The asymmetry of membrane properties manifests itself in the dependence of the membrane response to an external force on its orientation relative to the direction of that force. Membranes exhibiting asymmetric transport of ions and water, often referred to as Janus membranes, have attracted increasing attention due to their unique functional behavior and prospects for promising applications. In this work, the asymmetry of bilayer ion-exchange membranes with respect to electrolyte diffusion is analyzed. Two complementary approaches are applied. The phenomenological framework of nonequilibrium thermodynamics is used to determine how the differential diffusion permeability of each layer should vary with concentration to produce a significant dependence of the overall diffusion flux on the membrane orientation relative to the upstream and downstream solutions. The second approach, based on the microheterogeneous model of the membrane, allows identification of the structural and kinetic parameters of each layer that lead to the desired form of function. A homogeneous CJMC-3 cation-exchange membrane was studied both experimentally and theoretically using these approaches. It is shown that the observed asymmetry in diffusion permeability originates from the reinforcing fabric located near one of the membrane surfaces.
{"title":"Asymmetry of diffusion permeability of ion-exchange membranes: Modeling and experiment","authors":"A.E. Kozmai , M.A. Ponomar , S.A. Mareev , N.D. Pismenskaya , I.A. Moroz , K.G. Sabbatovskiy , V.V. Nikonenko","doi":"10.1016/j.memsci.2026.125145","DOIUrl":"10.1016/j.memsci.2026.125145","url":null,"abstract":"<div><div>The asymmetry of membrane properties manifests itself in the dependence of the membrane response to an external force on its orientation relative to the direction of that force. Membranes exhibiting asymmetric transport of ions and water, often referred to as <em>Janus membranes</em>, have attracted increasing attention due to their unique functional behavior and prospects for promising applications. In this work, the asymmetry of bilayer ion-exchange membranes with respect to electrolyte diffusion is analyzed. Two complementary approaches are applied. The phenomenological framework of nonequilibrium thermodynamics is used to determine how the differential diffusion permeability <span><math><mrow><msup><mi>P</mi><mo>*</mo></msup></mrow></math></span> of each layer should vary with concentration to produce a significant dependence of the overall diffusion flux on the membrane orientation relative to the upstream and downstream solutions. The second approach, based on the microheterogeneous model of the membrane, allows identification of the structural and kinetic parameters of each layer that lead to the desired form of <span><math><mrow><msup><mi>P</mi><mo>*</mo></msup><mrow><mo>(</mo><mi>c</mi><mo>)</mo></mrow></mrow></math></span> function. A homogeneous CJMC-3 cation-exchange membrane was studied both experimentally and theoretically using these approaches. It is shown that the observed asymmetry in diffusion permeability originates from the reinforcing fabric located near one of the membrane surfaces.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125145"},"PeriodicalIF":9.0,"publicationDate":"2026-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941170","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-07DOI: 10.1016/j.memsci.2026.125128
Nasser AL-Hamdani , Giuseppe Costanzo , Giorgio Purpura , J. Luque Di Salvo , Giorgio De Luca
Many works focused on predicting water permeability in polyamides utilized in osmotic membranes, but few of them provide Multi-Scale (MS) calculations free from tunable parameters. In this paper, the phenomenological water permeability was calculated by a novel MS approach. Two biphasic models, water/FT-30 polyamide and dilute salt solution/polyamide, were simulated. Molecular Dynamics (MD) –based simulations were first performed to obtain the equilibrium water volume fraction and the water mass concentrations in the polymeric phase. Then the analytical solution of Fick's second law, provided by Penetration Theory, was used to obtain the water diffusion coefficient, exploiting the MD water mass concentrations. The computed water uptake was found to be in good agreement with the values available in the literature using both biphasic models. Moreover, the MS method yields water diffusion coefficients comparable with the smallest available theoretical and experimental values. Water permeability as well, is in agreement with the experimental values referring to ultrathin polyamide membranes, while the agreement is lost for membranes with thicker active layers. Therefore, the proposed MS methodology is reliable for predicting water permeability in this kind of promising membranes and for designing new ultrathin polymer membranes since it is based on atomistic-scale simulations. The strength of the method lies in the suitable assembly of advanced nanoscale simulations with the macroscopic Fick's transport equation.
{"title":"Water permeability of ultrathin polyamide membranes: a computation study from molecular to macro scale","authors":"Nasser AL-Hamdani , Giuseppe Costanzo , Giorgio Purpura , J. Luque Di Salvo , Giorgio De Luca","doi":"10.1016/j.memsci.2026.125128","DOIUrl":"10.1016/j.memsci.2026.125128","url":null,"abstract":"<div><div>Many works focused on predicting water permeability in polyamides utilized in osmotic membranes, but few of them provide Multi-Scale (MS) calculations free from tunable parameters. In this paper, the phenomenological water permeability was calculated by a novel MS approach. Two biphasic models, water/FT-30 polyamide and dilute salt solution/polyamide, were simulated. Molecular Dynamics (MD) –based simulations were first performed to obtain the equilibrium water volume fraction and the water mass concentrations in the polymeric phase. Then the analytical solution of Fick's second law, provided by Penetration Theory, was used to obtain the water diffusion coefficient, exploiting the MD water mass concentrations. The computed water uptake was found to be in good agreement with the values available in the literature using both biphasic models. Moreover, the MS method yields water diffusion coefficients comparable with the smallest available theoretical and experimental values. Water permeability as well, is in agreement with the experimental values referring to ultrathin polyamide membranes, while the agreement is lost for membranes with thicker active layers. Therefore, the proposed MS methodology is reliable for predicting water permeability in this kind of promising membranes and for designing new ultrathin polymer membranes since it is based on atomistic-scale simulations. The strength of the method lies in the suitable assembly of advanced nanoscale simulations with the macroscopic Fick's transport equation.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125128"},"PeriodicalIF":9.0,"publicationDate":"2026-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941166","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-07DOI: 10.1016/j.memsci.2026.125142
Ning Yan, Rui-Xin Liu, Jia-Min Wu, Zhao-Qing Lu
High-performance fiber-based nanofluidic membranes exhibit significant potential in osmotic energy harvesting, yet conventional aramid nanofibers (ANFs) membrane is limited by insufficient ion selectivity for efficient power generation. This study proposes a simple yet ingenious proton donor-induced phase deposition strategy to construct ANFs membrane with ultrafast ion transport capabilities. By introducing negatively charged cellulose acetate (CA) as proton donor in aramid deprotonation system (KOH/DMSO), a CA-cellulose-water ternary proton-donor system spontaneously forms in this strong alkaline environment. This system markedly enhances ANFs dispersion through a mild and stepwise proton release mechanism. Even more fortunately, during the reaction, the deacetylation of CA generates insoluble cellulose, which is deposited in situ on the fibers, narrowing the fiber spacing. This endows the membrane with sub-nanometer ion transport channels, featuring an interlayer spacing of 4.59 Å and channel diameters of 2 nm. The fabricated membrane exhibits exceptional ion selectivity (cation transport number of 0.9), achieves a power density of 22.13 W/m2 and 28.14 W/m2 using simulated- and natural seawater-river water, outperforming most current membranes. Simultaneously, it demonstrates high mechanical strength (122 MPa tensile strength at 1 μm thickness). This research provides novel insights into the application of ANFs membranes for efficient osmotic energy conversion.
{"title":"Proton donor-induced phase deposition in aramid nanofiber membranes for efficient osmotic energy harvesting","authors":"Ning Yan, Rui-Xin Liu, Jia-Min Wu, Zhao-Qing Lu","doi":"10.1016/j.memsci.2026.125142","DOIUrl":"10.1016/j.memsci.2026.125142","url":null,"abstract":"<div><div>High-performance fiber-based nanofluidic membranes exhibit significant potential in osmotic energy harvesting, yet conventional aramid nanofibers (ANFs) membrane is limited by insufficient ion selectivity for efficient power generation. This study proposes a simple yet ingenious proton donor-induced phase deposition strategy to construct ANFs membrane with ultrafast ion transport capabilities. By introducing negatively charged cellulose acetate (CA) as proton donor in aramid deprotonation system (KOH/DMSO), a CA-cellulose-water ternary proton-donor system spontaneously forms in this strong alkaline environment. This system markedly enhances ANFs dispersion through a mild and stepwise proton release mechanism. Even more fortunately, during the reaction, the deacetylation of CA generates insoluble cellulose, which is deposited in situ on the fibers, narrowing the fiber spacing. This endows the membrane with sub-nanometer ion transport channels, featuring an interlayer spacing of 4.59 Å and channel diameters of 2 nm. The fabricated membrane exhibits exceptional ion selectivity (cation transport number of 0.9), achieves a power density of 22.13 W/m<sup>2</sup> and 28.14 W/m<sup>2</sup> using simulated- and natural seawater-river water, outperforming most current membranes. Simultaneously, it demonstrates high mechanical strength (122 MPa tensile strength at 1 μm thickness). This research provides novel insights into the application of ANFs membranes for efficient osmotic energy conversion.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125142"},"PeriodicalIF":9.0,"publicationDate":"2026-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941169","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-07DOI: 10.1016/j.memsci.2026.125143
Wooyoung Choi , Woo Jin Jang , Jiwon Kim , Hanim Kim , Ryan P. Lively , Dae Woo Kim
The energy-intensive recovery of butanol from dilute fermentation broths remains a critical barrier to economical biobutanol production. This work introduces a hybrid membrane developed through the molecular integration of lignin into a graphene oxide (GO) laminate, which fundamentally alters transport properties to enable butanol-selective permeation via a sorpvection mechanism. Under a hydraulic pressure of 50 bar, the GOL membrane achieved a total flux of 23.3 L m−2 h−1 with a butanol separation factor of 2.1 in dilute solutions. In contrast to pristine GO membranes, which exhibited significantly lower flux (3.0 L m−2 h−1) and butanol rejection. Furthermore, the GOL membrane demonstrated robust structural integrity, maintaining stable performance during a 10-day continuous operation. Unlike conventional pervaporation limited by phase-change thermodynamics, this pressure-driven system enables high-flux liquid-phase separation. These results indicate that lignin intercalation successfully reverses the transport selectivity of GO. Consequently, this high-flux, phase-change-free separation approach presents a promising, energy-efficient pathway for overcoming the economic bottlenecks of biobutanol recovery.
从稀发酵液中回收丁醇的能源密集型技术仍然是经济生产生物丁醇的关键障碍。这项工作介绍了一种通过木质素分子整合到氧化石墨烯（GO）层压板上开发的杂交膜，它从根本上改变了运输特性，通过吸附机制实现丁醇选择性渗透。在50 bar的水力压力下，GOL膜在稀溶液中的总通量为23.3 L m−2 h−1，丁醇分离系数为2.1。与原始氧化石墨烯膜相比，原始氧化石墨烯膜的通量（3.0 L m−2 h−1）和丁醇排斥率明显较低。此外，GOL膜具有坚固的结构完整性，可以在连续10天的作业中保持稳定的性能。与受相变热力学限制的传统渗透蒸发不同，这种压力驱动系统能够实现高通量的液相分离。这些结果表明木质素嵌入成功地逆转了氧化石墨烯的转运选择性。因此，这种高通量、无相变的分离方法为克服生物丁醇回收的经济瓶颈提供了一条有希望的、节能的途径。
{"title":"Lignin/graphene oxide membrane for sorpvection-driven butanol recovery","authors":"Wooyoung Choi , Woo Jin Jang , Jiwon Kim , Hanim Kim , Ryan P. Lively , Dae Woo Kim","doi":"10.1016/j.memsci.2026.125143","DOIUrl":"10.1016/j.memsci.2026.125143","url":null,"abstract":"<div><div>The energy-intensive recovery of butanol from dilute fermentation broths remains a critical barrier to economical biobutanol production. This work introduces a hybrid membrane developed through the molecular integration of lignin into a graphene oxide (GO) laminate, which fundamentally alters transport properties to enable butanol-selective permeation via a sorpvection mechanism. Under a hydraulic pressure of 50 bar, the GOL membrane achieved a total flux of 23.3 L m<sup>−2</sup> h<sup>−1</sup> with a butanol separation factor of 2.1 in dilute solutions. In contrast to pristine GO membranes, which exhibited significantly lower flux (3.0 L m<sup>−2</sup> h<sup>−1</sup>) and butanol rejection. Furthermore, the GOL membrane demonstrated robust structural integrity, maintaining stable performance during a 10-day continuous operation<strong>.</strong> Unlike conventional pervaporation limited by phase-change thermodynamics, this pressure-driven system enables high-flux liquid-phase separation. These results indicate that lignin intercalation successfully reverses the transport selectivity of GO. Consequently, this high-flux, phase-change-free separation approach presents a promising, energy-efficient pathway for overcoming the economic bottlenecks of biobutanol recovery.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125143"},"PeriodicalIF":9.0,"publicationDate":"2026-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974092","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-06DOI: 10.1016/j.memsci.2025.125120
Ruixuan Lv , Zhenbei Peng , Yang Wu , Mahmoud M. Gomaa , Jingshuai Yang
Thiazole-containing polymers are widely explored in semiconductors and photocatalysis, yet their potential as high temperature proton exchange membranes (HT-PEMs) for fuel cells remains unexplored. Here we present a new, simple and efficient superacid-catalyzed polyhydroxyalkylation strategy to synthesize six ether-free polyarylenes bearing pendant thiazole, benzothiazole, or thiazoline groups. To our knowledge, it represents the first demonstration of pendant thiazole-based polymers as HT-PEMs. Systematic structural variations, combined with theoretical calculations, reveal that freely rotating thiazole moieties engage in strong acid-base interactions and hydrogen bonding with phosphoric acid (PA), enabling high PA uptake and enhancing proton transport. Polymers derived from aldehyde monomers with methine (–CH–) linkages exhibit superior chemical and thermal stability relative to ketone-derived analogs with α-methyl (–C(CH3)–) bridges. Among them, the poly (terphenyl thiazole-4-carboxaldehyde) (P (TP-4TA)) membrane achieves the best balance of physicochemical properties, retaining 87.2 % of its mass after 450 h in Fenton's reagent. The PA doped P (TP-4TA) membrane with an acid doping content of 158 % sustains 17.2 MPa tensile strength, and delivers 52.2 mS cm−1 proton conductivity at 180 °C. A single fuel cell employing above membrane attains a peak power density of 684 mW cm−2 and an open-circuit voltage of 1.0 V at 180 °C under H2/O2 without humidification or backpressure. This work establishes pendant thiazole-containing polyarylenes as a new platform for HT-PEMs, offering a versatile molecular design strategy for next-generation fuel cells and other advanced energy technologies.
含噻唑的聚合物在半导体和光催化领域得到了广泛的研究，但它们作为燃料电池高温质子交换膜（HT-PEMs）的潜力仍未得到开发。本文提出了一种新的、简单高效的超强酸催化聚羟基烷基化策略，以合成六种无醚的含悬垂噻唑、苯并噻唑或噻唑啉基团的聚丙烯。据我们所知，它代表了悬垂噻唑基聚合物作为HT-PEMs的首次演示。系统的结构变化，结合理论计算，揭示了自由旋转的噻唑部分参与强酸碱相互作用和与磷酸（PA）的氢键，从而实现高PA摄取和增强质子传输。与具有α-甲基（- c (CH3) -）键的酮类类似物相比，由乙醛单体衍生的具有甲基（- c (CH3) -）键的聚合物具有更好的化学和热稳定性。其中聚（terphenyl噻唑-4-carboxaldehyde） （P (TP-4TA)）膜的理化性能达到最佳平衡，在Fenton试剂中450 h后仍保持87.2%的质量。酸掺杂量为158%的PA掺杂P （TP-4TA）膜的抗拉强度为17.2 MPa，在180℃下的质子电导率为52.2 mS cm−1。采用上述膜的单个燃料电池在180°C H2/O2条件下，无加湿或背压，峰值功率密度为684 mW cm - 2，开路电压为1.0 V。本研究为HT-PEMs提供了一个新的平台，为下一代燃料电池和其他先进能源技术提供了一种通用的分子设计策略。
{"title":"Rational design of pendant thiazole functionalized polyarylenes and their applications in high temperature proton exchange membrane fuel cells","authors":"Ruixuan Lv , Zhenbei Peng , Yang Wu , Mahmoud M. Gomaa , Jingshuai Yang","doi":"10.1016/j.memsci.2025.125120","DOIUrl":"10.1016/j.memsci.2025.125120","url":null,"abstract":"<div><div>Thiazole-containing polymers are widely explored in semiconductors and photocatalysis, yet their potential as high temperature proton exchange membranes (HT-PEMs) for fuel cells remains unexplored. Here we present a new, simple and efficient superacid-catalyzed polyhydroxyalkylation strategy to synthesize six ether-free polyarylenes bearing pendant thiazole, benzothiazole, or thiazoline groups. To our knowledge, it represents the first demonstration of pendant thiazole-based polymers as HT-PEMs. Systematic structural variations, combined with theoretical calculations, reveal that freely rotating thiazole moieties engage in strong acid-base interactions and hydrogen bonding with phosphoric acid (PA), enabling high PA uptake and enhancing proton transport. Polymers derived from aldehyde monomers with methine (–CH–) linkages exhibit superior chemical and thermal stability relative to ketone-derived analogs with α-methyl (–C(CH<sub>3</sub>)–) bridges. Among them, the poly (terphenyl thiazole-4-carboxaldehyde) (P (TP-4TA)) membrane achieves the best balance of physicochemical properties, retaining 87.2 % of its mass after 450 h in Fenton's reagent. The PA doped P (TP-4TA) membrane with an acid doping content of 158 % sustains 17.2 MPa tensile strength, and delivers 52.2 mS cm<sup>−1</sup> proton conductivity at 180 °C. A single fuel cell employing above membrane attains a peak power density of 684 mW cm<sup>−2</sup> and an open-circuit voltage of 1.0 V at 180 °C under H<sub>2</sub>/O<sub>2</sub> without humidification or backpressure. This work establishes pendant thiazole-containing polyarylenes as a new platform for HT-PEMs, offering a versatile molecular design strategy for next-generation fuel cells and other advanced energy technologies.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125120"},"PeriodicalIF":9.0,"publicationDate":"2026-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145940539","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-06DOI: 10.1016/j.memsci.2026.125141
Jinhui Wang , Chao Chen , Yundong Xie , Jing Sun , Chongbo Zhao , Huanxian Shi , Xiaofei Zhang
Photocatalytic membrane integrates the merits of membrane separation and photocatalytic redox technology, have emerged as a new promising route for wastewater treatment owing to their high catalytic activity and ease of recycling. In this work, a novel FeVO4/BiOBr/PVDF photocatalytic membrane was synthesized for pharmaceutical wastewater treatment. The optimal FeVO4/BiOBr/PVDF photocatalytic membrane achieved 85.84 % tetracycline (TC) degradation efficiency within 90 min under visible light irradiation, and displayed a good self-cleaning ability. The mechanism of TC degradation pathway and enhanced removal property of FeVO4/BiOBr/PVDF membrane were systematically investigated by several techniques, including UV–Vis diffuse reflectance spectroscopy (DRS), photoelectrochemical measurements, high performance liquid chromatography-mass spectrometry (HPLC-MS), electron spin resonance (ESR) and density functional theory (DFT) calculation. The •O2− and 1O2 as the primary reactive oxygen species for TC degradation. In addition, the FeVO4/BiOBr/PVDF membrane demonstrated a water absorption rate of 81.63 %, a porosity of 75.61 %, and a 56 % increase in pure water flux (reaching 495.95 L m−2 h−1). The study offers new insights into designing a high-efficient and sustainability photocatalytic membrane for pharmaceutical wastewater purification.
光催化膜融合了膜分离技术和光催化氧化还原技术的优点，因其催化活性高、易于回收利用而成为污水处理的新途径。合成了一种新型的FeVO4/BiOBr/PVDF光催化膜，用于制药废水的处理。最优的FeVO4/BiOBr/PVDF光催化膜在可见光照射下90 min内降解四环素（TC）的效率达到85.84%，并表现出良好的自清洁能力。采用紫外-可见漫反射光谱（DRS）、光电化学测量、高效液相色谱-质谱（HPLC-MS）、电子自旋共振（ESR）和密度泛函理论（DFT）计算等技术，系统研究了TC降解途径的机理及其对FeVO4/BiOBr/PVDF膜去除性能的增强。•O2−和1O2是降解TC的主要活性氧。此外，FeVO4/BiOBr/PVDF膜的吸水率为81.63%，孔隙率为75.61%，纯水通量提高56%（达到495.95 L m−2 h−1）。该研究为设计高效、可持续的光催化膜净化制药废水提供了新的思路。
{"title":"Design and mechanistic insight into a highly efficient FeVO4/BiOBr/PVDF photocatalytic self-cleaning membrane for pharmaceutical wastewater treatment","authors":"Jinhui Wang , Chao Chen , Yundong Xie , Jing Sun , Chongbo Zhao , Huanxian Shi , Xiaofei Zhang","doi":"10.1016/j.memsci.2026.125141","DOIUrl":"10.1016/j.memsci.2026.125141","url":null,"abstract":"<div><div>Photocatalytic membrane integrates the merits of membrane separation and photocatalytic redox technology, have emerged as a new promising route for wastewater treatment owing to their high catalytic activity and ease of recycling. In this work, a novel FeVO<sub>4</sub>/BiOBr/PVDF photocatalytic membrane was synthesized for pharmaceutical wastewater treatment. The optimal FeVO<sub>4</sub>/BiOBr/PVDF photocatalytic membrane achieved 85.84 % tetracycline (TC) degradation efficiency within 90 min under visible light irradiation, and displayed a good self-cleaning ability. The mechanism of TC degradation pathway and enhanced removal property of FeVO<sub>4</sub>/BiOBr/PVDF membrane were systematically investigated by several techniques, including UV–Vis diffuse reflectance spectroscopy (DRS), photoelectrochemical measurements, high performance liquid chromatography-mass spectrometry (HPLC-MS), electron spin resonance (ESR) and density functional theory (DFT) calculation. The •O<sub>2</sub><sup>−</sup> and <sup>1</sup>O<sub>2</sub> as the primary reactive oxygen species for TC degradation. In addition, the FeVO<sub>4</sub>/BiOBr/PVDF membrane demonstrated a water absorption rate of 81.63 %, a porosity of 75.61 %, and a 56 % increase in pure water flux (reaching 495.95 L m<sup>−2</sup> h<sup>−1</sup>). The study offers new insights into designing a high-efficient and sustainability photocatalytic membrane for pharmaceutical wastewater purification.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125141"},"PeriodicalIF":9.0,"publicationDate":"2026-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941165","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-06DOI: 10.1016/j.memsci.2026.125130
Tianjia Chen , Heyao Wu , Yabin Ma , Yongfeng Zhang , Daqian Ding , Zhifei Hao , Yinmin Zhang , Yanbin Gong , Shaomin Liu
Ceramic-carbonate dual-phase (CCDP) hollow fiber membranes demonstrate superior CO2 permeability at elevated temperatures compared to their plate-shaped and conventional tubular counterparts with thick separation layer. However, their industrial deployment has been hindered by insufficient mechanical strength, stemming from intrinsic brittleness and structural vulnerabilities. To overcome this challenge, we developed a co-doping strategy for synthesizing particles as the membrane starting material to fabricate reinforced hollow fiber supports, thereby synergistically enhancing both CO2 separation efficiency and mechanical robustness. Using optimized synthesis protocols, we prepared two distinct ceramic powders: Ce0.8Sm0.1Nd0.1O2-δ (SNDC) via a one-pot approach and SDC-NDC composites (SNM) through mechanical mixing. Subsequent membrane fabrication revealed significant improvements in both separation and mechanical properties compared to baseline Ce0.8Nd0.2O2-δ (NDC)-MC membranes. The SNM-carbonate composite membrane possessed the CO2 fluxes up to 6.51 mL min−1·cm−2 at 900 °C, representing one of the highest value reported in the literatures and a bending strength of 157.3 MPa, more than double that of NDC-carbonate membranes prepared under identical calcination conditions. Moreover, the enhanced CO2 permeation of the SNDC-carbonate and SNM-carbonate membranes was attributed to the improved ceramic-phase conductivity enabled by Sm incorporation. Notably, both membranes maintained very stable permeation behavior over 100 h of continuous operation, demonstrating exceptional long-term durability. This concurrent improvement of both structural integrity and separation performance represents a good progress toward the practical implementation of CCDP hollow fiber membranes for CO2 separation applications.
陶瓷-碳酸盐双相（CCDP）中空纤维膜在高温下比具有厚分离层的板状和传统管状膜具有更好的CO2渗透性。然而，由于其固有脆性和结构脆弱性，其机械强度不足，阻碍了它们的工业部署。为了克服这一挑战，我们开发了一种共掺杂策略，通过合成颗粒作为膜起始材料来制造增强中空纤维支架，从而协同提高CO2分离效率和机械鲁棒性。采用优化后的合成工艺，采用一锅法制备了Ce0.8Sm0.1Nd0.1O2-δ (SNDC)陶瓷粉体，采用机械混合法制备了SDC-NDC复合材料（SNM）。与基线Ce0.8Nd0.2O2-δ (NDC)-MC膜相比，随后的膜制造显示出分离和力学性能的显着改善。在900℃下，snm -碳酸盐复合膜的CO2通量高达6.51 mL min - 1·cm - 2，是文献报道的最高通量之一，弯曲强度为157.3 MPa，是相同焙烧条件下制备的ndc -碳酸盐复合膜的两倍多。此外，sndc -碳酸盐和snm -碳酸盐膜的CO2渗透性增强是由于Sm的加入提高了陶瓷相的导电性。值得注意的是，两种膜在100小时的连续运行中都保持了非常稳定的渗透行为，表现出优异的长期耐久性。这种结构完整性和分离性能的同步改进代表了CCDP中空纤维膜在CO2分离应用中的实际实施的良好进展。
{"title":"Synergistic enhancement of CO2 permeation and mechanical robustness of fluorite-structured Ce-based/carbonate dual-phase hollow-fiber membranes via multi-element doping","authors":"Tianjia Chen , Heyao Wu , Yabin Ma , Yongfeng Zhang , Daqian Ding , Zhifei Hao , Yinmin Zhang , Yanbin Gong , Shaomin Liu","doi":"10.1016/j.memsci.2026.125130","DOIUrl":"10.1016/j.memsci.2026.125130","url":null,"abstract":"<div><div>Ceramic-carbonate dual-phase (CCDP) hollow fiber membranes demonstrate superior CO<sub>2</sub> permeability at elevated temperatures compared to their plate-shaped and conventional tubular counterparts with thick separation layer. However, their industrial deployment has been hindered by insufficient mechanical strength, stemming from intrinsic brittleness and structural vulnerabilities. To overcome this challenge, we developed a co-doping strategy for synthesizing particles as the membrane starting material to fabricate reinforced hollow fiber supports, thereby synergistically enhancing both CO<sub>2</sub> separation efficiency and mechanical robustness. Using optimized synthesis protocols, we prepared two distinct ceramic powders: Ce<sub>0.8</sub>Sm<sub>0.1</sub>Nd<sub>0.1</sub>O<sub>2-δ</sub> (SNDC) via a one-pot approach and SDC-NDC composites (SNM) through mechanical mixing. Subsequent membrane fabrication revealed significant improvements in both separation and mechanical properties compared to baseline Ce<sub>0.8</sub>Nd<sub>0.2</sub>O<sub>2-δ</sub> (NDC)-MC membranes. The SNM-carbonate composite membrane possessed the CO<sub>2</sub> fluxes up to 6.51 mL min<sup>−1</sup>·cm<sup>−2</sup> at 900 °C, representing one of the highest value reported in the literatures and a bending strength of 157.3 MPa, more than double that of NDC-carbonate membranes prepared under identical calcination conditions. Moreover, the enhanced CO<sub>2</sub> permeation of the SNDC-carbonate and SNM-carbonate membranes was attributed to the improved ceramic-phase conductivity enabled by Sm incorporation. Notably, both membranes maintained very stable permeation behavior over 100 h of continuous operation, demonstrating exceptional long-term durability. This concurrent improvement of both structural integrity and separation performance represents a good progress toward the practical implementation of CCDP hollow fiber membranes for CO<sub>2</sub> separation applications.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125130"},"PeriodicalIF":9.0,"publicationDate":"2026-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974089","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-05DOI: 10.1016/j.memsci.2026.125129
Zixuan Zhu, Xiangyang Qu, Fengyang Dong, Huaping Wang, Biao Wang
Ion-selective membranes are critical for vanadium redox flow battery (VRFB), yet balancing high proton conductivity with ion selectivity remains a significant challenge. Herein, we prepare polyetherimide (PEI) porous membranes with internal finger-like pores and surface micron-sized pores via non-solvent induced phase separation. Subsequently, polyethyleneimine (PI) and sodium lignosulfonate (SL) are layer-by-layer assembled on the PEI membrane to construct a bifunctional selective layer. As a result, the membrane surface features subnanometer pores (4.0–8.2 Å), which enhance vanadium ion exclusion through size sieving, while the internal finger-like pores facilitate rapid proton transport. In addition, the nitrogen-rich structure of the SL layer further improves ion selectivity through Donnan exclusion. The sulfonic acid groups of the surface SL layer act as proton transport sites, promoting rapid proton conduction. This dual ion-sieving and dual proton-conduction design, achieved through the synergy of pore and chemical structures, balances selectivity and conductivity. This outstanding performance has been demonstrated in VRFB, featuring high energy efficiency (85.67 % at 80 mA cm−2) and long-term stability (over 400 h after 500 cycles at 200 mA cm−2). This strategy of chemically synergistic subnanometer pores achieves a breakthrough in balancing selectivity and conductivity, offering a scalable method for high-performance and durable VRFB systems.
离子选择性膜对钒氧化还原液流电池（VRFB）至关重要，但平衡高质子电导率和离子选择性仍然是一个重大挑战。本文采用非溶剂诱导相分离的方法制备了具有指状孔和微米级孔的聚醚酰亚胺（PEI）多孔膜。随后，将聚乙烯亚胺（PI）和木质素磺酸钠（SL）逐层组装在PEI膜上，构建双功能选择层。因此，膜表面具有亚纳米孔径（4.0-8.2 Å），通过粒度筛分增强了钒离子的排除，而内部的指状孔径有利于质子的快速输送。此外，SL层的富氮结构通过Donnan排斥进一步提高了离子选择性。表面SL层的磺酸基充当质子转运位点，促进质子快速传导。这种双重离子筛分和双重质子传导设计，通过孔隙和化学结构的协同作用实现，平衡了选择性和导电性。这种优异的性能在VRFB中得到了证明，具有高能效（80 mA cm - 2时85.67%）和长期稳定性（200 mA cm - 2下500次循环后超过400小时）。这种化学协同的亚纳米孔隙策略在平衡选择性和导电性方面取得了突破，为高性能和耐用的VRFB系统提供了一种可扩展的方法。
{"title":"Chemically synergistic subnanometer-pore membrane with high ion selectivity and conductivity for flow battery","authors":"Zixuan Zhu, Xiangyang Qu, Fengyang Dong, Huaping Wang, Biao Wang","doi":"10.1016/j.memsci.2026.125129","DOIUrl":"10.1016/j.memsci.2026.125129","url":null,"abstract":"<div><div>Ion-selective membranes are critical for vanadium redox flow battery (VRFB), yet balancing high proton conductivity with ion selectivity remains a significant challenge. Herein, we prepare polyetherimide (PEI) porous membranes with internal finger-like pores and surface micron-sized pores via non-solvent induced phase separation. Subsequently, polyethyleneimine (PI) and sodium lignosulfonate (SL) are layer-by-layer assembled on the PEI membrane to construct a bifunctional selective layer. As a result, the membrane surface features subnanometer pores (4.0–8.2 Å), which enhance vanadium ion exclusion through size sieving, while the internal finger-like pores facilitate rapid proton transport. In addition, the nitrogen-rich structure of the SL layer further improves ion selectivity through Donnan exclusion. The sulfonic acid groups of the surface SL layer act as proton transport sites, promoting rapid proton conduction. This dual ion-sieving and dual proton-conduction design, achieved through the synergy of pore and chemical structures, balances selectivity and conductivity. This outstanding performance has been demonstrated in VRFB, featuring high energy efficiency (85.67 % at 80 mA cm<sup>−2</sup>) and long-term stability (over 400 h after 500 cycles at 200 mA cm<sup>−2</sup>). This strategy of chemically synergistic subnanometer pores achieves a breakthrough in balancing selectivity and conductivity, offering a scalable method for high-performance and durable VRFB systems.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125129"},"PeriodicalIF":9.0,"publicationDate":"2026-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145940538","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-05DOI: 10.1016/j.memsci.2026.125137
Dai Shi , Shan Luo , Jiamei Sun , Shunwen Xiao , Xianyu Sun , Yanyue Qu , Ruiyuan Zeng , Meijie Wang , Ran Chen , Youqing Tian , Yumeng Zhao , Beili Lu , Lirong Tang , Biao Huang , Hanyang Liu , Xinda You
Ionic covalent organic framework (iCOF) membranes are promising for nanofiltration, yet combining high charge density with confined pore size remains challenging because strong electrostatic repulsion disrupts ordered stacking and generates structural defects. Here, we propose a “moderately charged–highly charged–moderately charged” strategy to construct sandwich-like COF membranes (SCOFMs). By layer-by-layer assembly of TpPa-SO3H and TpPa-2SO3H nanosheets, SCOFMs with enhanced chargeability and narrowed nanopores are obtained. Increasing the outer-to-inner layer ratio from 10:0 to 7:3 raises the membrane surface charge density from −1.51 to −1.84 mC m−2 and reduces the pore diameter from 0.95 to 0.68 nm. This improvement originates from the higher chargeability and smaller pore size of TpPa-2SO3H, while the sandwich structure mitigates interlayer repulsion and promotes dense stacking. The synergistic Donnan exclusion and size-sieving endow SCOFM(7:3) with high rejection of 96.4 % for Na2SO4, 97.2 % for MgSO4, 84.4 % for NaCl, and >99 % for various antibiotics. Benefiting from this architecture, it also maintains Na2SO4 rejection larger than 91 % and stable water permeance for over 50 days. This approach simultaneously narrows nanopores and enhances the membrane surface charge density, offering a promising route for high-performance nanofiltration membranes.
离子共价有机框架（iCOF）膜在纳滤方面很有前景，但将高电荷密度与有限孔径相结合仍然具有挑战性，因为强静电斥力会破坏有序的堆叠并产生结构缺陷。在这里，我们提出了“中等电荷-高电荷-中等电荷”的策略来构建三明治状COF膜（SCOFMs）。通过层层组装TpPa-SO3H和TpPa-2SO3H纳米片，获得了具有增强的可充电性和缩小纳米孔的SCOFMs。将膜内外比从10:0增加到7:3，膜表面电荷密度从−1.51 mC m−2增加到−1.84 mC m−2，孔径从0.95 nm减小到0.68 nm。这种改善源于TpPa-2SO3H具有更高的电荷率和更小的孔径，而夹层结构减轻了层间斥力，促进了致密堆积。协同Donnan排除和筛分使SCOFM（7:3）对Na2SO4、MgSO4、NaCl和各种抗生素的拒绝率分别为96.4%、97.2%、84.4%和99%。得益于这种结构，它还保持了大于91%的Na2SO4截留率和超过50天的稳定透水性。该方法同时缩小了纳米孔，提高了膜表面电荷密度，为制备高性能纳滤膜提供了一条有前途的途径。
{"title":"Sandwich-like COF membranes with enhanced chargeability and narrowed nanopores for nanofiltration-based desalination","authors":"Dai Shi , Shan Luo , Jiamei Sun , Shunwen Xiao , Xianyu Sun , Yanyue Qu , Ruiyuan Zeng , Meijie Wang , Ran Chen , Youqing Tian , Yumeng Zhao , Beili Lu , Lirong Tang , Biao Huang , Hanyang Liu , Xinda You","doi":"10.1016/j.memsci.2026.125137","DOIUrl":"10.1016/j.memsci.2026.125137","url":null,"abstract":"<div><div>Ionic covalent organic framework (iCOF) membranes are promising for nanofiltration, yet combining high charge density with confined pore size remains challenging because strong electrostatic repulsion disrupts ordered stacking and generates structural defects. Here, we propose a “moderately charged–highly charged–moderately charged” strategy to construct sandwich-like COF membranes (SCOFMs). By layer-by-layer assembly of TpPa-SO<sub>3</sub>H and TpPa-2SO<sub>3</sub>H nanosheets, SCOFMs with enhanced chargeability and narrowed nanopores are obtained. Increasing the outer-to-inner layer ratio from 10:0 to 7:3 raises the membrane surface charge density from −1.51 to −1.84 mC m<sup>−2</sup> and reduces the pore diameter from 0.95 to 0.68 nm. This improvement originates from the higher chargeability and smaller pore size of TpPa-2SO<sub>3</sub>H, while the sandwich structure mitigates interlayer repulsion and promotes dense stacking. The synergistic Donnan exclusion and size-sieving endow SCOFM<sub>(7:3)</sub> with high rejection of 96.4 % for Na<sub>2</sub>SO<sub>4</sub>, 97.2 % for MgSO<sub>4</sub>, 84.4 % for NaCl, and >99 % for various antibiotics. Benefiting from this architecture, it also maintains Na<sub>2</sub>SO<sub>4</sub> rejection larger than 91 % and stable water permeance for over 50 days. This approach simultaneously narrows nanopores and enhances the membrane surface charge density, offering a promising route for high-performance nanofiltration membranes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125137"},"PeriodicalIF":9.0,"publicationDate":"2026-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941160","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-04DOI: 10.1016/j.memsci.2026.125127
Songbo Nan , Yin Qiao , Shuo Qiu , Siyu Liu , Tianxin Zhao , Shunqiang Ding , Ronghuan He
Crosslinking of the polymer is a usual strategy for providing compromise between proton conductivity and mechanical properties, but might bring on processing difficulty of ionic conducting membranes due to sacrificed solubility in solvents. To resolve the conflict for comprehensively superior properties, we graft 4-(bromomethyl) benzonitrile (BmBz) to crosslink poly(p-terphenyl pyridine, PTP) via conversion of the cyano groups into triazine units under an acidic environment. The occurrence of the crosslinking reaction is evidenced by the gel fraction measurement of the polymers in CH2Cl2, FT-IR spectra and XRD analysis. Notably, the crosslinked PTP-xBmBz membranes (x denotes the molar ratio of BmBz to the polymer PTP) retain excellent solubility in regular organic solvents, significantly enhancing their processability for membrane casting and electrode modification by ionomers. The crosslinked membranes exhibit superior antioxidant stability compared to the pristine PTP, which originates from the consumption of ·OH by spare cyano groups. The capturing ability of the cyano groups to free radicals has been investigated by FT-IR and 1H NMR as well as fluorescence analysis combining with the Fenton tests. In addition to enabling the crosslinking of polymer chains, the generated triazine units by trimerization of cyano groups can promote PA doping and anchoring of the membranes. As results, the proposed phosphoric acid (PA) doped PTP-0.21BmBz@315%PA membrane achieves an anhydrous proton conductivity of 133 mS cm−1 at 160 °C, which stems from the high PA uptake and well-defined microphase separation structure as revealed by SAXS and TEM results. Furthermore, the PTP-0.21BmBz@315%PA membrane-based single fuel cell delivers a high peak power density of 1014 mW cm−2 (corresponding to a specific power of 1.69 W mg−1) at 180 °C by feeding un-humidified H2 and O2 with a Pt loading of 0.6 mg cm−2. The smooth voltage profile is also obtained by operating under 200 mA cm−2 at 160 °C for 100 h. These results indicate that the PTP-0.21BmBz@315%PA membrane has the potential availability as a candidate for high performance high-temperature membranes.
聚合物的交联是一种折衷质子电导率和力学性能的常用策略，但由于牺牲了在溶剂中的溶解度，可能会给离子导电膜的加工带来困难。为了解决综合性能的冲突，我们在酸性环境下通过氰基转化为三嗪单元，将4-（溴甲基）苯腈（BmBz）接枝到交联聚（对三苯吡啶，PTP）上。聚合物在CH2Cl2中的凝胶分数测定、FT-IR光谱和XRD分析证实了交联反应的发生。值得注意的是，交联PTP- xbmbz膜（x表示BmBz与聚合物PTP的摩尔比）在常规有机溶剂中保持了良好的溶解度，显著提高了膜铸造和离子修饰的可加工性。与原始PTP相比，交联膜表现出更好的抗氧化稳定性，这是由于多余的氰基消耗了·OH。通过FT-IR和1H NMR以及结合Fenton试验的荧光分析研究了氰基对自由基的捕获能力。除了使聚合物链交联外，氰基三聚化生成的三嗪单元还可以促进PA的掺杂和膜的锚定。结果表明，在160°C下，掺PTP-0.21BmBz@315%PA的磷酸（PA）膜的无水质子电导率达到133 mS cm−1，这是由于SAXS和TEM结果显示的高PA吸收率和明确的微相分离结构。此外，PTP-0.21BmBz@315%PA膜基单燃料电池在180°C下，通过向未加湿的H2和O2注入0.6 mg cm - 2的Pt，可提供1014 mW cm - 2的峰值功率密度（对应于1.69 W mg - 1的比功率）。在200 mA cm−2下，在160°C下工作100小时，也获得了光滑的电压分布。这些结果表明PTP-0.21BmBz@315%PA膜具有作为高性能高温膜的候选材料的潜力。
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