Abstract
Ce and La incorporated ZSM-5 zeolitic materials with different metal loadings were synthesized via the multiple pH-adjusting procedures involving a co-hydrolysis of TEOS (tetraethyl-orthosilicate) with rare earth salts under a strong acidic condition, a further gelation under a weak acidic condition, and a final basic hydrothermal crystallization. Thus obtained Ce(La)-ZSM-5, as well as Ce or La ion-exchanged ZSM-5 samples, were characterized by XRD, SEM, TG, UV–vis, 29Si MAS NMR, FT-IR, N2-physisorption, and elemental analysis. The characterizations provide systematic and complementary evidences to demonstrate the incorporation of Ce(La) ions into the tetrahedral sites of ZSM-5 framework. The upper limits of the rare earth loadings in the synthesis gel and the final product are ca. 50 and 70 of the molar ratio of Si/Ce(La), respectively. It is observed that the synthesized Ce(La)-ZSM-5 zeolites possess an unusual morphology of microspheres that are assembled by numerous cubic prism-shaped nanocrystallines.
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C.S. Cundy, P.A. Cox, Chem. Rev. 103, 663 (2003)
W. Song, R.E. Justice, C.A. Jones, V.H. Grassian, S.C. Larsen, Langmuir 20, 8301 (2004)
H. Berndt, A. Martin, A. Brückner, E. Schreier, D. Müller, H. Kosslick, G.-U. Wolf and B. Lücke, J. Catal. 191, 384 (2000)
W. Fan, R.-G. Duan, T. Yokoi, P. Wu, Y. Kubota and T. Tatsumi. J. Am. Chem. Soc. 130, 10150 (2008)
J. Perez-Ramirez, J.C. Groen, A. Brückner, M.S. Kumar, U. Bentrup, M.N. Debbagh, L.A. Villaescusa, J. Catal. 232, 318 (2005)
C.T. Brigden, C.D. Williams, D. Apperley, Inorg. Mater. 43, 758 (2007)
K.B. Sidhpuria, P.A. Parikh, P. Bahadur, R.V. Jasra, J. Porous. Mater. 15, 481 (2008)
E. Nigro, F. Crea, F. Testa, R. Aiello, P. Lentz, J.B. Nagy, Microporous Mesoporous Mater. 30, 199 (1999)
A. Ghosh, N.G. Vargas, S.F. Mitchell, S. Stevenson, D.F. Shantz, J. Phys. Chem. C 113, 12252 (2009)
C. T. Brigden, D. Thompsett and C. D. Williams, Dalton Trans. (18), 2829 (2004)
P. Fejes, J.B. Nagy, K. Kovács, G. Vankó, Appl. Catal. A 145, 155 (1996)
G.F. Ghesti, J.L. de Macedo, V.C.I. Parente, J.A. Dias, S.C.L. Dias, Microporous Mesoporous Mater. 100, 27 (2007)
A. Arnold, S. Steuernagel, M. Hunger, J. Weitkamp, Microporous Mesoporous Mater. 62, 97–106 (2003)
Y.K. Hwang, J.-S. Chang, S.-E. Park, D.S. Kim, Y.-U. Kwon, S.H. Jhung, J.-S. Hwang, M.S. Park, Angew. Chem. Int. Ed. 44, 556 (2005)
R.H. Baney, M Itoh, A. Sakakibara and T. Suzuki. Chem. Rev. 95, 1409 (1995)
J. Gu, Y. Wu, J. Wang, J. Mater. Sci. 44, 3777 (2009)
Y. Wu, X. Ren, J. Wang, Mater. Chem. Phys. 113, 773 (2008)
F. Cao, Y. Wu, J. Gu, J. Wang, Mater. Chem. Phys. 130, 727 (2011)
Y. Wu, W. Wang, P. Liu, W. Zhang, J. Gu, X. Wang, J. Am. Chem. Soc. 132, 17989 (2010)
B.S. Popovic, J. Appl. Crystallogr. 4, 240 (1971)
B.S. Popovic, J. Appl. Crystallogr. 6, 122 (1973)
P. Wu, T. Komatsu, T. Yashima, Microporous Mesoporous Mater. 20, 139 (1998)
R. Fricke, H. Kosslick, G. Lischke, M. Richter, Chem. Rev. 100, 2303 (2000)
L.G.A. van de Water, J.C. van der Waal, J.C. Jansen, M. Cadoni, L. Marchese, T. Maschmeyer, J. Phys. Chem. B 107, 10423 (2003)
N. Phonthammachai, M. Krissanasaeranee, E. Gulari, A.M. Jamieson, S. Wongkasemjit, Mater. Chem. Phys. 97, 458 (2006)
H. Kosslick, V.A. Tuan, R. Fricke, Ch. Peuker, W. Pilz, W. Storek, J. Phys. Chem. 97, 5678 (1993)
M. Hunger, J. Weitkamp, Angew. Chem. Int. Ed. 40, 2954 (2001)
S.C. Laha, P. Mukherjee, S.R. Sainkar, R. Kumar, J. Catal. 207, 213 (2001)
M.D. Kadgaonkar, S.C. Laha, R.K. Pandey, P. Kumar, S.P. Mirajkar, R. Kumar, Catal. Today 97, 225 (2004)
W.H. Yao, Y.J. Chen, L. Min, H. Fang, Z. Yan, H. Wang, J. Wang, J. Mol. Catal. A: Chem. 246, 162 (2006)
W. Zhan, Y. Guo, Y. Wang, X. Liu, Y. Guo, Y. Wang, Z. Zhang, G. Lu, J. Phys. Chem. B 111, 12103 (2007)
C.I. Round, C.D. Williams, K. Latham, C.V.A. Duke, J. Therm. Anal. Calorim. 63, 329 (2001)
L. Shirazi, E. Jamshidi, M.R. Ghasemi, Cryst. Res. Technol. 43, 1300 (2008)
E. Nigro, F. Crea, F. Testa, R. Aiello, P. Lentz, J.B. Nagy, Microporous Mesoporous Mater. 30, 199 (1999)
Q. Zhao, X.H. Bao, X.W. Han, X.M. Liu, D.L. Tan, L.W. Lin, X.W. Guo, G. Li, X.S. Wang, Mater. Chem. Phys. 66, 41 (2000)
S.L. Burkett, M.E. Davis, Chem. Mater. 7, 920 (1995)
Acknowledgments
The authors thank the financial support from the National Natural Science Foundation of China (grant nos. 20976084, 21136005 and 21101094), and the Ph.D. innovation Program Foundation of Jiangsu Province (CX108-1712).
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Gu, J., Wu, Y., Jin, Y. et al. Hydrothermal incorporation of Ce(La) ions into the framework of ZSM-5 by a multiple pH-adjusting co-hydrolysis. J Porous Mater 20, 7–13 (2013). https://doi.org/10.1007/s10934-012-9569-y
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DOI: https://doi.org/10.1007/s10934-012-9569-y