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JOURNAL OF MEMBRANE SCIENCE · 2025 · IF 9

Highly efficient MnO2-modified antifouling loose nanofiltration membrane for dye/salt separation

Yanchuan Zhang,Yali Zhao,Yu Liu

Loose nanofiltration (NF) membranes are promising in textile wastewater treatment due to their selective separation capabilities for dyes and salts. However, their widespread applications are hindered by complex manufacturing processes and membrane fouling. This work focuses on fabricating antifouling loose NF membranes using a facile method. Thereinto, amine-functionalized loose NF matrixes were first prepared using polyelectrolyte-complex induced phase inversion, where polyethyleneimine (PEI) in a coagulation bath as an inducer triggered an instantaneous phase inversion via electrostatic interactions with sulfonated polysulfone (SPSF) in dope solution. The acquired NF matrix has a dense skin layer with a mean pore size of 0.72 nm, endowing it with excellent dye retention. Consequently, the Fenton catalyst, MnO 2 , was in situ grown on the membrane via the interaction between amine and Mn 2+ followed by a one-step mineralization reaction. The MnO 2 -loaded loose NF membrane could achieve 99.7 % CR rejection while allowing only 1.67 % rejection of Na 2 SO 4 in a mixed solution of 60 mg/L Congo Red (CR) and 20 g/L Na 2 SO 4 at the permeability of 51.6 L m −2  h −1 ·bar −1 . After cleaning with H 2 O 2 , the flux recovery rate of the membrane remains above 97 %, attributed to the catalytic effect of MnO 2 on the membrane surface. Additionally, the membrane displayed similar performance in dealing with real wastewater, underscoring its potential for practical applications in textile wastewater treatment.

研究领域: 环境科学 · 材料科学
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Robust loose nanofiltration membrane with fast solute transfer for dye/salt separation

Qieyuan Gao,Dennis Bouwen,Shushan Yuan,Xiahui Gui,Yaowen Xing,Junfeng Zheng,Hongbin Ling,Qingjuan Zhu,Yue Wang,Stef Depuydt,Junwei Li,Alexander Volodine,Pengrui Jin,Bart Van der Bruggen

In today's energy crisis and shortage of resources, resource recycling on the premise of saving energy is a crucial topic. Large volumes of wastewater containing dye/salt mixtures in the textile industry are generated. In the process of treating textile wastewater, a membrane with better solute transport properties can be used to selectively remove solutes at constant energy input to save energy. Moreover, due to the challenging environment of typical textile wastewater, the membrane also needs to have a certain robustness. In this study, β-cyclodextrin and mussel-inspired polydopamine were combined using host-guest chemistry and then cross-linked by glutaraldehyde to form a robust loose separation layer. The results show that the membranes obtained by this process have a dye rejection greater than 99% and a salt rejection of about 16%. With the high degree of crosslinking at the surface, the membrane was found to exhibit excellent robustness in corrosive media at different pH values. Due to the high degree of cross-linking of the surface, the modified membrane also has good anti-fouling and anti-bacterial properties. Filtration using different concentrations of dye/salt mixed solutions demonstrated the stability of the membrane for filtration in highly concentrated salt solutions. In addition, a long-term stability test proved that the membrane operates stably for more than 60 h, maintaining its selectivity. This membrane with excellent robustness can provide technical guidance and theoretical support for the large-scale application of loose nanofiltration membranes.

CAS / MDL: 111-30-8
研究领域: 环境科学 · 材料科学
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Journal of Environmental Chemical Engineering · 2022 · IF 7.968

High-flux PSF/PES-COOH hollow fiber loose nanofiltration membrane for high-efficiency dye-salt separation

Dongxue Yao,Fan Zhang,Guangli Feng,Yufeng Zhang,Jianqiang Meng

Loose nanofiltration membranes show great potential to realize the effective separation of dyes and salts but still show low capacity for treating textile wastewater due to low membrane flux . In this work, a high-flux hollow fiber nanofiltration membrane (HFNFM) for the separation of dyes and salts was fabricated through a simple one-step non-solvent induced phase separation (NIPS) method. A carboxylated polyethersulfone (PES-COOH) was synthesized by the polycondensation based on Williamson reaction using diallyl bisphenol sulfur as a commoner followed by the thio-ene reaction with thioglycolic acid. Then PES-COOH was blended with polysulfone (PSF) for hollow fiber spinning based on the NIPS method. The effects of the ratio of PSF to PES-COOH on the membrane structure and performance were studied with scanning electron microscope (SEM), differential scanning calorimetry (DSC), X-ray photoelectron spectrometer (XPS), water contact angle and zeta potential measurements . Upon optimization, the PSF/PES-COOH HFNFM displayed a water flux of 159.6 L m −2 h −1 bar −1 , and a rejection of 99.2 % for Congo red at a dye concentration of 100 mg/L and operating pressure of 0.1 MPa. With the effective dye-salt fractionation which was comparative to literature reports, the membrane showed unprecedentedly high flux, which can be attributed to the double layer finger-like structure and hydrophilic PES-COOH as additives. The membrane also presented excellent stability and antifouling property during the treatment of simulated textile wastewater.

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Loose nanofiltration membranes based on interfacial glutaraldehyde-amine polymerization for fast and highly selective dye/salt separation

Tengfei Pei,Miao Deng,Cai Ma,Hao Yan,Aimei Zhu,Liyi Ye,Qinglin Liu,Qiugen Zhang

Loose nanofiltration (NF) membranes based on the interfacial polymerization (IP) reaction between glutaraldehyde (GA) and amine are developed for dye/salt separation. Branched tris(2-aminoethyl)amine (TETA) and linear hydrazine (HZ) are chose as aqueous amine monomers. Due to the low reactivity of aldehyde and amine under room temperature, plenty of evenly distributional cavities with exposed amine groups form in the matrix, favoring to enhance the membrane permeance, hydrophilicity and dye/salt selectivity. Notably, sodium dodecylsulphate (SDS) is introduced to regulate the monomer diffusion behavior and narrow the reaction zone, facilitating the formation of thin and defect-free skin layer. The resulting GA-TETA/HZ-L membrane shows a high water permeance of 76 LMH bar −1 as well as an excellent dye/salt selectivity (99% rejection for methyl blue (MB) and 4.19% rejection for Na 2 SO 4 ). Furthermore, the membrane shows a good anti-fouling property for bovine serum albumin (BSA), humic acid (HA) and sodium alginate (SA), benefiting from its smooth surface, high hydrophilicity and negative zeta potential. The newly demonstrated SDS-assisted aldehyde-amine IP process provides a novel and facile approach to develop the high-performance loose NF membrane for various fields, especially dye recycle and purification.

研究领域: 材料科学 · 环境工程
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Journal of Water Process Engineering · 2024 · IF 6.3

Dual-functional TFNC polyester membranes utilizing maltitol for dye/salt separation and desalination

Tonghui Zhang,Yumeng Wang,Bo Ge,Shuangshuang Wang,Yanhu Zhan,Xuefen Wang

To achieve a promising application prospect in nanofiltration (NF) membrane separation , a strategic design tailored to particular functions is crucial. Here, tailor-made thin film nanofibrous composite (TFNC) NF membranes for specific applications were fabricated via interfacial polymerization (IP) between maltitol and trimesoyl chloride (TMC) on PAN nanofibrous substrates. Owing to the moderate reactivity of maltitol, a range of sugar alcohol based polyester membranes with different morphologies and cross-linking degrees were obtained by varying the monomer concentration as well as the reaction time. In this case, the finely tuned loose Mal1-TMC0.2-2 membrane exhibited a prominent permeability (110.34 L m −2  h −1  bar −1 ) and an extraordinary selectivity for dye/salt mixed solution, with the rejection of Congo Red up to 99.11 % and NaCl retention of only 7.41 %, indicating its suitability for textile wastewater treatment . Further, the dense Mal2-TMC0.4-10 membrane showed an excellent Na 2 SO 4 rejection of 97.40 % with a good permeability of 18.65 L m −2  h −1  bar −1 , making it a candidate for seawater and brackish water desalination . In addition, both membranes demonstrated reliable chlorine and pressure resistance along with long-term stability. This study provided new insights and inspiration to the design and preparation of NF membranes for specialized applications.

CAS / MDL: 585-88-6
研究领域: 材料科学 · 环境工程
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Surface Bioengineering of Mo2Ga2C MAX Phase to Develop Blended Loose Nanofiltration Membranes for Textile Wastewater Treatment

Samira Jabbarvand Behrouz,Alireza Khataee,Vahid Vatanpour,Yasin Orooji

The potential of blended loose nanofiltration membranes (LNMs) to fractionate dyes and inorganic salts in textile wastewater has become a focus of attention in recent years. In this research work, we fabricated LNMs based on polysulfone (PSf) membranes blended with l-histidine amino acid-functionalized Mo2Ga2C MAX phase (His-MAX). Scanning electron microscopy (SEM), atomic force microscopy (AFM), attenuated total reflectance-Fourier transform infrared spectroscopy (ATR-FTIR), contact angle, ζ-potential, porosity, and pore size analyses were employed to characterize the LNMs. Blending 0.75 wt % of His-MAX additive with the PSf tailored the LNM’s features by making it more water-friendly, increasing its porosity, enlarging its pores, and making its surface smoother. The pure water flux of 127.6 L/m2 h was achieved by LNM containing 0.75 wt % His-MAX, which was 2.5 times greater than the bare one. The mentioned LNM displayed a flux recovery ratio (FRR) of 68.27 and 98.57, 98.31, and 99.7% rejections for Direct red 23, Acid brown 75, and Reactive blue 21 solutions (100 mg/L), respectively. The 0.75 wt % His-MAX LNM could reject 99.1% of dye and 11.5% of salt while maintaining an FRR of 91.19% after four cycles of filtering a binary mixture solution containing Reactive blue 21 and Na2SO4. These findings highlight the potential of the fabricated LNM for desalinating dye solutions.

CAS / MDL: 7782-42-5
研究领域: 材料科学 · 环境工程 · 膜技术
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JOURNAL OF CHEMICAL EDUCATION · 2024 · IF 2.5

Interfacially Polymerized Nanofiltration Membranes: Fabrication, Characterization, and Dye/Salt Separation

Tiefan Huang,Ting Qin,Siren Li,Na Tao,Jianxian Zeng,Ming Wu,Lelin Zeng,Wangdong Zeng,Hu Zhou

This laboratory experiment aims to provide undergraduate students with research experience in water treatment by membrane separation. This experiment includes fabrication and characterization, as well as water treatment applications of the interfacially polymerized polyester nanofiltration membranes. Through participating in this experimental course, students could obtain not only knowledge of membrane synthesis and separation performance testing but also basic methodologies that are widely used in scientific research. A series of advanced characterization techniques, such as Fourier-transform infrared spectroscopy (FT-IR), ultraviolet–visible spectroscopy (UV–vis), water contact angle (WCA), and scanning electron microscopy (SEM), has been used to allow students to investigate the membrane structure and morphology in detail. The experiment highlights the considerable potential of the synthesized membrane material for practical applications, which is particularly demonstrated through its effectiveness in wastewater treatment. This not only emphasizes the potential practice of the research findings but also deepens students’ comprehension of the broader impact of membrane separation in chemical engineering and environmental applications. Furthermore, this provides instructors with an opportunity to situate the experiment within a wider scientific framework, inspiring students to investigate emerging advancements and innovations in the field.

研究领域: 化学工程 · 环境科学 · 材料科学
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Journal of Cleaner Production · 2024 · IF 9.7

Investigating the generation mechanism of nanobubbles and the ion-transport regulation on nanofiltration membranes for efficient salt-salt separation

Shiyi Yao,Hansi Zhang,Kaiwen Wang,Lixing Lin,Xiaoxia Sun,Jia Xu

Nanofoaming-assisted interfacial polymerization (IP) exhibits strong potential to regulate the structure and the separation performance of thin film composite (TFC) membranes. At present, it is recognized that when NaHCO 3 is employed as an aqueous foaming agent, the generation of nanobubbles is ascribed to the NaHCO 3 acidification and may be enhanced by increasing the NaHCO 3 dosage. However, to more accurately measure the generation of nanobubbles, it is necessary to analyze the content and composition of carbonates in the aqueous solution at the initial and final states of interfacial polymerization, which is currently lacking in research. In this work, based on the chemical equilibrium theory, the aqueous carbonate chemistry and the quantity of CO 2 released during IP was evaluated through monitoring the pH changes near the interface and calculating the carbonate distribution fraction. Results showed that the pH of the aqueous solution changed from 10.3 to 11.4 to 6.0–6.5 during interfacial polymerization when the NaHCO 3 dosage was 0.00–0.10 wt%. However, this variation in pH was subtle (from ∼9.3 to ∼8.8) when 1.00 wt% NaHCO 3 was added, leading to limited transformation of carbonate into H 2 CO 3 and, consequently, less generation of CO 2 . In the whole dosage range of NaHCO 3 , 0.10 wt% NaHCO 3 contributed to the maximum quantity of CO 2 during IP, which was also confirmed by the vesicle-like membrane morphology. The resultant membrane achieved a superior salt-salt separation, with selectivity for Mg 2+ and Li + /Na + /K + enhancements of more than 2 times compared to the membrane without NaHCO 3 dosage. This work proposed a new approach to evaluate the inner relationship between NaHCO 3 dosage and nanobubble quantity during IP, which provides an ion-transport regulation mechanism of nanofiltration membranes for efficient salt-salt separation.

CAS / MDL: 7447-41-8
研究领域: 材料科学 · 化学工程 · 环境科学
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JOURNAL OF MEMBRANE SCIENCE · 2018 · IF 6.578

Zwitterionic functionalized MoS2 nanosheets for a novel composite membrane with effective salt/dye separation performance

Xu Liang,Penghui Wang,Jing Wang,Yatao Zhang,Wenjia Wu,Jindun Liu,Bart Van der Bruggen

Polyethersulfone (PES) has been widely used as an ultrafiltration (UF) or nanofiltration (NF) membrane material in multiple industrial fields. But PES is hydrophobic in nature and easily contaminated. Thus, it is necessary to modify the PES membrane surface by physical or chemical methods for improving its hydrophilicity and other function. Herein, MoS 2 modified by zwitterionic 2-methacryloyloxy ethyl dimethyl (3-sulfopropyl)-ammonium hydroxide sulfobetaine methacrylate (MoS 2 -PSBMA) was synthesized with a reverse atom transfer radical polymerization method (RATRP) and used to prepare MoS 2 -PSBMA/PES composite membranes via conventional phase inversion. The effect of MoS 2 -PSBMA content on the structure and properties was investigated by SEM, FT-IR, AFM and contact angle measurements. It was found that the hydrophilicity of the composite membrane increased with the content of zwitterionic functionalized MoS 2 nanosheets. Moreover, the composite membranes possessed a higher water flux (108.3 L m −2 h −1 at 0.6 MPa) and dye retention, 98.2% for Reactive Black 5% and 99.3% for Reactive Green 19. However, the rejection of Na 2 SO 4 , MgCl 2 NaCl and MgSO 4 was low, i.e., 2.2%, 1.2%, 1.1% and 0.3%, respectively. In summary, the synthesized composite membrane exhibited high selectivity for dye/inorganic salts and had a large potential for dye waste water treatment.

研究领域: 材料科学 · 环境工程
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JOURNAL OF CHEMICAL AND ENGINEERING DATA · 2019 · IF 2.298

Study on the Phase Equilibrium of Na+, K+//Cl–, CO32––H2O and Single-Salt of Potassium Separation with the Aid of Compressed CO2

Zhongshu Li,Yuli Xue,Xiaoling Tan,Wenqing Li,Shaonan Xu,Ziyan Wang,Jian Wang,Lina Li,Shiding Miao

It is of great importance to separate potassium salts from carbonate-based lakes, especially the low-[K+] but high-[Na+] brine which has been discovered around the world. Here the phase diagram of the quaternary system Na+, K+//Cl–, CO32––H2O was experimentally studied at 298.15 K via the method of isothermal evaporation, and the results corrected the previous diagram reported by Blasdale (J. Am. Chem. Soc.1923, 45, 2935–2946). The type of salts appeared and their solubility during the evaporation, and the density vs composition diagram and the pH values were plotted based on the experimental data. It was found that there were six invariant points, seven univariant curves, and five crystallization fields in the equilibrium phase diagram. To extract single-salt of potassium, certain areas in the Na+, K+//Cl–, CO32––H2O diagram were chosen to be acidified by the compressed CO2, and potassium in the form of KHCO3 was precipitated from the mother solution. The compressed CO2 was able to avoid formation of NaKCO3·6H2O during evaporation of the original system Na+, K+//Cl–, CO32––H2O. Based on experiment data, the region area for potassium salt extraction was determined, and this area was suitable for extracting K+ salts from brines with a [Na+/K+] ratio even lower than 0.44. This strategy opened a new way to recovery of potassium with a maximum yield of 59.88% from the carbonate-chloride-based brine.

研究领域: 化学工程 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Nanofiltration membranes fabricated by plant polyphenol-intermediated MXene and polyethyleneimine layer-by-layer self-assembly for efficient dye/salt separation

Yijing Hu,Zhihao Chen,Yidan Ding,Yanchao Xu,Hongjun Lin,Wei Yu,Jiaheng Teng,Liguo Shen,Yang Jiao,Bao-Qiang Liao

The traditional layer-by-layer (LBL) self-assembly method used to prepare nanofiltration (NF) membranes with polyelectrolytes often suffers from low permeability caused by the restricted free volume of the selective layer. Furthermore, substrate surfaces typically require rigorous chemical treatment with potent acids or bases to achieve the necessary charge for adsorbing the initial polyelectrolyte layer. To address these issues, a green and straightforward aqueous immersion method was utilized in this investigation to form a coating of plant polyphenol tannic acid (TA) on the substrate surface. The TA coating served as an intermediary for the LBL self-assembly of negatively charged 2-dimensional material MXene nanosheets and positively charged polyethyleneimine (PEI), resulting in a well-structured NF membrane. By utilizing a 4-bilayer number, 0.05 mg/mL MXene concentration, 1.0 mg/mL PEI concentration, and PEI molecular weight of 1800 g mol −1 , an NF membrane with an ultrahigh pure water permeance of 204.0 L m −2 h −1 bar −1 and 99.9% Evans Blue rejection was produced. Furthermore, the membrane possesses an ultra-high dye/salt separation factor of 758.1, surpassing most of the previously reported data. The innovative plant polyphenol-mediated MXene and PEI LBL self-assembly strategy proposed can be applied not only in NF membrane preparation but also in inspiring the design of advanced MXene composite materials for environmental and energy applications.

研究领域: 材料科学 · 环境工程
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Surfaces and Interfaces · 2023 · IF 6.2

UiO-66-(OH)2-mediated transition layer for ultra-thin homogeneous defect-free polyamide membrane

Fan Xiao,Ming Cao,Yingbo Chen

The synthesis of ultra-thin, uniform and continuous polyamide (PA) membranes is a crucial prerequisite for enhancing their desalination performance. Research has indicated that effectively slowing down the interfacial polymerization (IP) reaction and promoting the interface stability are key strategies for achieving ultra-thin, uniformly nano-structured membranes with excellent performance. Herein, we have demonstrated the successful design of a continuous and uniform PA membrane, ranging from 10 to 20 nm, by utilizing the UiO-66-(OH) 2 n-hexane dispersion as a transition layer to regulate IP reaction and enable efficient water-salt separation. The results showed that the presence of the transition layer facilitated a bidirectional diffusion-contact reaction between the two monomers, resulting in improved interface stability and alleviating the occurrence of severe IP that may lead to heterogeneous membrane structures. As a result, the PA active layers formed through this approach exhibited superior thinness and uniformity compared to those produced via traditional IP methods. Moreover, the transition layer enabled uniform pre-polymerization of UiO-66-(OH) 2 at the reaction interface by pre-exposing it to down-diffusing acyl chloride monomers. This ensured the continuity of membrane structure while creating additional free volume within the membrane. This work presented a scalable method for manufacturing ultra-thin, defect-free, homogeneous, and high-performance nanofiltration membranes.

研究领域: 材料科学 · 膜技术 · 化学工程
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