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Applied Water Science · 2021 ·Vol. 11 ·期 7 ·1-10 · IF 3.874

Laminated graphene oxide membrane for recovery of mercury-containing wastewater by pervaporation

Wang Ziheng,Qin Yingzhe,Xu Xiangping,Sun Jiawei,Shen Jiancheng,Ning Xiaogang,Li Na

Mercury (Hg) is a toxic heavy metal contaminant and has very harmful effects for human health. In this work, Hg-containing wastewater with Hg concentration of 6.36 ppb and 9.4 ppb were recovered with polyethylenimine (PEI) cross-linked graphene oxide (GO) layered membrane (c-GO-PEI) by pervaporation. The influence of ionic type, the concentration of Hg and the feed temperature were investigated. The c-GO-PEI exhibited not only high rejection for salts (> 99.97%), Hg (77.5–100%) and non-purgeable organic carbon (NPOC) (67.3–90.8%) but also high flux (30.30 kg·m −2 ·h −1 ) to treat with the wastewater. In addition, the flux could be largely recovered after simple washing, indicating the excellent antifouling property of the membrane.

CAS / MDL: 9002-98-6
研究领域: 环境科学 · 材料科学 · 化学工程
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JOURNAL OF APPLIED POLYMER SCIENCE · 2021 ·Vol. 139 ·期 5 ·51573 · IF 3.125

Fabrication of MWCNTS-functionalized SA pervaporation composite membranes to enhance esterification

Jiayun Shi,Taishan Wang,Jie Han,Yao Liang,Yujia Tong,Weixing Li

A novel SA-f-MWCNTs/PAN composite membrane, sodium alginate- functionalized multi-walled carbon nanotubes/polyacrylonitrile, was prepared to enhance the esterification conversion rate with a pervaporation membrane reactor. The SA-f-MWCNTs/PAN membrane was investigated by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and scanning electron microscope. The hydrophilicity, mechanical properties, and separation performance of the composite membrane have been significantly improved. The flux of the composite membrane was 4374 g·m −2 ·h −1 , and the separation factor was 1249 (the water content in the feed was 10 wt%, at 75°C). The composite membrane the trade-off effect between flux and separation factor. The acid conversion rate of SA-f-MWCNTs/PAN membrane was up to 98.3% in 5 h at 75°C, which was a great increase of 18.3% compared with the equilibrium conversion rate of the batch reactor. In addition, SA-f-MWCNTs/PAN membrane exhibited good swelling resistance and reusability. The conversion rate of acetic acid was stable above 95.0% after 8 repetitive tests.

CAS / MDL: 6482-24-2
研究领域: 材料科学 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

High-performance 19-channel monolithic chabazite membranes for efficient separation of water/ethanol and water/isopropanol mixtures by pervaporation and vapor permeation

Zhigang Xue,Yuan Shen,Liang Chen,Bo Liu,Na Hu,Rongfei Zhou,Weihong Xing

Pervaporation (PV) and vapor permeation (VP) using selective zeolite membranes are more energy-saving in dealing with azeotropic mixtures compared with conventional distillation for organic solvent dehydration. Herein, we developed a monolithic supported chabazite membrane and exploited its dehydration performance. The membrane was fabricated by secondary growth method on the 19-channel alumina monolithic without organic template. By finely controlling the homogeneity of nuclei growth and minimizing the intracrystalline defects through the epitaxial growth of uniformly nanosized SSZ-13 seed layer using cesium hydroxide and sodium hydroxide as cooperative hydration-mismatched inorganic structure directing agents (ISDA). The resulting monolithic chabazite membrane exhibits excellent water-perm-selectivity. The effects of feed water composition and operating temperature on the dehydration performance of the monolithic chabazite membrane were investigated through PV and VP processes. The typical membrane displayed excellent selectivities of more than 10,000 and 30,000 in 10/90 wt% water/ethanol and water/isopropanol mixtures at 393 K. The membrane exhibited excellent hydrothermal stability in a VP with a 10/90 wt% water/ethanol at 393 K for 72 h. The robust monolithic chabazite membrane with high packing density, strong mechanical strength, large membrane area and excellent water-selective performance significantly outperforms state-of-the-art membranes for dehydration in practical applications.

CAS / MDL: 21351-79-1
研究领域: 化学工程 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Enhancing the pervaporation performance of PEBA/PVDF membrane by incorporating MAF-6 for the separation of phenol from its aqueous solution

Rehan Khan,Ihtisham Ul Haq,Heng Mao,Ao-Shuai Zhang,Li-Hao Xu,Hong-Gang Zhen,Zhi-Ping Zhao

Phenol is highly toxic and carcinogenic even at low concentrations. This study focused on preparing high-performance mixed matrix membranes (MMMs) for the pervaporation separation of phenol from its aqueous solution. A highly-efficient zeolitic metal azolate framework, RHO-[Zn(Heim) 2 ] (MAF-6, Heim = 2-ethylimidazole) was incorporated into the polyether block amide (PEBA-2533) supported on the polyvinylidene fluoride (PVDF) ultrafiltration membrane. The MAF-6 was chosen as the filler due to its inherent hydrophobic surfaces and aperture size (7.6 Å), which is larger than the molecular kinetic diameter of phenol (6.6 Å). Effects of the casting solution concentration, active layer thickness, MAF-6 loading, operating temperature, and phenol concentration were systematically investigated. With the increase of the MAF-6 loading ratio X from 0 to 7, the phenol flux of the membrane was gradually enhanced, but the water flux was reduced. For 1000 ppm phenol aqueous solution at 80 °C, MAF-6–7@MMM displayed the optimal separation factor of 25.9 with a phenol flux of 89.2 g∙m −2 ∙h −1 . The pervaporation separation index (PSI) of the MAF-6–7@MMM was 1317.7 kg∙µm∙m −2 ∙h −1 at 80 °C, which was much higher than the PEBA/PVDF membrane (787 kg∙µm∙m −2 ∙h −1 ). Impressively, an increasing feed temperature enhanced the phenol flux more prominently than water, owing to the hydrophobicity and porosity of MAF-6. Consequently, the resultant MAF-6-X@MMMs broke the trade-off limitation between phenol permeability and selectivity. The as-prepared membrane also exhibited exceptional long-term stability, suggesting its prospect of industrial application.

CAS / MDL: 1072-62-4
研究领域: 环境科学 · 材料科学
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JOURNAL OF MEMBRANE SCIENCE · 2020 · IF 7.183

Epoxide-based PDMS membranes with an ultrashort and controllable membrane-forming process for 1-butanol/water pervaporation

Zhihao Si,Chang Liu,Guozhen Li,Ze Wang,Jingfang Li,Tanlong Xue,Shuai Yang,Di Cai,Shufeng Li,Haoning Zhao,Peiyong Qin,Tianwei Tan

The ultrashort and controllable membrane-forming process is highly required in large-scale production of PDMS membrane. To shorten the cross-linking time, an UV-induced ring-opening polymerization of the epoxide groups was introduced to the preparation of PDMS membranes. PDMS was firstly functionalized with epoxide groups, providing the possibility of being cross-linked under UV irradiation. With this strategy, the membrane curing was finished within 200 s, hence shortened by two orders of magnitude in comparison with the conventional thermal-driven method. Meanwhile, the cationic photoinitiation of epoxide groups can be achieved without oxygen inhibition in an open-air environment. Moreover, the viscosity of the coating solution in the groove is kept constant when protected from light, thus meeting the requirement of the coatability. When applied to the pervaporation of a 1.5 wt% 1-butanol/water solution at 55 °C, the measured 1-butanol separation factor was 45 and the total flux was 1119 g m −2  h −1 . This novel strategy shows a great prospect in the continuous preparation of membrane.

CAS / MDL: 65799-47-5
研究领域: 材料科学 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2014 · IF 4.908

Iso-butanol dehydration by pervaporation using zeolite LTA membranes prepared on 3-aminopropyltriethoxysilane-modified alumina tubes

Bingxin Huang,Qian Liu,Jürgen Caro,Aisheng Huang

Dense and phase-pure zeolite LTA membranes were hydrothermally synthesized on 3-aminopropyltriethoxysilane (APTES)-modified macroporous Al 2 O 3 tubes without seeding. Pervaporation experiments were conducted for the separation of liquid water/iso-butanol and water/ethanol mixtures to evaluate the separation performances of the zeolite LTA membranes. A water flux of 4.5   kg/m 2   h is obtained at 100   °C for the separation of a 95.0   wt% iso-butanol/5.0   wt% water mixture, and the separation factors of water/iso-butanol are found to be about 3000 for all temperatures and concentrations studied.

CAS / MDL: 78-83-1 1310-73-2
研究领域: 化学工程 · 材料科学
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

Preparation of stable multilayer PDMS composite pervaporation membrane incorporated with in-situ transformed metal organic frameworks for enhanced butanol recovery

Xu Zhang,Lulu Xiao,Guoliang Zhang,Lusheng Xu,Zehai Xu,Qin Meng

In this study, stable and non-defective multilayer polydimethylsiloxane (PDMS) composite pervaporation mixed matrix membranes incorporated with in-situ transformed metal organic frameworks was successfully synthesized via ligand vapor phase infiltration and spin-coating. Metal zinc sources were uniformly distributed in PDMS which were in-situ transformed into homogeneous zeolitic imidazolate framework-8 (ZIF-8) nanoparticles, effectively alleviating the aggregation of ZIF-8. Thermal cross-linking of PDMS and the formation of MOFs occurred simultaneously, omitting the complicated preparation and re-dispersion steps of MOF nanoparticles. MOF nanoparticles and PDMS formed a more stabilized composite structure by in-situ transformation, in which PDMS and metal of MOFs can interact with the - Si - O - of silane coupling groups on membrane surface to construct solid multilayer composite membrane, ensuring long-term stability. Moreover, with the aid of hydrophobic interlayer, polymer infiltration into channels of substrate was restricted and casting solution spread out smoothly, facilitating the formation of defect-free PDMS selective layer. Various techniques including Attenuated Total Reflection-Fourier Transform Infrared Spectrometer, Field Emission Scanning Electron Microscopy, Atomic Force Microscope and X-ray Diffraction were applied to explore the morphology, composition and structure of nanoparticles and membranes, and pervaporation tests were taken to investigate the behavior of hydrophobic polymer-based multilayer membranes. For the recovery of low concentration n-butanol, the prepared non-defective multilayer TAO/ZIF-8/K-PDMS composite membrane displayed excellently total permeate flux of 2890 g m −2  h −1 with competitive separation factor of 40.3.

研究领域: 材料科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Formation process and pervaporation of high aluminum ZSM-5 zeolite membrane with fluoride-containing and organic template-free gel

Deyu Si,Meihua Zhu,Xinmei Sun,Miao Xue,Yuqin Li,Ting Wu,Tian Gui,Izumi Kumakiri,Xiangshu Chen,Hidetoshi Kita

The formation progress of the high aluminum ZSM-5 zeolite membrane was investigated and characterized with the organic template-free and fluoride-containing initial synthesis gel. The nano spherical Silicalite-1 seed crystals were dissolved into amorphous by the fluoride-containing precursor synthesis gel. The amorphous contained elementary structural units (TO 4 ) and isolated five-membered ring structure of MFI zeolites. These were retained to provide the nucleation sites for high aluminum ZSM-5 zeolite. The ZSM-5 zeolite nucleus was grown into fine needle-like ZSM-5 zeolites, which were gradually grown into twin crystals, aggregation and compact ZSM-5 zeolites layer on the support without the organic template initial synthesis gel. In addition, the high aluminum ZSM-5 zeolite membranes kept the identical morphology and structure for separation of high concentration acetic acid (H 2 O/HAc) or inorganic acid (1 M H 2 SO 4 ) aqueous mixtures by XRD, SEM and NMR characterization. Furthermore, the membrane had a good dehydration performance and acid-stability by pervaporation. The flux and separation factor of the membrane for 10 wt% H 2 O/HAc mixtures were 0.98 kg∙m −2 ∙h −1 and 3200 at 348 K, respectively.

研究领域: 材料科学 · 化学工程
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ACS Applied Nano Materials · 2021 · IF 5.097

(3-Aminopropyl) Triethoxysilane-Modified ZIF-90 Nanoparticle/Polydimethylsiloxane Mixed Matrix Membranes for Ethanol Recovery via Pervaporation

Zhentong Han,Yaxin Zhao,Haoji Jiang,Ao Sheng,Hao Li,Hao Jia,Zhiyuan Yun,Zhong Wei,Heyun Wang

The present study eliminated nonselective defects by amending the MOF-based mixed matrix membrane (MMM) interface with (3-aminopropyl) triethoxysilane (APTES) via Schiff’s base reaction. This modification on the ZIF-90 nanoparticle surfaces enhanced the polydimethylsiloxane (PDMS) matrix interaction in the MMMs. Interfacial defects were then minimized through APTES-ZIF-90 nanoparticle surface alkoxy and PDMS chain hydroxyl group cross-linking. Enhanced chemical interactions between the nanoparticles and the polymeric matrix in the APTES-ZIF-90/PDMS MMMs resulted in higher interface compatibility and separation performance than the ZIF-90 nanoparticle MMMs, which ultimately improved its ethanol affinity and hydrophobicity. When the load of APTES-ZIF-90 nanoparticles was 15% and the temperature was 40 °C, the pervaporation performance of APTES-ZIF-90/PDMS MMMs was optimal, the separation factor was 16.8, and the permeation flux was 223 g/(m2·h). Compared with pure PDMS, the separation factor and permeation flux increased by 91 and 67%, respectively. In addition, stable APTES-ZIF-90/PDMS MMM pervaporation performance was observed after an optimal operation time of 120 h. Overall, the present work presented methods to optimize MOF-based MMMs for enhanced interface morphology and separation performance for ethanol recovery.

研究领域: 材料科学 · 分离技术
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CHEMICAL ENGINEERING SCIENCE · 2014 · IF 2.613

Preparation of a highly water-selective membrane for dehydration of acetone by incorporating potassium montmorillonite to construct ionized water channel

Chengyun Gao,Minhua Zhang,Zhongyi Jiang,Jiayou Liao,Xianmei Xie,Tinghong Huang,Jing Zhao,Jinshuan Bai,Fusheng Pan

Novel polymer–inorganic hybrid membrane was prepared by incorporating potassium montmorillonite (K + MMT) into chitosan (CS) for the dehydration of water–acetone mixture. The morphology, chemical and physical structure, as well as the hydrophilicity were characterized. The results showed that MMT uniformly dispersed in the chitosan matrix, formed hydrogen bonds with chitosan, and enhanced the thermal stability of the film. The membrane doped with 10   wt% of K + MMT exhibited the highest performance with separation factor of 2200, which was almost 8 times higher than 249 of pristine CS membrane at 50   °C for 5   wt% of water in the feed. The results suggested that the ionized water channel constructed by MMT intergallery in the hybrid membrane could greatly enhance the separation factor of CS membrane. Moreover, a plausible model for water transportation in the CS-K + MMT hybrid membranes was proposed. The results proved that K + MMT had a potential prospect in application for pervaporation .

CAS / MDL: 9012-76-4
研究领域: 材料科学 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2019 · IF 7.015

Bola-amphiphile-imidazole embedded GO membrane with enhanced solvent dehydration properties

Yangyang Mao,Mengchen Zhang,Long Cheng,Jianwei Yuan,Gongping Liu,Libo Huang,Mihail Barboiu,Wanqin Jin

Inspired by fast and selective water transport in natural Aquaporin (AQP), imidazole-quartet water channels (IQWC) constructed by imidazole-ureido (IU) molecular scaffolds, are excellent candidates to design membranes with fast and selective water transport properties. In this work, a water binding IU bola-amphiphile-imidazole compound was embedded with the hydrophilic and laminated graphene oxide (GO) to prepare IU-GO membrane. H NMR, TG, XRD , SEM, AFM and FTIR were conducted to characterize physicochemical properties of IU and IU-GO membrane. It was demonstrated that IU could well interact with GO to generate a robust membrane structure. The resulting IU-GO membranes were applied for pervaporation dehydration of n -butanol-water. The total flux and the separation factor of the optimized IU-GO membrane were 3506 g·m -2 ·h -1 and 4454 respectively when the membrane was measured at 343 K with butanol content of 80 wt%. Furthermore, the membrane exhibited good stability and separation performance during 120 h continuous operation test, showing great potential in application of solvent dehydration.

CAS / MDL: 822-06-0
研究领域: 材料科学 · 化学工程 · 膜技术
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POLYMER BULLETIN · 2020 ·Vol. 78 ·期 1 ·335-358 · IF 2.014

Preparation of PVA-PFSA-Si pervaporative hybrid membrane and its dehydration performance

Yuan Haikuan,Wang Chengchong,Liu Xiaodi,Lu Jie

In order to ameliorate the trade-off effect in pervaporation process and to reduce the micro-phase separation of hybrid membrane, polyvinyl alcohol (PVA)-perfluorosulfonic acid (PFSA) blending materials were modified by two inorganic components to prepare PVA-PFSA-Si hybrid membrane. PVA-PFSA-Si membrane was characterized by Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), contact angle measurements, scanning electron microscopy (SEM), positron annihilation lifetime spectrometer (PALS) and swelling measurements. As a second inorganic modifier, the effect of γ-glycidyloxypropyl trimethoxysilane (GPTMS) on the morphology of hybrid membrane was better than that of γ-aminopropyl triethoxysilane (APTEOS). PVA-PFSA-Si/polyacrylonitrile (PAN) composite membrane was used to pervaporatively dehydrate ethyl acetate (EAc)/H 2 O binary, EAc/ethanol (EtOH)/H 2 O ternary EAc/acetic acid (HAc)/EtOH/H 2 O quaternary solutions. At feed temperature of 40 °C, M8 membrane had the permeation fluxes ( J ) of 262.7, 215.2 and 182.6 g m −2  h −1 and the separation factors ( α ) of 6673, 3453 and 5374 for pervaporative dehydration of EAc/H 2 O (98/2, wt%) binary, EAc/EtOH/H 2 O (96/2/2, wt%) ternary and EAc/HAc/EtOH/H 2 O (96/1/1/2, wt%) quaternary solutions, respectively. The pervaporative results showed that PVA-PFSA-Si membrane had the excellent dehydration performances for EAc binary or multicomponent aqueous solutions.

研究领域: 材料科学 · 化学工程
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