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Probing the Role of Atomic Defects in Photocatalytic Systems through Photoinduced Enhanced Raman Scattering

Glass, D; Quesada-Cabrera, R; Bardey, S; Promdet, P; Sapienza, R; Keller, V; Maier, SA; ... Cortés, E; + view all (2021) Probing the Role of Atomic Defects in Photocatalytic Systems through Photoinduced Enhanced Raman Scattering. ACS Energy Letters , 6 pp. 4273-4281. 10.1021/acsenergylett.1c01772. (In press). Green open access

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Abstract

Even in ultralow quantities, oxygen vacancies (VO) drastically impact key properties of metal oxide semiconductors, such as charge transport, surface adsorption, and reactivity, playing central roles in functional materials performance. Current methods used to investigate VO often rely on specialized instrumentation under far from ideal reaction conditions. Hence, the influence of VO generated in situ during catalytic processes has yet to be probed. In this work, we assess in situ extrinsic surface VO formation and lifetime under photocatalytic conditions which we compare to photocatalytic performance. We show for the first time that lifetimes of in situ generated atomic VO play more significant roles in catalysis than their concentration, with strong correlations between longer-lived VO and higher photocatalytic activity. Our results indicate that enhanced photocatalytic efficiency correlates with goldilocks VO concentrations, where VO densities must be just right to encourage carrier transport while avoiding charge carrier trapping.

Type: Article
Title: Probing the Role of Atomic Defects in Photocatalytic Systems through Photoinduced Enhanced Raman Scattering
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acsenergylett.1c01772
Publisher version: https://doi.org/10.1021/acsenergylett.1c01772
Language: English
Additional information: This is an Open Access article published under a Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0) Licence (https://creativecommons.org/licenses/by-nc-nd/4.0/).
Keywords: Photocatalysis, Oxides, Raman spectroscopy, Catalytic activity, Defects
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery-pp.ucl.ac.uk/id/eprint/10138998
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