Journal
ACS CATALYSIS
Volume 10, Issue 21, Pages 12696-12705Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c03464
Keywords
photocatalytic hydrogen production; single-atom catalysis; Pt/TiO2; operando spectroscopy; XAS
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Funding
- Region Auvergne-Rhone-Alpes (CMIRA 2016 project)
- Agence Nationale de la Recherche (UltraCat project) [ANR-17CE06-0008]
- Agence Nationale de la Recherche (LABEX iMUST) [ANR-10-LABX-0064/ANR11-IDEX-0007]
- French grand emprunt EquipEx (EcoX) [ANR-10-EQPX-27-01]
- CEA-CNRS CRG consortium
- INSU CNRS institute
- MICINN/FEDER [RTI2018-093996-B-C31, RTI2018-095498-J-I00]
- GC [2017 SGR 128]
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Photocatalytic hydrogen generation from water or oxygenates is foreseen as a sustainable energy production route. In spite of recent performance achievements through Pt particle downsizing, knowledge of the prototypical Pt/TiO2 photocatalyst operation mechanism, in particular the electronic state and the stability of the Pt phase under reaction conditions, remains limited. We have investigated atomically dispersed Pt/TiO2 catalysts by pre-/postreaction scanning transmission electron microscopy and operando X-ray absorption spectroscopy-mass spectrometry under gas-phase ethanol dehydrogenation conditions under ultraviolet-visible light irradiation. The catalysts were prepared by a simple impregnation method on two types of commercial titania. While the general effect of the reaction on initially fully oxidized (Pt-IV) single-atom catalysts (SACs) is Pt reduction and aggregation, this combined phenomenon can be inhibited in two manners. First, when it is supported on high-surface-area anatase, the Pt SAC retains an intermediate oxidation state, and its clustering is limited to Pt dimers and trimers. Second, with the same support, a mild reducing pretreatment generates, through the formation of Pt-Ti bonds, near-neutral and ultradispersed Pt species (from single atoms to nanometric clusters) with the highest stability and activity in photocatalytic hydrogen evolution.
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