期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 304, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120964
关键词
Alkene difunctionalization; Nb2O5; Photocatalysis; Oxygen vacancy engineering; alpha-sulfonyloxy ketones
资金
- National Natural Science Foundation of China [22078350, 22002178]
- Natural Science Foundation of Shandong Province [ZR2020KB016]
- Dalian National Laboratory for Clean Energy (DNL) Cooperation Fund, CAS [DNL201904]
- Royal Society (UK) [NAF\R2\180695]
An oxygen vacancy-rich Nb2O5 semiconductor was reported as a bifunctional heterogeneous photocatalyst for the unprecedented synthesis of a-sulfonyloxy ketones via oxidative alkene difunctionalization under visible light irradiation. The catalyst demonstrated high stability and recyclability, enhancing reaction activity and product selectivity through accelerated electron-hole pair separation and O-2 activation.
Herein, we report an oxygen vacancy (OVs)-rich Nb2O5 semiconductor (OVs-N-Nb2O5) as a bifunctional heterogeneous photocatalyst for unprecedent synthesis of a-sulfonyloxy ketones via oxidative alkene difunctionalization with sodium sulfinate under visible light irradiation and ambient conditions. A broad set of aromatic and aliphatic alkenes was efficiently difunctionalized into diverse a-sulfonyloxy ketones in high yields with a good functional group tolerance. The catalyst OVs-N-Nb2O5 is highly stable and could be easily recovered for at least 6 successive recycles with maintaining photoactivity and selectivity. Experimental and theoretical investigations reveal that the presence of OVs not only accelerates the separation and transfer of photogenerated electron-hole pairs, but also promotes O-2 adsorption and activation to form long-lived superoxide anion radical (O-2 center dot), which greatly boosts the reaction and modulates the reaction pathways together with the intrinsic Lewis acid sites, thereby resulting in an improved reaction activity and excellent selectivity to the desired product.
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