Synthesis and characterisation of titanosilicates used as catalysts for the epoxidation of cyclohexene

  • Amber Welch
  • Nguyen Khanh Dieu Hong
  • Sankar Gopinathan

Tóm tắt

In this work the synthesis of TS-1 from a titanosilicate cogel precursor is reported. The synthesis parameters were altered to optimise both the cogel and resultant framework material. The titanosilicate materials were characterised using a range of techniques including EDX analysis, XRD, 29Si NMR, IR, UV-vis and SEM. Those materials which demonstrated the most catalytic potential were used as catalysts for the epoxidation of cyclohexene reaction, in which the use of aqueous H2O2 and a urea-H2O2 adduct were compared. It was shown that the cogel precursors themselves exhibited some catalytic reactivity and selectivity for all of the catalysis reactions exploited. However the TS-1 materials were more catalytically active, which highlighted the need of the ordered framework for the most effective catalysis. The TS-1 materials prepared from the cogel precursors exhibited similar catalytic ability to those analogous standard materials prepared via conventional processes. Thus TS-1 preparation by the cogel route was shown to be a viable alternative preparation method to the conventional process.

Các tài liệu tham khảo

M.Taramasso, G.Perego, B.Notari. Preparation of porous crystalline synthetic material comprised of silicon and titanium oxides. U.S. Patent No.4 410 501. 1983; 4: p. 410 - 501.

U.Romano, A.Esposito, F.Maspero, C.Neri, M.G.Clerici. Selective oxidation with Ti-Silicalite. Studies of Surface Science and Catalysis. 1990; 55: p. 33 - 41.

K.T.Jung, Y.G.Shul. A new method for the synthesis of TS-1 monolithic zeolite. Microporous and Mesoporous Materials. 1998; 21(4 - 6): p. 281 - 288.

D.P.Serrano, M.A.Uguina, G.Ovejero, R.V.Grieken, M.Camacho. Synthesis of TS-1 by wetness impregnation of amorphous SiO2-TiO2 solids prepared by the sol-gel method. Microporous Materials. 1995; 4: p. 273 - 282.

P.Ratnasamy, D.Srinivas, H.Knözinger. Active sites and reactive intermediates in titanium silicate molecular sieves. Advances in Catalysis. 2004; 48: p. 1 - 169.

María A.Uguina, Gabriel Ovejero, Rafael Van Grieken, David P.Serrano, Marta Camacho. Synthesis of titanium silicalite-1 from an SiO2-TiO2 cogel using a wetness impregnation method. Journal of the Chemical Society, Chemical Communications. 1994; 1: p. 27 - 28.

D.P.Serrano, M.A.Uguina, G.Ovejero, R.V.Grieken, M.Camacho. Evidence of solid-solid transformations during the TS-1 crystallization from amorphous wetness impregnated SiO2-TiO2 xerogels. Microporous Materials. 1996; 7(6): p. 309 - 321.

U.Schuchardt; D.Cardoso, R.Sercheli, R. Pereira, R.S.D.Cruz, M.C.Guerrerio, D.Mandelli, E.V.Spinace, E. L.Pires. Cyclohexane oxidation continues to be a challenge. Applied Catalysis A: General. 2001; 1: p. 211 - 219.

D.R.C.Huybrechts, P.L.Buskens, P.A.Jacobs. Physicochemical and catalytic properties of titanium silicalites. Journal of Molecular Catalysis. 1992; 71: p. 129 - 147.

M.M.J.Treacy, J.B.Higgins. Collection of simulated XRD powder patterns for zeolites. Elsevier. 2001.

C.Beck, T.Mallat, T.Burgi, A.Baiker. Nature of active sites in sol-gel TiO2-SiO2 epoxidation catalysts. Journal of Catalysis. 2001; 204: p. 428 - 439.

M.A.Uguina, D.P.Serrano, G.Ovejero, R.V.Grieken, M.Camacho. TS-2 synthesis from wetness-impregnated SiO2-TiO2 xerogels. Applied Catalysis A: General. 1995; 124: p. 391 - 399.

B.Notari. Synthesis and catalytic properties of titanium containing zeolites. Studies in Surface Science and Catalysis. 1988; 37: p. 413 - 425.

F.Geobaldo, S.Bordiga, A.Zecchina, E.Gianello, G.Leofanti, G.Petrini. DRS UV-Vis and EPR spectroscopy of hydroperoxo and superoxo complexes in titanium silicalite. Catalysis Letters. 1992; 16: p. 109 - 113.

U.Wilkenhoner, G.Langhendries, F.V.Laar, G.V.Baron, D.W.Gammon, P.A.Jacobs, E.V.Steen, Influence of pore and crystal size of crystalline titanosilicates on phenol hydroxylation in different solvents. Journal of Catalysis. 2001; 203: p. 201 - 209.

A.Keshavaraja, V.Ramaswamy, H.S.Soni, A.V.Ramaswamy, P.Ratnasamy. Synthesis, characterization and catalytic properties of micro-mesoporous, amorphous titanosilicate catalysts. Journal of Catalysis. 1995; 157: p. 501 - 508.

K.Y.Kim, W.S.Ahn, D.W.Park, J.H.Oh, C M.Lee, W.P.Tai. Microwave synthesis of titanium silicalite-1 using solid phase precursors. Bulletin of the Korean Chemical Society. 2004; 25 (5): p. 634 - 638.

D.D.Eley, W.O.Hagg, B.Gates. Advances in catalysis. 1st ed. Academic Press. 1996.

R.Hutter, D.C.M.Dutoit, T.Mallat, M.Schneider, A.Baiker. Novel mesoporous titania-silica aerogels highly active for the selective epoxidation of cyclic olefins. Journal of the Chemical Society, Chemical Communications. 1995; 2: p. 163 - 164.

V.Lafond, P.H.Mutin, A. Vioux. Non-hydrolytic solgel routes based on alkyl halide elimination: toward better mixed oxide catalysts and new supports: Application to the preparation of a SiO2-TiO2 epoxidation catalyst. Journal of Molecular Catalysis A: Chemical. 2002; 182 - 183: p. 81 - 88.

Q.H.Xia, X.Chem, T.Tatsumi. Epoxidation of cyclic alkenes with hydrogen peroxide and tert-butyl hydroperoxide on Na-containing Ti beta zeolites. Journal of Molecular Catalysis A: Chemical. 2001; 176 (1-2): p. 179 - 193.

S.C.Laha, R.Kumar. Highly selective epoxidation of olefinic compounds over TS-1 and TS-2 redox molecular sieves using anhydrous urea-hydrogen peroxide as oxidizing agent. Journal of Catalysis. 2002, 208 (2), p: 339 - 344.

Đã đăng
2013-06-28
How to Cite
Welch, A., Hong, N. K. D., & Gopinathan, S. (2013). Synthesis and characterisation of titanosilicates used as catalysts for the epoxidation of cyclohexene. Tạp Chí Dầu Khí, 6, 28-37. Truy vấn từ https://pvj.vn/index.php/TCDK/article/view/680
Số tạp chí
Chuyên mục
Bài báo khoa học

Most read articles by the same author(s)