TY - JOUR
T1 - Probing the Role of Atomic Defects in Photocatalytic Systems through Photoinduced Enhanced Raman Scattering
AU - Glass, Daniel
AU - Quesada-Cabrera, Raul
AU - Bardey, Steven
AU - Promdet, Premrudee
AU - Sapienza, Riccardo
AU - Keller, Valérie
AU - Maier, Stefan A.
AU - Caps, Valérie
AU - Parkin, Ivan P.
AU - Cortés, Emiliano
N1 - Funding Information:
D.G. acknowledges funding from the UK MOD for the Ph.D. under contract DSTLX-1000116630. S.A.M. and E.C. acknowledge funding and support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany’s Excellence Strategy – EXC 2089/1-390776260, the Bavarian program Solar Energies Go Hybrid (SolTech), and the Center for NanoScience (CeNS). S.A.M. additionally acknowledges the Lee-Lucas Chair in Physics. E.C. acknowledges the European Commission through the ERC Starting Grant CATALIGHT (802989). P.P acknowledges funding from The Development and Promotion of Science and Technology Talents Project. S.B., V.K., and V.C. acknowledge funding and support from IFP Energies Nouvelles. I.P.P acknowledges support from the EPSRC Centre of Doctoral Training in Molecular Modelling and Material Science under grant EP/L015862/1. R.Q.C. would like to thank the Beatriz Galindo Program, Ministerio de Educación y Formación Profesional, Spain. The authors also acknowledge support from EPSRC - UK under the grant EP/M013812/1, Reactive Plasmonics.
Publisher Copyright:
©
PY - 2021/12/10
Y1 - 2021/12/10
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85119443134&partnerID=8YFLogxK
U2 - 10.1021/acsenergylett.1c01772
DO - 10.1021/acsenergylett.1c01772
M3 - Article
AN - SCOPUS:85119443134
SN - 2380-8195
VL - 6
SP - 4273
EP - 4281
JO - ACS Energy Letters
JF - ACS Energy Letters
IS - 12
ER -
