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J Am Chem Soc. 2019 Mar 6;141(9):3797-3801. doi: 10.1021/jacs.8b13051. Epub 2019 Feb 21.

Enhanced Superoxide Generation on Defective Surfaces for Selective Photooxidation.

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Hefei National Laboratory for Physical Science at the Microscale, CAS Center for Excellence in Nanoscience, iChEM , University of Science and Technology of China , Hefei 230026 , People's Republic of China.
College of Chemistry, Chemical Engineering and Materials Science , Shandong Normal University , Jinan 250014 , People's Republic of China.
National Synchrotron Radiation Laboratory , University of Science and Technology of China , Hefei 230029 , People's Republic of China.


Photocatalytic selective oxidation reactions hold great promise for the design of high-value-added organic intermediates, but many of these reactions suffer from low conversion efficiency and selectivity due to uncontrollable oxidation processes. In view of using photogenerated reactive oxygen species as the key oxidant in a selective oxidation reaction, we propose that a highly selective oxidation reaction can be achieved by modulating the corresponding photocatalytic molecular oxygen (O2) activation processes. Using cubic indium sulfide (β-In2S3) nanosheets as a model system, we show that the charge carriers involved in O2 activation can be optimized with the introduction of surface S vacancies. Benefiting from the enhanced charge separation and transfer processes, the In2S3 nanosheets with S vacancies could simultaneously activate O2 into superoxide radicals via electron transfer under visible-light irradiation to display outstanding activity for the selective oxidation of alcohols to aldehydes with high conversion and selectivity. This study offers a new strategy to optimize photocatalytic selective oxidation reactions.


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