Abstract
This paper describes a grafting technique that we developed for preparing highly dispersed Cs-tungstophosphoric acid (Cs-TPA) salt on a mesoporous silica carrier (MCM-41) using alcohols as solvents during impregnation. It is shown that this procedure leads to a novel class of catalysts with high dispersion of Cs-TPA salts which exhibit significantly improved catalytic performances for the alkylation of 1,3,5-trimethylbenzene with cyclohexene than those prepared using water as the solvent. Catalyst activity demonstrated to have a clear correlation with the type of alcohol used during impregnation which decreased in the following order: 1-butanol > 1-propanol ≈ ethanol > water. Adsorption data using molecules of various sizes suggest that our novel catalysts maintained open pore structures after the impregnation with tungstophosphoric acid (TPA). For comparison purposes, we also used a prior published method to prepare Cs-TPA on MCM-41, which seemed to have suffered unfavorable structural changes such as partial pore clogging leading to significant transport limitations for the reactants examined here.
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P.T. Anastas,L.B. Bartlett,M.M. Kirchhoff andT.C. Williamson, Catal. Today 55 (2000) 11.
A. Corma andA. Martínez, Catal. Rev. Sci. Eng. 35 (1993) 483.
A. Corma, Chem. Rev. 95 (1995) 559.
A. de Angelis,P. Ingallina,D. Berti,L. Montanari andM.G. Clerici, Catal. Lett. 61 (1999) 45.
M. Misono andT. Okuhara, ChemTech 11 (1993) 23.
T. Okuhara,N. Mizuno andM. Misono, Adv. Catal. 41 (1996) 113.
N. Mizuno andM. Misono, Chem. Rev. 98 (1998) 199.
M. Misono,N. Mizuno,K. Katamura,A. Kasai,Y. Konishi,K. Sakata,T. Okuhara andY. Yoneda, Bull. Chem. Soc. Jpn. 55 (1982) 400.
M. Misono, Catal. Rev. Sci. Eng. 29 (1987) 269.
I.V. Kozhevnikov, Catal. Rev. Sci. Eng. 37 (1995) 311.
T. Okuhara,T. Nishimura,H. Watanabe andM. Misono, J. Mol. Catal. 74 (1992) 247.
A. Corma,A. Martínez andC. Martínez, J. Catal. 164 (1996) 422.
M. Kimura,T. Nakato andT. Okuhara, Appl. Catal. A 165 (1997) 227.
G.I. Kapustin,T.R. Brueva,A.L. Klyachko,M.N. Timofeeva,S.M. Kulikov andI.V. Kozhevnikov, Kinet. Katal. 31 (1990) 1017.
I.V. Kozhevnikov,A. Sinnema,R.J.J. Jansen,K. Pamin andH. van Bekkum, Catal. Lett. 30 (1995) 241.
I.V. Kozhevnikov,K.R. Kloetstra,A. Sinnema,H.W. Zandbergen andH. van Bekkum, J. Mol. Catal. A 114 (1996) 287.
T. Blasco,A. Corma,A. Martínez andP. Martínez-Escolano, J. Catal. 177 (1998) 306.
L.R. Pizzio,C.V. Cáceres andM.N. Blanco, Appl. Catal. A 167 (1998) 283.
Y. Wang,A.Y. Kim,X.S. Li,L. Wang,C.H.F. Peden andB.C. Bunker, in: Shape-Selective Catalysis: Chemical Synthesis and Hydrocarbon Processing, eds. C. Song,J.M. Garces andY. Sugi ( Am. Chem. Soc., Washington, DC, 1998 ) ch. 25.
S. Soled,S. Miseo,G. McVicker,W.E. Gates,A. Gutierrez andJ. Paes, Catal. Today 36 (1997) 441.
S. Choi,Y. Wang,Z. Nie,J. Liu andC.H.F. Peden, Catal. Today 55 (2000) 117.
J.S. Beck,J.C. Vartuli,W.J. Roth,M.E. Leonowicz andC.T. Kresge, J. Am. Chem. Soc. 114 (1992) 10834.
C.T. Kresge,M.E. Leonowicz,W.J. Roth,J.C. Vartuli andJ.S. Beck, Nature 359 (1992) 710.
T. Okuhara,T. Nishimura andM. Misono, Chem. Lett. (1995) 155.
G.B. McGarvey andJ.B. Moffat, J. Mol. Catal. 69 (1991) 137.
J.C. Vartuli,C.T. Kresge,W.J. Roth,S.B. McCullen,J.S. Beck,K.D. Schmitt,M.E. Leonowicz,J.D. Lutner and E.W. Sheppard, Advanced Catalysts and Nanostructured Materials ( Academic Press, New York, 1996 ).
Y. Yoshinaga and T. Okuhara, J. Chem. Faraday Trans. 94 (1998) 2235.
S.J. Gregg andK.S.W. Sing, Adsorption, Surface Area and Porosity ( Academic Press, New York, 1982 ).
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Wang, Y., Peden, C.H. & Choi, S. Preparation of Highly Dispersed Cs-Tungstophosphoric Acid Salt on MCM-41 Silica. Catalysis Letters 75, 169–173 (2001). https://doi.org/10.1023/A:1016787820827
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DOI: https://doi.org/10.1023/A:1016787820827