Selective Oxidation of Cyclopentene to Glutaraldehyde by H2O2 over the WO3/SiO2 Catalyst

doi:10.1006/jcat.2001.3319

Journal of Catalysis

Volume 203, Issue 1, 1 October 2001, Pages 75-81

https://doi.org/10.1006/jcat.2001.3319 Get rights and content

Abstract

A novel WO₃/SiO₂ was prepared by incipient wetness impregnation of the SiO₂ support synthesized by the xerogel method with the W-containing salt solution. The as-prepared WO₃/SiO₂ catalyst exhibited a very high yield of glutaraldehyde in the liquid phase cyclopentene oxidation by aqueous H₂O₂ and the leach of WO₃ species during the reaction could be neglected. As a heterogeneous catalyst, it seems more suitable for the industrial process than those homogeneous catalysts owing to its easy separation from reaction products, which makes it possible to use the catalyst repetitively. According to the XRD patterns, the WO₃ was present in amorphous state due to its high dispersion on the SiO₂ support. These amorphous WO₃ species were proved to be the active sites since the crystallization at high temperature caused a considerable deactivation. The lifetime of the catalyst was measured and its regeneration method was proposed. Effects of various factors on the catalytic behaviors, such as the WO₃ loading, the calcination temperature, and the reaction media, were also investigated and discussed based on the characterizations of BET, XRD, DSC, TEM, EXAFS, and Raman spectra.

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Citation Excerpt :
Notably, there is no distinction between the XRD results before and after the reaction (see Fig. S5), suggesting its structural stability during the oxidation with H2O2. This finding differs abruptly with those WO3-based heterogeneous materials reported earlier (WO3/SiO2 [40,41] and WO3/TiO2 [42]), the WO3 species of which aggregated obviously during the recycling test. However, the conversion of cyclohexene oxide gradually drops from 98 to 88% after the fifth cycle and the selectivity to adipaldehyde remains constant.
Carbon nitride nanosheets decorated with WO₃ nanorods (WO₃/g-C₃N₄) were fabricated via ultrasonic-assisted dispersion and conventional incipient wetness impregnation method. It is found that ultrasonic promoted the formation of g-C₃N₄ nanosheets efficiently. The promotion effect in the structural evolution and catalytic performance for the rod-like structure of WO₃ caused by g-C₃N₄ nanosheets were well studied. For the first time, the novel WO₃/g-C₃N₄ nanocomposites were used as efficient catalysts in the green process of dialdehydes from the selective oxidation of cycloalkene oxides using H₂O₂ as a clean oxidant, owing to the high dispersion of active sites and the strong interaction between cycloalkene oxides and the NH or NH₂ groups on the surface of g-C₃N₄ sheets. Here, C₃N₄ nanosheets are considered as the catalyst support and co-catalyst as well. The novel nanocomposites are very stable and can be reused for five times without obvious loss of catalytic activity.

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Regular ArticleSelective Oxidation of Cyclopentene to Glutaraldehyde by H2O2 over the WO3/SiO2 Catalyst

Abstract

Appl. Catal. A

Stud. Surf. Sci. Catal.

J. Catal.

J. Non-Cryst. Solids

J. Non-Cryst. Solids

J. Catal.

Appl. Catal. A

Appl. Catal.

Appl. Catal. A

Bull. Chem. Soc. Jpn.

Catal. Lett.

Catal. Lett.

J. Chem. Soc., Chem. Comm.

J. Org. Chem.

Chem. Lett.

Regular Article
Selective Oxidation of Cyclopentene to Glutaraldehyde by H₂O₂ over the WO₃/SiO₂ Catalyst