Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 139, Issue 9, Pages 3513-3521Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b12850
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Funding
- Hong Kong RGC (TRS) [T23-407-13N]
- National Natural Science Foundation of China [21229101, 51472100]
- National Natural Science Funds for Distinguished Young Scholars [21425728]
- National Basic Research Program of China (973 Program) [2013CB632402]
- Excellent Doctorial Dissertation Cultivation Grant from Central China Normal University [2015YBZD018]
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Selective organic transformation under mild conditions constitutes a challenge in green chemistry, especially for alcohol oxidation, which typically requires environmentally unfriendly oxidants. Here, we report a new plasmonic catalyst of Au supported on BiOCl containing oxygen vacancies. It photocatalyzes selective benzyl alcohol oxidation with O-2 under visible light through synergistic action of plasmonic hot electrons and holes. Oxygen vacancies on BiOCl facilitate the trapping and transfer of plasmonic hot electrons to adsorbed O-2, producing center dot O-2(-) radicals, while plasmonic hot holes remaining on the Au surface mildly oxidize benzyl alcohol to corresponding carbon-centered radicals. The hypothesized concerted ring addition between these two radical species on the BiOCI surface highly favors the production of benzaldehyde along with an unexpected oxygen atom transfer from O-2 to the product. The results and understanding acquired in this study, based on the full utilization of hot charge carriers in a plasmonic metal deposited on a rationally designed support, will contribute to the development of more active and/or selective plasmonic catalysts for a wide variety of organic transformations.
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