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 |
DOI号: |
分类号: TQ028. 8 |
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. |
基金项目: |
作者简介: |
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. |
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