| 聚乙烯醇辅助的抗污染高通量Fe2O3/Al2O3陶瓷复合超滤膜制备 |
| 作者:卫晶茹1,2, 陈国硙1, 陈献富1, 柯威1, 邱鸣慧1, 蔡大牛3, 陈杰3, 范益群1 |
| 单位: 1. 材料化学工程国家重点实验室 南京工业大学 化工学院, 南京 211816; 2. 清源创新实验室, 泉州 362801; 3. 泉州师范学院, 泉州 362000 |
| 关键词: 氧化铁; 陶瓷复合膜; 聚乙烯醇; 抗污染; 油水分离 |
| DOI号: 10.16159/j.cnki.issn1007-8924.2026.01.007 |
| 分类号: TQ174 |
| 出版年,卷(期):页码: 2026,46(1):67-77 |
|
摘要: |
|
陶瓷膜因孔径分布窄、亲水性强等优势在含油废水处理方面备受关注。为开发抗污染高通量陶瓷膜,本研究采用具有高亲水性的Fe2O3作为膜层材料,结合聚乙烯醇(PVA)的空间位阻效应,在大孔Al2O3载体上制备完整无缺陷的Fe2O3膜层。系统考察了PVA添加量对溶胶及膜层的影响。结果表明,当PVA添加量为1.0%(质量分数)时,获得了完整的Fe2O3/Al2O3陶瓷复合超滤膜,其截留分子量约为450 kDa,对应的Stocks尺寸约为26 nm,纯水渗透率高达6 800 L/(m2·h·MPa)。接触角及表面张力测试结果表明,该复合膜具有优异的抗污染性能和亲水性能。在1 000 mg/L水包油乳液过滤分离中,该复合膜对油滴去除率接近100%,通量稳定在430 L/(m2·h)左右,是Al2O3微滤膜通量的2倍。经纯水简单冲洗后,复合膜通量即可恢复至70%左右,表现出良好的可清洗性与抗污染性能。本研究所制备的Fe2O3/Al2O3陶瓷复合膜在油水处理中展现出了潜力,有望为工业化应用提供技术参考。 |
|
Ceramic membranes have attracted much attention in the treatment of oily wastewater due to their advantages such as narrow pore size distribution and high hydrophilicity. To develop anti-fouling and high-flux ceramic membranes, Fe2O3 with high hydrophilicity was used as the membrane layer material in this study. By combining the steric hindrance effect of polyvinyl alcohol (PVA), an intact and defect-free Fe2O3 membrane layer was prepared on a macroporous Al2O3 support. The effects of PVA addition level on the sol and membrane layer were systematically investigated. The results showed that an intact Fe2O3/Al2O3 ceramic composite ultrafiltration membrane was obtained when the PVA addition level was 1.0% (mass fraction), with a molecular weight cut-off of about 450 kDa, a corresponding Stock size of about 26 nm, and a high pure water permeance of 6 800 L/(m2·h· MPa). The test results of contact angle and surface tension showed that the composite membrane had excellent anti-fouling performance and hydrophilic properties. In the filtration and separation of 1 000 mg/L oil-in-water emulsion, the removal rate of oil droplets by the composite membrane was close to 100%, and the flux was stable at about 430 L/(m2·h), which was almost twice of the flux of Al2O3 microfiltration membrane. After simple rinsing with pure water, the flux of the composite membrane could be restored to about 70%, indicating its excellent cleanability and anti-fouling performance. The Fe2O3/Al2O3 ceramic composite membrane prepared in this study shows potential in oily wastewater treatment, and is expected to provide technical reference for industrial application. |
|
基金项目: |
| 国家重点研发计划项目(2022YFB3805001); 清源创新实验室重大项目(00122003); 吉安市“揭榜挂帅”项目(pzzy-wtht-20220117014) |
|
作者简介: |
| 卫晶茹(1999-),女,山西运城人,硕士研究生,主要研究方向为分离膜的制备与应用 |
|
参考文献: |
| [1]Lin Y M, Song C, Rutledge G C. Functionalization of electrospun membranes with polyelectrolytes for separation of oil-in-water emulsions[J]. Adv Mater Interfaces, 2019, 6(23): 1901285. [2]Salhi B, Baig N, Abdulazeez I, et al. High flux polyaniline-coated ceramic membrane for effective separation of emulsified oil-in-water[J]. Ceram Int, 2022, 48(17): 25246-25253. [3]Asif M B, Zhang Z. Ceramic membrane technology for water and wastewater treatment: A critical review of performance, full-scale applications, membrane fouling and prospects[J]. Chem Eng J, 2021, 418: 129481. [4]古其林, 李军佑, 仲兆祥, 等. 油水高效分离用碳化硅膜的研究进展[J]. 膜科学与技术, 2024, 44(6): 145-157. [5]Chen M, Heijman S G J, Rietveld L C. State-of-the-art ceramic membranes for oily wastewater treatment: modification and application[J]. Membranes, 2021, 11(11): 888. [6]Wang D, Huang L, Sun H, et al. Enhanced photogenic self-cleaning of superhydrophilic Al2O3@GO-TiO2 ceramic membranes for efficient separation of oil-in-water emulsions[J]. Chem Eng J, 2024, 486: 150211. [7]Chen J, Ren J, Yang C, et al. Enhanced antifouling durability of zwitterionic polymer brush grafted ceramic membrane for sustainable oil/water separation applications[J]. Sep Purif Technol, 2025, 362(P3): 131963. [8]Lu D, Cheng W, Zhang T, et al. Hydrophilic Fe2O3 dynamic membrane mitigating fouling of support ceramic membrane in ultrafiltration of oil/water emulsion[J]. Sep Purif Technol, 2016, 165: 1-9. [9]Rezakazemi M, Dashti A, Riasat Harami H, et al. Fouling-resistant membranes for water reuse[J]. Environ Chem Lett, 2018, 16: 715-763. [10]Miller D J, Dreyer D R, Bielawski C W, et al. Surface modification of water purification membranes[J]. Angew Chem Int Ed, 2017, 56(17): 4662-4711. [11]Poli A, Sfeir R, Santos A F, et al. Backwashable dynamic membrane made of anchored CNT on SiC microfiltration membranes applied to oil in water emulsion filtration[J]. Sep Purif Technol, 2021, 278: 119566. [12]Paiman S H, Rahman M A, Uchikoshi T, et al. In situ growth of α-Fe2O3 on Al2O3/YSZ hollow fiber membrane for oily wastewater[J]. Sep Purif Technol, 2020, 236: 116250. [13]Barati N, Husein M M, Azaiez J. Modifying ceramic membranes with in situ grown iron oxide nanoparticles and their use for oily water treatment[J].J Membr Sci, 2021, 617: 118641. [14]严强, 陈奕山, 邱鸣慧, 等. 超声辅助的溶胶-凝胶法制备ZrO2纳滤膜[J]. 膜科学与技术, 2018, 38(6): 90-96. [15]Rezaei M, Mirkazemi S M, Alamolhoda S. The role of PVA surfactant on magnetic properties of MnFe2O34 nanoparticles synthesized by sol-gel hydrothermal method[J]. J Supercond Nov Magn, 2021, 34(5): 1397-1408. [16]马娟, 程从密, 刘琪, 等. 低成本多孔非对称陶瓷过滤膜的制备与性能研究进展[J]. 硅酸盐通报, 2022, 41(10): 3634-3646. [17]Dai C, Sun W, Chen X, et al. Preparation of hydrophobic PTFE/ceramic membranes featuring a tight and uniform pore size distribution through the solid-state sintering of PTFE nanoparticles[J]. Sep Purif Technol, 2024, 339: 126668. [18]Li Y X, Li P, Wu Y Z, et al. Preparation and antifouling performance of thin inorganic ultrafiltration membrane via assisted sol-gel method with different composition of dual additives[J]. Ceram Int, 2021, 47(2): 2180-2186. [19]Li A, Wang M, Sang H, et al. Enhancing anti-fouling performance of ceramic membranes through iron oxide modification for the separation of oil-containing fermentation broth[J]. Ceram Int, 2024, 50(19): 35993-36003. [20]Wang Y, Chen Z, Zhu Y, et al. An ultrathin Al2O3 ceramic membrane prepared by organic-inorganic blending with solvent evaporation and high-temperature sintering for highly efficient oil/water separation[J]. J Water Process Eng, 2025, 70: 107116. [21]戴永刚, 陆成龙, 张银凤, 等. 聚乙烯醇对溶胶-凝胶法氧化铝陶瓷膜制备的影响[J]. 中国陶瓷, 2022, 58(7): 53-59. [22]Mikhaylov V I. Optical and thermal properties of sol-gel Al(OH)3-Fe(OH)3-PVA composite films[J]. J Sol-Gel Sci Technol, 2019, 92: 282-292. [23]Yan C, Cheng Z, Wei J, et al. Efficient degradation of antibiotics by photo-Fenton reactive ceramic membrane with high flux by a facile spraying method under visible LED light[J]. J Clean Prod, 2022, 366: 132849. [24]Zou X, Gu S, Lu X, et al. Electroreduction of iron (Ⅲ) oxide pellets to iron in alkaline media: a typical shrinking-core reaction process[J]. Metall Mater Trans B, 2015, 46(3): 1262-1274. [25]王勇利, 陈亚飞, 王方建. 纳米Fe2O3改性聚丙烯纤维膜的制备及油水分离性能研究[J]. 当代化工研究, 2023(13): 171-173. [26]Wang X, Sun K, Zhang G, et al. Robust zirconia ceramic membrane with exceptional performance for purifying nano-emulsion oily wastewater[J]. Water Res, 2022, 208: 117859. [27]Luan W, Nie C, Chen X, et al. Effective construction of anti-fouling zwitterion-functionalized ceramic membranes for separation of oil-in-water emulsion based on PDA/PEI co-deposition[J]. J Environ Chem Eng, 2022, 10(5): 108396. |
|
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