Pub Date : 2026-01-12DOI: 10.1016/j.memsci.2026.125155
Zhongrui Lu, Zhuoran Yang, Xiaohang Li, Zhengwei Chang, Xiaoyang Jia, Shaojian He , Jun Lin
Cerium compounds are extensively utilized to enhance the chemical stability of proton exchange membranes (PEMs) due to their efficient scavenging of free radicals; however, cerium ions can reduce the proton conductivity of PEMs and can migrate out of PEMs. In this work, we synthesized a novel compound, cerium phosphotungstate (CeHPW), which effectively reduces the solubility of Ce ions while simultaneously enhancing the proton conductivity of PEMs. Moreover, quercetin was employed to anchor Ce ions further, thereby obtaining water-insoluble QCeHPW. QCeHPW exhibits superior free radical scavenging ability compared to either CeO2 or quercetin alone. Furthermore, the proton conductivity of sulfonated poly(ether ether ketone) (SPEEK) composite membrane containing 7.5 wt% QCeHPW in liquid water at 25 °C was 0.052 S cm−1, which represents a 53 % improvement over the SPEEK control membrane (0.034 S cm−1). The single-cell performance of this membrane is significantly better than that of SPEEK control membrane. In addition, compared to SPEEK membranes doped with quercetin or CeO2, the decay rate of the open-circuit voltage (OCV) for this membrane is lower.
铈化合物由于能有效清除自由基而被广泛用于提高质子交换膜的化学稳定性；然而，铈离子会降低PEMs的质子电导率，并会向外迁移。在这项工作中，我们合成了一种新的化合物，磷钨酸铈（CeHPW），它有效地降低了Ce离子的溶解度，同时提高了PEMs的质子电导率。此外，槲皮素进一步锚定Ce离子，得到不溶于水的QCeHPW。与单独使用CeO2或槲皮素相比，QCeHPW具有更强的自由基清除能力。此外，含有7.5 wt% QCeHPW的磺化聚醚醚酮（SPEEK）复合膜在25°C的液态水中的质子电导率为0.052 S cm - 1，比SPEEK对照膜（0.034 S cm - 1）提高了53%。该膜的单细胞性能明显优于SPEEK对照膜。此外，与槲皮素或CeO2掺杂的SPEEK膜相比，该膜的开路电压（OCV）衰减率更低。
{"title":"Using quercetin to anchor a novel Ce-doped acid to enhance the performance and chemical stability of proton exchange membranes","authors":"Zhongrui Lu, Zhuoran Yang, Xiaohang Li, Zhengwei Chang, Xiaoyang Jia, Shaojian He , Jun Lin","doi":"10.1016/j.memsci.2026.125155","DOIUrl":"10.1016/j.memsci.2026.125155","url":null,"abstract":"<div><div>Cerium compounds are extensively utilized to enhance the chemical stability of proton exchange membranes (PEMs) due to their efficient scavenging of free radicals; however, cerium ions can reduce the proton conductivity of PEMs and can migrate out of PEMs. In this work, we synthesized a novel compound, cerium phosphotungstate (CeHPW), which effectively reduces the solubility of Ce ions while simultaneously enhancing the proton conductivity of PEMs. Moreover, quercetin was employed to anchor Ce ions further, thereby obtaining water-insoluble QCeHPW. QCeHPW exhibits superior free radical scavenging ability compared to either CeO<sub>2</sub> or quercetin alone. Furthermore, the proton conductivity of sulfonated poly(ether ether ketone) (SPEEK) composite membrane containing 7.5 wt% QCeHPW in liquid water at 25 °C was 0.052 S cm<sup>−1</sup>, which represents a 53 % improvement over the SPEEK control membrane (0.034 S cm<sup>−1</sup>). The single-cell performance of this membrane is significantly better than that of SPEEK control membrane. In addition, compared to SPEEK membranes doped with quercetin or CeO<sub>2</sub>, the decay rate of the open-circuit voltage (OCV) for this membrane is lower.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125155"},"PeriodicalIF":9.0,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974004","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 : 2026-01-12DOI: 10.1016/j.memsci.2026.125156
Pengda Sun , Kai Hang , Zitong Huang , Zixuan Miao , Hao Li , Yiliang Guo , Jinhua Ji , Shaojie Liu , Xiaomeng Chu , Erjun Tang , Nanwen Li
Alkaline water electrolysis (AWE) requires separators with high ionic conductivity to ensure high efficiency in hydrogen production. While naphthyl-based polybenzimidazole (NPBI) ion-solvating membranes exhibit excellent alkaline stability, their dense morphologies limit electrolyte uptake and hydroxide conductivity. To overcome this limitation, we developed a hydrogel-reinforced NPBI composite membrane (NPBI-PAM-x) through in-situ thermal-induced free radical polymerization of acrylamide within NPBI polymer matrix. The resulting membranes featured with an asymmetric dual-layer architecture, where a porous polyacrylamide (PAM) hydrogel facilitated KOH absorption and ion transport, while a dense NPBI layer provided mechanical integrity and gas barrier properties. This unique structure enabled the NPBI-PAM-1.5 membrane to achieve a hydroxide conductivity of 163.7 mS cm−1 in 6 M KOH at 80 °C, which was substantially higher than that of pristine NPBI (118.9 mS cm−1), while also exhibiting controlled swelling and low gas permeability. NPBI-PAM-1.5 retained 90.1 % of its initial conductivity following a demanding 3200 h alkaline stability test in 6 M KOH at 80 °C. This result demonstrated the NPBI-PAM-x membrane materials’ excellent resistance to chemical degradation. In a single zero-gap alkaline water electrolyzer at 80 °C, the NPBI-PAM-1.5 membrane achieved a current density of 1.41 A cm−2 at 2.0 V using non-precious metal electrodes, and the current density increased to 1.65 A cm−2 at 90 °C. Furthermore, the single AWE device operated stably for 428 h at 500 mA cm−2 and 80 °C. This work demonstrates that incorporating a hydrophilic hydrogel into a chemically stable NPBI polymer matrix is an effective strategy to enhance the performance of NPBI-based ion-solvating membranes for AWE, offering a practical approach to advance green hydrogen production.
碱性电解（AWE）需要具有高离子电导率的分离器，以确保高效制氢。虽然萘基多苯并咪唑（NPBI）离子溶剂化膜具有优异的碱性稳定性，但其致密的形态限制了电解质的吸收和氢氧化物的导电性。为了克服这一限制，我们在NPBI聚合物基体中通过原位热诱导自由基聚合丙烯酰胺，开发了一种水凝胶增强NPBI复合膜（NPBI- pam -x）。所得膜具有不对称双层结构，其中多孔聚丙烯酰胺（PAM）水凝胶促进KOH吸收和离子传输，而致密的NPBI层具有机械完整性和气体屏障性能。这种独特的结构使NPBI- pam -1.5膜在80°C下，在6 M KOH条件下的氢氧化物电导率达到163.7 mS cm -1，大大高于原始NPBI (118.9 mS cm -1)，同时还表现出可控的膨胀和低透气性。NPBI-PAM-1.5在80°C、6m KOH条件下进行3200h碱性稳定性测试后，其初始电导率仍保持90.1%。这一结果证明了NPBI-PAM-x膜材料具有优异的耐化学降解性能。在80℃的单一零间隙碱水电解槽中，采用非贵金属电极制备的NPBI-PAM-1.5膜在2.0 V时电流密度达到1.41 a cm - 2，在90℃时电流密度提高到1.65 a cm - 2。此外，单个AWE装置在500 mA cm−2和80°C下稳定运行428 h。该研究表明，在化学稳定的NPBI聚合物基体中加入亲水性水凝胶是提高NPBI基离子溶剂化膜的性能的有效策略，为推进绿色制氢提供了一种实用的方法。
{"title":"Hydrogel-reinforced naphthyl-based polybenzimidazole ion-solvating membranes for optimized performance of alkaline water electrolysis","authors":"Pengda Sun , Kai Hang , Zitong Huang , Zixuan Miao , Hao Li , Yiliang Guo , Jinhua Ji , Shaojie Liu , Xiaomeng Chu , Erjun Tang , Nanwen Li","doi":"10.1016/j.memsci.2026.125156","DOIUrl":"10.1016/j.memsci.2026.125156","url":null,"abstract":"<div><div>Alkaline water electrolysis (AWE) requires separators with high ionic conductivity to ensure high efficiency in hydrogen production. While naphthyl-based polybenzimidazole (NPBI) ion-solvating membranes exhibit excellent alkaline stability, their dense morphologies limit electrolyte uptake and hydroxide conductivity. To overcome this limitation, we developed a hydrogel-reinforced NPBI composite membrane (NPBI-PAM-x) through in-situ thermal-induced free radical polymerization of acrylamide within NPBI polymer matrix. The resulting membranes featured with an asymmetric dual-layer architecture, where a porous polyacrylamide (PAM) hydrogel facilitated KOH absorption and ion transport, while a dense NPBI layer provided mechanical integrity and gas barrier properties. This unique structure enabled the NPBI-PAM-1.5 membrane to achieve a hydroxide conductivity of 163.7 mS cm<sup>−1</sup> in 6 M KOH at 80 °C, which was substantially higher than that of pristine NPBI (118.9 mS cm<sup>−1</sup>), while also exhibiting controlled swelling and low gas permeability. NPBI-PAM-1.5 retained 90.1 % of its initial conductivity following a demanding 3200 h alkaline stability test in 6 M KOH at 80 °C. This result demonstrated the NPBI-PAM-x membrane materials’ excellent resistance to chemical degradation. In a single zero-gap alkaline water electrolyzer at 80 °C, the NPBI-PAM-1.5 membrane achieved a current density of 1.41 A cm<sup>−2</sup> at 2.0 V using non-precious metal electrodes, and the current density increased to 1.65 A cm<sup>−2</sup> at 90 °C. Furthermore, the single AWE device operated stably for 428 h at 500 mA cm<sup>−2</sup> and 80 °C. This work demonstrates that incorporating a hydrophilic hydrogel into a chemically stable NPBI polymer matrix is an effective strategy to enhance the performance of NPBI-based ion-solvating membranes for AWE, offering a practical approach to advance green hydrogen production.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125156"},"PeriodicalIF":9.0,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974094","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 : 2026-01-11DOI: 10.1016/j.memsci.2025.125096
Jannis M. Focke , Kai P. Barbian , Paul-Luca Bonke , Ulrich Steinseifer , Jutta Arens , Michael Neidlin
Severe lung diseases can be clinically treated with extracorporeal blood oxygenation (ECMO), where blood oxygenators exchange gases across thousands of hollow fiber membranes. However, their large surface area increases blood trauma and the risk of device failure. Understanding and improving gas transfer efficiency through computational models can help to reduce the required membrane surface area for the design of smaller and safer oxygenators. However, existing models either oversimplify local flow and gas exchange or rely on experimental calibration.
To address this gap, we developed a reduced order model (ROM) that predicts oxygen transfer in fiber bundles modeled as porous media, without requiring a priori experiments. The model provides locally resolved oxygen source terms that account for fiber configuration, Reynolds number, and oxygen concentration, and were derived from and fitted to data from in-vitro validated fiber-scale computational fluid dynamics (CFD) simulations (RMSE <0.01). The ROM predicted oxygen transfer of the validated simulations with high accuracy (R-squared = 0.995) and an overestimation of 6 %. When applied to a lab-scale oxygenator, the ROM accurately predicted total oxygen transfer with a relative error of 2.3 % compared to experimental results and provided spatially resolved oxygen concentration distributions within the fiber bundle.
We provide source term functions and coefficients for the four most common fiber configurations and a CFD implementation in a full-scale oxygenator for further use.
{"title":"A reduced order model for spatially resolved gas transfer prediction in full scale oxygenators","authors":"Jannis M. Focke , Kai P. Barbian , Paul-Luca Bonke , Ulrich Steinseifer , Jutta Arens , Michael Neidlin","doi":"10.1016/j.memsci.2025.125096","DOIUrl":"10.1016/j.memsci.2025.125096","url":null,"abstract":"<div><div>Severe lung diseases can be clinically treated with extracorporeal blood oxygenation (ECMO), where blood oxygenators exchange gases across thousands of hollow fiber membranes. However, their large surface area increases blood trauma and the risk of device failure. Understanding and improving gas transfer efficiency through computational models can help to reduce the required membrane surface area for the design of smaller and safer oxygenators. However, existing models either oversimplify local flow and gas exchange or rely on experimental calibration.</div><div>To address this gap, we developed a reduced order model (ROM) that predicts oxygen transfer in fiber bundles modeled as porous media, without requiring <em>a priori</em> experiments. The model provides locally resolved oxygen source terms that account for fiber configuration, Reynolds number, and oxygen concentration, and were derived from and fitted to data from <em>in-vitro</em> validated fiber-scale computational fluid dynamics (CFD) simulations (RMSE <0.01). The ROM predicted oxygen transfer of the validated simulations with high accuracy (R-squared = 0.995) and an overestimation of 6 %. When applied to a lab-scale oxygenator, the ROM accurately predicted total oxygen transfer with a relative error of 2.3 % compared to experimental results and provided spatially resolved oxygen concentration distributions within the fiber bundle.</div><div>We provide source term functions and coefficients for the four most common fiber configurations and a CFD implementation in a full-scale oxygenator for further use.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125096"},"PeriodicalIF":9.0,"publicationDate":"2026-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974189","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 : 2026-01-11DOI: 10.1016/j.memsci.2026.125154
Yuting Yang , Subo Xu , Yao Jiang , Weilong Song , Pin Zhao , Xinhua Wang
The pervasive environmental presence and recalcitrance of per- and polyfluoroalkyl substances (PFAS), particularly perfluorooctanoic acid (PFOA), necessitate the development of advanced water treatment technologies. Thin film composite nanofiltration (TFC-NF) membranes present a promising solution but are fundamentally constrained by the pervasive trade-off between permeability and selectivity. This study introduced a novel strategy to overcome this limitation by reconstructing the polyamide active layer with enhanced adsorption properties and a Turing structure. This was achieved via the synergistic co-introduction of the cationic surfactant cetylpyridinium bromide (CPB) and covalent organic frameworks (COFs), namely TpPa and F–COF, during the interfacial polymerization (IP) process. The optimized membrane demonstrated exceptional performance, achieving a PFOA rejection rate exceeding 99 % coupled with a high water permeance of 31.0 LMH·bar−1, significantly surpassing the performance of commercial benchmarks such as NF90 and other membranes reported in the literature. CPB suppressed piperazine (PIP) diffusion by ∼41.5 %, while COFs enriched PIP and then mitigated diffusion fluctuations, promoting the formation of a thinner, denser, and more selective polyamide layer. Moreover, the enhanced PFOA removal was attributed to synergistic mechanisms including size exclusion (from the narrowed pore size), Donnan exclusion, and specific adsorption via fluorine–fluorine interactions provided by the COFs. This work provides a facile and effective strategy for fabricating high-performance NF membranes by leveraging the synergistic effect of surfactants and COFs to tailor the IP process, offering significant potential for the efficient removal of persistent organic pollutants in real-world applications.
{"title":"Synergistic integration of cetylpyridinium bromide and covalent organic frameworks for Constructing Turing-type nanofiltration membranes with superior PFOA removal","authors":"Yuting Yang , Subo Xu , Yao Jiang , Weilong Song , Pin Zhao , Xinhua Wang","doi":"10.1016/j.memsci.2026.125154","DOIUrl":"10.1016/j.memsci.2026.125154","url":null,"abstract":"<div><div>The pervasive environmental presence and recalcitrance of per- and polyfluoroalkyl substances (PFAS), particularly perfluorooctanoic acid (PFOA), necessitate the development of advanced water treatment technologies. Thin film composite nanofiltration (TFC-NF) membranes present a promising solution but are fundamentally constrained by the pervasive trade-off between permeability and selectivity. This study introduced a novel strategy to overcome this limitation by reconstructing the polyamide active layer with enhanced adsorption properties and a Turing structure. This was achieved via the synergistic co-introduction of the cationic surfactant cetylpyridinium bromide (CPB) and covalent organic frameworks (COFs), namely TpPa and F–COF, during the interfacial polymerization (IP) process. The optimized membrane demonstrated exceptional performance, achieving a PFOA rejection rate exceeding 99 % coupled with a high water permeance of 31.0 LMH·bar<sup>−1</sup>, significantly surpassing the performance of commercial benchmarks such as NF90 and other membranes reported in the literature. CPB suppressed piperazine (PIP) diffusion by ∼41.5 %, while COFs enriched PIP and then mitigated diffusion fluctuations, promoting the formation of a thinner, denser, and more selective polyamide layer. Moreover, the enhanced PFOA removal was attributed to synergistic mechanisms including size exclusion (from the narrowed pore size), Donnan exclusion, and specific adsorption via fluorine–fluorine interactions provided by the COFs. This work provides a facile and effective strategy for fabricating high-performance NF membranes by leveraging the synergistic effect of surfactants and COFs to tailor the IP process, offering significant potential for the efficient removal of persistent organic pollutants in real-world applications.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125154"},"PeriodicalIF":9.0,"publicationDate":"2026-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974096","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 : 2026-01-11DOI: 10.1016/j.memsci.2026.125148
Ping Hu , Mengyang Yang , Zewen Xu , Songwei Han , Pengcheng Yuan , Xiaozhuan Zhang , Bingbing Yuan , Q. Jason Niu
The stoichiometric equilibrium and diffusion kinetics of reaction monomers govern the morphology and structure of polyamide membranes formed via interfacial polymerization (IP). Here, we report the construction of polyamide nanofilms with ultra-high stripe density through a phosphate-rich additive-modulated IP process.
Various characterizations and molecular dynamics simulations reveal that sodium hexametaphosphate (HMP)-mediated electrostatic attractions can spatially enrich piperazine (PIP) monomers while temporally fetter their diffusion, enabling the formation of a thin, highly cross-linked polyamide nanofilm with narrowed pore size distribution. The constrained diffusion accelerates the differential diffusion kinetics between PIP and trimesoyl chloride, inducing violent interfacial instability that leads to the emergency of high-density stripe architectures, substantially expanding filtration area and enhancing void fraction. The resulting membrane exhibits an exceptional water permeance of 33.43 ± 2.3 L m−2 h−1 bar−1, nearly 3.0-fold improvement over controlled membrane, coupled with significantly enhanced Cl−/SO42− selectivity and water/organic micropollutant selectivity, surpassing state-of-the-art benchmarks. Importantly, the engineered morphology confers a lower and more homogeneous local flux across the membrane surface, imparting superior antifouling property, and effectively overcoming the permeability-antifouling trade-off in advanced crumpled TFC membranes.
反应单体的化学计量平衡和扩散动力学决定了界面聚合形成的聚酰胺膜的形态和结构。在这里，我们报告了通过富磷酸盐添加剂调制的IP工艺构建具有超高条纹密度的聚酰胺纳米膜。各种表征和分子动力学模拟表明，六偏磷酸钠（HMP）介导的静电吸引可以在空间上富集哌嗪（PIP）单体，同时在时间上抑制它们的扩散，从而形成一种薄的、高度交联的、孔径分布狭窄的聚酰胺纳米膜。受约束的扩散加速了PIP和三甲酰氯之间的差异扩散动力学，引起剧烈的界面不稳定，导致高密度条纹结构的出现，大大扩大了过滤面积，提高了空隙率。该膜的透水性为33.43±2.3 L m−2 h−1 bar−1，比对照膜提高了近3.0倍，同时显著提高了Cl−/SO42−的选择性和水/有机微污染物的选择性，超过了最先进的基准。重要的是，这种工程形态赋予了膜表面更低、更均匀的局部通量，赋予了优越的防污性能，并有效地克服了高级皱褶TFC膜的渗透性和防污权衡。
{"title":"Polyamide nanofilms with ultra-high stripe density for enhanced anion sieving and organic micropollutants removal","authors":"Ping Hu , Mengyang Yang , Zewen Xu , Songwei Han , Pengcheng Yuan , Xiaozhuan Zhang , Bingbing Yuan , Q. Jason Niu","doi":"10.1016/j.memsci.2026.125148","DOIUrl":"10.1016/j.memsci.2026.125148","url":null,"abstract":"<div><div>The stoichiometric equilibrium and diffusion kinetics of reaction monomers govern the morphology and structure of polyamide membranes formed via interfacial polymerization (IP). Here, we report the construction of polyamide nanofilms with ultra-high stripe density through a phosphate-rich additive-modulated IP process.</div><div>Various characterizations and molecular dynamics simulations reveal that sodium hexametaphosphate (HMP)-mediated electrostatic attractions can spatially enrich piperazine (PIP) monomers while temporally fetter their diffusion, enabling the formation of a thin, highly cross-linked polyamide nanofilm with narrowed pore size distribution. The constrained diffusion accelerates the differential diffusion kinetics between PIP and trimesoyl chloride, inducing violent interfacial instability that leads to the emergency of high-density stripe architectures, substantially expanding filtration area and enhancing void fraction. The resulting membrane exhibits an exceptional water permeance of 33.43 ± 2.3 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup>, nearly 3.0-fold improvement over controlled membrane, coupled with significantly enhanced Cl<sup>−</sup>/SO<sub>4</sub><sup>2−</sup> selectivity and water/organic micropollutant selectivity, surpassing state-of-the-art benchmarks. Importantly, the engineered morphology confers a lower and more homogeneous local flux across the membrane surface, imparting superior antifouling property, and effectively overcoming the permeability-antifouling trade-off in advanced crumpled TFC membranes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125148"},"PeriodicalIF":9.0,"publicationDate":"2026-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974091","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 : 2026-01-11DOI: 10.1016/j.memsci.2026.125153
Inyoung Jang , Haoyu Chen , Ian S. Metcalfe , Ryan P. Lively
While membrane-based CO2 capture is a promising technology for separating CO2 from low-concentration environments such as air, it is generally more energy-intensive than alternative separation methods like adsorption. The uphill diffusion of CO2, driven by the dissipation of the chemical potential difference of water, can potentially reduce the energy demand of membrane-based CO2 capture from dilute sources. In this analysis, we explore the coupling between CO2 flux and H2O's chemical potential gradient, hypothesizing that dissipation of H2O chemical potential gradients and CO2-selective sorption enable CO2 transport against its concentration gradient and even its chemical potential gradient. Through Onsager analysis and second-law thermodynamic evaluations, we demonstrate the feasibility of this mechanism under steady-state conditions from multiple perspectives, considering various thermodynamic and transport aspects. We also highlight how the level of CO2 enrichment from the diluted feed to the more concentrated permeate depends on the fraction of water free energy utilized to drive uphill CO2 diffusion. This analysis aims to provide a foundation and identify key targets for developing membrane materials and processes that are designed to exploit this coupling phenomenon.
{"title":"Analysis of uphill diffusion of CO2 driven by the chemical potential difference of H2O","authors":"Inyoung Jang , Haoyu Chen , Ian S. Metcalfe , Ryan P. Lively","doi":"10.1016/j.memsci.2026.125153","DOIUrl":"10.1016/j.memsci.2026.125153","url":null,"abstract":"<div><div>While membrane-based CO<sub>2</sub> capture is a promising technology for separating CO<sub>2</sub> from low-concentration environments such as air, it is generally more energy-intensive than alternative separation methods like adsorption. The uphill diffusion of CO<sub>2,</sub> driven by the dissipation of the chemical potential difference of water, can potentially reduce the energy demand of membrane-based CO<sub>2</sub> capture from dilute sources. In this analysis, we explore the coupling between CO<sub>2</sub> flux and H<sub>2</sub>O's chemical potential gradient, hypothesizing that dissipation of H<sub>2</sub>O chemical potential gradients and CO<sub>2</sub>-selective sorption enable CO<sub>2</sub> transport against its concentration gradient and even its chemical potential gradient. Through Onsager analysis and second-law thermodynamic evaluations, we demonstrate the feasibility of this mechanism under steady-state conditions from multiple perspectives, considering various thermodynamic and transport aspects. We also highlight how the level of CO<sub>2</sub> enrichment from the diluted feed to the more concentrated permeate depends on the fraction of water free energy utilized to drive uphill CO<sub>2</sub> diffusion. This analysis aims to provide a foundation and identify key targets for developing membrane materials and processes that are designed to exploit this coupling phenomenon.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125153"},"PeriodicalIF":9.0,"publicationDate":"2026-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146035009","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 : 2026-01-10DOI: 10.1016/j.memsci.2026.125151
Shuhui Chen , Dan Zhao , Qingdi Mu , Lele Wang , Huiping Huang , Yongtao Qiu , Jizhong Ren
Gas separation membrane technology, as an effective means of carbon capture, utilization and storage (CCUS) technology, plays an important role in the field of CO2 emission reduction. A polyetheramine gelation strategy was proposed in this study to construct Pebax 30R51/MIL-101-(OH)2/M2070 (where M2070 was referred to Jeffamine®M − 2070) ternary gel-mixed matrix membranes (g-MMMs) for CO2 separation from light gases (H2, CH4, O2, and N2) and the morphology, microstructure, and thermal properties of g-MMMs were evaluated through a series of characterizations. The polyetheramine M2070 as a gelling agent alleviated the problems of MIL-101-(OH)2 agglomeration and polymer chain rigidity. At the same time, its ether oxygen enhanced CO2 solution and its soft chains promoted gas mass transfer due to its high fractional free volume (FFV). The CO2 permeability of g-MMMs with 60 wt% M2070 content increased to 473.2 Barrer (140 % higher than corresponding mixed matrix membranes (MMMs)) and its CO2/N2, CO2/O2, CO2/CH4, and CO2/H2 selectivities remained at 30.8, 13.4, 9.9, 8.0, respectively. The CO2/N2 separation performance of prepared g-MMMs was close to the Robeson upper bound (2008). This study provided a novel strategy for breaking through the performance bottleneck of traditional MMMs and contributed to the practical application of high-efficiency CO2 separation membranes.
{"title":"Design of Pebax-based gel-mixed matrix membranes for efficient CO2 separation using a polyetheramine gelation strategy","authors":"Shuhui Chen , Dan Zhao , Qingdi Mu , Lele Wang , Huiping Huang , Yongtao Qiu , Jizhong Ren","doi":"10.1016/j.memsci.2026.125151","DOIUrl":"10.1016/j.memsci.2026.125151","url":null,"abstract":"<div><div>Gas separation membrane technology, as an effective means of carbon capture, utilization and storage (CCUS) technology, plays an important role in the field of CO<sub>2</sub> emission reduction. A polyetheramine gelation strategy was proposed in this study to construct Pebax 30R51/MIL-101-(OH)<sub>2</sub>/M2070 (where M2070 was referred to Jeffamine®M − 2070) ternary <em>gel</em>-mixed matrix membranes (<em>g</em>-MMMs) for CO<sub>2</sub> separation from light gases (H<sub>2</sub>, CH<sub>4</sub>, O<sub>2</sub>, and N<sub>2</sub>) and the morphology, microstructure, and thermal properties of <em>g</em>-MMMs were evaluated through a series of characterizations. The polyetheramine M2070 as a gelling agent alleviated the problems of MIL-101-(OH)<sub>2</sub> agglomeration and polymer chain rigidity. At the same time, its ether oxygen enhanced CO<sub>2</sub> solution and its soft chains promoted gas mass transfer due to its high fractional free volume (<em>FFV)</em>. The CO<sub>2</sub> permeability of <em>g</em>-MMMs with 60 wt% M2070 content increased to 473.2 Barrer (140 % higher than corresponding mixed matrix membranes (MMMs)) and its CO<sub>2</sub>/N<sub>2</sub>, CO<sub>2</sub>/O<sub>2</sub>, CO<sub>2</sub>/CH<sub>4</sub>, and CO<sub>2</sub>/H<sub>2</sub> selectivities remained at 30.8, 13.4, 9.9, 8.0, respectively. The CO<sub>2</sub>/N<sub>2</sub> separation performance of prepared <em>g</em>-MMMs was close to the Robeson upper bound (2008). This study provided a novel strategy for breaking through the performance bottleneck of traditional MMMs and contributed to the practical application of high-efficiency CO<sub>2</sub> separation membranes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125151"},"PeriodicalIF":9.0,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146035007","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 : 2026-01-09DOI: 10.1016/j.memsci.2026.125147
Guijing Chen , Zhaoyang Song , Xiaoqi Wang , Shengchi Bai , Yi Deng , Quanxun Liang , Songmiao Liang , Alberto Tiraferri , Baicang Liu
New nanofiltration membrane with larger volume output is one of the key parameters for selection in drinking water treatment applications. Moreover, evaluating the separation performance of NF membranes is crucial for ensuring the continued safety of effluent water quality when responding to sudden changes in water quality. In this study, the melamine, a highly reactive monomer containing a triazine ring, participates in the interfacial polymerization reaction between the piperazine and 1,3,5-benzenetricarbonyl trichloride, thus providing an opportunity to tune the polyamide layer properties. The reaction with melamine changes the structural parameters and decrease the diffusion rate of piperazine, while introducing more intermolecular hydrogen bonds in new hybrid polyamide layer compared to the conventional polyamide layer. These strong intermolecular hydrogen bonds are crucial for enabling high Na2SO4 rejection in melamine-modified membranes. This strategy resulted in membrane permeance of 2.5 times that of commercial membranes (VNF1 and NF270) and unmodified membrane in a complex mixed salts solution, with Cl−/SO42‒ selectivity factor increasing form 7.5 to 44.6. Furthermore, the new membrane can remove most dissolved substances from ultrafiltration effluent in treating drinking water source (Hulukou Reservoir) impacted by sudden shale gas wastewater spill, ensuring the safety of the treated water. The purified water quality parameters are inferior to those of the VNF1 and NF270 membranes, but slightly superior to the unmodified membrane. However, water recovery experiments revealed that all membranes suffered from severe scaling issues. Overall, the results suggest that melamine may be utilized to tune the performance of nanofiltration membrane through the scalable one-step polymerization procedure, providing an effective strategy for preparing high-performance membranes.
{"title":"Enhancing nanofiltration membranes performance by melamine modification for emergency treating deteriorated water quality in drinking water source","authors":"Guijing Chen , Zhaoyang Song , Xiaoqi Wang , Shengchi Bai , Yi Deng , Quanxun Liang , Songmiao Liang , Alberto Tiraferri , Baicang Liu","doi":"10.1016/j.memsci.2026.125147","DOIUrl":"10.1016/j.memsci.2026.125147","url":null,"abstract":"<div><div>New nanofiltration membrane with larger volume output is one of the key parameters for selection in drinking water treatment applications. Moreover, evaluating the separation performance of NF membranes is crucial for ensuring the continued safety of effluent water quality when responding to sudden changes in water quality. In this study, the melamine, a highly reactive monomer containing a triazine ring, participates in the interfacial polymerization reaction between the piperazine and 1,3,5-benzenetricarbonyl trichloride, thus providing an opportunity to tune the polyamide layer properties. The reaction with melamine changes the structural parameters and decrease the diffusion rate of piperazine, while introducing more intermolecular hydrogen bonds in new hybrid polyamide layer compared to the conventional polyamide layer. These strong intermolecular hydrogen bonds are crucial for enabling high Na<sub>2</sub>SO<sub>4</sub> rejection in melamine-modified membranes. This strategy resulted in membrane permeance of 2.5 times that of commercial membranes (VNF1 and NF270) and unmodified membrane in a complex mixed salts solution, with Cl<sup>−</sup>/SO<sub>4</sub><sup>2‒</sup> selectivity factor increasing form 7.5 to 44.6. Furthermore, the new membrane can remove most dissolved substances from ultrafiltration effluent in treating drinking water source (Hulukou Reservoir) impacted by sudden shale gas wastewater spill, ensuring the safety of the treated water. The purified water quality parameters are inferior to those of the VNF1 and NF270 membranes, but slightly superior to the unmodified membrane. However, water recovery experiments revealed that all membranes suffered from severe scaling issues. Overall, the results suggest that melamine may be utilized to tune the performance of nanofiltration membrane through the scalable one-step polymerization procedure, providing an effective strategy for preparing high-performance membranes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125147"},"PeriodicalIF":9.0,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974090","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 : 2026-01-09DOI: 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":"2026-01-09","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 : 2026-01-09DOI: 10.1016/j.memsci.2026.125149
Chunjia Wang , Yanan Liu , Xiaocui Wei , Fu Zhao , Tingyuan Wang , Enshen Shi , Yigui Du , Fenglong Dai , Shijie Liu , Chunyang Fan , Yuhan Wang , Zhongyi Jiang
Polyamide (PA) reverse osmosis thin-film composite (RO TFC) membranes constructed via interfacial polymerization (IP) process have been extensively employed in seawater desalination, and the crosslinking degree and thickness of PA layer play crucial role on their practical performance. Herein, an in-situ surface segregation strategy was adopted to fabricate hydrophilic and porous substrate with dopamine (DA) as surface segregation agent, thereby effectively regulating the IP process for enhanced desalination. During substrate fabrication process, DA self-polymerized to generate polydopamine (PDA), subsequently PDA segregated into surface, which could enrich amine monomers in the aqueous phase and slow their diffusion toward the organic phase, through hydrogen bonding and π-π interactions between PDA and amine monomers. Accordingly, the crosslinking degree increased from 79.1 % to 89.9 %, particularly improving boric acid rejection from 71.3 % to 88.9 %. Meanwhile, the thickness of PA layer decreased to 48.0 nm. The optimized membrane exhibited a water permeability of 1.91 L m−2 h−1 bar−1 and NaCl rejection of 99.9 %, while maintaining excellent stability over 100 h of continuous operation. Furthermore, the membrane showed outstanding desalination performance for real seawater, demonstrating that fabricating substrate through surface segregation method offered an efficient and easy pathway for high-performance RO membranes.
通过界面聚合（IP）工艺构建的聚酰胺（PA）反渗透薄膜复合膜（RO TFC）在海水淡化中得到了广泛应用，其交联度和厚度对其使用性能起着至关重要的作用。本文采用原位表面分离策略，以多巴胺（DA）为表面分离剂制备亲水性多孔底物，从而有效调节IP过程，增强海水淡化。在底物制备过程中，DA自聚合生成聚多巴胺（PDA），随后PDA分离到表面，通过PDA与胺单体之间的氢键和π-π相互作用富集水相中的胺单体，减缓其向有机相的扩散。交联度由79.1%提高到89.9%，硼酸去除率由71.3%提高到88.9%。同时，PA层厚度减小至48.0 nm。优化后的膜的透水性为1.91 L m−2 h−1 bar−1，NaCl去除率为99.9%，并且在连续运行100 h内保持良好的稳定性。此外，该膜对真实海水表现出优异的脱盐性能，表明通过表面分离法制备底物为制备高性能反渗透膜提供了一条高效、简便的途径。
{"title":"Enhanced performance of polyamide membrane through hydrophilic and porous substrate fabricated by surface segregation method","authors":"Chunjia Wang , Yanan Liu , Xiaocui Wei , Fu Zhao , Tingyuan Wang , Enshen Shi , Yigui Du , Fenglong Dai , Shijie Liu , Chunyang Fan , Yuhan Wang , Zhongyi Jiang","doi":"10.1016/j.memsci.2026.125149","DOIUrl":"10.1016/j.memsci.2026.125149","url":null,"abstract":"<div><div>Polyamide (PA) reverse osmosis thin-film composite (RO TFC) membranes constructed via interfacial polymerization (IP) process have been extensively employed in seawater desalination, and the crosslinking degree and thickness of PA layer play crucial role on their practical performance. Herein, an in-situ surface segregation strategy was adopted to fabricate hydrophilic and porous substrate with dopamine (DA) as surface segregation agent, thereby effectively regulating the IP process for enhanced desalination. During substrate fabrication process, DA self-polymerized to generate polydopamine (PDA), subsequently PDA segregated into surface, which could enrich amine monomers in the aqueous phase and slow their diffusion toward the organic phase, through hydrogen bonding and π-π interactions between PDA and amine monomers. Accordingly, the crosslinking degree increased from 79.1 % to 89.9 %, particularly improving boric acid rejection from 71.3 % to 88.9 %. Meanwhile, the thickness of PA layer decreased to 48.0 nm. The optimized membrane exhibited a water permeability of 1.91 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup> and NaCl rejection of 99.9 %, while maintaining excellent stability over 100 h of continuous operation. Furthermore, the membrane showed outstanding desalination performance for real seawater, demonstrating that fabricating substrate through surface segregation method offered an efficient and easy pathway for high-performance RO membranes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"742 ","pages":"Article 125149"},"PeriodicalIF":9.0,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974088","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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