Journal
ACS CATALYSIS
Volume 10, Issue 22, Pages 13650-13658Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c04098
Keywords
time-resolved photoelectron spectroscopy; ultrafast; photocatalysis; photochemistry; oxygen activation; TiO2; metal oxide; free electron laser
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Funding
- Initiative and Networking Funds of the Helmholtz Association [ExNet-0002]
- DFG within the excellence cluster Center for Ultrafast Imaging (CUI)
- European Union's Horizon 2020 research and innovation program under Marie Sklodowska-Curie grant [753874]
- European Research Council [ERC-2015-AdG-694097]
- NSAF [U1930402]
- Grupos Consolidados [IT1249-19]
- [SFB925]
- Marie Curie Actions (MSCA) [753874] Funding Source: Marie Curie Actions (MSCA)
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Femtosecond X-ray laser pulses synchronized with an optical laser were employed to investigate the reaction dynamics of the photooxidation of CO on the anatase TiO2 (101) surface in real time. Our time-resolved soft X-ray photoemission spectroscopy results provide evidence of ultrafast timescales and, coupled with theoretical calculations, clarify the mechanism of oxygen activation that is crucial to unraveling the underlying processes for a range of photocatalytic reactions relevant to air purification and self-cleaning surfaces. The reaction takes place between 1.2 and 2.8 (+/- 0.2) ps after irradiation with an ultrashort laser pulse leading to the formation of CO2, prior to which no intermediate species were observed on a picosecond time scale. Our theoretical calculations predict that the presence of intragap unoccupied O-2 levels leads to the formation of a charge-transfer complex. This allows the reaction to be initiated following laser illumination at a photon energy of 1.6 eV (770 nm), taking place via a proposed mechanism involving the direct transfer of electrons from TiO2 to physisorbed O-2.
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