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

• Autorzy: Samidha Saxena , Reena Dwivedi , Sheenu Bhadauria , V. Chumbhale , Rajendra Prasad
• Języki publikacji: EN

Abstrakty

EN

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 PO PH / (k1 PO + k2 PH) 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.

Słowa kluczowe

EN

Kinetics; Epoxidation; Au/TS-1; styrene; Styrene Oxide

• Czasopismo: Polish Journal of Chemical Technology
• Rocznik: 2010
• Tom: 12
• Numer: 4
• Strony: 72-78

Daty

wydano

2010-01-01

online

2010-12-28

Twórcy

autor

Samidha Saxena

• Catalysis and Nanomaterials Research Laboratory School of Chemical Sciences, Devi Ahilya University, Indore-452001 INDIA

autor

Reena Dwivedi

• Catalysis and Nanomaterials Research Laboratory School of Chemical Sciences, Devi Ahilya University, Indore-452001 INDIA

autor

Sheenu Bhadauria

• Catalysis and Nanomaterials Research Laboratory School of Chemical Sciences, Devi Ahilya University, Indore-452001 INDIA

autor

V. Chumbhale

• Catalysis Division, National Chemical Laboratory, Pune-8, INDIA

autor

Rajendra Prasad

• Catalysis and Nanomaterials Research Laboratory School of Chemical Sciences, Devi Ahilya University, Indore-452001 INDIA

Bibliografia

• 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.
• 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. J. Catal. 130, 1-8. DOI:10.1016/0021-9517(91)90086-J.[Crossref]
• Reddy, J. S., Kumar, R. & Ratnasamy, P. (1990). Titanium Silicalite-2: Synthesis, Characterization and Catalytic Properties. Appl. Catal. 58 L1.
• Reddy, J. S. & Kumar, R (1992). Crystallization kinetics of a new titanium silicate with MEL structure (TS-2). Zeolites, 12, 95-100. DOI:10.1016/0144-2449(92)90017-J.[Crossref]
• Huybrechts, D.R, Bruycker, L. D. & Jacobs, P. A. (1990). Oxyfunctionalization of alkanes with hydrogen peroxide on titanium silicalite. Nature, 345, 240-242. DOI:10.1038/345240a0.[Crossref]
• Reddy, R. S., Reddy, J. S., Kumar, R., Kumar, P. (1992). Sulfoxidation of thioethers using titanium silicate molecular sieve catalysts. J. Chem. Soc. Chem. Commun. 2, 84-85. DOI: 10.1039/C39920000084.[Crossref]
• 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 H2O2 as Oxidizing Agent. J. Catal. 156, 163-166. DOI:10.1006/jcat.1995.1242.[Crossref]
• Laha, S. C., Kumar, R. (2001). Selective Epoxidation of Styrene to Styrene Oxide over TS-1 Using Urea-Hydrogen Peroxide as Oxidizing Agent. J. Catal. 204, 64-70. DOI:10.1006/jcat.2001.3352.[Crossref]
• Haruta, M., Tsubota, S., Kobayashi, T., Kageyama, H., Genet, M. & Delmon, B. (1993). Low-Temperature Oxidation of CO over Gold Supported on TiO2, α-Fe2O3, and Co3O4. J. Catal. 144, 175-192. DOI:10.1006/jcat.1993.1322.[Crossref]
• Prati, L. & Porta, F. (2005). Oxidation of alcohols and sugars using Au/C catalysts: Part 1. Alcohols. Appl. Catal. A: General. 291, 199-203. DOI:10.1016/j.apcata.2004.11.050.
• 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. Ind. Eng. Chem. Res. 38, 884-891. DOI: 10.1021/ie980494x.[Crossref]
• Yadav, G. D. & Pujari, A. (2000). Epoxidation of Styrene to Styrene Oxide: Synergism of Heteropoly Acid and Phase-Transfer Catalyst under Ishii-Venturello Mechanism. Org. Proc. Res. & Dev. 4, 88-93. DOI: 10.1021/op990055p.[Crossref]
• Singh, U. K. & Vannice, M. A. (2001). Kinetics of liquid-phase hydrogenation reactions over supported metal catalysts-a review, Applied Catalysis A: Gen. 213, 1-24. DOI:10.1016/S0926-860X(00)00885-1[Crossref]
• Mars P., Van Krevelene D. W (1954). Oxidation carried out by means of vanadium oxide catalysts. Spec. suppl. to Chem. Eng, Sci., 3, 41-.
• Shetti, V. N., Manikandan, P., Srivinas, D. & Ratnasamy, P. (2003). Reactive oxygen species in epoxidation reactions over titanosilicate molecular sieves. J. Catal. 216, 461-467. DOI:10.1016/S0021-9517(02)00119-7.[Crossref]
• 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.[Crossref]
• 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. J. Am. Chem. Soc., 123, 2204-2212. DOI: 10.1021/ja003657t.[Crossref]
• 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. J. Am. Chem. Soc. 126, 2956-2962. DOI: 10.1021/ja037741v.[Crossref]
• 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. J. Phys. Chem. B., 110, 16439-16451. DOI: 10.1021/jp061754o.
• 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. J. Catal. 265, 238-244. doi:10.1016/j.jcat.2009.05.007[Crossref]
• 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. Appl. Catal. A: General, 337, 58-65. DOI: 10.1016/j.apcata.2007.11.037.[WoS][Crossref]
• 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. Appl. Cata. A: General, 258, 1-6. DOI: 10.1016/j.apcata.2003.06.002.[Crossref]
• Shetti, V. N., Srinivas, D. & Ratnasamy, P. (2004). Enhancement of chemoselective in epoxidation reactions over TS-1 catalysts by alkali and alkaline metal ions. J. Mol. Catal. A: Chemical, 210, 171-178. DOI: 10.1016/j.molcata.2003.09.014.[Crossref]

Identyfikatory

DOI

10.2478/v10026-010-0054-6