Citation: LIU Peng, SHEN Jian. Preparation of ZSM-5-SBA-15 composite molecular sieves and its performance for toluene alkylation with methanol[J]. Journal of Fuel Chemistry and Technology, ;2015, 43(9): 1147-1152. shu

Preparation of ZSM-5-SBA-15 composite molecular sieves and its performance for toluene alkylation with methanol

LIU Peng ,
SHEN Jian ^,

1.
College of Petrochemical Engineering, Liaoning Shihua University, Fushun 113001, China

Corresponding author: SHEN Jian,
Received Date: 10 November 2014
Available Online: 13 January 2015

A series of ZSM-5-SBA-15 composite molecular sieves were prepared by post-synthesis method and characterized by XRD, FT-IR, BET, NH₃-TPD and pyridine infrared. The results indicated that ZSM-5-SBA-15 has both ZSM-5 microporous and SBA-15 mesoporous structure. The adsorption-desorption measurement using pyridine and ammonia demonstrated that acidity of SBA-15 was heightened because ZSM-5 was introduced into. Compared with ZSM-5, the acidic sites on ZSM-5-SBA-15 were still accessible. However, the strength of acidity was weakened. In the probe reaction of the alkylation of toluene and methanol, the ZSM-5-SBA-15 composite exhibited higher para-xylene selectivity in comparison to pristine ZSM-5.
- ZSM-5-SBA-15,
- ZSM-5,
- SBA-15,
- para-xylene,
- alkylation
1. [1]
  [1] 陈强, 王永睿, 孙敏, 慕旭宏, 舒兴田. IM-5和TNU-9分子筛在甲苯甲醇烷基化反应中的催化性能[J]. 石油学报(石油加工), 2010, 26(2): 165-170. (CHEN Qiang, WANG Yong-rui, SUN Min, MU Xu-hong, SHU Xing-tian. Catalytic performance of zeolites IM-5 and TNU-9 in toluene alkylation with methanol[J]. Acta Petrol Sin (Petrol Proc Sect), 2010, 26(2): 165-170.)
2. [2]
  [2] 陈俊文, 张超, 王永睿, 孙敏, 慕旭宏, 舒兴田. 改性IM-5分子筛在甲苯甲醇烷基化反应中的催化性能[J].石油学报(石油加工), 2013, 29(5): 757-766. (CHEN Jun-wen, ZHANG Chao, WANG Yong-rui, SUN Min, MU Xu-hong, SHU Xing-tian. Catalytic performance of modified IM-5 zeolite in alkylation of toluene with methanol[J]. Acta Petrol Sin (Petrol Proc Sect), 2013, 29(5): 757-766.)
3. [3]
  [3] 丁春华, 王祥生, 郭新闻. 氧化物改性MCM-22上甲苯与甲醇的烷基化性能研究[J]. 石油学报(石油加工), 2007, 23(5): 38-42. (DING Chun-hua, WANG Xiang-sheng, GUO Xin-wen. Study on alyklation of toluene with methanol over oxide-modified MCM-22 zeolite[J]. Acta Petrol Sin (Petrol Proc Sect), 2007, 23(5): 38-42.)
4. [4]
  [4] 丁春华, 王祥生, 郭新闻. 水热处理对MCM-22催化剂酸性、孔结构及甲苯/甲醇烷基化性能的影响[J]. 高等学校化学学报, 2007, 28(5): 922-927. (DING Chun-hua, WANG Xiang-sheng, GUO Xin-wen. Effect of hydrothermal treatment of MCM-22 catalyst on the acidity, pore structure and alkylation properties of toluene with methanol[J]. Chem J Chin Univ, 2007, 28(5): 922-927.)
5. [5]
  [5] 陈强, 王永睿, 孙敏, 慕旭宏, 舒兴田. NU88分子筛的合成、表征及在甲苯甲醇烷基化中的催化性能[J]. 石油学报(石油加工), 2010, 26(4): 493-498. (CHEN Qiang, WANG Yong-rui, SUN Min, MU Xu-hong, SHU Xing-tian. Synthesis, characterization of zeolite NU88, and its catalytic properties in toluene alkylation with methanol[J]. Acta Petrol Sin (Petro Proc Sect), 2010, 26(4): 493-498.)
6. [6]
  [6] MIRTH G, CEJKA J, LERCHER J A. Transport and isomerization of xylenes over HZSM-5 zeolites[J]. J Catal, 1993, 139(1): 24-33.
7. [7]
  [7] MIRTH G, LERCHER J A. On the role of product isomerization for shape selective toluene methylation over HZSM5[J]. J Catal, 1994, 147(1): 199-206.
8. [8]
  [8] CEJKA J, ZILKOVA N, WICHTERLOVA B, ELDER-MIRTH G, LERCHER J A. Decisive role of transport rate of products for zeolite para-selectivity: Effect of coke deposition and external surface silylation on activity and selectivity of HZSM-5 in alkylation of toluene[J]. Zeolites, 1996, 17(3): 265-271.
9. [9]
  [9] 刘晔, 刘月明, 王勇, 吴海虹, 吴鹏. ZSM-5的组成和粒径对甲苯甲醇烷基化反应的影响[C].中国化工学会学术年会论文集, 2008. (LIU Ye, LIU Yue-ming, WANG Yong, WU Hai-hong, WU Peng. Effect of composition and grain size of ZSM-5 in toluene alkylation with methanol. Acad Ann Meet Coll CIESC, 2008.)
10. [10]
  [10] 张立东, 高俊华, 胡津仙, 李文怀, 王建国. Fe/ZSM-5的制备及其催化甲苯/甲醇烷基化反应行为[J]. 化工进展, 2009, 28(8): 1360-1364. (ZHANG Li-dong, GAO Jun-hua, HU Jin-xian, LI Wen-huai, WANG Jian-guo. Preparation of Fe/ZSM-5 and catalytic behavior for touene alkylation with methanol[J]. Chem Ind Eng Prog, 2009, 28(8): 1360-1364.)
11. [11]
  [11] 丁春华, 王祥生, 郭新闻. 水对改性ZSM-5催化剂上甲苯/甲醇烷基化性能的影响[J]. 分子催化, 2007, 21(8): 77-78. (DING Chun-hua, WANG Xiang-sheng, GUO Xin-wen. Effect of alyklation of toluene with methanol over water-modified ZSM-5 catalyst[J]. J Mol Catal (China), 2007, 21(8): 77-78.)
12. [12]
  [12] CEJKA J, KREJCI A, ZILKOVA N, KOTRLA J, ERNST S, WEBER A. Alkaline modification of MCM-22 to a 3D interconnected pore system and its application in toluene disproportionation and alkylation[J]. Microporous Mesoporous Mater, 2002, 53(1/3): 121-133.
13. [13]
  [13] KAEDING W W, CHU C, YOUNG L B. Selective alkylation of toluene with methanol to produce para-xylene[J]. J Catal, 1981, 67(1): 159-174.
14. [14]
  [14] HALGERI A B, DAS J. Recent advances in selectivation of zeolites for para-disubstituted aromatics[J]. Catal Today, 2002, 73(1/2): 65-73.
15. [15]
  [15] ZHU Z, XIE Z, CHEN Q, KONG D, LI W, YANG W. Chemical liquid deposition with polysiloxane of ZSM-5 and its effect on acidity and catalytic properties[J]. Microporous Mesoporous Mater, 2007, 101(1/2): 169-175.
16. [16]
  [16] HALGERI A B, DAS J. Recent advances in selectivation of zeolites for para-disubstituted aromatics[J]. Catal Today, 2002, 73(1/2): 65-73.
17. [17]
  [17] BAUER F, CHEN W H, BILZ E, FREYER A, SAUERLAND V, LIU S B. Surface modification of nano-sized HZSM-5 and HFER by pre-coking and silanization[J]. J Catal, 2007, 251(2): 258-270.
18. [18]
  [18] 纪永军, 张斌, 张坤, 徐乐, 彭洪根, 吴鹏. ZSM-5@mesosilica silica核壳复合结构分子筛的制备及其甲苯甲醇烷基化择形催化性能的研究[J]. 化学学报, 2013, 71(3): 371-380. (JI Yong-jun, ZHANG Bin, ZHANG Kun, XU Le, PENG Hong-gen, WU Peng. Core/shell-structured ZSM-5@mesosilica silica composites for shape-selective alkylation of toluene with methanol[J]. Acta Chim Sin, 2013, 71(3): 371-380.)
19. [19]
  [19] 王政, 陈娟, 王林, 马清祥, 赵天生. MFI型核壳分子筛在甲苯甲醇烷基化反应中的催化性能[J]. 石油学报(石油加工), 2011, 27(5): 812-816. (WANG Zheng, CHEN Juan, WANG Lin, MA Qing-xiang, ZHAO Tian-sheng. Catalytic activity of MFI type core-shell zeolite for alkylation of toluene with methanol[J]. Acta Petrol Sin (Petrol Proc Sect), 2011, 27(5): 812-816.)
20. [20]
  [20] 许峰, 顾建峰, 关乃佳, 袁忠勇. Mg改性ZSM-5/AlPO₄-5复合分子筛用于甲苯甲醇侧链烷基化反应[J]. 石油学报(石油加工), 2008, 24(z1): 346-349. (XU Feng, GU Jian-feng, GUAN Nai-jia, YUAN Zhong-yong. Magnesium modified ZSM-5/ALPO₄-5 composite zeolite for side-chain alkylation of toluene with methanol[J]. Acta Petrol Sin (Petrol Proc Sect), 2008, 24(zl): 346-349.)
21. [21]
  [21] 贾银娟, 刘志成, 高焕新. ZSM-5/silicalite-1核壳分子筛的合成与择形催化性能[J]. 化学反应工程与工艺, 2012, 28(6): 519-524. (JIA Yin-juan, LIU Zhi-cheng, GAO Huan-xin. Synthesis and shape-selective properties of core/shell-structured ZSM-5/ silicalite-1[J]. Chem React Eng Technol, 2012, 28(6): 519-524.)
22. [22]
  [22] LEONOWICZ M E, LAWTON J A, LAWTON S L. MCM-22: A molecular sieve with two independent sieve multidimensional channel systems[J]. Science, 1994, 264(5167): 1910-1913.
23. [23]
  [23] SERRANO D P, AGUADO J, ESCOLA J M. Catalytic properties in polyolefin cracking of hierarchical nanocrystalline HZSM-5 samples prepared according to different strategies[J]. J Catal, 2010, 276(1): 152-160.
24. [24]
  [24] 陈娟, 王燕, 魏慧丽, 马清祥, 王政, 赵天生. HZSM-5/silicalite-1复合分子筛的甲苯甲醇烷基化反应的催化性能[J]. 天然气化工, 2009, 34(6): 22-25. (CHEN Juan, WANG Yan, WEI Hui-li, MA Qing-xiang, WANG Zheng, ZHAO Tian-sheng. Selective alkylation of toluene catalyzed by HZSM-5/silicalite-1 composite[J]. Nat Gas Chem Ind, 2009, 34(6): 22-25.)
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