镧改性提高ZSM-5分子筛水热稳定性

doi:10.3866/PKU.WHXB20110130

Abstract

Abstract:

We carried out a theoretical investigation into the mechanism of steam dealumination of the ZSM-5 zeolite and into the mechanism for the increase in the hydrothermal stability of the La-modified ZSM-5 zeolite. This was done using density functional theory (DFT) with 12T cluster models that simulated the local structures of the zeolite materials. We demonstrate that because of the hydrogen bond interaction between the first adsorbed water molecule and the ZSM-5 zeolite framework, the Al—O bond is weakened and elongated. As the second water molecule is adsorbed, the Al—O bond near the second water molecule is further weakened and eventually broken because of the hydrogen bond interaction between the second adsorbed water molecule and the ZSM-5 zeolite framework. As more water molecules are adsorbed, the other Al—O bonds are broken sequentially resulting in a dealumination of the ZSM-5 zeolite. The introduced lanthanum coordinates with four zeolite framework oxygen atoms, thickens the zeolite framework, moves over the framework Al atom, increases the steric hindrances and partially prevents polar water molecules from attacking the Al—O bond. These actions retard the weakening of the Al—O bonds and improve the hydrothermal stability of the ZSM-5 zeolite. The calculated adsorption and hydrolysis energies of the water molecule further confirm that the presence of lanthanum enhances the hydrothermal stability of the ZSM-5 zeolite.

Key words: Zeolite, Density functional theory, Dealumination, La-modification, Hydrothermal stability

MSC2000:

O641

LI Yan-Feng, ZHU Ji-Qin, LIU Hui, WANG Peng, TIAN Hui-Ping. Increase in the Hydrothermal Stability of the La-Modified ZSM-5 Zeolite[J].Acta Phys. -Chim. Sin., 2011, 27(01): 52-58.

References

1 Wang,W. L.; Liu, B. J.; Zeng, X. J. Acta Phys. -Chim. Sin., 2008, 24: 2102
[王文兰, 刘百军, 曾贤君. 物理化学学报, 2008, 24: 2102]
2 Zheng, A.; Chen, L.; Yang, J.; Zhang, M.; Su, Y.; Yue, Y.; Ye, C.; Deng, F. J. Phys. Chem. B, 2005, 109: 24273
3 Sano, T.; Uno, Y.;Wang, Z. B.; Ahn, C. H.; Soga, K. Micropor.ous Mesoporous Mat., 1999, 31: 89
4 Wang, S. P.;Wang, Y. L.; Cao, L.; Xing, S. Y.; Zhou, D. H. Chin. J. Catal., 2009, 30: 305
[王善鹏, 王伊蕾, 曹亮, 邢双英, 周丹红. 催化学报, 2009, 30: 305]
5 Corma, A.;Wojciechowski, B. Catal. Rev. Sci. Eng., 1985, 27: 29
6 Sanchez-Castillo, M. A.; Madon, R. J.; Dumesic, J. A. J. Phys. Chem. B, 2005, 109: 2164
7 Sano, T.; Yamashita, N.; Iwami, Y.; Takeda, K.; Kawakami, Y. Zeolites, 1996, 16: 258
8 Agostini, G.; Lamberti, C.; Palin, L.; Milanesio, M.; Danilina, N.; Xu, B.; Janousch, M.; van Bokhoven, J. A. J. Am. Chem. Soc., 2009, 132: 667
9 Ma, G.W.; Xie, Z. K. Chin. J. Mater. Res., 2009, 23: 205
[马广伟, 谢在库. 材料研究学报, 2009, 23: 205
10 Gates, B. C.; Katzer, J. R.; Schuit, G. C. A. Chemistry of catalytic processes. New York: McGraw-Hill, 1979: 184-189
11 Xu, M.; Liu, X.; Madon, R. J. J. Catal., 2002, 207: 237
12 Kim, J. T.; Kim, M. C.; Okamoto, Y.; Imanaka, T. J. Catal., 1989, 115: 319
13 Sano, T.; Ikeya, H.; Kasuno, T.;Wang, Z. B.; Kawakami, Y.; Soga, K. Zeolites, 1997, 19: 80
14 Kooyman, P. J.; van derWaal, P.; van Bekkum, H. Zeolites, 1997, 18: 50
15 Yang, J.; Sun, H. Sci. China Ser. B-Chem., 2008, 38: 1
[杨静, 孙淮. 中国科学(B 辑: 化学), 2008, 38: 1]
16 Lamberov, A. A.; Kuznetsov, A. M.; Shapnik, M. S.; Masliy, A. N.; Borisevich, S. V.; Romanova, R. G.; Egorova, S. R. J. Mol. Catal. A-Chem., 2000, 158: 481
17 Ding, L.; Zheng, Y.; Hong, Y.; Ring, Z. Microporous Mesopor.ousMat., 2007, 101: 432
18 Jin, L.; Hu, H.; Zhu, S.; Ma, B. Catal. Today, 2010, 149: 207
19 Bhering, D. L.; Ramirez-Solis, A.; Mota, C. J. A. J. Phys. Chem. B, 2003, 107: 4342
20 Maijanen, A.; Derouane, E. G.; Nagy, J. B. Appl. Surf. Sci., 1994, 75: 204
21 Li, S.; Zheng, A.; Su, Y.; Zhang, H.; Chen, L.; Yang, J.; Ye, C.; Deng, F. J. Am. Chem. Soc., 2007, 129: 11161
22 Blasco, T.; Corma, A.; Martínez-Triguero, J. J. Catal., 2006, 237: 267
23 Yan, J. Y.; Sachtler,W. M. H.; Kung, H. H. Catal. Today, 1997, 33: 279
24 Budi, P.; Curry-Hyde, E.; Howe, R. F. Catal. Lett., 1996, 41: 47
25 Rokosz, M. J.; Kucherov, A. V.; Jen, H.W.; Shelef, M. Catal. Today, 1997, 35: 65
26 Li, R. S.;Wen, R.W.; Zhang,W. Y.;Wei, Q. Chem. J. Chin. Unvi., 1993, 14: 545
[李荣生, 温瑞武, 张武阳, 魏诠. 高等学校化学学报, 1993, 14: 545]
27 Ren, L. P.; Zhao, G. L.; Teng, J.W.;Wang, Y. D.; Xie, Z. K. Ind. Catal., 2007, 15: 30
[任丽萍, 赵国良, 滕加伟, 王仰东, 谢在库. 工业催化, 2007, 15: 30]
28 Wang, J.W.; Jin, G. Q.; Zhang, Z. X.;Wang, X. K. J. Chin. Rare Earth Soc., 2001, 19: 103
[王军威, 靳国强, 张志新, 王心葵. 中国稀土学报, 2001, 19: 103]
29 Li, M. H.; Yang, Y.;Wang, J. J. Dalian Inst. Light Ind., 2004, 23: 11
[李明慧, 杨毅, 王井. 大连轻工业学院学报, 2004, 23: 11]
30 Li, C. X.; Gao, Y. D.; Li, C. Y.; Shan, H. H.; Yang, C. H. J. Fuel Chem. Technol., 2006, 34: 47
[李成霞, 高永地, 李春义, 山红红, 杨朝合. 燃料化学学报, 2006, 34: 47]
31 Chang, C.; Zhang,W. Y.; Zhang, L. H.; Li, R. S.; Tian, M.W.; Yang, X. H.; Hou, L. Chem. J. Chin. Univ., 1996, 17: 1914
[常春, 张武阳, 张丽华, 李荣生, 田明文, 杨胥徽, 侯莉. 高等学校化学学报, 1996, 17: 1914]
32 Yang, G.; Zhuang, J. Q.;Wang, Y.; Zhou, D. H.; Yang, M. Q.; Liu, X. C.; Han, X.W.; Bao, X. H. J. Mol. Struct., 2005, 737: 271
33 Yang, G.;Wang, Y.; Zhou, D. H.; Zhuang, J. Q.; Liu, X. C.; Han, X.W.; Bao, X. H. Acta. Phys. -Chim. Sin., 2004, 20: 60
[杨刚, 王妍, 周丹红, 庄建勤, 刘宪春, 韩秀文, 包信和. 物理化学学报, 2004, 20: 60]
34 Yang, G.;Wang, Y.; Zhou, D. H.; Zhuang, J. Q.; Liu, X. C.; Han, X.W.; Bao, X. H. J. Chem. Phys., 2003, 119: 9765
35 Hartford, R.W.; Kojima, M.; O′ Connor, C. T. Ind. Eng. Chem. Res., 1989, 28: 1748
36 Tynj?l?, P.; Pakkanen, T. T. J. Mol. Catal. A-Chem., 1996, 110: 153
37 Ivanov, A. V.; Graham, G.W.; Shelef, M. Appl. Catal. BEnviron., 1999, 21: 243
38 Jiang, S.; Huang, S.; Qin, L.; Tu,W.; Zhu, J.; Tian, H.;Wang, P. J. Mol. Struc. Theochem., in press
39 Lee, C.; Yang,W.; Parr, R. G. Phys. Rev. B, 1988, 37: 785
40 Becke, A. D. Phys. Rev. A, 1988, 38: 3098
41 Frisch, M. J.; Trucks, G.W.; Schlegel, H. B.; et al. Gaussian 03. Revision D.01.Wallingford, CT: Gaussian Inc., 2004
42 Tajima, N.; Taketsugu, T.; Hirao, K. Chem. Phys., 1997, 218: 257
43 Krossner, M.; Sauer, J. J. Phys. Chem., 1996, 100: 6199
44 Olson, D. H.; Zygmunt, S. A.; Erhardt, M. K.; Curtiss, L. A.; Iton, L. E. Zeolites, 1997, 18: 347
45 Rice, M. J.; Chakraborty, A. K.; Bell, A. T. J. Phys. Chem. A, 1998, 102: 7498
46 Zygmunt, S. A.; Curtiss, L. A.; Iton, L. E.; Erhardt, M. K. J. Phys. Chem., 1996, 100: 6663
47 Zygmunt, S. A.; Curtiss, L. A.; Iton, L. E. J. Phys. Chem. B, 2001, 105: 3034
48 Ison, A.; Gorte, R. J. J. Catal., 1984, 89: 150

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Increase in the Hydrothermal Stability of the La-Modified ZSM-5 Zeolite

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