Journal of Membrane Science最新文献

Active electro-regulation of membrane-foulant interaction for superior separation and antifouling performance in oily wastewater treatment 膜-污染物相互作用的主动电调控在含油废水处理中具有优异的分离和防污性能

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2026-04-01 Epub Date: 2026-01-21 DOI: 10.1016/j.memsci.2026.125172

Hongyuan Zhu , Wangyi Zhou , Yifan Liu , Hang Jiang , Fan Feng , Shasha Yuan , Liguo Shen , Sui Zhang , Die Ling Zhao , Hongjun Lin

Electro responsive membranes offer an effective approach to actively regulate interfacial interactions and mitigate fouling during oil-water separation, yet their practical application is often limited by scalability-conductivity trade-offs and an incomplete understanding of electro-assisted antifouling mechanisms. Herein, conductive membranes were fabricated via a scalable blending strategy by incorporating Ketjen black (KB) nanoparticles into a PVDF matrix. The optimized membranes (0.5 KM) exhibited high electrical conductivity (7.42 S·m⁻¹), underwater superoleophobicity (UOCAs of 155°), and improved hydrophilicity, while maintaining mechanical integrity. Under a negative bias (−15 V), the membranes exhibited synergistic electroosmotic flow (EOF) and electrostatic repulsion for sodium dodecyl sulfate (SDS) stabilized oil/water emulsion, enabling high permeances (4863 L·m⁻²·h⁻¹·bar⁻¹) and oil rejection (>99.60 %) for multiple emulsified oils, alongside superior fouling resistance over five filtration-cleaning cycles. Positive bias, conversely, intensified fouling due to electrostatic attraction. Molecular dynamics (MD) simulations revealed that the electric field enhanced the water self-diffusion coefficient by ∼5.8-fold and facilitated net transmembrane water transfer, while reducing oil residence near pore entrances. This work demonstrates a simple and scalable route to fabricate conductive polymeric membranes, rendering new insights for electrically enhanced separation processes in oily wastewater treatment.

电响应膜提供了一种有效的方法来主动调节界面相互作用，减轻油水分离过程中的污染，但其实际应用往往受到可扩展性和导电性权衡以及对电辅助防污机制的不完整理解的限制。本文通过可扩展的混合策略，将Ketjen black （KB）纳米颗粒掺入PVDF基质中，制备了导电膜。优化后的膜（0.5 KM）具有高导电性（7.42 S·m−1）、水下超疏油性（UOCAs为155°）和亲水性，同时保持机械完整性。在负偏压（- 15 V）下，膜对十二烷基硫酸钠（SDS）稳定的油水乳液表现出协同的电渗透流（EOF）和静电斥力，对多种乳化油具有高渗透率（4863 L·m−2·h−1·bar−1）和高阻油率（99.60%），并且在5次过滤-清洗循环中具有优异的耐污性。相反，正偏压由于静电吸引而加剧了污垢。分子动力学（MD）模拟表明，电场使水的自扩散系数提高了约5.8倍，促进了净跨膜水传递，同时减少了孔隙入口附近的油滞留。这项工作展示了一种简单且可扩展的制造导电聚合物膜的途径，为含油废水处理中的电增强分离工艺提供了新的见解。

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引用次数: 0

Asymmetric support-side deposition strategy for high-permeance tubular CePO4/SiC catalytic membranes enabling synergistic PM and NOx removal 高渗透管状CePO4/SiC催化膜的非对称支撑侧沉积策略，可协同去除PM和NOx

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2026-04-01 Epub Date: 2026-02-12 DOI: 10.1016/j.memsci.2026.125277

Yiqing Zeng , Guangyu Zhou , Jiangxiao Qiao , Yunqi Shi , Jicheng Han , Xiangsen Xu , Junwei Wu , Zhaoxiang Zhong , Weihong Xing

Catalytic membranes are promising multifunctional materials for integrated pollutant control. However, conventional impregnation-based catalyst loading strategies often allow catalytic particles to infiltrate the separation layer, resulting in severe pore blockage and reduced permeance. Herein, we develop a rapid and low-cost asymmetric support-side deposition approach to fabricate tubular CePO₄/SiC–S catalytic membranes, which effectively prevents catalyst penetration into the separation layer, minimizes pore blockage, and thereby enhances the permeance. The results indicate that CePO₄ catalysts are mainly anchored within the pores of the SiC support, rather than in the separation-layer pores, thereby preserving efficient gas transport pathways and avoiding direct contact between particulate matter (PM) and catalytic sites. Compared with conventional vacuum impregnation, the proposed method achieves comparable ammonia selective catalytic reduction (NH₃-SCR) activity while reducing permeance loss from 35.44% to only 20.09%. The membrane demonstrated exceptional stability during a 240 h continuous operation at 350 °C, maintaining a dust rejection rate of >99.99% and NO conversion >90%. Notably, dust cake formation was found to further enhance catalytic efficiency, particularly under low filtration velocities (0.5 m min⁻¹). Computational fluid dynamics (CFD) simulations revealed that moderate cake deposition promotes uniform flow distribution and extends residence time, thereby improving catalyst utilization. This work provides a scalable fabrication strategy for high-permeance catalytic membranes, offering a practical pathway for synergistic control of multiple pollutants at high temperatures.

催化膜是一种很有前途的综合污染物治理的多功能材料。然而，传统的浸渍型催化剂加载策略往往允许催化颗粒渗透到分离层中，导致严重的孔隙堵塞和渗透率降低。本研究开发了一种快速、低成本的非对称支撑侧沉积方法来制备管状CePO4/ SiC-S催化膜，该方法有效地阻止了催化剂渗透到分离层中，最大限度地减少了孔隙堵塞，从而提高了渗透率。结果表明，CePO4催化剂主要锚定在SiC载体的孔隙中，而不是在分离层的孔隙中，从而保持了有效的气体输送途径，避免了颗粒物质（PM）与催化位点之间的直接接触。与传统的真空浸渍法相比，该方法具有相当的氨选择性催化还原（NH3-SCR）活性，同时将渗透损失从35.44%降低到20.09%。该膜在350°C下连续运行240小时时表现出优异的稳定性，保持了99.99%的除尘率和90%的NO转化率。值得注意的是，发现尘饼的形成进一步提高了催化效率，特别是在低过滤速度（0.5 m min - 1）下。计算流体动力学（CFD）模拟表明，适度的饼状沉积促进了流动均匀分布，延长了停留时间，从而提高了催化剂的利用率。这项工作提供了一种可扩展的高渗透催化膜制造策略，为高温下多种污染物的协同控制提供了一条实用途径。

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引用次数: 0

Tailoring multifunctional quaternized polyvinyl alcohol coatings for reverse osmosis membranes with enhanced permeability, fouling resistance and stability 为反渗透膜定制多功能季铵化聚乙烯醇涂料，具有增强的渗透性、抗污性和稳定性

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2026-04-01 Epub Date: 2026-01-22 DOI: 10.1016/j.memsci.2026.125179

Xueke Cai , Xiaoying Long , Huiqi Zhang , Yiwen Xu , Hai Huang , Sanchuan Yu , Congjie Gao

Polyvinyl alcohol (PVA) antifouling coatings are among the most commercially established materials in reverse osmosis (RO) membrane fabrication due to the excellent hydrophilicity. However, excessive hydrogen bonding within the PVA matrix often leads to significant permeability loss. In this study, a straightforward quaternization method to construct quaternized PVA coatings (QPVA) on the RO membranes surface. The introduction of quaternary ammonium groups disrupts the crystalline structure of PVA, thereby reducing transport resistance and mitigating flux decline, in which the water flux was enhanced from 26.4 to 33.8 L·m⁻²·h⁻¹ of the PVA-coated membrane. Moreover, QPVA-coated membranes exhibit near-neutral surfaces and antimicrobial properties, leading to a substantial reduction in both organic and biological fouling with the antibacterial efficiency increasing from 27.5 % for PVA-coated membranes to 97.5 % after quaternization. Furthermore, crosslinking treatment enhances the stability of QPVA coatings by improving coating adhesion and reducing leaching under hydraulic stress. Structural characterizations (FTIR, XPS and SEM) confirm the successful quaternization and the disruption of PVA crystallinity. Long-term filtration and antifouling tests demonstrate the superior performance and durability of QPVA-coated membranes. These findings highlight the potential of the quaternization strategy in developing multifunctional antifouling coatings with improved permeability and stability, which can be easily integrated into existing fabrication processes to extend membrane lifespan in advanced water purification.

聚乙烯醇（PVA）防污涂料由于其优异的亲水性而成为反渗透（RO）膜制造中最具商业价值的材料之一。然而，PVA基体中过量的氢键往往会导致显著的渗透率损失。本研究采用直接季铵化方法在反渗透膜表面构建季铵化PVA涂层（QPVA）。季铵基团的引入破坏了PVA的晶体结构，从而降低了传输阻力，减缓了通量的下降，其中PVA包覆膜的水通量从26.4 L·m−2·h−1提高到33.8 L·m−2·h−1。此外，qpva涂层膜具有近中性表面和抗菌性能，导致有机和生物污染大幅减少，抗菌效率从27.5%增加到季铵化后的97.5%。此外，交联处理通过改善涂层附着力和减少水力应力下的浸出，提高了QPVA涂层的稳定性。结构表征（FTIR， XPS和SEM）证实了成功的季铵化和PVA结晶度的破坏。长期过滤和防污试验表明，qpva涂层膜具有优异的性能和耐久性。这些发现突出了季铵化策略在开发具有改善渗透性和稳定性的多功能防污涂料方面的潜力，这些防污涂料可以很容易地集成到现有的制造工艺中，以延长高级水净化中膜的寿命。

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引用次数: 0

Overcoming cross–scale manufacturing barriers toward scalable nanoporous atomically thin membranes for gas–liquid separation 克服用于气液分离的可伸缩纳米多孔原子薄膜的跨尺度制造障碍

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2026-04-01 Epub Date: 2026-01-18 DOI: 10.1016/j.memsci.2026.125170

Dawei Lu , Shanshan Wang , Ying Zhang , Ye Liu , Jinze Zheng , Siyu Hu , Junhe Tong , Dongxu Zhang , Dandan Hou , Luda Wang

Nanoporous atomically thin membranes (NATMs) have considerable promise for molecular separations. However, their application has been hindered by several cross–scale manufacturing challenges, including non–selective leakage caused by large defects, mechanical damage during operation, and limited long–term operational stability. Graphene, as a representative NATM, offers tunable nanopores and outstanding molecular sieving, but these advantages remain unrealized without overcoming cross-scale barriers. Here, we propose a flow–resistance–matching strategy that integrates multiple structure levels to balance permeance, selectivity, and stability. It combines a porous PVDF support layer fabricated via phase separation for mechanical support, double–layer nanoporous graphene for molecular sieving, and an ultrathin PDMS (∼1.94 μm) coating to prevent non–selective leakage and protect graphene. This approach also enables scalable fabrication with areas up to 300 cm². The as-prepared membranes showed outstanding gas–liquid separation performance in precision total organic carbon (TOC) analyzers, with a coefficient of determination R² = 0.999. They also exhibited stable performance with an RSD of 0.78 % over 7 days and 2.31 % over 576 h (24 days), respectively whereas samples lacking cross-scale engineering typically failed within a few days. These results establish a scalable way for application of NATMs in industrial gas–liquid separation.

纳米多孔原子薄膜（NATMs）在分子分离方面具有广阔的应用前景。然而，它们的应用受到几个跨尺度制造挑战的阻碍，包括大缺陷引起的非选择性泄漏、操作过程中的机械损伤以及有限的长期运行稳定性。石墨烯作为新纳米材料的代表，具有可调的纳米孔和出色的分子筛分能力，但如果不克服跨尺度障碍，这些优势仍无法实现。在这里，我们提出了一种流动阻力匹配策略，该策略集成了多个结构水平，以平衡渗透，选择性和稳定性。它结合了通过相分离制备的多孔PVDF支撑层作为机械支撑，双层纳米多孔石墨烯用于分子筛分，超薄PDMS （~ 1.94 μm）涂层用于防止非选择性泄漏并保护石墨烯。这种方法还可以实现面积达300平方厘米的可扩展制造。制备的膜在精密总有机碳（TOC）分析仪中具有良好的气液分离性能，测定系数R2 = 0.999。它们也表现出稳定的性能，在7天内的RSD为0.78%，在576小时（24天）内的RSD为2.31%，而缺乏跨尺度工程的样品通常在几天内失效。这些结果为natm在工业气液分离中的应用开辟了一条可扩展的途径。

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引用次数: 0

Lamellar ZIF-8 nanosheets empowered thin-film nanocomposite membrane with synergistic sieving and rapid water transport for enhanced desalination 层状ZIF-8纳米片增强了薄膜纳米复合膜的协同筛分和快速水输送能力，增强了海水淡化

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2026-04-01 Epub Date: 2026-02-10 DOI: 10.1016/j.memsci.2026.125261

Hui You , Xiang Xu , Wencan Luo , Lancai Long , Jun Du , Shunmin Yi , Wanyu Liu

The development of reverse osmosis membranes that simultaneously achieve high water permeability and excellent salt rejection is an urgent yet challenging goal for sustainable desalination. Two-dimensional (2D) nanofillers offer a promising pathway to break the inherent trade-off by creating fast water-transport channels. Herein, we engineered a high-performance thin-film nanocomposite (TFN) membrane by incorporating lamellar zeolitic imidazolate framework-8 nanosheets (ZIF-8 NSs) into the polyamide selective layer. The ZIF-8 NSs, synthesized via a facile surfactant-directed approach, possess an ultrathin thickness of ∼5.5 nm and a large lateral size of ∼0.75 μm. When embedded at an optimal loading, the TFN membrane demonstrates a remarkable water permeability of 9.83 L m⁻² h⁻¹ MPa⁻¹, which is ∼37% higher than the pristine thin-film composite (TFC) membrane, while maintaining a high Na₂SO₄ rejection of 97.9%. This superior performance, significantly surpassing that of membranes filled with conventional ZIF-8 nanoparticles, is attributed to the synergistic effect of the molecular-sieving function of intrinsic ZIF-8 pores and the low-resistance nanochannels formed by the interlayer galleries between the well-dispersed nanosheets, which concurrently facilitate a more cross-linked polyamide network. This work provides a viable and scalable strategy for using 2D MOF nanosheets to design advanced separation membranes.

开发同时具有高透水性和优异的脱盐性能的反渗透膜是可持续海水淡化的一个紧迫而具有挑战性的目标。二维（2D）纳米填料提供了一种很有希望的途径，通过创建快速的水输送通道来打破固有的权衡。在此，我们设计了一种高性能的薄膜纳米复合材料（TFN）膜，将层状沸石咪唑酸框架-8纳米片（ZIF-8 NSs）纳入聚酰胺选择层。通过表面活性剂定向方法合成的ZIF-8 NSs具有~ 5.5 nm的超薄厚度和~ 0.75 μm的大横向尺寸。当以最佳负载嵌入时，TFN膜的透水性为9.83 L m−2 h−1 MPa−1，比原始薄膜复合材料（TFC）膜高约37%，同时保持97.9%的Na2SO4截留率。这种优异的性能明显超过了传统的ZIF-8纳米颗粒填充的膜，这是由于固有的ZIF-8孔的分子筛分功能和由分散良好的纳米片之间的层间通道形成的低电阻纳米通道的协同作用，同时促进了更多交联的聚酰胺网络。这项工作为使用二维MOF纳米片设计先进的分离膜提供了一个可行的和可扩展的策略。

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引用次数: 0

Preparation of hollow fibre braided polyvinylidene fluoride membranes by dip coating for membrane aerated bioreactor 浸涂法制备膜曝气生物反应器用中空纤维编织聚偏氟乙烯膜

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2026-04-01 Epub Date: 2026-02-02 DOI: 10.1016/j.memsci.2026.125227

Francesca Passaro , Marcello Pagliero , Ilaria Rizzardi , Antonio Comite

In this work, hollow fibre polyvinylidene fluoride (PVDF) supported membranes were prepared by dip coating a fibre glass sleeve in a PVDF solution, followed by precipitation via nonsolvent induced phase separation (NIPS) in 96% ethanol. The combination of these was optimized for obtaining membranes with a low-resistance thin polymeric layer and enhanced mechanical stability. The influence of both the withdrawal rate and the viscosity of the dope solution were investigated. The thickness of the PVDF coating layer was evaluated in the frame of the Landau-Levich model, which predicts that the film thickness results from the balance between viscous drag and surface tension forces. Among all the prepared membranes, the membranes prepared from a dope solution at 60 °C and with a withdrawal rate of 0.5 cm/s were selected to be used as support to grow biofilm for an application as Membrane Aerated Biological Reactor (MABR). The performance of the MABR, with the biofilm grown on the outer surface of the PVDF membranes and airflow supplied through the lumen of the fibre glass sleeve, was evaluated in terms of removal of Chemical Oxygen Demand (COD), ammoniacal nitrogen and total nitrogen. The MABR set up enabled the simultaneous abatement of the aforementioned parameters, with 78% of removal for COD, 21% for ammonia and 5% for total nitrogen, an interesting starting point for lab-made membranes exploited for this application.

在PVDF溶液中浸渍涂覆玻璃纤维套筒，然后在96%乙醇中通过非溶剂诱导相分离（NIPS）沉淀，制备了中空聚偏氟乙烯纤维（PVDF）支撑膜。优化了这两种方法的组合，以获得具有低电阻薄聚合物层的膜，并增强了机械稳定性。考察了萃取速率和溶液粘度对萃取效果的影响。在Landau-Levich模型框架下对PVDF涂层的厚度进行了评估，该模型预测薄膜厚度是粘性阻力和表面张力之间平衡的结果。在所有制备的膜中，选择在60°C下，提取速率为0.5 cm/s的溶液中制备的膜作为生物膜生长的载体，作为膜曝气生物反应器（MABR）的应用。生物膜生长在PVDF膜的外表面，气流通过玻璃纤维套管的管腔输送，对MABR的化学需氧量（COD）、氨态氮和总氮的去除率进行了评价。MABR装置可以同时去除上述参数，COD去除率为78%，氨去除率为21%，总氮去除率为5%，这对于用于该应用的实验室自制膜来说是一个有趣的起点。

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引用次数: 0

Fabrication of defect-free benzimidazole polyimide hollow fiber membranes for high performance gas separation 高性能气体分离用无缺陷苯并咪唑聚酰亚胺中空纤维膜的制备

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2026-04-01 Epub Date: 2026-02-05 DOI: 10.1016/j.memsci.2026.125246

Yuting Wang , Fan Luo , Xiaoni Du , Zhenggong Wang , Jian Jin

The rational design of polymer chain structures is crucial for constructing high-performance hollow fiber membranes (HFMs). In this study, a benzimidazole-based polyimide material was designed and synthesized, and applied to the large-scale fabrication of hollow fiber membranes. The benzimidazole groups can form π–π stacking and hydrogen bonding interactions between molecular chains. This strong interchain interaction effectively locks the polymer chains, significantly enhancing the gas selectivity of the HFMs while simultaneously improving their resistance to plasticization and aging. The adjustment of polymer dope composition coupled with optimization of spinning parameters enabled the fabrication of defect-free HFMs with high gas separation performance. The H₂ permeance of resulting HFMs is 181.5 GPU with a H₂/CH₄ selectivity of 171.5. The membranes also exhibit excellent mechanical properties, with a tensile stress of 66.7 MPa and a tensile strain of 16.5%. The H₂/CH₄ separation selectivity is maintained at 151 following a six-month operational period, demonstrating excellent long-term stability. This study presents benzimidazole-based polyimide HFMs that are notable for their superior gas separation performance, mechanical robustness, and stability, indicating significant application potential.

聚合物链结构的合理设计是构建高性能中空纤维膜的关键。本研究设计并合成了一种苯并咪唑基聚酰亚胺材料，并将其应用于中空纤维膜的大规模制备。苯并咪唑基团可以在分子链之间形成π -π堆叠和氢键相互作用。这种强大的链间相互作用有效地锁住了聚合物链，显著提高了HFMs的气体选择性，同时提高了它们的抗塑化和抗老化能力。通过对聚合物掺杂成分的调整和纺丝工艺参数的优化，制备出了具有高气体分离性能、无缺陷的HFMs。所得HFMs的H2透过率为181.5 GPU， H2/CH4选择性为171.5。拉伸应力为66.7 MPa，拉伸应变为16.5%，具有优异的力学性能。在6个月的运行周期后，H2/CH4的分离选择性保持在151，表现出良好的长期稳定性。本研究提出的以苯并咪唑为基础的聚酰亚胺HFMs具有优异的气体分离性能、机械稳健性和稳定性，具有重要的应用潜力。

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引用次数: 0

An integrated module with synergistic heating and turbulence promotion for enhanced vacuum membrane distillation 一个集成的模块与增强型真空膜蒸馏的协同加热和湍流促进

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2026-04-01 Epub Date: 2026-01-23 DOI: 10.1016/j.memsci.2026.125204

Fangli Zhang , Chenyang Gu , Yangming Cheng , Rizhi Chen , Zhaohui Wang , Zhaoliang Cui

Conventional membrane distillation (MD) experiences 50–80 % flux reduction due to temperature polarization (TP), while metallic heat exchangers are susceptible to corrosion when treating high-salinity feeds. To address these limitations, an integrated heat-exchange vacuum membrane distillation (IHEVMD) module was developed by incorporating polymer-based heat-exchange tubes within the MD process, enabling simultaneous in-situ feed heating and distillation. Heat transfer performance and MD flux were thoroughly examined in relation to heat-exchange temperature, heat-exchange area, feed, and heat-exchange fluid flow rates. Results demonstrate that the total heat transfer rate (Q) and overall heat transfer coefficient (K) are governed by the heat-exchange temperature and feed flow rate. The flux in MD was favorably influenced by the temperature and membrane area. The IHEVMD module D achieved an 83 % flux enhancement at 56 °C compared to conventional MD, along with a 90 % improvement in gained output ratio (GOR) and a 50 % reduction in specific thermal energy consumption (STEC). Notably, the module exhibited superior performance with high-salinity feeds (e.g., 3.5 and 5 wt% NaCl), leveraging brine's lower specific heat capacity for higher feed temperatures and fluxes. Long-term stability tests confirmed effective TP mitigation and anti-fouling properties. This work provides an energy-efficient, corrosion-resistant strategy for high-salinity water treatment utilizing low-grade heat sources.

由于温度极化（TP），传统的膜蒸馏（MD）会使通量降低50 - 80%，而金属热交换器在处理高盐度进料时容易受到腐蚀。为了解决这些限制，开发了集成热交换真空膜蒸馏（IHEVMD）模块，该模块在MD过程中集成了基于聚合物的热交换管，可以同时进行原位进料加热和蒸馏。传热性能和MD通量与换热温度、换热面积、进料和换热流体流速的关系进行了全面的研究。结果表明，总换热率Q和总换热系数K受换热温度和进料流量的影响。MD的通量受温度和膜面积的影响较大。与传统MD相比，IHEVMD模块D在56°C时实现了83%的通量增强，同时获得的输出比（GOR）提高了90%，比热能耗（STEC）降低了50%。值得注意的是，该模块在高盐度进料（例如，3.5 wt%和5 wt% NaCl）中表现出优异的性能，利用盐水较低的比热容来提高进料温度和通量。长期稳定性测试证实了有效的TP缓解和防污性能。这项工作为利用低品位热源进行高盐度水处理提供了一种节能、耐腐蚀的策略。

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引用次数: 0

Silicon-tailored carbon molecular sieve membranes enable precise and stable hydrogen separation 硅定制碳分子筛膜实现精确和稳定的氢分离

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2026-04-01 Epub Date: 2026-01-28 DOI: 10.1016/j.memsci.2026.125220

Chuning Fang , Xingyu Chen , Zhinan Fu , Zuoxiang Zeng , Linfeng Lei , Zhi Xu

The requirement for efficient CO₂ capture during hydrogen production from fossil fuels promotes the development of advanced, energy-efficient solutions, while the application of temperature/pressure-resistant membranes is a promising candidate. Polymer-derived carbon molecular sieve (CMS) membranes with precise molecular discrimination capability hold attractive promise in H₂/CO₂ separation. Nonetheless, microstructure tuning for the precise discrimination of H₂ and CO₂ has so far remained challenging, and physical aging is also an inevitable problem. Herein, we proposed a precursor-crosslinked strategy via chemical functionalization of cellulose precursor to enhance molecular sieving ability and simultaneously overcome physical aging of the derived CMS membranes. The membrane presents a remarkable H₂/CO₂ selectivity of 91.0 and shows only 14 % H₂ permeance loss in 120 days. Besides, it maintains excellent separation performance over 300 h under high pressure (up to 20 bar) and high temperature of 140 °C with a feeding of 50 mol% H₂/50 mol% CO₂. This study provides an effective way to construct the sub-nano-sized microporous structure of CMS membranes and demonstrates its potential for blue hydrogen purification under harsh conditions.

化石燃料制氢过程中对高效二氧化碳捕获的需求促进了先进、节能解决方案的发展，而耐温/耐压膜的应用是一个很有前途的候选者。聚合物衍生碳分子筛（CMS）膜具有精确的分子识别能力，在H2/CO2分离中具有广阔的应用前景。然而，精确区分H2和CO2的微观结构调整至今仍然具有挑战性，物理老化也是不可避免的问题。在此，我们提出了一种前体交联策略，通过纤维素前体的化学功能化来提高分子筛选能力，同时克服衍生的CMS膜的物理老化。该膜的H2/CO2选择性为91.0，在120天内仅损失14%的H2透性。此外，在高压（高达20 bar）和高温（140°C）下，在进料为50 mol% H2/50 mol% CO2的条件下，它在300 h内保持了优异的分离性能。本研究为构建亚纳米级CMS膜微孔结构提供了有效途径，并展示了其在恶劣条件下净化蓝氢的潜力。

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引用次数: 0

Covalently bonded nanofiltration membranes with enhanced interlayer stability and back-flush resistance 具有增强层间稳定性和抗反冲性的共价键纳滤膜

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2026-04-01 Epub Date: 2026-01-27 DOI: 10.1016/j.memsci.2026.125211

Xiyue Cai , Yonggang Li , Zejin Yu , Yingjie Fu , Jing Guo , Lei Dai , Yaohan Chen , Shenghai Li , Suobo Zhang

Nanofiltration (NF) membrane represents an environmental-friendly and easy-to-operate water purification technology. However, NF membranes inevitably suffer from fouling, resulting in significant deterioration of separation performance and shortened operational lifespan. The polyamide (PA) separating layer of commercial thin film composite nanofiltration (TFC-NF) membranes is typically fabricated via interfacial polymerization (IP) on supporting membrane. The interfacial adhesion between the PA layer and the supporting membrane is primarily governed by weak van der Waals interactions, rendering the PA layer susceptible to be damaged during operation and recycling. In this work, we synthesized and employed a carboxyl-functionalized polymer (PEAK-COOH) as the supporting membrane material. Through a one-step phase inversion-surface amination process conducted in an aqueous piperazine (PIP) solution, coupled with in-situ IP process, we successfully fabricated a TFC NF membrane (PEAK–COOH–NF) in which the separating layer and the supporting membrane were robustly integrated through extensive covalent bonds. The separation layer fabricated with such strong interfacial bonding remained intact even under a maximum normal load of 0.15 mN in nano-scratch test, whereas the commercial NF270 membrane and TFC-NF membrane prepared on polyethersulfone (PES) supporting membrane exhibited structural failure at only 0.065 mN and 0.073 mN, respectively. This excellent interlayer adhesion enables the membrane to withstand back-flushing cleaning treatment at pressures up to 0.9 MPa without exhibiting significant performance deterioration, with its rejection remaining at 98.60 % after back-flushing. Finite element simulations further elucidate how this robust covalent interfacial bonding enhances the overall structural stability of the membrane. Furthermore, PEAK–COOH–NF exhibited a higher Na₂SO₄ rejection than NF270 due to the high cross-linking degree with 94.12 %. This study not only introduces a continuous fabrication strategy that enables TFC-NF membranes with exceptionally strong interfacial bonding, but also provides both methodological insights and a robust material platform to support effective back-flush operations in practical nanofiltration applications.

纳滤（NF）膜是一种环境友好、易于操作的水净化技术。然而，纳滤膜不可避免地会受到污染，导致分离性能显著下降，使用寿命缩短。商用薄膜复合纳滤（TFC-NF）膜的聚酰胺（PA）分离层通常是在支撑膜上通过界面聚合（IP）制备的。聚苯乙烯层与支撑膜之间的界面粘附主要受弱范德华相互作用的支配，使得聚苯乙烯层在操作和回收过程中容易被破坏。在这项工作中，我们合成并使用了一种羧基功能化聚合物（PEAK-COOH）作为支撑膜材料。通过在哌嗪（PIP）水溶液中进行的一步相反表面胺化工艺，结合原位IP工艺，成功制备了一种分离层和支撑膜通过广泛的共价键牢固结合的TFC NF膜（峰cooh - NF）。在纳米划伤测试中，即使在0.15 mN的最大正常载荷下，具有如此强界面键合的分离层仍然保持完整，而在聚醚砜（PES）支撑膜上制备的商用NF270膜和TFC-NF膜分别在0.065 mN和0.073 mN下出现结构破坏。这种优异的层间附着力使膜能够承受高达0.9 MPa压力下的反冲洗清洗处理，而不会表现出明显的性能下降，反冲洗后的去除率仍为98.60%。有限元模拟进一步阐明了这种强大的共价界面键如何增强膜的整体结构稳定性。此外，由于交联度高，PEAK-COOH-NF的Na2SO4截留率高于NF270（94.12%）。这项研究不仅介绍了一种连续制造策略，使TFC-NF膜具有异常强大的界面键合，而且还提供了方法论见解和强大的材料平台，以支持实际纳滤应用中有效的反冲洗操作。

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