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Templated non-hydrolytic synthesis of mesoporous zirconium silicates and their catalytic properties

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Abstract

A novel non-hydrolytic sol–gel (NHSG) synthesis of mesoporous zirconium silicate xerogels is presented. The condensation between silicon acetate, Si(OAc)4, and Zr(NEt2)4 resulting in acetamide elimination leads to homogeneous zirconium silicate xerogels containing Si–O–Zr linkages. The addition of Pluronic P123 template provides stiff gels that are after template removal by calcination at 500 °C in air converted to stable mesoporous xerogels with wormhole-type pores, high surface area over 500 m2 g−1, and tetrahedrally coordinated Zr atoms in the framework. The composition and morphology of the xerogels, volatile reaction byproducts, and thermal transformations were followed by elemental analysis, IR spectroscopy, thermal analysis TG-DSC, nitrogen adsorption, 13C and 29Si solid-state NMR spectroscopy, DRUV–Vis spectroscopy, SAXS, and HT powder XRD. These potential catalysts were tested for the Meerwein–Ponndorf–Verley reduction of 4-tert-butylcyclohexanone and for aminolysis of styrene oxide with aniline. Resulting reaction systems display good activity and selectivity.

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Acknowledgements

Authors thank the project CEITEC—Central European Institute of Technology CZ.1.05/1.1.00/02.0068 and KONTAKT II LH11028 for the financial assistance. A.S. thanks the Brno City Municipality for Brno Ph.D. Talent Scholarship. Authors thank L. Simonikova and Dr. K. Novotny for ICP-OES analyses, L. Krauskova for DRUV-Vis spectra measurements, Dr. M. Klementova for TEM analyses, and Dr. T. Klumpler (Single Crystal X-ray Diffraction Core Facility CEITEC) for the SAXS 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. CEITEC MU, Masaryk University, Kamenice 735/5, 62500, Brno, Czech Republic

    David Skoda, Ales Styskalik & Jiri Pinkas

  3. Institute of Inorganic Chemistry, ASCR, 25068, Rez, Czech Republic

    Petr Bezdicka

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  1. David Skoda
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Correspondence to Jiri Pinkas.

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Skoda, D., Styskalik, A., Moravec, Z. et al. Templated non-hydrolytic synthesis of mesoporous zirconium silicates and their catalytic properties. J Mater Sci 50, 3371–3382 (2015). https://doi.org/10.1007/s10853-015-8888-1

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