Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 53, Issue 12, Pages 3205-3209Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201309660
Keywords
heterogeneous catalysis; oxygen activation; palladium; plasmonics; titania
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Funding
- 973 Program [2014CB848900, 2011CB921400, 2012CB922001, 2010CB923300]
- NSFC [21101145, 21121003, 51172223, 91127042, 21173205]
- Recruitment Program of Global Experts
- CAS Hundred Talent Program
- CAS Strategic Priority Research Program B [XDB01020000]
- Fundamental Research Funds for the Central Universities [WK2060190025, WK2060140014]
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The charge state of the Pd surface is a critical parameter in terms of the ability of Pd nanocrystals to activate O-2 to generate a species that behaves like singlet O-2 both chemically and physically. Motivated by this finding, we designed a metal-semiconductor hybrid system in which Pd nanocrystals enclosed by {100} facets are deposited on TiO2 supports. Driven by the Schottky junction, the TiO2 supports can provide electrons for metal catalysts under illumination by appropriate light. Further examination by ultrafast spectroscopy revealed that the plasmonics of Pd may force a large number of electrons to undergo reverse migration from Pd to the conduction band of TiO2 under strong illumination, thus lowering the electron density of the Pd surface as a side effect. We were therefore able to rationally tailor the charge state of the metal surface and thus modulate the function of Pd nanocrystals in O-2 activation and organic oxidation reactions by simply altering the intensity of light shed on Pd-TiO2 hybrid structures.
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