Kinetics studies and mechanism evolution of the epoxidation of styrene over nanoporous Au doped TS-1

Samidha Saxena; Reena Dwivedi; Sheenu Bhadauria; V. Chumbhale; Rajendra Prasad

doi:10.2478/v10026-010-0054-6

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Kinetics studies and mechanism evolution of the epoxidation of styrene over nanoporous Au doped TS-1

Green Sciences

Volume 12 (2010): Issue 4 (December 2010)

By: Samidha Saxena, Reena Dwivedi, Sheenu Bhadauria, V. Chumbhale and Rajendra Prasad

Open Access

|Dec 2010

Abstract

A kinetic investigation of the slurry phase epoxidation of styrene with hydrogen peroxide has been carried out, for the first time, over nanoporous Au doped TS-1 catalyst, in a batch reactor, in the temperature range of 313-333 K. It was found that product selectivity and the rate of reaction are greatly influenced by concentrations of styrene and hydrogen peroxide. Kinetics studies reveal that the mechanism of the reaction is of the "Redox" type. The rate equation, r = k₁ k₂ P_O P_H / (k₁ P_O + k₂ P_H) deduced, assuming a steady state involving two stage oxidation-reduction process, represent the data most satisfactorily for the conversion of styrene to styrene oxide. A tentative mechanism of the process has also been suggested.

References

Taramaso, M., Pergo, G. & Notari, B. (1983). Preparation of porous crystalline synthetic material comprised of silicon and titanium oxides. U. S. Patent No. 4,410,501.
Search in Google Scholar
Thangaraja, A., Kumar, R., Mirajker, S. P. & Ratnasamy, P. (1991). Catalytic properties of crystalline titanium silicalites I. Synthesis and characterization of titanium-rich zeolites with MFI structure.130, 1-8. DOI:10.1016/0021-9517(91)90086-J.
Open DOI Search in Google Scholar
Reddy, J. S., Kumar, R. & Ratnasamy, P. (1990). Titanium Silicalite-2: Synthesis, Characterization and Catalytic Properties.58 L1.
Open DOI Search in Google Scholar
Reddy, J. S. & Kumar, R (1992). Crystallization kinetics of a new titanium silicate with MEL structure (TS-2)., 12, 95-100. DOI:10.1016/0144-2449(92)90017-J.
Open DOI Search in Google Scholar
Huybrechts, D.R, Bruycker, L. D. & Jacobs, P. A. (1990). Oxyfunctionalization of alkanes with hydrogen peroxide on titanium silicalite., 345, 240-242. DOI:10.1038/345240a0.
Open DOI Search in Google Scholar
Reddy, R. S., Reddy, J. S., Kumar, R., Kumar, P. (1992). Sulfoxidation of thioethers using titanium silicate molecular sieve catalysts.2, 84-85. DOI: 10.1039/C39920000084.
Open DOI Search in Google Scholar
Kumar, S. B., Mirajkar, S. P., Govind, C. G., Kumar, P. & Kumar, R. (1995). Epoxidation of Styrene over a Titanium Silicate Molecular Sieve TS1 Using Dilute HOas Oxidizing Agent.156, 163-166. DOI:10.1006/jcat.1995.1242.
Open DOI Search in Google Scholar
Laha, S. C., Kumar, R. (2001). Selective Epoxidation of Styrene to Styrene Oxide over TS-1 Using Urea-Hydrogen Peroxide as Oxidizing Agent.204, 64-70. DOI:10.1006/jcat.2001.3352.
Open DOI Search in Google Scholar
Haruta, M., Tsubota, S., Kobayashi, T., Kageyama, H., Genet, M. & Delmon, B. (1993). Low-Temperature Oxidation of CO over Gold Supported on TiO, α-FeO, and CoO.144, 175-192. DOI:10.1006/jcat.1993.1322.
Open DOI Search in Google Scholar
Prati, L. & Porta, F. (2005). Oxidation of alcohols and sugars using Au/C catalysts: Part 1. Alcohols.291, 199-203. DOI:10.1016/j.apcata.2004.11.050.
Open DOI Search in Google Scholar
Nijhuis, T. A., Huizinga, B. T. & Makkee, J. A. (1999). Direct Epoxidation of Propene Using Gold Dispersed on TS-1 and Other Titanium-Containing Supports.38, 884-891. DOI: 10.1021/ie980494x.
Open DOI Search in Google Scholar
Yadav, G. D. & Pujari, A. (2000). Epoxidation of Styrene to Styrene Oxide: Synergism of Heteropoly Acid and Phase-Transfer Catalyst under Ishii-Venturello Mechanism.4, 88-93. DOI: 10.1021/op990055p.
Open DOI Search in Google Scholar
Singh, U. K. & Vannice, M. A. (2001). Kinetics of liquid-phase hydrogenation reactions over supported metal catalysts-a review,213, 1-24. DOI:10.1016/S0926-860X(00)00885-1
Open DOI Search in Google Scholar
Mars P., Van Krevelene D. W (1954). Oxidation carried out by means of vanadium oxide catalysts., 3, 41-.
Search in Google Scholar
Shetti, V. N., Manikandan, P., Srivinas, D. & Ratnasamy, P. (2003). Reactive oxygen species in epoxidation reactions over titanosilicate molecular sieves.216, 461-467. DOI:10.1016/S0021-9517(02)00119-7.
Open DOI Search in Google Scholar
Khouw, C.B, Dartt, C. B., Labinger, J. A. & Davis, M. E. (1994). Studies on the Catalytic-Oxidation of Alkanes and Alkenes by Titanium Silicates. J. Catal. 149, 195-205. DOI:10.1006/jcat.1994.1285.
Open DOI Search in Google Scholar
Lamberti, C., Bordiga, S., Zecchina, A., Artioli, G., Marra, G. & Spano, G. (2001). Ti Location in the MFI Framework of Ti-Silicalite-1: A Neutron Powder Diffraction Study., 123, 2204-2212. DOI: 10.1021/ja003657t.
Open DOI Search in Google Scholar
Wells, D. H., Delgass, W. N. & Thomson, K. T. (2004). Evidence of Defect-Promoted Reactivity for Epoxidation of Propylene in Titanosilicate (TS-1) Catalysts: A DFT Study.126, 2956-2962. DOI: 10.1021/ja037741v.
Open DOI Search in Google Scholar
Joshi, A. M., Delgass, W. N. & Thomson, K. T. (2006). Adsorption of small Aun (n=1-5) and Au-Pd clusters inside the TS-1 and S-1 pores., 110, 16439-16451. DOI: 10.1021/jp061754o.
Open DOI Search in Google Scholar
Corma, A., Domínguez, I., Doménech, A., Fornés, V., Gómez-García, C., Ródenas, T. & Sabater, M. J. (2009). Enantioselective epoxidation of olefins with molecular oxygen catalyzed by gold(III): A dual pathway for oxygen transfer.265, 238-244. doi:10.1016/j.jcat.2009.05.007
Open DOI Search in Google Scholar
Yang, G., Lan, X, huang, J. Z, Ma D., Zhou, L., Liu, X., Han, X. & Bao, X. (2008). Acidity and defect sites in titanium silicatlite catalyst., 337, 58-65. DOI: 10.1016/j.apcata.2007.11.037.
Open DOI Search in Google Scholar
Zhuang, J., Ma, D., Yan, Z., Liu, X., Han, X., Bao, X., Zhang, Y., Guo, X. & Wang, X. (2004). Effect of acidity in TS-1 zeolites on product distribution of the styrene oxidation reaction., 258, 1-6. DOI: 10.1016/j.apcata.2003.06.002.
Open DOI Search in Google Scholar
Shetti, V. N., Srinivas, D. & Ratnasamy, P. (2004). Enhancement of chemoselective in epoxidation reactions over TS-1 catalysts by alkali and alkaline metal ions., 210, 171-178. DOI: 10.1016/j.molcata.2003.09.014.
Open DOI Search in Google Scholar

Articles in this issue

DOI: https://doi.org/10.2478/v10026-010-0054-6 | Journal eISSN: 3072-0389 (formerly 1899-4741) | Journal ISSN: 1509-8117

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Language: English

Page range: 72 - 78

Published on: Dec 28, 2010

Published by: West Pomeranian University of Technology, Szczecin

In partnership with: Paradigm Publishing Services

Publication frequency: Volume open

Keywords:

Kinetics,

Epoxidation,

Au/TS-1,

styrene,

Styrene Oxide

Related subjects:

Industrial chemistry,

Biotechnology,

Chemical engineering,

Process engineering

© 2010 Samidha Saxena, Reena Dwivedi, Sheenu Bhadauria, V. Chumbhale, Rajendra Prasad, published by West Pomeranian University of Technology, Szczecin
This work is licensed under the Creative Commons License.

Volume 12 (2010): Issue 4 (December 2010)