4.8 Article

A mild and effective photo-catalytic protocol for triggering inert nitrous oxide to participate in oxidative dehydrogenation of alcohols under visible light illumination

期刊

APPLIED CATALYSIS B-ENVIRONMENTAL
卷 318, 期 -, 页码 -

出版社

ELSEVIER
DOI: 10.1016/j.apcatb.2022.121861

关键词

Nitrous oxide activation; Oxygen-transfer Decatungstate photo-catalysis; Visible light; Alcohol oxidation dehydrogenation

资金

  1. National Natural Science Fund of China [22008062, 22005117, 21676079, 21546010]
  2. Specialized Research Fund [11JJ6008]
  3. Natural Science Fund of Hunan Province [10JJ2007, 14K059, 11K044]
  4. Innovation Platform Open Fund of Hunan College
  5. Hunan 2011 Collaborative Innovation Center of Chemical Engineering Technology with Environmental Benignity and Effective Resource Utilization, Program for Science and Technology Innovative Research Team in Higher Educational Institutions of Hunan Provinc
  6. [20124306110005]
  7. [2018JJ3335]
  8. [14JJ2148]

向作者/读者索取更多资源

The development of a mild and efficient activation protocol for N2O-based selective oxidation has significant academic and applied values. This study reveals that decatungstate (DT) anion and its hybrids with metal ions are active for the N2O-involved oxidative dehydrogenation reactions. The best catalyst achieves high cyclohexanone yield and is efficient for the N2O-involved ODH reactions of various alcohols.
The development of a mild and efficient activation protocol for the nitrous oxide (N2O)-based selective oxidation has very important academic and applied values in the harmless treatment and high value-added utilization of N2O. This paper discloses that decatungstate (DT) anion and especially its hybrids with metal ions (1%M-DTs) are active for the N2O-involved oxidative dehydrogenation (ODH) of cyclohexanol in MeCN under visible light illumination. The best 1%Cu-DT achieves ca. 46.3% cyclohexanone yield and its turnover frequency (TOF) is up to 6.56 h(-1) at high substrate concentration (1 M). Also, 1%Cu-DT is efficient for the N2O-involved ODH reactions of aliphatic and especially aromatic primary/secondary alcohols. UV-vis spectra, the isotope tracing tests of (H2O)-O-18 and DFT calculations support that the double-reduced H2DT species in situ-generated during the photo -reaction may turn into its oxygen-vacant state through dehydration, which the latter plays a crucial role in the oxygen transfer from N2O to it.

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