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JOURNAL OF MEMBRANE SCIENCE · 2015 · IF 5.056

High-performance composite membranes incorporated with carboxylic acid nanogels for CO2 separation

Xueqin Li,Zhongyi Jiang,Yingzhen Wu,Haiyang Zhang,Youdong Cheng,Ruili Guo,Hong Wu

Composite membranes were fabricated by incorporating carboxylic acid nanogels (CANs) into a Pebax MH 1657 matrix for potential applications in CO 2 /CH 4 (or N 2 ) separation. CANs were synthesized by precipitation polymerization of N-isopropylacrylamide (NIPAM), acrylic acid (AA) monomer and N,N′-methylenebisacrylamide (BIS) crosslinker. The incorporation of CANs simultaneously tailored favorable water environment and increased CO 2 transport sites within the membranes. With increasing CANs loading, the homogeneously dispersed CANs in the Pebax matrix offered more favorable water environment and the additional carboxyl group sites for efficient CO 2 transport, thus constructing interconnected preferential CO 2 transport passageways. The Pebax-CANs-30 composite membrane exhibited the highest gas separation performance, with the CO 2 /CH 4 and CO 2 /N 2 selectivities of 33 and 85 respectively, and a CO 2 permeability of 2026 Barrer (1 Barrer=10 −10   cm 3 (STP) cm/(cm 2   s   cmHg), well surpassing the Robeson's upper bound limit reported in 2008. This effort will give rise to a new option to tailor water environment and increase CO 2 transport sites for fabricating high-performance CO 2 separation membranes .

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

Exfoliation-free layered double hydroxides laminates intercalated with amino acids for enhanced CO2 separation of mixed matrix membrane

Yanan Wang,Ning Zhang,Hong Wu,Yanxiong Ren,Leixin Yang,Xiaoyao Wang,Yingzhen Wu,Yutao Liu,Rui Zhao,Zhongyi Jiang

Harvesting energy from biogas is a potential way to retard the depletion of fossil fuels and fight against global warming simultaneously. Membrane technology holds great promise to achieve cost-effective biogas upgrading, along with advantages of low energy consumption and environmental friendliness, which leads to extensive exploration in fabricating CO 2 membranes with high separation performance. In this study, mixed matrix membranes are fabricated by incorporating exfoliation-free layered double hydroxides laminates intercalated with amino acids (Phe with hydrophobic side chains and Glu with hydrophilic side chains) into a low-cost commercial Pebax (poly (amide-b-ethylene oxide)) polymer. Both amino and carboxyl groups can facilitate the transport of CO 2 through quadrupole moment interaction, enlarged interlayer spacing and reversible reaction. Particularly, MMM containing 5 wt% AA-LDH exhibits an optimal permeability of 790 Barrer and a promising CO 2 /CH 4 selectivity of 31, which is 64.6% and 83.9% higher than the pristine Pebax membrane, respectively. The distinct advantages in terms of facile fabrication and processability confer the LDH-based membrane with great potential for large-scale CO 2 capture and separation.

CAS / MDL: 7784-27-2 63-91-2
研究领域: 材料科学 · 环境工程
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

Pebax-derived ultra-microporous carbon molecular sieve composite membrane assisted by organic interlayer for gas separation

Xu Zhang,Haibiao Xu,Qin Meng,Zheng Fan,Wenhai Zhang,Chong Shen,Guoliang Zhang

In this study, novel Pebax-derived ultra-microporous carbon molecular sieve composite membrane assisted by polydopamine (PDA) interlayer was synthesized by dip-coating and pyrolysis method. Pebax was first explored as the precursor and PDA was selected as flexible coating layer on the polymeric substrate in preparation of CMS composite membranes. Pebax had long linear chain polyamine structure and contained large number of carbonyl groups and hydrogen bonds that were pyrolyzed under relatively low temperature. Compared with incorporating inorganic interlayer, the PDA organic interlayer constructed under mild condition had excellent adhesion towards the polymeric support. Since the intrusion of precursor Pebax into the pore of substrate was prevented, the channels of passage were shortened and the transport of gas molecules was greatly promoted. Through designable chemical bonding resistant to harsh conditions, the adhesion between organic interlayer and CMS layer were kept strong due to natural compatibility of materials, leading to the formation of defect-free CMS membranes with enhanced stability in operation. The fabricated CMS membrane displayed excellent H 2 /CO 2 selectivity of 40.69 and very competitive permeability of 1.23 × 10 −7  mol m −2  Pa −1 s −1 .

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Membranes · 2021 ·Vol. 11 ·期 9 ·693 · IF 4.106

A Novel Composite Material UiO-66@HNT/Pebax Mixed Matrix Membranes for Enhanced CO2/N2 Separation

Fei Guo,Bingzhang Li,Rui Ding,Dongsheng Li,Xiaobin Jiang,Gaohong He,Wu Xiao

Mixing a polymer matrix and nanofiller to prepare a mixed matrix membrane (MMM) is an effective method for enhancing gas separation performance. In this work, a unique UiO-66-decorated halloysite nanotubes composite material (UiO-66@HNT) was successfully synthesized via a solvothermal method and dispersed into the Pebax-1657 matrix to prepare MMMs for CO2/N2separation. A remarkable characteristic of this MMM was that the HNT lumen provided the highway for CO2diffusion due to the unique affinity of UiO-66 for CO2. Simultaneously, the close connection of the UiO-66 layer on the external surface of HNTs created relatively continuous pathways for gas permeation. A suite of microscopy, diffraction, and thermal techniques was used to characterize the morphology and structure of UiO-66@HNT and the membranes. As expected, the embedding UiO-66@HNT composite materials significantly improved the separation performances of the membranes. Impressively, the as-obtained membrane acquired a high CO2permeability of 119.08 Barrer and CO2/N2selectivity of 76.26. Additionally, the presence of UiO-66@HNT conferred good long-term stability and excellent interfacial compatibility on the MMMs. The results demonstrated that the composite filler with fast transport pathways designed in this study was an effective strategy to enhance gas separation performance of MMMs, verifying its application potential in the gas purification industry.Keywords:composite material;UiO-66;HNT;mixed matrix membrane;CO2/N2separation

CAS / MDL: 62-31-7 10026-11-6
研究领域: 材料科学 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2022 · IF 10.53

Relationship between wet coating thickness and nanoparticle loadings based on the performance of mixed matrix composite membranes

Bo Wang,Guangyu Xing,Jun-rui Zhang,Menglong Sheng,Jixiao Wang,Zhi Wang

Wet coating thickness and nanoparticle loadings are two important parameters that greatly impact the performance of mixed matrix composite membranes (MMCMs). In this work, two kinds of MMCMs, with Pebax as the continuous phase polymer and MIL-101(Cr) and UiO-66(Zr) as the dispersed phase porous materials respectively, were fabricated to explore the internal relationship between the two parameters. The change of membrane performance via adjusting wet coating thickness and nanoparticle loadings is discussed through pure gas and mixed gas tests and shown by contour data analysis. Generally, the wet coating thickness is significant to keep the membrane densification and nanoparticle loadings to increase the permselectivity to some degree. In addition, the nanoparticle size shows great impact on membrane performance due to the small-size nanoparticles with huge surface energy. At last, this work verifies that reinforcing the interaction between nanoparticles and polymer matrix is beneficial to improve the membrane performance.

研究领域: 材料科学 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Metal-covalent organic framework nanosheets engineered facilitated transport membranes for toluene/n-heptane separation

Jin Du,Shuwei Liang,Meidi Wang,Yuhan Wang,Tianpei Yi,Zhiming Zhang,Fusheng Pan,Zhongyi Jiang

Facilitated transport membranes is a promising strategy to fabricate efficient separation membranes for aromatic/aliphatic mixtures. However, building up selective channels with uniformly distributed facilitated transport sites is still challenging. In this study, Cu-TAPB-COF (CuCOF) nanosheets , a kind of metal-covalent organic frameworks (MCOFs), were synthetized and introduced into poly (ether-block amide) (Pebax®2533) matrix to construct facilitated transport membranes for toluene/ n -heptane mixtures. As the aromatic skeleton linked by covalent interaction, CuCOF could provide continuous low mass transfer resistance channel. And Cu(I) exist in skeleton could serve as uniformly distributed facilitated transport sites and maintain a long-term stability. The resulting membrane exhibited a higher adsorption selectivity and lower swelling degree compared with pure Pebax membrane. The membrane exhibited high pervaporation separation performance for 50 wt% toluene/ n -heptane mixture. When the filling contents of CuCOF was 2.0 wt%, the membrane achieved a permeation flux of 937 g m −2  h −1 and the separation factor of 4.7.

CAS / MDL: 10031-43-3 35344-95-7
研究领域: 材料科学 · 化学工程 · 膜分离技术
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JOURNAL OF MEMBRANE SCIENCE · 2026 · IF 8.8

In-situ pyrrole polymerization modified Pebax membrane with enriched selective adsorption sites for aromatic/aliphatic hydrocarbon separation

Linhan Xie,Mengxin Shen,BeiBei Liu,Kai Zhao,Yushan Sun,Jie Li,Naixin Wang,Quan-Fu An

Pebax-PPy membranes are constructed for aromatic/aliphatic hydrocarbon separation. • The separation mechanism of the Pebax-PPy membrane is explored. • Pebax-PPy membrane achieves a good separation factor for toluene/ n -heptane mixture. Separation of low-cracking-activity aromatics from naphtha prior to steam cracking is critical for boosting olefin yields. Pervaporation technology utilizing aromatic-selective membranes enables efficient separation of aromatic/aliphatic hydrocarbon mixtures. In this work, an in-situ oxidative polymerization strategy is proposed to directly polymerize pyrrole monomers within a polyether block amide (Pebax) solution, followed by spin-coating to fabricate Pebax-Polypyrrole (PPy) membranes. The in-situ formed PPy is uniformly dispersed in the Pebax matrix, effectively avoiding filler agglomeration and interfacial defects generated in conventional mixed matrix membranes. Theoretical simulations reveal that π-π interactions and N-H···π hydrogen bonding between PPy and aromatics significantly improve the membrane's selectivity toward aromatics. The Pebax-PPy membrane achieves a separation factor of 7.16 and a permeation flux of 662 g m −2  h −1 for a 50 wt% toluene/ n -heptane mixture. Furthermore, the Pebax-PPy membrane enriches toluene from 15.0 wt% to 90.2 wt% in simulated naphtha via a two-stage membrane cascade process, demonstrating enormous application potential for the pre-separation of aromatics from naphtha. Download: Download high-res image (398KB) Download: Download full-size image

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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

An exploration of novel natural gas leak detection based on the efficient CH4/N2 separation of polymer blend membrane

Qingping Xin,Yucheng Pan,Chao Zhang,Lei Zhang,Chensheng Dong,Ligang Lin,Lizhi Zhao,Hui Ye,Yuzhong Zhang

The CH 4 /N 2 high-efficiency membrane separation technology is capable of effectively enriching CH 4 from natural gas, and holds great potential for application in the fields of biogas purification and natural gas pipeline leak detection. However, preparing high-performance separation membranes is challenging due to the similarity between CH 4 and N 2 molecules. To enhance the CH 4 /N 2 separation performance, block polyetheramide copolymer (Pebax)/EVA blended membranes were fabricated in this study. Additionally, a novel gas leakage detection tube was prepared. The EVA14 (14 wt% VA) membrane exhibits an optimal transport-facilitated channel among a series of pure EVA membranes, resulting in a CH 4 permeability of 21.41 Barrer and CH 4 /N 2 selectivity reaches 1.80 under mixed-gas feed conditions at 35 °C. The CH 4 permeability of Pebax/EVA (30 wt%) reaches 120.5 Barrer by physical blending, and the CH 4 permeability is increased by 191 % in comparison with pure EVA14 membrane. The Pebax/EVA (10 wt%) membrane exhibits the optimum CH 4 /N 2 selectivity, and compared with pure EVA membrane increased by 35.5 %. EVA and Pebax polymers are blended for the first time for CH 4 /N 2 separation, and the blending of block polyetheramide copolymer intensifies the membrane's separation performance comprehensively. The natural gas leak detection tube was fabricated with a membrane, offering a new and efficient CH 4 /N 2 separation strategy.

CAS / MDL: 71-36-3 1330-20-7
研究领域: 材料科学 · 环境工程
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY · 2023 · IF 6.1

Constructing mixed matrix membranes for CO2 separation based on light lanthanide fluoride nanosheets with mesoporous structure

Yanli Zhang,Meixue Zhao,Xu Li,Qingping Xin,Xiaoli Ding,Lizhi Zhao,Hui Ye,Ligang Lin,Hong Li,Yuzhong Zhang

The incorporation of porous nano-fillers into mixed matrix membranes (MMMs) has a great impact on CO 2 separation. In this study, a series of F-Ln (Ln is the Light Lanthanide, Ln = La, Ce, Pr, Nd) nanosheets with mesoporous structure was fabricated as a filler in Pebax®1657 matrix to improve the performance of CO 2 separation. F-Ln nanosheets are uniformly distributed in the membrane and the mesoporous structure can construct multiple channels for CO 2 fast transport in Pebax/F-Ln MMMs. The pore diameter of nanosheet is in order: F-La > F-Ce > F-Pr > F-Nd, and the smaller pore diameter of nanosheets is beneficial to improve the CO 2 separation performance. In humidified conditions, Pebax/F-Nd-6 MMMs show optimum separation performance among MMMs, and the CO 2 permeability is up to 1265 Barrer and CO 2 /CH 4 selectivity is 36.7, which are 2.3 times and 1.9 times higher than pure Pebax and approaches 2019 upper bound. Meanwhile, to demonstrate the potential universal applicability of F-Ln nanosheets in CO 2 separation, XLPEO/F-Ce MMMs were fabricated to separate CO 2 /N 2 and the performance exceeds the 2019 upper bound. The efficient CO 2 separation performance of 2D F-Ln nanosheets with mesoporous structure in membranes reveals the potential application of these nanosheets in industrial CO 2 separation.

研究领域: 材料科学 · 环境工程
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JOURNAL OF MEMBRANE SCIENCE · 2026 · IF 8.8

Supramolecularly engineered ZIF-L/GO/Pebax mixed-matrix membranes with intercalated network structures for enhanced CO2/N2 separation

Shumin Li,Wenjun Su,Zeyang Di,Suyue Zhong,Junjie Ma,Jian Li

Membrane separation has emerged as a competitive energy-efficient approach for carbon capture and flue gas treatment. Membrane materials and structures are the core of gas separation membranes, which collectively govern gas molecular mass transfer and separation behaviors. Two-dimensional (2D) graphene oxide (GO) porous nanosheets hold great promise for gas separation due to their nanoscale thickness and structural tunability, but they are often limited by low permeability. Herein, we propose a supramolecular strategy to fabricate ZIF-L/GO/Pebax mixed matrix membranes with intercalated network architectures for efficient CO 2 /N 2 separation. Leaf-like ZIF-L expands the interlayer spacing of GO nanosheets and constructs high-speed continuous gas transport pathways within the membrane. This unique intercalated structure provides abundant CO 2 -philic sites, significantly enhancing CO 2 solubility and enabling highly selective gas molecular sieving. Moreover, hydrogen bonds and chelation coordination interactions between ZIF-L/GO and polymer matrix ensure excellent interfacial compatibility while reinforcing structural stability. This supramolecular structural engineering approach effectively mitigates the limitations of traditional membranes, achieving CO 2 permeability of 1000.8 Barrer and CO 2 /N 2 selectivity of 45, exceeding the 2008 Robeson upper bound and approaching the 2019 limit. Additionally, the membrane displays superior mechanical properties and long-term operational stability, providing a promising avenue toward high-performance materials for efficient CO 2 capture.

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JOURNAL OF MEMBRANE SCIENCE · 2018 · IF 6.578

Mixed matrix membranes comprising aminosilane-functionalized graphene oxide for enhanced CO2 separation

Jinhui Zhang,Qingping Xin,Xu Li,Mingya Yun,Rui Xu,Shaofei Wang,Yifan Li,Ligang Lin,Xiaoli Ding,Hui Ye,Yuzhong Zhang

Mixed matrix membranes (MMMs) are challenged by the non-ideal interfacial morphologies that leads to the weakened gas separation performances and mechanical strength . Filler surface modification with organosilanes is an effective approach to build the linkage between polymer and the fillers. In this study, we fabricated MMMs by introducing aminosilane functionalized graphene oxide (f-GO) nanosheets into Pebax ® 1657 matrix. The introduction of f-GO decreased the crystallinity and increased chain mobility of Pebax matrix. Benefiting from the improved filler dispersion, semi-interpenetrated Pebax chains in the Si-O-Si network at the interface, and the high intrinsic mechanical strength of GO, the MMMs exhibit a 1.7-times higher Young's modulus and 1.1-times higher break strength. The amino groups on GO help to construct a facilitated transport pathway along the polymer-filler interface. With greatly improved CO 2 separation performances in dry state, the membranes exhibited even higher performances in humidified state. Particularly, Pebax/f-GO-0.9% membrane showed a high CO 2 permeability of 934.3 Barrer, and a CO 2 /CH 4 selectivity of 40.9, a CO 2 /N 2 selectivity of 71.1, surpassing the Robeson upper bound and quite promising for carbon capture.

CAS / MDL: 919-30-2
研究领域: 材料科学 · 环境工程
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JOURNAL OF MEMBRANE SCIENCE · 2018 · IF 6.578

Embedding Ag+@COFs within Pebax membrane to confer mass transport channels and facilitated transport sites for elevated desulfurization performance

Fusheng Pan,Meidi Wang,He Ding,Yimeng Song,Weidong Li,Hong Wu,Zhongyi Jiang,Baoyi Wang,Xingzhong Cao

In this study, covalent organic frameworks (COFs) are utilized as carriers to immobilize metal ions in facilitated transport membranes for organic solvent separation for the first time. SNW-1, a kind of COFs with high amount of amino groups, were loaded with Ag + ions and then incorporated into Pebax matrix to prepare hybrid membranes. Under optimal conditions, 48.11 wt% of Ag + was loaded onto SNW-1 through a facile approach, which greatly intensified the mass transfer of unsaturated penetrant molecules (thiophene) by π-complexation. The channels within SNW-1 decreased the mass transport resistance and imparted the molecular sieving ability. The organic nature of SNW-1 optimized the interfacial affinity between filler and polymer, and rendered appropriate free volume properties. The membranes displayed simultaneously enhanced permeation flux and selectivity in pervaporation gasoline desulfurization. Especially, when the content of Ag + @SNW-1 was 9 wt%, the optimum performance towards thiophene concentration of 1312 ppm under 60 °C, was achieved with permeation flux of 16.35 kg/(m 2 h) and enrichment factor of 6.8, which was increased by 78.5% and 30.0%, respectively, compared with pure Pebax membranes. In addition, the anti-swelling property of the membranes was improved and the membranes possessed superior long-term stability. This study demonstrates that COFs are superior carriers to immobilize metal ions within facilitated transport membrane for efficient liquid separation.

研究领域: 材料科学 · 化学工程
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