Abstract
Chromium-containing ethane-bridged hybrid periodic mesoporous organosilicas (Cr-PMO) were synthesized using 1,2-bis(triethoxysilyl)ethane (BTEE) and tetraethyl orthosilicate (TEOS) as silica sources and alkyltrimethyl ammonium salts as surfactants by two different synthesis routes. PXRD and N2 adsorption–desorption analysis shows that the original structure of the materials is maintained after chromium substitution while spectroscopic study proves the incorporation of chromium in the frame wall positions and show the existence of Cr2O3 species in the mixed silica source (BTEE-TEOS) synthesized chromium samples. The catalytic activity of the newly developed chromium samples was evaluated in the liquid phase oxidation of cyclohexane and ethylbenzene using air as an oxidant. Further, the Cr-PMO samples exhibited better cyclohexane conversion and cyclohexanone selectivity than the conventional Cr-MCM-41 and other metal-containing MCM-41 samples. The exceptional activity of the new chromium-containing molecular sieves is attributed to the hydrophobicity of the materials and to the complementary structural features that facilitates the accessibility of substrate to the active framework chromium sites.
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References
Sheldon RA, Kochi JK (1981) Metal-catalyzed oxidations of organic compounds. Academic Press, New York
Suresh KA, Sharma MM, Sridhar T (2000) Ind Eng Chem Res 39:3958–3997
Thomas JM, Raja R (2001) Chem Commun 675–687
Sankar G, Raja R, Thomas JM (1998) Catal Lett 55:15–23
Corma A (1997) Chem Rev 97:2373–2420
Sayari A (1996) Chem Mater 8:1840–1852
Tian P, Liu Z, Wu Z, Xu L, He Y (2004) Catal Today 93:735–742
Luna FJ, Ukawa SE, Wallau M, Schuchardt U (1997) J Mol Catal A Chem 117:405–411
Carvalho WA, Wallau M, Schuchardt U (1999) J Mol Catal A Chem 144:91–99
Sakthivel A, Selvam P (2002) J Catal 211:134–143
Inagaki S, Guan S, Fukushima Y, Ohsuna T, Terasaki O (1999) J Am Chem Soc 121:9611–9614
Asefa T, MacLachlan MJ, Coombs N, Ozin GA (1999) Nature 402:867–870
Melde BJ, Holland BT, Blanford CF, Stein A (1999) Chem Mater 11:3302–3308
Asefa T, MacLachlan MJ, Grondey H, Coombs N, Ozin GA (2000) Angew Chem Int Ed 39:1808–1811
Kapoor MP, Bhaumik A, Inagaki S, Kuraoka K, Yazawa T (2002) J Mater Chem 12:3078–3083
Dapurkar SE, Sakthivel A, Selvam P (2003) New J Chem 27:1184–1190
Rebbin V, Jakubowski M, Potz S, Froba M (2004) Microporous Mesoporous Mater 72:99–104
Wahab MA, Kim II, Ha C-S (2004) Microporous Mesoporous Mater 69:19–27
Shylesh S, Singh AP (2005) J Catal 233:359–371
Zhu Z, Chang Z, Kevan L (1999) J Phys Chem B 103:2680–2688
Weckhuysen BM, Wachs IE, Schoonheydt RA (1996) Chem Rev 96:3327–3350
Zhu Z, Hartmann M, Maes EM, Czernuszewicz RS, Kevan L (2000) J Phys Chem B 104:4690–4698
Reddy EP, Davydov L, Smirniotis PG (2002) J Phys Chem B 106:3394–3401
Lu G, Zhao R, Qian G, Qi Y, Wang X, Suo J (2004) Catal Lett 97:115–118
Raja R, Sankar G, Thomas JM (1999) J Am Chem Soc 121:11926–11927
Acknowledgments
APS thanks FY2007 JSPS (Japan Society for the Promotion of Science) Invitation Fellowship Programme for Research in Japan (Long-Term-ID No. L-07548) for the financial support. We thank Mr. R. K. Jha for the adsorption analysis and Dr. S. P. Mirajkar for the TPR analysis.
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Singh, A.P., Torita, N., Shylesh, S. et al. Catalytic Aerobic Oxidation of Cyclohexane and Ethyl Benzene Over Chromium-Containing Mesoporous Organosilicas. Catal Lett 132, 492–499 (2009). https://doi.org/10.1007/s10562-009-0121-x
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DOI: https://doi.org/10.1007/s10562-009-0121-x