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Journal of Materials Chemistry A · 2014 ·Vol. 3 ·期 6 ·2650-2657 · IF 0

Mussel-inspired tailoring of membrane wettability for harsh water treatment

Zhen-Xing Wang,Cher-Hon Lau,Nai-Qing Zhang,Yong-Ping Bai,Lu Shao

Novel hybrid coatings with excellent wettability are architecturally constructed on the surfaces of different types of separation membranes via simultaneous polymerization of mussel-inspired dopamine and hydrolysis of commercially available and low-cost silane through a highly efficient one-step approach. After coating with the designed hybrid coatings, the ultrafiltration (UF) membranes possess high hydrophilicity and excellent dry storage ability while the microfiltration (MF) membranes are endorsed with superhydrophilicity and underwater superoleophobicity. Such unique UF and MF membranes can be deployed for treating protein-rich water with drastically enhanced functions and separating oily water (oil-in-water emulsion) under atmospheric conditions with ultrahigh water flux and superior antifouling abilities. This versatile strategy to tailor membrane surface wettability paves the way for separation membranes to be used in harsh water environmental remediation and greatly stimulates the rapid development of mussel-inspired pDA based hybrid materials for advanced applications.

研究领域: 材料科学 · 环境科学 · 生物仿生学
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CHINESE JOURNAL OF POLYMER SCIENCE · 2011 ·Vol. 30 ·期 2 ·152-163 · IF 0.478

Hydrophilic nanofiltration membranes with self-polymerized and strongly-adhered polydopamine as separating layer

Li Xiao-lin,Zhu Li-ping,Jiang Jin-hong,Yi Zhuan,Zhu Bao-ku,Xu You-yi

Inspired by the self-polymerization and strong adhesion characteristics of dopamine in aqueous conditions, a novel hydrophilic nanofiltration (NF) membrane was fabricated by simply dipping polysulfone (PSf) ultrafiltration (UF) substrate in dopamine solution. The changes in surface chemical composition and morphology of membranes were determined by Fourier transform infrared spectroscopy (FTIR-ATR), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and atomic force microscopy (AFM). The experimental results indicated that the self-polymerized dopamine formed an ultrathin and defect-free barrier layer on the PSf UF membrane. The surface hydrophilicity of membranes was evaluated through water contact angle measurements. It was found that membrane hydrophilicity was significantly improved after coating a polydopamine (pDA) layer, especially after double coating. The dyes filtration experiments showed that the double-coated membranes were able to reject completely the dyes of brilliant blue, congo red and methyl orange with a pure water flux of 83.7 L/(m 2 ·h) under 0.6 MPa. The zeta potential determination revealed the positively-charged characteristics of PSf/pDA composite membrane in NF process. The salt rejection of the membranes was characterized by 0.01 mmol/L of salts filtration experiment. It was demonstrated that the salts rejections followed the sequence: NaCl < Na 2 SO 4 < MgSO 4 < MgCl 2 < CaCl 2 , and the rejection to CaCl 2 reached 68.7%. Moreover, the composite NF membranes showed a good stability in water-phase filtration process.

研究领域: 材料科学 · 环境工程
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CHEMOSPHERE · 2020 · IF 5.778

Effects of feed solution characteristics and membrane fouling on the removal of THMs by UF/NF/RO membranes

Chao Fang,Tian Ou,Xingyu Wang,Min Rui,Wenhai Chu

Ultrafiltration (UF), nanofiltration (NF) and reverse osmosis (RO) are widely used in drinking water treatment and wastewater recycling. However, limited information was available regarding their performance in removing trihalomethanes (THMs). The present study investigated the effect of feed solution characteristics and membrane fouling on THM removal by UF/NF/RO membranes. The results indicated that THMs were poorly removed by UF membrane, and the removal was dominated by hydrophobic adsorption. In contrast, high removal of THMs was observed for NF/RO membranes, which was contributed by both size exclusion and hydrophobic adsorption. By comparing the adsorption of THMs on NF/RO membranes at different feed concentration, it was found that the role of hydrophobic adsorption was more important at lower feed concentration. The removal of THMs by UF/NF/RO membranes increased with increasing feed concentration, which can be ascribed to the enhanced diffusion at higher concentration gradient. With increasing ionic strength, THM removal was decreased significantly for UF membrane, but the removal by NF/RO membranes remained largely unchanged. By comparing THM removal by clean and fouled membranes, the effect of membrane fouling was examined. The removal of most THMs (except trichloromethane) decreased after fouling for UF membrane, whereas decreased removal was only observed for iodinated THMs for fouled NF/RO membranes.

研究领域: 环境科学 · 水处理工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2018 · IF 3.927

From ultrafiltration to nanofiltration: Nanofiltration membrane fabricated by a combined process of chemical crosslinking and thermal annealing

Chunli Liu,Yuxuan Sun,Zhenbin Chen,Suobo Zhang

An integrally skinned dense ultrafiltration (UF) membrane was prepared using partially di-quaternized poly(sulfone- co -ethernitrile) random copolymer (PSF- co -DQAPEN) via classical nonsolvent induced phase inversion process (NIPS). Then the original UF membrane was molecularly restructured through a combined process of chemical quaternization-crosslinking reaction and thermal annealing for the preparation of a crosslinked nanofiltration (NF) membrane, in which p -xylylene dichloride (PXDC) and isopropanol were employed as crosslinking agent and nonsolvent treating medium, respectively. The influence of reaction time and crosslinker concentration on membrane performance were investigated. X-ray photoelectron spectroscopy (XPS) of membrane surface and solubility test of membrane were employed to study the chemical composition and crosslinking properties of membranes, and those results revealed that the original membrane had been successfully crosslinked after this post treatment process. The separation performance of membrane was ultimately changed from UF-level to NF-level after the quaternization-crosslinking reaction and thermal annealing treatment process. The optimum crosslinked NF membrane possessed MgCl 2 rejection of 98.2% and water permeate flux of 4.12 L m −2  h −1  bar −1 . Moreover, owning to the excellent chemical stability of membrane material, the crosslinked membrane had outstanding resistance to chlorine, acid and base, thus it can be used for water softening and removing of positive dyes. Given the convenience and feasibility of this modification method, integrally skinned NF membrane could be easily fabricated via the post chemical crosslinking and thermal annealing process of UF membrane using proper treating approaches.

CAS / MDL: 3779-42-8 623-25-6
研究领域: 材料科学 · 环境工程
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Journal of Water Process Engineering · 2023 · IF 7

Nanofiltration membrane with a zwitterion-g-C3N4 composite interlayer for Mg2+/Li+ separation

Lei Ma,Qiuyan Bi,Wanji Zhou,Xingliang Liu,Fuju Qi,Hao Zhang,Yifan Gao,Shiai Xu

Nanofiltration (NF) membrane with high selectivity and permeance is important for recovering lithium from salt lake brine. In this work, sandwich-like NF membranes were prepared using polyamide (PA) as the interfacial polymerization (IP) layer, dopamine (DA) and zwitterion-g-C 3 N 4 as the composite interlayer and polyethersulfone (PES) ultrafiltration (UF) membrane as the substrate. Three NF membranes were prepared with different zwitterion-g-C 3 N 4 : M3 membrane modified with C 5 H 12 ClNO 2 -g-C 3 N 4 , M4 membrane modified with C 12 H 24 N 2 O 4 S-g-C 3 N 4 and M5 membrane modified with C 19 H 39 NO 2 -g-C 3 N 4 , and their physical and chemical properties, separation capacity, and antifouling behaviour were analyzed. The zwitterion-g-C 3 N 4 composite interlayer improves the hydrophilicity and pore structure of NF membranes. The water contact angle (CA) of M5 membrane is 25.5°and its pore size is 0.49 nm. M5 membrane shows a high retention rate of 96.66 % for Mg 2+ in mixed salt solution (Mg 2+ /Li +  = 84) and performs well in salt lake brine with a rejection of 97.90 % to Mg 2+ . The flux recovery ratio (FRR) can be kept above 93 %. This study may give ideas for the preparation of composite NF membrane for water softening and lithium utilization.

研究领域: 材料科学 · 环境科学 · 化学工程
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Desalination and Water Treatment · 2016 · IF 1.272

Desalinated seawater into pilot-scale drinking water distribution system: chlorine decay and trihalomethanes formation

Xunchao Li,Cong Li,Mingda Bayier,Taotao Zhao,Tuqiao Zhang,Xinbo Chen,Xinwei Mao

Residual chlorine decay and trihalomethanes (THM) formation of desalinated seawater by ultrafiltration (UF) and nanofiltration (NF) membranes in a pilot-scale water distribution system (DWDS) were investigated. Three-dimensional fluorescent features of two source waters including NF permeate and municipal water were studied. Sixteen groups of data-sets were obtained to explore the effects of initial chlorine concentration (ICC), dissolved organic carbon (DOC), and temperature on chlorine decay and THM formation in laboratory conditions and pilot-scale DWDS, respectively. A first-order model was applied to evaluate the chlorine decay of desalinated seawater and a new model combining ICC, DOC concentration, and temperature was obtained to determine the first-order decay coefficient. Other seven models describing the kinetics of chlorine decay were also applied and compared in this study. Total trihalomethanes (TTHM) formation kinetics was studied and first-order model was suggested to describe this formation. The relationship between TTHM formation and chlorine demand was demonstrated and the results showed that second-order polynomial model better described the relationship.

研究领域: 环境科学 · 水处理工程
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Journal of Environmental Sciences · 2023 · IF 6.9

Ultrathin organic solvent nanofiltration membrane with polydopamine-HKUST-1 interlayer for organic solvent separation

Haike Li,Xindong Li,Guozai Ouyang,Lijinhong Huang,Lang Li,Wenhao Li,Wanfu Huang,Duokun Li

Polydopamine (PDA) and metal-organic skeleton HKUST-1 were co-deposited on the base membrane of hexamethylenediamine (HDA)-crosslinked polyetherimide (PEI) ultrafiltration membrane as the interlayer, and high-throughput organic solvent nanofiltration membrane (OSN) was prepared by interfacial polymerization and solvent activation reaction. The polyamide (PA) layer surface roughness from 28.4 nm in PA/PEI to 78.3 nm in PA/PDA-HKUST-1 0.6 /PEI membrane, reduced the thickness of the separation layer from 79 to 14 nm, and significantly improved the hydrophilic, thermal and mechanical properties. The flux of the PA/PDA-HKUST-1 0.6 /PEI membrane in a 0.1 g/L Congo red (CR) ethanol solution at 0.6 MPa test pressure reached 21.8 L/(m 2 ·hr) and the rejection of CR was 92.8%. Solvent adsorption test, N, N-dimethylformamide (DMF) immersion experiment, and long-term operation test in ethanol showed that the membranes had high solvent tolerance. The solvent flux test demonstrated that, under the test pressure of 0.6 MPa, the flux of different solvents ranked as follows: methanol (56.9 L/(m 2 ·hr)) > DMF (39.6 L/(m 2 ·hr)) > ethanol (31.2 L/(m 2 ·hr)) > IPA (4.5 L/(m 2 ·hr)) > N - hexane (1.9 L/(m 2 ·hr)). The ability of the membranes to retain dyes in IPA/water dyes solution was also evaluated. The flux of the membrane was 30.4 L/(m 2 ·hr) and the rejection of CR was 91.6% when the IPA concentration reached 50%. This OSN membrane-making strategy is economical, environment-friendly and efficient, and has a great application prospect in organic solvent separation systems.

研究领域: 材料科学 · 化学工程 · 环境科学
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DESALINATION · 2020 · IF 7.098

How to fabricate a negatively charged NF membrane for heavy metal removal via the interfacial polymerization between PIP and TMC?

Jiayu Tian,Hailin Chang,Shanshan Gao,Ruijun Zhang

The potential toxicity of heavy metals arising from the discharge of industrial wastewater has become a serious public concern. Fabrication of a thin film composite (TFC) NF membrane with desirable rejection of heavy metal ions is an attracting route to solve this problem. Hereon, we proposed a facile strategy for fabricating a TFC NF membrane with excellent heavy metal removal. The ratio of PIP and TMC was greatly enlarged by decreasing the concentration of TMC to an exceptional low extent. Thus a polyamide film with weak electronegativity and small pore size was successfully constructed on an ultrafiltration substrate membrane. Comprehensive characterizations were adopted to reveal the micro-variation of the resulted NF membranes when regulating TMC concentration . The optimized membrane prepared only with PIP and TMC can exhibit a high pure water permeability of 14.6 L m −2  h −1  bar −1 , desirable rejection of over 98% against Ni 2+ , Zn 2+ , Cu 2+ , and >92.7% against Cd 2+ . This performance could go beyond most of the reported candidates which were prepared with other complicated methods. The simplicity, low cost and scaling up feasibility of the current strategy is expected to well meet the requirements of industrial production of TFC NF membrane for heavy metal removal.

研究领域: 环境科学 · 材料科学
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DESALINATION · 2023 · IF 9.9

An antifouling loose nanofiltration membrane prepared by cross-linking HPAN ultrafiltration membrane with zwitterionic polymer PEI-CA for efficient dye desalination

Shao-Lu Li,Yaxu Guan,Yiwen Qin,Youcai Chen,Dandan Cheng,Genghao Gong,Yunxia Hu

In this study, a novel antifouling loose nanofiltration (LNF) membrane was prepared by the cross-linking and grafting of hydrolyzed polyacrylonitrile ultrafiltration (HPAN UF) substrate with a polyethylenimine (PEI) based zwitterionic polymer PEI-CA through the covalent amide bond. The successful introduction of PEI-CA was verified by various techniques. The tailored membrane HPAN-PEICA exhibited ultra-high water permeance (73.5 L m −2  h −1  bar −1 ) and meanwhile maintained excellent rejection (~99.9 %) for dye Brilliant Blue R (BBR), Methyl Blue (MB), Congo red (CR) and Chrome Black T (CBT). In addition, it exhibited ultralow rejection (below ~6 %) towards the inorganic salts (NaCl, Na 2 SO 4 , MgCl 2 and MgSO 4 ), with excellent dye/salt selectivity of ~65. The as-fabricated membrane HPAN-PEICA was proved having good long-term operation stability and pressure resistance properties. Dynamic fouling experiments confirmed that the membrane HPAN-PEICA presented excellent antifouling performance towards four typical model foulants (LYZ, SA , HA and BSA). Over all, we believed that the tailored LNF membrane HPAN-PEICA having great application prospects in textile effluent treatment.

研究领域: 材料科学 · 环境工程
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Coatings · 2021 ·Vol. 11 ·期 2 ·184 · IF 2.881

Euler’s Numerical Method for Ions Rejection Reassessment of a Defect-Free Synthesized Nanofiltration Membrane with Ultrathin Titania Film as the Selective Layer

Chabi Noël Worou,Jing Kang,Jimin Shen,Arcadius Degan,Pengwei Yan,Weiqiang Wang,Yingxu Gong,Zhonglin Chen

Titanium (Ti) nanoparticles (NPs) were successfully seeded on the platform of a polyacrylonitrile (PAN) ultrafiltration (UF) membrane previously coated with bio-glue (a co-deposition of dopamine hydrochloric bicarbonate buffer having undergone pyrocatechol deprotonation). The tools in vogue, especially field emission scanning electron microscopy (FESEM), energy dispersive spectroscopy (EDS), and atomic force microscopy (AFM), have made it possible to fully characterize the structure of the new organic-inorganic nanofiltration (NF) membrane, namely NF_PAN_Ti. A soft computing model has been applied to make commonplace the complex and implicit extended Nernst–Planck equations that govern the transport of ions through NF membranes. Euler’s numerical method was applied with a small step-size and the results obtained were very interesting. The filtration velocity approach of GUEROUT-ELFORD-FERRY helped to estimate the average pore size of NF_PAN_Ti torp= 0.538 nm. A six-day test carried out on NF_PAN_Ti demonstrated its long-term stability and showed a steady-rejection rate of 89.3% of MgCl2salt and permeate flux of 56 L·m−2·h−1. The Euler’ numerical method corroborated perfectly the experimental findings since the relative error was found to be very low at 0.33% for Cl−and 0.09% for Mg2+(RE << 0.1). These practical prediction tools may henceforth help in the choice and calibration of next-generation NF membranes’ synthesis.

研究领域: 材料科学 · 环境工程 · 计算模拟
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Alkaline pre-treatment enables controllable downcycling of Si-Al fouled end-of-life RO membrane to NF and UF membranes

Hailan Wang,Ya Xu,Bozhan Ma,Wenxuan Zou,Jin Zeng,Ruobin Dai,Zhiwei Wang

Environmental and economic concerns necessitate the recycle of end-of-life (EOL) reverse osmosis (RO) membranes. Controlled downcycling of EOL RO membrane to nanofiltration (NF)-like or ultrafiltration (UF)-like membrane through regulating sodium hypochlorite (NaClO) exposure doses has been developed in recent years. However, the impact of foulants on the chlorination-based membrane downcycling is often overlooked. An alkaline-NaClO treatment strategy was employed to downcycle Si-Al complex-fouled EOL RO membrane. Alkaline cleaning not only partially removed Si-Al complex foulants via dissolution, but also converted Al 2 O 3 ·SiO 2 to Al-O-Si amorphous oxides . Subsequent NaClO treatment gradually deconstructed the Si-Al complex fouling layer by dissolving Al contained in Al-O-Si amorphous oxides and degraded the polyamide (PA) layer with extended exposure time, resulting in membrane with loose NF-like characteristic. Moreover, the conversion of Al-contained component with alkaline pre-treatment prevented Al 3+ -catalyzed degradation of PA layer and ensure controlled downcycling. For the downcycling to UF-like membrane, complete removal of PA layer with sufficient chlorine oxidation was essential while alkaline pre-treatment process was optional. Both downcycled loose NF-like and UF-like membranes exhibited satisfactory filtration and antifouling performance. Our study presents an effective and robust protocol for controllable downcycling of EOL RO membrane with alkaline pre-treatment based on their fouling characteristic.

CAS / MDL: 68-12-2 151-21-3
研究领域: 环境科学 · 材料科学 · 水处理工程
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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

High-flux, high-selectivity loose nanofiltration membrane mixed with zwitterionic functionalized silica for dye/salt separation

Yatao Zhang,Qiangqiang Song,Xu Liang,Jing Wang,Yuanli Jiang,Jindun Liu

A kind of charged nano-material SiO 2 -SBMA was prepared by reverse atom transfer radical polymerization (RATRP) with nano SiO 2 and 2-methacryloyloxy ethyl dimethyl (3-sulfopropyl)-ammonium hydroxide sulfobetaine methacrylate (SBMA). This material was dispersed with polyvinylpyrrolidone (PVP) and polyethersulfone (PES) in N, N-dimethylacetamide (DMAc) to obtain a casting solution, with which the loose nanofiltration (NF) membrane SiO 2 -PSBMA/PES was constructed using phase inversion on a sheet of glass with the automatic film applicator. The membrane structure and separation performance were investigated. The results indicated that the surface roughness, hydrophilicity, pure water flux and permeability selectivity of the loose NF membrane all improved. When the addition amount of SiO 2 -PSBMA was 0.5%, the order for retention of inorganic salts was R (Na 2 SO 4 ) > R (NaCl) > R (MgCl 2 ), which exhibited typical characteristics of the negatively charged membrane. At 0.4 MPa, the rejection of the membrane for Na 2 SO 4 was 11.4%. The rejection of reactive black 5 (RB5) and reactive green 19 (RG19) were 97.9% and 99.0%, and the corresponding permeation flux were 32.3 L m −2 h −1 bar −1 and 28.1 L m −2 h −1 bar −1 , respectively. The prepared membrane had higher flux and selectivity in dye wastewater treatment and was expected to be used in the treatment of salt-containing dye wastewater.

研究领域: 材料科学 · 环境工程 · 化学工程
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