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Membranes · 2022 ·Vol. 12 ·期 11 ·1071 · IF 4.562

Tailoring Morphology and Properties of Tight Utrafiltration Membranes by Two-Dimensional Molybdenum Disulfide for Performance Improvement

Huali Tian,Xing Wu,Kaisong Zhang

To enhance the permeation and separation performance of the polyethersulfone (PES) tight ultrafiltration (TUF) membrane, two-dimensional molybdenum disulfide (MoS2) was applied as a modifier in low concentrations. The influence of different concentrations of MoS2(0, 0.25, 0.50, 1.00, and 1.50 wt%) on TUF membranes was investigated in terms of morphology, mechanical strength properties, permeation, and separation. The results indicate that the blending of MoS2tailored the microstructure of the membrane and enhanced the mechanical strength property. Moreover, by embedding an appropriate amount of MoS2into the membrane, the PES/MoS2membranes showed improvement in permeation and without the sacrifice of the rejection of bovine serum protein (BSA) and humic acid (HA). Compared with the pristine membrane, the modified membrane embedded with 0.5 wt% MoS2showed a 36.08% increase in the pure water flux, and >99.6% rejections of BSA and HA. This study reveals that two-dimensional MoS2can be used as an effective additive to improve the performance and properties of TUF membranes for water treatment.Keywords:tight ultrafiltration membrane;molybdenum disulfide;humic acid rejection;BSA rejection

CAS / MDL: 9048-46-8 1317-33-5
研究领域: 材料科学 · 环境工程
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JOURNAL OF MEMBRANE SCIENCE · 2021 · IF 8.742

Tuning of nanofiltration membrane by multifunctionalized nanovesicles to enable an ultrahigh dye/salt separation at high salinity

Huimin Zhou,Xuesong Li,Yang Li,Ruobin Dai,Zhiwei Wang

A nanofiltration (NF) membrane capable of efficiently separating dye and salt at high-salinity is of great interest for the effective treatment of the textile wastewater. However, existing NF membranes exhibit either an excessively high salt rejection or a compromised dye rejection at high salinity. To overcome these challenges, herein the highly uniform nanovesicles functionalized with positively-charged molecules and nonreactive polymers were employed to tune the surface charge density and pore size of the thin-film composite (TFC) NF membrane via interfacial polymerization. The tuning proved efficient to simultaneously reduce surface charge density and enlarge pore size to the desired extent, which enabled a very low retention of salts (∼7% for NaCl) while maintaining a rather high dye rejection (∼99.8% for Direct red 23) with a high salt/dye separation factor of 464. Additionally, the separation stability of the finely-tuned membrane was superior to most of other reported NF membranes when treating a high-salinity dye/salt mixture. Meanwhile, the water permeability of the modified TFC membrane was enhanced by a factor of 2.6, reaching up to 205.8 L m −2  h −1  MPa. This study paves a new route to the high-performance NF membrane for an effective treatment of the high-salinity textile wastewater.

研究领域: 环境工程 · 膜科学 · 水处理
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Tailoring the asymmetric structure of polyamide reverse osmosis membrane with self-assembled aromatic nanoparticles for high-efficient removal of organic micropollutants

Yan-Li Ji,Hong-Hao Lu,Bing-Xin Gu,Run-Feng Ye,Yong Zhou,Quan-Fu An,Cong-Jie Gao

The widespread occurrence of organic micropollutants (OMPs) in water has serious effects on the environment and human health. Recently, reverse osmosis (RO) membrane technology has been used for resolving this emerging concern, and the state-of-the-art polyamide RO membranes are normally fabricated by the interfacial polymerization method. Further reducing the energy consumption and operation cost, developing high-performance polyamide RO membranes will be the key for resolving the issue of effective removal of OMPs. Herein, a new strategy is proposed for fabricating robust and high-efficient polyamide RO membranes via the self-assembled aromatic nanoparticles (SANs) controlled interfacial polymerization (SANCIP) method. The membrane surface characteristics and interior microstructures of polyamide layer could be conveniently manipulated by regulating the SAN nanoparticles size and content. The SANs tuned polyamide membrane (PAM-SAN) with asymmetric structure, e.g., much looser and crumpled front surface and much denser and smooth rear surface, exhibits ultra-high water flux ~ 67.8 L∙m −2 ∙h −1 and satisfactory NaCl rejection (>98.3%), as well as very high OMPs rejection (>99.4%). Moreover, the PAM-SAN membrane has good stability and anti-fouling performance in long-term RO running process. This facile and cost-effective strategy provides a useful guideline in designing high-performance polyamide membranes with a vast potential in the removal of OMPs for advanced water treatment.

研究领域: 水处理 · 膜科学 · 环境工程 · 纳米技术
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JOURNAL OF MEMBRANE SCIENCE · 2022 · IF 10.53

A novel polyester-amide loose composite nanofiltration membrane for effective dye/salt separation: The effect of long molecule on the interfacial polymerization

Jun Cheng,Zheyu Li,Xian Bao,Ruijun Zhang,Suyao Yin,Wenqiang Huang,Kai Sun,Wenxin Shi

Loose nanofiltration (LNF) membrane with exclusively high dye rejection and inorganic salt permeation are remarkable method to treatment dye/salt wastewater for the achievement of zero liquid discharge. Herein, a long molecule bis-tris propane with amines and hydroxyl groups was firstly chosen as aqueous monomer in interfacial polymerization to fabricate a novel polyester-amide LNF membrane. Noteworthily, the investigation of morphology characterization and preparation conditions revealed that the size of molecule was a vital influence factor for the formation mechanism of unique loose structure of LNF made by long molecule. A new insight about the size of long molecule to form ultrathin thickness of self-repression layer on the formation mechanism of LNF was proposed in this work to replenish the previous theory. A series of characterization verified that the polyester-amide layer is negatively charged and hydrophilic due to the carboxyl and hydroxyl groups on the surface. Meanwhile, the tailored 0.3-LNF exhibited high water permeability (114.9 L m −2  h −1 ), dye rejection (98.83% RB 5) and low salt rejection (11.72% NaCl) under 0.5 MPa, which displayed good performance for the fractionation of dye/salt mixtures. In addition, the polyester-amide LNF membrane possesses a superior antifouling and stability performance.

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

Regulation of interfacial polymerization by organic base for high-permselective nanofiltration

Huiying Ding,Yuting Liu,Zhong Zhang,Yanjun Cheng,Jiahao Mo,Lu Elfa Peng,Cheng Xiang,Hongchang Pei,Xianhui Li

In the synthesis of the polyamide nanofiltration (NF) membrane, the hydrogen chloride is a by-product generated at the organic interface from interfacial polymerization , which reduces the reactivity of amine monomers due to protonation . Herein, a strategy of addition of an organic base in the organic phase to neutralize the H + was reported. The performances of the membranes produced using three organic bases with different chain lengths were explored. The results showed that the organic base neutralized the H + and promoted the rate of interfacial condensation reaction , which facilitated the formation of a dense and thin polyamide layer. Moreover, compared to control membrane, the membrane modified by organic base exhibited higher water permeance without sacrificing salt rejection. Higher diffusion rate of HCl through PES substrate compared to NF membrane indicated that HCl diffusion was mainly affected by the resistance of polyamide layer. Molecular simulations demonstrated that triethylamine (TEA) has lower energy barrier of neutralization and higher reaction heat in comparison with tripropylamine and N, N-diisopropylethylamine. The TEA modified membrane thereby displayed a permeance up to 24.3 L h −1  m −2  bar −1 and Na 2 SO 4 rejection of 98.8 %. This work provided a promising strategy for the regulation of interfacial polymerization in achieving high-permselective nanofiltration.

研究领域: 材料科学 · 环境工程
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2019 · IF 3.375

Enhancing Permeability of Thin Film Nanocomposite Membranes via Covalent Linking of Polyamide with the Incorporated Metal–Organic Frameworks

Hengrao Liu,Jing Gao,Guanhua Liu,Miyu Zhang,Yanjun Jiang

Thin film nanocomposite (TFN) membranes were invented in 2007 to enhance the permeability of thin film composite (TFC) membranes. Surface modification of nanofillers was a common method to improve the interaction and compatibility at polymer/nanofiller interfaces. Accordingly, as an amino-functionalized zirconium-based metal–organic framework (MOF), UiO-66-NH2 was synthesized and introduced into the preparation of TFN membranes via interfacial polymerization in this study. The superhydrophilic characteristic of UiO-66-NH2 made it possible to be well dispersed in aqueous solution and the amino groups on particle surfaces could react with 1,3,5-benzenetricarboxylic acid chloride (TMC) to form covalent interaction with polymer thus inhibiting the formation of nonselective defects at PA/nanofiller interfaces. The morphology images and FT-IR spectra revealed the PA selective layer successfully formed on the top of hydrolyzed polyacrylonitrile (HPAN) supports. The EDX characterization demonstrated UiO-66-NH2 nanoparticles were successfully introduced into the TFN membranes. The UiO-66-NH2 nanoparticles increased the surface hydrophilicity and roughness of the membranes, and provided additional passageways for mass transfer. Pure water permeability increased from 6.89 LMH/bar for TFC membrane to 14.55 LMH/bar for TFN-0.10 membrane indicating the distinct permeability elevation after the incorporation of UiO-66-NH2 nanoparticles. And the Na2SO4 rejection of TFN-0.10 membrane was up to about 99.0% and NaCl rejection was 38.1% at 4 bar, which was higher than that of TFN membrane incorporated with pristine UiO-66.

研究领域: 材料科学 · 化学工程 · 膜技术 · 纳米技术
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Chemistry-An Asian Journal · 2019 ·Vol. 15 ·期 15 ·2341-2345 · IF 3.698

Sub-10 nm Polyamide Nanofiltration Membrane for Molecular Separation

Junjun Hou,Meihuizi Jiang,Xiao He,Pengchao Liu,Chang Long,Lian Yu,Zhiwei Huang,Jin Huang,Lianshan Li,Zhiyong Tang

Graphical A sub-10 nm polyamide nanofiltration membrane was synthesized through interfacial polymerization due to the extremely low solubility of the ethidium bromide monomer in organic phase, which strictly limits the polymerization process at the interface of the water and hexane. Thanks to the ultrathin thickness, these membranes show excellent water permeance and high dye rejection. To separate small molecules from the solvent with high permeability and selectivity, the membrane process is thought to be highly effective with much lower energy consumption when compared to the traditional thermal-based separation process. To achieve high solvent permeance, a sub-10 nm thick polyamide nanofiltration membrane was synthesized through interfacial polymerization of ethidium bromide (EtBr) and trimesoyl chloride (TMC). Thanks to the extremely low solubility of the EtBr monomer in the organic phase, the polymerization process was strictly limited at the interface of the water and hexane, leading to an ultrathin polyamide membrane with a thickness down to sub-10 nm. When used in nanofiltration, these ultrathin membranes display ultrafast water permeation of 40 liter per square meter per hour per bar (L m −2 h −1 bar −1 ), and a high Congo red rejection rate of 93 %. This work demonstrates a new route to synthesize ultrathin polyamide membranes by the traditional interfacial polymerization.

CAS / MDL: 108-45-2
研究领域: 化学工程 · 材料科学 · 环境科学
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Triphenylamine-based COFs composite membrane fabricated through oligomer-triggered interfacial polymerization

Song Zhao,Nanxi Di,Ran Lei,Jixiao Wang,Zhi Wang

Covalent organic frameworks (COFs) are attractive innovative crystalline porous materials that have immense potential for the production of high-performance nanofiltration membranes. Although the conventional water-organic interfacial polymerization process has been broadly applied to fabricate COFs composite membranes on polymeric substrates, it cannot be applicable for COFs constructed by poorly water-soluble aromatic amine monomers . Herein, we report the fabrication of triphenylamine-based COFs composite membranes via an oligomer-triggered interfacial polymerization (OT-IP) process on a hydrolyzed polyacrylonitrile (HPAN) substrate, in which the interfacial reaction occurred between an acetic acid aqueous solution and an organic solution of 1,3,5-triformylphloroglucinol (Tp) in n-hexane and tris(4-aminophenyl)amine (TAPA) in mesitylene premixed in a short time. The Tp-TAPA oligomers generated during the premixing were characterized in terms of morphology and molecular weight. The TpTAPA film formation during the OT-IP process was in situ observed through an optical contact angle measurement device. The TpTAPA/HPAN composite membranes displayed a water permeance of 68.1 L⋅m −2 ⋅h −1 ·bar −1 , and the rejections of different dye (EBT, CR) and drug (DG, AG) molecules above 92.0%. In addition, the composite membrane showed excellent stability in acidic solution and continuous filtration for 75 h. The results indicated that the OT-IP approach is a feasible and efficient approach to fabricate triphenylamine-based COF composite membranes with water-insoluble monomers.

CAS / MDL: 5981-09-9
研究领域: 材料科学 · 化学工程 · 膜技术 · 纳米技术
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JOURNAL OF MEMBRANE SCIENCE · 2014 · IF 4.908

High flux polyethylene glycol based nanofiltration membranes for water environmental remediation

Xi Quan Cheng,Lu Shao,Cher Hon Lau

A hydrophilic thin-film-composite (TFC) nanofiltration (NF) membrane has been developed through the interfacial polymerization (IP) of amino-functional polyethylene glycol (PEG) and trimesoyl chloride. The selective layer is formed on a polyethersulfone (PES) support that is characterized using FTIR, XPS and SEM, and is dependent on monomer immersion duration, and the concentration of monomers and additives. The higher hydrophilicity alongside the larger pore size of the PEG-based selective layer is the key to a high water flux of 66.0   L   m −2   h −1 at 5.0   bar. With mean pore radius of 0.42   nm and narrow pore size distribution , the MgSO 4 rejections of the PEG based PA TFC NF membranes can reach up to 80.2%. The rejection rates for different salts of the novel membranes are in the order of R (MgCl 2 )> R (MgSO 4 )> R (NaCl)> R (Na 2 SO 4 ); indicating a membrane with positive surface charges. The pore sizes and water permeability of these membranes are tailored by varying the molecular weight and molecular architecture of amino-functional PEG. These newly developed TFC NF membranes show great potential for water softening, wastewater treatment and separation and purification of active, pharmaceutical molecules.

研究领域: 环境科学 · 材料科学
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

Optimal cross-linking of MXene-based membranes for high rejection and low adsorption with long-term stability for water treatment

Mao Mu,Nigel Graham,Wenzheng Yu,Kening Sun,Xiyan Xu,Ting Liu

The unique layered structure and abundant 2D nanochannels of MXene membranes have demonstrated outstanding permeability, indicating their great potential in the field of water treatment . However, their unstable interlayer spacing and irregular layer structure have limited their ability to separate small molecular pollutants effectively. In this study, we successfully prepared composite MXene membranes with high rejection and low adsorption properties by exploiting the differences in the surface functional groups and chain lengths of dopamine (DA) and polyethylene glycol (PEG) through an optimal cross-linking approach. These composite membranes exhibited excellent stability in terms of interlayer spacing and mitigated the adverse effects of stacking defects. Compared to MXene membranes, the composite membranes achieved a 1.76-fold increase in dye rejection efficiency, reaching 98.7% at most, with an adsorption ratio of only 1.8%. Moreover, outstanding performances were also exhibited in pressure and concentration load tests. Furthermore, in the context of forward osmosis applications, the composite membranes demonstrated excellent Na + rejection of 99.9%. More importantly, these membranes showed no performance deterioration throughout 50 filtration cycles, with only a slight increase in permeance of 19.3% over a 38-day testing period. Thus, this work presents a novel solution for fabricating MXene composite membranes with low swelling, minimal defects, and high stability, enhancing its potential in the field of water and wastewater treatment .

研究领域: 材料科学 · 水处理工程 · 环境科学
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Enhanced molecular sieving performance of thick graphene membranes self-assembled from weakly-oxidized graphene nanosheets

Shuo Li,Wenyu Wu,Huaxin Ma,Zhao Zhang,Yu Gu,Jingjie Zhang,Ruijun Zhang

Graphene oxide (GO)-based membranes have attracted extensive attention in water purification but still face great challenge due to their poor service life. To overcome this issue, weakly oxidized graphene nanosheets have been chemically exfoliated from natural graphite via a newly-developed strategy for preparing layer-tunable graphene. When an 80 μm-thick graphene membrane is assembled from the graphene nanosheets with an average layer number of 3, it exhibits a high rejection rate of 99.9 % for Rhodamine B and a water flux of up to 3452.6 L m −2 h −1 bar −1 . This should be ascribed to the unique hierarchically nanochannel structure within the membrane. This finding may provide a new insight into the design and fabrication of the thick membrane having excellent sieving performance. Furthermore, the rejection rate of RB can be maintained at 99.9 % even after 24 cycles of filtrations, demonstrating a superior service performance for the membrane.

研究领域: 材料科学 · 环境工程
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RSC Advances · 2014 ·Vol. 4 ·期 95 ·52808-52814 · IF 3.708

Polyelectrolyte complex nanofiltration membranes: performance modulation via casting solution pH

Qiang Zhao,Yan-Li Ji,Jia-Kai Wu,Ling-Ling Shao,Quan-Fu An,Cong-Jie Gao

Nanofiltration (NF) membranes were prepared from a solution processable polyelectrolyte complex (PEC) between sodium carboxymethyl cellulose (CMCNa) and poly(2-methacryloyloxy ethyl trimethylammonium chloride) (PDMC). Electrostatic complexation structures of the PEC were studied by light transmittance and field emission electron scanning microscopy (FESEM). It is found that the electrostatic complexation structure of the PEC membranes determines their NF performance, which is conveniently tailored via the pH values of casting solutions. For membranes prepared at the optimum solution pH 2.1, their water flux and salt rejection to K2SO4 (1 g L−1) are 18 g m−2 h−1 and 97%, respectively, when the operation pressure and temperature are 0.6 MPa and 25 °C. Both the water permeability and the salt selectivity are substantially improved compared to the pristine CMCNa NF membrane. In addition, antifouling performance of the PEC membrane is improved, coupled with an exceptional stability versus the operation time.

研究领域: 材料科学 · 环境工程
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