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Polyethersulfone-modulated Matrimid®-derived carbon molecular sieve membranes for enhanced C3H6/C3H8 separation

JOUrNAL OF membrane science 2025年 727卷

作者： Sun, Fake Gao, Zeyuan Sun, Yongchao Liu, Yijun Guan, Jianyu Li, Hongjin Li, Tianyou He, Gaohong Ma, Canghai Dalian Univ Technol R&D Ctr Membrane Science& Technol Sch Chem Engn State Key Lab Fine Chem Dalian 116024 Peoples R China

Polymer-derived carbon molecular sieve (CMS) membranes hold significant potentials for propylene/propane (C3H6/C3H8) separation;however, further enhancement of their molecular sieving properties remains a critical challenge. In this study, we present a novel approach to regulating the pore structure of CMS membranes by incorporating the rubbery polyethersulfone (PES) into the Matrimid (r) precursor to fabricate CMS membranes. The incorporation of PES during pyrolysis creates voids between Matrimid (r) molecular chains, increasing the chain d-spacing and the content of ultramicropores, significantly enhancing the C3H6/C3H8 separation performance of the CMS membranes. As the PES content in the precursor membrane increases, the rising content of ultramicropores leads to improved C3H6/C3H8 selectivity, along with a minor increase in gas permeability. Notably, the 60 %Matrimid (r)+40 %PES-550 CMS membrane displays a C3H6 permeability of 70.3 Barrer with a C3H6/C3H8 selectivity of 21.4, representing increases of 194 % and 188 %, respectively, compared to Matrimid (r)- 550 and exceeding the C3H6/C3H8 separation upper bound. Furthermore, under mixed gas separation conditions with a 50/50 (mol%) C3H6/C3H8 feed, this membrane exhibited a C3H6 permeability of 47.6 Barrer with a C3H6/ C3H8 selectivity of 18.3, also surpassing the mixed gas upper bound for C3H6/C3H8 separation. The design principle of CMS membranes in this work provides a new approach for the preparation of high-performance CMS membranes, with the potential for separating the challenging C3H6/C3H8 mixture.

关键词： Carbon molecular sieve (CMS) membranes Propylene and propane Gas separation

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Ethanol activation of polyester membrane for superior dye/salt separation performance

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SEPArATION ANd PUrIFICATION TECHNOLOGY 2025年第PartB期353卷

作者： Tang, Meng-Meng Jin, Xiao-Gang Tang, Xin Yu, Miao Ma, Xiao-Hua Xu, Zhen-Liang East China Univ Sci & Technol Chem Engn Res Ctr Sch Chem Engn Membrane Science& Engn R&D Lab Shanghai 200237 Peoples R China

dye wastewater poses a severe danger to the environment and human health. The purification of dye wastewater is the focus and hotspot of most researchers. In this work, ethylene glycol (EG) was selected as an aqueous phase monomer to fabricate polyester membranes through an interfacial polymerization reaction. Then the polyester membrane was activated by ethanol aqueous solution. By adjusting the activation time and concentration of the ethanol, the network of the polyester membrane can be reshaped to endow the membrane with excellent performance. The activation mechanism was also explored here. Compared to the membrane without activation (PE0%), the permeability of the optimized membrane (PE-40%) was increased by 8.3 times, and a high rejection was maintained (Cr: 99.2%). Importantly, the PE-40% membrane also presented good acid and alkali resistance, chlorine resistance, and excellent antifouling performance. Our work provides an effective and feasible strategy for the development of high-performance polyester membranes.

关键词： Polyester membrane Ethanol activation Chlorine resistance Antifouling performance dye/salt separation

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

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JOUrNAL OF membrane science 2025年 715卷

作者： Yang, Jia-rui Lin, Yu-Fei Xu, Zhen-Liang Jia, rui Fang, Yin-Xin East China Univ Sci & Technol Chem Engn Res Ctr State Key Lab Chem Engn Membrane Science& Engn R&D LabSch Chem Engn 130 Meilong Rd Shanghai 200237 Peoples R China

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-C3N4 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( degrees)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.

关键词： G-C 3 N 4 quantum dots Thin-film nanocomposite membrane with an interlayer Pervaporation

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Mixed matrix membrane based N2/CF4 separation intensified by "window-cage dual sieving" strategy

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JOUrNAL OF membrane science 2025年 717卷

作者： Li, Ziheng Li, Tiantian Zheng, Wenji Li, Xiangcun Zhu, Jiadong Yu, Miao Jiang, Xiaobin Wu, Xuemei He, Gaohong Zhang, Jianjun Dalian Univ Technol R&D Ctr Membrane Science& Technol Sch Chem Engn Ocean & Life Sci State Key Lab Fine Chem Panjin 124221 Liaoning Peoples R China Dalian Univ Technol Sch Chem Engn R&D Ctr Membrane Sci & Technol State Key Lab Fine Chem Dalian 116023 Liaoning Peoples R China Zhejiang Res Inst Chem Ind State Key Lab Fluorinated Greenhouse Gases Replace Hangzhou 310032 Peoples R China

The perfluorocarbons (PFCs), such as CF4, serving as crucial plasma etching gases, have caused a significant threat to the global greenhouse effect. Therefore, the enrichment and recycling of CF4 is particularly important. However, since the CF4/N2 mixture used for plasma etching with CF4 content lower than 10 vol %, it is urgently necessary to develop N2-preferred transmissible membranes. Herein, cyclic crown ethers with hollow cavity were proposed to be encapsulated within ZIF-7 cages to sieving N2 and CF4 by "window-cage dual sieving", while minimizing the sacrifice of N2 permeance. Specifically, due to its larger size than the window size of ZIF-7, 15- crown-5 (15C5) was physically restricted into ZIF-7 cages, achieving permanent size sieving. As characterized by TEM and BET results, with the 15C5 modification ratio increasing, the ZIF-7 cage size was tuned from 0.46 nm to 0.43 nm, leading to improved N2/CF4 selectivity. Meanwhile, the ether-oxygen bonding of 15C5 enhanced the interfacial compatibility between the 6FdA-dAM polymer matrix and ZIF-7, improving the filler loading as high as 50 wt%. The resultant 15C53@ZIF-7/PI MMMs at filler loading of 40 wt% achieved N2 permeability and N2/ CF4 ideal selectivity of up to 83.2 Barrer and 6.79, which were improved by 253.0 % and 223.3 %, compared to the pure PI membrane. Together with the good long-term stability and mechanical properties, 15C5@ZIF-7/PI MMMs provide a bright prospect in the membrane based recovery of PFCs for industrial applications.

关键词： Mixed matrix membranes Crown ether ZIF-7 CF4

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Quantitative analysis of the influence of PVA interlayer on the permeation resistance of TFC NF membranes

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dESALINATION 2024年 584卷

作者： Tang, Yong-Jian Cheng, Liang Wu, Tong Xu, Zhen-Liang East China Univ Sci & Technol Chem Engn Res Ctr State Key Lab Chem Engn Membrane Science& Engn R&D LabSch Chem Engn 130 Meilong Rd Shanghai 200237 Peoples R China

The interfacial polymerization based on the interlayer is an effective method for enhancing thin-film composite (TFC) nanofiltration (NF) membranes permeability. In this study, a polyvinyl alcohol (PVA) interlayer was constructed on a polyethersulfone substrate through a physical deposition method. Then the TFC NF membranes regulated by PVA interlayer were prepared, and conducted a quantitative analysis of the impact of the PVA interlayer on the permeation resistance of TFC NF membranes. The results indicated that after regulated by the PVA interlayer, the permeation resistance of the polyamide layer decreased slightly, from 0.130 to 0.106 bar h m -1 , while the permeation resistance of the substrate decreased significantly, from 0.277 to 0.087 bar h m -1 . These results indicated that the dramatic decrease in permeation resistance of substrate caused by PVA interlayer was main reason for enhanced permeability, enriching our understanding of the mechanism of the interlayer.

关键词： Nanofiltration Polyvinyl alcohol interlayer Permeation resistance

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A novel loose nanofiltration membrane with high permeance based on aqueous monomer 2,4,6-Trimethyl-m-phenylenediamine for efficient dye/ salt separation

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SEPArATION ANd PUrIFICATION TECHNOLOGY 2025年 363卷

作者： Wang, Jiao Jin, Xiao-Gang Pang, Huizi Zheng Hao, Changqing Li, Li Ma, Xiao-Hua Xu, Zhen-Liang East China Univ Sci & Technol Chem Engn Res Ctr State Key Lab Chem Engn Membrane Science& Engn R&D LabSch Chem Engn Shanghai 200237 Peoples R China Guangdong Ospura Co Ltd Guangzhou Peoples R China

The process of recovering water, salts, and toxic dyes from intricate saline textile wastewater faces difficulties in isolating dissolved ionic substances and reclaiming organic components during the desalination process. In this work, 2,4,6-Trimethyl-m-phenylenediamine (TMPdA) was employed to react with trimesoyl chloride (TMC) through interfacial polymerization reaction to fabricate nanofiltration membrane. Molecular dynamic simulation results show that the TMPdA with unique trimethyl groups has slower diffusion rate, forming a honeycomb-like structure and loose selective layer with more free volume. The obtained TMPdA/TMC membrane exhibits a high permeance of 113.8 L m(-2)h(- 1) bar(-1), high Cr rejection (99.6 %) and low salt rejection (< 5 %), as well as excellent stability and anti-fouling performance. Our work sheds light on the fabrication of loose nanofiltration membrane with specific functional monomer and offers a potential application in the treatment of dye wastewater.

关键词： Interfacial polymerization Loose nanofiltration Molecular dynamic simulation dye desalination 2,4,6-Trimethyl-m-phenylenediamine

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How do salt additives improve the permeability of the thin-film composite membrane?

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dESALINATION 2024年 576卷

作者： Wu, Tong Xu, Zhen-Liang Tang, Yong-Jian East China Univ Sci & Technol Chem Engn Res Ctr State Key Lab Chem Engn Membrane Science& Engn R&D Lab 130 Meilong Rd Shanghai 200237 Peoples R China

Various salt additives were widely used to enhance the permeability of thin-film composite (TFC) membranes. researchers attributed the improvement in TFC membranes to the change in the polyamide (PA) layer. However, the contribution degree of PA layer to TFC membrane permeability enhancement and the effect of salt additives on the substrate are ambiguous. In this study, the effect of salt additives on the permeation resistance of FTC membranes was analyzed. The results showed that the salt additives could reduce both the permeation resistance of the PA layer and substrate, but the effect on the substrate was more pronounced. For example, after adding NaCl, the permeation resistance of the substrate in the heat curing membrane reduced from 0.1764 to 0.0201 bar h m-1, which was much more than that in the PA layer. This study revealed a new mechanism of salt additives improving the permeability of TFC membranes and deepened the understanding of the action mechanism of salt additives.

关键词： TFC membrane Salt additive Permeation resistance

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development of high permeability nanofiltration membranes through porous 2d MOF nanosheets

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CHEMICAL engineering JOUrNAL 2023年第1期471卷

作者： Jin, Xiao-Gang Liang, Xiao-Kang Liu, Jia-Hao Mo, Jia-Wei ren, Tian-Xiang Ma, Xiao-Hua Xu, Zhen-Liang East China Univ Sci & Technol Chem Engn Res Ctr Sch Chem Engn Membrane Science& Engn R&D LabState Key Lab Chem Shanghai 200237 Peoples R China

High-performance nanofiltration membrane is of great importance to alleviate the worldwide freshwater crisis. recent studies have shown that the performance of nanofiltration membranes can be enhanced by optimizing the properties of the substrates. Substrates with large pores are favorable to mass transfer but difficult to prepare highly selective polyamide layers on them by interfacial polymerization reaction. Here we employed porous twodimensional (2d) aluminum-metal organic framework (Al-MOF) nanosheets to tune the commercial Nylon microfiltration substrate, and then prepared polyamide nanofiltration membranes by interfacial polymerization. 2d Al-MOF nanosheets were chosen for the tuning material except for their obvious advantages of easy synthesis and structural stability, the most important thing was their high porosity, which provided additional water transport channels. The morphologies as well as the separation properties were analyzed systematically. The best-performing Nylon-2.5 TFC membrane achieved an ultrahigh permeability (42.4 L m � 2 h 1 bar � 1), 13 times that of a control (PES-0) TFC membrane prepared on commercial PES substrate under the same interfacial polymerization conditions while ensuring the high rejection of Na2SO4 (97.0%). Our work provides insights for optimizing substrate properties to prepare high-performance nanofiltration membranes.

关键词： Porous 2d MOF nanosheets High permeability Nanofiltration Interfacial polymerization Water transport

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A soluble highly-sulfonated polybenzimidazole with high molecular weight as membrane for vanadium flow battery with enhanced performance and long-term stability

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JOUrNAL OF membrane science 2024年 710卷

作者： Liu, Jie Song, Ziwei Gao, Li di, Mingting ruan, Xuehua Zheng, Wenji Wu, Xuemei Zhang, Xiaopeng Yan, Xiaoming He, Gaohong Dalian Univ Technol R&D Ctr Membrane Science& Technol State Key Lab Fine Chem Dalian 116023 Peoples R China Dalian Univ Technol Sch Chem Engn Ocean & Life Panjin 124221 Peoples R China

A series of novel sulfonated polybenzimidazole (SPBI) membranes containing flexible double ether segments, having high ion exchange capacity (IEC), good solubility as well as high molecular weight, are designed for vanadium flow batteries (VFBs). The bis-ether structure of self-synthesized sulfonic acid monomer, 4,4'-((2-sulfo1,4-phenylene)bis(oxy))dibenzoic acid, improves the solubility of produced SPBI and the microphase separation structure of prepared membrane by disrupting the regularity of the backbone through a non-planar structure and attenuating the interchain stacking effect of the polymer backbone. Such a highly reactive bis-ether monomer also leads to high molecular weights (2.37-2.82 dL g-1).-1 ). The copolymerization using another sulfonic acid monomer, Monosodium-5-Sulfoisophthalate monomer, leads to a high IEC of up to 2.08 mmol g- 1 . As a result, the SPBI membrane shows a low area resistance of 0.21 Omega cm2 2 and a low vanadium ion permeability of 3.36 x 10-9-9 cm2 2 s-1.-1 . The VFB cell employing SPBI membrane achieves a very high energy efficiency exceeding 82 % at 200 mA cm-- 2 . In addition, an ultra-long lifetime of over 3400 cycles is accomplished.

关键词： Sulfonated polybenzimidazoles Solubility Vanadium flow batteries membranes

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Novel ultrafiltration membrane fabricated using nanofiber layer as integral filler: Taking PAN and C3N4 as example

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JOUrNAL OF membrane science 2023年第1期684卷

作者： Zhou, Luolu Chen, Meng Yang, Hu Xu, Zhen-liang East China Univ Sci & Technol Chem Engn Res Ctr State Key Lab Chem Engn Membrane Science& Engn R&D Lab 130 Meilong Rd Shanghai 200237 Peoples R China

This study introduces a novel ultrafiltration (UF) membrane, called NFFM, which utilizes a nanofiber (NF) layer as an integral filler during the phase inversion process. The photoactive NFFM was prepared using photoactive PAN-C3N4 (PCN) NF, which is made using C3N4 nanosheets as a visible light responsive photocatalyst with a loading ratio of up to 20%. NFFM membranes made using PAN NF, hydrophilic modified PAN-C3N4 (HPC) NF as filler, and PAN-C3N4 blend membrane were also prepared for comparison. NFFMs showed special morphologies, such as porous surfaces, selective layer located at the internal interface in cross-section, diverse pore sizes and pore size distribution, which are different from that of the traditional blend membrane made with the same ratio of components. Because the dissolving of NF layer into the casting solution changes the composition, polymer distribution, and property of the casting solution, thus change the membrane property. Thickness, composition and surface states of NF Layer can influence its dissolution process. membrane filled with PCN NF (NFFM-PCN) showed a smaller pore size than membrane filled with HPC (NFFM-HPC), due to the low solubility of HPC. Moreover, a longer contacting time can cause the casting solution penetrate into the surface of the HPC layer, leading to a smooth surface. Finally, dye rejection and photoactivity test showed that NFFM-PCN showed better dye rejection property and photoactivity than other membranes, despite the lower photoactivity of C3N4 due to the coverage effect of PAN. Overall, this primitive study provides a new method for preparing a new type of membrane for some potential applications.

关键词： Nanofiber layer filler Ultrafiltration membrane Phase inversion Photocatalyst

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