Oxidative catalytic versatility of a trivacant polyoxotungstate incorporated into MIL-101(Cr)
authors Granadeiro, CM; Barbosa, ADS; Ribeiro, S; Santos, ICMS; de Castro, B; Cunha-Silva, L; Balula, SS
nationality International
journal CATALYSIS SCIENCE & TECHNOLOGY
keywords LIQUID-PHASE OXIDATION; HETEROGENEOUS CATALYSTS; KEGGIN-TYPE; COMPLEX HETEROPOLYTUNGSTATES; DEEP DESULFURIZATION; LIMONENE EPOXIDATION; PHOSPHOTUNGSTIC ACID; POLYOXOMETALATE; H2O2; PERFORMANCE
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, N-2 adsorption-desorption isotherms and P-31 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.
publisher ROYAL SOC CHEMISTRY
issn 2044-4753
year published 2014
volume 4
issue 5
beginning page 1416
ending page 1425
digital object identifier (doi) 10.1039/c3cy00853c
web of science category Chemistry, Physical
subject category Chemistry
unique article identifier WOS:000335893200026
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journal impact factor 5.365
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