Response surface analysis and optimization of membrane permeation vaporization by Silicalite-1 molecular sieve

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

Abstract

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

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

CLC Number:

TQ028

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.

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.

Figures/Tables 13

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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	—	—	—	—