitat Jaume I)
Rao, Akshay (University of Cambridge)
Durrant, James R. (Swansea University. Department of Materials Science and Engineering)
Pandya, Raj (University of Warwick. Department of Chemistry)

Data:	2024
Resum:	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-FeO) photoelectrodes. We demonstrate that regions of α-FeO, 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.
Ajuts:	"la Caixa" Foundation 100010434 Agencia Estatal de Investigación PID2020-116093RB-C41
Nota:	Camilo A. Mesa present address: Institut Català de Nanociència i Nanotecnologia
Drets:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, fins i tot amb finalitats comercials, sempre i quan es reconegui l'autoria de l'obra original.
Llengua:	Anglès
Document:	Article ; recerca ; Versió publicada
Publicat a:	Nature communications, Vol. 15 (May 2024) , art. 3908, ISSN 2041-1723

DOI: 10.1038/s41467-024-47870-9
PMID: 38724495

12 p, 6.2 MB

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