Controlling Crystal Transformation between Zeolite ZSM-5 and Mordenite without Organic Structure-Directing Agent

doi:10.1016/S1872-2067(11)60400-2

Abstract

Abstract: Zeolite crystals were synthesized at a lower temperature (150 °C) by adding a nucleation solution prepared at higher temperature (190 °C) to the mother solution. The effects of the Na₂O/SiO₂ ratio, nucleation time of the nucleation solution, and the ratio of Na₂O/SiO₂ ratio in the mother solution on crystal transformation between ZSM-5 and mordenite were investigated. The transformation between zeolite ZSM-5 and mordenite could be controlled effectively by changing the overall Na₂O/SiO₂ ratio in the overall solution. A Na₂O/SiO₂ ratio of 0.18 formed a boundary between ZSM-5 and mordenite phases when the overall solution had a composition of xNa₂O:100SiO₂:2.5Al₂O₃: 12SO₄^2-:4000H₂O. When the Na₂O/SiO₂ ratio was increased higher than 0.18 by altering the composition of the mother solution, the ZSM-5 product formed by nucleation at higher temperature (190 °C) could be transformed into mordenite crystals during crystallization at lower temperature (150 °C). When the Na2O/SiO2 ratio was ≤ 0.18, a product containing both ZSM-5 and mordenite crystals was obtained during nucleation at higher temperature that could be transformed into ZSM-5 crystals during crystallization at lower temperature. A precondition for crystal transformation between ZSM-5 and mordenite was that the crystallinity of the product formed during nucleation at higher temperature must be ≤ 30%.

Key words: ZSM-5 zeolite, template-free, mordenite, crystal transformation, controlling

HUANG Xian-Liang, ZHANG Rong-Rong, WANG Zheng-Bao. Controlling Crystal Transformation between Zeolite ZSM-5 and Mordenite without Organic Structure-Directing Agent[J]. Chinese Journal of Catalysis, 2012, 33(8): 1290-1298.

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References

1 Argauer R J, Landolt G R. US 3 702 886. 1972
2 Uguina M A, Delucas A, Ruiz F, Serrano D P. Ind Eng Chem Res, 1995, 34: 451
3 Kim S D, Noh S H, Park J W, Kim W J. Microporous Mesoporous Mater, 2006, 92: 181
4 王德举, 李学礼, 刘仲能, 谢在库. 工业催化 (Wang D J, Li X L, Liu Zh N, Xie Z K. Ind Catal), 2008, 16(4): 19
5 Pan H H, Pan Q X, Zhao Y S, Luo Y B, Shu X T, He M Y. Ind Eng Chem Res, 2010, 49: 7294
6 Ren N, Broni? J, Suboti? B, Lv X C, Yang Z J, Tang Y. Microporous Mesoporous Mater, 2011, 139: 197
7 Trianta C S, Vlessidis A G, Nalbandian L, Evmiridis N P. Microporous Mesoporous Mater, 2001, 47: 369
8 Ali M A, Brisdon B, Thomas W J. Appl Catal A, 2003, 252: 149
9 Tosheva L, Valtchev V P. Chem Mater, 2005, 17: 2494
10 Kordatos K, Gavela S, Ntziouni A, Pistiolas K N, Kyritsi A, Kasselouri-Rigopoulou V. Microporous Mesoporous Mater, 2008, 115: 189
11 吴健, 王瑜, 黄峰, 杨阳, 孟长功. 物理化学学报 (Wu J, Wang Y, Huang F, Yang Y, Meng Ch G. Acta Phys-Chim Sin), 2010, 26: 1705
12 Rownaghi A A, Hedlund J. Ind Eng Chem Res, 2011, 50: 11872
13 刘百军, 曾贤君. 物理化学学报 (Liu B J, Zeng X J. Acta Phys-Chim Sin), 2009, 25: 2055
14 于素霞, 杨建华, 初乃波, 李刚, 鲁金明, 王金渠. 催化学报 (Yu S X, Yang J H, Chu N B, Li G, Lu J M, Wang J Q. Chin J Catal), 2009, 30: 1035
15 杨建华, 于素霞, 胡慧晔, 初乃波, 鲁金明, 殷德宏, 王金渠. 催化学报 (Yang J H, Yu S X, Hu H Y, Chu N B, Lu J M, Yin D H, Wang J Q. Chin J Catal), 2011, 32: 362
16 Grose R W, Flanigen E M. US 4 257 885. 1981
17 Shiralkar V P, Clearfield A. Zeolites, 1989, 9: 363

图 7 不同 Na2O:SiO2 比 E 系列样品的 SEM 照片
Fig. 7. SEM images of samples of series E with different Na2O/SiO2 ratios. Crystallization conditions: 190 oC, 24 h.
18 Pradhan A R, Viswanadham N, Suresh S, Gupta O P, Ray N, Muralidhar G, Shanker U, Rao T S R P. Catal Lett, 1994, 28: 231
19 Machado F J, Lopez C M, Centeno M A, Urbina C. Appl Catal A, 1999, 181: 29
20 Kim S D, Noh S H, Seong K H, Kim W J. Microporous Mesoporous Mater, 2004, 72: 185
21 Han W, Jia Y X, Xiong G X, Yang W S. Sci Technol Adv Mater, 2007, 8: 101
22 Cheng Y, Liao R H, Li J S, Sun X Y, Wang L J. J Mater Process Technol, 2008, 206: 445
23 黄先亮, 王正宝. 催化学报 (Huang X L, Wang Z B, Chin J Catal), 2011, 32: 1702
24 Ren N, Broni? J, Suboti? B, Song Y M, Lv X C, Tang Y. Microporous Mesoporous Mater, 2012, 147: 229
25 刘百军, 曾贤君, 王辉, 黄永, 汪梅. 物理化学学报 (Liu B J, Zeng X J, Wang H, Huang Y, Wang M. Acta Phys Chim Sin), 2007, 23:503
26 彭建彪, 谢素娟, 王清遐, 徐龙伢. 催化学报(Peng J B, Xie S J, Wang Q X, Xu L Y. Chin J Catal), 2002, 23: 363

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