于银瑞,闫超,曲琦,张先华,张子明,何燕,徐瑾.磁场诱导低维磁性碳材料对聚砜膜结构及流通特性的影响[J].表面技术,2023,52(11):355-365.
YU Yin-rui,YAN Chao,QU Qi,ZHANG Xian-hua,ZHANG Zi-ming,HE Yan,XU Jin.Effects of Magnetic Field-induced Low-dimensional Magnetic Carbon Materials on the Structure and Flow Characteristics of Polysulfone Membranes[J].Surface Technology,2023,52(11):355-365 |
| 磁场诱导低维磁性碳材料对聚砜膜结构及流通特性的影响 |
| Effects of Magnetic Field-induced Low-dimensional Magnetic Carbon Materials on the Structure and Flow Characteristics of Polysulfone Membranes |
| 投稿时间：2022-09-09 修订日期：2023-03-08 |
| DOI：10.16490/j.cnki.issn.1001-3660.2023.11.030 |
| 中文关键词: 磁性碳纳米材料 微反应器 聚砜 磁场诱导 混合基质膜 |
| 英文关键词:magnetic carbon nanomaterials microreactor polysulfone magnetic field-induced hybrid matrix membrane |
| 基金项目:山东省泰山学者项目(ts20190937) |
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| Author | Institution |
| YU Yin-rui | School of Mechanical and Electrical Engineering, Qingdao University of Science and Technology, Shandong Qingdao 266100, China |
| YAN Chao | School of Mechanical and Electrical Engineering, Qingdao University of Science and Technology, Shandong Qingdao 266100, China |
| QU Qi | School of Mechanical and Electrical Engineering, Qingdao University of Science and Technology, Shandong Qingdao 266100, China |
| ZHANG Xian-hua | School of Mechanical and Electrical Engineering, Qingdao University of Science and Technology, Shandong Qingdao 266100, China |
| ZHANG Zi-ming | School of Mechanical and Electrical Engineering, Qingdao University of Science and Technology, Shandong Qingdao 266100, China |
| HE Yan | School of Mechanical and Electrical Engineering, Qingdao University of Science and Technology, Shandong Qingdao 266100, China |
| XU Jin | School of Mechanical and Electrical Engineering, Qingdao University of Science and Technology, Shandong Qingdao 266100, China |
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| 中文摘要: |
| 目的 在膜的形成过程中，利用磁场力将亲水性磁性碳纳米材料吸引至膜表面，可以在膜表面附加亲水性和磁性，提高膜的渗透通量和截留率，改善膜污染问题。方法 将氧化石墨烯/碳纳米管混合溶液与Fe3+和Fe2+的混合溶液通入微反应器中预混合后，利用一步水热法引入四氧化三铁(Fe3O4)，制备具有优异磁性能的磁性碳纳米材料(MCN)，并将其共混于聚砜(PSF)基底中，采用磁场诱导非溶剂致相分离法(NIPS)制备磁性混合基质膜(PSF/MCN)。对MCN的形貌结构及磁性等进行表征，并通过改变PSF的浓度研究磁场作用下MCN的定向迁移对膜表面形貌结构及性能的影响。结果 亲水性磁性MCN的饱和磁化强度高达53.17 emu/g(1 emu/g=1 A.m2/kg)，表现出超顺磁性，且MCN在磁场作用下向膜表面定向移动。在相同的磁场强度下，不同聚砜浓度的膜表面表现出不同的形貌特征，并在聚砜的质量分数从15%升至17.5%的过程中，膜表面粗糙度的构成由细微密集的波动形貌转变为宽泛的浮动形貌。此外，MCN的加入改善了膜的内部结构和流通特性，当PSF的质量分数为15%时，膜的平均孔径从0.034 1 μm增至1.186 5 μm。与同浓度下的纯PSF膜相比，PSF/MCN的亲水角分别降低了18.34%、15.37%、14.69%、18.43%，其纯水通量分别增加了32.51%、23.62%、167.27%、233.88%，且它对牛白蛋白(BSA)的截留率均高达90%以上。结论 在磁场力的作用下，MCN向分离膜表面迁移，大大增加了膜表面亲水基团的数量，提高了分离膜的亲水性和渗透性。同时，MCN均匀分散在膜表面，形成了一层保护膜，提高了膜的分离特性和抗污染性。 |
| 英文摘要: |
| The magnetic force is used to attract hydrophilic magnetic carbon nanomaterials to the membrane surface during the formation of the membrane, which can attach hydrophilicity and magnetism to the membrane surface. This changes the physicochemical properties of the membrane surface, improves the permeate flux of the membrane, and solves or minimizes membrane contamination problems. Magnetic carbon nanomaterials (MCN) with excellent magnetic properties were prepared by introducing triiron tetroxide (Fe3O4) by a one-step hydrothermal method after premixing the graphene oxide/carbon nanotube mixture solution with Fe3+ and Fe2+ by passing it into a microreactor. The microreactor could provide microchannels and anaerobic environment to protect Fe2+ from oxidation while achieving uniform mixing of the two solutions. The one-step hydrothermal method provided a mild environment to promote the complete nucleation and growth of Fe3O4, and the magnetic carbon nanomaterials with uniform Fe3O4 distribution could be prepared quickly and easily. The magnetic hybrid matrix membrane (PSF/MCN) was prepared by magnetic field-induced non-solventogenic phase separation (NIPS) with co-blending MCN in polysulfone (PSF) substrate. The morphological structure and magnetic properties of MCN were characterized, and the effect of the directional migration of MCN on the morphological structure and properties of the film surface was investigated by changing the PSF concentration. The results showed that the saturation magnetization strength of hydrophilic magnetic MCN was as high as 53.17 emu/g (1 emu/g=1 A.m2/kg), which exhibited superparamagnetism and the MCN moved toward the membrane surface under the action of magnetic field. The membrane surfaces with different PSF contents exhibited different morphological characteristics under the same magnetic field strength, and the composition of membrane surface roughness changed from fine and dense fluctuations to broad floating during the increase of PSF concentration from 15% to 17.5%. It was shown that when the PSF concentration was between 15% and 17.5%, the MCN on the membrane surface changed from relatively complete movement to the surface to incomplete movement to the surface, and the change of PSF concentration affected the shedding of MCN on the membrane surface. In addition, the addition of MCN improved the internal structure and circulation characteristics of the membrane, and the average pore size of the membrane increased from 0.034 1 nm to 1.186 5 nm when the PSF content was 15%. Compared with pure PSF membranes at the same concentration, the hydrophilic angle of PSF/MCN decreased by 18.34%, 15.37%, 14.69%, 18.43%, and its pure water flux increased by 32.51%, 23.62%, 167.27%, 233.88% and its retention rate of bovine albumin (BSA) was above 90%, which exhibited good selective permeability. The addition of MCN improves the hydrophilicity of the separation membrane, thus facilitating the rapid phase transition process. In addition, under the action of magnetic field force, MCN migrates to the surface of the separation membrane, which greatly increases the amount of hydrophilic groups on the membrane surface and improves the permeation characteristics of the separation membrane. At the same time, MCN is uniformly dispersed on the membrane surface, which nearly forms a protective film and improves the separation characteristics and contamination resistance of the membrane. |
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