Ceramic membranes with different pore sizes modified by silane and their oil-water separation performance |
Authors: GOU Limin, Duan Lijun, KE Wei, CHEN Xianfu, QIU Minghui, FAN Yiqun |
Units: 1. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China 2. Nanjing Membrane Material Industry Technology Institute Co., Ltd, Nanjing 211800, China |
KeyWords: ceramic membrane; hydrophobic surface; silane graft; oil-water separation |
ClassificationCode:TQ028.4 |
year,volume(issue):pagination: 2024,44(1):16-26 |
Abstract: |
Hydrophobic ceramic membranes with low surface energy are often used for containing-water oil separation, and the improvement of flux is the key to improve the economy of membrane separation process. In this study, hydrophobic ceramic membranes were prepared through organosilane modification. The impact of silane modification on the structure and oil-water separation performance of ceramic membranes with various pore sizes of 1000 nm, 100 nm, and 10 nm was investigated. We examined the changes in membrane surface micromorphology, wettability, and permeability resistance before and after modification for each pore size category. Additionally, we evaluated the stability of modified membranes in organic solvents, acid, and alkali. Subsequently, we assessed membrane performance in separating water-in-oil emulsions with varying water contents. The results show that the silane modification significantly increased the membrane permeability resistance for smaller pore sizes. Employing a low transmembrane pressure operation mode combined with high crossflow contributed to enhanced flux for modified membranes. Regarding W/O emulsion, when water content was 1000 mg/L, all three modified membranes achieved a water rejection exceeding 93%, while maintaining a permeate side water content below 70 mg/L. Among them, the 1μm modified membrane exhibited the highest flux at 375 L·m-2·h-1. However, when the volume fraction of water reached 10vol%, severe contamination occurred on the surface of the 1000 nm modified membrane resulting in significant drop in flux to only 14.1 L·m-2·h-1. Conversely, the 100 nm modified membrane showed less contamination and higher flux. |
Funds: |
国家重点研发计划项目(2022YFC2105101);国家自然科学基金(21921006,22078147);天津市合成生物技术创新能力提升项目(TSBICIP-KJGG-002);江苏省教育厅青蓝计划 |
AuthorIntro: |
苟立民(1999-),男,四川省巴中市人,硕士研究生,研究方向为陶瓷膜材料及应用,E-mail:goulimin2020025293@163.com |
Reference: |
[1] 尹延梅, 吴秀丽, 柯永文, 等. 膜法液压油过滤净化技术研究[J]. 膜科学与技术, 2021, 41(5):139-145. [2] Zhu X B, Dudchenko A, Gu X T, et al. Surfactant-stabilized oil separation from water using ultrafiltration and nanofiltration[J]. J Membr Sci, 2017, 529:159-169. [3] Tummons E N, Tarabara V V, Chew J W, et al. Behavior of oil droplets at the membrane surface during crossflow microfiltration of oil–water emulsions[J]. J Membr Sci, 2016, 500:211-224. [4] 李梅, 高能文, 范益群. 疏水陶瓷膜脱除油中水分的研究[J]. 膜科学与技术, 2012, 32(3):86-90. [5] Zhu YY, Lu Y Q, Yu H, et al. Super-hydrophobic F-TiO2@PP membranes with nano-scale “coral”-like synapses for waste oil recovery[J]. Sep Purif Technol, 2021, 267:118579. [6] Usman J, Othman M H D, Ismail A F, et al. An overview of superhydrophobic ceramic membrane surface modification for oil-water separation[J]. J Mater Res Technol, 2021, 12:643-667. [7] Song J L, Huang S, Lu Y, et al. Self-driven one-step oil removal from oil spill on water via selective-wettability steel mesh[J]. Acs Appl Mater Interfaces, 2014, 6(22):19858-19865. [8] 左继浩, 陈嘉慧, 文秀芳, 等. 用于分离油水乳液的先进材料[J]. 化学进展, 2019, 31(10):1440-1458. [9] Chen X F, Dai C W, Zhang T Y, et al. Efficient construction of a robust PTFE/Al2O3 hydrophobic membrane for effective oil purification[J]. Chem Eng J, 2022, 435(3):139472. [10] Yao X Y, Hou X B, Zhang R B. Flexible and mechanically robust polyimide foam membranes with adjustable structure for separation and recovery of oil-water emulsions and heavy oils[J]. Polymer, 2022,250:124889. [11] 杨思民, 王建强, 刘富. 油水分离膜研究进展[J]. 膜科学与技术, 2019, 39(3):132-141. [12] Ikhsan S N W, Yusof N , Aziz F, et al. Superwetting materials for hydrophilic-oleophobic membrane in oily wastewater treatment[J]. J Environ Manage, 2021, 290:112565. [13] Gao N W, Li M, Jing W H, et al. Improving the filtration performance of ZrO2 membrane in non-polar organic solvents by surface hydrophobic modification[J]. J Membr Sci, 2011, 375(1-2):276-283. [14] 李秀秀, 魏逸彬, 谢子萱, 等. Al2O3和SiC微滤膜的疏水改性及其油固分离性能研究[J]. 化工学报, 2019, 70(7):2737-2747. [15] He S J, Zhang Y Q, Bai Y L, et al. Gravity-driven and high flux super-hydrophobic/super-oleophilic poly(arylene ether nitrile) nanofibrous composite membranes for efficient water-in-oil emulsions separation in harsh environments[J]. Composites Part B, 2019, 177: 107439. [16] Monash P, Pugazhenthi G. Effect of TiO2 addition on the fabrication of ceramic membrane supports: a study on the separation of oil droplets and bovine serum albumin (BSA) from its solution[J]. Desalination, 2011:279:104-114. [17] Zhang D S, Abadikhah H, Wang J W, et al. Beta-SiAlON ceramic membranes modified with SiO2 nanoparticles with high rejection rate in oil-water emulsion separation[J]. Ceram Int, 2019, 45(4):4237-4242. [18] Gao N W, Fan Y Q, Quan X J, et al. Modified ceramic membranes for low fouling separation of water-in-oil emulsions[J]. J Mater Sci, 2016, 51(13):6379-6388. [19] George J K, Verma N. Super-hydrophobic/super-oleophilic carbon nanofiber-embedded resorcinol-formaldehyde composite membrane for effective separation of water-in-oil emulsion[J]. J Membr Sci, 2022, 654:120538. [20] 张凯滨, 罗平, 柯威, 等. 陶瓷膜在透平油脱水中的应用研究[J].膜科学与技术, 2023, 43(3):116-122. [21] Godin M, Williams P J, Tabard-Cossa V, et al. Surface stress, kinetics, and structure of alkanethiol self-assembled monolayers[J]. Langmuir, 2004, 20:7090-7096. [22] Jadhav S A. Self-assembled monolayers (SAMs) of carboxylic acids: an overview[J]. Cent Eur J Chem, 2011,9(3):369-378. [23] Gao W, Dickinson L, Grozinger C, et al. Self-assembled monolayers of alkylphosphonic acids on metal oxides[J]. Langmuir, 1996, 12:6429-6435. [24] 郭寒雨, 刘四华, 薛白, 等. 膜蒸馏用PDMS/PVDF中空纤维疏水膜的研制[J]. 膜科学与技术, 2019, 39(4):63-68+75. [25] Li Z, Wang X S, Bai H Y, et al. Advances in bioinspired superhydrophobic surfaces made from silicones: Fabrication and Application[J]. Polymer, 2023, 15(3):543. [26] Ding D, Mao H Y, Chen X F, et al. Underwater superoleophobic-underoil superhydrophobic Janus ceramic membrane with its switchable separation in oil/water emulsions[J]. J Membr Sci, 2018, 565:303-310. [27] Basak S, Barma S, Majumdar S, et al. Role of silane grafting in the development of a superhydrophobic clay-alumina composite membrane for separation of water in oil emulsion[J]. Ceram Int, 2022, 48(18):26638-26650. [28] Lue S J, Chow J, Chien C F, et al. Cross-flow microfiltration of oily water using a ceramic membrane: flux decline and oil adsorption[J]. Sep Sci Technol, 2009, 44(14):3435-3454. [29] Almojjly A, Johnson D, Hilal N. Investigations of the effect of pore size of ceramic membranes on the pilot-scale removal of oil from oil-water emulsion[J]. J Water Process Eng, 2019, 31:100868. [30] 张婷, 李雪, 熊峰, 等. 介孔陶瓷膜表面接枝氨基硅烷的孔径调节研究[J]. 膜科学与技术, 2016, 36(1):45-49+54. [31] 柯威, 高能文, 李梅, 等. 疏水性Al2O3膜表面的化学稳定性[J]. 南京工业大学学报(自然科学版), 2010, 32(6):45-49. [32] Schatzberg P. Solubilities of water in several normal alkanes from C7 to C16[J]. J Phys Chem, 1963, 67, 776-779. [33] Wei Y B, Xie Z X, Qi H. Superhydrophobic-superoleophilic SiC membranes with micro-nano hierarchical structures for high-efficient water-in-oil emulsion separation[J]. J Membr Sci, 2020, 601:117842. [34] Usman J, Othman M H D, Ismail A F, et al. Impact of organosilanes modifiedsuperhydrophobic-superoleophilickaolin ceramic membrane on efficiency of oil recovery from produced water[J]. J Chem Technol Biotechnol, 2020, 95(12):3300-3315. |
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