PEG交联有机硅/陶瓷杂化膜的制备及反渗透脱盐性能

doi:10.15541/jim20180019

无机材料学报 ›› 2018, Vol. 33 ›› Issue (11): 1154-1160.DOI: 10.15541/jim20180019 CSTR: 32189.14.10.15541/jim20180019

PEG交联有机硅/陶瓷杂化膜的制备及反渗透脱盐性能

徐荣, 姜万, 戚律, 张琪, 钟璟

常州大学石油化工学院, 江苏省绿色催化材料与技术重点实验室, 常州213164

收稿日期:2018-01-10 修回日期:2018-03-23 出版日期:2018-11-16 网络出版日期:2018-10-20
作者简介:徐荣(1983-), 男, 副教授. E-mail:xurong@cczu.edu.cn
基金资助:
国家自然科学基金(21406018);常州市科技计划(CJ20179053);江苏省先进催化与绿色制造协同创新中心项目(常州大学);中国石油化工股份有限公司科技项目(216078)

Fabrication of PEG Crosslinked Organosilica Hybrid Membranes for Reverse Osmosis Desalination

XU Rong, JIANG Wan, QI Lv, ZHANG Qi, ZHONG Jing

Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou 213164, China

Received:2018-01-10 Revised:2018-03-23 Published:2018-11-16 Online:2018-10-20
About author:XU Rong. E-mail:xurong@cczu.edu.cn
Supported by:
National Natural Science Foundation of China (21406018);Changzhou Sci&Tech Program (CJ20179053);Advanced Catalysis and Green Manufacturing Collaborative Innovation Center (Changzhou University);Scientific Project of China Petrochemical Corporatim (216078)

摘要/Abstract

摘要：

采用聚乙二醇(PEG)和1,2-双(三乙氧基硅基)乙烷(BTESE)进行交联共聚, 以多孔α-Al₂O₃陶瓷膜为支撑体制备了一系列PEG交联的有机硅杂化膜。通过原子力显微镜(AFM)、场发射扫描电镜(FE-SEM)、傅里叶红外光谱(FT-IR)、热重分析(TGA)和水接触角测试(CA)对膜结构和物化性质进行了表征。将制备的BTESE/PEG杂化膜应用于反渗透脱盐, 考察了PEG含量、操作压力、进料浓度和操作温度等因素对改性杂化膜分离性能的影响。实验结果表明, 相比于未改性的BTESE膜, 10wt% PEG交联的有机硅杂化膜BTESE/PEG-10的水渗透率和盐离子表观截留率均有所提高。随着操作压力的升高和进料盐含量的下降, NaCl截留率上升而水渗透率基本恒定。在高达70℃的温度循环实验中, BTESE/PEG-10杂化膜表现出优异的水热稳定性, NaCl表观截留率始终保持在97%以上, 水渗透率高达1.2×10^-12m³/(m²·s·Pa)。

关键词: 聚乙二醇, 有机硅, 反渗透, 脱盐

Abstract:

A series of poly(ethylene glycol)(PEG) crosslinked organosilica hybrid membranes were fabricated via co-polymerization with PEG as crosslinker and bis(triethoxylsilyl)ethane(BTESE) as the Si precursor, using porous α-Al₂O₃ membranes as the support. The membrane structure and physicochemical properties were characterized by atomic force microscopy (AFM), field emission scanning electron microscopy (FE-SEM), Fourier transform infrared spectroscopy (FT-IR), thermal gravimetric analysis (TGA) and water contact angle measurements (CA). The prepared BTESE/PEG hybrid membranes were applied to desalination by reverse osmosis (RO). The effects of PEG content, operating pressure, feed concentration, and operating temperature on RO performances of the membrane were investigated. Compared with the un-modified BTESE membrane, the BTESE/PEG hybrid membrane with an optimum PEG content of 10wt% exhibited higher water permeability and observed NaCl rejection in RO experiments. In addition, the observed NaCl rejection increased whereas the water permeability remained almost constant with an increase in operating pressure and a decrease in salt concentration. Moreover, the BTESE/PEG-10 membrane exhibited high hydrothermal stability in temperature cycles up to 70℃, always delivering high NaCl rejections of >97% and excellent water permeabilities of up to 1.2×10^-12m³/(m²·s·Pa).

Key words: poly(ethylene glycol), organosilica, reverse osmosis, desalination

中图分类号:

TQ028

徐荣, 姜万, 戚律, 张琪, 钟璟. PEG交联有机硅/陶瓷杂化膜的制备及反渗透脱盐性能[J]. 无机材料学报, 2018, 33(11): 1154-1160.

XU Rong, JIANG Wan, QI Lv, ZHANG Qi, ZHONG Jing. Fabrication of PEG Crosslinked Organosilica Hybrid Membranes for Reverse Osmosis Desalination[J]. Journal of Inorganic Materials, 2018, 33(11): 1154-1160.

图/表 10

图1 BTESE/PEG杂化膜的网络结构示意图

Fig. 1 Schematic structure of the BTESE/PEG hybrid membrane

图2 反渗透试验装置示意图

Fig. 2 Scheme of the RO experimental apparatus

图3 BTESE和BTESE/PEG-10膜的AFM照片

Fig. 3 AFM images of (a) BTESE and (b) BTESE/PEG-10 membranes

图4 BTESE/PEG-10膜的断面SEM照片

Fig. 4 Cross-sectional SEM image of the BTESE/PEG-10 membrane

图5 (a) BTESE和BTESE/PEG-10膜的FT-IR谱图和(b)BTESE/PEG-10膜的热重曲线

Fig. 5 (a) FT-IR spectra of the BTESE and BTESE/PEG-10 membranes and (b) TG curve for the BTESE/PEG-10 membrane

图6 BTESE/PEG膜的水接触角

Fig. 6 Contact angles of BTESE/PEG membranes

图7 BTESE中PEG含量对水渗透率和盐截留率的影响(25℃, 1.2 MPa, 2000 mg/L)

Fig. 7 Effect of PEG content in BTESE membranes on water permeability and salt rejection (25℃, 1.2 MPa, 2000 mg/L)

图8 压力对BETSE/PEG-10膜的反渗透性能影响(25℃, 2000 mg/L NaCl进料)

Fig. 8 Effect of pressure on the RO performance of BTESE/ PEG-10 membrane (25℃, 2000×10-6 mg/L NaCl feed)

图9 NaCl浓度对BETSE/PEG-10膜的反渗透性能影响(25℃, 1.2 MPa)

Fig. 9 Influence of NaCl concentration on the RO performance of BTESE/PEG-10 membrane (25℃, 1.2 MPa)

图10 (a)操作温度和(b)操作时间对BTESE/PEG-10膜的反渗透性能影响(1.2 MPa, 2000 mg/L NaCl进料)

Fig. 10 Effects of (a) operating temperature and (b) time on RO performance of the BTESE/PEG-10 membrane (1.2 MPa and 2000 mg/L NaCl feed)

参考文献 22

[1]	LARSON R E, CADOTTE J E, PETERSEN R J.The FT-30 seawater reverse osmosis membrane--element test results.Desalination, 1981, 38: 473-483.
[2]	DAER S, KHARRAZ J, GIWA A, et al.Recent applications of nanomaterials in water desalination: a critical review and future opportunities.Desalination, 2015, 367: 37-48.
[3]	PAN CHUN-YOU, XU GUO-RONG, LI LU, et al.Developments and perspectives on the polyamide-based reverse osmosis desalination membranes.Membrane Science and Technology, 2016, 36(6): 133-138.
[4]	KIM S J, OH B S, YU H W, et al.Foulant characterization and distribution in spiral wound reverse osmosis membranes from different pressure vessels.Desalination, 2015, 370: 44-52.
[5]	GUTMAN J, HERZBERG M, WALKER S L.Biofouling of reverse osmosis membranes: positively contributing factors of Sphingomonas.Environmental Science & Technology, 2014, 48(23): 13941-13950.
[6]	SAIDANI H, AMAR N B, PALMERI J, et al.Interplay between the transport of solutes across nanofiltration membranes and the thermal properties of the thin active layer.Langmuir, 2010, 26(4): 2574-2583.
[7]	ASEFA T, MACLACHLAN M J, COOMBS N, et al.Periodic mesoporous organosilicas with organic groups inside the channel walls.Nature, 1999, 402(6764): 867-871.
[8]	CASTRICUM H L, KREITER R, VAN VEEN H M, et al.High-performance hybrid pervaporation membranes with superior hydrothermal and acid stability.Journal of Membrane Science, 2008, 324(1/2): 111-118.
[9]	QI H, HAN J, JIANG X L, et al.Preparation and hydrothermal stability of organic-inorganic hybrid silica membrane.Journal of Inorganic Materials, 2010, 25(7): 758-764.
[10]	XU R, WANG J, KANEZASHI M, et al.Development of robust organosilica membranes for reverse osmosis.Langmuir, 2011, 27(23): 13996-13999.
[11]	PARADIS G G, KREITER R, VAN TUEL M M A, et al. Amino-functionalized microporous hybrid silica membranes.Journal of Materials Chemistry, 2012, 22(15): 7258-7264.
[12]	BARCZAK M, BOROWSKI P, DąBROWSKI A. Structure- adsorption properties of ethylene-bridged polysilsesquioxanes and polysiloxanes functionalized with different groups.Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2009, 347(1/2/3): 114-120.
[13]	XU R, IBRAHIM S M, KANEZASHI M, et al.New insights into the microstructure-separation properties of organosilica membranes with ethane, ethylene, and acetylene bridges.ACS applied Materials & Interfaces, 2014, 6(12): 9357-9364.
[14]	NIE F Q, XU Z K, HUANG X J, et al.Acrylonitrile-based copolymer membranes containing reactive groups: surface modification by the immobilization of poly(ethylene glycol) for improving antifouling property and biocompatibility.Langmuir, 2003, 19(23): 9889-9895.
[15]	SAGLE A C, VAN WAGNER E M, JU H, et al. PEG-coated reverse osmosis membranes: desalination properties and fouling resistance.Journal of Membrane Science, 2009, 340(1): 92-108.
[16]	HONG ANH NGO T, MORI S,THI TRAN D. Photo-induced grafting of poly(ethylene glycol) onto polyamide thin film composite membranes.Journal of Applied Polymer Science, 2017, 134(43): 45454-1-9.
[17]	ASAEDA M, YANG J, SAKOU Y.Porous silica-zirconia (50%) membranes for pervaporation of iso-propyl alcohol (IPA)/water mixtures.Journal of chemical Engineering of Japan, 2002, 35(4): 365-371.
[18]	XU R, WANG J, KANEZASHI M, et al.Reverse osmosis performance of organosilica membranes and comparison with the pervaporation and gas permeation properties.AIChE Journal, 2013, 59(4): 1298-1307.
[19]	GEISE G M, PARK H B, SAGLE A C, et al.Water permeability and water/salt selectivity tradeoff in polymers for desalination.Journal of Membrane Science, 2011, 369(1/2): 130-138.
[20]	GONG G, NAGASAWA H, KANEZASHI M, et al.Tailoring the separation behavior of polymer-supported organosilica layered- hybrid membranes via facile post-treatment using HCl and HN3 vapors.ACS Applied Materials & Interfaces, 2016, 8(17): 11060-11069.
[21]	CHENG Q, ZHENG Y, YU S, et al.Surface modification of a commercial thin-film composite polyamide reverse osmosis membrane through graft polymerization of n-isopropylacrylamide followed by acrylic acid.Journal of Membrane Science, 2013, 447: 236-245.
[22]	XU R, LIN P, ZHANG Q, et al.Development of ethenylene- bridged organosilica membranes for desalination applications.Industrial & Engineering Chemistry Research, 2016, 55(7): 2183-2190.

PEG交联有机硅/陶瓷杂化膜的制备及反渗透脱盐性能

Fabrication of PEG Crosslinked Organosilica Hybrid Membranes for Reverse Osmosis Desalination

RichHTML

PDF (PC)

可视化

被引次数

摘要/Abstract

引用本文

使用本文

图/表 10

参考文献 22

相关文章 15

编辑推荐

Metrics

本文评价

[1]	罗艺, 夏书海, 牛波, 张亚运, 龙东辉. 柔性有机硅气凝胶的制备及其高温无机化转变研究[J]. 无机材料学报, 2022, 37(12): 1281-1288.
[2]	张文君, 赵雪莹, 吕江维, 曲有鹏. 中空有序介孔有机硅的研究进展: 制备及在肿瘤治疗中的应用[J]. 无机材料学报, 2022, 37(11): 1192-1202.
[3]	席文, 李海波. TiO₂/Ti₃C₂T_x复合材料的制备及其杂化电容脱盐特性的研究[J]. 无机材料学报, 2021, 36(3): 283-291.
[4]	曾雨淋, 陈佳杰, 田正芳, 朱敏, 朱钰方. 介孔有机硅为载体的纳米递送系统制备及其体外化疗-光热联合治疗性能研究[J]. 无机材料学报, 2020, 35(12): 1365-1372.
[5]	朱春晖, 徐荣, 任秀秀, 左士祥, 龚耿浩, 钟璟. ZIF-8-NH₂/有机硅杂化膜的制备及渗透汽化脱盐性能研究[J]. 无机材料学报, 2020, 35(11): 1239-1246.
[6]	史忠祥, 王晶, 关昕. Er³⁺掺杂调控NaY(WO₄)₂: Dy³⁺的上转换发光性能[J]. 无机材料学报, 2018, 33(5): 521-527.
[7]	路淑娟, 王唱, 赵博文, 汪浩, 刘晶冰, 严辉. PEG改性氧化钨薄膜的电致变色特性[J]. 无机材料学报, 2017, 32(2): 185-190.
[8]	马平平, 刘志坚, 夏建华, 卢志超. 聚乙二醇为碳源合成0.7LiFePO₄ּ0.3Li₃V₂(PO₄)₃/C 复合正极材料及性能研究[J]. 无机材料学报, 2015, 30(2): 122-128.
[9]	安建国, 高翔, 金军江, 顾金楼, 李亮, 李永生, 施剑林. 以聚乙二醇为模板凝胶转化制备介孔ZSM-5沸石及其催化性能[J]. 无机材料学报, 2015, 30(11): 1148-1154.
[10]	卢剑萍, 李国荣, 郑嘹赢, 曾江涛, 曾华荣, 卞建江. 电泳沉积法制备PNN-PZT厚膜的研究[J]. 无机材料学报, 2012, 27(4): 379-384.
[11]	朱振峰, 王小枫, 刘辉, 刘佃光. 准单分散SnO₂微球的微波溶剂热合成[J]. 无机材料学报, 2012, 27(3): 311-316.
[12]	付芳, 杨卫华, 王鸿辉. 聚乙二醇改性钛基PbO₂电极的制备及性质研究[J]. 无机材料学报, 2010, 25(6): 653-658.
[13]	卿玉长,周万城,罗发,朱冬梅. 多壁碳纳米管/环氧有机硅树脂吸波涂层的介电和吸波性能研究[J]. 无机材料学报, 2010, 15(2): 181-185.
[14]	田昂,王超,薛向欣,吴安华,管格非,王丽,仇波. 纳米羟基磷灰石对人脑胶质母细胞瘤U87细胞活性抑制效应的研[J]. 无机材料学报, 2010, 25(1): 101-106.
[15]	张晏清,张雄. 空心微珠铁氧体复合粉体的改性与吸波性能[J]. 无机材料学报, 2009, 24(4): 732-736.