蒸汽相转化涂晶法SAPO-34分子筛膜的制备及表征

doi:10.15541/jim20140487

无机材料学报 ›› 2015, Vol. 30 ›› Issue (3): 294-298.DOI: 10.15541/jim20140487

蒸汽相转化涂晶法SAPO-34分子筛膜的制备及表征

周亮, 杨建华, 王金渠, 鲁金明, 张艳, 殷德宏

(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, 大连116024)

收稿日期:2014-09-23 修回日期:2014-11-03 出版日期:2015-03-20 网络出版日期:2015-03-06
作者简介:周亮(1986–), 女, 博士研究生. E-mail: zhouliang5851@163.com
基金资助:
国家自然科学基金(21076029) Natural Science Foundation of China (21076029)

Synthesis of SAPO-34 Molecular Sieve Membranes by Steam-assisted Conversion Seeding and Their Characterization

ZHOU Liang, YANG Jian-Hua, WANG Jin-Qu, LU Jin-Ming, ZHANG Yan, YIN De-Hong

(Institute of Adsorption and Inorganic Membrane, State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116024, China)

Received:2014-09-23 Revised:2014-11-03 Published:2015-03-20 Online:2015-03-06
About author:ZHOU Liang. E-mail: zhouliang5851@163.com

摘要/Abstract

摘要：

采用一种新型涂晶方法即蒸汽相转化涂晶法, 在廉价大孔α-Al₂O₃载体上水热合成制备高质量的SAPO-34分子筛膜。该方法能够有效修复α-Al₂O₃载体的大孔缺陷, 通过制备平整均匀的晶种层, 最终得到了连续并且无明显“针孔”缺陷的SAPO-34膜。实验考察了浆料中添加尺寸分别为2 μm、1 μm、500 nm及100 nm的晶种对形成晶种层及分子筛膜的影响, 并将制备的分子筛膜用于渗透汽化异丙醇脱水实验。在75℃下对90wt%的异丙醇/水混合物具有优良的分离性能, 其通量和分离系数分别为1.396 kg/(m²·h)和973。

关键词: SAPO-34膜, 大孔载体, 蒸汽相转化涂晶, 渗透汽化

Abstract:

A new seeding method, the steam-assisted conversion seeding, was used to prepare the high-quality SAPO-34 molecular sieve membranes by secondary growth method on the low cost macroporous α-Al₂O₃ supports. The seeds with different sizes of 2 μm, 1 μm, 500 nm, and 100 nm were mixed in the synthesis solution to prepare the seeds-containing pastes which was coated on the surface of the support. The effects of the particle size on the paste layers, seed layers and membranes were investigated. A perfect seed layer was formed and effectively modified the defects of the macroporous α-Al₂O₃ support and then, induced a continuous, compact and unconspicuousl pinholes SAPO-34 membrane. The SAPO-34 membrane displayed high performance in the pervaporation dehydration of 90wt% IPA/water mixtures at 348 K, showing water ?ux up to 1.396 kg/(m²·h) and separation factor at 973.

Key words: SAPO-34 membrane, macroporous support, steam-assisted conversion, pervaporation performance

中图分类号:

O614

周亮, 杨建华, 王金渠, 鲁金明, 张艳, 殷德宏. 蒸汽相转化涂晶法SAPO-34分子筛膜的制备及表征[J]. 无机材料学报, 2015, 30(3): 294-298.

ZHOU Liang, YANG Jian-Hua, WANG Jin-Qu, LU Jin-Ming, ZHANG Yan, YIN De-Hong. Synthesis of SAPO-34 Molecular Sieve Membranes by Steam-assisted Conversion Seeding and Their Characterization[J]. Journal of Inorganic Materials, 2015, 30(3): 294-298.

图/表 6

表1 不同大小晶种浆料所制备的SAPO-34膜

Table 1 SAPO-34 membranes prepared from paste composed of various sizes of seeds

Membrane	Seed layer				Membrane
Membrane	Seed layer	Seed size/μm	SAC temperature/K	SAC time/h	Synthesis temperature/K	Synthesis time/h
M1	S1	2.0	473	24	473	24
M2	S2	1.0	473	24	473	24
M3	S3	0.5	473	24	473	24
M4	S4	0.1	473	24	473	24

图1 α-Al2O3载体及涂不同尺寸晶种浆料后的扫描电镜照片

Fig. 1 SEM images of the α-Al2O3 support (a, b) and the paste layer with different sizes of seeds (2 μm (c, d), 1 μm (e, f), 0.5 μm (g, h) and 0.1 μm (i, j)) on the supports

图2 晶种层S1~ S4的扫描电镜照片

Fig. 2 SEM images of seed layers of S1 (a, b), S2 (c, d), S3 (e, f), and S4 (g, h)

图3 膜M1~M4的XRD图谱

Fig. 3 XRD patterns of membranes M1-M4

表2 膜M1~M4在75℃下的PV结果

Table 2 PV performances of membranes M1-M4 at 75℃

Membrane	Water/IPA (10/90 w/w)
Membrane	Flux/ (kg·m^-2·h^-1)	α_W/IPA
M1	0.624	1093
M2	0.587	1122
M3	1.396	973
M4	2.785	34

图4 膜M1~M4的扫描电镜照片

Fig. 4 SEM images of membranes of M1(a, b), M2(c, d), M3 (e, f), and M4 (g, h)

参考文献 13

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蒸汽相转化涂晶法SAPO-34分子筛膜的制备及表征

Synthesis of SAPO-34 Molecular Sieve Membranes by Steam-assisted Conversion Seeding and Their Characterization

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