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JOURNAL OF THE CHINESE CHEMICAL SOCIETY · 2020 ·Vol. 67 ·期 10 ·1807-1817 · IF 1.554

Alteration of the morphology of polyvinylidene fluoride membrane by incorporating MOF-199 nanomaterials for improving water permeation with antifouling and antibacterial property

Hai-Tao Wang,De Ao,Mei-Chan Lu,Na Chang

MOF-199@PVDF composite membranes are prepared by blending with different amounts of ultrasonic synthesized MOF-199 nanomaterials for improving the pure water flux (PWF) and achieving better antifouling and antibacterial performance. The membrane morphology, elemental composition, and surface properties are analyzed by various means of characterizations, including scanning electron microscopy, energy-dispersive X-ray spectroscopy, and water contact angle measurements. The performance of the modified membranes is also determined from the perspective of the PWF, bovine serum albumin rejection, as well as antifouling and antibacterial properties. Due to the variation in the viscosity of dope solution, the composite membranes possess remarkably different morphology, and the M5 membrane, which exhibited a sponge-like structure, the largest surface pore size, and the highest porosity, shows the highest PWF, reaching up to 185.05 L/m 2 h. Moreover, with the incorporation of MOF-199 nanocrystals, the antifouling property, together with the antibacterial property, toward both gram-negative bacteria and gram-positive bacteria, based on M5 and M7 membranes, increases dramatically compared with the pristine polyvinylidene fluoride membrane. In addition, the long-term permeation performance and copper leakage of the membrane are investigated. As a result, the composite membrane, M5, shows great potential in real water treatment.

研究领域: 材料科学 · 环境工程 · 膜技术
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DESALINATION · 2022 · IF 11.211

Structures and performance of alcohol activated thin film composite polyamide (TFC-PA) nanofiltration (NF) membranes prepared with and without Co(II) modulation

Xiumin Zhang,Yongping Dong,Qingyi Wang,Hang Yu,Congjie Gao,Lixin Xue

Structures and NF performance of TFC-Co and TFC membranes activated with 50 % alcohol solutions were studied. Methanol and glycol solution activation increased water flux 2–4 times without trading off salt rejection while glycerin solution activation increased water flux 3–4 times with reduced salt rejection and increased dye/salt retention selectivity . The Stokes radius of TFC-Co membrane changed from 0.77 nm to 0.66, 0.78 and 0.92 nm while the TFC membrane changed from 0.54 nm to 0.55, 0.65 and 0.70 nm after activation with methanol, glycol and glycerin solutions, respectively. Capillary pore filling models were developed from pure alcohol absorption experiments including the stages of initial pore filling, pore expansion, pore relaxation and pore adjustment, while most Stokes radius after 50 % solutions activation were found to be close to the relaxed pore radius values (r rx ) or half of the expanded pore radius values (r ex ) from pure alcohol absorption experiments.

研究领域: 材料科学 · 环境工程
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CHEMICAL ENGINEERING RESEARCH & DESIGN · 2022 · IF 4.119

MXene-based composite forward osmosis (FO) membrane intercalated by halloysite nanotubes with superior water permeance and dye desalination performance

Hongdan Wu,Ming Li,Yehao Zhao,Zhihui Zhou,Shaoqiang Hua,Jian Zhang

MXene two-dimensional (2D) laminate membranes have attracted many researchers in the field of membrane separation due to its adjustable interlayer spacing. However, MXene 2D laminate membranes has been inability to achieve dye desalination due to simultaneous rejection of both dyes and salts in salt-containing dye. The looser MXene/C-HNTs composite forward osmosis (FO) membrane was successfully prepared via vacuum filtering, in which halloysite nanotubes modified with cetyltrimethylammonium bromide (C-HNTs) and MXene (Ti 3 C 2 T x ) nanosheets were self-assembled by electrostatic interactions. The insertion of C-HNTs effectively increased the interlayer spacing and enhanced the compression resistance of the composite membranes. With a mass ratio of 1:3 between Ti 3 C 2 T x nanosheets and C-HNTs, the composite membrane's pure water flux was raised to 191.4 L/(m 2 ·h). The insertion of C-HNTs not only enabled the composite membrane to keep a superior dye rejection rate (CR rejection rate >99%), but also effectively reduced the rejection rate of monovalent salt (NaCl <5%) and divalent salt (<13% and <10% for Na 2 SO 4 and MgSO 4 , respectively).

CAS / MDL: 314-13-6
研究领域: 膜科学 · 材料科学 · 环境工程 · 纳米技术
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JOURNAL OF MEMBRANE SCIENCE · 2018 · IF 6.578

Novel functionalized forward osmosis (FO) membranes for FO desalination: Improved process performance and fouling resistance

Wenxuan Xu,Qingchun Ge

The potential of forward osmosis (FO) for water treatment can only be maximized with appropriate FO membranes . In this work, novel FO membranes functionalized with hydrophilic materials carrying both amine and sulfonate or carboxylate groups were synthesized via amidation reaction occurred on thin film composite (TFC) FO membranes. The performance of the newly explored FO membranes was evaluated in FO desalination and antifouling studies. Significant improvement in FO performance was observed for the novel FO membranes, in which the water flux increases more than 19% for the sodium taurine (ST) modified membrane (ST-modified membrane) relative to the pristine TFC FO membrane when pure water and 0.5–2.0 M MgCl 2 as the respective feed and draw solutions. Meanwhile, the ST-modified membrane produced a water flux 33% higher than that by the pristine TFC FO membrane in seawater (3.5 wt% NaCl) desalination with 2.0 M MgCl 2 as the draw solution, drastically increasing water recovery efficiency. The water flux decline of the ST-modified membrane is 46% lower than that of the pristine membrane with sodium alginate as a foulant. Introducing sulfonate or carboxylate ionic groups onto FO membrane surface is crucial to enhance the membrane antifouling ability and thus improves FO performance, which provides new insight in novel FO membrane exploration.

研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Deciphering the role of camphor sulfonic acid and triethylamine in Thin-Film composite reverse osmosis membranes for water desalination

Miao-Miao Jia,Si-Yuan Yang,Ke-Ke Chen,Pan-Pan Zhang,Wei Shao,Zhen Chen,Zi-Meng Xu,Qing-Yun Wu,Yi Li,Ming Xue

Thin-film composite (TFC) reverse osmosis (RO) membranes, fabricated by interfacial polymerization, have achieved significant success in addressing the global water scarcity. Over the past three decades, the camphor sulfonic acid (CSA)/triethylamine (TEA) has been widely used in fabrication of TFC RO membranes. However, the mechanism of this unique formula remains elusive and contentious. In this work, for the first time, deciphering that introducing CSA/TEA into the aqueous phase has negligible impact on the selective polyamide (PA) layer but facilitate the aqueous solution impregnating of porous polysulfone (PSf) support. Specifically, the acidic CSA significantly hinders amine diffusion yet preserves the porosity of the PSf support during high-temperature curing. TEA is essential in modulating the pH changes and balancing the monomer diffusion rate that results from CSA. The COMSOL simulations have further elucidated that the presence of an aqueous solution within the porous support can mitigate the thermal expansion of the PSf, consequently inhibiting the shrinkage of surface pores. The TFC membrane demonstrated a substantial improvement in water permeance due to the preservation of its pore structure. The obtained TFC membrane demonstrated an exceptional NaCl rejection of 99.3 % and a high water flux of 76.8 L m –2 h −1 (2000 ppm NaCl, 15.5 bar), exceeding that of the state-of-the-art TFC RO membranes. Moreover, the RO membrane manifested with long-term stability and good fouling resistance. The mechanistic insights have important implications to more efficient membrane-based desalination and water reuse, thereby reducing energy consumption and minimizing environmental carbon footprint.

研究领域: 材料科学 · 环境工程
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DESALINATION · 2017 · IF 5.527

Positively charged capillary nanofiltration membrane with high rejection for Mg2 + and Ca2 + and good separation for Mg2 + and Li +

Hai-Zhen Zhang,Zhen-Liang Xu,Hao Ding,Yong-Jian Tang

High water permeability and good separation property are greatly desired in water production due to energy concerns. To explore nanofiltration (NF) membrane with high permeability for cations separation, a positively charged NF membrane was fabricated via interfacial polymerization using polyethersulfone (PES) three-channel capillary ultrafiltration (UF) membrane as substrate, polyethyleneimine (PEI) as the aqueous precursor. The NF membrane preparation conditions were optimized. To enhance the permeability of the prepared NF membrane, modified hydroxyl contained multi-walled carbon nanotubes (MWCNTs-OH), grafting with piperazine (PIP), were utilized. The resultant NF membrane showed increased water flux from 20.8   L·m −   2 ·h −   1 to 56.1   L·m −   2 ·h −   1 at 4   bar after adding 0.01   wt% modified MWCNTs-OH in aqueous solution. Interestingly, MgCl 2 rejection of the membrane also increased from 94.2% to 96.9%. The positively charged NF membrane exhibited above 97% rejection for divalent cations (Mg 2   + and Ca 2   + ) and low rejection (<   70%) for monovalent cations (Na + and Li + ), and it also showed long durability and good separation for Mg 2   + and Li + when the membrane was used to separate mixed salts solution simulated the composition of salt lake brine. The fabricated membrane would have potential for effective water softening and for reclamation of lithium from brine or seawater with high Mg 2   + /Li + ratio.

研究领域: 环境科学 · 材料科学
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JOURNAL OF MEMBRANE SCIENCE · 2020 · IF 7.183

Novel thin-film reverse osmosis membrane with MXene Ti3C2Tx embedded in polyamide to enhance the water flux, anti-fouling and chlorine resistance for water desalination

Xiaoying Wang,Qingqing Li,Jianfeng Zhang,Haimeng Huang,Shaoyu Wu,Yan Yang

The development of high performance reverse osmosis (RO) membranes still remains a big challenge due to not only the trade-off between water flux and salt rejection, but also their easy fouling and chlorine attacking. In this paper, a novel thin-film nanocomposite RO membrane with two-dimensional MXene Ti 3 C 2 T x embedded in the polyamide (PA) layer was fabricated by in-situ interfacial polymerization with m-phenylenediamine aqueous solution and trimesoyl chloride. Due to the outstanding diffusion regulating effect of Ti 3 C 2 T x in accordance with the Fick's first law, the water permeability was elevated to a maximum value of 2.53 L m −2  h −1  bar −1  at a high NaCl salt rejection of 98.5%. Simultaneously, the enhanced anti-fouling, and chlorine resistance of the as-obtained PA-Ti 3 C 2 T x membrane were also obtained, outperforming the pristine PA and other related RO membranes in literature. Especially after a chlorine-resistance test at 10000 ppm h, a high salt rejection of 97.1% for the PA-Ti 3 C 2 T x membrane was still retained. Based on the microstructural observation and mechanism analysis, such an improvement in chlorine resistance was mainly ascribed to the interaction between surface functional groups of Ti 3 C 2 T x nanosheets with active chlorine, which effectively protected the PA matrix from being chlorine attacked. This work illustrates successfully a very new use of Ti 3 C 2 T x to improve the comprehensive performance for water desalination membranes for practical applications.

研究领域: 材料科学 · 环境科学 · 水处理技术
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MOLECULES · 2022 ·Vol. 27 ·期 10 ·3214 · IF 4.927

Synthesis of PNIPAAm-g-P4VP Microgel as Draw Agent in Forward Osmosis by RAFT Polymerization and Reverse Suspension Polymerization to Improve Water Flux

Yi Gao,Xuesong Yao,Qinggeng Jiang,Jianhe Liao,Yongping Chen,Rentong Yu

Microgels have unique and versatile properties allowing their use in forward osmosis areas as a draw agent. In this contribution, poly(4-vinylpyridine) (P4VP) was synthesized via RAFT polymerization and then grafted to a poly(N-Isopropylacrylamide) (PNIPAAm) crosslinking network by reverse suspension polymerization. P4VP was successfully obtained by the quasiliving polymerization with the result of nuclear magnetic resonance and gel permeation chromatography characterization. The particle size and particle size distribution of the PNIPAAm-g-P4VP microgels containing 0, 5, 10, 15 and 20 wt% P4VP were measured by means of a laser particle size analyzer. It was found that all the microgels were of micrometer scale and the particle size was increased with the P4VP load. Inter/intra-molecular-specific interactions, i.e., hydrogen bond interactions were then investigated by Fourier infrared spectroscopy. In addition, the water flux measurements showed that all the PNIPAAm-g-P4VP microgels can draw water more effectively than a blank PNIPAAm microgel. For the copolymer microgel incorporating 20 wt% P4VP, the water flux was measured to be 7.48 L∙m−2∙h−1.Keywords:microgel;forward osmosis;draw agent;P4VP

CAS / MDL: 107-96-0
研究领域: 材料科学 · 化学工程
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Journal of Cleaner Production · 2021 · IF 9.297

Adopting vibration to alleviate the solute buildup and membrane fouling in a forward osmosis system

Jing-Xiao Zhang,Tian Tian,Wen-Jie Du,Yan-Fang Guan,Yun-Jie Wang,Yu-Sheng Li,Han-Qing Yu

Forward osmosis (FO) is limited by solute buildup and membrane fouling . Although current solutions (e.g., influent pretreatment and membrane modification) have partially compensated these drawbacks, they are still enslaved to the uncertainties and costs from the complex operational requirements and large use of chemicals. Therefore, developing simply-operated and chemical-free methods is highly required. In this work, a lab-scale vibrating FO device was constructed and its water permeability and anti-fouling capacity were evaluated. The results of flux tests show that the vibration could effectively enhance the water flux and mitigate solute buildup, mainly resulted from changing the flow field on the membrane surface through the computational fluid dynamic simulations . In addition, the vibrating FO was also proven to be effective in controlling the fouling caused by model organic foulants like bovine serum albumin, humic acid , alginate , and biofouling by different ways. The results of anti-fouling tests and fouling characteristics show that the organic fouling was alleviated by disintegrating the fouling layer and reducing the solute buildup, while the biofouling was mitigated through retarding the early microbial attachment and growth. This work provides a feasibility of applying vibration as an effective strategy to control solute buildup and fouling in FO systems.

研究领域: 环境工程 · 化学工程
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DESALINATION · 2025 · IF 9.8

Regulation of polyamide reverse osmosis membrane structure by nanobubbles: Unraveling the mystery of structure-property relationships

Houkang Pu,Hanjing Xue,Xiaojuan Wang,Huacheng Xu,Yijun Huang,Jiayan Xu,Xinyan Wang,Weizheng Zhang,Congjie Gao,Xueli Gao

The development of nanofoaming strategies presents a new avenue for designing polyamide (PA) thin film composite reverse osmosis membrane structures. However, the precise mechanism by which nanobubbles regulate the overall structure of the PA layer and the relationship between the influence on membrane structures and properties remain unclear. In this study, the PA layer structure was precisely regulated with H 2 nanobubbles based on free interfacial polymerization, and the impact of H 2 nanobubbles on the backside opening properties, internal nanovoids, and surface morphology of membranes was comprehensively analyzed. Furthermore, this strategy has been successfully extended to CO 2 and O 2 nanobubble systems. Through analyzing the robust correlation between nanovoid size and PA layer thickness in all membranes, an innovative “volcano” relationship between membrane structure and water permeance was proposed. Upon this basis, a model of nanovoid size ratio was developed and revealed that the water permeance of PA membranes increased with the increase of nanovoid size ratio. Remarkably, the H 2 -0.05 % membrane, located at the apex of the “volcano” with the highest nanovoid size ratio (0.56), exhibited outstanding water permeance (2.61 L·m −2 ·h −1 ·bar −1 ) and reasonable salt rejection (97.9 %). This study provides valuable insights into the intricate relationship between the structure and property of PA membranes.

CAS / MDL: 5872-08-2
研究领域: 材料科学 · 环境工程
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

How to understand the effect of relative humidity on the morphology and performance of polypiperazine-amide NF membrane during heat curing process

Ke Xiang,Zhen-Liang Xu,Yong-Jian Tang

Recent studies have shown that the temperature and time of the heat curing process have important effects on the nanofiltration (NF) membrane structure and properties. However, the mechanism of the relative humidity (RH), as one of the important factors in the heat curing of NF membranes, is still unclear. To analyze the specific effect of RH, we compared the heat curing results of the NF polyamide (PA) membranes fabricated with different monomer concentrations at various RH. The nanofiltration performance of the membranes appeared to be non-uniform when the RH was in the range of 40 %–60 %. Within the appropriate RH range , the rejection of Na 2 SO 4 was preserved at about 98.5 % for the manufactured NF membranes. At high concentrations, the increasing RH created a discontinuous condensate layer on the PA layer surface, which affected the morphology and physicochemical properties of the NF membrane causing a doubling of pure water permeability (PWP) to 8.33 L m −2  h −1 ·bar −1 . At low concentrations, the PA layer was not significantly changed with the increase of RH, but the evaporation of water from the smaller capillary pores in its PES substrate was slowed down, which reduced the capillary stress on the substrate and prevented the collapse of the substrate pore size, resulting in a nearly 20 times increase in its PWP to 39.7 L m −2  h −1 ·bar −1 . This work reveals the effect of RH during heat curing and gives significant guidance to the design and synthesis of high-performance NF membranes.

研究领域: 材料科学 · 环境工程
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DESALINATION · 2010 · IF 2.034

Fabrication of polysulfone ultrafiltration membranes of a density gradient cross section with good anti-pressure stability and relatively high water flux

Zhenghua Zhang,Quanfu An,Tao Liu,Yong Zhou,Jinwen Qian,Congjie Gao

Polysulfone ultrafiltration membranes were prepared via the wet phase-inversion process with the same coagulation bath . Three different kinds of systems including polysulfone (PSF)/N, N-Dimethylacetamide (DMAC)/poly(vinyl pyrrolidone) (PVP), PSF/DMAC/Ethanol ternary systems and PSF/DMAC/Ethanol/PVP quaternary system were used as casting solutions . The zero shear viscosity of the casting solutions was measured and the phase-inversion process was monitored by the light transmittance apparatus. The surface and cross-section morphology of the corresponding membranes were characterized by SEM. The water flux and the anti-pressure stability of the membranes were performed in the permeation experiment. The pore size and porosity of the fresh and pressurized membranes were calculated. These experimental results suggest that the PSF ultrafiltration membrane of a density gradient structure prepared from the quaternary system by using PVP and ethanol together in PSF/DMAC/Ethanol/PVP solution with the respective amounts of 3.05   wt.%, 15.5   wt.%, has a good anti-pressure stability and a relatively high water flux (only changed from 162   L/m 2   h to 155   L/m 2   h ) even by continuous operation (0.5   MPa) for 200   min, which is valuable as the sub-supporting membrane of composite membranes.

CAS / MDL: 9003-39-8
研究领域: 材料科学 · 膜技术
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