APTES改性ZIF-L/PEBA混合基质膜强化渗透汽化分离苯酚研究

doi:10.11949/0438-1157.20211358

化工学报 ›› 2022, Vol. 73 ›› Issue (3): 1389-1402.doi: 10.11949/0438-1157.20211358

• 材料化学工程与纳米技术 • 上一篇下一篇

APTES改性ZIF-L/PEBA混合基质膜强化渗透汽化分离苯酚研究

毛恒(),王月,王森,刘伟民,吕静,陈甫雪,赵之平()

北京理工大学化学与化工学院，北京 102488

收稿日期:2021-09-22 修回日期:2021-11-24 出版日期:2022-03-15 发布日期:2022-03-14
通讯作者: 赵之平 E-mail:maoheng@bit.edu.cn;zhaozp@bit.edu.cn
作者简介:毛恒(1989—)，男，博士，maoheng@bit.edu.cn
基金资助:
国家自然科学基金项目(21736001);中国博士后科学基金项目(2020M670165)

APTES-modified ZIF-L/PEBA mixed matrix membranes for enhancing phenol perm-selective pervaporation

Heng MAO(),Yue WANG,Sen WANG,Weimin LIU,Jing LYU,Fuxue CHEN,Zhiping ZHAO()

School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, China

Received:2021-09-22 Revised:2021-11-24 Published:2022-03-15 Online:2022-03-14
Contact: Zhiping ZHAO E-mail:maoheng@bit.edu.cn;zhaozp@bit.edu.cn

摘要/Abstract

摘要：

渗透汽化(PV)膜分离是一种高效节能、无污染的化工分离技术，在有机废水处理领域的应用潜力巨大。以3-氨丙基三乙氧基硅烷(APTES)改性二维ZIF-L(AZLs)，将其引入聚醚嵌段酰胺(PEBA)内制备AZLs/PEBA混合基质膜，用于分离水溶液中的苯酚。系统表征了所制膜的微结构与物化特性，考察了APTES添加量、AZLs填充量、操作温度、料液浓度等对膜分离性能的影响。结果表明：AZLs均匀分散在PEBA基质中，表明两者具有良好的界面相容性。AZLs的加入使得膜疏水性增强而表面自由能降低，从而提高了PEBA膜的选择性。当分离80℃、1000 mg/kg苯酚水溶液时，AZLs/PEBA膜总通量可达2046 g/(m²·h)，分离因子为25.4，并且具有一定的稳定性。所制AZLs/PEBA混合基质膜在含酚废水处理方面具有应用前景。

关键词: 膜, 分离, 废水, 聚醚嵌段酰胺, 金属有机框架材料, 混合基质膜, 渗透汽化, 苯酚

Abstract:

As an efficient, energy-saving, and pollution-free chemical separation technology, pervaporation(PV) has great application potential for organic wastewater treatment. In this study, the AZLs were synthesized by modifying two-dimensional ZIF-L with 3-aminopropyltriethoxysilane(APTES). The AZLs were incorporated into the poly(ether-block-amide)(PEBA) to prepare AZLs/PEBA mixed matrix membranes for phenol separation from aqueous solution. The membrane microstructures and physicochemical properties were characterized in detail. Effects of the APTES addition amount, AZLs loading, operating temperature, and feed concentration on separation performance of the membranes were investigated. The AZLs were uniformly dispersed within PEBA matrix, indicating their good interfacial compatibility. The addition of AZLs increased the hydrophobicity and reduced the surface free energy of PEBA membrane, thereby enhancing membrane selectivity. The AZLs/PEBA membrane had a total flux of 2046 g/(m²·h) and a separation factor of 25.4 in separating 1000 mg/kg phenol aqueous solution at 80℃. The AZLs/PEBA membrane also displayed a certain stability. The as-prepared AZLs/PEBA mixed matrix membranes were promising candidates in the phenolic wastewater treatment.

Key words: membrane, separation, wastewater, poly(ether-block-amide), metal-organic frameworks, mixed matrix membranes, pervaporation, phenol

中图分类号:

TQ 028.8

毛恒, 王月, 王森, 刘伟民, 吕静, 陈甫雪, 赵之平. APTES改性ZIF-L/PEBA混合基质膜强化渗透汽化分离苯酚研究[J]. 化工学报, 2022, 73(3): 1389-1402.

MAO Heng, WANG Yue, WANG Sen, LIU Weimin, LYU Jing, CHEN Fuxue, ZHAO Zhiping. APTES-modified ZIF-L/PEBA mixed matrix membranes for enhancing phenol perm-selective pervaporation[J]. CIESC Journal, 2022, 73(3): 1389-1402.

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样品	分离层厚度/μm	表面自由能/(mN/m)	断裂强度/MPa	最大伸长率/%	弹性模量/MPa
PEBA膜	18.6	46.5	2.1±0.3	548±23	98.0±4.5
ZIF-L/PEBA-20	19.4	37.3	6.9±0.2	990±34	146.0±6.3
AZLs-0.25/PEBA-20	16.7	34.8	8.0±0.4	1088±57	161.0±8.7
AZLs-0.5/PEBA-20	20.5	30.5	6.8±0.5	726±43	188.0±5.7
AZLs-0.75/PEBA-20	24.1	33.4	7.6±0.6	891±62	136.0±7.3
AZLs-1.0/PEBA-20	25.3	35.1	6.1±0.6	1047±48	124.0±9.5

样品	E_A,_i /( kJ/ mol)		ΔH_evp,_i (80 ^oC) /( kJ/ mol)		E_P,_i /( kJ/mol)
样品	苯酚	水	苯酚	水	苯酚	水
PEBA膜	45.31	34.25	54.67	41.63	-9.36	-7.38
AZLs-0.5/PEBA-20	43.32	27.94	54.67	41.63	-11.35	-13.69

膜	温度/ ℃	浓度/ %(质量)	总通量/ (g/(m²?h))	分离因子	PSI	文献
PDMS	70	1	370	21	7400	[34]
PEBA-4033	60	2	350	23	7700	[35]
PEBA-4033	60	1	620	20	11780	[36]
PERVAP-1060	60	2	6840	6	34200	[35]
OA-PDMS	70	0.5	320	6.3	1696	[37]
ZSM-5/PDMS	80	0.01	1590	4.5	5565	[38]
Polyimide	70	1	370	7.5	2405	[39]
PIM-1	70	1	210	16	3150	[40]
PEBA-2533	70	0.1	800	52.6	41280	[1]
PEBA-2533	80	0.1	1430	25	34320	[41]
PU/ZSM-ECD	80	0.3	980	9.3	8134	[42]
PUCD	70	3	70	49	3360	[43]
PEBA/PVDF	80	0.1	6560	9	52480	[3]
AZLs/PEBA	70	0.1	1362	22.3	29011	本文
AZLs/PEBA	80	0.1	2046	25.4	49922	本文

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APTES改性ZIF-L/PEBA混合基质膜强化渗透汽化分离苯酚研究

APTES-modified ZIF-L/PEBA mixed matrix membranes for enhancing phenol perm-selective pervaporation

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