气相转移法制备多孔双相沸石复合物

doi:10.15541/jim20130667

无机材料学报 ›› 2014, Vol. 29 ›› Issue (9): 985-990.DOI: 10.15541/jim20130667 CSTR: 32189.14.10.15541/jim20130667

气相转移法制备多孔双相沸石复合物

张球, 谭薇, 郑家军, 赵强强, 王广帅, 易玉明, 李瑞丰

(太原理工大学能源化工与催化研究中心, 太原 030024)

收稿日期:2013-12-17 修回日期:2014-02-28 出版日期:2014-09-17 网络出版日期:2014-08-21
作者简介:张球(1985–), 男, 硕士研究生. E-mail: 13623628237@163.com
基金资助:
国家自然科学基金(21371129, 21376157, 21246003);“十二五”国家科技支撑计划项目子课题(SQ2011GX04E 05929);中国石油化工股份有限公司(111110);山西省自然科学基金(2012011005-4);National Natural Science Foundation of China (21371129, 21376157, 21246003);Key Projects in the National Science & Technology Pillar Program during the Twelfth Five-Year Plan Period (SQ2011GX04E05929);SinoPEC (111110);Natural Science Foundation of Shanxi Province (2012011005-4)

Hierachical Zeolite-Zeolite Composite Prepared by a Vapor Phase Transport Method

ZHANG Qiu, Tan Wei, ZHENG Jia-Jun, ZHAO Qiang-Qiang, WANG Guang-Shuai, YI Yu-Ming, LI Rui-Feng

(Research Centre of Energy Chemical & Catalytic Technology, Taiyuan University of Technology, Taiyuan 030024, China)

Received:2013-12-17 Revised:2014-02-28 Published:2014-09-17 Online:2014-08-21
About author:ZHANG Qiu. E-mail: 13623628237@163.com

摘要/Abstract

摘要：

采用气相转移法制备了同时含有Y和ZSM-5沸石的双相沸石复合物。采用X射线衍射仪(XRD)、扫描电子显微镜(SEM)、N₂吸附-脱附和骨架红外(FT-IR)等手段对合成的样品进行了表征。结果表明, 合成的样品受Y型沸石的添加量、干胶制备条件和气相转移法转化条件的影响; 水热预处理后的ZSM-5沸石前驱体中具有ZSM-5沸石的骨架特征振动峰, 归结于ZSM-5沸石晶核或微晶的形成, 这有利于在气相转移法转化过程中引导或促使体系向ZSM-5沸石相的转变, 并有利于抑制ZSM-35杂晶的形成; Y型沸石在蒸汽处理过程中的脱铝过程导致合成的沸石复合物具有介孔结构。

关键词: 气相转移法, 多级孔, 沸石复合物, ZSM-5, Y

Abstract:

A zeolite-zeolite composite composed of Y and ZSM-5 was successfully prepared by a vapor phase transport (VPT) method. The as-synthesized samples were characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), N₂ adsorption-desorption and FT-IR. The results display that the synthesis is influenced by the Y content, preparing condition of dry gel and transfering condition for VPT method. FT-IR spectra show the characteristic peaks of MFI framework on ZSM-5 precursor after hydrothermal pre-treatment for 16 h. The result can be attributed to the crystal nucleus or microcrystal of ZSM-5 zeolite, either of which may promote growth of ZSM-5 crystals during the VPT procedure, and depresse formation of ZSM-35 crystals. The mesopores structure, created in as-synthesized zeolite-zeolite composite, can be ascribed to the extracted aluminum from Y zeolite crystals by VPT procedure.

Key words: vapor phase transport method, hierachical pores, zeolite-zeolite composite, ZSM-5, Y

中图分类号:

TQ426

张球, 谭薇, 郑家军, 赵强强, 王广帅, 易玉明, 李瑞丰. 气相转移法制备多孔双相沸石复合物[J]. 无机材料学报, 2014, 29(9): 985-990.

ZHANG Qiu, Tan Wei, ZHENG Jia-Jun, ZHAO Qiang-Qiang, WANG Guang-Shuai, YI Yu-Ming, LI Rui-Feng. Hierachical Zeolite-Zeolite Composite Prepared by a Vapor Phase Transport Method[J]. Journal of Inorganic Materials, 2014, 29(9): 985-990.

图/表 7

图1 样品的XRD图谱

Fig. 1 XRD patterns of the reference ZSM-5/Y-r (a), Y (b), ZSM-5 transferred from dry-gel without Y zeolite by the vapor phase transport method (c), as-synthesized zeolite-zeolite composite ZSM-5/Y (d), ZSM-5 precursor pre-treated hydrothermally for 16 h (e)

图2 样品的FT-IR图谱

Fig. 2 FT-IR spectra of samples of ZSM-5/Y (a), ZSM-5 (b) and Y (c)

图3 样品的扫描电镜照片

Fig. 3 SEM images of samples of pure ZSM-5 (a), pure Y (b) and ZSM-5/Y (c)

图4 ZSM-5/Y和Y+ZSM-5的N2吸附-脱附等温线及ZSM-5/Y孔径分布图(插图)

Fig. 4 N2adsorption-desorption isotherm of ZSM-5/Y, Y+ ZSM-5 and pore size distribution curve of ZSM-5/Y (inset)

图5 烘干温度的影响

Fig. 5 Effect of drying temperature (a) XRD patterns of zeolite-zeolite composite ZSM-5/Y transferred by a vapor phase method from dry-gel dried at different temperatures; (b) FT-IR spectra of dry-gel dried at (1) 60℃ and (2) 90℃

图6 Y不同添加量时所合成样品的XRD图谱

Fig. 6 XRD patterns of as-synthesized samples with different Y contents

图7 不同晶化时间下沸石复合物的XRD图谱

Fig. 7 XRD patterns of zeolite-zeolite composite with different crystallizing time

参考文献 24

[1]	DZIKH I P, LOPES J M, LEMOS F, et al. Temperature dependence of the USHY+HZSM-5 mixing effect on the n-heptane transfor-mation. Catal. Today, 2001, 65(2/3/4): 143-148.
[2]	CHEN H L, SHEN B J, PAN H F. In situ formation of ZSM-5 in NaY gel and characterization of ZSM-5/Y composite zeolite. Chem. Lett., 2003, 32(8): 726-727.
[3]	CHEN H L, SHEN B J, PAN H F. Physicochemical and catalytic properties of ZSM-5/Y composite zeolites dealuminated by the steaming. Acta Phy.-Chim. Sin., 2004, 20(8): 854-859.
[4]	JIA W, GUO Q, CUI X J, et al. Synthesis of Y-ZSM-5 composite molecular sieve with ethylenediamine as template. Petrochemical Technology, 2006, 35(9): 832-836.
[5]	GUO D L, ZHENG J J, YI Y M, et al. Synthesis and characterization of FMZ bi-phases composite zeolites. Acta Petrolei Sinica (Petroleum Processing Section), 2013, 29(4): 591-596.
[6]	ZHENG J J, YI Y M, WANG W L, et al. Synthesis of bi-phases composite zeolites MFZ and its hierarchical effects in isopropylbenzene catalytic cracking. Micropor. Mesopor. Mater., 2013, 171: 44-52.
[7]	GUO W P, HUANG L M, DENG P, et al. Characterization of β/MCM-41 composite molecular sieve compared with the mechanical mixture. Micropor. Mesopor. Mater., 2001, 44-45: 427-434.
[8]	KARLSSON A, STOCKER M, SCHMIDT R. Composites of micro- and mesoporous materials: simultaneous syntheses of FI/MCM-41 like phases by a mixed template approach. Micropor. Mesopor. Mater., 1999, 27(2/3): 181-192.
[9]	LIU H T, BAO X J, WEI W S, et al. Synthesis and characterization of kaolin/NaY/MCM-41 composites. Micropor. Mesopor. Mater., 2003, 66(1): 117-125.
[10]	GOTO Y, FUKUSHIMA Y, OGURA M, et al. Mesoporous material from zeolite. J. Porous Mater., 2002, 9(1): 43-48.
[11]	RAJA H P R P, CHRISTOPHER C L. Synthesis, characterization, and catalytic properties of a microporous/mesoporous material, MMM-1. J. Solid State Chem., 2002, 167(2): 363-369.
[12]	XU W Y, DONG J X, LI J P, et al. A novel method for the preparation of zeolite ZSM-5. J. Chem. Soc., Chem. Commun., 1990, 755-756.
[13]	MOLLER K, YILMAZ B, JACUBINAS R M, et al. One-step synthesis of hierarchical zeolite β via network formation of uniform nanocrystals. J. Am. Chem. Soc., 2011, 133(14): 5284-5295.
[14]	ZHANG Q, LI C Y, SHAN H H, et al. Comparison of core/shell binary structure zeolite ZSM-5/SAPO-5 synthesized by vapor- phase transport and hydrothermal synthesis. Chin. J. Catal., 2007, 28(6): 541-546.
[15]	ZHANG Q, LI C Y, SHAN H H, et al. ZSM-5/SAPO-5 composite molecular sieves synthesized by vapor-phase transport technique. Chem. J. Chinese U., 2007, 28(11): 2030-2034.
[16]	ZHENG J J, ZHANG X W, ZHANG Y, et al. Structural effects of hierarchical pores in zeolite composite. Micropor. Mesopor. Mater., 2009, 122(1/2/3): 264-269.
[17]	ZHENG J J, MA J H, WANG Y, et al. Synthesis and catalytic property of a zeolite composite for preparation of dimethyl ether from methanol dehydration. Catal. Lett., 2009, 130(3/4): 672-678.
[18]	ZHENG J J, ZENG Q H, MA J H, et al. Synthesis of hollow zeolite composite spheres by using β-zeolite crystal as template. Chem. Lett., 2010, 39(4): 330-331.
[19]	ZHENG J J, ZENG Q H, ZHANG Y Y, et al. Hierarchical porous zeolite composite with a core-shell structure fabricated using β-zeolite crystals as nutrients as well as cores. Chem. Mater., 2010, 22(22): 6065-6074.
[20]	FLANIGEN E M, KHATAMI H, SZYMANSKI H. Molecular sieve Zeolites-I (Infrared Structural Studies of Zeolite Frameworks). Advances in Chemistry. Washington, DC, 1974: 201-229.
[21]	GROEN J C, BACH T, ZIESE U, et al. Creation of hollow zeolite architectures by controlled desilication of Al-Zoned ZSM-5 crystals. J. Am. Chem. Soc., 2005, 127(31): 10792-10793.
[22]	GROEN J C, ZHU W D, BROUWER S, et al. Direct demonstration of enhanced diffusion in mesoporous ZSM-5 zeolite obtained via controlled desilication. J. Am. Chem. Soc., 2007, 129(2): 355-360.
[23]	VAN DONK S, JANSSEN A H, BITTER J H, et al. Generation, characterization, and impact of mesopores in zeolite catalysts. Catal. Rev., 2003, 45(2): 297-319.
[24]	JUNG J S, PARK J W, SEO G. Catalytic cracking of n-octane over alkli-treated MFI zeolites. Appl. Catal. A-Gen., 2005, 288(1/2): 149-157.

气相转移法制备多孔双相沸石复合物

Hierachical Zeolite-Zeolite Composite Prepared by a Vapor Phase Transport Method

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