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Enantiomeric separation of chiral hyper-crosslinked polymer based nanotube membranes
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-22 DOI: 10.1016/j.memsci.2025.124016
Rutong Zhang, Fang Wang, Meng Li, Wenhui Gong, Qibin Chen
The separation of racemic mixtures remains a great challenge due to the similar physicochemical properties of enantiomers in an achiral environment. Currently, membrane-based separations often face a trade-off between permeability and enantioselectivity. In this study, a uniquely fibrous nanotube membrane, derived from a chiral hyper-crosslinked polymer (CHCP), was constructed and used to separate racemates, motivated by the need for more efficient and scalable separation methods. The results show that such the CHCP-based nanotube membrane exhibits a 2–4 orders of magnitude increase in flux compared to conventional chiral separation membranes and a ca. one order of magnitude improvement relative to GO-based membranes, while maintaining the superior enantioselectivity. This can be attributed to the CHCP-based nanotube that is rich in the micropore and mesopore, thereby resulting in the ultimate membrane that is characteristic of the hierarchically porous structure and the high porosity. Moreover, this membrane displays a great stability, which offers a significant potential for scalable and continuous operations. Experimental studies, combined with density functional theory calculations, substantiate that this membrane follows the retarded transport mechanism, having a great promise in resolving the inherent trade-off. Our findings suggest that this CHCP-based nanotube can find applications in various fields, e.g., separation, catalysis, etc., due to its intrinsic porosity, good processability and ease of synthesis and modifiability.
{"title":"Enantiomeric separation of chiral hyper-crosslinked polymer based nanotube membranes","authors":"Rutong Zhang,&nbsp;Fang Wang,&nbsp;Meng Li,&nbsp;Wenhui Gong,&nbsp;Qibin Chen","doi":"10.1016/j.memsci.2025.124016","DOIUrl":"10.1016/j.memsci.2025.124016","url":null,"abstract":"<div><div>The separation of racemic mixtures remains a great challenge due to the similar physicochemical properties of enantiomers in an achiral environment. Currently, membrane-based separations often face a trade-off between permeability and enantioselectivity. In this study, a uniquely fibrous nanotube membrane, derived from a chiral hyper-crosslinked polymer (CHCP), was constructed and used to separate racemates, motivated by the need for more efficient and scalable separation methods. The results show that such the CHCP-based nanotube membrane exhibits a 2–4 orders of magnitude increase in flux compared to conventional chiral separation membranes and a ca. one order of magnitude improvement relative to GO-based membranes, while maintaining the superior enantioselectivity. This can be attributed to the CHCP-based nanotube that is rich in the micropore and mesopore, thereby resulting in the ultimate membrane that is characteristic of the hierarchically porous structure and the high porosity. Moreover, this membrane displays a great stability, which offers a significant potential for scalable and continuous operations. Experimental studies, combined with density functional theory calculations, substantiate that this membrane follows the retarded transport mechanism, having a great promise in resolving the inherent trade-off. Our findings suggest that this CHCP-based nanotube can find applications in various fields, e.g., separation, catalysis, etc., due to its intrinsic porosity, good processability and ease of synthesis and modifiability.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"725 ","pages":"Article 124016"},"PeriodicalIF":8.4,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143684850","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}
引用次数: 0
Crosslinking PDADMAC/PSS polyelectrolyte multilayer membranes for stability at high salinity 交联 PDADMAC/PSS 聚电解质多层膜,实现高盐度下的稳定性
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-22 DOI: 10.1016/j.memsci.2025.124007
Xiao Zhang , Antoine J.B. Kemperman , Henk Miedema , Esra te Brinke , Wiebe M. de Vos
Polyelectrolyte multilayer (PEM) nanofiltration (NF) membranes based on PDADMAC (poly(diallyldimethylammoniumchloride)) and PSS (poly(sodium 4-styrenesulfonate)) are known for their high physical and chemical stability. However, under high salinity conditions, the stability of these membranes is compromised due to weakened electrostatic interactions, leading to increased permeability and decreased retention. This study addresses this challenge by crosslinking PDADMAC/PSS multilayers with the photosensitive, negatively charged crosslinker DAS (disodium 4,4’-diazidostilbene-2,2’-disulfonate tetrahydrate). Initially, this crosslinking is studied on model surfaces, demonstrating full stability against desorption by surfactants at high enough DAS concentrations (1 g·L-1) and at long enough UV exposure (10 minutes). Experiments on PEM membranes demonstrate that DAS crosslinking significantly enhanced the stability of PDADMAC/PSS membranes at high salinity, with no permeability increase or loss of selectivity observed up to 1.5 M NaCl, in contrast to non-crosslinked membranes showing a reversible 61% permeability increase and an irreversible loss in MgSO4 retention of 15%. At 4 M NaCl, the permeability of non-crosslinked membranes increased by 300% versus 90% for crosslinked membranes, again indicating the improved stability of the latter. Crosslinking with DAS further allows tuning of the membrane properties, denser membranes are formed with a lower molecular weight cut-off (MWCO), from around 861 Da of non-crosslinked membranes to around 354 Da of membranes crosslinked with a low DAS concentration (1 g·L-1). DAS introduces negative charges (sulfonic acid groups) into the PEMs, changing the membrane charge from positive to highly negative, as evidenced by the high Na2SO4 retention (∼95%) and low CaCl2 retention (∼7%) of crosslinked membranes. This study demonstrates the potential of crosslinking with DAS to produce stable PDADMAC/PSS NF membranes with tunable selectivity for challenging separation processes in high-salinity environments.
{"title":"Crosslinking PDADMAC/PSS polyelectrolyte multilayer membranes for stability at high salinity","authors":"Xiao Zhang ,&nbsp;Antoine J.B. Kemperman ,&nbsp;Henk Miedema ,&nbsp;Esra te Brinke ,&nbsp;Wiebe M. de Vos","doi":"10.1016/j.memsci.2025.124007","DOIUrl":"10.1016/j.memsci.2025.124007","url":null,"abstract":"<div><div>Polyelectrolyte multilayer (PEM) nanofiltration (NF) membranes based on PDADMAC (poly(diallyldimethylammoniumchloride)) and PSS (poly(sodium 4-styrenesulfonate)) are known for their high physical and chemical stability. However, under high salinity conditions, the stability of these membranes is compromised due to weakened electrostatic interactions, leading to increased permeability and decreased retention. This study addresses this challenge by crosslinking PDADMAC/PSS multilayers with the photosensitive, negatively charged crosslinker DAS (disodium 4,4’-diazidostilbene-2,2’-disulfonate tetrahydrate). Initially, this crosslinking is studied on model surfaces, demonstrating full stability against desorption by surfactants at high enough DAS concentrations (1 g·L<sup>-1</sup>) and at long enough UV exposure (10 minutes). Experiments on PEM membranes demonstrate that DAS crosslinking significantly enhanced the stability of PDADMAC/PSS membranes at high salinity, with no permeability increase or loss of selectivity observed up to 1.5 M NaCl, in contrast to non-crosslinked membranes showing a reversible 61% permeability increase and an irreversible loss in MgSO<sub>4</sub> retention of 15%. At 4 M NaCl, the permeability of non-crosslinked membranes increased by 300% versus 90% for crosslinked membranes, again indicating the improved stability of the latter. Crosslinking with DAS further allows tuning of the membrane properties, denser membranes are formed with a lower molecular weight cut-off (MWCO), from around 861 Da of non-crosslinked membranes to around 354 Da of membranes crosslinked with a low DAS concentration (1 g·L<sup>-1</sup>). DAS introduces negative charges (sulfonic acid groups) into the PEMs, changing the membrane charge from positive to highly negative, as evidenced by the high Na<sub>2</sub>SO<sub>4</sub> retention (∼95%) and low CaCl<sub>2</sub> retention (∼7%) of crosslinked membranes. This study demonstrates the potential of crosslinking with DAS to produce stable PDADMAC/PSS NF membranes with tunable selectivity for challenging separation processes in high-salinity environments.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"725 ","pages":"Article 124007"},"PeriodicalIF":8.4,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143687886","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
“One tube killing two birds”: Simultaneously boosting the separation and mechanical performances of block copolymer membranes by sparsely doping carbon nanotubes
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-22 DOI: 10.1016/j.memsci.2025.124019
Xiang Ying , Shoutian Qiu , Zhuo Li , Lei Wang , Kang Zhou , Xiangyue Ye , Jiemei Zhou , Sheng Cui , Yong Wang
Selective swelling of block copolymers as an emerging process to prepare ultrafiltration membranes is receiving growing interests. Herein, we report that very little dosages of carbon nanotubes (CNTs) are able to significantly enhance both the separation and mechanical performances of melt-spun polysulfone-block-poly(ethylene glycol) (PSF-b-PEG) hollow-fiber membranes. CNTs are adequately dispersed in the block copolymer by melt processing, and exhibit π–π interaction to the PSF continuous phase but repulsion to the PEG dispersed phase. The incompatibility between CNTs and PEG leads to interfacial gaps between CNTs and the PEG phase, thus providing another set of pores facilitating water permeance. Both dosages and aspects of CNTs significantly influence the pore structure and performances of the membranes. Higher dosages of CNTs produce more interfacial gaps and lead to increased porosity and permeance. While CNTs with lower aspects tend to be distributed in the PSF phase, thus producing smaller pores and decreasing permeance by refraining selective swelling to a larger degree. The hollow-fiber membrane doped with 0.01 wt% CNTs having a diameter of ∼10–20 nm and a length of ∼50 μm shows a water permeance increased by three times and a rejection increased by 1.6 times. Moreover, thus-doped membrane exhibits over 1.5 times increase both in tensile stress and the strain at break and multiple times increase in swing tolerance. Such an extremely low dosage of CNTs synchronously boosting membrane permeance, rejection, and mechanical properties is highly desired in practical applications and is expected to be extended in the performance-upgrading of other membranes with multiphases.
{"title":"“One tube killing two birds”: Simultaneously boosting the separation and mechanical performances of block copolymer membranes by sparsely doping carbon nanotubes","authors":"Xiang Ying ,&nbsp;Shoutian Qiu ,&nbsp;Zhuo Li ,&nbsp;Lei Wang ,&nbsp;Kang Zhou ,&nbsp;Xiangyue Ye ,&nbsp;Jiemei Zhou ,&nbsp;Sheng Cui ,&nbsp;Yong Wang","doi":"10.1016/j.memsci.2025.124019","DOIUrl":"10.1016/j.memsci.2025.124019","url":null,"abstract":"<div><div>Selective swelling of block copolymers as an emerging process to prepare ultrafiltration membranes is receiving growing interests. Herein, we report that very little dosages of carbon nanotubes (CNTs) are able to significantly enhance both the separation and mechanical performances of melt-spun polysulfone-<em>block</em>-poly(ethylene glycol) (PSF-<em>b</em>-PEG) hollow-fiber membranes. CNTs are adequately dispersed in the block copolymer by melt processing, and exhibit π–π interaction to the PSF continuous phase but repulsion to the PEG dispersed phase. The incompatibility between CNTs and PEG leads to interfacial gaps between CNTs and the PEG phase, thus providing another set of pores facilitating water permeance. Both dosages and aspects of CNTs significantly influence the pore structure and performances of the membranes. Higher dosages of CNTs produce more interfacial gaps and lead to increased porosity and permeance. While CNTs with lower aspects tend to be distributed in the PSF phase, thus producing smaller pores and decreasing permeance by refraining selective swelling to a larger degree. The hollow-fiber membrane doped with 0.01 wt% CNTs having a diameter of ∼10–20 nm and a length of ∼50 μm shows a water permeance increased by three times and a rejection increased by 1.6 times. Moreover, thus-doped membrane exhibits over 1.5 times increase both in tensile stress and the strain at break and multiple times increase in swing tolerance. Such an extremely low dosage of CNTs synchronously boosting membrane permeance, rejection, and mechanical properties is highly desired in practical applications and is expected to be extended in the performance-upgrading of other membranes with multiphases.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"725 ","pages":"Article 124019"},"PeriodicalIF":8.4,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143715941","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}
引用次数: 0
Revealing the internal β-phase PVDF membrane fouling tendency using double layer piezoelectrics
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-22 DOI: 10.1016/j.memsci.2025.124017
Qian Wang , Juan Li , Qiuyueming Zhou , Ting He , Zhaoliang Cui , Young Moo Lee , Weihong Xing
Dissolved organic matter (DOM) is recognized as a crucial factor contributing to the irreversible fouling of ultrafiltration membranes. Quartz crystal microbalance with dissipation (QCM-D) offers insights into the kinetics of fouling layer formation and its structure in-situ on a model membrane. However, a clear correlation between the membrane fouling process and the adsorption-desorption results obtained from QCM-D has yet to be established. In this study, piezoelectric β-phase PVDF membranes were prepared, and their fouling behavior in response to three model compounds (humic acid (HA), dextran (DEX), bovine serum albumin (BSA), and their mixed solutions was examined. It was firstly proposed that the spin-coated model PVDF membrane surface exhibited a typical β-phase structure, characterized by regular undulations resulting from strong stretching effects. A novel double layer piezoelectric sensor, consisting of a β-phase layer over a piezoelectric quartz substrate, was designed for QCM-D analysis to assess the mass and stiffness variations of the absorbed DOM layer. The fouling tendency followed the order of BSA > Mixture > DEX > HA, with the foulant monomeric units having a similar molecular mass of around tens of kDa. Irreversible fouling resistance in series model as well as frequency drop in QCM-D were listed as indicators of irreversible fouling caused by foulant-membrane interaction, which realized a well-defined match for the first time.
{"title":"Revealing the internal β-phase PVDF membrane fouling tendency using double layer piezoelectrics","authors":"Qian Wang ,&nbsp;Juan Li ,&nbsp;Qiuyueming Zhou ,&nbsp;Ting He ,&nbsp;Zhaoliang Cui ,&nbsp;Young Moo Lee ,&nbsp;Weihong Xing","doi":"10.1016/j.memsci.2025.124017","DOIUrl":"10.1016/j.memsci.2025.124017","url":null,"abstract":"<div><div>Dissolved organic matter (DOM) is recognized as a crucial factor contributing to the irreversible fouling of ultrafiltration membranes. Quartz crystal microbalance with dissipation (QCM-D) offers insights into the kinetics of fouling layer formation and its structure in-situ on a model membrane. However, a clear correlation between the membrane fouling process and the adsorption-desorption results obtained from QCM-D has yet to be established. In this study, piezoelectric β-phase PVDF membranes were prepared, and their fouling behavior in response to three model compounds (humic acid (HA), dextran (DEX), bovine serum albumin (BSA), and their mixed solutions was examined. It was firstly proposed that the spin-coated model PVDF membrane surface exhibited a typical β-phase structure, characterized by regular undulations resulting from strong stretching effects. A novel double layer piezoelectric sensor, consisting of a β-phase layer over a piezoelectric quartz substrate, was designed for QCM-D analysis to assess the mass and stiffness variations of the absorbed DOM layer. The fouling tendency followed the order of BSA &gt; Mixture &gt; DEX &gt; HA, with the foulant monomeric units having a similar molecular mass of around tens of kDa. Irreversible fouling resistance in series model as well as frequency drop in QCM-D were listed as indicators of irreversible fouling caused by foulant-membrane interaction, which realized a well-defined match for the first time.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"724 ","pages":"Article 124017"},"PeriodicalIF":8.4,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143681843","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}
引用次数: 0
Solvent-assisted insertion of molecular supports for enhanced separation performance and stability of thin film composite reverse osmosis membranes
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-21 DOI: 10.1016/j.memsci.2025.124005
Chia-Ming Chang , Qipeng Zhao , Shing Bor Chen
This study presents an innovative approach to enhance the separation performance and stability of thin-film composite (TFC) reverse osmosis (RO) membranes through post-treatment by inserting 15-crown-5 (CE15) as molecular supports, assisted by methanol. By varying the CE15 concentration (0–4 wt%), the physicochemical properties of the membranes can be regulated with significantly improved separation performance. Comprehensive characterizations reveal that an optimal CE15 concentration of 1 wt% increases the water permeance by 148 % (from 1.86 to 4.61 LMH bar−1) while maintaining a high salt rejection of 98.9 %. Additionally, the chelation of CE15 with Li+ or Na+ further enhances the membrane's structural robustness, ensuring long-term stability. Over a 72-h period, the treated membranes exhibit only a 3.4 % reduction in water permeance, compared to a 15.8 % decline observed for the untreated membranes. This facile post-treatment method offers a scalable and effective solution to improve the permeability, selectivity, and durability of TFC membranes, presenting a promising advancement for desalination and water treatment applications.
{"title":"Solvent-assisted insertion of molecular supports for enhanced separation performance and stability of thin film composite reverse osmosis membranes","authors":"Chia-Ming Chang ,&nbsp;Qipeng Zhao ,&nbsp;Shing Bor Chen","doi":"10.1016/j.memsci.2025.124005","DOIUrl":"10.1016/j.memsci.2025.124005","url":null,"abstract":"<div><div>This study presents an innovative approach to enhance the separation performance and stability of thin-film composite (TFC) reverse osmosis (RO) membranes through post-treatment by inserting 15-crown-5 (CE15) as molecular supports, assisted by methanol. By varying the CE15 concentration (0–4 wt%), the physicochemical properties of the membranes can be regulated with significantly improved separation performance. Comprehensive characterizations reveal that an optimal CE15 concentration of 1 wt% increases the water permeance by 148 % (from 1.86 to 4.61 LMH bar<sup>−1</sup>) while maintaining a high salt rejection of 98.9 %. Additionally, the chelation of CE15 with Li<sup>+</sup> or Na<sup>+</sup> further enhances the membrane's structural robustness, ensuring long-term stability. Over a 72-h period, the treated membranes exhibit only a 3.4 % reduction in water permeance, compared to a 15.8 % decline observed for the untreated membranes. This facile post-treatment method offers a scalable and effective solution to improve the permeability, selectivity, and durability of TFC membranes, presenting a promising advancement for desalination and water treatment applications.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"725 ","pages":"Article 124005"},"PeriodicalIF":8.4,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143684925","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The complex influence of membrane roughness on colloidal fouling: A dialectical perspective 膜粗糙度对胶体堵塞的复杂影响:辩证的视角
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-21 DOI: 10.1016/j.memsci.2025.124014
Dongsheng Zhao , Linchun Chen , Mingxin Peng , Bingchao Xue , Zhikan Yao , Weiwei Huang , Zhihong Wang , Junxia Liu
Roughness is a key feature of membrane surface topography, yet its impact on fouling remains unclear. Herein, we present a coupled collision attachment-wettability framework to investigate the impact of membrane roughness on fouling from a dialectical perspective. Our findings show that for hydrophilic membranes, increasing surface roughness enhances the interfacial hydration repulsion barrier, reducing fouling. In contrast, for hydrophobic membranes, rougher surfaces lower the interfacial energy barrier, increasing fouling. The effect of roughness is also influenced by the membrane's intrinsic contact angle (θ0), initial water flux (J0), and solution ionic strength (Is). Membranes with lower θ0 maintain higher stable flux, even when smooth, while fouling resistance for higher θ0 membranes depends more on surface roughness. At lower J0 or Is, flux remains relatively stable with slight/mild reductions, due to reduced permeate drag or enhanced electrostatic repulsion. In contrast, severe fouling occurs under high J0 or Is, irrespective of surface roughness. Our simulations reveal the various mechanisms (i.e., hydration repulsion, permeate drag, and electrostatic interactions) that govern the role of surface roughness in fouling, providing valuable implications for membrane design, operational optimization, and feedwater pretreatment.
{"title":"The complex influence of membrane roughness on colloidal fouling: A dialectical perspective","authors":"Dongsheng Zhao ,&nbsp;Linchun Chen ,&nbsp;Mingxin Peng ,&nbsp;Bingchao Xue ,&nbsp;Zhikan Yao ,&nbsp;Weiwei Huang ,&nbsp;Zhihong Wang ,&nbsp;Junxia Liu","doi":"10.1016/j.memsci.2025.124014","DOIUrl":"10.1016/j.memsci.2025.124014","url":null,"abstract":"<div><div>Roughness is a key feature of membrane surface topography, yet its impact on fouling remains unclear. Herein, we present a coupled collision attachment-wettability framework to investigate the impact of membrane roughness on fouling from a dialectical perspective. Our findings show that for hydrophilic membranes, increasing surface roughness enhances the interfacial hydration repulsion barrier, reducing fouling. In contrast, for hydrophobic membranes, rougher surfaces lower the interfacial energy barrier, increasing fouling. The effect of roughness is also influenced by the membrane's intrinsic contact angle (<em>θ</em><sub>0</sub>), initial water flux (<em>J</em><sub>0</sub>), and solution ionic strength (<em>I</em><sub><em>s</em></sub>). Membranes with lower <em>θ</em><sub>0</sub> maintain higher stable flux, even when smooth, while fouling resistance for higher <em>θ</em><sub>0</sub> membranes depends more on surface roughness. At lower <em>J</em><sub>0</sub> or <em>I</em><sub><em>s</em></sub>, flux remains relatively stable with slight/mild reductions, due to reduced permeate drag or enhanced electrostatic repulsion. In contrast, severe fouling occurs under high <em>J</em><sub>0</sub> or <em>I</em><sub><em>s</em></sub>, irrespective of surface roughness. Our simulations reveal the various mechanisms (i.e., hydration repulsion, permeate drag, and electrostatic interactions) that govern the role of surface roughness in fouling, providing valuable implications for membrane design, operational optimization, and feedwater pretreatment.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"725 ","pages":"Article 124014"},"PeriodicalIF":8.4,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143687888","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}
引用次数: 0
Enhanced xylose/salt separation of nanofiltration membrane via a CTAB-assisted shedding strategy toward polyamide oligomers
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-21 DOI: 10.1016/j.memsci.2025.124013
Rongze Sun, Jianlong Dai, Danrong Cai, Wentao Yan, Yong Zhou, Congjie Gao
Xylose is a small organic molecule with great economic value in fine chemical production. High-quality xylose production requires removing salt from the feed solution, which is typically an expensive process. Polyamide nanofiltration membranes, characterized by their high rejection of salts (e.g., Na2SO4) and low rejection of small organic molecules (such as xylose), are an effective separation technique. The present study proposes a CTAB-assisted shedding strategy toward polyamide oligomers to enhance the xylose/salt separation. When the membrane contacts CTAB solution at appropriate concentrations, CTAB aggregates adsorb onto the membrane surface due to electrostatic and hydrophobic interactions. The hydrophilic outer layer of these aggregates, attributed to the quaternary ammonium groups, facilitates the migration of polyamide oligomers into the solution, increasing membrane pore size and thereby decreasing xylose rejection. This mild process preserves the membrane structure and its strong negative charge, maintaining effective charge repulsion and ensuring high salt rejection. The increased pore size also enhances membrane flux. Results show that xylose rejection decreased from 44.2 % to 20.3 %, while Na2SO4 rejection remained above 98 %. The separation factor increased by 117 %, and flux increased by 104 %. Investigation of the shedding mechanism revealed that the variation of membrane flux with CTAB concentration aligns with the S-shaped adsorption isotherm model of surfactants at the solid-liquid interface. This suggests that the adsorption form of CTAB on the membrane surface is the dominant factor influencing this process. This work shows the promising potential of polyamide nanofiltration membrane technique for the xylose purification and the proposed strategy in small organic molecule/salt separation.
{"title":"Enhanced xylose/salt separation of nanofiltration membrane via a CTAB-assisted shedding strategy toward polyamide oligomers","authors":"Rongze Sun,&nbsp;Jianlong Dai,&nbsp;Danrong Cai,&nbsp;Wentao Yan,&nbsp;Yong Zhou,&nbsp;Congjie Gao","doi":"10.1016/j.memsci.2025.124013","DOIUrl":"10.1016/j.memsci.2025.124013","url":null,"abstract":"<div><div>Xylose is a small organic molecule with great economic value in fine chemical production. High-quality xylose production requires removing salt from the feed solution, which is typically an expensive process. Polyamide nanofiltration membranes, characterized by their high rejection of salts (e.g., Na<sub>2</sub>SO<sub>4</sub>) and low rejection of small organic molecules (such as xylose), are an effective separation technique. The present study proposes a CTAB-assisted shedding strategy toward polyamide oligomers to enhance the xylose/salt separation. When the membrane contacts CTAB solution at appropriate concentrations, CTAB aggregates adsorb onto the membrane surface due to electrostatic and hydrophobic interactions. The hydrophilic outer layer of these aggregates, attributed to the quaternary ammonium groups, facilitates the migration of polyamide oligomers into the solution, increasing membrane pore size and thereby decreasing xylose rejection. This mild process preserves the membrane structure and its strong negative charge, maintaining effective charge repulsion and ensuring high salt rejection. The increased pore size also enhances membrane flux. Results show that xylose rejection decreased from 44.2 % to 20.3 %, while Na<sub>2</sub>SO<sub>4</sub> rejection remained above 98 %. The separation factor increased by 117 %, and flux increased by 104 %. Investigation of the shedding mechanism revealed that the variation of membrane flux with CTAB concentration aligns with the S-shaped adsorption isotherm model of surfactants at the solid-liquid interface. This suggests that the adsorption form of CTAB on the membrane surface is the dominant factor influencing this process. This work shows the promising potential of polyamide nanofiltration membrane technique for the xylose purification and the proposed strategy in small organic molecule/salt separation.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"725 ","pages":"Article 124013"},"PeriodicalIF":8.4,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143715939","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}
引用次数: 0
In-situ cross-linking and shear-driven coating enable defect-free tubular ZIF-8 membranes toward efficient C3H6/C3H8 separation
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-20 DOI: 10.1016/j.memsci.2025.124010
Luogang Wu , Jingxian Hua , Yawei Gu, Jian Sun, Qian Wang, Lixiong Zhang, Haiqian Lian, Yichang Pan
Eliminating potential defects is crucial for making tubular ZIF-8 (T-ZIF-8) membranes widely adopted in chemical process industries. However, the geometric restriction of the inner T-ZIF-8 membrane and the high viscosity of cross-linked PDMS solution pose challenges in uniform polymer deposition and interfacial adhesion that traditional dip-coating methods may not effectively address. Herein, we propose an in-situ cross-linking and rolling coating (ISCL&RC) strategy to overcome these challenges. During the rolling coating process, the PDMS solution gradually solidifies on the surface of the T-ZIF-8 membrane under the shear force induced by gravity, forming a PDMS coating with uniform thickness. The in-situ cross-linking allows the low-viscosity PDMS solution to adequately infiltrate the surface of the T-ZIF-8 membrane, forming a desirable interface. Compared with the pristine T-ZIF-8 membrane, the T-ZIF-8/PDMS membrane demonstrates remarkable improvement in C3H6/C3H8 separation selectivity (2.6–18.5 times higher than the unmodified membrane), while the C3H6 permeance remains nearly unchanged. Notably, the T-ZIF-8/PDMS membrane sustains coating integrity under high pressure and industrial raw gas for 780 h without exhibiting bubbling or delamination. This work establishes a paradigm for defect engineering in confined tubular membrane systems, effectively bridging the gap between laboratory-scale synthesis and industrial module fabrication.
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引用次数: 0
High-performance graphene oxide / sodium alginate composite membrane for marine osmotic energy conversion
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-20 DOI: 10.1016/j.memsci.2025.123987
Tao Liu , Suan Huang , Weiwen Xin , Xiaohan He , Shicheng Wan , Chaowen Yang , Juncheng Zhao , Liuyong Shi , Hong Yan , Teng Zhou , Liping Wen
With advancements in Reverse Electrodialysis (RED) technology, an increasing number of high-power-density permeable membranes have been proposed for salinity gradient power generation. Two-dimensional (2D) materials, characterized by their abundant surface charges, can form nanochannels with high surface charge density during the stacking process to achieve exceptional ion selectivity. Additionally, the stacked structure aids in creating a highly porous permeable membrane surface, facilitating substantial ion flux during ion transport. Consequently, permeable membranes composed of 2D materials such as graphene oxide (GO) and MXenes exhibit particularly outstanding performance in the field of salinity gradient power generation. In this context, we designed an ion-selective composite membrane formed by the mixed crosslinking of graphene oxide and sodium alginate. The composite membrane utilizes stacked graphene oxide nanosheets to provide a two-dimensional layered framework, while sodium alginate, rich in negatively charged functional groups, crosslinks between the nanosheets to create abundant spatial charge, significantly enhancing the power density for salinity gradient power generation. This composite membrane exhibits a power density of approximately 14.75 W/m2 under a 50-fold NaCl solution salinity gradient, and an astonishing 20.94 W/m2 under a 50-fold KCl solution salinity gradient. In real seawater, it also achieves a high power density of 19.39 W/m2, far exceeding the industry benchmark of 5.0 W/m2 and outperforming most existing materials. These results are expected to promote the practical application of marine salinity gradient energy and provide new design strategies for the development of marine salinity gradient resources.
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引用次数: 0
Ultra-thin, scalable, and MOF network-reinforced composite solid electrolyte for all-solid-state lithium metal batteries
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-20 DOI: 10.1016/j.memsci.2025.124009
Guoxu Wang , Xiaomeng Fan , Fanfan Liu , Shoujiang Li , Wei Ding , Xiaoyan Liu , Chengbiao Wei , Feng Lin , Li-Zhen Fan
Ultra-thin, scalable solid-state electrolytes with high mechanical strength are essential for achieving high-performance all-solid-state lithium metal batteries (ASSLMBs). Among various types of solid-state electrolytes, composite solid electrolytes (CSEs) have emerged as an appealing option due to their ability to overcome the limitations of single-component solid-state electrolytes. In this study, ZIF-67 metal-organic framework (MOF) nanoparticles were self-assembled in situ on polyimide (PI) film fibers (referred to as PI@ZIF-67) to create continuous Li+ transport channels. The ultra-thin, robust PI fiber film combined with MOF particles imparts high mechanical strength and excellent flexibility to the CSE. Additionally, the abundant sub-nanopores and surface Lewis acidic sites in ZIF-67 nanoparticles facilitate the dissociation of lithium salts and enhance the rapid transport of Li+. Consequently, 95 % of the discharge capacity retention of the all-solid-state Li/PI60@ZIF-67-PEO/LFP cell was maintained after 300 cycles at 0.2C and 60 °C. Furthermore, an ultra-long lifespan of 3500 h at 0.2 mA cm−2 and 0.2 mAh cm−2 was achieved for the symmetric Li/PI60@ZIF-67-PEO/Li cell. The superior electrochemical performances are attributed to the effective Li+ transport network and the high mechanical properties established by the continuous ZIF-67 particles within the PI60@ZIF-67-PEO CSE. This work presents a promising method for the integrated design of ultrathin CSEs that exhibit high ionic conductivity and exceptional mechanical robustness, making them suitable for ASSLMBs.
{"title":"Ultra-thin, scalable, and MOF network-reinforced composite solid electrolyte for all-solid-state lithium metal batteries","authors":"Guoxu Wang ,&nbsp;Xiaomeng Fan ,&nbsp;Fanfan Liu ,&nbsp;Shoujiang Li ,&nbsp;Wei Ding ,&nbsp;Xiaoyan Liu ,&nbsp;Chengbiao Wei ,&nbsp;Feng Lin ,&nbsp;Li-Zhen Fan","doi":"10.1016/j.memsci.2025.124009","DOIUrl":"10.1016/j.memsci.2025.124009","url":null,"abstract":"<div><div>Ultra-thin, scalable solid-state electrolytes with high mechanical strength are essential for achieving high-performance all-solid-state lithium metal batteries (ASSLMBs). Among various types of solid-state electrolytes, composite solid electrolytes (CSEs) have emerged as an appealing option due to their ability to overcome the limitations of single-component solid-state electrolytes. In this study, ZIF-67 metal-organic framework (MOF) nanoparticles were self-assembled in situ on polyimide (PI) film fibers (referred to as PI@ZIF-67) to create continuous Li<sup>+</sup> transport channels. The ultra-thin, robust PI fiber film combined with MOF particles imparts high mechanical strength and excellent flexibility to the CSE. Additionally, the abundant sub-nanopores and surface Lewis acidic sites in ZIF-67 nanoparticles facilitate the dissociation of lithium salts and enhance the rapid transport of Li<sup>+</sup>. Consequently, 95 % of the discharge capacity retention of the all-solid-state Li/PI<sub>60</sub>@ZIF-67-PEO/LFP cell was maintained after 300 cycles at 0.2C and 60 °C. Furthermore, an ultra-long lifespan of 3500 h at 0.2 mA cm<sup>−2</sup> and 0.2 mAh cm<sup>−2</sup> was achieved for the symmetric Li/PI<sub>60</sub>@ZIF-67-PEO/Li cell. The superior electrochemical performances are attributed to the effective Li<sup>+</sup> transport network and the high mechanical properties established by the continuous ZIF-67 particles within the PI<sub>60</sub>@ZIF-67-PEO CSE. This work presents a promising method for the integrated design of ultrathin CSEs that exhibit high ionic conductivity and exceptional mechanical robustness, making them suitable for ASSLMBs.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"724 ","pages":"Article 124009"},"PeriodicalIF":8.4,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143681795","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}
引用次数: 0
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Journal of Membrane Science
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