期刊
JOURNAL OF CATALYSIS
卷 349, 期 -, 页码 156-162出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2017.01.014
关键词
Tandem reactions; Benzothiazoles; Fe-based MOFs; Transient absorption spectroscopy; Light-induced organic transformations
资金
- 973 Program [2014CB239303]
- NSFC [21273035]
- National Key Technologies R&D Program of China [2014BAC13B03]
- Independent Research Project of the State Key Laboratory of Photocatalysis on Energy and Environment [2014A03]
- Spanish Ministry of Economy and Competitiveness (Severo Ochoa) [CTQ2015-69153-CO2-1-R]
- Award Program for Minjiang Scholar Professorship
MIL-100(Fe) and MIL-68(Fe), two Fe-based MOFs, were found to be active for oxidative condensation between alcohols and o-aminothiophenols to form 2-substituted benzothiazoles under visible light irradiation using oxygen (02) as oxidant. This reaction can be applied to a wide range of substrates with medium to high yield. Controlled experiments and ESR results revealed a superoxide radical (O-2(center dot-))-mediated pathway, which is derived from the reduction of O-2 by photogenerated Fe2+ on Fe-O clusters. The whole multistep reaction is limited by the step of the photo-oxidation of alcohols to aldehydes. MIL-100(Fe) showed catalytic performance superior to that of MIL-68(Fe) because its higher concentration of long-lived (mu s time scale) positive holes can be photogenerated over MIL-100(Fe), in contrast to MIL-68(Fe). This study not only provides an economical, sustainable, and thus green process for the production of 2-substituted benzothiazoles, but also illustrates the potential of using transient absorption spectroscopy as an important tool for understanding the photophysics of MOFs, which are believed to show great potential as multifunctional catalysts for light-induced organic transformations. (C) 2017 Elsevier Inc. All rights reserved.
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