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Issue 5, 2014
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Oxidative catalytic versatility of a trivacant polyoxotungstate incorporated into MIL-101(Cr)

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Abstract

The first immobilization of the trivacant Keggin-type polyoxometalate ([A-PW9O34]9−, PW9) to prepare a novel heterogeneous oxidative catalyst is here reported. PW9 was incorporated into the cavities of the chromium terephthalate metal–organic framework MIL-101(Cr). Characterization of the composite PW9@MIL-101 by powder X-ray diffraction, SEM-EDX, FT-IR, FT-Raman spectroscopy, N2 adsorption–desorption isotherms and 31P solid-state NMR confirmed that the structures of MIL-101 and the polyoxometalate anion were retained after immobilization. The composite PW9@MIL-101 revealed versatility as a heterogeneous catalyst to oxidize efficiently monoterpenes as well as to reach a complete desulfurization of a model oil containing the most refractory sulfur compounds in fuel, using in both systems acetonitrile as the solvent and H2O2 as the oxidant. Complete conversion of geraniol to 2,3-epoxygeraniol was achieved after the first 30 min at room temperature, while the total desulfurization of the model oil containing 1707 ppm of sulfur was attained after 2 h. In both systems the catalyst was recyclable for various cycles without a significant loss of activity. The stability and heterogeneity of the catalyst were confirmed by several techniques and by leaching tests.

Graphical abstract: Oxidative catalytic versatility of a trivacant polyoxotungstate incorporated into MIL-101(Cr)

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Publication details

The article was received on 28 Oct 2013, accepted on 10 Feb 2014 and first published on 11 Feb 2014


Article type: Paper
DOI: 10.1039/C3CY00853C
Catal. Sci. Technol., 2014,4, 1416-1425

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    Oxidative catalytic versatility of a trivacant polyoxotungstate incorporated into MIL-101(Cr)

    C. M. Granadeiro, A. D. S. Barbosa, S. Ribeiro, I. C. M. S. Santos, B. de Castro, L. Cunha-Silva and S. S. Balula, Catal. Sci. Technol., 2014, 4, 1416
    DOI: 10.1039/C3CY00853C

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