聚酰亚胺/UIO-66薄层纳米复合膜的制备及其纳滤性能
作者:代新雷,马文中,钟 璟,张新妙,孟凡宁
单位: 1. 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, 江苏 常州213164;2. 常州大学 材料科学与工程学院, 江苏省环境友好高分子材料重点实验室, 江苏 常州213164;3. 中国石化北京化工研究院环境保护研究所
关键词: UiO-66,水相添加,有机相添加,聚酰亚胺
DOI号:
分类号: TQ028.8
出版年,卷(期):页码: 2024,44(2):89-96

摘要:
 传统纳滤膜面临“trade-off”效应,不能够在保证截留的情况下提高膜通量。为解决这一问题,将UiO-66和UiO-66-NH22种金属有机框架(MOFs)纳米材料分别引入水相和有机相,通过界面聚合反应,辅以亚胺化处理制备4种不同的聚酰亚胺(PI)复合纳滤(NF)膜,研究UiO-66的氨基化及不同添加方式对膜的结构及分离性能的影响。结果表明,与纯PI NF膜相比,4种PI复合NF膜具有更好的亲水性。UiO-66-NH2添加水相具有最佳的纳滤性能,对CaSO4的截留为91%,水通量为219L/(m2·h·MPa)。4种PI复合NF膜在有机溶剂(THF、DMAc、MT、NMP)中浸泡48 h后,其通量衰减<0.1%,CaSO4的截留率变化<1%;在120 h的长期运行中,通量衰减量在9~17 L/(m2·h·MPa)之间,具有较好的稳定性。
 
 Traditional nanofiltration membranes still experience a "trade-off" phenomenon, where they cannot enhance membrane flux without compromising rejection. To solve this problem, Introduce two metal-organic frameworks (MOFs), UiO-66 and UiO-66-NH2, as nanomaterials into aqueous and organic phases, respectively. Four different polyimide (PI) composite nanofiltration (NF) membranes were prepared by interfacial polymerization reaction and imidization treatment. to study the effects of UiO-66 amination and the influence of different adding methods on membrane structure and separation performance. The water contact results showed that the four PI composite NF membranes had better hydrophilic properties compared to pure PI NF membranes. The nanofiltration performance showed that the UiO-66-NH2-doped aqueous phase had the best nanofiltration performance with 91% CaSO4 rejection and 219 L/(m2·h·MPa) water flux. The fluxes of the four PI composite NF membranes were attenuated by less than 0.1% after soaking in organic solvents (THF, DMAc, MT, NMP) for 48 h. CaSO4 rejection did not change much (attenuation <1%); flux attenuation ranged from 9~17 L/(m2·h·MPa) during 120 h of long-term operation, indicating good stability.
 

基金项目:
中国石油化工股份有限公司科技项目(219020-2),江苏省研究生科研与实践创新计划项目(KYCX22_3096)

作者简介:
代新雷(1998-),男,安徽宿州人,硕士研究生,研究方向膜分离,E-mail:daixinlei7501@163.com

参考文献:
 [1] Yadav D, Karki S, Ingole P G. Nanofiltration (NF) membrane processing in the food industry[J]. Food Eng Rev, 2022, 14(4): 579-595.
[2] Duan J, Litwiller E, Pinnau I. Preparation and water desalination properties of POSS-polyamide nanocomposite reverse osmosis membranes[J]. J Membr Sci, 2015, 473: 157-164.
[3] Mohammad A W, Teow Y H, Ang W L, et al. Nanofiltration membranes review: Recent advances and future prospects[J]. Desalination, 2015, 356: 226-254.
[4] Shi G M, Feng Y, Li B, et al. Recent progress of organic solvent nanofiltration membranes[J]. Prog Polym Sci, 2021, 123: 101470.
[5] Vandezande P, Gevers L E M, Vankelecom I F J. Solvent resistant nanofiltration: separating on a molecular level[J]. Chem. Soc. Rev, 2008, 37(2): 365-405.
[6] Chi X Y, Zhang P Y, Guo X J, et al. A novel TFC forward osmosis (FO) membrane supported by polyimide (PI) microporous nanofiber membrane[J]. Appl Surf Sci, 2018, 427: 1-9.
[7] 何鹏鹏, 赵颂, 毛晨岳, 等. 耐溶剂复合纳滤膜的研究进展[J]. 化工学报, 2021, 72(2): 727-747.
[8] Zhu J, Qin L, Uliana A, et al. Elevated performance of thin film nanocomposite membranes enabled by modified hydrophilic MOFs for nanofiltration[J]. ACS Appl Mater Interfaces, 2017, 9(2): 1975-1986.
[9] Liu X, Demir N K, Wu Z, et al. Highly water-stable zirconium metal–organic framework UiO-66 membranes supported on alumina hollow fibers for desalination[J]. J Am Chem Soc, 2015, 137(22): 6999-7002.
[10] Xiao F, Hu X, Chen Y, et al. Porous Zr-based metal-organic frameworks (Zr-MOFs)-incorporated thin-film nanocomposite membrane toward enhanced desalination performance[J]. ACS Appl Mater Interfaces, 2019, 11(50): 47390-47403.
[11] Aghili F, Ghoreyshi A A, Van der Bruggen B, et al. Introducing gel-based UiO-66-NH2 into polyamide matrix for preparation of new super hydrophilic membrane with superior performance in dyeing wastewater treatment[J]. J Environ Chem Eng, 2021, 9(4): 105484.
[12] 蒋超, 马文中, 李太雨, 等. 界面聚合法合成聚酰亚胺渗透汽化膜及表征[J]. 高校化学工程学报, 2019, 33(3): 724-731.
[13] 梁梦迪, 任秀秀, 陈乐, 等. 改性UiO-66材料的制备及二甲苯异构体吸附性能研究[J]. 高校化学工程学报, 2020, 34(6): 8.
[14] Ma W, Dai X, Qiu P, et al. A cross-linking modification toward a high-performance polyimide nanofiltration membrane for efficient desalination[J]. Acs Es&T Water, 2021, 1(12): 2485-2496.
[15] Liu H, Gao J, Liu G, et al. Enhancing permeability of thin film nanocomposite membranes via covalent linking of polyamide with the incorporated metal–organic frameworks[J]. Ind Eng Chem Res, 2019, 58(20): 8772-8783.
[16] Xu R, Gao F, Wu Y, et al. Influences of support layer hydrophilicity on morphology and performances of polyamide thin-film composite membrane[J]. Sep Purif Technol, 2022, 281: 119884.
[17] Tan Z, Chen S, Peng X, et al. Polyamide membranes with nanoscale Turing structures for water purification[J]. Science, 2018, 360(6388): 518-521. 
[18] Zhao Y, Liu Y, Wang X, et al. Impacts of metal–organic frameworks on structure and performance of polyamide thin-film nanocomposite membranes[J]. ACS Appl Mater Interfaces, 2019, 11(14): 13724-13734.
[19] Huo X, Jing Z, Wang H, et al. Sodium dodecyl sulfate/C-UIO-66 regulation of nanofiltration membrane with pleated and thin polyamide layer structure[J]. Desalination, 2022, 538: 115927.
[20] Gu Z, Yu S, Zhu J, et al. Incorporation of lysine-modified UiO-66 for the construction of thin-film nanocomposite nanofiltration membrane with enhanced water flux and salt selectivity[J]. Desalination, 2020, 493: 114661.
[21] Zhang X, Zhang Y, Wang T, et al. A thin film nanocomposite membrane with pre-immobilized UiO-66-NH 2 toward enhanced nanofiltration performance[J]. RSC Adv, 2019, 9(43): 24802-24810.
[22] Liu H, Gao J, Liu G, et al. Enhancing permeability of thin film nanocomposite membranes via covalent linking of polyamide with the incorporated metal–organic frameworks[J]. Ind Eng Chem Res, 2019, 58(20): 8772-8783.
[23] 祝学东, 董丹, 马燕林, 等. 碳纳米管径向尺寸对碳纳米管自支撑膜孔隙结构及通量的影响[J]. 环境科学学报, 2019, 39(11): 3839-3848.
[24] Wang K Y, Chung T S, Rajagopalan R. Novel polybenzimidazole (PBI) nanofiltration membranes for the separation of sulfate and chromate from high alkalinity brine to facilitate the chlor-alkali process[J]. Ind Eng Chem Res, 2007, 46(5): 1572-1577.

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