Novel Three Dimensional Cubic Fm3m Mesoporous Aluminosilicates with Tailored Cage Type Pore Structure and High Aluminum Content

Authors

  • Pavuluri Srinivasu,

    1. International Center for Materials Nanoarchitectonics World Premier International (WPI) Research Center National Institute for Materials Science 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan)
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  • Sher Alam,

    1. International Center for Materials Nanoarchitectonics World Premier International (WPI) Research Center National Institute for Materials Science 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan)
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  • Veerappan V. Balasubramanian,

    1. International Center for Materials Nanoarchitectonics World Premier International (WPI) Research Center National Institute for Materials Science 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan)
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  • Sivan Velmathi,

    1. International Center for Materials Nanoarchitectonics World Premier International (WPI) Research Center National Institute for Materials Science 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan)
    2. National Institute of Technology Tiruchirappalli – 620 015 (India)
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  • Dhanashri P. Sawant,

    1. International Center for Materials Nanoarchitectonics World Premier International (WPI) Research Center National Institute for Materials Science 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan)
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  • Winfred Böhlmann,

    1. Fakultät für Physik und Geowissenschaften, Universität Leipzig Linnestr. 5, 04103 Leipzig (Germany)
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  • Subhash P. Mirajkar,

    1. National Chemical Laboratory Pune – 411 008 (India)
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  • Katsuhiko Ariga,

    1. International Center for Materials Nanoarchitectonics World Premier International (WPI) Research Center National Institute for Materials Science 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan)
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  • Shivappa B. Halligudi,

    1. International Center for Materials Nanoarchitectonics World Premier International (WPI) Research Center National Institute for Materials Science 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan)
    2. National Chemical Laboratory Pune – 411 008 (India)
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  • Ajayan Vinu

    Corresponding author
    1. International Center for Materials Nanoarchitectonics World Premier International (WPI) Research Center National Institute for Materials Science 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan)
    • International Center for Materials Nanoarchitectonics World Premier International (WPI) Research Center National Institute for Materials Science 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan).
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  • This work was financially supported by Japan Science and technology under the Strategic Program for Building an Asian Science and Technology Community Scheme. Supporting Information is available online from Wiley InterScience or from the authors.

Abstract

Novel three dimensional cubic Fm3m mesoporous aluminosilicates (AlKIT-5) with very high structural order and unprecedented loadings of Al in the silica framework have been successfully prepared for the first time by using non ionic surfactant as a template in a highly acidic medium. The obtained materials have been unambiguously characterized in detail by several sophisticated techniques such as XRD, N2 adsorption, HRTEM, HRSEM, EDS, elemental mapping, 27Al MAS NMR, and NH3-TPD. We also demonstrate that the nature, and the amount of Al incorporation in the silica framework can easily be controlled by simply varying the nH2O/nHCl and the nSi/nAl ratios, and the Al sources in the synthesis gel. Among the Al sources examined, the Al isopropoxide (AiPr) is superior over other Al sources. 27Al MAS NMR results reveal that the amount of tetrahedral Al in the framework can be controlled by simply adjusting the nSi/nAl ratio in the synthesis gel, which increases with increasing the Al incorporation. One of the interesting findings in the work is the increase of the specific surface area, specific pore volume and the pore diameter of AlKIT-5 with increasing the Al incorporation in the silica framework (up to nSi/nAl ratio of 10) while retaining the well-ordered three dimensional cage type porous structure, and the mechanism for the unusual behavior has been discussed in detail. Finally, the acidity and the catalytic activity in the acetylation of veratrole of the AlKIT-5 catalysts have been studied and the results have been compared with the several zeolites catalysts. Among the catalysts examined, AlKIT-5(10) is found to be superior over the zeolites catalysts such as mordenite, zeolite H-Y, zeolite H-β, and ZSM-5.

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