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Electrically induced modulation of pore size and surface potential in conductive nanofiltration membranes for enhanced dye/salt selective separation
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-18 DOI: 10.1016/j.memsci.2025.123993
Jiajin Hao, Jingxian Li, Lei Wang, Miaolu He, Jin Wang, Xudong Wang, Xinyue Zhang, JunWei Xin
Precise modulation of the pore size sieving and electrostatic repulsion forces within nanofiltration membranes is crucial for achieving efficient dye desalination processes. This work presents a novel approach to enhance the dye desalination performance of nanofiltration membranes through electrical stimulation, fundamentally overcoming the current precision limitations in membrane material fabrication and modification. Specifically, polyaniline tetramer (AT) nanoparticles were incorporated into the interlayer channels of reduced graphene oxide (rGO) to fabricate a conductive nanofiltration membrane with electro-responsive characteristics for dynamic pore size and charge modulation. This membrane enables flexible modulation of the membrane pore size and charge through adjustment of the external voltage. Under a voltage of 2.5V, the membrane exhibits pronounced differences in the rejection for dyes and salts. Specifically, the separation factors for Congo red (CR)/Na2SO4 and CR/NaCl reach 231.4 and 245.2, respectively, whereas the flux increase by a factor of approximately 10.5 compared with that for an rGO membrane. This work contributes to a deeper understanding of engineering control of smart nanofiltration membranes and provides new insights into the design of separation mechanisms for dye desalting. These findings hold promising potential for applications in ion separation, material purification, and resource recovery, among other related fields.
{"title":"Electrically induced modulation of pore size and surface potential in conductive nanofiltration membranes for enhanced dye/salt selective separation","authors":"Jiajin Hao,&nbsp;Jingxian Li,&nbsp;Lei Wang,&nbsp;Miaolu He,&nbsp;Jin Wang,&nbsp;Xudong Wang,&nbsp;Xinyue Zhang,&nbsp;JunWei Xin","doi":"10.1016/j.memsci.2025.123993","DOIUrl":"10.1016/j.memsci.2025.123993","url":null,"abstract":"<div><div>Precise modulation of the pore size sieving and electrostatic repulsion forces within nanofiltration membranes is crucial for achieving efficient dye desalination processes. This work presents a novel approach to enhance the dye desalination performance of nanofiltration membranes through electrical stimulation, fundamentally overcoming the current precision limitations in membrane material fabrication and modification. Specifically, polyaniline tetramer (AT) nanoparticles were incorporated into the interlayer channels of reduced graphene oxide (rGO) to fabricate a conductive nanofiltration membrane with electro-responsive characteristics for dynamic pore size and charge modulation. This membrane enables flexible modulation of the membrane pore size and charge through adjustment of the external voltage. Under a voltage of 2.5V, the membrane exhibits pronounced differences in the rejection for dyes and salts. Specifically, the separation factors for Congo red (CR)/Na<sub>2</sub>SO<sub>4</sub> and CR/NaCl reach 231.4 and 245.2, respectively, whereas the flux increase by a factor of approximately 10.5 compared with that for an rGO membrane. This work contributes to a deeper understanding of engineering control of smart nanofiltration membranes and provides new insights into the design of separation mechanisms for dye desalting. These findings hold promising potential for applications in ion separation, material purification, and resource recovery, among other related fields.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"724 ","pages":"Article 123993"},"PeriodicalIF":8.4,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682464","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
Corrigendum to “Transport characterization and modelling of Donnan dialysis for ammonium recovery from aqueous solutions” [J. Membr. Sci. 674 (2023) 121496]
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-18 DOI: 10.1016/j.memsci.2025.123971
H.J. Zwijnenberg, A.A.E. Elozeiri , J. de Grooth, W.G.J. van der Meer, J.A. Wood
{"title":"Corrigendum to “Transport characterization and modelling of Donnan dialysis for ammonium recovery from aqueous solutions” [J. Membr. Sci. 674 (2023) 121496]","authors":"H.J. Zwijnenberg,&nbsp;A.A.E. Elozeiri ,&nbsp;J. de Grooth,&nbsp;W.G.J. van der Meer,&nbsp;J.A. Wood","doi":"10.1016/j.memsci.2025.123971","DOIUrl":"10.1016/j.memsci.2025.123971","url":null,"abstract":"","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"723 ","pages":"Article 123971"},"PeriodicalIF":8.4,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143686519","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
Anion-encapsulated porous liquids with ZIF-8 preferential adsorption for ultrahigh-performance separation of organic-organic mixtures
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-18 DOI: 10.1016/j.memsci.2025.123994
Xiao Xu , Yusak Hartanto , Gilles Van Eygen , Zirui He , Bart Van der Bruggen , Jie Zheng , Patricia Luis
Despite the growing interest in porous liquids, their potential for membrane-based liquid separations remains largely unexplored. Herein, we report an anion-encapsulated type III porous liquid developed by homogeneously dispersing ZIF-8 in the ionic liquid trihexyltetradecylphosphonium chloride ([P6,6,6,14][Cl]). Both experimental and computational studies confirm that the resulting ZIF-8/[P6,6,6,14][Cl] system exhibits high fluidity at room temperature due to the enhanced mobility of chloride ions within the ZIF-8 framework. When used as a selective component for the separation of challenging mixtures such as dimethyl carbonate and methanol, the membrane exhibits superior performance, with significantly higher selectivity and an order of magnitude higher permeance of dimethyl carbonate compared to previously reported membranes. This enhanced separation capability is attributed to the unique liquid properties of the porous liquid and the selective adsorption affinity of ZIF-8. These results highlight the promising role of type III porous liquids in facilitating efficient membrane separations.
{"title":"Anion-encapsulated porous liquids with ZIF-8 preferential adsorption for ultrahigh-performance separation of organic-organic mixtures","authors":"Xiao Xu ,&nbsp;Yusak Hartanto ,&nbsp;Gilles Van Eygen ,&nbsp;Zirui He ,&nbsp;Bart Van der Bruggen ,&nbsp;Jie Zheng ,&nbsp;Patricia Luis","doi":"10.1016/j.memsci.2025.123994","DOIUrl":"10.1016/j.memsci.2025.123994","url":null,"abstract":"<div><div>Despite the growing interest in porous liquids, their potential for membrane-based liquid separations remains largely unexplored. Herein, we report an anion-encapsulated type III porous liquid developed by homogeneously dispersing ZIF-8 in the ionic liquid trihexyltetradecylphosphonium chloride ([P<sub>6</sub>,<sub>6</sub>,<sub>6</sub>,<sub>14</sub>][Cl]). Both experimental and computational studies confirm that the resulting ZIF-8/[P<sub>6</sub>,<sub>6</sub>,<sub>6</sub>,<sub>14</sub>][Cl] system exhibits high fluidity at room temperature due to the enhanced mobility of chloride ions within the ZIF-8 framework. When used as a selective component for the separation of challenging mixtures such as dimethyl carbonate and methanol, the membrane exhibits superior performance, with significantly higher selectivity and an order of magnitude higher permeance of dimethyl carbonate compared to previously reported membranes. This enhanced separation capability is attributed to the unique liquid properties of the porous liquid and the selective adsorption affinity of ZIF-8. These results highlight the promising role of type III porous liquids in facilitating efficient membrane separations.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"725 ","pages":"Article 123994"},"PeriodicalIF":8.4,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143725836","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 synthesis of ultrathin MOF-808 membranes exhibiting superior antibiotic desalination
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-17 DOI: 10.1016/j.memsci.2025.123961
Mingming Wu , Kunpeng Yu , Jiahui Yan , Yumei Meng , Yanwei Sun , Taotao Ji , Chen Wang , Wenwen Dong , Yi Liu , Wenjing Hu , Yi Liu
Multi-scale structural optimization has been proven to significantly enhance separation performance of metal–organic framework (MOF) membranes. Aiming at high-efficiency antibiotic desalination, in this work, we developed an in situ modulation strategy to synthesize defect-rich ultrathin MOF-808 membrane on tubular substrate. Among various synthetic parameters, addition of trifluoroacetic acid (TFA) as competitive modulator not only enhanced missing-linker number within the framework but also facilitated heterogeneous nucleation, thus enabling precise control over the multi-scale structure of MOF-808 membrane. Obtained membrane achieved not only rejection rate as low as 8.9 % for NaCl but also near-complete rejection of diverse antibiotics (e.g., 100 % for Rifampicin and Bacitracin, 99.8 % for Berberine chloride, and 99.6 % for Tetracycline). Of particular note, our membrane exhibited excellent NaCl/antibiotic separation factor (SF) of 787 with high water flux of 11.95 L m−2 h−1, which far surpassed state-of-the-art MOF membranes as reported in the literature. Moreover, our membrane displayed excellent operation stability over 10-cycle continuous operation, demonstrating great promise for practical antibiotic desalination in pharmaceutical industry.
{"title":"In situ synthesis of ultrathin MOF-808 membranes exhibiting superior antibiotic desalination","authors":"Mingming Wu ,&nbsp;Kunpeng Yu ,&nbsp;Jiahui Yan ,&nbsp;Yumei Meng ,&nbsp;Yanwei Sun ,&nbsp;Taotao Ji ,&nbsp;Chen Wang ,&nbsp;Wenwen Dong ,&nbsp;Yi Liu ,&nbsp;Wenjing Hu ,&nbsp;Yi Liu","doi":"10.1016/j.memsci.2025.123961","DOIUrl":"10.1016/j.memsci.2025.123961","url":null,"abstract":"<div><div>Multi-scale structural optimization has been proven to significantly enhance separation performance of metal–organic framework (MOF) membranes. Aiming at high-efficiency antibiotic desalination, in this work, we developed an in situ modulation strategy to synthesize defect-rich ultrathin MOF-808 membrane on tubular substrate. Among various synthetic parameters, addition of trifluoroacetic acid (TFA) as competitive modulator not only enhanced missing-linker number within the framework but also facilitated heterogeneous nucleation, thus enabling precise control over the multi-scale structure of MOF-808 membrane. Obtained membrane achieved not only rejection rate as low as 8.9 % for NaCl but also near-complete rejection of diverse antibiotics (e.g., 100 % for Rifampicin and Bacitracin, 99.8 % for Berberine chloride, and 99.6 % for Tetracycline). Of particular note, our membrane exhibited excellent NaCl/antibiotic separation factor (SF) of 787 with high water flux of 11.95 L m<sup>−2</sup> h<sup>−1</sup>, which far surpassed state-of-the-art MOF membranes as reported in the literature. Moreover, our membrane displayed excellent operation stability over 10-cycle continuous operation, demonstrating great promise for practical antibiotic desalination in pharmaceutical industry.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"724 ","pages":"Article 123961"},"PeriodicalIF":8.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682395","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
Ionic liquid functionalized ZIF-8 modified PVDF nanofiber-based composite proton exchange membranes towards direct methanol fuel cells applications
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-17 DOI: 10.1016/j.memsci.2025.123990
Ning Liu , Jie Wang , Huiyu Yang , Fan Cheng , Shuguang Bi , Guoliang Liu , Ying Ou , Hai Liu , Chunli Gong
In order to improve the proton conductivity, CH3OH barrier performance and long-term durability of proton exchange membranes in direct methanol fuel cells (DMFCs), herein, a novel functional nanofiber substrate (IL-ZIF-8@PVDF) was prepared by in situ growing metal-organic framework (ZIF-8) on poly(vinylidene fluoride) (PVDF) nanofibers, followed by modification with ionic liquid (IL) containing sulfonic acid groups. PVDF nanofibers can provide flexible mechanical support for ZIF-8, thereby effectively solving the processing difficulties of ZIF-8 caused by its brittleness. Further IL modification of ZIF-8 can not only increase the compatibility between ZIF-8@PVDF and the filling polymer, but also utilize the continuous PVDF nanofiber network to establish long-distance continuous H+ transport pathways within the membrane. The as-prepared sulfonated poly (ether ether ketone) impregnated IL-ZIF-8@PVDF composite membrane showed a very high proton conductivity of 161.92 mS cm−1 (80 °C). Meanwhile, the presence of nanofiber backbone and ZIF-8 inside the membrane effectively limited the swelling and methanol permeation. The peak power density (PPD) of the DMFC output equipped with the membrane is up to 114.86 mW cm−2 (2 M methanol, 80 °C), 1.28 times that of the commercial Nafion 211. The durability test suggested that the composite membrane assembled DMFC possessed excellent open circuit voltage stability (only 6.3 % attenuation after 320 h of continuous testing). This work provides a new design idea for PEMs for DMFCs.
{"title":"Ionic liquid functionalized ZIF-8 modified PVDF nanofiber-based composite proton exchange membranes towards direct methanol fuel cells applications","authors":"Ning Liu ,&nbsp;Jie Wang ,&nbsp;Huiyu Yang ,&nbsp;Fan Cheng ,&nbsp;Shuguang Bi ,&nbsp;Guoliang Liu ,&nbsp;Ying Ou ,&nbsp;Hai Liu ,&nbsp;Chunli Gong","doi":"10.1016/j.memsci.2025.123990","DOIUrl":"10.1016/j.memsci.2025.123990","url":null,"abstract":"<div><div>In order to improve the proton conductivity, CH<sub>3</sub>OH barrier performance and long-term durability of proton exchange membranes in direct methanol fuel cells (DMFCs), herein, a novel functional nanofiber substrate (IL-ZIF-8@PVDF) was prepared by <em>in situ</em> growing metal-organic framework (ZIF-8) on poly(vinylidene fluoride) (PVDF) nanofibers, followed by modification with ionic liquid (IL) containing sulfonic acid groups. PVDF nanofibers can provide flexible mechanical support for ZIF-8, thereby effectively solving the processing difficulties of ZIF-8 caused by its brittleness. Further IL modification of ZIF-8 can not only increase the compatibility between ZIF-8@PVDF and the filling polymer, but also utilize the continuous PVDF nanofiber network to establish long-distance continuous H<sup>+</sup> transport pathways within the membrane. The as-prepared sulfonated poly (ether ether ketone) impregnated IL-ZIF-8@PVDF composite membrane showed a very high proton conductivity of 161.92 mS cm<sup>−1</sup> (80 °C). Meanwhile, the presence of nanofiber backbone and ZIF-8 inside the membrane effectively limited the swelling and methanol permeation. The peak power density (PPD) of the DMFC output equipped with the membrane is up to 114.86 mW cm<sup>−2</sup> (2 M methanol, 80 °C), 1.28 times that of the commercial Nafion 211. The durability test suggested that the composite membrane assembled DMFC possessed excellent open circuit voltage stability (only 6.3 % attenuation after 320 h of continuous testing). This work provides a new design idea for PEMs for DMFCs.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"724 ","pages":"Article 123990"},"PeriodicalIF":8.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143645057","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
Sustainable spray coating fabrication of acid-resistant polyamine nanofiltration membrane to separate heavy metal ions and treat acid wastewater
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-17 DOI: 10.1016/j.memsci.2025.123989
Kayode Hassan Lasisi , Baifu Tao , Shurui Shao , Maoyu Liu , Kaisong Zhang
The fabrication of a scalable and economic acid-resistant polyamine-based NF membrane by a spray coating polymerization-based technique for heavy metals removal and acid wastewater treatment is herein reported for the first time. The process was optimized to produce a well crosslinked selective layer network membrane (named SC-TFC-N) with controlled thickness of ∼75 nm and effective mean pore radius of ∼6.2 Å. Two membranes having similar chemical compositions, christened SC-TFC-R and DC-TFC-N were also developed by reverse interfacial polymerization (RIP) spray coating and conventional dip-coating IP techniques, respectively for comparison. All the fabricated membranes displayed high rejections to divalent cations such as MgCl2 (2000 ppm) reaching rejection up to 98.6 %, but the optimized SC-TFC-N membrane achieves a water permeance of 9.1 L m−2 h−1 bar−1, which was about 1.7 and 1.4 times that of SC-TFC-R and DC-TFC-N membranes, respectively. Specifically, the SC-TFC-N membrane exhibits great stability under high salt concentrations, continuous filtration performance, and excellent fouling resistance after five-filtration stages. Consequently, the membranes displayed over 90 % rejections of the heavy metal ions, in the order of Pb2+ > Zn2+ > Cu2+, and also exhibit excellent acid resistance by maintaining high divalent cations salt rejection performances after being subjected to different acidic conditions. In addition, density functional theory (DFT) calculations carried out proved the stability of the polyamine NF membrane against nucleophilic and electrophilic attacks. This work thus demonstrates an efficient and sustainable approach for producing NF membrane with good potential application in heavy metal ions removal and acid mine drainage wastewater treatment.
{"title":"Sustainable spray coating fabrication of acid-resistant polyamine nanofiltration membrane to separate heavy metal ions and treat acid wastewater","authors":"Kayode Hassan Lasisi ,&nbsp;Baifu Tao ,&nbsp;Shurui Shao ,&nbsp;Maoyu Liu ,&nbsp;Kaisong Zhang","doi":"10.1016/j.memsci.2025.123989","DOIUrl":"10.1016/j.memsci.2025.123989","url":null,"abstract":"<div><div>The fabrication of a scalable and economic acid-resistant polyamine-based NF membrane by a spray coating polymerization-based technique for heavy metals removal and acid wastewater treatment is herein reported for the first time. The process was optimized to produce a well crosslinked selective layer network membrane (named <em>S</em>C-TFC-N) with controlled thickness of ∼75 nm and effective mean pore radius of ∼6.2 Å. Two membranes having similar chemical compositions, christened <em>S</em>C-TFC-R and DC-TFC-N were also developed by reverse interfacial polymerization (RIP) spray coating and conventional dip-coating IP techniques, respectively for comparison. All the fabricated membranes displayed high rejections to divalent cations such as MgCl<sub>2</sub> (2000 ppm) reaching rejection up to 98.6 %, but the optimized <em>S</em>C-TFC-N membrane achieves a water permeance of 9.1 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup>, which was about 1.7 and 1.4 times that of <em>S</em>C-TFC-R and DC-TFC-N membranes, respectively. Specifically, the <em>S</em>C-TFC-N membrane exhibits great stability under high salt concentrations, continuous filtration performance, and excellent fouling resistance after five-filtration stages. Consequently, the membranes displayed over 90 % rejections of the heavy metal ions, in the order of Pb<sup>2+</sup> &gt; Zn<sup>2+</sup> &gt; Cu<sup>2+</sup>, and also exhibit excellent acid resistance by maintaining high divalent cations salt rejection performances after being subjected to different acidic conditions. In addition, density functional theory (DFT) calculations carried out proved the stability of the polyamine NF membrane against nucleophilic and electrophilic attacks. This work thus demonstrates an efficient and sustainable approach for producing NF membrane with good potential application in heavy metal ions removal and acid mine drainage wastewater treatment.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"724 ","pages":"Article 123989"},"PeriodicalIF":8.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682392","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
Molecular-level side chain engineering on comb-shaped sulfonated poly(ether ether ketone) equilibrium-modified atmosphere packaging membrane
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-17 DOI: 10.1016/j.memsci.2025.123982
Xiaojuan Zhang , Kexin Yang , Jiaqian Guo , Chang Yan , Xiaotong Zou , Changqing Fang
In the fabrication of equilibrium-modified atmosphere packaging (EMAP) membranes, precise control over the membrane properties can be achieved by manipulating their chemical and chain structures. This study synthesized four types of comb-shaped sulfonated poly(ether ether ketone) (SPEEK)-based EMAP membranes, incorporating tertiary amines, imidazole, dodecyl chains, and methoxy polyethylene glycol terminal pendants via a sulfonamide electrophilic substitution reaction. These functionalized pendants acted as “valves” to modulate the membrane properties, with the “valve” size controlled by the grafting degree of each substituent and its microstructures. Among these engineered membranes, the SPEEK-12C-25 membrane, with moderate 12-C side chains, exhibited the best overall performance. It demonstrated robust mechanical strength (tensile stress >218 MPa), controllable hydrophilicity and dimensional stability across temperatures, favorable visible light transmittance (T > 85 %), and UV shielding (SUVA > 84 %, SUVB > 99 %). Notably, the well-defined hydrophilic/hydrophobic microphase separation structure within its matrix (characteristic separation length (d) value of 2.94 nm) provided a second-phase selective gas transport pathway, optimizing gas permeability and the CO2/O2 separation coefficient (5.51). Furthermore, these features facilitated rapid air balance within the packaging and timely removal of moisture to prevent water vapor condensation, allowing the packaged cherry tomatoes to maintain 88.70 % of their weight, 53.10 % of firmness, 97.30 % of total soluble solids, and controllable levels of titratable acidity, phenolic, and flavonoids content. Evidently, understanding the underlying principles of molecular-level engineering for the SPEEK side chains is critical for designing EMAP materials with optimal overall performance.
{"title":"Molecular-level side chain engineering on comb-shaped sulfonated poly(ether ether ketone) equilibrium-modified atmosphere packaging membrane","authors":"Xiaojuan Zhang ,&nbsp;Kexin Yang ,&nbsp;Jiaqian Guo ,&nbsp;Chang Yan ,&nbsp;Xiaotong Zou ,&nbsp;Changqing Fang","doi":"10.1016/j.memsci.2025.123982","DOIUrl":"10.1016/j.memsci.2025.123982","url":null,"abstract":"<div><div>In the fabrication of equilibrium-modified atmosphere packaging (EMAP) membranes, precise control over the membrane properties can be achieved by manipulating their chemical and chain structures. This study synthesized four types of comb-shaped sulfonated poly(ether ether ketone) (SPEEK)-based EMAP membranes, incorporating tertiary amines, imidazole, dodecyl chains, and methoxy polyethylene glycol terminal pendants via a sulfonamide electrophilic substitution reaction. These functionalized pendants acted as “valves” to modulate the membrane properties, with the “valve” size controlled by the grafting degree of each substituent and its microstructures. Among these engineered membranes, the SPEEK-12C-25 membrane, with moderate 12-C side chains, exhibited the best overall performance. It demonstrated robust mechanical strength (tensile stress &gt;218 MPa), controllable hydrophilicity and dimensional stability across temperatures, favorable visible light transmittance (T &gt; 85 %), and UV shielding (S<sub>UVA</sub> &gt; 84 %, S<sub>UVB</sub> &gt; 99 %). Notably, the well-defined hydrophilic/hydrophobic microphase separation structure within its matrix (characteristic separation length (d) value of 2.94 nm) provided a second-phase selective gas transport pathway, optimizing gas permeability and the CO<sub>2</sub>/O<sub>2</sub> separation coefficient (5.51). Furthermore, these features facilitated rapid air balance within the packaging and timely removal of moisture to prevent water vapor condensation, allowing the packaged cherry tomatoes to maintain 88.70 % of their weight, 53.10 % of firmness, 97.30 % of total soluble solids, and controllable levels of titratable acidity, phenolic, and flavonoids content. Evidently, understanding the underlying principles of molecular-level engineering for the SPEEK side chains is critical for designing EMAP materials with optimal overall performance.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"724 ","pages":"Article 123982"},"PeriodicalIF":8.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682396","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
Anchored highly stable Fe–Mn bimetallic catalyst in Al2O3 ceramic membranes for boosting Oxone activation and efficient degradation of emerging micropollutants
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-17 DOI: 10.1016/j.memsci.2025.123988
Zhenkai Wang , Yifan Li , Yanfang Su , Sheng-Peng Sun , Xiaoning Wang , Zhangxiong Wu , Winston Duo Wu , Xiao Dong Chen
Catalytic membrane integrating membrane filtration and advanced oxidation in one single-step is promising in addressing emerging micropollutants issue in water, the challenges in catalytic activity and stability still limit their practical application. This study successfully anchored highly stable Fe–Mn bimetallic catalyst (FMBC) in Al2O3-based microfiltration and ultrafiltration ceramic membranes channel (named as FMBC@Al2O3-MF or UF) via a novel in situ fabrication strategy. Characterization results revealed that FMBC was anchored on the membrane channel wall of Al2O3-MF/UF, which enabled boosting Oxone activation to generate sulfate radical and hydroxyl radical at circumneutral pH (e.g., 7.0–9.0) and with great stability. Notably, FMBC@Al2O3-UF exhibited a remarkable activity and anti-interference capability in actual water matrices, which resulted in efficient degradation of emerging micropollutants such as carbamazepine, crotamiton, diethyltoluamide, gemfibrozil and ibuprofen in lake water and municipal wastewater treatment plant secondary effluent at environmentally relevant concentrations. Moreover, FMBC@Al2O3-MF/UF also displayed high cleaning efficiency toward natural organic matter (NOM) and effluent organic matter (EfOM) fouling via Oxone activation. Besides, the intermediates of carbamazepine degradation were identified, and most of them had decreased aquatic toxicity based on Ecological Structure Activity Relationship (ECOSAR) prediction. The high activity, stability and environmentally friendly property of the as-prepared FMBC@Al2O3-MF/UF make them promising application for advanced treatment of emerging micropollutants in water.
{"title":"Anchored highly stable Fe–Mn bimetallic catalyst in Al2O3 ceramic membranes for boosting Oxone activation and efficient degradation of emerging micropollutants","authors":"Zhenkai Wang ,&nbsp;Yifan Li ,&nbsp;Yanfang Su ,&nbsp;Sheng-Peng Sun ,&nbsp;Xiaoning Wang ,&nbsp;Zhangxiong Wu ,&nbsp;Winston Duo Wu ,&nbsp;Xiao Dong Chen","doi":"10.1016/j.memsci.2025.123988","DOIUrl":"10.1016/j.memsci.2025.123988","url":null,"abstract":"<div><div>Catalytic membrane integrating membrane filtration and advanced oxidation in one single-step is promising in addressing emerging micropollutants issue in water, the challenges in catalytic activity and stability still limit their practical application. This study successfully anchored highly stable Fe–Mn bimetallic catalyst (FMBC) in Al<sub>2</sub>O<sub>3</sub>-based microfiltration and ultrafiltration ceramic membranes channel (named as FMBC@Al<sub>2</sub>O<sub>3</sub>-MF or UF) via a novel in situ fabrication strategy. Characterization results revealed that FMBC was anchored on the membrane channel wall of Al<sub>2</sub>O<sub>3</sub>-MF/UF, which enabled boosting Oxone activation to generate sulfate radical and hydroxyl radical at circumneutral pH (e.g., 7.0–9.0) and with great stability. Notably, FMBC@Al<sub>2</sub>O<sub>3</sub>-UF exhibited a remarkable activity and anti-interference capability in actual water matrices, which resulted in efficient degradation of emerging micropollutants such as carbamazepine, crotamiton, diethyltoluamide, gemfibrozil and ibuprofen in lake water and municipal wastewater treatment plant secondary effluent at environmentally relevant concentrations. Moreover, FMBC@Al<sub>2</sub>O<sub>3</sub>-MF/UF also displayed high cleaning efficiency toward natural organic matter (NOM) and effluent organic matter (EfOM) fouling via Oxone activation. Besides, the intermediates of carbamazepine degradation were identified, and most of them had decreased aquatic toxicity based on Ecological Structure Activity Relationship (ECOSAR) prediction. The high activity, stability and environmentally friendly property of the as-prepared FMBC@Al<sub>2</sub>O<sub>3</sub>-MF/UF make them promising application for advanced treatment of emerging micropollutants in water.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"724 ","pages":"Article 123988"},"PeriodicalIF":8.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682397","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
Polyethylene Glycol Functionalized Alumina-Based Composite Membrane with High-performance for Alkaline Water Electrolysis
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-17 DOI: 10.1016/j.memsci.2025.123986
Jinyu Lu , Jian You , Ben Chang , Wei Wang , Yongzhao Li , Jiabin Lin , Xiangbo Luo , Huaiyin Chen , Yuekun Lai , Meihua Wu , Weilong Cai
Green hydrogen is currently the dominant trend in the evolution of hydrogen energy, producing almost no greenhouse gas emissions. Alkaline water electrolysis (AWE) is recognized as a leading and well-established technology for producing green hydrogen. However, safety hazards may occur during hydrogen production currently as defective commercial separate membranes used in the AWE process. Therefore, it is imperative to create a membrane characterized by low area resistance, high stability, and high bubble point pressure (BPP) to realize high-performance AWE. Herein, we synthesize alumina-based composite membranes with Y2O3-added and polyethylene glycol functionalized Al2O3 for AWE through a phase inversion method. The porous composite membrane exhibits excellent hydrophilicity, with a lower contact angle of approximately 55°. It also presents exceptional performance metrics, including a low area resistance of about 0.17 Ω cm2, an ultra-high BBP of approximately 4.4 bar, and excellent mechanical properties with a tensile strength of around 25 MPa. The membranes achieved a current density of up to 2.5 A cm-2 under 2.0 V voltage in a 30 wt% KOH solution at 80 °C by utilizing commercial catalysts. Notably, the composite membranes exhibited remarkable stability, maintaining operation for over 1200 hours at a 2.0 A cm-2 current density without any performance degradation at 80°C. Furthermore, this composite membrane possesses outstanding gas-barrier capability with H2 and O2 purity higher than 98.70% and 99.69%, respectively. The above results demonstrate that the prepared novel high-performance alumina-based composite membrane for hydrogen generation has significant potential for applications within the AWE process.
{"title":"Polyethylene Glycol Functionalized Alumina-Based Composite Membrane with High-performance for Alkaline Water Electrolysis","authors":"Jinyu Lu ,&nbsp;Jian You ,&nbsp;Ben Chang ,&nbsp;Wei Wang ,&nbsp;Yongzhao Li ,&nbsp;Jiabin Lin ,&nbsp;Xiangbo Luo ,&nbsp;Huaiyin Chen ,&nbsp;Yuekun Lai ,&nbsp;Meihua Wu ,&nbsp;Weilong Cai","doi":"10.1016/j.memsci.2025.123986","DOIUrl":"10.1016/j.memsci.2025.123986","url":null,"abstract":"<div><div>Green hydrogen is currently the dominant trend in the evolution of hydrogen energy, producing almost no greenhouse gas emissions. Alkaline water electrolysis (AWE) is recognized as a leading and well-established technology for producing green hydrogen. However, safety hazards may occur during hydrogen production currently as defective commercial separate membranes used in the AWE process. Therefore, it is imperative to create a membrane characterized by low area resistance, high stability, and high bubble point pressure (BPP) to realize high-performance AWE. Herein, we synthesize alumina-based composite membranes with Y<sub>2</sub>O<sub>3</sub>-added and polyethylene glycol functionalized Al<sub>2</sub>O<sub>3</sub> for AWE through a phase inversion method. The porous composite membrane exhibits excellent hydrophilicity, with a lower contact angle of approximately 55°. It also presents exceptional performance metrics, including a low area resistance of about 0.17 Ω cm<sup>2</sup>, an ultra-high BBP of approximately 4.4 bar, and excellent mechanical properties with a tensile strength of around 25 MPa. The membranes achieved a current density of up to 2.5 A cm<sup>-2</sup> under 2.0 V voltage in a 30 wt% KOH solution at 80 °C by utilizing commercial catalysts. Notably, the composite membranes exhibited remarkable stability, maintaining operation for over 1200 hours at a 2.0 A cm<sup>-2</sup> current density without any performance degradation at 80°C. Furthermore, this composite membrane possesses outstanding gas-barrier capability with H<sub>2</sub> and O<sub>2</sub> purity higher than 98.70% and 99.69%, respectively. The above results demonstrate that the prepared novel high-performance alumina-based composite membrane for hydrogen generation has significant potential for applications within the AWE process.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"725 ","pages":"Article 123986"},"PeriodicalIF":8.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143687885","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
Efficient activation of peroxymonosulfate by sulfur-coordinated iron-based two-dimensional composite membrane (S–Fe@G) via sulfur doping and nanoconfined catalysis
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-03-17 DOI: 10.1016/j.memsci.2025.123984
Wenwa Weng , Jiawei Hou , Nigel Graham , Xinyu Yu , Wenzheng Yu , Kening Sun , Ting Liu
The combination of nanoconfined catalysis, sulfate radicals based-advanced oxidation processes (SR-AOPs) and membrane filtration processes, can remove organic pollutants efficiently while eliminating the need for secondary recovery of heterogeneous catalysts. In this study, sulfur-doped iron-based carbonaceous two-dimensional composite nanoconfined catalytic membranes (S–Fe@G membranes) were prepared to rapidly activate peroxymonosulfate (PMS) for efficient water purification. The best performing 2S–20Fe@G catalytic membrane/PMS system achieved an ultra-rapid (158.7 ms retention time) removal (94.9 %) and high mineralization (>66.7 %) of tetracycline (TC, 20 mg/L) due to the generation of 1O2, Fe(IV)=O and •OH. The introduction of sulfur was found to significantly improve the electronic structure and electron transfer efficiency of S–Fe@G. This enhancement promoted the activity of Fe reaction sites and increased the multivalent distribution of Fe. Additionally, sulfur incorporation lowered the reaction energy barrier for PMS dissociation and accelerated the Fe(II)/Fe(III) cycle. These combined effects resulted in the rapid degradation of pollutants and ensured the stable operation of the catalytic system over extended periods. In addition, the nanoconfined space composed of the two-dimensional carbonaceous structure was conducive to the accumulation of pollutants and the rapid activation of PMS. The 2S–20Fe@G catalytic membrane achieved a high selective removal of TC (>94.5 %) and substantial mineralization of pollutants (>52.1 %) in both simulated (Humic acid + TC) and real (Lake water + TC) waters, demonstrating its potential for practical applications.
{"title":"Efficient activation of peroxymonosulfate by sulfur-coordinated iron-based two-dimensional composite membrane (S–Fe@G) via sulfur doping and nanoconfined catalysis","authors":"Wenwa Weng ,&nbsp;Jiawei Hou ,&nbsp;Nigel Graham ,&nbsp;Xinyu Yu ,&nbsp;Wenzheng Yu ,&nbsp;Kening Sun ,&nbsp;Ting Liu","doi":"10.1016/j.memsci.2025.123984","DOIUrl":"10.1016/j.memsci.2025.123984","url":null,"abstract":"<div><div>The combination of nanoconfined catalysis, sulfate radicals based-advanced oxidation processes (SR-AOPs) and membrane filtration processes, can remove organic pollutants efficiently while eliminating the need for secondary recovery of heterogeneous catalysts. In this study, sulfur-doped iron-based carbonaceous two-dimensional composite nanoconfined catalytic membranes (S–Fe@G membranes) were prepared to rapidly activate peroxymonosulfate (PMS) for efficient water purification. The best performing 2S–20Fe@G catalytic membrane/PMS system achieved an ultra-rapid (158.7 ms retention time) removal (94.9 %) and high mineralization (&gt;66.7 %) of tetracycline (TC, 20 mg/L) due to the generation of <sup>1</sup>O<sub>2</sub>, Fe(IV)=O and •OH. The introduction of sulfur was found to significantly improve the electronic structure and electron transfer efficiency of S–Fe@G. This enhancement promoted the activity of Fe reaction sites and increased the multivalent distribution of Fe. Additionally, sulfur incorporation lowered the reaction energy barrier for PMS dissociation and accelerated the Fe(II)/Fe(III) cycle. These combined effects resulted in the rapid degradation of pollutants and ensured the stable operation of the catalytic system over extended periods. In addition, the nanoconfined space composed of the two-dimensional carbonaceous structure was conducive to the accumulation of pollutants and the rapid activation of PMS. The 2S–20Fe@G catalytic membrane achieved a high selective removal of TC (&gt;94.5 %) and substantial mineralization of pollutants (&gt;52.1 %) in both simulated (Humic acid + TC) and real (Lake water + TC) waters, demonstrating its potential for practical applications.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"724 ","pages":"Article 123984"},"PeriodicalIF":8.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143681796","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
期刊
Journal of Membrane Science
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