Surface hydrogen bonds assisted meso-porous WO^sub 3^ photocatalysts for high selective oxidation of benzylalcohol to benzylaldehyde

Selective photo-oxidation of alcohols displays high potential in solar energy conversion and reducing environmental pollution, yet its selectivity and conversion in aqueous phase is still far from expectation. Here we report a fluorinated meso-porous WO3 photocatalyst (Fm-WO3) exhibits significant s...

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Bibliographic Details
Published in:Applied catalysis. B, Environmental Environmental, 2017-11, Vol.217, p.108
Main Authors: Su, Yang, Han, Zhongkang, Zhang, Ling, Wang, Wenzhong, Duan, Manyi, Li, Xiaoman, Zheng, Yali, Wang, Yanggang, Lei, Xiaoling
Format: Article
Language:English
Subjects:
Alcohols
Benzaldehyde
Conversion
Energy conversion
First principles
Fluorination
Hydrogen
Hydrogen bonding
Hydrogen bonds
Hydroxyl groups
Irradiation
Oxidation
Photocatalysis
Photocatalysts
Photooxidation
Pollution control
Radiation
Reaction mechanisms
Selectivity
Solar energy
Solar energy conversion
Studies
Synergistic effect
Tungsten oxides
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Summary:Selective photo-oxidation of alcohols displays high potential in solar energy conversion and reducing environmental pollution, yet its selectivity and conversion in aqueous phase is still far from expectation. Here we report a fluorinated meso-porous WO3 photocatalyst (Fm-WO3) exhibits significant selectivity (-99%) and conversion (-57%) in transforming benzylalcohol to benzaldehyde in the aqueous solution under the simulated sunlight irradiation. This high reactivity is attributed to the synergistic effect between meso-porous nanostructure and surface fluorination, where meso-porous structure supplies active sites to promote the multi-electron reduction of O2 and the surface fluorination assists the transmission of photogenerated holes. First-principles calculations further suggest that surface fluorination brings in an unoccupied impurity state in the band structure of WO3, which exhibits a strong correlation with the hydroxyl group of benzyalcohol and thus bridges the interaction between surfaces and alcohols. Meanwhile, the fluorination promotes the generation of OH by holes which can be considered as another way to oxidize benzyatcohol. Finally, a generalized reaction mechanism for selective photo-oxidation has been proposed.
ISSN:0926-3373
1873-3883