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Fabrication and characterization of polycrystalline MFI membranes on coarse macroporous supports for the separation of butane isomers
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-04-11 DOI: 10.1016/j.memsci.2025.124065
Hammad Saulat , Weiquan Feng , Zhongzhuang Hu , Mengxing He , Jinming Lu , Yan Zhang , Jianhua Yang , Cheng He
<div><div>Separation of butane isomers holds substantial importance across various industrial sectors due to their divergent chemical characteristics and pervasive applications. Their efficient separation into high-purity iso-butane (i-C<sub>4</sub>) and normal butane (n-C<sub>4</sub>) allows their optimal utilization while maximizing economic benefit and minimizing waste, though their separation presents significant challenges due to their similar physicochemical properties and energy-intensive separation requirements. Polycrystalline zeolite-based membrane separation processes emerge as an energy-efficient approach for separating butane isomers by reducing the total operating energy consumption as compared to the conventional distillation process. However, the fabrication cost of polycrystalline zeolite membranes is high, predominantly dictated by the production cost of the support (≈ 50-70 %) rather than the polycrystalline zeolite layer. Herein, we report the fabrication of polycrystalline MFI membranes on inexpensive coarse macroporous α-Al<sub>2</sub>O<sub>3</sub> tube supports (symmetrical supports) with an average pore size in the range of 2 ∼ 3μm for separating butane isomers. Macroporous α-Al<sub>2</sub>O<sub>3</sub> tube supports are coated with single (sheet-like MFI crystals) and dual (sheet-like MFI crystals + MFI crystals) seed layers to achieve the desired separation performances. For coating a single seed layer, MFI nanocrystals were employed as precursors for synthesizing sheet-like MFI crystals with a high aspect ratio as compared to the conventional MFI crystals. Taking advantage of the high aspect ratio of sheet-like MFI crystals, single seed layer was fabricated on coarse macroporous α-Al<sub>2</sub>O<sub>3</sub> tube support, eliminating the time-intensive steps to reduce the support pore size and reducing the problem of pore plugging. Subsequently, a dual seed layer (sheet-like MFI crystals + MFI crystals) was also created by hot dip coating the MFI crystals on the surface of a single seed layer with the aim of fabricating a more compact, continuous, and molecular sieving polycrystalline MFI membrane with enhanced separation performance for the separation butane isomers. After hydrothermal crystallization, polycrystalline MFI membrane (M-2) fabricated on a single seed layer exhibits a separation factor and n-butane permeance of 33.80 and 2.00x10<sup>-7</sup> mol/m<sup>2</sup>.Pa.s, respectively. In contrast, the polycrystalline MFI membrane (D-3) formed on a dual seed layer demonstrates a separation factor and n-butane permanence of 40.60 and 1.47x10<sup>-7</sup> mol/m<sup>2</sup>.Pa.s, respectively. Both these membranes demonstrate good stability and reproducibility. Fabrication of polycrystalline MFI membranes on inexpensive coarse macroporous tube supports is a crucial advancement in reducing fabrication costs and facilitating industrial implementation. However, substantial potential remains for further scaling up and e
{"title":"Fabrication and characterization of polycrystalline MFI membranes on coarse macroporous supports for the separation of butane isomers","authors":"Hammad Saulat ,&nbsp;Weiquan Feng ,&nbsp;Zhongzhuang Hu ,&nbsp;Mengxing He ,&nbsp;Jinming Lu ,&nbsp;Yan Zhang ,&nbsp;Jianhua Yang ,&nbsp;Cheng He","doi":"10.1016/j.memsci.2025.124065","DOIUrl":"10.1016/j.memsci.2025.124065","url":null,"abstract":"&lt;div&gt;&lt;div&gt;Separation of butane isomers holds substantial importance across various industrial sectors due to their divergent chemical characteristics and pervasive applications. Their efficient separation into high-purity iso-butane (i-C&lt;sub&gt;4&lt;/sub&gt;) and normal butane (n-C&lt;sub&gt;4&lt;/sub&gt;) allows their optimal utilization while maximizing economic benefit and minimizing waste, though their separation presents significant challenges due to their similar physicochemical properties and energy-intensive separation requirements. Polycrystalline zeolite-based membrane separation processes emerge as an energy-efficient approach for separating butane isomers by reducing the total operating energy consumption as compared to the conventional distillation process. However, the fabrication cost of polycrystalline zeolite membranes is high, predominantly dictated by the production cost of the support (≈ 50-70 %) rather than the polycrystalline zeolite layer. Herein, we report the fabrication of polycrystalline MFI membranes on inexpensive coarse macroporous α-Al&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;3&lt;/sub&gt; tube supports (symmetrical supports) with an average pore size in the range of 2 ∼ 3μm for separating butane isomers. Macroporous α-Al&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;3&lt;/sub&gt; tube supports are coated with single (sheet-like MFI crystals) and dual (sheet-like MFI crystals + MFI crystals) seed layers to achieve the desired separation performances. For coating a single seed layer, MFI nanocrystals were employed as precursors for synthesizing sheet-like MFI crystals with a high aspect ratio as compared to the conventional MFI crystals. Taking advantage of the high aspect ratio of sheet-like MFI crystals, single seed layer was fabricated on coarse macroporous α-Al&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;3&lt;/sub&gt; tube support, eliminating the time-intensive steps to reduce the support pore size and reducing the problem of pore plugging. Subsequently, a dual seed layer (sheet-like MFI crystals + MFI crystals) was also created by hot dip coating the MFI crystals on the surface of a single seed layer with the aim of fabricating a more compact, continuous, and molecular sieving polycrystalline MFI membrane with enhanced separation performance for the separation butane isomers. After hydrothermal crystallization, polycrystalline MFI membrane (M-2) fabricated on a single seed layer exhibits a separation factor and n-butane permeance of 33.80 and 2.00x10&lt;sup&gt;-7&lt;/sup&gt; mol/m&lt;sup&gt;2&lt;/sup&gt;.Pa.s, respectively. In contrast, the polycrystalline MFI membrane (D-3) formed on a dual seed layer demonstrates a separation factor and n-butane permanence of 40.60 and 1.47x10&lt;sup&gt;-7&lt;/sup&gt; mol/m&lt;sup&gt;2&lt;/sup&gt;.Pa.s, respectively. Both these membranes demonstrate good stability and reproducibility. Fabrication of polycrystalline MFI membranes on inexpensive coarse macroporous tube supports is a crucial advancement in reducing fabrication costs and facilitating industrial implementation. However, substantial potential remains for further scaling up and e","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"727 ","pages":"Article 124065"},"PeriodicalIF":8.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143844643","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 monitoring of nonlinear physical aging and anti-aging in polymer-based separation membranes
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-04-11 DOI: 10.1016/j.memsci.2025.124054
Junjie Liu , Ping Xue , Xiao Yan , Ning Qi , Zhiquan Chen , Zhengbang Wang , Nanwen Li
Glassy polymers are systems out of equilibrium, the theoretical description of physical aging effects on polymeric membranes for gas separation has thus far remained elusive. Herein, we introduce an in situ positron annihilation method combined with a series of time-dependent permeability for thermally rearranged polymer (TR-1), polymer with intrinsic microporosity (PIM-1), carbon molecular sieve (CMS) membrane and mixed matrix membrane (PIM-1-C, PIM-1+10wt% COF-316) during the aging process, to provide a fundamental micro-mechanism of relaxation and the form of expression for transport behavior. The challenging issues of accurate quantifying free volume and defining that in terms of measurable quantity have been addressed. The results indicate that the aging dynamics follow a stretched exponential decay function. Physical aging in PIM-1 differs from TR-1, as the different molding methods. Compared to semi-rigid polymer materials, CMS membranes exhibit the most demanding size-sensitive pairs due to their ultra-microporous structure during the densification process. The restricted diffusion of larger gases leads to irregular transport behavior, resulting in enhanced selectivity in aged membranes. Furthermore, a comprehensive understanding of the anti-aging process based on confinement effect is also monitored.
{"title":"In situ monitoring of nonlinear physical aging and anti-aging in polymer-based separation membranes","authors":"Junjie Liu ,&nbsp;Ping Xue ,&nbsp;Xiao Yan ,&nbsp;Ning Qi ,&nbsp;Zhiquan Chen ,&nbsp;Zhengbang Wang ,&nbsp;Nanwen Li","doi":"10.1016/j.memsci.2025.124054","DOIUrl":"10.1016/j.memsci.2025.124054","url":null,"abstract":"<div><div>Glassy polymers are systems out of equilibrium, the theoretical description of physical aging effects on polymeric membranes for gas separation has thus far remained elusive. Herein, we introduce an in situ positron annihilation method combined with a series of time-dependent permeability for thermally rearranged polymer (TR-1), polymer with intrinsic microporosity (PIM-1), carbon molecular sieve (CMS) membrane and mixed matrix membrane (PIM-1-C, PIM-1+10wt% COF-316) during the aging process, to provide a fundamental micro-mechanism of relaxation and the form of expression for transport behavior. The challenging issues of accurate quantifying free volume and defining that in terms of measurable quantity have been addressed. The results indicate that the aging dynamics follow a stretched exponential decay function. Physical aging in PIM-1 differs from TR-1, as the different molding methods. Compared to semi-rigid polymer materials, CMS membranes exhibit the most demanding size-sensitive pairs due to their ultra-microporous structure during the densification process. The restricted diffusion of larger gases leads to irregular transport behavior, resulting in enhanced selectivity in aged membranes. Furthermore, a comprehensive understanding of the anti-aging process based on confinement effect is also monitored.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"727 ","pages":"Article 124054"},"PeriodicalIF":8.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143850839","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
MoS2/MoO3 heterostructure ceramic membrane for nanofiltration
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-04-11 DOI: 10.1016/j.memsci.2025.124098
Yue Liu , Shaomin Liu , Wen-Hai Zhang , Boyuan Xuan , Changwei Zhao , Hongxia Guo
Two-dimensional molybdenum disulfide (MoS2) has been recognized an excellent membrane material owing to its exceptional chemical stability, structural integrity, and high mechanical strength. However, the hydrophilic modification of the MoS2 membrane remains a significant challenge. Herein, we present an in-situ oxidation strategy to construct MoS2/MoO3 heterostructure nanosheets with an outer layer of MoO3 and an internal layer of MoS2 through a thermal annealing process, resulting in the ideal MoS2/MoO3 heterostructure ceramic membrane. This approach enhanced the membrane surface hydrophilicity without blocking channels of MoS2 for mass transfer. The resultant MoS2/MoO3 heterostructure membrane exhibited excellent water permeance of 32.8 L m2 h−1·bar−1 and Xylenol Orange (XO) rejection up to 97.4 %, and demonstrated outstanding pressure resistance and long-term operational stability.
{"title":"MoS2/MoO3 heterostructure ceramic membrane for nanofiltration","authors":"Yue Liu ,&nbsp;Shaomin Liu ,&nbsp;Wen-Hai Zhang ,&nbsp;Boyuan Xuan ,&nbsp;Changwei Zhao ,&nbsp;Hongxia Guo","doi":"10.1016/j.memsci.2025.124098","DOIUrl":"10.1016/j.memsci.2025.124098","url":null,"abstract":"<div><div>Two-dimensional molybdenum disulfide (MoS<sub>2</sub>) has been recognized an excellent membrane material owing to its exceptional chemical stability, structural integrity, and high mechanical strength. However, the hydrophilic modification of the MoS<sub>2</sub> membrane remains a significant challenge. Herein, we present an <em>in-situ</em> oxidation strategy to construct MoS<sub>2</sub>/MoO<sub>3</sub> heterostructure nanosheets with an outer layer of MoO<sub>3</sub> and an internal layer of MoS<sub>2</sub> through a thermal annealing process, resulting in the ideal MoS<sub>2</sub>/MoO<sub>3</sub> heterostructure ceramic membrane. This approach enhanced the membrane surface hydrophilicity without blocking channels of MoS<sub>2</sub> for mass transfer. The resultant MoS<sub>2</sub>/MoO<sub>3</sub> heterostructure membrane exhibited excellent water permeance of 32.8 L m<sup>2</sup> h<sup>−1</sup>·bar<sup>−1</sup> and Xylenol Orange (XO) rejection up to 97.4 %, and demonstrated outstanding pressure resistance and long-term operational stability.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"727 ","pages":"Article 124098"},"PeriodicalIF":8.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143847841","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
Multistage nanofiltration membranes with adsorptive substrate for enhanced removal of emerging organic pollutants
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-04-10 DOI: 10.1016/j.memsci.2025.124095
Yaoli Guo , Lei Jiang , Shengchao Zhao , Sabrine Ghazouani , Yanyan Liu , Shushan Yuan , Shengchao Wei , Shuangmei Xue , Yingfei Hou , Zhouyou Wang , Idris Okeowo , Q. Jason Niu , Pengrui Jin , Bart Van der Bruggen
Nanofiltration (NF) membranes, characterized by a molecular weight (MW) cut-off above 350 Da, demonstrate excellent water permeance and efficient rejection of large molecules. However, these membranes are inadequate for the removal of emerging organic pollutants (EOPs) around or below 300 Da. The presence of these EOPs is an increasing public concern due to their potential chronic health impacts and ecological disruptions, even at trace levels. In this study, we report a three-dimensional Kevlar hydrogel modified with polyaniline (PANI) nanofibers, which serves as the support membrane for creating multistage NF membranes with adsorptive substrate. These membranes feature an ultrathin polyamide active layer with a uniform distribution of pore size. Furthermore, the doping/dedoping chemistry of polyaniline endows the NF membrane with a tunable charge, allowing for improved selective [adsorption and small organic molecule separation from pharmaceutical and municipal wastewater. The prepared NF membranes have high adsorption capacity, enabling selective and fast molecular separation, and exhibit excellent dynamic processing capacity. The NF adsorption membrane achieves over 95 % removal of various EOPs (such as Methyl Orange, Bisphenol A, Tramadol) far exceeding the around 50 % rejection of commercial NF membranes and offers double the water permeance. Efficient EOPs capture through combined adsorption and NF rejection offers a strategy for preparing high-performance NF membranes for precise separation.
{"title":"Multistage nanofiltration membranes with adsorptive substrate for enhanced removal of emerging organic pollutants","authors":"Yaoli Guo ,&nbsp;Lei Jiang ,&nbsp;Shengchao Zhao ,&nbsp;Sabrine Ghazouani ,&nbsp;Yanyan Liu ,&nbsp;Shushan Yuan ,&nbsp;Shengchao Wei ,&nbsp;Shuangmei Xue ,&nbsp;Yingfei Hou ,&nbsp;Zhouyou Wang ,&nbsp;Idris Okeowo ,&nbsp;Q. Jason Niu ,&nbsp;Pengrui Jin ,&nbsp;Bart Van der Bruggen","doi":"10.1016/j.memsci.2025.124095","DOIUrl":"10.1016/j.memsci.2025.124095","url":null,"abstract":"<div><div>Nanofiltration (NF) membranes, characterized by a molecular weight (MW) cut-off above 350 Da, demonstrate excellent water permeance and efficient rejection of large molecules. However, these membranes are inadequate for the removal of emerging organic pollutants (EOPs) around or below 300 Da. The presence of these EOPs is an increasing public concern due to their potential chronic health impacts and ecological disruptions, even at trace levels. In this study, we report a three-dimensional Kevlar hydrogel modified with polyaniline (PANI) nanofibers, which serves as the support membrane for creating multistage NF membranes with adsorptive substrate. These membranes feature an ultrathin polyamide active layer with a uniform distribution of pore size. Furthermore, the doping/dedoping chemistry of polyaniline endows the NF membrane with a tunable charge, allowing for improved selective [adsorption and small organic molecule separation from pharmaceutical and municipal wastewater. The prepared NF membranes have high adsorption capacity, enabling selective and fast molecular separation, and exhibit excellent dynamic processing capacity. The NF adsorption membrane achieves over 95 % removal of various EOPs (such as Methyl Orange, Bisphenol A, Tramadol) far exceeding the around 50 % rejection of commercial NF membranes and offers double the water permeance. Efficient EOPs capture through combined adsorption and NF rejection offers a strategy for preparing high-performance NF membranes for precise separation.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"727 ","pages":"Article 124095"},"PeriodicalIF":8.4,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143823572","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
Performance improvement of water and heat recovery from stripped gas in a carbon capture process: Assembling different pore-sized ceramic membranes in a transport membrane condenser
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-04-10 DOI: 10.1016/j.memsci.2025.124092
Enyu Wang , Tao Sun , Fushuai Li , Yusen Shao , Shuiping Yan
Recently, the transport membrane condenser (TMC) has demonstrated remarkable performance in recovering waste heat and condensate from hot and moist gases streams by simultaneous mass and heat transfer capabilities. Notably, in the solvent-based CO2 chemical absorption process, TMC has also experimentally shown a good energy-saving potential through acting as the heat exchange medium between the hot stripped gas (i.e., the gas mixture of CO2 and water vapor) and bypassed cold CO2-rich solvent to drive an enhancement of waste heat recovery. In this work, a novel TMC structure was proposed by assembling ceramic membranes with different pore sizes to further improve the energy-saving potential. Ceramic membranes with pore sizes of 30 nm and 100 nm were initially selected for constructing the TMC due to their superior waste heat recovery performance. Subsequently, eight ceramic membranes with 30 nm and 100 nm pore sizes were encapsulated within a shell to assemble the TMC, and then its energy-saving potential was experimentally investigated, focusing on waste heat recovery performance. Results showed, among the five investigated TMC structures, where the stripped gas first contacted 100 nm membranes followed by 30 nm membranes demonstrated superior energy-saving potential in which the area ratio of 100 nm–30 nm membranes was maintained at 1:1 to 1:3. Notably, at a 1:1 area ratio, the TMC with 100 nm spaced by 30 nm membrane layout was achieved a maximum energy-saving potential of 0.94 MJ/kg-CO2, representing a 13.2 % increase over TMCs using only 30 nm membranes. Current finding offers a promising new direction for TMC structural design.
{"title":"Performance improvement of water and heat recovery from stripped gas in a carbon capture process: Assembling different pore-sized ceramic membranes in a transport membrane condenser","authors":"Enyu Wang ,&nbsp;Tao Sun ,&nbsp;Fushuai Li ,&nbsp;Yusen Shao ,&nbsp;Shuiping Yan","doi":"10.1016/j.memsci.2025.124092","DOIUrl":"10.1016/j.memsci.2025.124092","url":null,"abstract":"<div><div>Recently, the transport membrane condenser (TMC) has demonstrated remarkable performance in recovering waste heat and condensate from hot and moist gases streams by simultaneous mass and heat transfer capabilities. Notably, in the solvent-based CO<sub>2</sub> chemical absorption process, TMC has also experimentally shown a good energy-saving potential through acting as the heat exchange medium between the hot stripped gas (i.e., the gas mixture of CO<sub>2</sub> and water vapor) and bypassed cold CO<sub>2</sub>-rich solvent to drive an enhancement of waste heat recovery. In this work, a novel TMC structure was proposed by assembling ceramic membranes with different pore sizes to further improve the energy-saving potential. Ceramic membranes with pore sizes of 30 nm and 100 nm were initially selected for constructing the TMC due to their superior waste heat recovery performance. Subsequently, eight ceramic membranes with 30 nm and 100 nm pore sizes were encapsulated within a shell to assemble the TMC, and then its energy-saving potential was experimentally investigated, focusing on waste heat recovery performance. Results showed, among the five investigated TMC structures, where the stripped gas first contacted 100 nm membranes followed by 30 nm membranes demonstrated superior energy-saving potential in which the area ratio of 100 nm–30 nm membranes was maintained at 1:1 to 1:3. Notably, at a 1:1 area ratio, the TMC with 100 nm spaced by 30 nm membrane layout was achieved a maximum energy-saving potential of 0.94 MJ/kg-CO<sub>2</sub>, representing a 13.2 % increase over TMCs using only 30 nm membranes. Current finding offers a promising new direction for TMC structural design.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"727 ","pages":"Article 124092"},"PeriodicalIF":8.4,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143823571","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
Preparation of hollow fiber nanofiltration membranes with intensified charge density for Li+/Mg2+ separation from brines with high Mg2+/Li+ ratios
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-04-08 DOI: 10.1016/j.memsci.2025.124091
Le Shi , Li Ding , Sihua Liu , Haifu Gao , Jingguo She , Jianhua Zhang , Xiaolong Lu , Chunrui Wu
To achieve efficient separation of Li+/Mg2+, nanofiltration membranes (NFMs) with intensified positive charge density were fabricated by surface grafting of guanazole (GAZ) on the surface of piperazine (PIP)/trimesoyl chloride (TMC) NFMs. GAZ is rich in amino groups with smaller molecular size, could contact and react more sufficiently with reaction sites on membrane surface, and give less potential blockage of surface pores, compared to traditional surface grafting molecules. The influence of the chargeability and pore size of pristine PIP/TMC NFMs and surface grafting reaction on the structure and performance of GAZ grafted NFMs was investigated. Simulated brine with Mg2+/Li+ ratio of 150 was utilized to evaluate the feasibility of GAZ grafted NFMs in treating salt-lake brine with high Mg2+/Li + ratios. The results showed that the positive charge density on the NFMs surface was improved and the percentage of larger pores was reduced with the successful grafting of GAZ. The optimal GAZ grafted NFMs exhibited higher MgCl2 rejection (94.2 %) than that of PIP/TMC NFMs (64.2 %) and maintained a stable pure water permeance. It was worth noting that the Li+/Mg2+ separation factor for simulated brine of 2000 mg L−1 (Mg2+/Li+ ratio of 150) reached 25.7, which was potentially applicable for treating salt-lake brine with high Mg2+/Li+ ratios.
为了实现Li+/Mg2+的高效分离,研究人员在哌嗪(PIP)/三甲基甲酰氯(TMC)纳滤膜(NFMs)表面接枝了胍唑(GAZ),从而制备了具有更高正电荷密度的纳滤膜(NFMs)。与传统的表面接枝分子相比,GAZ富含氨基,分子尺寸较小,能与膜表面的反应位点更充分地接触和反应,对表面孔隙的潜在阻塞也较小。研究了原始 PIP/TMC NFM 的电荷率和孔径以及表面接枝反应对 GAZ 接枝 NFM 的结构和性能的影响。利用 Mg2+/Li+ 比率为 150 的模拟盐水来评估 GAZ 接枝 NFMs 处理高 Mg2+/Li+ 比率盐湖盐水的可行性。结果表明,随着 GAZ 的成功接枝,NFMs 表面的正电荷密度得到了提高,较大孔隙的比例降低了。与 PIP/TMC NFMs(64.2%)相比,最佳 GAZ 接枝 NFMs 的氯化镁排斥率(94.2%)更高,并能保持稳定的纯水渗透率。值得注意的是,在模拟 2000 mg L-1 的盐水(Mg2+/Li+比率为 150)中,Li+/Mg2+分离因子达到 25.7,可用于处理高 Mg2+/Li+ 比率的盐湖盐水。
{"title":"Preparation of hollow fiber nanofiltration membranes with intensified charge density for Li+/Mg2+ separation from brines with high Mg2+/Li+ ratios","authors":"Le Shi ,&nbsp;Li Ding ,&nbsp;Sihua Liu ,&nbsp;Haifu Gao ,&nbsp;Jingguo She ,&nbsp;Jianhua Zhang ,&nbsp;Xiaolong Lu ,&nbsp;Chunrui Wu","doi":"10.1016/j.memsci.2025.124091","DOIUrl":"10.1016/j.memsci.2025.124091","url":null,"abstract":"<div><div>To achieve efficient separation of Li<sup>+</sup>/Mg<sup>2+</sup>, nanofiltration membranes (NFMs) with intensified positive charge density were fabricated by surface grafting of guanazole (GAZ) on the surface of piperazine (PIP)/trimesoyl chloride (TMC) NFMs. GAZ is rich in amino groups with smaller molecular size, could contact and react more sufficiently with reaction sites on membrane surface, and give less potential blockage of surface pores, compared to traditional surface grafting molecules. The influence of the chargeability and pore size of pristine PIP/TMC NFMs and surface grafting reaction on the structure and performance of GAZ grafted NFMs was investigated. Simulated brine with Mg<sup>2+</sup>/Li<sup>+</sup> ratio of 150 was utilized to evaluate the feasibility of GAZ grafted NFMs in treating salt-lake brine with high Mg<sup>2+</sup>/Li <sup>+</sup> ratios. The results showed that the positive charge density on the NFMs surface was improved and the percentage of larger pores was reduced with the successful grafting of GAZ. The optimal GAZ grafted NFMs exhibited higher MgCl<sub>2</sub> rejection (94.2 %) than that of PIP/TMC NFMs (64.2 %) and maintained a stable pure water permeance. It was worth noting that the Li<sup>+</sup>/Mg<sup>2+</sup> separation factor for simulated brine of 2000 mg L<sup>−1</sup> (Mg<sup>2+</sup>/Li<sup>+</sup> ratio of 150) reached 25.7, which was potentially applicable for treating salt-lake brine with high Mg<sup>2+</sup>/Li<sup>+</sup> ratios.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"727 ","pages":"Article 124091"},"PeriodicalIF":8.4,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143823527","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
Rapid and effective self-healing of graphene oxide membranes enabled by alginate functionalization
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-04-08 DOI: 10.1016/j.memsci.2025.124084
Shouyuan Hu , Jie Jiang , Junbo Wang, Jiahao Hu, Yalong Li, Pei Li, Liang Chen
Cross-linking graphene oxide (GO) membranes enhances separation performance by meticulously regulating nanochannels and interactions between GO flakes. However, achieving self-healing for localized damage, such as mechanical scratches, still remains a crucial challenge in prolonging membrane lifespan and minimizing costs. Here, we have innovatively designed a reduced GO membrane functionalized with sodium alginate (SA@rGO), which demonstrates rapid and effective self-healing performance. For blade damages with a width of ∼10 μm, rapid repair can be achieved within 10 min by the addition of a minute quantity of CaCl2 solution. Through various dye rejection experiments, it was observed that both the rejection rate and permeance of the damaged membrane were rapidly restored to their original levels. During the long-term separation experiments over 100 h, our membrane exhibited exceptional rejection stability, further underscoring its excellent healing capabilities. Element mapping via scanning electron microscopy (SEM) and synchrotron radiation-based Fourier-transform infrared (SR-FTIR) spectroscopy indicated that calcium ions interact with SA molecules to form a hydrogel network, effectively 'stitching' the damaged areas together and enabling self-repair. Consequently, our self-healing functionality significantly elevates the potential of GO membranes for nanofiltration applications.
{"title":"Rapid and effective self-healing of graphene oxide membranes enabled by alginate functionalization","authors":"Shouyuan Hu ,&nbsp;Jie Jiang ,&nbsp;Junbo Wang,&nbsp;Jiahao Hu,&nbsp;Yalong Li,&nbsp;Pei Li,&nbsp;Liang Chen","doi":"10.1016/j.memsci.2025.124084","DOIUrl":"10.1016/j.memsci.2025.124084","url":null,"abstract":"<div><div>Cross-linking graphene oxide (GO) membranes enhances separation performance by meticulously regulating nanochannels and interactions between GO flakes. However, achieving self-healing for localized damage, such as mechanical scratches, still remains a crucial challenge in prolonging membrane lifespan and minimizing costs. Here, we have innovatively designed a reduced GO membrane functionalized with sodium alginate (SA@rGO), which demonstrates rapid and effective self-healing performance. For blade damages with a width of ∼10 μm, rapid repair can be achieved within 10 min by the addition of a minute quantity of CaCl<sub>2</sub> solution. Through various dye rejection experiments, it was observed that both the rejection rate and permeance of the damaged membrane were rapidly restored to their original levels. During the long-term separation experiments over 100 h, our membrane exhibited exceptional rejection stability, further underscoring its excellent healing capabilities. Element mapping via scanning electron microscopy (SEM) and synchrotron radiation-based Fourier-transform infrared (SR-FTIR) spectroscopy indicated that calcium ions interact with SA molecules to form a hydrogel network, effectively 'stitching' the damaged areas together and enabling self-repair. Consequently, our self-healing functionality significantly elevates the potential of GO membranes for nanofiltration applications.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"727 ","pages":"Article 124084"},"PeriodicalIF":8.4,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143823528","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
Deep eutectic solvent- and nanocellulose-tuned MXene membranes for efficient gas separation
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-04-08 DOI: 10.1016/j.memsci.2025.124090
Mengjie Li , Chuan Xu , Miaomiao Wu, Xiong-Fei Zhang, Jianfeng Yao
MXene-based membranes exhibit significant potential for gas separation. However, two major challenges persist: regulating the interlayer spacing of 2D MXenes and mitigating non-selective voids within the membrane structure. In this work, composite membranes comprising cellulose nanocrystals (CNCs), MXenes, and choline chloride/urea deep eutectic solvent (DES) were fabricated, and they contained carbon dioxide (CO2)-selective nanochannels. The incorporation of DES effectively modulates the interlayer spacing of MXene nanosheets to match CO2 molecules. Moreover, CNCs act as a continuous polymer skeleton, forming hydrogen bonds with adjacent MXenes to increase the inorganic‒organic interface affinity. This design facilitates CO2 transport through multiple mechanisms: (i) the solution-diffusion properties of the CNC-based polymer phase; (ii) optimized 2D MXene channels with an appropriate interlayer spacing to accelerate CO2 permeation; and (iii) the amine groups in the alkaline DES as CO2 carriers. The membrane demonstrated exceptional gas separation capabilities, attaining a maximum CO2 permeability of 496.7 Barrer, along with ideal selectivities for CO2/N2 and CO2/CH4 of 78.8 and 90.3, respectively. This research proposes a novel strategy for regulating the interlayer spacing of MXenes and designing nanocellulose-based separation membranes.
{"title":"Deep eutectic solvent- and nanocellulose-tuned MXene membranes for efficient gas separation","authors":"Mengjie Li ,&nbsp;Chuan Xu ,&nbsp;Miaomiao Wu,&nbsp;Xiong-Fei Zhang,&nbsp;Jianfeng Yao","doi":"10.1016/j.memsci.2025.124090","DOIUrl":"10.1016/j.memsci.2025.124090","url":null,"abstract":"<div><div>MXene-based membranes exhibit significant potential for gas separation. However, two major challenges persist: regulating the interlayer spacing of 2D MXenes and mitigating non-selective voids within the membrane structure. In this work, composite membranes comprising cellulose nanocrystals (CNCs), MXenes, and choline chloride/urea deep eutectic solvent (DES) were fabricated, and they contained carbon dioxide (CO<sub>2</sub>)-selective nanochannels. The incorporation of DES effectively modulates the interlayer spacing of MXene nanosheets to match CO<sub>2</sub> molecules. Moreover, CNCs act as a continuous polymer skeleton, forming hydrogen bonds with adjacent MXenes to increase the inorganic‒organic interface affinity. This design facilitates CO<sub>2</sub> transport through multiple mechanisms: (i) the solution-diffusion properties of the CNC-based polymer phase; (ii) optimized 2D MXene channels with an appropriate interlayer spacing to accelerate CO<sub>2</sub> permeation; and (iii) the amine groups in the alkaline DES as CO<sub>2</sub> carriers. The membrane demonstrated exceptional gas separation capabilities, attaining a maximum CO<sub>2</sub> permeability of 496.7 Barrer, along with ideal selectivities for CO<sub>2</sub>/N<sub>2</sub> and CO<sub>2</sub>/CH<sub>4</sub> of 78.8 and 90.3, respectively. This research proposes a novel strategy for regulating the interlayer spacing of MXenes and designing nanocellulose-based separation membranes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"727 ","pages":"Article 124090"},"PeriodicalIF":8.4,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143820765","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
Carbon nitride 2D nanosheets enhanced rGO membranes for water treatment: Forward osmosis and photocatalysis
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-04-08 DOI: 10.1016/j.memsci.2025.124089
Yiyang Liu, Mengyang Lu, Hao Fang, Hanmin Zhang
Although forward osmosis (FO) offers the advantage of high desalination capacity without additional driving forces, it faces two challenges: the trade-off effect and membrane fouling. Embedding 2D nanosheets into the membrane effectively enhances its properties by modulating the interlayer spacing and imparting catalytic functionality, providing a key strategy to address the outlined challenges. In this work, 2D nanomaterials with photocatalytic properties, specifically carbon nitride (gCN), were intercalated into reduced graphene oxide (rGO) laminates to prepare rGO@gCN composite FO membranes. Atomically 2D gCN nanosheets acted as nanospacers, increasing the interlayer spacing between rGO nanosheets and enhancing the membrane's surface hydrophilicity, thereby providing a direct water transport channel and reducing resistance to water transport. The rGO@gCN membrane exhibited optimal performance, with a water flux of 48.4 LMH (an 11-fold increase compared to the pristine rGO membrane), without sacrificing the rejection of divalent ions and organic dyes, thereby overcoming the constraints of the trade-off effect. Additionally, the rGO@gCN membrane demonstrated self-cleaning capabilities for methylene blue (MB) fouling on the surface during both static and dynamic photocatalytic performance tests. The rGO@gCN membrane maintained 70 % of the initial water flux even after 4 h FO filtration under visible light, and the MB-contaminated membrane could be self-cleaning to restore its original appearance and water permeability. Overall, this work provides a multifaceted strategy and valuable design insights for achieving high FO performance and enhanced resistance to membrane fouling in various potential applications of 2D nanomaterial-based FO membranes.
尽管前向渗透(FO)具有无需额外驱动力即可实现高脱盐能力的优势,但它也面临着两个挑战:权衡效应和膜堵塞。将二维纳米片嵌入膜中可通过调节膜层间距和赋予催化功能有效增强膜的性能,为解决上述挑战提供了一种关键策略。在这项工作中,具有光催化特性的二维纳米材料,特别是氮化碳(gCN),被插层到还原氧化石墨烯(rGO)层中,以制备 rGO@gCN 复合 FO 膜。原子二维 gCN 纳米片起到纳米垫片的作用,增加了 rGO 纳米片之间的层间距,增强了膜的表面亲水性,从而提供了直接的水传输通道,减少了水传输阻力。rGO@gCN 膜表现出最佳性能,水通量达到 48.4 LMH(与原始 rGO 膜相比增加了 11 倍),同时不影响对二价离子和有机染料的抑制,从而克服了权衡效应的限制。此外,在静态和动态光催化性能测试中,rGO@gCN 膜对表面的亚甲基蓝(MB)污垢具有自清洁能力。即使在可见光下经过 4 小时的 FO 过滤,rGO@gCN 膜仍能保持 70% 的初始水通量,而被甲基溴污染的膜也能通过自清洁恢复其原始外观和透水性。总之,这项工作为基于二维纳米材料的 FO 膜在各种潜在应用中实现高 FO 性能和增强抗膜堵塞能力提供了多方面的策略和宝贵的设计见解。
{"title":"Carbon nitride 2D nanosheets enhanced rGO membranes for water treatment: Forward osmosis and photocatalysis","authors":"Yiyang Liu,&nbsp;Mengyang Lu,&nbsp;Hao Fang,&nbsp;Hanmin Zhang","doi":"10.1016/j.memsci.2025.124089","DOIUrl":"10.1016/j.memsci.2025.124089","url":null,"abstract":"<div><div>Although forward osmosis (FO) offers the advantage of high desalination capacity without additional driving forces, it faces two challenges: the trade-off effect and membrane fouling. Embedding 2D nanosheets into the membrane effectively enhances its properties by modulating the interlayer spacing and imparting catalytic functionality, providing a key strategy to address the outlined challenges. In this work, 2D nanomaterials with photocatalytic properties, specifically carbon nitride (gCN), were intercalated into reduced graphene oxide (rGO) laminates to prepare rGO@gCN composite FO membranes. Atomically 2D gCN nanosheets acted as nanospacers, increasing the interlayer spacing between rGO nanosheets and enhancing the membrane's surface hydrophilicity, thereby providing a direct water transport channel and reducing resistance to water transport. The rGO@gCN membrane exhibited optimal performance, with a water flux of 48.4 LMH (an 11-fold increase compared to the pristine rGO membrane), without sacrificing the rejection of divalent ions and organic dyes, thereby overcoming the constraints of the trade-off effect. Additionally, the rGO@gCN membrane demonstrated self-cleaning capabilities for methylene blue (MB) fouling on the surface during both static and dynamic photocatalytic performance tests. The rGO@gCN membrane maintained 70 % of the initial water flux even after 4 h FO filtration under visible light, and the MB-contaminated membrane could be self-cleaning to restore its original appearance and water permeability. Overall, this work provides a multifaceted strategy and valuable design insights for achieving high FO performance and enhanced resistance to membrane fouling in various potential applications of 2D nanomaterial-based FO membranes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"726 ","pages":"Article 124089"},"PeriodicalIF":8.4,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143815368","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
Modeling of ceramic hollow fiber membrane self-heated with electrical current for oxygen separation from air
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-04-08 DOI: 10.1016/j.memsci.2025.124088
Hamed Abdolahimansoorkhani, Xingjian Xue
Oxygen permeation process through a gas-tight mixed conducting membrane is thermally activated in nature. To maintain elevated temperatures for membrane operations, a high temperature furnace is usually utilized. This leads to low efficiencies for heating power utilization and is difficult to change the temperature fast way due to the high volume of the furnace. Recently, a novel strategy has been employed to directly apply external electrical power to a hollow fiber membrane, achieving self-heating in a compact way. To better understand the fundamental mechanisms, herein, a mathematical model is developed for self-heated hollow fiber oxygen separation membrane assisted with vacuum conditions applied at the outlet of lumen side. Comprehensive simulations are conducted to study self-heating effects on Multiphysics transport processes and oxygen permeation performance. Simulations are also performed to investigate the effects of the orientations of electrical fields applied to hollow fiber membrane and the vacuum levels applied to the outlet of lumen side. The associated fundamental mechanisms are discussed and elaborated.
{"title":"Modeling of ceramic hollow fiber membrane self-heated with electrical current for oxygen separation from air","authors":"Hamed Abdolahimansoorkhani,&nbsp;Xingjian Xue","doi":"10.1016/j.memsci.2025.124088","DOIUrl":"10.1016/j.memsci.2025.124088","url":null,"abstract":"<div><div>Oxygen permeation process through a gas-tight mixed conducting membrane is thermally activated in nature. To maintain elevated temperatures for membrane operations, a high temperature furnace is usually utilized. This leads to low efficiencies for heating power utilization and is difficult to change the temperature fast way due to the high volume of the furnace. Recently, a novel strategy has been employed to directly apply external electrical power to a hollow fiber membrane, achieving self-heating in a compact way. To better understand the fundamental mechanisms, herein, a mathematical model is developed for self-heated hollow fiber oxygen separation membrane assisted with vacuum conditions applied at the outlet of lumen side. Comprehensive simulations are conducted to study self-heating effects on Multiphysics transport processes and oxygen permeation performance. Simulations are also performed to investigate the effects of the orientations of electrical fields applied to hollow fiber membrane and the vacuum levels applied to the outlet of lumen side. The associated fundamental mechanisms are discussed and elaborated.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"727 ","pages":"Article 124088"},"PeriodicalIF":8.4,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143814868","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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