Pub Date : 2026-04-01Epub Date: 2026-01-09DOI: 10.1016/j.memsci.2026.125146
Seyed Amirhossein Zahedi Ghoddoosi , Toraj Mohammadi , Abbas Akbarzadeh
Forward osmosis (FO) has gained popularity as an energy-efficient separation technique, but its efficiency is still restricted due to an intrinsic trade-off between water permeability and solute leakage. In this study, two machine learning (ML) approaches, namely multilayer perceptron (MLP) model and support vector machine (SVM) were developed for predicting water flux (WF; Jw) as well as reverse solute flux (RSF; Js) of cellulose acetate (CA)/cellulose triacetate (CTA) membrane in FO process. Experimental dataset including 26 input features were gathered from relevant literature, highlighting the predominant role of casting solution composition, phase inversion process condition, and the FO process operating condition. Comparison between the ML models performance revealed that the MLP architecture with 2 hidden layers containing 11, and 9 neurons, Bayesian-Regularization as training algorithm, and ‘tanh’ activation function in hidden layer outperforms the SVM, achieving R2 values above 0.95. To identify the best trade-off, the optimal MLP model was further introduced to non-dominated sorting genetic algorithm (NSGA-II). Following 81 iterations, the optimization convergence yielded an optimal condition with WF ≈ 78.57 L m−2 h−1 (LMH) and RSF ≈ 4.39 g m−2 h−1 (GMH). These outcomes emphasize the potential of hybrid ML–optimization strategies to accelerate the FO membrane design by quantitatively balancing permeability and selectivity.
正渗透（FO）作为一种高效节能的分离技术已经得到了广泛的应用，但由于水渗透性和溶质泄漏之间的内在权衡，其效率仍然受到限制。本研究采用多层感知器（MLP）模型和支持向量机（SVM）两种机器学习方法，预测了醋酸纤维素(CA)/三醋酸纤维素（CTA）膜在FO过程中的水通量（WF; Jw）和反溶质通量（RSF; Js）。从相关文献中收集了包含26个输入特征的实验数据集，突出了铸造溶液组成、相转化工艺条件和FO工艺操作条件的主导作用。通过对ML模型性能的比较发现，包含11个神经元和9个神经元的2隐层MLP架构，贝叶斯正则化作为训练算法，隐层“tanh”激活函数优于SVM， R2值在0.95以上。为了确定最佳权衡，将最优MLP模型进一步引入非支配排序遗传算法（NSGA-II）。经过81次迭代，优化收敛得到WF≈78.57 L m−2 h−1 （LMH）和RSF≈4.39 g m−2 h−1 （GMH）的最优条件。这些结果强调了混合ml优化策略的潜力，通过定量平衡渗透性和选择性来加速FO膜的设计。
{"title":"Machine learning-driven performance prediction and optimization of CA/CTA forward osmosis membranes for sustainable water desalination applications","authors":"Seyed Amirhossein Zahedi Ghoddoosi , Toraj Mohammadi , Abbas Akbarzadeh","doi":"10.1016/j.memsci.2026.125146","DOIUrl":"10.1016/j.memsci.2026.125146","url":null,"abstract":"<div><div>Forward osmosis (FO) has gained popularity as an energy-efficient separation technique, but its efficiency is still restricted due to an intrinsic trade-off between water permeability and solute leakage. In this study, two machine learning (ML) approaches, namely multilayer perceptron (MLP) model and support vector machine (SVM) were developed for predicting water flux (WF; J<sub>w</sub>) as well as reverse solute flux (RSF; J<sub>s</sub>) of cellulose acetate (CA)/cellulose triacetate (CTA) membrane in FO process. Experimental dataset including 26 input features were gathered from relevant literature, highlighting the predominant role of casting solution composition, phase inversion process condition, and the FO process operating condition. Comparison between the ML models performance revealed that the MLP architecture with 2 hidden layers containing 11, and 9 neurons, Bayesian-Regularization as training algorithm, and ‘tanh’ activation function in hidden layer outperforms the SVM, achieving R<sup>2</sup> values above 0.95. To identify the best trade-off, the optimal MLP model was further introduced to non-dominated sorting genetic algorithm (NSGA-II). Following 81 iterations, the optimization convergence yielded an optimal condition with WF ≈ 78.57 L m<sup>−2</sup> h<sup>−1</sup> (LMH) and RSF ≈ 4.39 g m<sup>−2</sup> h<sup>−1</sup> (GMH). These outcomes emphasize the potential of hybrid ML–optimization strategies to accelerate the FO membrane design by quantitatively balancing permeability and selectivity.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"744 ","pages":"Article 125146"},"PeriodicalIF":9.0,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146075891","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 : 2026-04-01Epub Date: 2026-01-21DOI: 10.1016/j.memsci.2026.125196
Xiaochang Cao , Rongqing Feng , Fang Cheng , Jianming Liu , Zhi Wang
Oxygen/nitrogen (O2/N2) separation technology is crucial in industrial and environmental fields, yet traditional membrane materials struggle to overcome selectivity limitations because of the similar kinetic diameters and polarities of O2 and N2. Inspired by the reversible metalloporphyrin–O2 coordination mechanism in hemoglobin, in this study, a porphyrin-based metal–organic framework (PorMOF) embedding high-density biomimetic sites was designed and synthesized, which was then coated onto magnetic CoFe2O4 particles to form a core–shell collaborative structure. The magnetic core attracts paramagnetic O2 to aggregate within the biomimetic shell for dynamic transport. Thereon, the ordered biomimetic sites driven by the magnetic field construct efficient channels in PIM-1 membranes that prioritize oxygen permeation, structurally enhancing separation performance. A systematic investigation was conducted on (i) the mechanisms of site interactions in different biomimetic structures, (ii) the collaboration between magnetic enrichment and biomimetic effects, and (iii) the influence of loading on O2/N2 separation performance. Under a magnetic field of 80 mT, the 20 wt% dual-site CoFe2O4@PorMOF/PIM membrane achieved an O2 permeability coefficient of 975 Barrer and an O2/N2 separation factor of 8.13, significantly exceeding the 2015 upper limit. During 240 h of testing, the membrane maintained stable performance and demonstrated robustness under magnetic field fluctuations. This work provides a magnetic-biomimetic synergistic strategy that offers a bioinspired avenue for functional membrane design.
{"title":"Hemoglobin-inspired PorMOFs synergizing with magnetic enrichment for efficient O2/N2 separation membranes","authors":"Xiaochang Cao , Rongqing Feng , Fang Cheng , Jianming Liu , Zhi Wang","doi":"10.1016/j.memsci.2026.125196","DOIUrl":"10.1016/j.memsci.2026.125196","url":null,"abstract":"<div><div>Oxygen/nitrogen (O<sub>2</sub>/N<sub>2</sub>) separation technology is crucial in industrial and environmental fields, yet traditional membrane materials struggle to overcome selectivity limitations because of the similar kinetic diameters and polarities of O<sub>2</sub> and N<sub>2</sub>. Inspired by the reversible metalloporphyrin–O<sub>2</sub> coordination mechanism in hemoglobin, in this study, a porphyrin-based metal–organic framework (PorMOF) embedding high-density biomimetic sites was designed and synthesized, which was then coated onto magnetic CoFe<sub>2</sub>O<sub>4</sub> particles to form a core–shell collaborative structure. The magnetic core attracts paramagnetic O<sub>2</sub> to aggregate within the biomimetic shell for dynamic transport. Thereon, the ordered biomimetic sites driven by the magnetic field construct efficient channels in PIM-1 membranes that prioritize oxygen permeation, structurally enhancing separation performance. A systematic investigation was conducted on (i) the mechanisms of site interactions in different biomimetic structures, (ii) the collaboration between magnetic enrichment and biomimetic effects, and (iii) the influence of loading on O<sub>2</sub>/N<sub>2</sub> separation performance. Under a magnetic field of 80 mT, the 20 wt% dual-site CoFe<sub>2</sub>O<sub>4</sub>@PorMOF/PIM membrane achieved an O<sub>2</sub> permeability coefficient of 975 Barrer and an O<sub>2</sub>/N<sub>2</sub> separation factor of 8.13, significantly exceeding the 2015 upper limit. During 240 h of testing, the membrane maintained stable performance and demonstrated robustness under magnetic field fluctuations. This work provides a magnetic-biomimetic synergistic strategy that offers a bioinspired avenue for functional membrane design.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"744 ","pages":"Article 125196"},"PeriodicalIF":9.0,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146037365","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 : 2026-04-01Epub Date: 2026-02-03DOI: 10.1016/j.memsci.2026.125233
Peng Zhang , Wenjing Wang , Wenqing Wang , Kun Jiang , Ming Teng , Shuaishuai Han , Chongyuan Ma , Jianyan Feng , Xiaomin Luo
The large-scalable fabrication of graphene oxide (GO)-based nanofiltration (NF) membranes is still hindered by interfacial instability and insufficient structural robustness, which limit their practical deployment. Here, we propose a dual interlocking strategy that synergistically combines "rooting" anchoring and confined interfacial polymerization to construct stable GO-based NF membranes. Poly(ethylene terephthalate) (PET) nonwoven fabric is mechanically polished to generate a burr-like surface for physical anchoring, while solid-state interfacial polymerization between trimesoyl chloride (TMC) and amino-functionalized GO (NH2–GO) formed a polyamide (PA) layer for surface locking, ensuring durable interfacial adhesion. The optimized membrane achieves high rejection of dyes (96.2–98.5% for Congo Red) and salts (70.9% for NaCl) while maintaining comparable water permeance (1.78–2.23 L m−2 h−1·bar−1). Moreover, the membrane demonstrates outstanding long-term stability, antifouling performance (84.47% flux recovery), and strong resistance to harsh conditions (>95% rejection after 48 h solvent immersion, stable under pH 2–12). The interlocked architecture significantly enhances peeling and deformation resistance, validating a facile and scalable pathway for robust NF membrane fabrication. This work establishes an effective interfacial engineering paradigm, offering a promising platform for the practical application of GO-based NF membranes in advanced water purification and molecular separation technologies.
基于氧化石墨烯（GO）的纳滤（NF）膜的大规模制备仍然受到界面不稳定性和结构鲁棒性不足的阻碍，这限制了其实际部署。在这里，我们提出了一种双联锁策略，将“生根”锚定和受限界面聚合协同结合，以构建稳定的氧化石墨烯基NF膜。聚对苯二甲酸乙酯（PET）非织造布通过机械抛光产生毛刺状表面，用于物理锚定，而三聚氯胺（TMC）和氨基功能化氧化石墨烯（NH2-GO）之间的固态界面聚合形成聚酰胺（PA）层，用于表面锁定，确保持久的界面粘附。优化后的膜对染料（刚果红为96.2-98.5%）和盐（NaCl为70.9%）的去除率较高，同时保持了相当的透水性（1.78-2.23 L m−2 h−1·bar−1）。此外，该膜具有良好的长期稳定性、防污性能（通量回收率为84.47%）和较强的耐恶劣条件（浸溶剂48 h后去除率为95%，在pH 2-12下稳定）。联锁结构显著增强了剥离和抗变形能力，验证了一个简单和可扩展的途径，用于稳健的NF膜制造。这项工作建立了一个有效的界面工程范例，为氧化石墨烯基纳滤膜在高级水净化和分子分离技术中的实际应用提供了一个有前景的平台。
{"title":"Interfacially confined polymerization-mediated laminated interlocking strategy for constructing scalable graphene oxide nanofiltration membranes with enhanced stability and selectivity","authors":"Peng Zhang , Wenjing Wang , Wenqing Wang , Kun Jiang , Ming Teng , Shuaishuai Han , Chongyuan Ma , Jianyan Feng , Xiaomin Luo","doi":"10.1016/j.memsci.2026.125233","DOIUrl":"10.1016/j.memsci.2026.125233","url":null,"abstract":"<div><div>The large-scalable fabrication of graphene oxide (GO)-based nanofiltration (NF) membranes is still hindered by interfacial instability and insufficient structural robustness, which limit their practical deployment. Here, we propose a dual interlocking strategy that synergistically combines \"rooting\" anchoring and confined interfacial polymerization to construct stable GO-based NF membranes. Poly(ethylene terephthalate) (PET) nonwoven fabric is mechanically polished to generate a burr-like surface for physical anchoring, while solid-state interfacial polymerization between trimesoyl chloride (TMC) and amino-functionalized GO (NH<sub>2</sub>–GO) formed a polyamide (PA) layer for surface locking, ensuring durable interfacial adhesion. The optimized membrane achieves high rejection of dyes (96.2–98.5% for Congo Red) and salts (70.9% for NaCl) while maintaining comparable water permeance (1.78–2.23 L m<sup>−2</sup> h<sup>−1</sup>·bar<sup>−1</sup>). Moreover, the membrane demonstrates outstanding long-term stability, antifouling performance (84.47% flux recovery), and strong resistance to harsh conditions (>95% rejection after 48 h solvent immersion, stable under pH 2–12). The interlocked architecture significantly enhances peeling and deformation resistance, validating a facile and scalable pathway for robust NF membrane fabrication. This work establishes an effective interfacial engineering paradigm, offering a promising platform for the practical application of GO-based NF membranes in advanced water purification and molecular separation technologies.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"745 ","pages":"Article 125233"},"PeriodicalIF":9.0,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146172332","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 : 2026-04-01Epub Date: 2026-02-07DOI: 10.1016/j.memsci.2026.125245
Lei Wu , Yiqiang Deng , Dayi Guo , Guoshuai Zhang , Tanlai Yu , Xiuling Chen , Nanwen Li
Carbon molecular sieve (CMS) membranes represent a class of high-performance separation materials capable of surpassing the conventional permeability-selectivity trade-off. Introducing fillers into polymer precursors can further enhance the performance of the resulting CMS membranes; however, incompatibility between fillers and the polymer matrix often results in interfacial defects. In this study, the small-molecule cross-linker N,N′-1,3-phenylenedimaleimide (PDM) was incorporated into a 6FDA-BPDA/TFDB polyimide to prepare optically transparent, uniform, and defect-free PDM-x precursor membranes. These precursor membranes were first subjected to thermal treatment at 300 °C for 1 h to form a semi-interpenetrating polymer network (SIPN) structure, and then pyrolyzed at 550 °C to obtain PDM-x-SIPN CMS membranes. The successful formation of a cross-linked semi-interpenetrating polymer network (SIPN) in the precursor was verified by TGA, ATR-FTIR, and XRD analyses. The resulting PDM-20-SIPN CMS membrane delivered exceptional gas-separation performance, with O2 and CO2 permeabilities of 1631 and 9904 Barrer, and O2/N2 and CO2/CH4 selectivities of 6.7 and 67.8, respectively—exceeding the latest upper-bound limits. Furthermore, the membrane showcased outstanding aging resistance over 720 h, significantly outperforming the conventional 6FDA-BPDA/TFDB CMS membrane. This study not only offers a robust precursor-design strategy, but also provides a foundation for the future development of high-performance CMS materials in sustainable separation processes.
{"title":"Semi-interpenetrating polymer networks for efficient carbon molecular sieve gas separation membrane","authors":"Lei Wu , Yiqiang Deng , Dayi Guo , Guoshuai Zhang , Tanlai Yu , Xiuling Chen , Nanwen Li","doi":"10.1016/j.memsci.2026.125245","DOIUrl":"10.1016/j.memsci.2026.125245","url":null,"abstract":"<div><div>Carbon molecular sieve (CMS) membranes represent a class of high-performance separation materials capable of surpassing the conventional permeability-selectivity trade-off. Introducing fillers into polymer precursors can further enhance the performance of the resulting CMS membranes; however, incompatibility between fillers and the polymer matrix often results in interfacial defects. In this study, the small-molecule cross-linker <em>N,N</em>′-1,3-phenylenedimaleimide (PDM) was incorporated into a 6FDA-BPDA/TFDB polyimide to prepare optically transparent, uniform, and defect-free PDM-x precursor membranes. These precursor membranes were first subjected to thermal treatment at 300 °C for 1 h to form a semi-interpenetrating polymer network (SIPN) structure, and then pyrolyzed at 550 °C to obtain PDM-x-SIPN CMS membranes. The successful formation of a cross-linked semi-interpenetrating polymer network (SIPN) in the precursor was verified by TGA, ATR-FTIR, and XRD analyses. The resulting PDM-20-SIPN CMS membrane delivered exceptional gas-separation performance, with O<sub>2</sub> and CO<sub>2</sub> permeabilities of 1631 and 9904 Barrer, and O<sub>2</sub>/N<sub>2</sub> and CO<sub>2</sub>/CH<sub>4</sub> selectivities of 6.7 and 67.8, respectively—exceeding the latest upper-bound limits. Furthermore, the membrane showcased outstanding aging resistance over 720 h, significantly outperforming the conventional 6FDA-BPDA/TFDB CMS membrane. This study not only offers a robust precursor-design strategy, but also provides a foundation for the future development of high-performance CMS materials in sustainable separation processes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"745 ","pages":"Article 125245"},"PeriodicalIF":9.0,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146172333","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 : 2026-04-01Epub Date: 2026-02-04DOI: 10.1016/j.memsci.2026.125241
Hui-Qian Huo , Ze-Jian Chen , Bing-Xin Gu , Xiang-Yun Xie , Yan-Li Ji , Cong-Jie Gao
Selective cation exchange membranes (SCEMs) are crucial for renewable energy storage and conversion, seawater softening and wastewater treatment, and ionic resource extraction and purification. However, precisely controlling the pore microstructure of SCEMs to efficiently separate mono-/divalent cations with similar hydrated radii remains a critical challenge in electrodialysis (ED) membrane research. Herein, we report a surface-programmed cross-linking strategy to fabricate an ultrathin, asymmetric modification layer on a commercial CEM (CTG) using diaminoethyl imidazole bromide (DAIB) monomers and polyethyleneimine (PEI) macromolecules. A hydrophilic, loose cross-linked DAIB-rich sub-layer was first formed on the CTG surface via the Debus–Radziszowski reaction, followed by the construction of a densely cross-linked PEI-rich upper layer through secondary surface cross-linking. The asymmetric architecture and chemical design of the PEI-DAIB composite modification layer facilitate rapid monovalent ion transport while efficiently rejecting divalent ions, thus overcoming the permeability-selectivity trade-off. The optimized PEI-DAIB composite membrane exhibits a high Li+ permeation rate (0.75 mol m−2 h−1) and exceptional Li+/Mg2+ permselectivity (72), outperforming most state-of-the-art ED membranes reported in the literature. Furthermore, the membrane demonstrates excellent stability and efficient Li+ extraction from simulated salt-lake brines via two-stage ED, ultimately achieving 99.9% Li+ purity with low energy consumption (∼0.2 kWh mol−1 Li+). This work provides a promising strategy for developing high-performance SCEMs to achieve sustainable ionic resource extraction and purification.
{"title":"Surface-engineered cation exchange membranes with asymmetric structural modification layers: Toward high-efficient Li+ recovery from salt lakes via electrodialysis","authors":"Hui-Qian Huo , Ze-Jian Chen , Bing-Xin Gu , Xiang-Yun Xie , Yan-Li Ji , Cong-Jie Gao","doi":"10.1016/j.memsci.2026.125241","DOIUrl":"10.1016/j.memsci.2026.125241","url":null,"abstract":"<div><div>Selective cation exchange membranes (SCEMs) are crucial for renewable energy storage and conversion, seawater softening and wastewater treatment, and ionic resource extraction and purification. However, precisely controlling the pore microstructure of SCEMs to efficiently separate mono-/divalent cations with similar hydrated radii remains a critical challenge in electrodialysis (ED) membrane research. Herein, we report a surface-programmed cross-linking strategy to fabricate an ultrathin, asymmetric modification layer on a commercial CEM (CTG) using diaminoethyl imidazole bromide (DAIB) monomers and polyethyleneimine (PEI) macromolecules. A hydrophilic, loose cross-linked DAIB-rich sub-layer was first formed on the CTG surface via the Debus–Radziszowski reaction, followed by the construction of a densely cross-linked PEI-rich upper layer through secondary surface cross-linking. The asymmetric architecture and chemical design of the PEI-DAIB composite modification layer facilitate rapid monovalent ion transport while efficiently rejecting divalent ions, thus overcoming the permeability-selectivity trade-off. The optimized PEI-DAIB composite membrane exhibits a high Li<sup>+</sup> permeation rate (0.75 mol m<sup>−2</sup> h<sup>−1</sup>) and exceptional Li<sup>+</sup>/Mg<sup>2+</sup> permselectivity (72), outperforming most state-of-the-art ED membranes reported in the literature. Furthermore, the membrane demonstrates excellent stability and efficient Li<sup>+</sup> extraction from simulated salt-lake brines via two-stage ED, ultimately achieving 99.9% Li<sup>+</sup> purity with low energy consumption (∼0.2 kWh mol<sup>−1</sup> Li<sup>+</sup>). This work provides a promising strategy for developing high-performance SCEMs to achieve sustainable ionic resource extraction and purification.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"745 ","pages":"Article 125241"},"PeriodicalIF":9.0,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146172336","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 : 2026-04-01Epub Date: 2026-01-19DOI: 10.1016/j.memsci.2026.125150
Yue Sun , Yu Zhao , Xiaoxia Sun , Qingshan Liu , Jia Xu
Polyurea (PU) materials show great potential for pH-stable reverse osmosis (RO) membranes essential in sustainable water treatment. However, PU membranes derived from 2,4-toluene diisocyanate (TDI) suffer from intrinsic alkaline resistance limitations due to steric hindrance from 1-position methyl groups, which reduce reaction kinetics and cross-linking density. Here, we introduce a triethylamine (TEA)-mediated strategy to accelerate TDI hydrolysis and form semi-interpenetrating networks (semi-IPN), integrating reticulated aliphatic and linear aromatic polyurea chains into a robust selective layer. The resulting membranes achieve outstanding desalination performance, with NaCl and MgCl2 rejections exceeding 98 % at water permeance over 1.3 L m−2 h−1 bar−1, ∼38 % improvement in NaCl rejection over conventional PU membranes. Notably, after 216 h in 0.1 M NaOH, the membranes maintain NaCl and MgCl2 rejections above 92 % with only ∼5 % reduction, outperforming TEA-free PU and commercial polyamide membranes, which lose ∼9 % and ∼12 % rejection, respectively. Dynamic anti-alkali tests confirm sustained performance above 95 % in highly alkaline environments. Mechanistic investigations attribute the enhanced alkaline resistance to tortuous diffusion pathways, increased cross-linking density, and enriched double hydrogen bonds, reducing swelling and improving hydrolytic stability. This work highlights semi-IPN PU membranes as a durable solution for extending desalination and wastewater treatment to highly alkaline industrial effluents.
聚脲（PU）材料在ph稳定反渗透（RO）膜的可持续水处理中显示出巨大的潜力。然而，由2,4-甲苯二异氰酸酯（TDI）衍生的PU膜由于1位甲基的位阻而受到固有的耐碱性限制，从而降低了反应动力学和交联密度。在这里，我们引入了一种三乙胺（TEA）介导的策略来加速TDI水解并形成半互穿网络（半ipn），将网状脂肪族和线性芳香聚脲链整合到一个强大的选择层中。所得膜具有出色的脱盐性能，在渗透率超过1.3 L m−2 h−1 bar−1时，NaCl和MgCl2的去除率超过98%，比传统PU膜的NaCl去除率提高约38%。值得注意的是，在0.1 M NaOH中浸泡216小时后，膜的NaCl和MgCl2截留率保持在92%以上，仅下降了~ 5%，优于不含tea的PU膜和商用聚酰胺膜，后者的截留率分别下降了~ 9%和~ 12%。动态抗碱测试证实，在高碱性环境下，性能持续保持在95%以上。机理研究将增强的抗碱性归因于弯曲的扩散途径、增加的交联密度和丰富的双氢键，减少膨胀和提高水解稳定性。这项工作突出了半ipn PU膜作为一种持久的解决方案，扩展海水淡化和废水处理到高碱性工业废水。
{"title":"Catalyst-enhanced semi-interpenetrating polyurea networks for alkaline-resistant reverse osmosis membranes","authors":"Yue Sun , Yu Zhao , Xiaoxia Sun , Qingshan Liu , Jia Xu","doi":"10.1016/j.memsci.2026.125150","DOIUrl":"10.1016/j.memsci.2026.125150","url":null,"abstract":"<div><div>Polyurea (PU) materials show great potential for pH-stable reverse osmosis (RO) membranes essential in sustainable water treatment. However, PU membranes derived from 2,4-toluene diisocyanate (TDI) suffer from intrinsic alkaline resistance limitations due to steric hindrance from 1-position methyl groups, which reduce reaction kinetics and cross-linking density. Here, we introduce a triethylamine (TEA)-mediated strategy to accelerate TDI hydrolysis and form semi-interpenetrating networks (semi-IPN), integrating reticulated aliphatic and linear aromatic polyurea chains into a robust selective layer. The resulting membranes achieve outstanding desalination performance, with NaCl and MgCl<sub>2</sub> rejections exceeding 98 % at water permeance over 1.3 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup>, ∼38 % improvement in NaCl rejection over conventional PU membranes. Notably, after 216 h in 0.1 M NaOH, the membranes maintain NaCl and MgCl<sub>2</sub> rejections above 92 % with only ∼5 % reduction, outperforming TEA-free PU and commercial polyamide membranes, which lose ∼9 % and ∼12 % rejection, respectively. Dynamic anti-alkali tests confirm sustained performance above 95 % in highly alkaline environments. Mechanistic investigations attribute the enhanced alkaline resistance to tortuous diffusion pathways, increased cross-linking density, and enriched double hydrogen bonds, reducing swelling and improving hydrolytic stability. This work highlights semi-IPN PU membranes as a durable solution for extending desalination and wastewater treatment to highly alkaline industrial effluents.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"744 ","pages":"Article 125150"},"PeriodicalIF":9.0,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146075893","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 : 2026-04-01Epub Date: 2026-01-24DOI: 10.1016/j.memsci.2026.125202
Kevin E. Pataroque , Subhamoy Mahajan , Jonathan Mejia , Martina del Cerro , Jishan Wu , Hanqing Fan , Ying Li , Eric M.V. Hoek , Menachem Elimelech
Understanding transport mechanisms in thin-film composite membranes is critical for advancing membrane technology. While the solution-friction model, or more appropriately, the sorption-friction (SF) model, can describe water and salt transport behavior, the contribution of frictional forces towards salt–water selectivity in different membranes has not been explored. In this study, we establish relationships between intrinsic membrane properties and transport parameters based on the SF model, using permeation experiments and molecular dynamics (MD) simulations. Pore sizes of various commercial thin-film composite membranes are quantified by measuring the rejection of neutral organic solutes. Salt partitioning is measured using quartz crystal microbalance, while salt permeance is determined in a stirred dead-end cell. Our results show that as pore size increased from 0.6 to 0.7 nm, salt partitioning increased by 21.2 %, while salt permeance increased more than tenfold. These results suggest that transport within the membrane, rather than salt partitioning at the membrane surface, is more sensitive to changes in membrane structure. Using the SF model, we show that ion-membrane and water-membrane interactions decrease with larger pore sizes, which may explain the observed differences in salt and water permeances. These findings are supported by MD simulations used to determine ion and water self-diffusion coefficients in five distinct membranes. Through these simulations, we confirmed that water and ion mobilities are greater in membranes with larger pores due to weaker frictional interactions between these species and the membrane. This study demonstrates how frictional forces are related to membrane pore size and can be effectively used to model salt and water transport through the membrane.
{"title":"Role of frictional forces in salt and water transport through polyamide reverse osmosis membranes","authors":"Kevin E. Pataroque , Subhamoy Mahajan , Jonathan Mejia , Martina del Cerro , Jishan Wu , Hanqing Fan , Ying Li , Eric M.V. Hoek , Menachem Elimelech","doi":"10.1016/j.memsci.2026.125202","DOIUrl":"10.1016/j.memsci.2026.125202","url":null,"abstract":"<div><div>Understanding transport mechanisms in thin-film composite membranes is critical for advancing membrane technology. While the solution-friction model, or more appropriately, the sorption-friction (SF) model, can describe water and salt transport behavior, the contribution of frictional forces towards salt–water selectivity in different membranes has not been explored. In this study, we establish relationships between intrinsic membrane properties and transport parameters based on the SF model, using permeation experiments and molecular dynamics (MD) simulations. Pore sizes of various commercial thin-film composite membranes are quantified by measuring the rejection of neutral organic solutes. Salt partitioning is measured using quartz crystal microbalance, while salt permeance is determined in a stirred dead-end cell. Our results show that as pore size increased from 0.6 to 0.7 nm, salt partitioning increased by 21.2 %, while salt permeance increased more than tenfold. These results suggest that transport within the membrane, rather than salt partitioning at the membrane surface, is more sensitive to changes in membrane structure. Using the SF model, we show that ion-membrane and water-membrane interactions decrease with larger pore sizes, which may explain the observed differences in salt and water permeances. These findings are supported by MD simulations used to determine ion and water self-diffusion coefficients in five distinct membranes. Through these simulations, we confirmed that water and ion mobilities are greater in membranes with larger pores due to weaker frictional interactions between these species and the membrane. This study demonstrates how frictional forces are related to membrane pore size and can be effectively used to model salt and water transport through the membrane.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"744 ","pages":"Article 125202"},"PeriodicalIF":9.0,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146075894","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}
Boron removal from brackish water remains a challenge for potable water production due to the poor rejection of neutral boric acid by conventional reverse osmosis (RO) membranes. Here, we report a nanohybrid-incorporated polyamide membrane for efficient boron separation. The unique “brick-and-cement” configuration, formed by exfoliated layered double hydroxide (LDH) nanosheets (i.e., brick) and phytic acid-doped polyaniline (i.e., cement), endows the selective layer with enhanced hydrophilicity and additional water transport channels. Correspondingly, the newly developed membrane shows a water contact angle of 36° and a selective layer thickness on the order of 400 nm. The optimized membrane exhibited a water permeance of 2.76 LMH bar−1 and achieved high rejection rates of 99.25 % for NaCl and 81.95 % for boron when tested with a feed solution containing 15 ppm boron and 2000 ppm NaCl. A long-term operation over 400 h confirmed its structural stability without loss of permeability or selectivity. Moreover, a real seawater permeate was employed as feed to enhance practical relevance. Using this feed with 1.5 ppm boron and 250 ppm NaCl, the developed membrane had a water permeance of 4.82 LMH bar−1, salt rejection of 99.51 %, and boron rejection of 87.30 %. Complementary molecular dynamics (MD) simulation revealed the presence of interconnected free volumes as pathways for selective transport, thereby providing mechanistic evidence for the observed macroscopic performance. This work demonstrates a rational interfacial engineering approach to designing RO membranes with balanced permeability and selectivity. It may offer a promising strategy for tackling boron removal in desalination processes.
{"title":"Brick-and-cement structured polyamide membranes enabling to selectively separate boron from brackish water and real seawater permeate","authors":"Sidi Zhu , M. Shahnawaz Khan , Kaihong Xiao , Chia-Ming Chang , Qipeng Zhao , Tai-Shung Chung , Shing Bor Chen","doi":"10.1016/j.memsci.2026.125198","DOIUrl":"10.1016/j.memsci.2026.125198","url":null,"abstract":"<div><div>Boron removal from brackish water remains a challenge for potable water production due to the poor rejection of neutral boric acid by conventional reverse osmosis (RO) membranes. Here, we report a nanohybrid-incorporated polyamide membrane for efficient boron separation. The unique “brick-and-cement” configuration, formed by exfoliated layered double hydroxide (LDH) nanosheets (i.e., brick) and phytic acid-doped polyaniline (i.e., cement), endows the selective layer with enhanced hydrophilicity and additional water transport channels. Correspondingly, the newly developed membrane shows a water contact angle of 36° and a selective layer thickness on the order of 400 nm. The optimized membrane exhibited a water permeance of 2.76 LMH bar<sup>−1</sup> and achieved high rejection rates of 99.25 % for NaCl and 81.95 % for boron when tested with a feed solution containing 15 ppm boron and 2000 ppm NaCl. A long-term operation over 400 h confirmed its structural stability without loss of permeability or selectivity. Moreover, a real seawater permeate was employed as feed to enhance practical relevance. Using this feed with 1.5 ppm boron and 250 ppm NaCl, the developed membrane had a water permeance of 4.82 LMH bar<sup>−1</sup>, salt rejection of 99.51 %, and boron rejection of 87.30 %. Complementary molecular dynamics (MD) simulation revealed the presence of interconnected free volumes as pathways for selective transport, thereby providing mechanistic evidence for the observed macroscopic performance. This work demonstrates a rational interfacial engineering approach to designing RO membranes with balanced permeability and selectivity. It may offer a promising strategy for tackling boron removal in desalination processes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"744 ","pages":"Article 125198"},"PeriodicalIF":9.0,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146037368","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 : 2026-04-01Epub Date: 2026-02-03DOI: 10.1016/j.memsci.2026.125207
Zhidong Guo , Jingwen Si , Huijie Zheng , Liangliang Dong , Hao Li
Efficient separation of organic molecules from inorganic salts in high-salt, multi-component systems remains a significant challenge in fine chemical processes. Traditional membrane materials often exhibit limitations in flux, selectivity, and chemical stability, which restrict their performance and applicability in industrial separation processes. Herein, this study proposes a strategy for fabricating COF membranes using fluorinated monomers to simultaneously enhance the flux, selectivity, and chemical stability. Specifically, a highly crystalline fluorinated COF membrane was synthesized on an alumina tube using a solvothermal method. This approach achieves three key goals: (i) creating low-surface-energy channels to facilitate the rapid transport of solvents, (ii) narrowing the pore size of the one-dimensional channels of the COF membrane to enhance sieving selectivity, and (iii) enhancing the framework stability to confer robust chemical stability to the membrane system. The resulting membrane demonstrated high permeability (102.34 L m−2 h−1 bar−1) and an outstanding retention rate of over 99.9% for Congo red, corresponding to a CR/NaCl separation factor of 906. It also maintains a selective window for high antibiotic retention and low salt retention in antibiotic/salt system. This study offers an effective method for creating fluorinated COF membranes with high permeability and precise sieving capabilities, providing high-performance membrane materials suitable for high-salt dye desalination, antibiotic purification, and other specialized separation applications.
高盐、多组分体系中有机分子与无机盐的有效分离是精细化工过程中的重大挑战。传统膜材料在通量、选择性和化学稳定性等方面存在局限性，制约了其在工业分离过程中的性能和适用性。在此，本研究提出了一种利用氟化单体制备COF膜的策略，以同时提高通量、选择性和化学稳定性。具体而言，采用溶剂热法在氧化铝管上合成了高结晶氟化碳膜。该方法实现了三个关键目标：(i)创建低表面能通道，以促进溶剂的快速运输；（ii）缩小COF膜一维通道的孔径，以提高筛选选择性；（iii）增强框架稳定性，以赋予膜系统强大的化学稳定性。所得膜具有高透性（102.34 L m−2 h−1 bar−1），对刚果红的保留率超过99.9%，CR/NaCl分离系数为906。它还在抗生素/盐系统中保持了高抗生素滞留和低盐滞留的选择性窗口。本研究为制备具有高渗透性和精确筛分能力的氟化COF膜提供了有效的方法，为高盐染料脱盐、抗生素纯化和其他专业分离应用提供了高性能膜材料。
{"title":"In situ construction of fluorinated covalent organic framework membranes for high-efficiency nanofiltration","authors":"Zhidong Guo , Jingwen Si , Huijie Zheng , Liangliang Dong , Hao Li","doi":"10.1016/j.memsci.2026.125207","DOIUrl":"10.1016/j.memsci.2026.125207","url":null,"abstract":"<div><div>Efficient separation of organic molecules from inorganic salts in high-salt, multi-component systems remains a significant challenge in fine chemical processes. Traditional membrane materials often exhibit limitations in flux, selectivity, and chemical stability, which restrict their performance and applicability in industrial separation processes. Herein, this study proposes a strategy for fabricating COF membranes using fluorinated monomers to simultaneously enhance the flux, selectivity, and chemical stability. Specifically, a highly crystalline fluorinated COF membrane was synthesized on an alumina tube using a solvothermal method. This approach achieves three key goals: (i) creating low-surface-energy channels to facilitate the rapid transport of solvents, (ii) narrowing the pore size of the one-dimensional channels of the COF membrane to enhance sieving selectivity, and (iii) enhancing the framework stability to confer robust chemical stability to the membrane system. The resulting membrane demonstrated high permeability (102.34 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup>) and an outstanding retention rate of over 99.9% for Congo red, corresponding to a CR/NaCl separation factor of 906. It also maintains a selective window for high antibiotic retention and low salt retention in antibiotic/salt system. This study offers an effective method for creating fluorinated COF membranes with high permeability and precise sieving capabilities, providing high-performance membrane materials suitable for high-salt dye desalination, antibiotic purification, and other specialized separation applications.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"745 ","pages":"Article 125207"},"PeriodicalIF":9.0,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146172390","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 : 2026-04-01Epub Date: 2026-02-09DOI: 10.1016/j.memsci.2026.125269
Siheng Zhao , Xiaoqi Ma , Shengchao Zhao , Kuo Chen , Jianquan Peng , Zilong Huang , Bingbing Yuan , Q. Jason Niu
The construction of functionalized interlayers has been identified as a highly effective strategy for the regulation of interfacial polymerization (IP) and the enhancement of the performance of thin-film composite (TFC) reverse osmosis (RO) membranes. However, most hydrophilic interlayers reported to date, although capable of improving monomer wetting and loading, tend to suppress the formation of the characteristic ridge-valley morphology, thereby reducing the effective mass-transfer area and ultimately limiting further enhancements in water permeability. Herein, a heterogeneous covalent organic framework (COF)/metal-organic framework (MOF) interlayer was constructed in situ on the surface of a polysulfone (PSF) support layer, in which an ultrathin COF layer was formed via sulfonic-acid-containing Pa-SO3H and 2,4,6-triformylphloroglucinol to repair defects in the substrate. A ZIF-8 layer was subsequently grown in situ using the sulfonic acid groups on the COF as anchoring sites. Experimental results demonstrate that the COF/MOF interlayer structure significantly enhances the adsorption capacity of amine monomers and modulates their diffusion behavior, leading to a more pronounced leaf-like surface morphology, an optimized active-layer thickness, and an enhanced hydrophilicity of the polyamide (PA) layer. The i-TFCC/M-T membrane, based on the rigid trimesoyl chloride monomer, exhibits a water permeance of approximately 5.20 L m−2 h−1 bar−1, which is about 2.2 times higher than that of the control group, while maintaining a NaCl rejection of approximately 99.10%. The novel interlayer design was also proven to be suitable for the flexible cyclohexane-1,3,5-tricarbonyl trichloride system. This study demonstrates that the COF/MOF heterogeneous interlayer can shift the performance balance point of RO membrane flux without significantly compromising ion exclusion, thereby providing a general and effective strategy for designing high-performance aromatic PA RO membranes for brackish water desalination.
功能化中间层的构建是调控界面聚合（IP）和提高薄膜复合（TFC）反渗透（RO）膜性能的有效策略。然而，迄今为止报道的大多数亲水中间层虽然能够改善单体润湿和负载，但往往会抑制特征脊-谷形态的形成，从而减少有效传质面积，最终限制了透水性的进一步增强。本文在聚砜（PSF）支撑层表面原位构建了非均相共价有机骨架(COF)/金属有机骨架（MOF）中间层，通过含磺酸的Pa-SO3H和2,4,6-三甲酰间苯三酚形成超薄的COF层来修复底物中的缺陷。随后使用COF上的磺酸基作为锚定位点原位生长ZIF-8层。实验结果表明，COF/MOF层间结构显著增强了胺类单体的吸附能力，调节了它们的扩散行为，使聚酰胺（PA）层具有更明显的叶状表面形态，优化了活性层厚度，增强了亲水性。基于刚性三甲基氯单体的i-TFCC/ m - t膜的透水性约为5.20 L m−2 h−1 bar−1，是对照组的2.2倍，同时保持约99.10%的NaCl去除率。这种新型中间层设计也被证明适用于柔性环己烷-1,3,5-三氯化三羰基体系。本研究表明，COF/MOF非均相中间层可以改变反渗透膜通量的性能平衡点，而不会显著影响离子的排除，从而为设计用于微咸水淡化的高性能芳香PA反渗透膜提供了一种通用而有效的策略。
{"title":"In situ growth of a COF/MOF heterogeneous interlayer for high-performance reverse osmosis membranes","authors":"Siheng Zhao , Xiaoqi Ma , Shengchao Zhao , Kuo Chen , Jianquan Peng , Zilong Huang , Bingbing Yuan , Q. Jason Niu","doi":"10.1016/j.memsci.2026.125269","DOIUrl":"10.1016/j.memsci.2026.125269","url":null,"abstract":"<div><div>The construction of functionalized interlayers has been identified as a highly effective strategy for the regulation of interfacial polymerization (IP) and the enhancement of the performance of thin-film composite (TFC) reverse osmosis (RO) membranes. However, most hydrophilic interlayers reported to date, although capable of improving monomer wetting and loading, tend to suppress the formation of the characteristic ridge-valley morphology, thereby reducing the effective mass-transfer area and ultimately limiting further enhancements in water permeability. Herein, a heterogeneous covalent organic framework (COF)/metal-organic framework (MOF) interlayer was constructed in situ on the surface of a polysulfone (PSF) support layer, in which an ultrathin COF layer was formed via sulfonic-acid-containing Pa-SO<sub>3</sub>H and 2,4,6-triformylphloroglucinol to repair defects in the substrate. A ZIF-8 layer was subsequently grown in situ using the sulfonic acid groups on the COF as anchoring sites. Experimental results demonstrate that the COF/MOF interlayer structure significantly enhances the adsorption capacity of amine monomers and modulates their diffusion behavior, leading to a more pronounced leaf-like surface morphology, an optimized active-layer thickness, and an enhanced hydrophilicity of the polyamide (PA) layer. The i-TFC<sub>C/M-T</sub> membrane, based on the rigid trimesoyl chloride monomer, exhibits a water permeance of approximately 5.20 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup>, which is about 2.2 times higher than that of the control group, while maintaining a NaCl rejection of approximately 99.10%. The novel interlayer design was also proven to be suitable for the flexible cyclohexane-1,3,5-tricarbonyl trichloride system. This study demonstrates that the COF/MOF heterogeneous interlayer can shift the performance balance point of RO membrane flux without significantly compromising ion exclusion, thereby providing a general and effective strategy for designing high-performance aromatic PA RO membranes for brackish water desalination.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"745 ","pages":"Article 125269"},"PeriodicalIF":9.0,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146172381","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}
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