Citation:
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 Physico-Chimica Sinica,
;2011, 27(01): 52-58.
doi:
10.3866/PKU.WHXB20110130
-
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.
-
-
-
[1]
1 Wang,W. L.; Liu, B. J.; Zeng, X. J. Acta Phys. -Chim. Sin., 2008, 24: 2102
-
[2]
[王文兰, 刘百军, 曾贤君. 物理化学学报, 2008, 24: 2102]
-
[3]
2 Zheng, A.; Chen, L.; Yang, J.; Zhang, M.; Su, Y.; Yue, Y.; Ye, C.; Deng, F. J. Phys. Chem. B, 2005, 109: 24273
-
[4]
3 Sano, T.; Uno, Y.;Wang, Z. B.; Ahn, C. H.; Soga, K. Micropor.ous Mesoporous Mat., 1999, 31: 89
-
[5]
4 Wang, S. P.;Wang, Y. L.; Cao, L.; Xing, S. Y.; Zhou, D. H. Chin. J. Catal., 2009, 30: 305
-
[6]
[王善鹏, 王伊蕾, 曹亮, 邢双英, 周丹 红. 催化学报, 2009, 30: 305]
-
[7]
5 Corma, A.;Wojciechowski, B. Catal. Rev. Sci. Eng., 1985, 27: 29
-
[8]
6 Sanchez-Castillo, M. A.; Madon, R. J.; Dumesic, J. A. J. Phys. Chem. B, 2005, 109: 2164
-
[9]
7 Sano, T.; Yamashita, N.; Iwami, Y.; Takeda, K.; Kawakami, Y. Zeolites, 1996, 16: 258
-
[10]
8 A stini, G.; Lamberti, C.; Palin, L.; Milanesio, M.; Danilina, N.; Xu, B.; Janousch, M.; van Bokhoven, J. A. J. Am. Chem. Soc., 2009, 132: 667
-
[11]
9 Ma, G.W.; Xie, Z. K. Chin. J. Mater. Res., 2009, 23: 205
-
[12]
[马广伟, 谢在库. 材料研究学报, 2009, 23: 205
-
[13]
10 Gates, B. C.; Katzer, J. R.; Schuit, G. C. A. Chemistry of catalytic processes. New York: McGraw-Hill, 1979: 184-189
-
[14]
11 Xu, M.; Liu, X.; Madon, R. J. J. Catal., 2002, 207: 237
-
[15]
12 Kim, J. T.; Kim, M. C.; Okamoto, Y.; Imanaka, T. J. Catal., 1989, 115: 319
-
[16]
13 Sano, T.; Ikeya, H.; Kasuno, T.;Wang, Z. B.; Kawakami, Y.; Soga, K. Zeolites, 1997, 19: 80
-
[17]
14 Kooyman, P. J.; van derWaal, P.; van Bekkum, H. Zeolites, 1997, 18: 50
-
[18]
15 Yang, J.; Sun, H. Sci. China Ser. B-Chem., 2008, 38: 1
-
[19]
[杨静, 孙淮. 中国科学(B 辑: 化学), 2008, 38: 1]
-
[20]
16 Lamberov, A. A.; Kuznetsov, A. M.; Shapnik, M. S.; Masliy, A. N.; Borisevich, S. V.; Romanova, R. G.; E rova, S. R. J. Mol. Catal. A-Chem., 2000, 158: 481
-
[21]
17 Ding, L.; Zheng, Y.; Hong, Y.; Ring, Z. Microporous Mesopor.ousMat., 2007, 101: 432
-
[22]
18 Jin, L.; Hu, H.; Zhu, S.; Ma, B. Catal. Today, 2010, 149: 207
-
[23]
19 Bhering, D. L.; Ramirez-Solis, A.; Mota, C. J. A. J. Phys. Chem. B, 2003, 107: 4342
-
[24]
20 Maijanen, A.; Derouane, E. G.; Nagy, J. B. Appl. Surf. Sci., 1994, 75: 204
-
[25]
21 Li, S.; Zheng, A.; Su, Y.; Zhang, H.; Chen, L.; Yang, J.; Ye, C.; Deng, F. J. Am. Chem. Soc., 2007, 129: 11161
-
[26]
22 Blasco, T.; Corma, A.; Martínez-Triguero, J. J. Catal., 2006, 237: 267
-
[27]
23 Yan, J. Y.; Sachtler,W. M. H.; Kung, H. H. Catal. Today, 1997, 33: 279
-
[28]
24 Budi, P.; Curry-Hyde, E.; Howe, R. F. Catal. Lett., 1996, 41: 47
-
[29]
25 Rokosz, M. J.; Kucherov, A. V.; Jen, H.W.; Shelef, M. Catal. Today, 1997, 35: 65
-
[30]
26 Li, R. S.;Wen, R.W.; Zhang,W. Y.;Wei, Q. Chem. J. Chin. Unvi., 1993, 14: 545
-
[31]
[李荣生, 温瑞武, 张武阳, 魏诠. 高等学 校化学学报, 1993, 14: 545]
-
[32]
27 Ren, L. P.; Zhao, G. L.; Teng, J.W.;Wang, Y. D.; Xie, Z. K. Ind. Catal., 2007, 15: 30
-
[33]
[任丽萍, 赵国良, 滕加伟, 王仰东, 谢在库. 工业催化, 2007, 15: 30]
-
[34]
28 Wang, J.W.; Jin, G. Q.; Zhang, Z. X.;Wang, X. K. J. Chin. Rare Earth Soc., 2001, 19: 103
-
[35]
[王军威, 靳国强, 张志新, 王心葵. 中国稀土学报, 2001, 19: 103]
-
[36]
29 Li, M. H.; Yang, Y.;Wang, J. J. Dalian Inst. Light Ind., 2004, 23: 11
-
[37]
[李明慧, 杨毅, 王井. 大连轻工业学院学报, 2004, 23: 11]
-
[38]
30 Li, C. X.; Gao, Y. D.; Li, C. Y.; Shan, H. H.; Yang, C. H. J. Fuel Chem. Technol., 2006, 34: 47
-
[39]
[李成霞, 高永地, 李春义, 山红红, 杨朝合. 燃料化学学报, 2006, 34: 47]
-
[40]
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
-
[41]
[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]
-
[42]
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
-
[43]
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
-
[44]
[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]
-
[45]
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
-
[46]
35 Hartford, R.W.; Kojima, M.; O′ Connor, C. T. Ind. Eng. Chem. Res., 1989, 28: 1748
-
[47]
36 Tynj?l?, P.; Pakkanen, T. T. J. Mol. Catal. A-Chem., 1996, 110: 153
-
[48]
37 Ivanov, A. V.; Graham, G.W.; Shelef, M. Appl. Catal. BEnviron., 1999, 21: 243
-
[49]
38 Jiang, S.; Huang, S.; Qin, L.; Tu,W.; Zhu, J.; Tian, H.;Wang, P. J. Mol. Struc. Theochem., in press
-
[50]
39 Lee, C.; Yang,W.; Parr, R. G. Phys. Rev. B, 1988, 37: 785
-
[51]
40 Becke, A. D. Phys. Rev. A, 1988, 38: 3098
-
[52]
41 Frisch, M. J.; Trucks, G.W.; Schlegel, H. B.; et al. Gaussian 03. Revision D.01.Wallingford, CT: Gaussian Inc., 2004
-
[53]
42 Tajima, N.; Taketsugu, T.; Hirao, K. Chem. Phys., 1997, 218: 257
-
[54]
43 Krossner, M.; Sauer, J. J. Phys. Chem., 1996, 100: 6199
-
[55]
44 Olson, D. H.; Zygmunt, S. A.; Erhardt, M. K.; Curtiss, L. A.; Iton, L. E. Zeolites, 1997, 18: 347
-
[56]
45 Rice, M. J.; Chakraborty, A. K.; Bell, A. T. J. Phys. Chem. A, 1998, 102: 7498
-
[57]
46 Zygmunt, S. A.; Curtiss, L. A.; Iton, L. E.; Erhardt, M. K. J. Phys. Chem., 1996, 100: 6663
-
[58]
47 Zygmunt, S. A.; Curtiss, L. A.; Iton, L. E. J. Phys. Chem. B, 2001, 105: 3034
-
[59]
48 Ison, A.; rte, R. J. J. Catal., 1984, 89: 150
-
[1]
-
-
-
[1]
Hao XU , Ruopeng LI , Peixia YANG , Anmin LIU , Jie BAI . Regulation mechanism of halogen axial coordination atoms on the oxygen reduction activity of Fe-N4 site: A density functional theory study. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 695-701. doi: 10.11862/CJIC.20240302
-
[2]
Kaifu Zhang , Shan Gao , Bin Yang . Application of Theoretical Calculation with Fun Practice in Raman Spectroscopy Experimental Teaching. University Chemistry, 2025, 40(3): 62-67. doi: 10.12461/PKU.DXHX202404045
-
[3]
Jie ZHAO , Sen LIU , Qikang YIN , Xiaoqing LU , Zhaojie WANG . Theoretical calculation of selective adsorption and separation of CO2 by alkali metal modified naphthalene/naphthalenediyne. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 515-522. doi: 10.11862/CJIC.20230385
-
[4]
Jie ZHAO , Huili ZHANG , Xiaoqing LU , Zhaojie WANG . Theoretical calculations of CO2 capture and separation by functional groups modified 2D covalent organic framework. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 275-283. doi: 10.11862/CJIC.20240213
-
[5]
Pei Li , Yuenan Zheng , Zhankai Liu , An-Hui Lu . Boron-Containing MFI Zeolite: Microstructure Control and Its Performance of Propane Oxidative Dehydrogenation. Acta Physico-Chimica Sinica, 2025, 41(4): 100034-. doi: 10.3866/PKU.WHXB202406012
-
[6]
Xiaochen Zhang , Fei Yu , Jie Ma . 多角度数理模拟在电容去离子中的前沿应用. Acta Physico-Chimica Sinica, 2024, 40(11): 2311026-. doi: 10.3866/PKU.WHXB202311026
-
[7]
Weina Wang , Lixia Feng , Fengyi Liu , Wenliang Wang . Computational Chemistry Experiments in Facilitating the Study of Organic Reaction Mechanism: A Case Study of Electrophilic Addition of HCl to Asymmetric Alkenes. University Chemistry, 2025, 40(3): 206-214. doi: 10.12461/PKU.DXHX202407022
-
[8]
Meifeng Zhu , Jin Cheng , Kai Huang , Cheng Lian , Shouhong Xu , Honglai Liu . Classical Density Functional Theory for Understanding Electrochemical Interface. University Chemistry, 2025, 40(3): 148-152. doi: 10.12461/PKU.DXHX202405166
-
[9]
Shanghua Li , Malin Li , Xiwen Chi , Xin Yin , Zhaodi Luo , Jihong Yu . 基于高离子迁移动力学的取向ZnQ分子筛保护层实现高稳定水系锌金属负极的构筑. Acta Physico-Chimica Sinica, 2025, 41(1): 2309003-. doi: 10.3866/PKU.WHXB202309003
-
[10]
Xuyang Wang , Jiapei Zhang , Lirui Zhao , Xiaowen Xu , Guizheng Zou , Bin Zhang . Theoretical Study on the Structure and Stability of Copper-Ammonia Coordination Ions. University Chemistry, 2024, 39(3): 384-389. doi: 10.3866/PKU.DXHX202309065
-
[11]
Baitong Wei , Jinxin Guo , Xigong Liu , Rongxiu Zhu , Lei Liu . Theoretical Study on the Structure, Stability of Hydrocarbon Free Radicals and Selectivity of Alkane Chlorination Reaction. University Chemistry, 2025, 40(3): 402-407. doi: 10.12461/PKU.DXHX202406003
-
[12]
Yuhao SUN , Qingzhe DONG , Lei ZHAO , Xiaodan JIANG , Hailing GUO , Xianglong MENG , Yongmei GUO . Synthesis and antibacterial properties of silver-loaded sod-based zeolite. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 761-770. doi: 10.11862/CJIC.20230169
-
[13]
Jiali CHEN , Guoxiang ZHAO , Yayu YAN , Wanting XIA , Qiaohong LI , Jian ZHANG . Machine learning exploring the adsorption of electronic gases on zeolite molecular sieves. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 155-164. doi: 10.11862/CJIC.20240408
-
[14]
Yiping HUANG , Liqin TANG , Yufan JI , Cheng CHEN , Shuangtao LI , Jingjing HUANG , Xuechao GAO , Xuehong GU . Hollow fiber NaA zeolite membrane for deep dehydration of ethanol solvent by vapor permeation. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 225-234. doi: 10.11862/CJIC.20240224
-
[15]
Xuewei BA , Cheng CHENG , Huaikang ZHANG , Deqing ZHANG , Shuhua LI . Preparation and luminescent performance of Sr1-xZrSi2O7∶xDy3+ phosphor with high thermal stability. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 357-364. doi: 10.11862/CJIC.20240096
-
[16]
Shitao Fu , Jianming Zhang , Cancan Cao , Zhihui Wang , Chaoran Qin , Jian Zhang , Hui Xiong . Study on the Stability of Purple Cabbage Pigment. University Chemistry, 2024, 39(4): 367-372. doi: 10.3866/PKU.DXHX202401059
-
[17]
Maitri Bhattacharjee , Rekha Boruah Smriti , R. N. Dutta Purkayastha , Waldemar Maniukiewicz , Shubhamoy Chowdhury , Debasish Maiti , Tamanna Akhtar . Synthesis, structural characterization, bio-activity, and density functional theory calculation on Cu(Ⅱ) complexes with hydrazone-based Schiff base ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1409-1422. doi: 10.11862/CJIC.20240007
-
[18]
Yufang GAO , Nan HOU , Yaning LIANG , Ning LI , Yanting ZHANG , Zelong LI , Xiaofeng LI . Nano-thin layer MCM-22 zeolite: Synthesis and catalytic properties of trimethylbenzene isomerization reaction. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1079-1087. doi: 10.11862/CJIC.20240036
-
[19]
Junke LIU , Kungui ZHENG , Wenjing SUN , Gaoyang BAI , Guodong BAI , Zuwei YIN , Yao ZHOU , Juntao LI . Preparation of modified high-nickel layered cathode with LiAlO2/cyclopolyacrylonitrile dual-functional coating. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1461-1473. doi: 10.11862/CJIC.20240189
-
[20]
Xiaoning TANG , Junnan LIU , Xingfu YANG , Jie LEI , Qiuyang LUO , Shu XIA , An XUE . Effect of sodium alginate-sodium carboxymethylcellulose gel layer on the stability of Zn anodes. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1452-1460. doi: 10.11862/CJIC.20240191
-
[1]
Metrics
- PDF Downloads(1404)
- Abstract views(3819)
- HTML views(2)