Publication Type |
Journal Article |
Title |
Oxidovanadium(IV) acetylacetonate immobilized onto CMK-3 for heterogeneous epoxidation of geraniol |
Authors |
S. Dorbes Andre M. Pereira Marta A. Andrade D. Barros S. L. H. Rebelo Joao P. Araujo J. M. P. Silva Ana P. Carvalho C Freire |
Groups |
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Journal |
MICROPOROUS AND MESOPOROUS MATERIALS |
Year |
2012 |
Month |
September |
Volume |
160 |
Number |
|
Pages |
67-74 |
Abstract |
Heterogeneous catalysts based on oxidovanadium(IV) acetylacetonate ([VO(acac)(2)]) immobilized onto nanostructured ordered carbon material CMK-3 were prepared using two different strategies: (i) direct anchoring of the metal complex through the surface oxygen groups of the pristine support (CAT I) and (ii) immobilization via 3-aminopropyltriethoxysilane spacer previously grafted onto the support (CAT II). The metal complex immobilization through both methods was confirmed by X-ray photoelectron spectroscopy, elemental analysis. Fourier transform infrared spectroscopy and thermogravimetry. Xray diffraction (XRD) analysis provided insights on the materials rod-like structure and suggested the existence of some expansion of the CMK-3 network upon the complex immobilization. The new materials were tested as heterogeneous catalysts in the epoxidation of geraniol using tertbutyl hydroperoxide as oxidant leading to substrate conversions higher than 98\% after 2.5 h and 98-99\% selectivity for the 2,3-epoxygeraniol product. The improved catalytic performance observed for the new materials when compared to other heterogenized [VO(acac)(2)] based catalysts was attributed to an efficient mass transfer provided by the rod-like structure of CMK-3 supports. When APTES was used as the linker for complex immobilization (CAT II), negligible catalyst leaching and higher substrate conversions were observed when compared to CAT I upon recycling and reuse. Furthermore, XRD provided evidence for the preservation of the rod-like structure of the support upon the catalytic reactions. (C) 2012 Elsevier Inc. All rights reserved. |
DOI |
http://dx.doi.org/10.1016/j.micromeso.2012.03.041 |
ISBN |
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Publisher |
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Book Title |
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ISSN |
1387-1811 |
EISSN |
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Conference Name |
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Bibtex ID |
ISI:000307150700008 |
Observations |
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