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Mesoporous titanosilicates by templated non-hydrolytic sol–gel reactions

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Abstract

A novel templated non-hydrolytic sol–gel synthesis of titanosilicate xerogels is reported. Acetamide elimination from silicon acetate and titanium diethylamide allows obtaining titanosilicates with a high content of Si–O–Ti bonds but low surface areas. These xerogels lose porosity on calcination. However, with addition of Pluronic P123 as a structure-directing agent, we synthesized mesoporous titanosilicate materials with large surface areas (up to 615 m2 g−1) and well dispersed tetrahedral Ti that are stable at temperatures up to 500 °C. These potential catalysts were characterized by variety of physico-chemical methods (IR, GC–MS, XRD, 29Si and 13C CPMAS NMR, DRUV-Vis, and N2 porosimetry) and tested in cyclohexene epoxidation with cumyl hydroperoxide in toluene. They display catalytic activity with the 100 % selectivity to cyclohexene oxide and high catalytic yields up to 96 % which is comparable to previously reported titanosilicate catalysts.

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Acknowledgments

Authors thank the project CEITEC–Central European Institute of Technology CZ.1.05/1.1.00/02.0068, KONTAKT II LH11028 and GACR P207/11/0555 for the financial assistance. J.P. thanks to the Fulbright Foundation for a scholarship. A.S. thanks to the Brno City Municipality for Brno Ph.D. Talent Scholarship. Authors thank to L. Simonikova and Dr. K. Novotny for ICP-OES analyses, L. Elenchin and L. Krauskova for DRUV-Vis spectra, Dr. M. Klementova for TEM analyses and Dr. J. Literak for GC-FID measurements.

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Authors and Affiliations

  1. Department of Chemistry, Masaryk University, Kotlarska 2, 61137, Brno, Czech Republic

    David Skoda, Ales Styskalik, Zdenek Moravec & Jiri Pinkas

  2. Masaryk University, CEITEC MU, Kamenice 5, 62500, Brno, Czech Republic

    David Skoda, Ales Styskalik & Jiri Pinkas

  3. Institute of Inorganic Chemistry of the ASCR, v.v.i., 25068, Husinec-Rez, Czech Republic

    Petr Bezdicka

  4. Department of Chemistry, University of Tennessee, Knoxville, TN, 37996-1600, USA

    Craig E. Barnes

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  1. David Skoda
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  2. Ales Styskalik
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Correspondence to Jiri Pinkas.

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Dedicated to Professor Malcolm H. Chisholm on the occasion of his 70th birthday.

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Skoda, D., Styskalik, A., Moravec, Z. et al. Mesoporous titanosilicates by templated non-hydrolytic sol–gel reactions. J Sol-Gel Sci Technol 74, 810–822 (2015). https://doi.org/10.1007/s10971-015-3666-8

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