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Scalable synthesis of ultrathin MoS2 membranes for dye desalination 染料脱盐用超薄二硫化钼膜的规模化合成
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-08-09 DOI: 10.1016/j.memlet.2023.100058
Rodrigo Schneider , Ameya Manoj Tandel , Erda Deng , Daniel S. Correa , Haiqing Lin

Molybdenum disulfide (MoS2) has been fabricated into thin-film composite (TFC) membranes for dye desalination due to its excellent underwater stability and tunable interlay spacing. However, it remains challenging to synthesize thin layers of MoS2 with high water permeance and high dye rejection due to the difficulty in fabricating large crystalline sheets or exfoliation. Herein, we report a scalable method coupling bottom-up hydrothermal synthesis and top-down ultrasonic exfoliation to obtain well-dispersed MoS2 nanosheets and a vacuum filtration method to prepare ultrathin membranes (thickness: 30 – 60 nm) for dye desalination. The MoS2 nanosheets and membranes are thoroughly characterized for their chemistries and nanostructures. The membrane with 60-nm MoS2 exhibits water permeance of 32 LMH/bar, Na2SO4 rejection of 2.3%, and Direct Red-80 rejection of 99.0%. The MoS2 membranes exhibit dye desalination performance superior to state-of-the-art commercial polyamide membranes and many leading membranes based on two-dimensional materials.

二硫化钼(MoS2)具有良好的水下稳定性和可调的层间距,已被制备成用于染料脱盐的薄膜复合材料(TFC)膜。然而,由于难以制造大的结晶片或剥离,合成具有高透水性和高染料截留率的MoS2薄层仍然具有挑战性。在此,我们报道了一种可扩展的方法,将自下而上的水热合成和自上而下的超声剥离相结合,以获得分散良好的MoS2纳米片,以及一种真空过滤方法,以制备用于染料脱盐的超薄膜(厚度:30–60 nm)。对MoS2纳米片和膜的化学性质和纳米结构进行了全面表征。具有60nm MoS2的膜表现出32LMH/bar的透水性、2.3%的Na2SO4截留率和99.0%的Direct Red-80截留率。MoS2膜表现出优于最先进的商业聚酰胺膜和许多基于二维材料的领先膜的染料脱盐性能。
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引用次数: 0
In-situ rapid construction of aliphatic amine combined polyamide seawater reverse osmosis membrane for efficient boron removal 原位快速构建脂肪胺复合聚酰胺海水反渗透膜高效除硼
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-07-18 DOI: 10.1016/j.memlet.2023.100056
Can Li , Gwo Sung Lai , Yali Zhao , Rong Wang

Polyamide (PA) reverse osmosis membranes are commonly employed in seawater desalination owing to their effective salt rejection and water permeability; however, the elimination of small and neutral boron molecules from seawater remains a significant hurdle in energy-efficient and cost-effective desalination processes. In this work, a seawater reverse osmosis (SWRO) membrane with powerful boron removal competence was designed by adopting an in-situ rapid integration protocol, which utilized aliphatic amines as hydrophobic barriers by bonding the residual chloride groups upon the membrane surface and as molecular plugs by embedding in the PA networks. Consequently, it resulted in a notable improvement in the rejection of neutral boron molecules due to enhanced steric hindrance caused by immobilized amine plugs and synergistically tunned hydrophobic interactions. The permeability coefficient of boron decreased from 4.8 to 0.9 L m−2 h−1, and the boron rejection increased from 80.7 to 90.5% under the modification conditions with the optimal type and concentration of amines, while displaying a NaCl rejection of 99.8% and an acceptable water permeability of 0.55 L m−2 h−1 bar−1. Meanwhile, the alteration of membrane chemical compositions and structure properties was kept to a minimum. This study offers intuitive insights into the critical roles played by the aliphatic amines in the selective layer of the membrane for the removal of neutral boron molecules and salts, thereby enabling the fabrication of highly selective SWRO membranes, which may have significant implications for more efficient membrane-based seawater desalination and boron removal.

聚酰胺(PA)反渗透膜由于其有效的排盐性和透水性而通常用于海水淡化;然而,从海水中消除小的中性硼分子仍然是节能和成本效益高的海水淡化工艺中的一个重要障碍。在这项工作中,通过采用原位快速集成方案,设计了一种具有强大除硼能力的海水反渗透(SWRO)膜,该膜利用脂族胺作为疏水屏障,将残留的氯基团结合在膜表面,并通过嵌入PA网络作为分子塞。因此,由于固定化胺塞和协同调节的疏水相互作用引起的空间位阻增强,它显著改善了中性硼分子的排斥。在胺的最佳类型和浓度的改性条件下,硼的渗透系数从4.8降至0.9 L m−2 h−1,硼截留率从80.7%提高到90.5%,同时表现出99.8%的NaCl截留率和0.55 L m−1 h−1 bar−1的可接受透水性。同时,膜的化学组成和结构性能的变化保持在最低限度。这项研究为脂族胺在膜的选择性层中去除中性硼分子和盐所起的关键作用提供了直观的见解,从而使高选择性SWRO膜的制造成为可能,这可能对更有效的基于膜的海水淡化和硼去除具有重要意义。
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引用次数: 0
Opportunities for isoporous membranes in the manufacture of genomic medicines 异孔膜在基因组药物制造中的机会
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-07-06 DOI: 10.1016/j.memlet.2023.100052
Ke Meng , Thomas F. Johnson , Alberto Alvarez-Fernandez , Stefan Guldin , Daniel G. Bracewell

Viral and non-viral vectors have revolutionised in the last 5 years the approaches to tackling pandemics, cancers and genetic diseases. The intrinsic properties of these vectors present new separation challenges to their manufacture in terms of both the process-related impurities to be removed and the complex labile nature of the target products. These characteristics make them susceptible to heterogeneity and the formation of product-related impurities.

Conventional polyethersulfone membrane filters used for sterile filtration and ultrafiltration of viral vectors and lipid nanoparticles can display limited selectivity and cause product losses. To address these challenges, novel membrane materials and fabrication techniques to overcome the boundary of selectivity-permeability performance have become of interest. Isoporous membranes with well-defined pore size and pore dispersity at the nano-scale show promising separation performance but have only been demonstrated at small scales to date.

This review summarises the decision process for the development of new membrane candidates for vector manufacturing in genomic medicine, including membranes fabricated by lithography, track-etched membranes, anodic aluminium oxide (AAO) membranes and self-assembled block copolymer membranes. By comparing these membranes to existing commercially available products, the possible advantages presented by novel materials and fabrication approaches are identified.

在过去的5年里,病毒和非病毒载体彻底改变了应对流行病、癌症和遗传疾病的方法。这些载体的固有性质对其制造提出了新的分离挑战,既有要去除的工艺相关杂质,也有目标产物的复杂不稳定性质。这些特性使它们容易受到异质性和产品相关杂质形成的影响。用于病毒载体和脂质纳米颗粒的无菌过滤和超滤的常规聚醚砜膜过滤器可能显示出有限的选择性并导致产品损失。为了应对这些挑战,克服选择性-渗透性能边界的新型膜材料和制造技术已经引起了人们的兴趣。具有明确孔径和纳米级孔分散性的等孔膜显示出有希望的分离性能,但迄今为止仅在小规模上得到证明。这篇综述总结了开发用于基因组医学载体制造的新型候选膜的决策过程,包括通过光刻制造的膜、轨道蚀刻膜、阳极氧化铝(AAO)膜和自组装嵌段共聚物膜。通过将这些膜与现有的商业产品进行比较,确定了新型材料和制造方法可能带来的优势。
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引用次数: 0
Effect of surfactant structure on MPD diffusion for interfacial polymerization 表面活性剂结构对界面聚合中MPD扩散的影响
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-07-04 DOI: 10.1016/j.memlet.2023.100055
Shahriar Habib, Bryn E. Larson, Steven T. Weinman

Polyamide membranes made with surfactant-assisted interfacial polymerization (IP) have demonstrated the potential for excellent membrane performance. The presence of surfactants accelerates amine diffusion into the organic phase causing a more complete IP reaction. Even though surfactant-assisted IP has been used in polyamide membranes, the structure-property relationship of the surfactants on amine transport into the organic phase has not been explored in a systematic manner. In this work, MPD diffusion from a membrane support into n-dodecane in the presence of seven different surfactants, which were anionic, cationic, and non-ionic, was evaluated. When the surfactants were used at different concentrations, the MPD concentration was increased in the presence of anionic (48–80%), cationic (32–75%) and non-ionic (26%) surfactants. The MPD concentration was increased in the presence of anionic (by 48–72%), cationic (by 32–75%), and non-ionic surfactants (by 26%) at 15–60 s contact time. For further understanding, the interfacial tension in n-dodecane for the surfactants was measured, however, it did not correlate with our data. This study provides a better understanding of MPD diffusion in the presence of different types of surfactants during RO membrane synthesis, which will help us to engineer membranes with better permeability and selectivity.

表面活性剂辅助界面聚合(IP)制备的聚酰胺膜已显示出优异膜性能的潜力。表面活性剂的存在加速了胺向有机相中的扩散,导致更完全的IP反应。尽管表面活性剂辅助的IP已用于聚酰胺膜,但表面活性剂对胺向有机相中传输的结构-性质关系尚未得到系统的探索。在这项工作中,评估了在阴离子、阳离子和非离子七种不同表面活性剂存在下,MPD从膜载体扩散到正十二烷中。当表面活性剂以不同浓度使用时,在阴离子(48–80%)、阳离子(32–75%)和非离子(26%)表面活性剂的存在下,MPD浓度增加。在阴离子(48–72%)、阳离子(32–75%)和非离子表面活性剂(26%)存在的情况下,MPD浓度在15–60 s的接触时间内增加。为了进一步理解,测量了表面活性剂在正十二烷中的界面张力,然而,它与我们的数据无关。这项研究更好地了解了在反渗透膜合成过程中,不同类型表面活性剂存在下MPD的扩散,这将有助于我们设计具有更好渗透性和选择性的膜。
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引用次数: 1
Epoxide-based TFC membranes with tunable performance in the tight nanofiltration range 在紧密纳滤范围内具有可调性能的环氧化物基TFC膜
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-07-04 DOI: 10.1016/j.memlet.2023.100054
Rhea Verbeke , Douglas M. Davenport , Caroline Bogaerts , Samuel Eyley , Wim Thielemans , Ivo F.J. Vankelecom

Membrane technology offers promise as a breakthrough separation technology in many applications, but is frequently limited by the chemical stability of currently available membrane materials. Recently developed membranes utilizing epoxide-based chemistry have shown great potential as intrinsically stable thin-film composite membranes in water-based applications. However, as these membranes are in their infancy, many synthesis parameters are still to be explored. In this study, the versatility of epoxide chemistry is exploited to demonstrate its potential to serve as a new platform for membrane synthesis, even beyond the field of aqueous applications. It is proven here how the membrane performance can be tailored in a controllable way between 20 – 85% NaCl rejection with a water permeance between 0.5 – 3 L m−2 h−1 bar−1 by simply selecting epoxide monomers and initiators of different size and functionality. A systematic increase in water permeance and salt passage was observed for epoxide monomers that exhibit a lower functionality and a lower number of aromatic groups, while a threshold nucleophilicity and aliphatic chain length of the initiator are required to obtain a salt-selective layer. This work demonstrates the possibility to easily and predictably tune membrane performance in the tight nanofiltration range, while simultaneously achieving a better understanding of the synthesis-structure-performance relationship of this new class of promising membranes.

膜技术有望成为许多应用中的突破性分离技术,但经常受到目前可用膜材料化学稳定性的限制。最近开发的利用环氧基化学的膜在水性应用中显示出作为本质稳定的薄膜复合膜的巨大潜力。然而,由于这些膜还处于起步阶段,许多合成参数仍有待探索。在这项研究中,环氧化物化学的多功能性被用来证明其作为膜合成新平台的潜力,甚至超越了水应用领域。这里证明了如何通过简单地选择不同尺寸和功能的环氧化物单体和引发剂,在20–85%的NaCl截留率和0.5–3 L m−2 h−1 bar−1的透水率之间,以可控的方式调整膜性能。对于表现出较低官能度和较低芳族基团数的环氧化物单体,观察到透水性和盐通道的系统性增加,同时需要引发剂的阈值亲核性和脂肪族链长度来获得盐选择性层。这项工作证明了在严格的纳滤范围内容易且可预测地调节膜性能的可能性,同时更好地理解这类有前途的新型膜的合成结构-性能关系。
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引用次数: 0
Mixed-linker MOF-303 membranes for pervaporation 混合连接MOF-303膜渗透蒸发
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-06-28 DOI: 10.1016/j.memlet.2023.100053
Fang-Hsuan Hu , Li-Tang Chi , Guan-Bo Syu , Tsyr-Yan Yu , Ming-Pei Lin , Jiun-Jen Chen , Wen-Yueh Yu , Dun-Yen Kang

Metal-organic frameworks (MOFs) hold great promise as porous materials for pervaporation applications. However, the exploration of MOF membranes in this field is still in its early stages. One of the main challenges is the relatively low mass flux and stability of pure MOF membranes compared to other materials used in pervaporation. In this study, we propose a novel approach to enhance the separation performance of MOF membranes for water and ethanol separation. Our strategy involves incorporating the 2,5-thiophenedicarboxylic acid (TDC) linker into the MOF-303 structure, partially replacing the 3,5-pyrazoledicarboxylic acid (PDC) linker. The goal is to increase the aperture size of the microporous channels in the pristine MOF-303 membrane, thereby improving the mass flux. X-ray diffraction characterization, combined with Rietveld refinement, confirmed that the partial substitution of PDC with TDC resulted in an increased pore-limiting diameter (PLD) of MOF-303. For instance, the pristine MOF-303 exhibited a PLD of 5.78 Å, while MOF-303(70/30) with 70% TDC replacement displayed a PLD of 6.02 Å. To fabricate the mixed-linker MOF-303 membranes, we utilized a seeded growth method, which yielded membranes with dense layers, as confirmed by scanning electron microscopy and air permeation characterization. The prepared membranes were subjected to pervaporation tests to evaluate their performance in separating 90 wt.% ethanol at 60 °C. The pristine MOF-303 membrane exhibited notable separation capabilities, with an average flux of 0.071 kg·m−2·hr−1 and a water/ethanol separation factor of 5371. Surpassing the unmodified MOF-303, the mixed-linker MOF-303(50/50) membrane demonstrated improved mass flux and water/ethanol separation factor. Specifically, the MOF-303(50/50) membrane displayed an average flux of 0.092 kg·m−2·hr−1 and a water/ethanol separation factor of 8500. Importantly, the unmodified MOF-303 membrane exhibited instability during prolonged pervaporation operation, whereas the mixed-linker MOF-303(50/50) membrane effectively addressed this issue. Further analysis using in situ Fourier transform infrared spectroscopy and water adsorption characterization revealed that MOF-303(50/50) possessed a strong affinity for water, comparable to the pristine MOF-303. Overall, our study highlights the potential of the mixed-linker approach to optimize the separation performance and stability of MOF-based membranes for pervaporation application.

金属有机框架(MOFs)作为渗透蒸发应用的多孔材料具有很大的前景。然而,MOF膜在该领域的探索仍处于早期阶段。主要挑战之一是与渗透蒸发中使用的其他材料相比,纯MOF膜的质量通量和稳定性相对较低。在本研究中,我们提出了一种新的方法来提高MOF膜在水和乙醇分离中的分离性能。我们的策略包括将2,5-噻吩二羧酸(TDC)连接体结合到MOF-303结构中,部分取代3,5-吡唑二羧酸(PDC)连接体。目标是增加原始MOF-303膜中微孔通道的孔径大小,从而提高质量通量。X射线衍射表征,结合Rietveld细化,证实PDC与TDC的部分取代导致MOF-303的孔极限直径(PLD)增加。例如,原始MOF-303的PLD为5.78Å,而具有70%TDC置换的MOF-303(70/30)的PLD则为6.02Å。为了制备混合连接体MOF-303膜,我们使用了种子生长方法,该方法产生了具有致密层的膜,如扫描电子显微镜和空气渗透表征所证实的。对制备的膜进行渗透蒸发测试,以评估它们在分离90重量%中的性能60°C下的乙醇。原始MOF-303膜表现出显著的分离能力,平均通量为0.071 kg·m−2·hr−1,水/乙醇分离因子为5371。超过未改性的MOF-303,混合连接体MOF-303(50/50)膜表现出改进的质量通量和水/乙醇分离因子。具体而言,MOF-303(50/50)膜的平均通量为0.092 kg·m−2·hr−1,水/乙醇分离系数为8500。重要的是,未改性的MOF-303膜在长时间的渗透蒸发操作中表现出不稳定性,而混合连接体MOF-303(50/50)膜有效地解决了这个问题。使用原位傅立叶变换红外光谱和水吸附表征的进一步分析表明,MOF-303(50/50)对水具有很强的亲和力,与原始MOF-303相当。总之,我们的研究强调了混合连接体方法在优化渗透蒸发应用中基于MOF的膜的分离性能和稳定性方面的潜力。
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引用次数: 4
Engineering Ultra-Permeable and Antifouling Water Channel-based Biomimetic Membranes toward Sustainable Water Purification 面向可持续水净化的工程超透防污水渠仿生膜
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-06-12 DOI: 10.1016/j.memlet.2023.100049
Xuesong Li , Linyan Yang , Jaume Torres , Rong Wang

Water channel-based biomimetic membranes (WBMs) are gaining increasing attention due to the effectiveness of water channels in enhancing water permeability and breaking the permselectivity trade-off. However, the ultra-permeable WBMs may suffer from severe membrane fouling issue because a high-water flux tends to result in an accelerated fouling and thus compromises the benefits gained from the usage of water channels. Herein, a novel in-situ modification protocol was proposed to enhance the antifouling performance of ultra-permeable WBMs. The nanovesicles incorporated with aquaporin (AQP) water channels were functionalized with polyethylene glycol brushes (i.e., PEGylation) via a facile self-assembly approach and subsequently encapsulated in the selective layer of thin-film composite membranes through interfacial polymerization. The modification had minimal impact on the function of AQPs, resulting in WBMs with a high water permeance (∼8.2 LMH/bar) and good NaCl rejection (96.4%) comparable to the unmodified WBMs. Moreover, the in-situ modification drastically enhanced the surface hydrophilicity, which endowed the membrane with a superior fouling resistance to organic foulants. The improved fouling resistance ensured a more sustainable operation of ultra-permeable WBMs, particularly in scenarios that favor high water fluxes. This facile modification strategy provides an efficient way to fabricate ultra-permeable and antifouling WBMs for sustainable water purification.

基于水道的仿生膜(WBM)由于水道在提高透水性和打破渗透选择性权衡方面的有效性而越来越受到关注。然而,超渗透WBM可能会遇到严重的膜污染问题,因为高的水通量往往会导致加速污染,从而损害从使用水道中获得的好处。本文提出了一种新的原位改性方案,以提高超渗透WBM的防污性能。通过简单的自组装方法,用聚乙二醇刷(即聚乙二醇化)对掺入水通道蛋白(AQP)水通道的纳米囊泡进行功能化,然后通过界面聚合将其封装在薄膜复合膜的选择性层中。改性对AQP功能的影响最小,导致WBM具有高透水性(~8.2LMH/bar)和良好的NaCl截留率(96.4%),与未改性的WBM相当。此外,原位改性大大提高了膜的表面亲水性,使膜对有机污染物具有优异的防污性能。防污性的提高确保了超渗透WBM的更可持续的运行,特别是在有利于高水通量的情况下。这种简单的改性策略为制造用于可持续水净化的超渗透和防污WBM提供了一种有效的方法。
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引用次数: 0
Orientation matters: Measuring the correct surface of polyamide membranes with quartz crystal microbalance 取向问题:用石英晶体微天平测量聚酰胺膜的正确表面
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-06-10 DOI: 10.1016/j.memlet.2023.100048
Luis Francisco Villalobos , Kevin E. Pataroque , Weiyi Pan , Tianchi Cao , Masashi Kaneda , Camille Violet , Cody L. Ritt , Eric M.V. Hoek , Menachem Elimelech

The surface of polyamide reverse osmosis (RO) membranes which regulates interface-dominated phenomena, such as partitioning and fouling, is the one facing the feed during operation. However, the opposite surface of the polyamide selective layer, the one facing the permeate and in contact with the polysulfone porous support, is commonly analyzed in quartz crystal microbalance (QCM) measurements due to limitations of state-of-the-art transfer methodologies. Such measurements on the back surface cannot be generalized because the polyamide layer is chemically and morphologically asymmetric. Herein, we introduce a simple method to coat QCM sensors with polyamide active layers in the correct orientation (i.e., exposing their front surface) and show that interface-dominated phenomena differ significantly between orientations. We start by describing a transfer protocol to coat any surface with a polyamide layer on its front surface orientation. We then systematically analyze the chemical and morphological differences between the two surfaces of the polyamide layer of a commercial RO membrane. Finally, we demonstrate that interface-dominated phenomena depend on the orientation by showing that NaCl partitioning at pH 6 was 1.3 to 2.3-fold higher on the front surface and that organic fouling with humic acid occurred at a lower rate on this surface. The new method presented herein enables measurements on the front surface of polyamide RO membranes, which should be the standard in any future QCM studies.

聚酰胺反渗透(RO)膜的表面是操作过程中面对进料的表面,它调节界面主导的现象,如分配和结垢。然而,由于最先进的转移方法的限制,聚酰胺选择层的相对表面,即面向渗透物并与聚砜多孔载体接触的表面,通常在石英晶体微天平(QCM)测量中进行分析。由于聚酰胺层在化学和形态上是不对称的,因此不能对背面的这种测量进行推广。在此,我们介绍了一种简单的方法,以正确的取向(即暴露其前表面)在QCM传感器上涂覆聚酰胺活性层,并表明界面主导的现象在不同的取向之间存在显著差异。我们首先描述了在任何表面的前表面方向上涂覆聚酰胺层的转移协议。然后,我们系统地分析了商业反渗透膜聚酰胺层两个表面之间的化学和形态差异。最后,我们证明了界面主导的现象取决于取向,表明在pH 6时,NaCl在前表面的分配高1.3至2.3倍,而腐殖酸在该表面的有机污染发生率较低。本文提出的新方法能够对聚酰胺反渗透膜的前表面进行测量,这应该是未来任何QCM研究的标准。
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引用次数: 0
Helium recovery from natural gas over CC3 membranes 利用CC3膜从天然气中回收氦气
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-05-01 DOI: 10.1016/j.memlet.2023.100042
Keerthana Krishnan, Ashley L. Potter, Carolyn A. Koh, Moises A. Carreon

Although helium is a valuable inert gas available in abundance in the earth's atmosphere, the major source of helium is from natural gas reservoirs. Membrane based separation processes pose many advantages like being cost effective and non-energy intensive. In this current study, we have successfully demonstrated the synthesis of continuous Porous Organic Cage: CC3 membranes to separate equimolar helium methane mixture with permeance of 4.45 × 10−7 mol/ (m2s Pa) and separation selectivity (α) as high as 8. We also compared the diffusion coefficients of the gases through the membrane to evaluate the dominant mechanism for separation. Lastly, we compared the performance of our membranes to the state-of-the-art membranes with the help of a Robeson plot and found that our membranes outperformed the upper bound.

尽管氦是地球大气层中丰富的一种有价值的惰性气体,但氦的主要来源是天然气藏。基于膜的分离工艺具有许多优点,如成本效益和非能源密集型。在本研究中,我们成功地合成了连续多孔有机笼:CC3膜,用于分离等摩尔氦-甲烷混合物,其渗透率为4.45×10−7 mol/(m2s Pa),分离选择性(α)高达8。我们还比较了气体通过膜的扩散系数,以评估分离的主要机制。最后,我们借助罗伯逊图将我们的膜的性能与最先进的膜进行了比较,发现我们的膜优于上限。
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引用次数: 0
Sulfur-resistant MoO2/TS-1 zeolite armored PdCu alloy composite membrane for hydrogen separation under H2S containing steam 耐硫MoO2/TS-1沸石铠装PdCu合金复合膜在含H2S蒸汽下的氢分离
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-05-01 DOI: 10.1016/j.memlet.2023.100037
Chenyang Zhao , Yujia Liu , Hui Li , Fei An , Wei Xu , Zhe Yang , Bing Sun

Sulfur poisoning could result in fast deterioration of Pd-based membranes by the formation of metal sulfides and reduction of hydrogen purity. The introduction of an MoO2/TS-1 layer could provide an effective protection of the Pd layer. Therefore, in this paper a synthetic method is presented for preparation of sulfur-resistant MoO2/TS-1 zeolite modified PdCu alloy composite membranes and their application in hydrogen separation under H2S containing steam. According to the stability test results, the MoO2/TS-1 zeolite armored layer obviously prolonged the stability of Pd based membrane. After 50 h stability test with 100 ppm H2S, there were no obvious structural changes and metal sulfide formation detected in the PdCu bulk from SEM images and XRD patterns, indicating that MoO2/TS-1 armor structure was good enough for protecting the PdCu alloy bulk.

硫中毒可通过金属硫化物的形成和氢纯度的降低导致钯基膜的快速劣化。MoO2/TS-1层的引入可以提供对Pd层的有效保护。因此,本文提出了一种制备抗硫MoO2/TS-1沸石改性PdCu合金复合膜的合成方法,并将其应用于含H2S蒸汽中的氢气分离。稳定性测试结果表明,MoO2/TS-1分子筛包覆层明显提高了钯基膜的稳定性。在用100ppm H2S进行50小时稳定性测试后,从SEM图像和XRD图谱中,PdCu本体中没有检测到明显的结构变化和金属硫化物的形成,表明MoO2/TS-1装甲结构足以保护PdCu合金本体。
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引用次数: 2
期刊
Journal of Membrane Science Letters
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