Pub Date : 2024-11-07DOI: 10.1016/j.memsci.2024.123482
Baek-Gyu Im , Seong-Yong Woo , Min-Gyu Ham , Ho Ji , Young-Deuk Kim
In water-gap membrane distillation (WGMD), natural convection within the water gap significantly impacts performance and thermal efficiency. Previous studies have used empirical or modified empirical correlation models to predict the Nusselt number within the water gap, investigating how natural convection affects WGMD performance and thermal efficiency. However, these models are specific to certain operating conditions, limiting their application in developing a comprehensive numerical model for the WGMD process. To address this limitation, we developed a numerical model by integrating a two-dimensional natural convection model within the water gap. Experimental investigations were conducted across a wide range of feed temperatures and water gap sizes to assess the influence of key operating parameters on performance. To validate the effectiveness of the proposed numerical model, the experimental results were compared with those from the proposed model and with results from numerical models used in previous studies. The proposed numerical model demonstrated a maximum deviation of 8.5 % from the measured data, whereas the numerical models used in previous studies exhibited deviations of 22.9 %. In addition, the flow characteristics within the water gap were analyzed through isotherms and streamlines, and the improved thermal efficiency of WGMD compared to direct contact membrane distillation (DCMD) was explored.
{"title":"A novel approach to detailed modeling and simulation of water-gap membrane distillation: Establishing a numerical baseline model","authors":"Baek-Gyu Im , Seong-Yong Woo , Min-Gyu Ham , Ho Ji , Young-Deuk Kim","doi":"10.1016/j.memsci.2024.123482","DOIUrl":"10.1016/j.memsci.2024.123482","url":null,"abstract":"<div><div>In water-gap membrane distillation (WGMD), natural convection within the water gap significantly impacts performance and thermal efficiency. Previous studies have used empirical or modified empirical correlation models to predict the Nusselt number within the water gap, investigating how natural convection affects WGMD performance and thermal efficiency. However, these models are specific to certain operating conditions, limiting their application in developing a comprehensive numerical model for the WGMD process. To address this limitation, we developed a numerical model by integrating a two-dimensional natural convection model within the water gap. Experimental investigations were conducted across a wide range of feed temperatures and water gap sizes to assess the influence of key operating parameters on performance. To validate the effectiveness of the proposed numerical model, the experimental results were compared with those from the proposed model and with results from numerical models used in previous studies. The proposed numerical model demonstrated a maximum deviation of 8.5 % from the measured data, whereas the numerical models used in previous studies exhibited deviations of 22.9 %. In addition, the flow characteristics within the water gap were analyzed through isotherms and streamlines, and the improved thermal efficiency of WGMD compared to direct contact membrane distillation (DCMD) was explored.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123482"},"PeriodicalIF":8.4,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660141","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 : 2024-11-07DOI: 10.1016/j.memsci.2024.123480
Zhenyuan Li , Wei Lai , Ying Sun , Tianliang Han , Xing Liu , Chunfa Liao , Shuangjiang Luo
Plasticization can significantly impair the gas separation performance of gas separation membranes, especially for hollow fiber membranes (HFMs) with ultrathin skin layer. While conventional thermal crosslinking is an effective method to address this issue, it often leads to the transition layer collapse in HFMs, resulting in a significant decrease in gas permeance. Herein, we fabricate polyimide-cerium (PI–Ce) complex HFMs using a carboxylic group-containing 6FDA-mPDA0.65-DABA0.3-TFMB0.05 copolyimide through metal ion coordination to achieve plasticization-resistance helium recovery from natural gas. We optimized dope compositions and spinning conditions to produce defect-free hollow fiber membranes with a skin layer as thin as 300 nm. The coordination between carboxyl groups and cerium ions was characterized using Fourier Transform Infrared Spectroscopy (FTIR) and Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy. The polymer-metal coordinated membranes exhibited enhanced gas selectivities compared to the pristine HFMs due to the tailored microporosity achieved through polymer-metal coordination. Furthermore, the PI-Ce HFMs demonstrated only a 10.8 % decline in mixed-gas He/CH4 selectivity, which is significantly lower than the 55.4 % decline observed in pristine HFMs when exposed to CO2-containing feed pressures below 400 PSIA. Molecular dynamics simulations confirmed that coordination confined molecular chain swelling, thereby suppressing plasticization caused by CO2. The exceptional plasticization resistance of the PI-Ce complex HFMs provides a novel strategy for recovering helium from aggressive natural gas environments.
{"title":"Enhanced plasticization resistance of hollow fiber membranes via metal ion coordination for advanced helium recovery","authors":"Zhenyuan Li , Wei Lai , Ying Sun , Tianliang Han , Xing Liu , Chunfa Liao , Shuangjiang Luo","doi":"10.1016/j.memsci.2024.123480","DOIUrl":"10.1016/j.memsci.2024.123480","url":null,"abstract":"<div><div>Plasticization can significantly impair the gas separation performance of gas separation membranes, especially for hollow fiber membranes (HFMs) with ultrathin skin layer. While conventional thermal crosslinking is an effective method to address this issue, it often leads to the transition layer collapse in HFMs, resulting in a significant decrease in gas permeance. Herein, we fabricate polyimide-cerium (PI–Ce) complex HFMs using a carboxylic group-containing 6FDA-mPDA<sub>0.65</sub>-DABA<sub>0.3</sub>-TFMB<sub>0.05</sub> copolyimide through metal ion coordination to achieve plasticization-resistance helium recovery from natural gas. We optimized dope compositions and spinning conditions to produce defect-free hollow fiber membranes with a skin layer as thin as 300 nm. The coordination between carboxyl groups and cerium ions was characterized using Fourier Transform Infrared Spectroscopy (FTIR) and Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy. The polymer-metal coordinated membranes exhibited enhanced gas selectivities compared to the pristine HFMs due to the tailored microporosity achieved through polymer-metal coordination. Furthermore, the PI-Ce HFMs demonstrated only a 10.8 % decline in mixed-gas He/CH<sub>4</sub> selectivity, which is significantly lower than the 55.4 % decline observed in pristine HFMs when exposed to CO<sub>2</sub>-containing feed pressures below 400 PSIA. Molecular dynamics simulations confirmed that coordination confined molecular chain swelling, thereby suppressing plasticization caused by CO<sub>2</sub>. The exceptional plasticization resistance of the PI-Ce complex HFMs provides a novel strategy for recovering helium from aggressive natural gas environments.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123480"},"PeriodicalIF":8.4,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660139","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 : 2024-11-06DOI: 10.1016/j.memsci.2024.123490
Heguo Han , Zheng Liu , Huiting Yu , Yuxuan Sun , Shenghai Li , Suobo Zhang
For thin-film composite (TFC) membranes applied in organic solvent nanofiltration (OSN), enhancing the adhesion between the active layers and the substrates can effectively improve the stability of the membranes. In this work, TFC OSN membranes with polyetherketone bearing amino group (PEK-NH2) asymmetric substrates and amino-contained polyarylate active layers were fabricated by interfacial polymerization technique, and subsequently reacted with dialdehydes to form crosslinking between and within the substrates and the active layers. Crosslinking improved both of the solvent resistance of the substrates and the separation selectivity of the active layers. In addition, reverse pressure testing demonstrated that crosslinking allowed the active layers to adhere more strongly to the substrates. The optimized integrally crosslinked membranes exhibited methanol permeance of 10.4 L m−2 h−1 bar−1 and a molecular weight cut-off of about 320 g mol−1 in methanol. Moreover, the integrally crosslinked membranes maintained good stability for OSN operation in methanol for 12 days, and also exhibited unchanged OSN performance after soaked in N,N-dimethylformamide for 2 days. This work demonstrated a novel solvent-resistant membrane material and membrane-fabrication strategy with prospect for OSN application.
对于应用于有机溶剂纳滤（OSN）的薄膜复合（TFC）膜而言，增强活性层与基底之间的粘附力能有效提高膜的稳定性。在这项工作中，采用界面聚合技术制备了带有氨基的聚醚酮（PEK-NH2）不对称基底和含氨基的聚芳酸酯活性层的 TFC OSN 膜，随后与二醛反应在基底和活性层之间及内部形成交联。交联改善了基底的耐溶剂性和活性层的分离选择性。此外，反向压力测试表明，交联使活性层更牢固地附着在基底上。经过优化的整体交联膜的甲醇渗透率为 10.4 L m-2 h-1 bar-1，在甲醇中的截留分子量约为 320 g mol-1。此外，整体交联膜在甲醇中运行 12 天后仍能保持良好的稳定性，在 N,N-二甲基甲酰胺中浸泡 2 天后，其 OSN 性能也保持不变。这项工作展示了一种新型耐溶剂膜材料和膜制造策略，有望在 OSN 中得到应用。
{"title":"Imine-linked integrally crosslinked thin-film composite membrane for organic solvent nanofiltration","authors":"Heguo Han , Zheng Liu , Huiting Yu , Yuxuan Sun , Shenghai Li , Suobo Zhang","doi":"10.1016/j.memsci.2024.123490","DOIUrl":"10.1016/j.memsci.2024.123490","url":null,"abstract":"<div><div>For thin-film composite (TFC) membranes applied in organic solvent nanofiltration (OSN), enhancing the adhesion between the active layers and the substrates can effectively improve the stability of the membranes. In this work, TFC OSN membranes with polyetherketone bearing amino group (PEK-NH<sub>2</sub>) asymmetric substrates and amino-contained polyarylate active layers were fabricated by interfacial polymerization technique, and subsequently reacted with dialdehydes to form crosslinking between and within the substrates and the active layers. Crosslinking improved both of the solvent resistance of the substrates and the separation selectivity of the active layers. In addition, reverse pressure testing demonstrated that crosslinking allowed the active layers to adhere more strongly to the substrates. The optimized integrally crosslinked membranes exhibited methanol permeance of 10.4 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup> and a molecular weight cut-off of about 320 g mol<sup>−1</sup> in methanol. Moreover, the integrally crosslinked membranes maintained good stability for OSN operation in methanol for 12 days, and also exhibited unchanged OSN performance after soaked in <em>N,N</em>-dimethylformamide for 2 days. This work demonstrated a novel solvent-resistant membrane material and membrane-fabrication strategy with prospect for OSN application.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123490"},"PeriodicalIF":8.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660136","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 : 2024-11-06DOI: 10.1016/j.memsci.2024.123486
Li-ping Yue , Fan-xin Kong , Yi Wang , Jin-fu Chen , Ai-guo Zhou
The nanofiltration (NF) membrane with better hydrophilicity, uniform pore size distribution, and dually charged properties is highly desirable to improve the pharmaceutical rejection, especially for the neutral and positively charged pharmaceuticals. Herein, a TpPa membrane was first in-situ crystallized via p-toluenesulfonic acid (PTSA)-mediated interfacial catalytic polymerization (ICP) strategy using 1,3,5-triformylphloroglucinol (Tp) and p-phenylenediamine (Pa), followed by the post-functionalization with polyethylene-imine (PEI) to narrow the pore size, improve hydrophilicity, and tailor membrane charges to enhance pharmaceutical rejection. PTSA was used as a catalyst to enhance the crystallinity of the TpPa membrane. The PEI introduction narrowed the pore radius from 0.382 ± 0.50 nm to 0.272 ± 0.33 nm, improved surface hydrophilicity from 74.8° to 37.0°, and shifted surface charge from −19.25 mV to 11.15 mV. This PEI-functionalized TpPa (TpPa-PEI) layers exhibited heterogeneous charges on both sides with a positively charged top and negatively charged bottom. MgCl2 rejection increased from 13.7 % to 83.0 % without sacrificing water permeance. Additionally, pharmaceutical rejection and the water permeance of the optimal TpPa-PEI membrane exceeded those of the TpPaIP-PEI membrane fabricated without PTSA by about 3.3 and 1.3 times, respectively. Furthermore, compared to the pristine TpPa membranes, the substantially enhanced electropositivity of the optimal TpPa-PEI membrane led to 3–5 times increase in positively charged pharmaceutical rejection (94.1 % for propranolol, 97.2 % for sulpiride, and 71.2 % for metformin). The synergy between the negatively charged TpPa-PEI bottom layers and the reduced pore size maintained a sulfadiazine rejection of 62.1 %. Mechanistic study further revealed that PEI penetrated 100 nm into the TpPa layer and cross-linked with the aldehyde groups, leading to tailored chargeability, improved hydrophilicity, and reduced pore size of the membranes. Via a PEI cross-linking strategy, sub-nanometer channels of crystalline COF layers can be rationally designed, featuring precisely tailored chargeability and hydrophilicity, promising functionalization of the membrane pores and remarkably robust for water reuse.
{"title":"Crystalline covalent organic framework membrane with tailored chargeability for efficient pharmaceutical rejection by in-situ functionalization of polyethylene-imine","authors":"Li-ping Yue , Fan-xin Kong , Yi Wang , Jin-fu Chen , Ai-guo Zhou","doi":"10.1016/j.memsci.2024.123486","DOIUrl":"10.1016/j.memsci.2024.123486","url":null,"abstract":"<div><div>The nanofiltration (NF) membrane with better hydrophilicity, uniform pore size distribution, and dually charged properties is highly desirable to improve the pharmaceutical rejection, especially for the neutral and positively charged pharmaceuticals. Herein, a TpPa membrane was first in-situ crystallized via p-toluenesulfonic acid (PTSA)-mediated interfacial catalytic polymerization (ICP) strategy using 1,3,5-triformylphloroglucinol (Tp) and p-phenylenediamine (Pa), followed by the post-functionalization with polyethylene-imine (PEI) to narrow the pore size, improve hydrophilicity, and tailor membrane charges to enhance pharmaceutical rejection. PTSA was used as a catalyst to enhance the crystallinity of the TpPa membrane. The PEI introduction narrowed the pore radius from 0.382 ± 0.50 nm to 0.272 ± 0.33 nm, improved surface hydrophilicity from 74.8° to 37.0°, and shifted surface charge from −19.25 mV to 11.15 mV. This PEI-functionalized TpPa (TpPa-PEI) layers exhibited heterogeneous charges on both sides with a positively charged top and negatively charged bottom. MgCl<sub>2</sub> rejection increased from 13.7 % to 83.0 % without sacrificing water permeance. Additionally, pharmaceutical rejection and the water permeance of the optimal TpPa-PEI membrane exceeded those of the TpPa<sub>IP</sub>-PEI membrane fabricated without PTSA by about 3.3 and 1.3 times, respectively. Furthermore, compared to the pristine TpPa membranes, the substantially enhanced electropositivity of the optimal TpPa-PEI membrane led to 3–5 times increase in positively charged pharmaceutical rejection (94.1 % for propranolol, 97.2 % for sulpiride, and 71.2 % for metformin). The synergy between the negatively charged TpPa-PEI bottom layers and the reduced pore size maintained a sulfadiazine rejection of 62.1 %. Mechanistic study further revealed that PEI penetrated 100 nm into the TpPa layer and cross-linked with the aldehyde groups, leading to tailored chargeability, improved hydrophilicity, and reduced pore size of the membranes. Via a PEI cross-linking strategy, sub-nanometer channels of crystalline COF layers can be rationally designed, featuring precisely tailored chargeability and hydrophilicity, promising functionalization of the membrane pores and remarkably robust for water reuse.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"716 ","pages":"Article 123486"},"PeriodicalIF":8.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142720992","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 : 2024-11-06DOI: 10.1016/j.memsci.2024.123489
Bo Hu , Hao Deng , Yu Zheng , Zixuan Zhang , Tao Wu , Zaichuang Liu , Beixi Jia , Hanqi Lin , Runnan Zhang , Zhongyi Jiang
Developing membranes with ordered channels and high positive charge density is crucial for Li+/Mg2+ separation. Ionic covalent organic framework (COF) membranes are promising candidates, yet they face challenges like pore size mismatch with ions and the liable structural defects. Herein, we proposed a hydrogen bond-mediated strategy to assemble membranes from homo-charged COF nanosheets and polyelectrolytes. Compared with the quaternary amines in poly (diallyl dimethyl ammonium chloride), the abundant primary and secondary amines in polyethyleneimine facilitate multiple hydrogen bonding interactions with COF nanosheets. These interactions effectively overcome the electrostatic repulsion between positive charges, endowing membrane with structural robustness. Furthermore, the intercalation of polyelectrolytes eliminates the structural defects, reduces the membrane pore size, and enhances the Donnan effect. The optimized COF membrane exhibited a pure water flux of 10.2 L m−2 h−1 bar−1, separation factor of up to 30 at high Mg2+/Li+ mass ratio of 100, and excellent stability under various operating conditions. Strikingly, our strategy facilitates the fabrication of membranes in large area (>450 cm2) while maintaining consistent separation performance, showcasing substantial potential of scalable manufacturing.
{"title":"Hydrogen bond-mediated assembly of homo-charged COF nanosheets and polyelectrolytes towards robust Li+/Mg2+ separation membrane","authors":"Bo Hu , Hao Deng , Yu Zheng , Zixuan Zhang , Tao Wu , Zaichuang Liu , Beixi Jia , Hanqi Lin , Runnan Zhang , Zhongyi Jiang","doi":"10.1016/j.memsci.2024.123489","DOIUrl":"10.1016/j.memsci.2024.123489","url":null,"abstract":"<div><div>Developing membranes with ordered channels and high positive charge density is crucial for Li<sup>+</sup>/Mg<sup>2+</sup> separation. Ionic covalent organic framework (COF) membranes are promising candidates, yet they face challenges like pore size mismatch with ions and the liable structural defects. Herein, we proposed a hydrogen bond-mediated strategy to assemble membranes from homo-charged COF nanosheets and polyelectrolytes. Compared with the quaternary amines in poly (diallyl dimethyl ammonium chloride), the abundant primary and secondary amines in polyethyleneimine facilitate multiple hydrogen bonding interactions with COF nanosheets. These interactions effectively overcome the electrostatic repulsion between positive charges, endowing membrane with structural robustness. Furthermore, the intercalation of polyelectrolytes eliminates the structural defects, reduces the membrane pore size, and enhances the Donnan effect. The optimized COF membrane exhibited a pure water flux of 10.2 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup>, separation factor of up to 30 at high Mg<sup>2+</sup>/Li<sup>+</sup> mass ratio of 100, and excellent stability under various operating conditions. Strikingly, our strategy facilitates the fabrication of membranes in large area (>450 cm<sup>2</sup>) while maintaining consistent separation performance, showcasing substantial potential of scalable manufacturing.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123489"},"PeriodicalIF":8.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660214","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 : 2024-11-06DOI: 10.1016/j.memsci.2024.123487
Chenglin Zhang , Guangzhe Wang , Yangbo Qiu , Chao Wang , Feng Li , Long-Fei Ren , Jiahui Shao , Yiliang He
Covalent organic framework (COF) has great advantages in the field of membrane separation, but the efficient and convenient preparation of COF membranes is still a challenge. Herein, we propose a novel method with green solvent for the preparation of COF membranes based on electrostatic spraying, which can be successfully prepared within 10 min, forming the TpPa COF with a pore size of 1.8 nm. Molecular dynamics simulations demonstrate that electrostatic spraying enhances the reaction rate by lowering the energy barrier and increasing the movement of reacting monomers. Atomization of the solvent in electrostatic spraying causes the rapid volatilization of the solvent, resulting in supersaturation of the generated TpPa, precipitation and crystallization, and promotes the formation of TpPa COF structure. The optimal COF membrane for the separation of Congo red wastewater is prepared by adjusting the voltage, concentration, and spraying time, with selectivity of Na2SO4 for Congo Red attaining 118 and water permeance reaching 70.2 L m-2 h-1 bar-1. This work not only elaborates the membrane preparation mechanism in the electrostatic spraying process, but also greatly shortens the time of COF membrane preparation compared to the traditional method (2–3 days), which contributes to the possibility for practical application of COF membranes.
{"title":"Rapid preparation and mechanism investigation of covalent organic framework membranes by 3D printing based on electrostatic spraying","authors":"Chenglin Zhang , Guangzhe Wang , Yangbo Qiu , Chao Wang , Feng Li , Long-Fei Ren , Jiahui Shao , Yiliang He","doi":"10.1016/j.memsci.2024.123487","DOIUrl":"10.1016/j.memsci.2024.123487","url":null,"abstract":"<div><div>Covalent organic framework (COF) has great advantages in the field of membrane separation, but the efficient and convenient preparation of COF membranes is still a challenge. Herein, we propose a novel method with green solvent for the preparation of COF membranes based on electrostatic spraying, which can be successfully prepared within 10 min, forming the TpPa COF with a pore size of 1.8 nm. Molecular dynamics simulations demonstrate that electrostatic spraying enhances the reaction rate by lowering the energy barrier and increasing the movement of reacting monomers. Atomization of the solvent in electrostatic spraying causes the rapid volatilization of the solvent, resulting in supersaturation of the generated TpPa, precipitation and crystallization, and promotes the formation of TpPa COF structure. The optimal COF membrane for the separation of Congo red wastewater is prepared by adjusting the voltage, concentration, and spraying time, with selectivity of Na<sub>2</sub>SO<sub>4</sub> for Congo Red attaining 118 and water permeance reaching 70.2 L m<sup>-2</sup> h<sup>-1</sup> bar<sup>-1</sup>. This work not only elaborates the membrane preparation mechanism in the electrostatic spraying process, but also greatly shortens the time of COF membrane preparation compared to the traditional method (2–3 days), which contributes to the possibility for practical application of COF membranes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123487"},"PeriodicalIF":8.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660137","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 : 2024-11-06DOI: 10.1016/j.memsci.2024.123485
Fabricio Eduardo Bortot Coelho , Sandra Isabella Sohn , Victor M. Candelario , Nanna Isabella Bloch Hartmann , Claus Hélix-Nielsen , Wenjing Zhang
The release of microplastics (MPs) through industrial laundry wastewater accounts for 35 % of global MPs emissions into the environment and it is a significant environmental problem, especially because MPs can absorb contaminants of emerging concern (CECs) from garments. This study is the first to evaluate and perform a cost estimation of the MP removal from hospital laundry wastewater (HLWW) using a combination of ceramic membranes and a pilot-scale photocatalytic membrane reactor (PMR) as a fouling mitigation strategy. The HLWW, from a hospital in Copenhagen, Denmark, contained a total organic carbon (TOC) of 345 mg L⁻1 and 1.4 × 106 MP L−1, mainly of polyethylene terephthalate (PET) ranging between 100 and 200 μm in size. The pre-treatment with an ultrafiltration (UF) ZrO₂ membrane successfully removed 96 % of MPs and over 98 % of suspended solids and turbidity at an estimated cost of 0.45 US$ per m3 of permeate. In the PMR stage, ultraviolet light emitting diodes (UV LED) irradiation reduced irreversible fouling, improving permeate flow and minimizing the need for chemical cleaning. The Ce–Y–ZrO2/TiO2 photocatalytic membrane achieved over 99 % removal of turbidity, colour, and suspended solids, as well as 99.9 % removal of MPs, allowing the potential effluent reuse within the hospital laundry. Additionally, the retentate from the PMR process had lower TOC, easing the discharge of this concentrated stream. The cost estimation demonstrated that the photocatalytic degradation combined with traditional techniques, i.e. backflush and chemical cleaning, is more economical than using these techniques separately. Therefore, the total treatment cost was 1.09 US$ per m3 of permeate, which is lower than the cost of fresh water in Denmark. In conclusion, this innovative treatment strategy offers a sustainable and cost-effective solution for HLWW management, not only reducing water consumption by enabling water reuse in the hospital laundry but also advances towards achieving net-zero liquid discharge and contributing to the UN Sustainable Development Goals for clean water (Goal 6) and climate action (Goal 13).
{"title":"Microplastics removal from a hospital laundry wastewater combining ceramic membranes and a photocatalytic membrane reactor: Fouling mitigation, water reuse, and cost estimation","authors":"Fabricio Eduardo Bortot Coelho , Sandra Isabella Sohn , Victor M. Candelario , Nanna Isabella Bloch Hartmann , Claus Hélix-Nielsen , Wenjing Zhang","doi":"10.1016/j.memsci.2024.123485","DOIUrl":"10.1016/j.memsci.2024.123485","url":null,"abstract":"<div><div>The release of microplastics (MPs) through industrial laundry wastewater accounts for 35 % of global MPs emissions into the environment and it is a significant environmental problem, especially because MPs can absorb contaminants of emerging concern (CECs) from garments. This study is the first to evaluate and perform a cost estimation of the MP removal from hospital laundry wastewater (HLWW) using a combination of ceramic membranes and a pilot-scale photocatalytic membrane reactor (PMR) as a fouling mitigation strategy. The HLWW, from a hospital in Copenhagen, Denmark, contained a total organic carbon (TOC) of 345 mg L⁻<sup>1</sup> and 1.4 × 10<sup>6</sup> MP L<sup>−1</sup>, mainly of polyethylene terephthalate (PET) ranging between 100 and 200 μm in size. The pre-treatment with an ultrafiltration (UF) ZrO₂ membrane successfully removed 96 % of MPs and over 98 % of suspended solids and turbidity at an estimated cost of 0.45 US$ per m<sup>3</sup> of permeate. In the PMR stage, ultraviolet light emitting diodes (UV LED) irradiation reduced irreversible fouling, improving permeate flow and minimizing the need for chemical cleaning. The Ce–Y–ZrO<sub>2</sub>/TiO<sub>2</sub> photocatalytic membrane achieved over 99 % removal of turbidity, colour, and suspended solids, as well as 99.9 % removal of MPs, allowing the potential effluent reuse within the hospital laundry. Additionally, the retentate from the PMR process had lower TOC, easing the discharge of this concentrated stream. The cost estimation demonstrated that the photocatalytic degradation combined with traditional techniques, <em>i.e.</em> backflush and chemical cleaning, is more economical than using these techniques separately. Therefore, the total treatment cost was 1.09 US$ per m<sup>3</sup> of permeate, which is lower than the cost of fresh water in Denmark. In conclusion, this innovative treatment strategy offers a sustainable and cost-effective solution for HLWW management, not only reducing water consumption by enabling water reuse in the hospital laundry but also advances towards achieving net-zero liquid discharge and contributing to the UN Sustainable Development Goals for clean water (Goal 6) and climate action (Goal 13).</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123485"},"PeriodicalIF":8.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660138","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 : 2024-11-05DOI: 10.1016/j.memsci.2024.123483
Seho Lee , Chanhee Choi , Sung Min Lee , Hyunhee Lee , Jusung Han , Junghwan Kim , Jinseok Kim , Jinwook Park , Kihyun Kim , Jong-Chan Lee
We propose a novel strategy to develop sulfonated poly(arylene ether sulfone) (SPAES) composite membranes that can simultaneously improve the physicochemical stability and proton conductivity of hydrocarbon-based membranes for PEMFC applications. This strategy involves the use of a sulfonated poly(arylene thioether sulfone)-grafted 2D crown ether framework coordinated with cerium3+ ions (SATS–C2O–Ce) as a promising filler material. SATS-C2O, a highly sulfonated polymer-grafted 2D framework containing crown ether holes in its skeletal structure, was prepared via self-condensation using halogenated phloroglucinol as a multifunctional building unit to form C2O, followed by condensation using SATS to graft the sulfonated polymer onto its edge. Ce3+ ions were directly coordinated within the crown ether holes of SATS-C2O via a simple doping process using aqueous Ce solution. The SPAES composite membranes containing SATS–C2O–Ce (SPAES/SATS–C2O–Ce) exhibited exceptional dimensional stability and mechanical toughness. The remarkable chemical stability of SPAES/SATS–C2O–Ce compared to that of pristine SPAES and SPAES/Ce (containing the same amount of Ce3+ ions but without SATS-C2O) was attributed to the well-dispersed state of Ce3+ ions within the SPAES matrix. Furthermore, the enhanced proton conductivity of SPAES/SATS–C2O–Ce surpassed those of pristine SPAES, SPAES/C2O, and SPAES/Ce by the formation of additional proton-conducting channels provided by the sulfonic acid groups of SATS–C2O–Ce, along with the improved water uptake capability of SPAES.
{"title":"Hydrocarbon-based composite membranes containing sulfonated Poly(arylene thioether sulfone)-grafted 2D crown ether framework coordinated with cerium ions for PEMFC applications","authors":"Seho Lee , Chanhee Choi , Sung Min Lee , Hyunhee Lee , Jusung Han , Junghwan Kim , Jinseok Kim , Jinwook Park , Kihyun Kim , Jong-Chan Lee","doi":"10.1016/j.memsci.2024.123483","DOIUrl":"10.1016/j.memsci.2024.123483","url":null,"abstract":"<div><div>We propose a novel strategy to develop sulfonated poly(arylene ether sulfone) (SPAES) composite membranes that can simultaneously improve the physicochemical stability and proton conductivity of hydrocarbon-based membranes for PEMFC applications. This strategy involves the use of a sulfonated poly(arylene thioether sulfone)-grafted 2D crown ether framework coordinated with cerium<sup>3+</sup> ions (SATS–C<sub>2</sub>O–Ce) as a promising filler material. SATS-C<sub>2</sub>O, a highly sulfonated polymer-grafted 2D framework containing crown ether holes in its skeletal structure, was prepared via self-condensation using halogenated phloroglucinol as a multifunctional building unit to form C<sub>2</sub>O, followed by condensation using SATS to graft the sulfonated polymer onto its edge. Ce<sup>3+</sup> ions were directly coordinated within the crown ether holes of SATS-C<sub>2</sub>O via a simple doping process using aqueous Ce solution. The SPAES composite membranes containing SATS–C<sub>2</sub>O–Ce (SPAES/SATS–C<sub>2</sub>O–Ce) exhibited exceptional dimensional stability and mechanical toughness. The remarkable chemical stability of SPAES/SATS–C<sub>2</sub>O–Ce compared to that of pristine SPAES and SPAES/Ce (containing the same amount of Ce<sup>3+</sup> ions but without SATS-C<sub>2</sub>O) was attributed to the well-dispersed state of Ce<sup>3+</sup> ions within the SPAES matrix. Furthermore, the enhanced proton conductivity of SPAES/SATS–C<sub>2</sub>O–Ce surpassed those of pristine SPAES, SPAES/C<sub>2</sub>O, and SPAES/Ce by the formation of additional proton-conducting channels provided by the sulfonic acid groups of SATS–C<sub>2</sub>O–Ce, along with the improved water uptake capability of SPAES.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123483"},"PeriodicalIF":8.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660178","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 : 2024-11-05DOI: 10.1016/j.memsci.2024.123481
Zakawat Ali , Xiaochun Zhang , Palwasha Khan , Jie Li , Nai Zhang , Qixin Wang , Muhammad Yasin , Mazhar Amjad Gilani , Asim Laeeq Khan , Linglong Shan , Xiangping Zhang
Achieving strong interaction with the targeted composition and constructing abundant transport channels is crucial to obtain the pervaporation (PV) membrane with high selectivity and flux. Here, three ionic liquids (ILs) were screened out based on their relative selectivity and capacity targeting for bioethanol dehydration by COSMO-RS. The interaction energies analysis between ILs, EtOH, and H2O suggests that the ILs can form strong hydrogen bonds with water and disrupt the hydrogen bond in the EtOH–H2O azeotropic mixture, which is beneficial for improving the selectivity. Furthermore, driven by the multiple hydrogen bonds, electrostatic interactions, and van der Waals forces, ILs could self-assemble with polyvinyl alcohol (PVA) to fabricate the PV membrane with well-ordered micelle nanostructure, as its structure was revealed by MD simulations. The formation of the ILs-PVA micelle dramatically influenced membrane surface morphology, roughness, and water contact angle, providing an extra transport channel for the membrane. The optimal membrane (at the cmc point) exhibited a superior ethanol dehydration separation factor of 1627, along with a flux of 684 g/m2h at 50 °C. It can be expected that this novel self-assembled ILs-PVA micelle nanostructure strategy will find promising applications in other azeotropic mixture separation processes, like ethanol-ethyl acetate, water-butanol, etc.
{"title":"Self-assembled ILs-PVA micelle nanostructure impart the pervaporation membrane with high ethanol dehydration performance","authors":"Zakawat Ali , Xiaochun Zhang , Palwasha Khan , Jie Li , Nai Zhang , Qixin Wang , Muhammad Yasin , Mazhar Amjad Gilani , Asim Laeeq Khan , Linglong Shan , Xiangping Zhang","doi":"10.1016/j.memsci.2024.123481","DOIUrl":"10.1016/j.memsci.2024.123481","url":null,"abstract":"<div><div>Achieving strong interaction with the targeted composition and constructing abundant transport channels is crucial to obtain the pervaporation (PV) membrane with high selectivity and flux. Here, three ionic liquids (ILs) were screened out based on their relative selectivity and capacity targeting for bioethanol dehydration by COSMO-RS. The interaction energies analysis between ILs, EtOH, and H<sub>2</sub>O suggests that the ILs can form strong hydrogen bonds with water and disrupt the hydrogen bond in the EtOH–H<sub>2</sub>O azeotropic mixture, which is beneficial for improving the selectivity. Furthermore, driven by the multiple hydrogen bonds, electrostatic interactions, and van der Waals forces, ILs could self-assemble with polyvinyl alcohol (PVA) to fabricate the PV membrane with well-ordered micelle nanostructure, as its structure was revealed by MD simulations. The formation of the ILs-PVA micelle dramatically influenced membrane surface morphology, roughness, and water contact angle, providing an extra transport channel for the membrane. The optimal membrane (at the cmc point) exhibited a superior ethanol dehydration separation factor of 1627, along with a flux of 684 g/m<sup>2</sup>h at 50 °C. It can be expected that this novel self-assembled ILs-PVA micelle nanostructure strategy will find promising applications in other azeotropic mixture separation processes, like ethanol-ethyl acetate, water-butanol, etc.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123481"},"PeriodicalIF":8.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660177","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}
The emerging contaminants with high toxicity and bioaccumulation potentially threaten to human health, which was difficult removed by traditional biological treatment or membrane separation. In view of this, a novel type of fluorine (F)-doped carbon hollow fiber microfiltration membrane was prepared for realizing emerging contaminants removal through metal-free electro-Fenton. Herein, polyaniline (PANI) was used as a precursor for preparation of porous carbon membrane. The graphitic N and pyridinic N on porous carbon were used as the active sites for H2O2 production and its further activation to ·OH, which realized metal-free electro-Fenton reaction. According to the results, the carbon nanotubes with F-PANI at the ratio of 1:1 and calcination temperature at 300 °C endowed the membrane moderate resistance and pure water permeability of 430 Ω and 48.51 L/(m2 h bar), respectively. Importantly, the intensity of ·OH generation was further significant enhanced by introducing C–F bonding into the membrane. Therefore, the bisphenol A (BPA), sulfamethoxazole (SMZ) and atrazine (ATZ) removal rates were 92.63 %, 38.47 % and 27.05 %, respectively. For control group without bias, the removal rates of above contaminants were 0 % removal rates. Moreover, the membrane permeate loss by filtrating BPA, SMZ and ATZ were 0.13, 0.15 and 0.05, which were 0.20, 0.24 and 0.21 for control group.
{"title":"Emerging contaminants removal through fluorine-doped carbon hollow fiber microfiltration membrane based on metal-free electro-Fenton","authors":"Yue Yang, Zhongcheng Yang, Xiong Liu, Lanyue Qi, Yujun Zhou, Zhigao Zhu, Junwen Qi, Jiansheng Li","doi":"10.1016/j.memsci.2024.123477","DOIUrl":"10.1016/j.memsci.2024.123477","url":null,"abstract":"<div><div>The emerging contaminants with high toxicity and bioaccumulation potentially threaten to human health, which was difficult removed by traditional biological treatment or membrane separation. In view of this, a novel type of fluorine (F)-doped carbon hollow fiber microfiltration membrane was prepared for realizing emerging contaminants removal through metal-free electro-Fenton. Herein, polyaniline (PANI) was used as a precursor for preparation of porous carbon membrane. The graphitic N and pyridinic N on porous carbon were used as the active sites for H<sub>2</sub>O<sub>2</sub> production and its further activation to ·OH, which realized metal-free electro-Fenton reaction. According to the results, the carbon nanotubes with F-PANI at the ratio of 1:1 and calcination temperature at 300 °C endowed the membrane moderate resistance and pure water permeability of 430 Ω and 48.51 L/(m<sup>2</sup> h bar), respectively. Importantly, the intensity of ·OH generation was further significant enhanced by introducing C–F bonding into the membrane. Therefore, the bisphenol A (BPA), sulfamethoxazole (SMZ) and atrazine (ATZ) removal rates were 92.63 %, 38.47 % and 27.05 %, respectively. For control group without bias, the removal rates of above contaminants were 0 % removal rates. Moreover, the membrane permeate loss by filtrating BPA, SMZ and ATZ were 0.13, 0.15 and 0.05, which were 0.20, 0.24 and 0.21 for control group.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123477"},"PeriodicalIF":8.4,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660176","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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