不同粒径UiO-66混掺改性TFN-FO膜的构建及性能评价

doi:10.11949/0438-1157.20240081

摘要/Abstract

摘要：

以锆基金属-有机骨架材料(MOFs) UiO-66作为研究对象，制备了三种不同粒径的UiO-66纳米颗粒，并将其混掺到薄层复合膜(TFC)的聚酰胺(PA)层内，研究了UiO-66纳米颗粒的粒径对薄层复合纳米正渗透(TFN-FO)膜性能的影响。通过扫描电子显微镜(SEM)、原子力显微镜(AFM)、水接触角(WCA)测量仪、X射线光电子能谱仪(XPS)等表征手段，探究了TFN-FO膜的性质变化。结果表明，减小UiO-66的粒径不会影响TFN-FO膜的高亲水性，并且随着UiO-66粒径的减小，TFN-FO膜的粗糙度降低、交联度升高。通过以去离子水和2 mol/L氯化钠溶液作为进料液和汲取液的实验室自制的正渗透系统对膜性能进行评价，发现混掺小粒径(50 nm) UiO-66的TFN-FO膜可以在保持较低反向盐通量的同时实现35%的水通量提升。有机污染实验表明，TFN-FO膜具有良好的抗污染性能。

关键词: 膜, 过滤, 纳米粒子, 正渗透, MOFs, 粒径, 混掺改性

Abstract:

With zirconiumv (Ⅳ)-carboxylate metal-organic framework (MOF) UiO-66 nanoparticles as representative, UiO-66 nanoparticles with different particle sizes were prepared and incorporated in polyamide (PA) layer of thin-film composite (TFC) membranes to investigate the impact of UiO-66 nanoparticle size on the performance of thin film composite nano-forward osmosis (TFN-FO) membranes. The effects of incorporated UiO-66 nanoparticle on the property of TFN-FO membranes were characterized by scanning electron microscopy (SEM), atomic force microscopy (AFM), water contact angle (WCA) instrument and X-ray photoelectron spectroscopy (XPS). The results showed that reducing the particle size of UiO-66 would not affect the high hydrophilicity of TFN-FO membrane. Meanwhile, as the particle size of UiO-66 decreased, the roughness of TFN-FO membrane decreased and the crosslinking degree increased. Moreover, the performance of TFN-FO membrane was evaluated by a home made forward osmosis system with deionized water and 2 mol/L sodium chloride solution as feed and draw solution. TFN-FO membrane incorporated with small particle size (50 nm) UiO-66 achieved 35% water flux improvement while maintaining a low reverse salt flux. Moreover, organic pollution experiments show that the TFN-FO membrane has good anti-fouling properties.

Key words: membrane, filtration, nanoparticles, forward osmosis, MOFs, particle size, incorporate

中图分类号:

TQ 028.8

张文焱, 刘浩, 宋伟龙, 赵频, 王新华. 不同粒径UiO-66混掺改性TFN-FO膜的构建及性能评价[J]. 化工学报, 2024, 75(5): 1920-1928.

Wenyan ZHANG, Hao LIU, Weilong SONG, Pin ZHAO, Xinhua WANG. Construction and performance evaluation of TFN-FO membranes incorporated with UiO-66 nanoparticles of different sizes[J]. CIESC Journal, 2024, 75(5): 1920-1928.

图/表 10

图1 混掺有UiO-66纳米颗粒的TFN膜的制备

Fig.1 Schematic diagram of the fabrication of TFN membrane incorporated with UiO-66 nanoparticles

图2 膜性能评价装置

Fig.2 Schematic diagram of membranes evaluation system

图3 不同粒径UiO-66的SEM图像

Fig.3 SEM images of UiO-66 with different particle sizes

图4 不同粒径UiO-66的XRD谱图a—50 nm UiO-66; b—100 nm UiO-66; c—150 nm UiO-66

Fig.4 XRD patterns of UiO-66 with different particle sizes

图5 TFC膜和TFN膜的SEM及AFM图像

Fig.5 SEM and AFM images of TFC and TFN membranes

表1 TFC膜和TFN膜的XPS分析

Table 1 XPS of TFC and TFN membranes

膜	C含量	N含量	O含量	Zr含量	O/N原子比	O/N原子比^①	交联度/%
TFC	74.45	10.80	14.71	0	1.36	1.36	54
TFN-50	73.19	10.08	16.28	0.42	1.60	1.39	51
TFN-100	72.72	10.15	16.68	0.40	1.64	1.43	47
TFN-150	73.23	9.80	16.35	0.35	1.70	1.47	43

图6 TFC膜和TFN膜的红外光谱图a—TFN-150; b—TFN-100; c—TFN-50; d—TFC

Fig.6 ATR-FIIR of TFC and TFN membranes

图7 TFC膜和TFN膜的水接触角

Fig.7 Water contact angle of TFC and TFN membranes

图8 TFC膜和TFN膜在不同混掺浓度下的渗透性能a—TFN-50; b—TFN-100; c—TFN-150

Fig.8 Permeability of TFC and TFN membranes

图9 TFC膜和TFN膜的污染实验水通量和归一化通量

Fig.9 Flux and normalized flux curve of TFC and TFN membranes

参考文献 38

1	Cath T, Childress A, Elimelech M. Forward osmosis: principles, applications, and recent developments[J]. Journal of Membrane Science, 2006, 281(1/2): 70-87.
2	Suwaileh W, Pathak N, Shon H, et al. Forward osmosis membranes and processes: a comprehensive review of research trends and future outlook[J]. Desalination, 2020, 485: 114455.
3	Lutchmiah K, Verliefde A R D, Roest K, et al. Forward osmosis for application in wastewater treatment: a review[J]. Water Research, 2014, 58: 179-197.
4	齐亚兵, 张思敬, 杨清翠. 正渗透水处理技术研究现状及进展[J]. 现代化工, 2021, 41(8): 52-57.
	Qi Y B, Zhang S J, Yang Q C. Research status and progress on forward osmosis water treatment technologies[J]. Modern Chemical Industry, 2021, 41(8): 52-57.
5	Chekli L, Phuntsho S, Kim J E, et al. A comprehensive review of hybrid forward osmosis systems: performance, applications and future prospects[J]. Journal of Membrane Science, 2016, 497: 430-449.
6	Wang J L, Liu X J. Forward osmosis technology for water treatment: recent advances and future perspectives[J]. Journal of Cleaner Production, 2021, 280: 124354.
7	Ibrar I, Altaee A, Zhou J L, et al. Challenges and potentials of forward osmosis process in the treatment of wastewater[J]. Critical Reviews in Environmental Science and Technology, 2020, 50(13): 1339-1383.
8	Alihemati Z, Hashemifard S A, Matsuura T, et al. Current status and challenges of fabricating thin film composite forward osmosis membrane: a comprehensive roadmap[J]. Desalination, 2020, 491: 114557.
9	杨碧野, 姚之侃, 林赛赛, 等. 聚酰胺薄层复合膜性能劣化机理及表面改性策略[J]. 膜科学与技术, 2020, 40(3): 161-167.
	Yang B Y, Yao Z K, Lin S S, et al. Deterioration mechanism and modification strategie of polyamide thin film composite membranes[J]. Membrane Science and Technology, 2020, 40(3): 161-167.
10	Lau W J, Gray S, Matsuura T, et al. A review on polyamide thin film nanocomposite (TFN) membranes: history, applications, challenges and approaches[J]. Water Research, 2015, 80: 306-324.
11	孙艳, 刘士涛, 邓尚, 等. 负载羧基化球状介孔纳米颗粒TFN膜的研究[J]. 化工学报, 2020, 71(S1): 454-460.
	Sun Y, Liu S T, Deng S, et al. Study on TFN membrane loaded with carboxylated spherical mesoporous nanoparticles[J]. CIESC Journal, 2020, 71(S1): 454-460.
12	Al M A. Important approaches to enhance reverse osmosis (RO) thin film composite (TFC) membranes performance[J]. Membranes, 2018, 8(3): 68.
13	Jeong B H, Hoek E M V, Yan Y S, et al. Interfacial polymerization of thin film nanocomposites: a new concept for reverse osmosis membranes[J]. Journal of Membrane Science, 2007, 294(1/2): 1-7.
14	Ma X H, Guo H, Yang Z, et al. Carbon nanotubes enhance permeability of ultrathin polyamide rejection layers[J]. Journal of Membrane Science, 2019, 570/571: 139-145.
15	Yuan S S, Li X, Zhu J Y, et al. Covalent organic frameworks for membrane separation[J]. Chemical Society Reviews, 2019, 48(10): 2665-2681.
16	Zhao D L, Feng F, Shen L, et al. Engineering metal-organic frameworks (MOFs) based thin-film nanocomposite (TFN) membranes for molecular separation[J]. Chemical Engineering Journal, 2023, 454: 140447.
17	Liu X G, Shan Y Y, Zhang S T, et al. Application of metal organic framework in wastewater treatment[J]. Green Energy & Environment, 2023, 8(3): 698-721.
18	Xiao F, Hu X Y, Chen Y B, et al. Porous Zr-based metal-organic frameworks (Zr-MOFs)-incorporated thin-film nanocomposite membrane toward enhanced desalination performance[J]. ACS Applied Materials & Interfaces, 2019, 11(50): 47390-47403.
19	Wu L K, Xu Z L, Tong M, et al. Dissecting the role of nanomaterials on permeation enhancement of the thin-film nanocomposite membrane: ZIF-8 as an example[J]. Journal of Membrane Science, 2023, 673: 121494.
20	Samsami S, Sarrafzadeh M H, Ahmadi A. Surface modification of thin-film nanocomposite forward osmosis membrane with super-hydrophilic MIL-53 (Al) for doxycycline removal as an emerging contaminant and membrane antifouling property enhancement[J]. Chemical Engineering Journal, 2022, 431: 133469.
21	Ma D C, Peh S B, Han G, et al. Thin-film nanocomposite (TFN) membranes incorporated with super-hydrophilic metal-organic framework (MOF) UiO-66: toward enhancement of water flux and salt rejection[J]. ACS Applied Materials & Interfaces, 2017, 9(8): 7523-7534.
22	Basu S, Balakrishnan M. Polyamide thin film composite membranes containing ZIF-8 for the separation of pharmaceutical compounds from aqueous streams[J]. Separation and Purification Technology, 2017, 179: 118-125.
23	Bayrami A, Bagherzadeh M, Navi H, et al. Thin-film nanocomposite membranes containing aspartic acid-modified MIL-53-NH₂ (Al) for boosting desalination and anti-fouling performance[J]. Desalination, 2022, 521: 115386.
24	Liao Z P, Fang X F, Xie J, et al. Hydrophilic hollow nanocube-functionalized thin film nanocomposite membrane with enhanced nanofiltration performance[J]. ACS Applied Materials & Interfaces, 2019, 11(5): 5344-5352.
25	Bonnett B L, Smith E D, De La Garza M, et al. PCN-222 metal-organic framework nanoparticles with tunable pore size for nanocomposite reverse osmosis membranes[J]. ACS Applied Materials & Interfaces, 2020, 12(13): 15765-15773.
26	Ren J W, Langmi H W, North B C, et al. Modulated synthesis of zirconium-metal organic framework (Zr-MOF) for hydrogen storage applications[J]. International Journal of Hydrogen Energy, 2014, 39(2): 890-895.
27	Lu Y, Wang R Y, Zhu Y Z, et al. Two-dimensional fractal nanocrystals templating for substantial performance enhancement of polyamide nanofiltration membrane[J]. Proceedings of the National Academy of Sciences of the United States of America, 2021, 118(37): e2019891118.
28	Seoane B, Castellanos S, Dikhtiarenko A, et al. Multi-scale crystal engineering of metal organic frameworks[J]. Coordination Chemistry Reviews, 2016, 307: 147-187.
29	Cavka J H, Jakobsen S, Olsbye U, et al. A new zirconium inorganic building brick forming metal organic frameworks with exceptional stability[J]. Journal of the American Chemical Society, 2008, 130(42): 13850-13851.
30	Huang H, Qu X Y, Dong H, et al. Role of NaA zeolites in the interfacial polymerization process towards a polyamide nanocomposite reverse osmosis membrane[J]. RSC Advances, 2013, 3(22): 8203-8207.
31	Hotze E M, Phenrat T, Lowry G V. Nanoparticle aggregation: challenges to understanding transport and reactivity in the environment[J]. Journal of Environmental Quality, 2010, 39(6): 1909-1924.
32	Knebel A, Friebe S, Bigall N C, et al. Comparative study of MIL-96(Al) as continuous metal-organic frameworks layer and mixed-matrix membrane[J]. ACS Applied Materials & Interfaces, 2016, 8(11): 7536-7544.
33	Duan J T, Pan Y C, Pacheco F, et al. High-performance polyamide thin-film-nanocomposite reverse osmosis membranes containing hydrophobic zeolitic imidazolate framework-8[J]. Journal of Membrane Science, 2015, 476: 303-310.
34	Wang F H, Zheng T, Xiong R H, et al. Strong improvement of reverse osmosis polyamide membrane performance by addition of ZIF-8 nanoparticles: effect of particle size and dispersion in selective layer[J]. Chemosphere, 2019, 233: 524-531.
35	Lind M L, Ghosh A K, Jawor A, et al. Influence of zeolite crystal size on zeolite-polyamide thin film nanocomposite membranes[J]. Langmuir, 2009, 25(17): 10139-10145.
36	Kim E S, Deng B L. Fabrication of polyamide thin-film nano-composite (PA-TFN) membrane with hydrophilized ordered mesoporous carbon (H-OMC) for water purifications[J]. Journal of Membrane Science, 2011, 375(1/2): 46-54.
37	Perez E V, Balkus K J, Ferraris J P, et al. Mixed-matrix membranes containing MOF-5 for gas separations[J]. Journal of Membrane Science, 2009, 328(1/2): 165-173.
38	周倩, 赵频, 刘浩, 等. 氧化石墨烯表面改性正渗透膜制备及其抗污染性能[J]. 膜科学与技术, 2022, 42(4): 81-88, 95.
	Zhou Q, Zhao P, Liu H, et al. Thin-film composite forward osmosis membranes modified by graphene oxide surface grafting for enhancing the anti-fouling capacity[J]. Membrane Science and Technology, 2022, 42(4): 81-88, 95.

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