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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

A novel TFNi pervaporation membrane with g-C3N4 quantum dots for high-efficiency IPA dehydration

Jia-Rui Yang,Yu-Fei Lin,Zhen-Liang Xu,Rui Jia,Yin-Xin Fang

Pervaporation (PV) shows significant potential for the highly selective isopropanol (IPA). The pursuit of developing PV membranes with outstanding separation effect and enduring high purity permeation is an indispensable goal. Based on polyamide (PA) separation layers, a polydopamine (PDA) mixed g-C 3 N 4 quantum dots (gCNQDs) coating as the interlayer was deposited onto a porous ceramic hollow fiber substrate to fabricate thin-film nanocomposite membranes with an interlayer (TFNi). The nanocomposite interlayer enabled the formation of a smoother and highly separated selective polyamide layer. The separation factor exhibited a 31-fold enhancement with the augmentation of the blending fraction of gCNQDs during the PDA coating process. The resulting TFNi membrane attained an exceedingly high separation factor of 10270 ± 90 with a permeate water concentration of 99.9 % and demonstrated a satisfactory flux of 1.40 ± 0.08 kg m −2  h −1 during the PV process of 90 wt% IPA dehydration at 60 °C. This study presents a fresh perspective on the implementation of nanocomposite interlayers, which is expected to expand the application of high-performance TFNi membranes in PV dehydration processes.

CAS / MDL: 62-31-7 77-86-1
研究领域: 材料科学 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

Self-assembled ILs-PVA micelle nanostructure impart the pervaporation membrane with high ethanol dehydration performance

Zakawat Ali,Xiaochun Zhang,Palwasha Khan,Jie Li,Nai Zhang,Qixin Wang,Muhammad Yasin,Mazhar Amjad Gilani,Asim Laeeq Khan,Linglong Shan,Xiangping Zhang

Achieving strong interaction with the targeted composition and constructing abundant transport channels is crucial to obtain the pervaporation (PV) membrane with high selectivity and flux. Here, three ionic liquids (ILs) were screened out based on their relative selectivity and capacity targeting for bioethanol dehydration by COSMO-RS. The interaction energies analysis between ILs, EtOH, and H 2 O suggests that the ILs can form strong hydrogen bonds with water and disrupt the hydrogen bond in the EtOH–H 2 O azeotropic mixture, which is beneficial for improving the selectivity. Furthermore, driven by the multiple hydrogen bonds, electrostatic interactions, and van der Waals forces, ILs could self-assemble with polyvinyl alcohol (PVA) to fabricate the PV membrane with well-ordered micelle nanostructure, as its structure was revealed by MD simulations. The formation of the ILs-PVA micelle dramatically influenced membrane surface morphology, roughness, and water contact angle, providing an extra transport channel for the membrane. The optimal membrane (at the cmc point) exhibited a superior ethanol dehydration separation factor of 1627, along with a flux of 684 g/m 2 h at 50 °C. It can be expected that this novel self-assembled ILs-PVA micelle nanostructure strategy will find promising applications in other azeotropic mixture separation processes, like ethanol-ethyl acetate, water-butanol, etc.

研究领域: 材料科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Robust MIL-96 tubular membranes for efficient separation of acetic acid/water mixtures by pervaporation

Yumeng Zhao,Guoshu Gao,Peng Zhu,Cun Liu,Xiongfu Zhang,Feichao Wu,Guohui Yang

Metal-organic framework (MOF) membranes hold great potential for acetic acid dehydration by pervaporation. However, it remains challenging to develop stable MOF membranes suitable for this application due to the corrosion of membranes by acetic acid. Herein, we report a robust aluminum (Al)-based MIL-96 membrane on porous ceramic tubes for acetic acid pervaporation dehydration. It is prepared by an induction strategy with Al-Sol@MIL-96-C layer, obtained by calcining an Al-based sol layer containing small MIL-96 seeds. The induced layer possesses a sponge-like structure and high reactivity, favoring the uniform growth of MIL-96 crystals and establishing a strong connection between the membrane layer and the support. The achieved MIL-96 membrane, with a thickness of ∼2 μm, exhibits excellent performance in separating 90 wt% acetic acid/water mixtures by pervaporation, showing a high separation factor of ∼3000 with a permeation flux of 1.54 kg/(m 2 ·h). Notably, due to the connectivity of the Al-Sol@MIL-96-C layer, these membranes show long-term operational stability for over 200 h, as well as great tolerance to ultrasonic treatment, highlighting the enormous potential for applications. This work provides a feasible approach to fabricate robust MOF membranes for pervaporation separation of acetic acid/water mixtures.

CAS / MDL: 554-95-0
研究领域: 材料科学 · 化学工程
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2025 · IF 3.9

MOF UiO-66 Membranes for Pervaporation Prepared by Secondary Growth Using Zr(n-OPr)4

Shenyi Tang,Chenglian Luo,Zhi Wang,Xinlei Liu

A defect-free and stable metal–organic framework (MOF) membrane is a promising candidate for the separation of methanol/methyl tertiary butyl ether (MeOH/MTBE) mixtures. In this work, a structural-integrity and low-thickness (∼400 nm) UiO-66 membrane was fabricated by regulating the metal ion/ligand molar ratio in the synthesis solution and optimizing the preparation process using the secondary growth method with safer and more environment-friendly Zr(n-OPr)4 metal source. Based on the effective pore size and inherent amphiphilic structure of UiO-66, the membrane exhibits exceptional pervaporation (PV) performance. For the separation of MeOH/MTBE (5:95 wt/wt %) mixtures, the membrane displays an outstanding separation performance with an average separation factor of 2.23 × 104 and an average total flux of 3.61 kg·m–2·h–1 at 40 °C, which is superior to most membranes reported for the PV separation of MeOH/MTBE mixtures. In addition, a 72 h PV process was used to further confirm the structural stability of the membrane.

CAS / MDL: 23519-77-9 100-21-0
研究领域: 材料科学 · 化学工程
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JOURNAL OF APPLIED POLYMER SCIENCE · 2017 ·Vol. 134 ·期 17 · IF 1.86

Three-component mixed matrix organic/inorganic hybrid membranes for pervaporation separation of ethanol–water mixture

Zhigao Zhu,Deng Hu,Yuanren Liu,Ying Xu,Gaofeng Zeng,Wei Wang,Yanfeng Zhang,Fuyi Cui

Mixed matrix membranes (MMMs) were made by incorporating vinyltrimethoxysilane (VTMS)-modified Silicalite-1 zeolite nanoparticles (V-Silicalite-1 NPs) into fluorinated polybenzoxazine (F-PBZ) modified polydimethylsiloxane (PDMS) polymer through in situ polymerization method. The membrane morphology, surface wettability, and pervaporation performance were systematically investigated. The addition of F-PBZ into PDMS membranes resulted in substantially improved flux and marginal increase of separation factor, which is the result of higher free volume and higher hydrophobicity caused by the addition of F-PBZ. The modification of Silicalite-1 NPs improved the interfacial contact between zeolite crystals and polymer phase. The incorporation of hydrophobic V-Silicalite-1 zeolite NPs into the PDMS membranes led to much higher separation factor but reduced flux, which is the result of increased hydrophobicity and reduced free volume. The three-component MMMs with V-Silicalite-1 zeolite NPs in the F-PBZ fluorinated PDMS exhibited separation factor of 28.7 and flux of 0.207 kg m −2 h −1 for 5 wt % ethanol aqueous solution at 50 °C, while the pure PDMS membranes only had separation factor of 4.8 and flux of 0.088 kg m −2 h −1 . The substantial increase of both flux and separation factor were attributed to the higher hydrophobicity and free volume caused by the incorporation of both hydrophobic zeolite crystals and F-PBZ polymer into the PDMS membranes. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134 , 44753.

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AICHE JOURNAL · 2021 ·Vol. 67 ·期 5 ·e17144 · IF 3.993

Second interfacial polymerization of thin-film composite hollow fibers with amine-cyclodextrins for pervaporation dehydration

Xi Yu,Tengyang Zhu,Sheng Xu,Xuan Zhang,Ming Yi,Shu Xiong,Shutong Liu,Liang Shen,Yan Wang

High performance thin-film composite (TFC) hollow fiber membranes have been developed for pervaporation dehydration by second interfacial polymerization (SIP) modification with three kinds of amine-functionalized β -cyclodextrin (amine-CDs), which were synthesized by modifying β -CD with ammonia, ethylenediamine (EDA), and tris(2-aminoethyl)amine, respectively. The chemical properties of amine-CDs and SIP-modified TFC membranes were characterized by various techniques. The effects of amine-CD type and SIP parameters (pH or concentration of CD-EDA solution) were studied systematically to acquire the optimized selective layer of TFC membranes for ethanol dehydration. Among all SIP-modified TFC membranes, the one with SIP by 2 wt% CD-EDA aqueous solution (pH = 2) exhibited the most outstanding separation performance with a ultrahigh permeation flux (3,018.0 ± 12.0 g/m 2 hr) and permeate concentration (98.7 ± 0.2 wt% water) at 50°C (equivalent to separation factor of 415), contributed by the effectively incorporated CD with rich hydrophilic functional groups and intrinsic nanocavities facilitating the passage of water molecules.

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

Optimizing nanostrands-inserted graphene oxide membrane with polyelectrolyte protective layer for enhanced ethanol pervaporation dehydration

Wanhui Hao,Ziqiang Tong,Xiufeng Liu,Baoquan Zhang

Graphene oxide (GO) composite membranes were fabricated on polyacrylonitrile (PAN) substrates via inserting copper hydroxide nanostrands (CHNs) between GO sheets and coupling with an ultrathin hydrophilic sodium alginate (SA) top-layer. The prepared membranes were characterized by using FESEM, FTIR, XRD, water contact angle and nanoscratch measurements. The intercalation of CHNs could enlarge ultrafast water permeation channels in base GO membrane without destroying its interlayered structure. Hydrogen bonding and electrostatic interaction ensured SA layer could firmly adhere onto base GO membrane, which should be conducive to swelling prevention and selective moisture enrichment. The dehydration performance was investigated as a function of SA deposit, CHNs intercalation, and feed temperature. Under optimal SA deposit, the permeation flux could be improved by 30 wt% after the intercalation of CHNs between GO sheets. The permeation flux through the prepared membrane could reach up to 3.65 kg m −2 h −1 with an excellent separation selectivity (99.70 wt% water content in permeate) at 70 °C for 10 wt% water–ethanol solution. The permeation flux and separation selectivity both increased with elevated temperatures, revealing the complete anti-trade-off behavior. The prepared membrane also possessed enhanced mechanical strength and firm interfacial adhesion, which ensured its integrity in practical operating conditions.

CAS / MDL: 9005-38-3
研究领域: 材料科学 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2019 · IF 7.015

Construction of well-arranged graphene oxide/polyelectrolyte complex nanoparticles membranes for pervaporation ethylene glycol dehydration

Jia-Kai Wu,Chun-Chun Ye,Wen-Hai Zhang,Nai-Xin Wang,Kueir-Rarn Lee,Quan-Fu An

Dehydration of ethylene glycol (EG), a valued product in chemical industries, was efficiently implemented by pervaporation with a graphene oxide (GO)-incorporated polyelectrolyte complex nanoparticles (PEC NPs) membrane. GO-incorporated PEC NPs with solution processability were prepared through a new strategy of “complex precipitation–redispersion”. The PEC NPs-based membranes were prepared via solution casting, and their structural characteristics and hydrophilic property were investigated systematically. Spherical PEC NPs building blocks increase cavities and thus flux of the membranes, while the tightly associated ion-pair structure coupled with strong interface interactions between regularly-arranged GO nanosheets and PEC matrix led to good separation factor. In detail, the resulted membrane PEC NPM/GO-3 presented a flux of 961 g m −2 h −1 and water in permeate of 99.25 wt% in dehydrating 10.0 wt% water/EG mixtures at 60 °C. Moreover, the PEC NPM/GO-3 showed a tensile strength of 139.1 MPa and higher long-term operation stability, which was important for commercial application.

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

Ionic liquid modified graphene oxide-PEBA mixed matrix membrane for pervaporation of butanol aqueous solutions

Wangyang Tang,He Lou,Yifang Li,Xiangbin Kong,Yanhui Wu,Xuehong Gu

This work explored a novel way to modify graphene oxide (GO) with ionic liquid (IL) and incorporate the modified GO into polyether block amide (PEBA) membrane for pervaporation of butanol aqueous solutions. The adsorption properties of GO and ionic liquid N -octylpyridiniunm bis (trifluoromethyl) sulfonyl imide [OPY][Tf2N] modified graphene oxide (IL-GO) for butanol and water were investigated via molecular simulation . Because ionic liquid [OPY][Tf2N] has good butanol affinity and hydrophobicity , the adsorption selectivity of butanol over water by the IL-modified GO increased by about 4 times compared with the pristine GO. Then IL-GO was incorporated into PEBA to fabricate mixed matrix membrane. The membrane was characterized, and the pervaporation performance of the membrane was evaluated. Pervaporation experiments showed that the incorporation of IL-GO is in favour of enhancing the membrane performance. Compared with pristine PEBA membrane, at 35 °C, for 2.5 wt% butanol aqueous solutions, the separation factor and permeation flux of the mixed matrix membrane with 1 wt% content of IL-GO were increased by 31.5% and 18.2%, respectively. Meanwhile, connecting ionic liquid to GO can effectively improve the membrane stability by preventing the loss of ionic liquid in the pervaporation process.

CAS / MDL: 5089-70-3
研究领域: 材料科学 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2019 · IF 7.015

Covalent cross-linking for interface engineering of high flux UiO-66-TMS/PDMS pervaporation membranes

Hui Wang,Sihan Tang,Yunxia Ni,Chongrui Zhang,Xiangwei Zhu,Qiang Zhao

Interface compatibility between hydrophilic metal-organic frameworks (MOFs) and hydrophobic polydimethylsiloxane (PDMS) is less effectively reconciled through supramolecular modifications such as surfactant and polymer wrapping. Here we report a covalent cross-linking strategy to strengthen MOFs ~ PDMS interfaces. Zirconium MOFs (UiO-66-NH 2 ) were modified with trimethoxysilan (TMS), which could further react with silanol terminated PDMS to enhance UiO-66 ~ PDMS interface compatibility. High content UiO-66-TMS (up to 50 wt%) were loaded into PDMS while retaining good membrane formation ability, mechanical properties and pervaporation selectivity, in contrast to pristine UiO-66-NH 2 that decreases membrane strength and separation performances even at much lower loading content (10 wt%). Flux of mixed matrix membranes in dehydrating ethanol-water mixtures was highly improved while retaining the selectivity. It allows for the efficient production of concentrated ethanol (equivalent flux: 2234 g/m 2 h; ethanol in permeate: 53 wt%) from dilute feed through two-times consecutive pervaporation at 40 °C. Moreover, the membrane with covalently enhanced interfaces exhibit stable performance during 100 h continuous operation.

研究领域: 材料科学 · 化学工程
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Petroleum Science · 2018 ·Vol. 15 ·期 1 ·146-156 · IF 1.624

Fabrication of high-performance PVA/PAN composite pervaporation membranes crosslinked by PMDA for wastewater desalination

Zhang Rui,Xu Xiaoying,Cao Bing,Li Pei

The pyromellitic dianhydride (PMDA) crosslinked poly(vinyl alcohol) (PVA) was coated on top of the PAN ultrafiltration membrane to form a PVA/PAN composite PV membranes for wastewater desalination. The composite membranes have high application value in industrial wastewater treatment. By varying the membrane fabrication parameters including the weight percent (wt%) of the PMDA, the crosslink temperature and duration, membrane with the best desalination performance was obtained. The composite membrane with a 2-μm-thick PVA selective layer containing 20 wt% of PMDA and being crosslinked at 100 °C for 2 h showed the highest NaCl rejection of 99.98% with a water flux of 32.26 L/(m 2  h) at 70 °C using the 35,000 ppm NaCl aqueous solution as feed. FTIR spectroscopy, wide-angle X-ray diffraction, thermogravimetric analysis and scanning electron microscope have been used to characterize the structures and properties of both the crosslinked PVA dense films and PVA/PAN composite membranes. The effects of the concentrations of PMDA, the crosslinking time and temperature to the membrane water contact angle, swelling degree, salt rejection and water flux were systematically studied.

CAS / MDL: 89-32-7
研究领域: 材料科学 · 环境工程
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CHEMIE INGENIEUR TECHNIK · 2021 · IF 1.672

Synthesis of Graphene Oxide Membrane for Separation of p-Xylene and o-Xylene by Pervaporation

Hao Guo,Zheng Wan,Yanhong Li,Xiao He,Aisheng Huang

In this study, a graphene oxide (GO) membrane is developed for the separation of p -xylene (PX, 0.58 nm) from o -xylene (OX, 0.68 nm). Attributing to the suitable d-spacing size (0.58 nm), the GO membrane allows more PX to pass through than OX, leading to a high PX/OX selectivity. At 110 °C for the separation of equimolar PX/OX mixture, the PX/OX separation factor is 9.4 and PX flux is 145.3 g m −2 h −1 , respectively, which is promising for the separation of xylene isomers by pervaporation. The separation performance of the GO membrane is further confirmed by simulation studies.

研究领域: 材料科学 · 化学工程 · 分离技术
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