Silicalite-1分子筛膜渗透蒸发条件的响应面分析与优化

doi:10.16085/j.issn.1000-6613.2022-1345

摘要/Abstract

摘要：

采用Silicalite-1分子筛膜用于低浓度乙醇/水溶液的渗透蒸发分离，运用单因素实验考察了晶种质量分数、晶化温度、晶化时间3个制备条件对Silicalite-1分子筛膜渗透蒸发分离性能的影响，借助响应面分析（RSM）研究了料液温度、乙醇质量分数、真空压力3个运行条件对分离系数和渗透通量的影响。单因素实验结果表明，在晶种质量分数为0.3%、晶化温度为175℃、晶化时间为7h条件下制备的Silicalite-1分子筛膜对乙醇/水的渗透蒸发分离效果较好。RSM结果表明，料液温度、料液配比、真空压力对分离系数和渗透通量的影响显著，根据RSM建立多项式模型并对该模型预测的最佳条件进行了实验验证，实验结果与模型预测较为吻合。在进料温度为70℃、乙醇质量分数为3.49%、真空压力为7.82kPa条件下，实际分离系数和渗透通量与预测值偏差分别小于5.46%和7.39%。

关键词: 分子筛, 渗透蒸发, 乙醇, 分离, 响应面分析

Abstract:

The pervaporation separation of low concentration ethanol/water solutions by Silicalite-1 molecular sieve membranes was studied. The effects of seed concentration, crystallization temperature and crystallization time on the pervaporation separation performance of Silicalite-1 molecular sieve membrane were investigated by single factor experiment. Response surface analysis (RSM) was used to study the effects of feed liquid temperature, ethanol concentration and vacuum pressure on the separation coefficient and permeate flux. The results of single factor experiments showed that the Silicalite-1 molecular sieve membrane prepared under the conditions of seed concentration 0.3%, crystallization temperature 175℃ and crystallization time 7h exhibited the preferable pervaporation separation of ethanol aqueous solutions. According to the RSM results,the separation coefficient and permeate flux were significantly affected by feed liquid temperature, feed liquid ratio, and vacuum pressure. A polynomial model was established according to RSM results and the optimal conditions of the model prediction were verified by experiments. At feed temperature of 70℃, ethanol concentration of 3.49%, and vacuum pressure of 7.82kPa, the deviations of the actual separation coefficient and permeate flux from the predicted values were less than 5.46% and 7.39%, respectively.

Key words: molecular sieve, pervaporation, ethanol, separation, response surface analysis

中图分类号:

TQ028

赵尧, 周志辉, 吴红丹, 胡传智, 张国春, 吴睿鹏. Silicalite-1分子筛膜渗透蒸发条件的响应面分析与优化[J]. 化工进展, 2023, 42(5): 2586-2594.

ZHAO Yao, ZHOU Zhihui, WU Hongdan, HU Chuanzhi, ZHANG Guochun, WU Ruipeng. Response surface analysis and optimization of membrane permeation vaporization by Silicalite-1 molecular sieve[J]. Chemical Industry and Engineering Progress, 2023, 42(5): 2586-2594.

图/表 13

参考文献 31

1	ALI N, BILAL M, KHAN A, et al. Understanding the hierarchical assemblies and oil/water separation applications of metal-organic frameworks[J]. Journal of Molecular Liquids, 2020, 318: 114273.
2	DÍAZ V H G, TOST G O. Butanol production from lignocellulose by simultaneous fermentation, saccharification, and pervaporation or vacuum evaporation[J]. Bioresource Technology, 2016, 218: 174-182.
3	LIU Song, ZHOU Guangyuan, CHENG Gongbi, et al. Emerging membranes for separation of organic solvent mixtures by pervaporation or vapor permeation[J]. Separation and Purification Technology, 2022, 299: 121729.
4	董道敏, 刘宾, 柴永明, 等. 动态水热法制备Silicalite-1分子筛膜包覆多孔缺陷Al₂O₃微球[J]. 化工进展, 2018, 37(10): 3943-3948.
	DONG Daomin, LIU Bin, CHAI Yongming, et al. Dynamic hydrothermal synthesis of Silicalite-1 zeolite membrane to encapsulate defective porous alumina spheres[J]. Chemical Industry and Engineering Progress, 2018, 37(10): 3943-3948.
5	UENO K, NEGISHI H, MIYAMOTO M, et al. Effect of deposition seed crystal amount on the α-Al₂O₃ support and separation performance of silicalite-1 membranes for acetic acid/water mixtures[J]. Separation and Purification Technology, 2017, 174: 57-65.
6	赵文博, 沈润生, 傅雯倩. 多孔Silicalite-1沸石负载Ni对肉桂醛的选择性加氢[J]. 精细石油化工, 2019, 36(1): 40-46.
	ZHAO Wenbo, SHEN Runsheng, FU Wenqian. Selective hydrogenation of cinnamaldehyde in porous Silicalite-1 zeolite supported by Ni[J]. Speciality Petrochemicals, 2019, 36(1): 40-46.
7	LI Jiexin, SHI Chunhong, ZHANG Huifeng, et al. Silicalite-1 zeolite membrane: Synthesis by seed method and application in organics removal[J]. Chemosphere, 2019, 218: 984-991.
8	樊丽虹, 李裕, 宋尧, 等. 原位水热合成b轴Silicalite-1膜时间控制及乙醇-水物系分离[J]. 中北大学学报(自然科学版), 2018, 39(3): 316-321, 349.
	FAN Lihong, LI Yu, SONG Yao, et al. Timing control on b-oriented Silicalite-1 synthesized by in situ hydrothermal and separation of system of ethanol and water[J]. Journal of North University of China（Natural Science Edition), 2018, 39(3): 316-321, 349.
9	ZHANG Lejian, WANG Xinping, CHEN Yong. Rapid synthesis of uniform nano-sized silicalite-1 zeolite crystals under atmospheric pressure without wastes discharge[J]. Chemical Engineering Journal, 2020, 382(2): 122913.
10	KUJAWSKA A, KNOZOWSKA K, KUJAWA J, et al. Influence of downstream pressure on pervaporation properties of PDMS and POMS based membranes[J]. Separation and Purification Technology, 2016, 159: 68-80.
11	SHARAFI S M, MOGHIMI S M, VAEZI M J, et al. Synthesis a low template B-ZSM-5 membrane with suitable morphology and high performance for the separation of acetone/water mixtures[J]. Journal of Environmental Chemical Engineering, 2022, 10(2): 107079.
12	LI Yan, LI Shenhui, XU Lihao, et al. Highly selective PDMS membranes embedded with ILs-decorated halloysite nanotubes for ethyl acetate pervaporation separation[J]. Separation and Purification Technology, 2022, 298: 121552.
13	BEZERRA M A, SANTELLI R E, OLIVEIRA E P, et al. Response surface methodology (RSM) as a tool for optimization in analytical chemistry[J]. Talanta, 2008, 76(5): 965-977.
14	HUANG Zhen, RU Xiaofei, ZHU Yatong, et al. Poly (vinyl alcohol)/ZSM-5 zeolite mixed matrix membranes for pervaporation dehydration of isopropanol/water solution through response surface methodology[J]. Chemical Engineering Research and Design, 2019, 144: 19-34.
15	CATARINO M, FERREIRA A, MENDES A. Study and optimization of aroma recovery from beer by pervaporation[J]. Journal of Membrane Science, 2009, 341(1/2): 51-59.
16	XIANGLI Fenjuan, WEI Wang, CHEN Yiwei, et al. Optimization of preparation conditions for polydimethylsiloxane (PDMS)/ceramic composite pervaporation membranes using response surface methodology[J]. Journal of Membrane Science, 2008, 311(1/2):23-33.
17	WEE S L, TYE C T, BHATIA S. Process optimization studies for the dehydration of alcohol-water system by inorganic membrane based pervaporation separation using design of experiments (DOE)[J]. Separation and Purification Technology, 2010, 71(2):192-199.
18	YEONG Y F, ABDULLAH A Z, AHMAD A L, et al. Process optimization studies of p-xylene separation from binary xylene mixture over silicalite-1 membrane using response surface methodology[J]. Journal of Membrane Science, 2009, 341(1/2): 96-108.
19	ZHAO Qingyu, WANG Jinqu, CHU Naibo, et al. Preparation of high-permeance MFI membrane with the modified secondary growth method on the macroporous α-alumina tubular support[J]. Journal of Membrane Science, 2008, 320(1/2): 303-309.
20	LIN Xiao, KITA H, OKAMOTO K I. Silicalite membrane preparation, characterization, and separation performance[J]. Industrial & Engineering Chemistry Research, 2001, 40(19): 4069-4078.
21	LIU Guoping, JIN Wanqin. Pervaporation membrane materials: Recent trends and perspectives[J]. Journal of Membrane Science, 2021, 636(15): 119557.
22	TAWALBEH M, TEZEL F H, AL-ISMAILY M, et al. Highly permeable tubular silicalite-1 membranes for CO₂ capture[J]. Science of the Total Environment, 2019, 676: 305-320.
23	ZHANG Fazhi, FUJI M, TAKAHASHI M. In situ growth of continuous b-oriented MFI zeolite membranes on porous α-alumina substrates precoated with a mesoporous silica sublayer[J]. Chemistry of Materials, 2005, 17(5): 1167-1173.
24	UENO K, NEGISHI H, MIYAMOTO M, et al. Effect of Si/Al ratio and amount of deposited MFI-type seed crystals on the separation performance of silicalite-1 membranes for ethanol/water mixtures in the presence of succinic acid[J]. Microporous and Mesoporous Materials, 2018, 267: 1-8.
25	REN Xiuxiu, YU Huan, GUO Meng, et al. Long alkyl chain-containing organosilica/silicalite-1 composite membranes for alcohol recovery[J]. Microporous and Mesoporous Materials, 2022, 338: 111947.
26	QIU Heng’e, XU Ning, KONG Lin, et al. Fast synthesis of thin silicalite-1 zeolite membranes at low temperature[J]. Journal of Membrane Science, 2020, 611:118361.
27	KAMELIAN F S, MOHAMMADI T, NAEIMPOOR F. Fast, facile and scalable fabrication of novel microporous silicalite-1/PDMS mixed matrix membranes for efficient ethanol separation by pervaporation[J]. Separation and Purification Technology, 2019, 229: 115820.
28	YANG Xiaobo, DIB E, LANG Qiaolin, et al. Silicalite-1 formation in acidic medium: Synthesis conditions and physicochemical properties[J]. Microporous and Mesoporous Materials, 2022, 329: 111537.
29	FARZANEH A, ZHOU M, ANTZUTKIN O N, et al. Adsorption of butanol and water vapors in silicalite-1 films with a low defect density[J]. Langmuir, 2016, 32(45): 11789-11798.
30	SHU Xiaojun, WANG Xuerui, KONG Qingqing, et al. High-flux MFI zeolite membrane supported on YSZ hollow fiber for separation of ethanol/water[J]. Industrial & Engineering Chemistry Research, 2012, 51(37): 12073-12080.
31	WU Amei, TANG Congyong, ZHONG Shenglai, et al. Synthesis optimization of (h 0 h)-oriented silicalite-1 membranes for butane isomer separation[J]. Separation and Purification Technology, 2019, 214: 51-60.

因子代码	因子名称	最小值（-1）	最大值（+1）	中心值（0）
A	乙醇质量分数/%	1	15	8
B	料液温度/℃	50	70	60
C	真空压力/kPa	5	15	10

因子代码	因子名称	最小值（-1）	最大值（+1）	中心值（0）
A	乙醇质量分数/%	1	15	8
B	料液温度/℃	50	70	60
C	真空压力/kPa	5	15	10

序号	A	B	C	分离系数	渗透通量/g·m^-2·h^-1
1	0	1	1	26.46	345.86
2	0	1	-1	19.08	956.48
3	1	0	-1	33.16	1733.81
4	0	0	0	32.65	969.84
5	0	-1	1	28.95	156.16
6	1	0	1	39.13	584.31
7	0	0	0	32.92	1076.74
8	1	1	0	26.14	1018.73
9	0	-1	-1	27.29	845.31
10	-1	-1	0	11.75	289.71
11	-1	0	-1	5.53	810.19
12	0	0	0	33.21	931.69
13	-1	0	1	12.89	465.78
14	1	-1	0	50.31	301.13
15	0	0	0	32.14	1037.01
16	0	0	0	30.49	1045.86
17	-1	1	0	14.08	321.54

序号	A	B	C	分离系数	渗透通量/g·m^-2·h^-1
1	0	1	1	26.46	345.86
2	0	1	-1	19.08	956.48
3	1	0	-1	33.16	1733.81
4	0	0	0	32.65	969.84
5	0	-1	1	28.95	156.16
6	1	0	1	39.13	584.31
7	0	0	0	32.92	1076.74
8	1	1	0	26.14	1018.73
9	0	-1	-1	27.29	845.31
10	-1	-1	0	11.75	289.71
11	-1	0	-1	5.53	810.19
12	0	0	0	33.21	931.69
13	-1	0	1	12.89	465.78
14	1	-1	0	50.31	301.13
15	0	0	0	32.14	1037.01
16	0	0	0	30.49	1045.86
17	-1	1	0	14.08	321.54

方差来源	平方和	自由度	均方	F值	p值	显著性
模型	1975.52	9	219.50	64.65	＜0.0001	显著
A	1364.77	1	1364.77	401.94	＜0.0001	显著
B	132.36	1	132.36	38.98	0.0004	显著
C	62.55	1	62.55	18.42	0.0036	显著
AB	175.56	1	175.56	51.70	0.0002	显著
AC	0.48	1	0.48	0.14	0.7172	不显著
BC	8.18	1	8.18	2.41	0.1646	不显著
A²	94.59	1	94.59	27.86	0.0012	显著
B²	16.38	1	16.38	4.82	0.0641	不显著
C²	99.65	1	99.65	29.35	0.0010	显著
总残差	23.77	7	3.40	—	—	—
失拟误差	19.13	3	6.38	5.50	0.0665	不显著
纯误差	4.64	4	1.16	—	—	—
总和	1999.29	16	—	—	—	—