膜科学与技术

液相氧化-低温煅烧脱除Silicalite-1膜模板剂及其性能研究

作者：沈东，杨建华，肖伟，李田生，鲁金明，王金渠

单位：大连理工大学精细化工国家重点实验室吸附与无机膜研究所

关键词： Silicalite-1沸石膜；液相氧化；渗透蒸发；气体渗透

出版年,卷(期):页码： 2011,31(1):61-65

摘要：

采用原位生长法在管状大孔α-Al2O3载体外表面上合成致密连续Silicalite-1沸石膜，利用双氧水和稀硝酸混合液液相氧化-低温煅烧方法脱除Silicalite-1沸石膜的模板剂，并用扫描电镜(SEM)、气体渗透测试，渗透蒸发（PV）等表征手段对沸石膜的性能进行评价。结果表明所制备的Silicalite-1膜表面晶粒交互生长，致密，连续，膜的厚度约为10 μm。在293 K，0.1 MPa 压差条件下，N2的渗透速率为8.16×10-7 mol/(m2•s•Pa)，N2/i-C4H10理想分离系数为达到425，428 K下CO2/N2的理想分离系数为2.89。在333 K下，渗透蒸发分离5% wt乙醇/水混合液，乙醇/水的分离系数αA/W达到40.3，通量J为0.83kg/(m2•h)。

Silicalite-1 zeolite membrane was prepared on macro porous α-Al2O3 support by in-situ crystallization method. Liquid phase oxidation and low-temperature calcination method was used to remove template molecules from Silicalite-1 membrane, which replaced the conventional high temperature calcination method. SEM, single gas permeation and pervaporation (PV) performance tests as a function of temperature were used to characterize the as-synthesized zeolite membrane. The results showed that the prepared membrane was typical Silicalite-1, continuous, dense and no obvious defects. The permeance of N2 is 8.16×10-7 mol/(m2•s•Pa) and the ideal selectivity of N2/i-C4H10 was up to 425 at 293 K and ideal selectivity of CO2/N2 was 2.89 at 428 K. The fluxes of Silicalite-1 membrane at 333 K is 0.83 kg/(m2•h) towards ethanol/H2O mixtures, and the corresponding separation factors was 40.3.

沈东(1981 - )，男，河北保定人，在读硕士，电话：13940908256，从事Silicalite-1沸石膜的制备、表征及其应用研究。

参考文献：

[1] Feng X, Huang R Y M. Liquid separation by membrane pervaporation: a review. [J].Ind Eng Chem Res, 1997, 36: 1048–1066.
[2] Coronas J, Santamaria J. Separations using zeolite membranes. [J].Sep Purif Meth, 1999, 28: 127–177.
[3] Tavolaro A, Drioli E. Zeolite membranes. [J]. Adv Mater, 1999, 11: 975–996.
[4] Tsuru T. Inorganic porous membrane for liquid phase separation. [J]. Sep Purif Meth, 2001, 30: 191–220。
[5] Julbe A, Farrusseng D, Guizard C. Porous ceramic membranes for catalytic reactors-overview and new ideas. [J]. J Membr Sci , 2001, 181: 3–20.
[6] Chen H L, Li Y S, Yang W S. Preparation of silicalite-1 membrane by solution-filling method and its alcohol extraction properties. [J]. J Memb Sci, 2007, 296: 122–130
[7] Morigami Y, Kondo M, Abe J. The first large-scale pervaporation plant using tubular-type module with zeolite NaA membrane. [J]. Sep Purif Technol, 2001, 25: 251–260.
[8] Wan C W, Ariso C T, Yeung K L. Effects of synthesis parameters on the zeolite membrane growth. [J].J Memb Sci, 2001, 191: 143–163
[9] Pachtova O, Kocirik M, Zikanova A, et al. A comparative study of template removal from silicalite-1 crystals in pyrolytic and oxidizing regimes. [J]. Micropor Mesopor Mater, 2002, 55: 285–296.
[10] Geus E R, Bekkum H van. Calcination of large MFI-type single crystals 2.crack formation and thermomechanical properties in view of the preparation of zeolite membranes. [J]. Zeolites, 1995, 15: 333–341.
[11] Henga S, Laua P P S, Yeung K L, et al. Low-temperature ozone treatment for organic template removal from zeolite membrane. [J]. J Memb Sci, 2004, 243: 69–78
[12] Teruoki T,Yuta N, Ayaka K, Takao Masuda. Preparation of hydrophilic silicalite-1 nanocrystal-layered membranes and their application to separating water from water–acetone solution. [J]. Micropor Mesopor Mater, 2008, 115: 176–183
[13] 徐如人,庞文琴. 分子筛与多孔材料化学[M] .北京: 科学出版社, 2004 : 3.
[14] Wridzer J W Bakker, Leo J P van den Broeke, Freek K, et al. Temperature Dependence of One-Component Permeation through a Silicalite-I Membrane. [J]. AIChE Journal, 1997, 43: 2203-2214
[15] Masuda T, Otani S, Tsuji T, et al. Preparation of hydrophilic and acid-proof silicalite-1 zeolite membrane and its application to selective separation of water from water solutions of concentrated acetic acid by pervaporation. [J]. Sep Purif Technol, 2003, 32: 181-189.
[16] Zhao QY Wang JQ, Chu N B et al. Preparation of high-permeance MFI membrane with the modified secondary growth method on the macroporous α-alumina tubular support.[J]. J Membr Sci, 2008, 320: 303–309.
[17] Noack M, Kölsch P, Schäfer R et al. Molecular Sieve Membranes for Industrial Application: Problems, Progress, Solutions. [J]. Chem Eng Technol, 2002, 25 (3): 221-230.

服务与反馈：

【文章下载】【加入收藏】

《膜科学与技术》编辑部地址：北京市朝阳区北三环东路19号蓝星大厦邮政编码：100029 电话：010-64426130/64433466 传真：010-80485372邮箱：mkxyjs@163.com