季铵盐两性离子陶瓷膜制备及抗污染性能研究
作者:覃琦清,王 芮,尤 宏,谢冰涵,谭海丽,柳 锋,李之鹏
单位: 1.哈尔滨工业大学(威海),海洋科学与技术学院环境工程系,山东 威海 264209; 2. 哈尔滨工业大学,城市水资源与水环境国家重点实验室,黑龙江 哈尔滨 150090
关键词: 两性离子;陶瓷膜;抗污染;硅氧烷;溶胶凝胶
出版年,卷(期):页码: 2022,42(5):102-112

摘要:
 以3-氨丙基三甲基硅烷(KH551)与3-缩水甘油基氧基丙基三甲氧基硅烷(KH560)为基体,合成含叔胺基硅氧烷溶胶后涂覆于陶瓷膜表面,并在2-溴乙基磺酸钠(SBTS)作用下生成季铵盐,制备出季铵盐两性离子复合陶瓷膜。表征结果证明,季铵盐成功接枝于膜表面,优化后改性膜接触角约为39.4 °,且通量受凝胶负载影响程度小。微生物吸附实验表明,改性后膜相比改性前减少90.5 %的活菌吸附,动态过滤通量至少提高8.2 %。以污泥中溶解性微生物产物(SMP)、松散结合的胞外聚合物(LB-EPS)作为有机污染物模型,将改性前后膜通过SMP、LB-EPS溶液,考察通量变化,并通过Hermia模型分析污染机理,激光共聚焦显微镜(CLSM)观察污染物粘附于膜表面情况。结果表明,过滤SMP、LB-EPS至稳定时,膜改性后比通量比改性前分别高38.9 %、29.3 %,反洗后通量提高了11.6 %、32.3 %,且改性膜表面污染物残留量分别减少27.2 %、41.5 %。以上结果均表明,通过季铵盐两性离子进行表面修饰能有效提高陶瓷膜抗污染性能。[收稿日期:2022-02-15;修改稿收到日期:2022-04-17
基金项目:项目来源 “山东省自然科学基金项目”(ZR2019QEE012)
第一作者简介:覃琦清 (1997—),男,硕士研究生,研究方向为水污染控制,E-mail:qqq13307729990@163.com 
通讯作者,E-mail: lizhipengcn@hit.edu.cn]
 Using 3-Aminopropyltrimethoxysilane (KH551), 3-Glycidyloxypropyltrimethoxysilanen (KH560) as substrates, the siloxane sol containing tertiary amino was synthesized and coated on the ceramic membrane. The Quaternary Ammonium Salt-Zwitterion composite ceramic membrane was prepared by reacting with sodium 2-bromoethyl sulfonate (SBTS) for retarding the fouling in the MBR system. The surface properties, permeability, biofouling and organic fouling resistance of the modified membrane were characterized. The results showed that the quaternary ammonium salt was successfully grafted onto the surface of the membrane. After optimization, the contact angle of the modified membrane was about 39.4 °, and the flux was almost unaffected by gelation. The results of static adsorption experiment showed that the adsorption of live bacteria decreased by 90.6 % after modified, and the flux increased by at least 8.2 %. Taking soluble microbial products (SMP) and loosely bound extracellular polymeric substances (LB-EPS) in sludge as organic fouling models, the flux changes of the membrane were characterized through SMP and LB-EPS solutions, the fouling mechanism was analyzed by Hermia model, and the adhesion of fouling to the membrane surface was observed by CLSM. The results showed when SMP and LB-EPS were filtered to stable flux, the specific flux of modified membrane was 38.9 % and 29.3 % higher than primary membrane, the flux after backwashing was increased by 11.6 % and 32.3 %, and the attached fouling on the surface of modified membrane were reduced by 27.2 % and 41.5 % respectively. The above results indicate the surface modification by Quaternary Ammonium Salt-Zwitterion can effectively improve the antifouling performance of ceramic membrane.
覃琦清 (1997—),男,硕士研究生,广西柳州人,研究方向为水污染控制,E-mail:qqq13307729990@163.com

参考文献:
 [1] 范益群, 漆虹, 徐南平. 多孔陶瓷膜制备技术研究进展 [J]. 化工学报, 2013, 64(01): 107-15.
[2] 卢志华, 李呈顺, 马育栋. 多孔氧化铝陶瓷制备技术研究进展 [J]. 中国陶瓷, 2018, 54(02): 1-7.
[3] Zhang R, Liu Y, He M, et al. Antifouling membranes for sustainable water purification: strategies and mechanisms [J]. Chemical Society Reviews, 2016, 10.1039.C5CS00579E.
[4] Lee H, Yeo S Y, Jeong S H. Antibacterial effect of nanosized silver colloidal solution on textile fabrics [J]. Journal of Materials Science, 2003, 38(10): 2199-204.
[5] Gao N, Mei L, Jing W, et al. Improving the filtration performance of ZrO2 membrane in non-polar organic solvents by surface hydrophobic modification [J]. Journal of Membrane Science, 2011, 375(1-2): 276-83.
[6] Yang Y F, Wan L S, Xu Z K. Surface hydrophilization of microporous polypropylene membrane by the interfacial crosslinking of polyethylenimine [J]. Journal of Membrane Science, 2009, 337(1-2): 70-80.
[7] 邢卫红, 仲兆祥, 景文珩, et al. 基于膜表面与界面作用的膜污染控制方法 [J]. 化工学报, 2013, 64(001): 173-81.
[8] Wu J, Wang Z, Wang Y, et al. Polyvinylamine-grafted polyamide reverse osmosis membrane with improved antifouling property [J]. Journal of Membrane Science, 2015, 495(1-13.
[9] Shahbazi M, Rajabzadeh G, Rafe A, et al. The physico-mechanical and structural characteristics of blend film of poly (vinyl alcohol) with biodegradable polymers as affected by disorder-to-order conformational transition [J]. Food Hydrocolloids, 2016, 60(393-404.
[10] Lowe S, O'brien-Simpson N, Connal L. Antibiofouling polymer interfaces: poly(ethylene glycol) and other promising candidates [J]. POLYMER CHEMISTRY, 2015, 
[11] Yan W, Wang Z, Zhao S, et al. Combining co-solvent-optimized interfacial polymerization and protective coating-controlled chlorination for highly permeable reverse osmosis membranes with high rejection [J]. Journal of Membrane Science, 2018, 
[12] He M, Gao K, Zhou L, et al. Zwitterionic materials for antifouling membrane surface construction [J]. Acta biomaterialia, 2016, 40(142-52.
[13] Jiang S, Cao Z. Ultralow‐fouling, functionalizable, and hydrolyzable zwitterionic materials and their derivatives for biological applications [J]. Advanced materials, 2010, 22(9): 920-32.
[14] Zolk M, Eisert F, Pipper J, et al. Solvation of Oligo(ethylene glycol)-Terminated Self-Assembled Monolayers Studied by Vibrational Sum Frequency Spectroscopy [J]. 2000, 16(14): 5849-52.
[15] Jie Z, Li L, Chen S, et al. Molecular simulation study of water interactions with oligo (ethylene glycol)-terminated alkanethiol self-assembled monolayers [J]. 2004, 20(20): 8931.
[16] Abdelhamid A E, Elawady M M, El-Ghaffar M, et al. Surface modification of reverse osmosis membranes with zwitterionic polymer to reduce biofouling [J]. Water Science, 2015, 15(5): 999-1010.
[17] Storms M, Kadhem A J, Xiang S, et al. Enhancement of the Fouling Resistance of Zwitterion Coated Ceramic Membranes [J]. 2020, 10(9): 210.
[18] Tashiro T, Engineering. Antibacterial and Bacterium Adsorbing Macromolecules [J]. Macromolecular Materials, 2001, 286(2): 63–87.
[19] Yao F, Fu G D, Zhao J, et al. Antibacterial effect of surface-functionalized polypropylene hollow fiber membrane from surface-initiated atom transfer radical polymerization [J]. Journal of Membrane Science, 2008, 319(1-2): 149-57.
[20] Angelis L D, Cortalezzi M D J J O M S. Improved membrane flux recovery by Fenton-type reactions [J]. 2016, 500(255-64.
[21] A E C C, B C J, C H C C, et al. Robust multifunctional superhydrophobic coatings with enhanced water/oil separation, self-cleaning, anti-corrosion, and anti-biological adhesion [J]. Chemical Engineering Journal, 2017, 314(347-57.
[22] 李雪, 张婷, 邱鸣慧, et al. 两步法制备两性离子陶瓷复合膜及抗污染研究 [J]. 膜科学与技术, 2017, 37(003): 27-33.
[23] Zhang X, Wang Z, Tang C Y, et al. Modification of microfiltration membranes by alkoxysilane polycondensation induced quaternary ammonium compounds grafting for biofouling mitigation [J]. Journal of Membrane Science, 2017, S0376738817331265.
[24] Xu T, Xin M, Li M, et al. Synthesis, characterization, and antibacterial activity of N,O-quaternary ammonium chitosan [J]. Carbohydrate research, 2011, 346(15): 2445-50.
[25] Tang R, Ying Z, Yang Z, et al. Synthesis and characterization of chitosan based dye containing quaternary ammonium group [J]. Carbohydrate Polymers, 2016, 139(191-6.
[26] Zhang D Y, Xiong S, Shi Y S, et al. Antifouling enhancement of polyimide membrane by grafting DEDA-PS zwitterions [J]. Chemosphere, 2018, 198(30-9.
[27] Kothekar A T, Kulkarni A P. Basic Principles of Disinfection and Sterilization in Intensive Care and Anesthesia and Their Applications during COVID-19 Pandemic [J]. Indian Journal of Critical Care Medicine: Peer-reviewed, Official Publication of Indian Society of Critical Care Medicine, 2020, 24(11): 1114.

服务与反馈:
文章下载】【加入收藏

《膜科学与技术》编辑部 地址:北京市朝阳区北三环东路19号蓝星大厦 邮政编码:100029 电话:010-64426130/64433466 传真:010-80485372邮箱:mkxyjs@163.com

京公网安备11011302000819号