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利用具有临界溶解温度的体系开发用于超滤的高通量纳米复合聚苯砜/氧化多壁碳纳米管膜

Development of High Flux Nanocomposite Polyphenylsulfone/Oxidized Multiwalled Carbon Nanotubes Membranes for Ultrafiltration Using the Systems with Critical Solution Temperatures.

作者信息

Plisko Tatiana V, Burts Katsiaryna S, Bildyukevich Alexandr V

机构信息

Institute of Physical Organic Chemistry, National Academy of Sciences of Belarus, 220072 Minsk, Belarus.

出版信息

Membranes (Basel). 2022 Jul 22;12(8):724. doi: 10.3390/membranes12080724.

Abstract

The study deals with the investigation of the effect of the modification of polyphenylsulfone (PPSU) flat sheet membranes for ultrafiltration using oxidized multiwalled carbon nanotubes (O-MWCNT) in order to enhance membrane permeability and antifouling performance. The effect of O-MWCNT loading to the PPSU-polyethylene glycol (PEG-20,000, M = 20,000 g·mol)-polyvinylpyrrolidone (PVP K-30, M = 40,000 g·mol)-N-methy-2-pyrrolidinone (NMP) colloid systems on the phase state and viscosity was studied. It was found that PPSU-PEG-20,000-PVP K-30-O-MWCNT-NMP colloid systems feature a gel point (T = 35-37 °C) and demixing temperature (T = 127-129 °C) at which two bulk phases are formed and a polymer system delaminates. According to the study of the phase state and viscosity of these colloid systems, a method for the preparation of high flux PPSU membranes is proposed which includes processing of the casting solution at the temperature higher than gel point (40 °C) and using a coagulation bath temperature lower than gel point (25 °C) or lower than demixing temperature (40 °C and 70 °C). Membrane structure, topology and hydrophilic-hydrophobic balance were investigated by scanning electron microscopy (SEM), atomic force microscopy (AFM) and water contact angle measurements. The effect of coagulation bath temperature and O-MWCNT concentration on the membrane separation and antifouling performance in ultrafiltration of human serum albumin and humic acids solutions was studied. It was found that the modification of PPSU ultrafiltration membranes by O-MWCNTs yielded the formation of a thinner selective layer and hydrophilization of the membrane surface (water contact angle decreased from 53-56° for the reference PPSU membrane down to 33° for the nanocomposite membrane with the addition of 0.19 wt.% O-MWCNT). These changes resulted in the increase in membrane flux (from 203-605 L·m·h at transmembrane pressure of 0.1 MPa for the reference membrane up to 512-983 L·m·h for nanocomposite membrane with the addition of 0.19 wt.% O-MWCNT depending on coagulation bath temperature) which significantly surpasses the performance of PPSU ultrafiltration membranes reported to date while maintaining a high level of human serum albumin rejection (83-92%). It was revealed that nanocomposite membrane demonstrated better antifouling performance (the flux recovery ratio increased from 47% for the reference PPSU membrane up to 62% for the nanocomposite membrane) and higher total organic carbon removal compared to the reference PPSU membrane in humic acids solution ultrafiltration.

摘要

本研究旨在探究使用氧化多壁碳纳米管(O-MWCNT)对聚亚苯基砜(PPSU)平板超滤膜进行改性,以提高膜的渗透性和抗污染性能。研究了O-MWCNT负载量对PPSU-聚乙二醇(PEG-20,000,M = 20,000 g·mol)-聚乙烯吡咯烷酮(PVP K-30,M = 40,000 g·mol)-N-甲基-2-吡咯烷酮(NMP)胶体体系的相态和粘度的影响。结果发现,PPSU-PEG-20,000-PVP K-30-O-MWCNT-NMP胶体体系具有凝胶点(T = 35-37 °C)和分层温度(T = 127-129 °C),在此温度下会形成两个本体相,聚合物体系会分层。根据对这些胶体体系相态和粘度的研究,提出了一种制备高通量PPSU膜的方法,该方法包括在高于凝胶点(40 °C)的温度下处理铸膜液,并使用低于凝胶点(25 °C)或低于分层温度(40 °C和70 °C)的凝固浴温度。通过扫描电子显微镜(SEM)、原子力显微镜(AFM)和水接触角测量研究了膜的结构、拓扑结构和亲水-疏水平衡。研究了凝固浴温度和O-MWCNT浓度对人血清白蛋白和腐殖酸溶液超滤过程中膜分离和抗污染性能的影响。结果发现,用O-MWCNTs对PPSU超滤膜进行改性可形成更薄的选择性层,并使膜表面亲水化(水接触角从参考PPSU膜的53-56°降至添加0.19 wt.% O-MWCNT的纳米复合膜的33°)。这些变化导致膜通量增加(在0.1 MPa的跨膜压力下,参考膜的通量为203-605 L·m⁻²·h,添加0.19 wt.% O-MWCNT的纳米复合膜的通量根据凝固浴温度可达512-983 L·m⁻²·h),这在保持高水平的人血清白蛋白截留率(83-92%)的同时,显著超过了迄今为止报道的PPSU超滤膜的性能。结果表明,在腐殖酸溶液超滤中,纳米复合膜表现出更好的抗污染性能(通量恢复率从参考PPSU膜的47%提高到纳米复合膜的62%),并且与参考PPSU膜相比,总有机碳去除率更高。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/665c/9330833/3146e89d29ef/membranes-12-00724-g011.jpg

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