Preparation of mesoporous titanosilicate molecular sieves with a cage type 3D porous structure for cyclohexene epoxidation

Chokkalingam Anand, Pavuluri Srinivasu, Gurudas P. Mane, Siddulu N. Talapaneni, Dattatray Dhawale, Mohammad A. Wahab, Subramaniam Vishnu Priya, Shaji Varghese, Yoshihiro Sugi, Ajayan Vinu

Research output: Contribution to journalArticle

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Abstract

We report on the preparation of mesoporous titanosilicate with a 3D porous structure and Fm3m symmetry using Pluronic F127 as structure directing agent and titanium isopropoxide as a titanium source. The amount of titanium in the silica framework of the materials is controlled by a simple adjustment of the molar water to hydrochloric acid (nH2O/nHCl) ratio. The materials with different nSi/nTi ratios are also prepared by varying the amount of titanium source in the synthesis gel at an optimized nH2O/nHCl of 463. The structural order, the textural parameters, morphology, the nature and co-ordination of Ti species, and the amount of Ti content in the samples are analyzed by various techniques including X-ray diffraction (XRD), N2 adsorption, high resolution scanning electron microscopy (HRSEM), UV-vis diffused reflectance spectroscopy (UV-vis DRS), and inductively coupled plasma emission spectroscopy (ICP), respectively. All the materials prepared with various nSi/nTi ratios exhibit well-ordered porous structure and possess high BET surface areas (673-941 m2 g-1) and large pore volumes (0.46-0.71 cm 3 g-1). The pore diameter of the samples also increases with increasing the Ti content in the samples. UV-vis results confirm that most of the Ti atoms are in the tetrahedral co-ordination. Finally, the materials are subjected to cyclohexene epoxidation using TBHP/H2O2 as oxidant and acetonitrile as solvent in order to investigate their catalytic activity. Ti-KIT-5 samples display a high catalytic activity with TBHP as oxidant and remain inactive when H2O2 was used. The amount of Ti plays a crucial role in controlling the catalytic activity of the samples. Of the catalysts studied, Ti-KIT-5(5) where the number in the parenthesis indicates the Si/Ti ratio shows the best activity, affording a high conversion to cyclohexene. Among the catalysts studied, Ti-KIT-5-5 exhibited better catalytic activity with respect to reaction time, reaction temperature, conversion and epoxide selectivity.

Original languageEnglish
Pages (from-to)159-166
Number of pages8
JournalMicroporous and Mesoporous Materials
Volume160
DOIs
Publication statusPublished - 15 Sep 2012
Externally publishedYes

Fingerprint

epoxidation
Epoxidation
Molecular sieves
absorbents
Catalyst activity
Titanium
catalytic activity
titanium
preparation
UCON 50-HB-5100
Inductively coupled plasma
Oxidants
Poloxamer
Catalysts
Hydrochloric Acid
High resolution electron microscopy
Epoxy Compounds
Emission spectroscopy
porosity
Hydrochloric acid

Keywords

  • Catalysis
  • Epoxidation
  • Mesoporous
  • Nanoporous
  • Zeolite

ASJC Scopus subject areas

  • Materials Science(all)
  • Mechanics of Materials
  • Chemistry(all)
  • Condensed Matter Physics

Cite this

Preparation of mesoporous titanosilicate molecular sieves with a cage type 3D porous structure for cyclohexene epoxidation. / Anand, Chokkalingam; Srinivasu, Pavuluri; Mane, Gurudas P.; Talapaneni, Siddulu N.; Dhawale, Dattatray; Wahab, Mohammad A.; Priya, Subramaniam Vishnu; Varghese, Shaji; Sugi, Yoshihiro; Vinu, Ajayan.

In: Microporous and Mesoporous Materials, Vol. 160, 15.09.2012, p. 159-166.

Research output: Contribution to journalArticle

Anand, Chokkalingam ; Srinivasu, Pavuluri ; Mane, Gurudas P. ; Talapaneni, Siddulu N. ; Dhawale, Dattatray ; Wahab, Mohammad A. ; Priya, Subramaniam Vishnu ; Varghese, Shaji ; Sugi, Yoshihiro ; Vinu, Ajayan. / Preparation of mesoporous titanosilicate molecular sieves with a cage type 3D porous structure for cyclohexene epoxidation. In: Microporous and Mesoporous Materials. 2012 ; Vol. 160. pp. 159-166.
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AU - Talapaneni, Siddulu N.

AU - Dhawale, Dattatray

AU - Wahab, Mohammad A.

AU - Priya, Subramaniam Vishnu

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N2 - We report on the preparation of mesoporous titanosilicate with a 3D porous structure and Fm3m symmetry using Pluronic F127 as structure directing agent and titanium isopropoxide as a titanium source. The amount of titanium in the silica framework of the materials is controlled by a simple adjustment of the molar water to hydrochloric acid (nH2O/nHCl) ratio. The materials with different nSi/nTi ratios are also prepared by varying the amount of titanium source in the synthesis gel at an optimized nH2O/nHCl of 463. The structural order, the textural parameters, morphology, the nature and co-ordination of Ti species, and the amount of Ti content in the samples are analyzed by various techniques including X-ray diffraction (XRD), N2 adsorption, high resolution scanning electron microscopy (HRSEM), UV-vis diffused reflectance spectroscopy (UV-vis DRS), and inductively coupled plasma emission spectroscopy (ICP), respectively. All the materials prepared with various nSi/nTi ratios exhibit well-ordered porous structure and possess high BET surface areas (673-941 m2 g-1) and large pore volumes (0.46-0.71 cm 3 g-1). The pore diameter of the samples also increases with increasing the Ti content in the samples. UV-vis results confirm that most of the Ti atoms are in the tetrahedral co-ordination. Finally, the materials are subjected to cyclohexene epoxidation using TBHP/H2O2 as oxidant and acetonitrile as solvent in order to investigate their catalytic activity. Ti-KIT-5 samples display a high catalytic activity with TBHP as oxidant and remain inactive when H2O2 was used. The amount of Ti plays a crucial role in controlling the catalytic activity of the samples. Of the catalysts studied, Ti-KIT-5(5) where the number in the parenthesis indicates the Si/Ti ratio shows the best activity, affording a high conversion to cyclohexene. Among the catalysts studied, Ti-KIT-5-5 exhibited better catalytic activity with respect to reaction time, reaction temperature, conversion and epoxide selectivity.

AB - We report on the preparation of mesoporous titanosilicate with a 3D porous structure and Fm3m symmetry using Pluronic F127 as structure directing agent and titanium isopropoxide as a titanium source. The amount of titanium in the silica framework of the materials is controlled by a simple adjustment of the molar water to hydrochloric acid (nH2O/nHCl) ratio. The materials with different nSi/nTi ratios are also prepared by varying the amount of titanium source in the synthesis gel at an optimized nH2O/nHCl of 463. The structural order, the textural parameters, morphology, the nature and co-ordination of Ti species, and the amount of Ti content in the samples are analyzed by various techniques including X-ray diffraction (XRD), N2 adsorption, high resolution scanning electron microscopy (HRSEM), UV-vis diffused reflectance spectroscopy (UV-vis DRS), and inductively coupled plasma emission spectroscopy (ICP), respectively. All the materials prepared with various nSi/nTi ratios exhibit well-ordered porous structure and possess high BET surface areas (673-941 m2 g-1) and large pore volumes (0.46-0.71 cm 3 g-1). The pore diameter of the samples also increases with increasing the Ti content in the samples. UV-vis results confirm that most of the Ti atoms are in the tetrahedral co-ordination. Finally, the materials are subjected to cyclohexene epoxidation using TBHP/H2O2 as oxidant and acetonitrile as solvent in order to investigate their catalytic activity. Ti-KIT-5 samples display a high catalytic activity with TBHP as oxidant and remain inactive when H2O2 was used. The amount of Ti plays a crucial role in controlling the catalytic activity of the samples. Of the catalysts studied, Ti-KIT-5(5) where the number in the parenthesis indicates the Si/Ti ratio shows the best activity, affording a high conversion to cyclohexene. Among the catalysts studied, Ti-KIT-5-5 exhibited better catalytic activity with respect to reaction time, reaction temperature, conversion and epoxide selectivity.

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