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Constructing heterogeneously wettable nanofiber membrane for highly efficient oil refining 用于高效炼油的非均质可湿纳米纤维膜的构建
Pub Date : 2025-01-01 DOI: 10.1016/j.advmem.2025.100135
Mi Zhou , Jiayu Tong , Fangru Zhou , Linlin Yan , Pengju Gao , Kai Wang , Xiquan Cheng
Superhydrophobic membranes are highly energy-efficient for refining the oil from water-in-oil emulsions. Nevertheless, the poor solvent resistance and the ineffectiveness in separating nano-sized water droplets (below 100 nm) of the superhydrophobic membrane undermine their application in the water/oil separation process, especially for the separation of water-in-dichloromethane (CH2Cl2) and water-in-chloroform (CHCl3) emulsions. Herein, inspired by the desert beetle, we provided a facile approach to enhance the separation efficiency of cross-linked asymmetric nanofiber membrane (CNMs) towards water-in-oil emulsions by well-dispersed superabsorbent sodium polyacrylates (SAPs) particles between nanofibers through coaxial electrospinning technology. Interestingly, the hydrophilic SAPs surrounding by hydrophobic nanofibers form a heterogeneously wettable structure which is like to the structure of desert beetle backs. The unique structure could adjust the surface tension components of the membrane, leading to faster permeance of oil droplets. Moreover, as a superabsorbent resin, SAPs could absorb the nano-sized water droplets in the water-in-oil emulsion, thereby increasing the separation efficiency of the membrane. For water in CH2Cl2 emulsions, the finely tailored nanofiber membrane completely removed water droplets larger than 63 nm, demonstrated permeance above 3.5 ×104 L∙m−2∙h−1∙bar−1 with significant separation efficiency above 98.8%, and showed fantastic stability in organic solvent, exhibiting strong promise in oil refining.
超疏水膜是一种高效节能的从油包水乳剂中提炼油的方法。然而,超疏水膜耐溶剂性差,不能有效分离纳米级(小于100 nm)水滴,影响了其在水/油分离中的应用,特别是在二氯甲烷水(CH2Cl2)和氯仿水(CHCl3)乳剂分离中的应用。在此,受沙漠甲虫的启发,我们提供了一种简单的方法来提高交联不对称纳米纤维膜(CNMs)对油包水乳液的分离效率,通过同轴静电纺丝技术在纳米纤维之间分散良好的高吸水性聚丙烯酸钠(sap)颗粒。有趣的是,疏水纳米纤维包围的亲水sap形成了类似于沙漠甲虫背部结构的非均质可湿结构。这种独特的结构可以调节膜的表面张力成分,使油滴的渗透速度更快。此外,sap作为一种高吸水性树脂,可以吸附油包水乳液中的纳米级水滴,从而提高膜的分离效率。对于CH2Cl2乳状液中的水,精心定制的纳米纤维膜完全去除了大于63 nm的水滴,渗透率在3.5 ×104 L∙m−2∙h−1∙bar−1以上,分离效率在98.8%以上,并且在有机溶剂中表现出良好的稳定性,在炼油方面具有很强的应用前景。
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引用次数: 0
Insights into the role of aromatic cationic surfactants in tailoring interfacial polymerization for high-performance reverse osmosis membranes 芳香族阳离子表面活性剂在高性能反渗透膜界面聚合中的作用
Pub Date : 2025-01-01 DOI: 10.1016/j.advmem.2025.100157
Jie Gao , Yongkai Xu , Nanxiang Wang , Dingxian Jia , Mingjie Wei , Shuang Hao , Yunxia Hu
Surfactant-mediated interfacial polymerization (IP) has been recognized as a promising strategy for accurately modulation of the structure and performance of polyamide (PA) reverse osmosis (RO) membranes. While aromatic cationic surfactants have demonstrated potential in regulating IP processes, the influence of their molecular structure on IP process and their incorporation integrated into the PA layer remain unexplored. This work systematically investigates two model surfactants—benzalkonium chloride (BAC, single benzene) versus benzethonium chloride (BEC, dual benzene)—as molecular regulators during PA layer formation. The results reveal that both aromatic cationic surfactants facilitate the diffusion of m-phenylenediamine (MPD) from the aqueous to the organic phase, enhancing PA cross-linking, while simultaneously embedding into the PA matrix to modulate surface properties. Notably, BEC, due to its distinctive dual-benzene-ring structure, exhibits a superior ability to accelerate MPD diffusion, triggering more pronounced Marangoni convection during IP, which contributes to a higher leaf-like structure area (0.017 ​μm2) of the resulting PA layer. Additionally, the strong π–π interaction between BEC and the PA network leads to a high embedding ratio of BEC within the membrane. Consequently, the BEC-regulated RO membranes demonstrate enhanced perm-selectivity, alongside improved antifouling and antibacterial properties. This study presents novel perspectives on the strategic design of cost-effective and high-performance fabrication methods for RO membranes, demonstrating substantial promise for industrial applications.
表面活性剂介导的界面聚合(IP)被认为是精确调节聚酰胺(PA)反渗透(RO)膜结构和性能的一种有前途的策略。虽然芳香族阳离子表面活性剂在调控IP过程中表现出潜力,但其分子结构对IP过程的影响及其与PA层的结合仍未被探索。本研究系统地研究了两种模型表面活性剂——苯扎氯铵(BAC,单苯)和苯扎氯铵(BEC,双苯)——在PA层形成过程中作为分子调节剂的作用。结果表明,这两种芳香族阳离子表面活性剂均能促进间苯二胺(MPD)从水相向有机相的扩散,增强PA交联,同时嵌入PA基质中调节其表面性质。值得注意的是,BEC由于其独特的双苯环结构,表现出更强的加速MPD扩散的能力,在IP过程中触发更明显的Marangoni对流,这使得得到的PA层具有更高的叶状结构面积(0.017 μm2)。此外,BEC与PA网络之间强烈的π -π相互作用导致BEC在膜内的高嵌入率。因此,becc调控的反渗透膜表现出增强的热选择性,以及改善的防污和抗菌性能。这项研究为反渗透膜的成本效益和高性能制造方法的战略设计提供了新的视角,展示了工业应用的巨大前景。
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引用次数: 0
Charge-selective nanoconfined boron nitride membranes for ultrafast and enhanced water decontamination 电荷选择性纳米氮化硼膜用于超快速和强化水净化
Pub Date : 2025-01-01 DOI: 10.1016/j.advmem.2025.100159
Wenjing Geng , Chuchu Cheng , Baoxin Ge , Yaohui Xu , Yufei Liu , Xinxin Ye , Caijin Huang , Weiwei Lei , Yang Wang , Dengrong Sun , Cheng Chen
Membrane separation techniques could address global water scarcity and ensure water safety. However, the unavoidable concentration polarization effect remains a formidable challenge. Here, we present a nanoconfined catalysis boron nitride membrane confining active nanoparticles to elaborately regulate molecular separation and pollutant degradation. For positively charged pollutant, the nanoconfined catalysis membrane demonstrates a water permeance reaching high up to 1549 ​L ​m−2 ​h−1 ​bar−1, which also substantially increases the removal efficiency of organic pollutants from 71.9 ​% to above 99.9 ​%. For negatively charged pollutant, the membrane achieves nearly 100 ​% reduction to p-aminophenol within 4.06 ms retention time across 100 operational cycles. Density functional theory calculation results further confirm the charge selection of nanoconfined catalysis boron nitride membranes for enhanced water decontamination. The superior performance of nanoconfined catalysis membranes arises from synergistically integrating stable 2D nanochannels, uniform catalytic layers, and controlled charge transfer, effectively mitigating concentration polarization in wastewater treatment.
膜分离技术可以解决全球水资源短缺问题,确保水安全。然而,不可避免的集中极化效应仍然是一个巨大的挑战。在这里,我们提出了一种纳米限制的催化氮化硼膜,限制活性纳米颗粒来精细地调节分子分离和污染物降解。对于带正电的污染物,纳米限制催化膜的透水性高达1549 L m−2 h−1 bar−1,有机污染物的去除率也从71.9%大幅提高到99.9%以上。对于带负电荷的污染物,在100个操作循环中,膜在4.06 ms的保留时间内实现了近100%的对氨基酚还原。密度泛函理论计算结果进一步证实了纳米限制催化氮化硼膜的电荷选择对水净化的增强作用。纳米约束催化膜的优异性能源于稳定的二维纳米通道、均匀的催化层和可控的电荷转移协同整合,有效缓解了废水处理中的浓度极化。
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引用次数: 0
Hierarchical structure control for ultra-high-flux helium separation membranes based on fluorinated polyimide materials 基于氟化聚酰亚胺材料的超高通量氦分离膜的分级结构控制
IF 9.5 Pub Date : 2025-01-01 DOI: 10.1016/j.advmem.2025.100166
Lixin Xing , Mengshi Wei , Jiaming Wang , Shiqi Huang , Wenji Zheng , Xiaobin Jiang , Shouhai Zhang , Gaohong He , Xuehua Ruan
Polyimide materials with multiple trifluoromethyl groups in repeating units, e.g., 6FDA-TFMB, have excellent intrinsic performance for membrane-based helium enrichment. Nevertheless, these fluorinated groups would seriously weaken cohesive energy density and then decelerate molecular chain aggregation in supersaturated solution. For asymmetric membrane fabrication using dry-wet phase inversion technology, this variation is negative to form dense and selective skin layer during solvent evaporation. In this research, EtOH, because it possesses low boiling point and little effect on solution stability, is utilized to enhance surface evaporation and accelerate polymer inspissation locally to construct defect-free skin layer. Meanwhile, formamide, because it could simultaneously motivate gelation and increase viscosity for polymer solution, is used to speed solidification during nonsolvent induced phase inversion, so that the transitional layer next to the surface could be formed instantaneously with artful sponge structure to consolidate and protect the nascent dense layer. The membrane casting solution is optimized with 22.0 ​wt% 6FDA-TFMB, 30.0 ​wt% EtOH, 3.0 ​wt% formamide, 31.5 ​wt% NMP, and 13.5 ​wt% THF, approximately. The defect-free dense layer could be thinner than 150 ​nm through this favorable formula. Besides, helium permeance is tested to be 760 GPU, the selectivity between helium and methane is tested to be 157, and the allowable operation pressure is higher than 4.0 MPaG, respectively. After adequate aging treatment, helium permeance is stabilized at 398 GPU, and the selectivity is increased to 239.5. On the whole, this work supplied an effective strategy to overcome the weakness in low cohesive energy density and construct highly fluorinated polyimide materials into excellent membranes with ultrathin and defect-free selective layer.
具有重复单元中多个三氟甲基的聚酰亚胺材料,如6FDA-TFMB,具有优异的膜基氦富集性能。然而,这些氟化基团会严重削弱内聚能密度,从而减缓过饱和溶液中的分子链聚集。对于使用干湿相转化技术的非对称膜制造,该变化是负的,在溶剂蒸发过程中形成致密和选择性的表皮层。本研究利用EtOH沸点低、对溶液稳定性影响小的特点,增强表面蒸发,局部加速聚合物凝聚,构建无缺陷的表皮层。同时,由于甲酰胺可以同时激发聚合物溶液的凝胶化和增加聚合物溶液的粘度,因此在非溶剂诱导的相变过程中,甲酰胺可以加速固化,从而可以在瞬间形成靠近表面的过渡层,并具有巧妙的海绵结构,以巩固和保护新生的致密层。优化后的膜铸造溶液中6FDA-TFMB约为22.0%,EtOH约为30.0%,甲酰胺约为3.0 wt%, NMP约为31.5%,THF约为13.5 wt%。该配方可使无缺陷致密层厚度小于150nm。氦气的渗透率测试为760 GPU,氦气与甲烷的选择性测试为157,允许操作压力分别高于4.0 MPaG。经过充分的时效处理,氦气渗透率稳定在398 GPU,选择性提高到239.5。总的来说,本工作为克服低内聚能密度的缺点,构建具有超薄、无缺陷选择层的高氟聚酰亚胺材料提供了一种有效的策略。
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引用次数: 0
Vapor permeation (VP) of water (H2O)/ acetic acid (AcOH) mixtures via bis(triethoxysily)ethane (BTESE) membranes 通过双(三乙氧基硅基)乙烷(BTESE)膜对水(H2O)/醋酸(AcOH)混合物进行蒸汽渗透(VP)
Pub Date : 2025-01-01 DOI: 10.1016/j.advmem.2025.100140
Suhaina Mohd Ibrahim , Kennedy Mawunya Hayibor , Xin Yu , Shigeru Miyata , Kengo Mishina , Feridoun Salak , Toshinori Tsuru , Ken-ichi Sawamura
Bis(triethoxysilyl)ethane (BTESE)-derived organosilica membranes prepared using sol-gel processing, were used in vapor permeation (VP) to dehydrate aqueous acetic acid (AcOH) solutions. It was discovered that BTESE-derived membranes had outstanding stability and great permselectivity. BTESE-derived organosilica membranes showed a H2O/AcOH separation factor of 3000–5800 and a H2O/AcOH permeance ratio of 3000–5800 with the permeate flux of 12–28 ​kg ​m−2 ​h−1 for H2O/AcOH mixtures (AcOH: 50 ​wt%) under 120 ​°C and 100 kPaA. The superior durability of organosilica membranes was confirmed by long-term stability tests conducted in aqueous AcOH mixtures, which indicates that BTESE membranes maintained almost the stable flux and separation factors. A comparison with gas permeation properties indicates that the molecular sieving effect dominates the separation mechanism.
采用溶胶-凝胶法制备了双(三乙氧基硅基)乙烷(BTESE)衍生有机硅膜,并将其用于蒸汽渗透(VP)脱水醋酸水溶液(AcOH)。结果表明,btese衍生膜具有良好的稳定性和选择性。在120°C和100 kPaA条件下,bte衍生的有机二氧化硅膜对H2O/AcOH混合物(AcOH: 50 wt%)的水/AcOH分离系数为3000-5800,水/AcOH渗透比为3000-5800,渗透通量为12-28 kg m−2 h−1。在AcOH水溶液中进行的长期稳定性试验证实了有机硅膜优越的耐久性,表明BTESE膜保持了几乎稳定的通量和分离因子。与气体渗透性能的比较表明,分子筛分作用在分离机理中起主导作用。
{"title":"Vapor permeation (VP) of water (H2O)/ acetic acid (AcOH) mixtures via bis(triethoxysily)ethane (BTESE) membranes","authors":"Suhaina Mohd Ibrahim ,&nbsp;Kennedy Mawunya Hayibor ,&nbsp;Xin Yu ,&nbsp;Shigeru Miyata ,&nbsp;Kengo Mishina ,&nbsp;Feridoun Salak ,&nbsp;Toshinori Tsuru ,&nbsp;Ken-ichi Sawamura","doi":"10.1016/j.advmem.2025.100140","DOIUrl":"10.1016/j.advmem.2025.100140","url":null,"abstract":"<div><div>Bis(triethoxysilyl)ethane (BTESE)-derived organosilica membranes prepared using sol-gel processing, were used in vapor permeation (VP) to dehydrate aqueous acetic acid (AcOH) solutions. It was discovered that BTESE-derived membranes had outstanding stability and great permselectivity. BTESE-derived organosilica membranes showed a H<sub>2</sub>O/AcOH separation factor of 3000–5800 and a H<sub>2</sub>O/AcOH permeance ratio of 3000–5800 with the permeate flux of 12–28 ​kg ​m<sup>−2</sup> ​h<sup>−1</sup> for H<sub>2</sub>O/AcOH mixtures (AcOH: 50 ​wt%) under 120 ​°C and 100 kPaA. The superior durability of organosilica membranes was confirmed by long-term stability tests conducted in aqueous AcOH mixtures, which indicates that BTESE membranes maintained almost the stable flux and separation factors. A comparison with gas permeation properties indicates that the molecular sieving effect dominates the separation mechanism.</div></div>","PeriodicalId":100033,"journal":{"name":"Advanced Membranes","volume":"5 ","pages":"Article 100140"},"PeriodicalIF":0.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143704147","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Integration of oxidation processes and ceramic membrane filtration for advanced water treatment: A review of foulant-membrane interactions 氧化过程和陶瓷膜过滤在深度水处理中的集成:污染物-膜相互作用的综述
Pub Date : 2025-01-01 DOI: 10.1016/j.advmem.2025.100138
Bin Lin , Xinyue Deng , Jiahao Chen , Ze-Xian Low , Zhaoxiang Zhong , Weihong Xing
Membrane filtration technology emerges as a robust and efficient solution in the global effort to alleviate water scarcity, offering a reliable means to deliver clean and safe drinking water. However, its effectiveness is compromised by severe membrane fouling, particularly under conditions of high organic load and prolonged operation. Integrating oxidation processes with ceramic membrane filtration offers promising solutions to these challenges, leveraging the excellent resistance of ceramic membranes to aggressive oxidation environments. Despite this, the complex interactions between ceramic membranes and organic foulants under various oxidation processes remain inadequately understood, yet they are pivotal in fouling dynamics. This review examines the integration of oxidation processes with ceramic membrane filtration systems. We focus on the fundamental mechanisms of molecular-scale interactions between ceramic membranes and organic foulants, which are crucial for developing effective strategies to mitigate fouling. Practical applications of the integrated processes in advanced water treatment are also discussed. We first examine the mechanisms underlying the unique surface chemistry of ceramic membranes and their interactions with organic foulants. We then explore the influence of oxidation processes on these interactions and fouling behaviour. Finally, we discuss the challenges and future prospects for expanding this integrated technology to broader applications in water decontamination and reuse.
膜过滤技术作为一种强大而有效的解决方案出现在全球缓解水资源短缺的努力中,提供了一种可靠的方法来提供清洁和安全的饮用水。然而,它的有效性受到严重的膜污染,特别是在高有机负荷和长时间运行的条件下。将氧化过程与陶瓷膜过滤相结合,为这些挑战提供了有希望的解决方案,利用陶瓷膜对侵略性氧化环境的优异抵抗力。尽管如此,在各种氧化过程中,陶瓷膜与有机污染物之间的复杂相互作用仍然没有得到充分的了解,但它们在污染动力学中是关键的。本文综述了氧化过程与陶瓷膜过滤系统的集成。我们关注陶瓷膜与有机污染物之间分子尺度相互作用的基本机制,这对于制定有效的减少污染的策略至关重要。讨论了综合工艺在深度水处理中的实际应用。我们首先研究了陶瓷膜独特的表面化学及其与有机污染物相互作用的机制。然后我们探讨氧化过程对这些相互作用和污染行为的影响。最后,我们讨论了将这种集成技术扩展到更广泛的水净化和再利用应用中的挑战和未来前景。
{"title":"Integration of oxidation processes and ceramic membrane filtration for advanced water treatment: A review of foulant-membrane interactions","authors":"Bin Lin ,&nbsp;Xinyue Deng ,&nbsp;Jiahao Chen ,&nbsp;Ze-Xian Low ,&nbsp;Zhaoxiang Zhong ,&nbsp;Weihong Xing","doi":"10.1016/j.advmem.2025.100138","DOIUrl":"10.1016/j.advmem.2025.100138","url":null,"abstract":"<div><div>Membrane filtration technology emerges as a robust and efficient solution in the global effort to alleviate water scarcity, offering a reliable means to deliver clean and safe drinking water. However, its effectiveness is compromised by severe membrane fouling, particularly under conditions of high organic load and prolonged operation. Integrating oxidation processes with ceramic membrane filtration offers promising solutions to these challenges, leveraging the excellent resistance of ceramic membranes to aggressive oxidation environments. Despite this, the complex interactions between ceramic membranes and organic foulants under various oxidation processes remain inadequately understood, yet they are pivotal in fouling dynamics. This review examines the integration of oxidation processes with ceramic membrane filtration systems. We focus on the fundamental mechanisms of molecular-scale interactions between ceramic membranes and organic foulants, which are crucial for developing effective strategies to mitigate fouling. Practical applications of the integrated processes in advanced water treatment are also discussed. We first examine the mechanisms underlying the unique surface chemistry of ceramic membranes and their interactions with organic foulants. We then explore the influence of oxidation processes on these interactions and fouling behaviour. Finally, we discuss the challenges and future prospects for expanding this integrated technology to broader applications in water decontamination and reuse.</div></div>","PeriodicalId":100033,"journal":{"name":"Advanced Membranes","volume":"5 ","pages":"Article 100138"},"PeriodicalIF":0.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143610951","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Preparation of high-performance pervaporation membranes for ethanol dehydration using a layer-by-layer self-assembly method 采用逐层自组装方法制备乙醇脱水用高性能渗透蒸发膜
Pub Date : 2025-01-01 DOI: 10.1016/j.advmem.2025.100132
Zhenhan Sun , Guoke Zhao , Gongqing Tang , Zhihu Zhao , Pei Li
To achieve fuel-grade purity (≥99.5 ​wt%), raw bioethanol needs to be purified. Adopting pervaporation membrane for bioethanol enrichment can greatly reduce the energy consumption compared with distillation. However, this requires the membrane having a high flux and high water to ethanol selectivity as well as good stability. In this study, a layer-by-layer self-assembled composite pervaporation membrane was prepared by alternately dip-coating polyallylamine hydrochloride (PAH) and sodium alginate (SA) solutions on the surface of a polyacrylonitrile (PAN) microfiltration membrane. The membrane flux and separation performance under different feed conditions are measured independently, and the results are mutually independent. These tests are conducted as short-term experiments to evaluate the membrane's separation performance under specific feed conditions. By optimizing the concentrations of PAH and SA, best separation performance of the composite membranes was obtained with a flux of 2.02 ​kg ​m−2 ​h−1 and a water to ethanol separation factor of 10993 using a 90 ​% ethanol water solution as feed at 70 ​°C. The composite membrane showed good stability in water. When keeping all other conditions unchanged, the feed ethanol concentration is adjusted to 50 ​wt%, the membrane flux increase to 12.61 ​kg ​m⁻2 ​h⁻1, and the water concentration in the permeate reach 99.7743 ​wt%.
为了达到燃料级纯度(≥99.5 wt%),原料生物乙醇需要纯化。采用渗透蒸发膜富集生物乙醇与精馏相比,可大大降低能耗。然而,这要求膜具有高通量和高水对乙醇的选择性以及良好的稳定性。在本研究中,通过在聚丙烯腈(PAN)微滤膜表面交替浸渍涂覆聚丙烯胺盐酸盐(PAH)和海藻酸钠(SA)溶液,制备了一层一层自组装的复合渗透蒸发膜。对不同进料条件下的膜通量和分离性能进行了独立的测定,结果是相互独立的。这些试验是作为短期实验进行的,以评估膜在特定进料条件下的分离性能。通过对PAH和SA的浓度进行优化,在70℃条件下,以90%乙醇水溶液为原料,在通量为2.02 kg m−2 h−1,水乙醇分离系数为10993的条件下,复合膜的分离性能最佳。复合膜在水中表现出良好的稳定性。在其他条件不变的情况下,将原料乙醇浓度调整到50 wt%,膜通量增加到12.61 kg m - 2 h - 1,渗透膜中的水浓度达到99.7743 wt%。
{"title":"Preparation of high-performance pervaporation membranes for ethanol dehydration using a layer-by-layer self-assembly method","authors":"Zhenhan Sun ,&nbsp;Guoke Zhao ,&nbsp;Gongqing Tang ,&nbsp;Zhihu Zhao ,&nbsp;Pei Li","doi":"10.1016/j.advmem.2025.100132","DOIUrl":"10.1016/j.advmem.2025.100132","url":null,"abstract":"<div><div>To achieve fuel-grade purity (≥99.5 ​wt%), raw bioethanol needs to be purified. Adopting pervaporation membrane for bioethanol enrichment can greatly reduce the energy consumption compared with distillation. However, this requires the membrane having a high flux and high water to ethanol selectivity as well as good stability. In this study, a layer-by-layer self-assembled composite pervaporation membrane was prepared by alternately dip-coating polyallylamine hydrochloride (PAH) and sodium alginate (SA) solutions on the surface of a polyacrylonitrile (PAN) microfiltration membrane. The membrane flux and separation performance under different feed conditions are measured independently, and the results are mutually independent. These tests are conducted as short-term experiments to evaluate the membrane's separation performance under specific feed conditions. By optimizing the concentrations of PAH and SA, best separation performance of the composite membranes was obtained with a flux of 2.02 ​kg ​m<sup>−2</sup> ​h<sup>−1</sup> and a water to ethanol separation factor of 10993 using a 90 ​% ethanol water solution as feed at 70 ​°C. The composite membrane showed good stability in water. When keeping all other conditions unchanged, the feed ethanol concentration is adjusted to 50 ​wt%, the membrane flux increase to 12.61 ​kg ​m⁻<sup>2</sup> ​h⁻<sup>1</sup>, and the water concentration in the permeate reach 99.7743 ​wt%.</div></div>","PeriodicalId":100033,"journal":{"name":"Advanced Membranes","volume":"5 ","pages":"Article 100132"},"PeriodicalIF":0.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402573","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Swelling polymer-regulated green synthesis of flexible ZIF-8 membrane 膨胀聚合物调控的柔性ZIF-8膜的绿色合成
Pub Date : 2025-01-01 DOI: 10.1016/j.advmem.2025.100144
Hongyu Ma , Ruoxin Wang , Kaiqiang He , Yaoxin Hu , George P. Simon , Huanting Wang
Metal-organic framework (MOF)-based membranes are promising for the development of high flux separation applications while maintaining high selectivities. Since pure MOF membranes typically suffer from brittleness, the fabrication of flexible MOF membranes with minimal defects and good mechanical strength is valuable. Herein, we report a swelling polymer-regulated method for the in situ green synthesis of a flexible zeolitic imidazolate framework-8 (ZIF-8) membrane for gas separation. By applying reactant solutions with different solvents in the contra-diffusion process, ZIF-8 particles were gradually grown with binding to alginate polymers. Moreover, the directional swelling of the composite layer allowed the selective layer to grow further into the pores of the substrate. This membrane demonstrated good structural integrity and mechanical stability whilst achieving an H2 permeance of 6.81 ​× ​10−7 ​mol ​m−2 ​s−1·pa−1 and an ideal H2/CH4 selectivity of 24, which was able to retain its gas separation performance after 10 mild bends. This approach thus shows great potential for the further development of other flexible MOF membranes.
金属有机骨架(MOF)基膜在保持高选择性的同时,具有发展高通量分离应用的前景。由于纯MOF膜通常具有脆性,因此制造具有最小缺陷和良好机械强度的柔性MOF膜是有价值的。在这里,我们报道了一种膨胀聚合物调节的方法,用于原位绿色合成用于气体分离的柔性沸石咪唑酸框架-8 (ZIF-8)膜。通过在反扩散过程中加入不同溶剂的反应物溶液,ZIF-8颗粒逐渐生长并与海藻酸盐聚合物结合。此外,复合层的定向膨胀允许选择层进一步生长到衬底的孔隙中。该膜具有良好的结构完整性和机械稳定性,H2透过率为6.81 × 10−7 mol m−2 s−1·pa−1,H2/CH4选择性为24,在10次轻微弯曲后仍能保持其气体分离性能。因此,这种方法为进一步开发其他柔性MOF膜显示了巨大的潜力。
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引用次数: 0
Size effect of porous filler in mixed matrix membranes for faster hydrogen permeation from methane-containing mixtures 混合基质膜中多孔填料对含甲烷混合物中氢更快渗透的尺寸效应
Pub Date : 2025-01-01 DOI: 10.1016/j.advmem.2025.100136
Yuebing Shen , Fanfan Jiang , Qian Liu , Zhiquan Chen , Kai Ge , Junfeng Bai , Jingui Duan
One potential solution for the transport of hydrogen (H2) is the injection of hydrogen into natural gas pipelines. Therefore, it is imperative to develop an efficient purification technology. Membrane separation has great potential to meet this challenge due to its effective energy consumption and cost. Here, a series of mixed matrix membranes (MMMs) containing ZIF-71 fillers of different sizes are reported for faster H2 permeation. The uniform distribution of nanosized ZIF-71 (0.1 ​μm) in 6FDA-DAM provides an attractive diffusion channel, allowing the membrane to show rapid H2 permeation of 1050 Barrer and good H2/CH4 separation factor of 43. This performance is markedly superior to that of the larger-sized ZIF-71 (1.0 ​μm and 3.5 ​μm) in 6FDA-DAM and the same-sized ZIF-71 (0.1 ​μm) in 6FDA-Durene and PEI, and also exceeds the upper bound. Moreover, the long-term stable H2/CH4 separation suggests a high potential for practical applications. The findings here demonstrate the importance of the filler size, which has a strong influence on the formation of mass transfer channels, and also provide straightforward method for the development of high-performance MMMs.
氢(H2)运输的一个潜在解决方案是将氢注入天然气管道。因此,开发一种高效的净化技术势在必行。膜分离因其有效的能耗和成本而具有很大的潜力来应对这一挑战。本文报道了一系列含有不同尺寸的ZIF-71填料的混合基质膜(MMMs),它们可以更快地渗透H2。纳米尺寸的ZIF-71 (0.1 μm)均匀分布在6FDA-DAM中,提供了一个有吸引力的扩散通道,使膜表现出1050 Barrer的快速H2渗透和43的良好H2/CH4分离系数。该性能明显优于6FDA-DAM中较大尺寸的ZIF-71 (1.0 μm和3.5 μm),以及6FDA-Durene和PEI中相同尺寸的ZIF-71 (0.1 μm),也超过了上界。此外,长期稳定的H2/CH4分离具有很高的实际应用潜力。研究结果表明,填料尺寸对传质通道的形成有重要影响,并为高性能mm材料的开发提供了直接的方法。
{"title":"Size effect of porous filler in mixed matrix membranes for faster hydrogen permeation from methane-containing mixtures","authors":"Yuebing Shen ,&nbsp;Fanfan Jiang ,&nbsp;Qian Liu ,&nbsp;Zhiquan Chen ,&nbsp;Kai Ge ,&nbsp;Junfeng Bai ,&nbsp;Jingui Duan","doi":"10.1016/j.advmem.2025.100136","DOIUrl":"10.1016/j.advmem.2025.100136","url":null,"abstract":"<div><div>One potential solution for the transport of hydrogen (H<sub>2</sub>) is the injection of hydrogen into natural gas pipelines. Therefore, it is imperative to develop an efficient purification technology. Membrane separation has great potential to meet this challenge due to its effective energy consumption and cost. Here, a series of mixed matrix membranes (MMMs) containing ZIF-71 fillers of different sizes are reported for faster H<sub>2</sub> permeation. The uniform distribution of nanosized ZIF-71 (0.1 ​μm) in 6FDA-DAM provides an attractive diffusion channel, allowing the membrane to show rapid H<sub>2</sub> permeation of 1050 Barrer and good H<sub>2</sub>/CH<sub>4</sub> separation factor of 43. This performance is markedly superior to that of the larger-sized ZIF-71 (1.0 ​μm and 3.5 ​μm) in 6FDA-DAM and the same-sized ZIF-71 (0.1 ​μm) in 6FDA-Durene and PEI, and also exceeds the upper bound. Moreover, the long-term stable H<sub>2</sub>/CH<sub>4</sub> separation suggests a high potential for practical applications. The findings here demonstrate the importance of the filler size, which has a strong influence on the formation of mass transfer channels, and also provide straightforward method for the development of high-performance MMMs.</div></div>","PeriodicalId":100033,"journal":{"name":"Advanced Membranes","volume":"5 ","pages":"Article 100136"},"PeriodicalIF":0.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143488712","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Hydrophobic DD3R modified by perfluorooctyl-trimethoxysilane incorporates into PEBAX membrane for ethanol recovery via pervaporation 经全氟辛基-三甲氧基硅烷修饰的疏水DD3R加入PEBAX膜,通过渗透蒸发回收乙醇
Pub Date : 2025-01-01 DOI: 10.1016/j.advmem.2025.100146
Chengyun Gao , Yuxuan Zhang , Junling Lin , Weijie Sun , Yangyang Wang , Fanhui Meng , Jiayou Liao , Xianjie Meng
A novel class of mixed-matrix membranes was synthesized through strategic integration of Polyether-block-amide (PEBAX) with Deca-dodecasil 3R (DD3R) zeolitic fillers, targeting efficiency-driven ethanol recovery in pervaporation separation systems. The DD3R molecular sieve was synthesized using adamantylamine (ADA) as a structure-directing agent and Sigma-1 seed crystals in a pure silicon precursor system. To improve compatibility with the polymer matrix, the DD3R particles were surface-modified with a silane coupling agent. Comprehensive characterization through Fourier Transform Infrared Spectroscopy (FTIR), Scanning Electron Microscopy (SEM), X-ray Photoelectron Spectra (XPS), Water Contact Angle (WCA), X-ray diffraction (XRD), swelling degree tests, and mechanical properties confirmed the successful bonding of the silane coupling agent to both DD3R and PEBAX. The optimized membrane containing 0.75 ​wt% DD3R achieved a flux of 1152.06 ​g/m2h and a separation factor of 4.52 ​at 60°C with a 5 ​wt% ethanol feed concentration, representing a 115 ​% enhancement in flux and a 68 ​% increase in separation factor compared to the pristine PEBAX membrane. Additionally, the PEBAX/DD3R membrane displayed excellent long-term stability. This work provided a foundation for developing membranes with DD3R incorporated therein for a wide range of liquid or gas mixture separation processes.
通过将聚醚嵌段酰胺(PEBAX)与十-十二烷基3R (DD3R)沸石填料的策略整合,合成了一类新型混合基质膜,旨在提高渗透蒸发分离系统中乙醇的效率。在纯硅前驱体体系中,以金刚胺(ADA)为结构导向剂和Sigma-1种子晶体合成了DD3R分子筛。为了提高与聚合物基体的相容性,用硅烷偶联剂对DD3R颗粒进行了表面改性。通过傅里叶变换红外光谱(FTIR)、扫描电镜(SEM)、x射线光电子能谱(XPS)、水接触角(WCA)、x射线衍射(XRD)、溶胀度测试和力学性能的综合表征,证实了硅烷偶联剂与DD3R和PEBAX的成功结合。在60°C、乙醇浓度为5 wt%的条件下,优化后的含0.75 wt% DD3R的膜通量为1152.06 g/m2h,分离系数为4.52,与原始PEBAX膜相比,通量提高了115%,分离系数提高了68%。此外,PEBAX/DD3R膜表现出优异的长期稳定性。这项工作为开发用于各种液体或气体混合物分离工艺的含有DD3R的膜提供了基础。
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引用次数: 0
期刊
Advanced Membranes
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