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Mechanisms determining water permeability and ion selectivity of multilayered glycine-functionalized graphene oxide membranes in saline water reverse osmosis processes: A computational investigation 决定盐水反渗透过程中多层甘氨酸功能化氧化石墨烯膜透水性和离子选择性的机理:计算研究
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-23 DOI: 10.1016/j.memsci.2024.123361
K. Karatasos , G.S. Fanourgakis , I. Zuburtikudis , Hadil Abu Khalifeh
Non-Equilibrium Molecular Dynamics simulations were performed to examine in detail the mechanisms involved in a reverse osmosis process for the removal of monovalent (Na+, Cl) and divalent (Mg2+) ions from saline water, using multilayered glycine-functionalized graphene oxide (GO) membranes. We varied parameters such as the degree of functionalization of the GO flakes and the structural flexibility of the membranes and examined their performance in a wide range of applied pressure gradients. In all models examined, water permeability was found to be almost 2 orders of magnitude larger compared to that in conventional reverse osmosis (RO) membranes. High structural flexibility of the membranes was found to increase water permeability due to the formation of additional nanochannels that favor faster water transport. Functionalization of the GO flakes by the glycinate groups resulted in a decrease in water permeability due to the formation of a denser hydrogen-bonding network within the membranes. Three main mechanisms were identified regarding ion selectivity. Due to the overall negative charge of the membranes, the strong adsorption of the Mg2+ ions onto the GO flakes resulted in their full rejection. Weaker adsorption of the Na+ ions led only to their partial rejection. At the same time, the electrostatic repulsion of the Cl ions by the membranes was found to result in almost full removal levels at high pressure gradients. The rejection of the monovalent ions was found to decrease with the structural flexibility of the membranes and increase with the functionalization of the GO flakes, in response to the changes observed in water permeability on these membrane modifications. The pressure-dependent deformability of the structurally flexible membranes combined with charge accumulation close to the membrane's entrance, resulted in a non-monotonic dependence of the monovalent ion rejection on the applied pressure difference.
我们利用多层甘氨酸功能化氧化石墨烯(GO)膜进行了非平衡分子动力学模拟,详细研究了从盐水中去除一价(Na+、Cl-)和二价(Mg2+)离子的反渗透过程所涉及的机理。我们改变了 GO 薄片的功能化程度和膜的结构柔韧性等参数,并考察了它们在各种应用压力梯度下的性能。在所有研究的模型中,我们发现与传统的反渗透膜相比,透水性几乎大了两个数量级。由于形成了更多的纳米通道,有利于加快水的传输速度,因此发现膜的高结构柔性提高了透水性。甘氨酸基团对 GO 薄片进行官能化后,由于膜内形成了更密集的氢键网络,从而降低了透水性。在离子选择性方面发现了三种主要机制。由于膜的整体带负电荷,Mg2+ 离子在 GO 薄片上的强吸附性导致其被完全排斥。对 Na+ 离子的吸附较弱,只能将其部分排斥。同时,在高压梯度下,膜对 Cl- 离子的静电排斥几乎达到了完全去除的水平。研究发现,膜对单价离子的排斥作用会随着膜结构的灵活性而降低,并随着 GO 片的功能化而增加,这与在这些膜改性时观察到的水渗透性变化是一致的。结构柔性膜随压力变化的变形能力加上靠近膜入口处的电荷积累,导致单价离子排斥量与所施加的压力差呈非单调关系。
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引用次数: 0
Preparation of mixed matrix membranes with PVP-induced fluorinated Zr-MOF for high-efficiency hydrogen purification under high humidity conditions 制备具有 PVP 诱导氟化 Zr-MOF 的混合基质膜,用于高湿度条件下的高效氢气纯化
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-22 DOI: 10.1016/j.memsci.2024.123351
Xinya Wang , Weiqiu Huang , Xufei Li , Xiaotong Li , Xinhan Chai , Yankang Zhou , Jing Zhong , Rongfei Zhou
Given that hydrogen production often involves impurities such as CO2, CH4, H2O, and alkanes, hydrogen purification is crucial for global green energy applications. Mixed matrix membranes (MMMs) using metal-organic framework (MOF) materials offer a non-thermal, energy-efficient method for hydrogen purification. These membranes have controllable structures and promote environmental sustainability. However, challenges such as filler aggregation and matrix-filler incompatibility during the preparation of MOF-MMMs are difficult to avoid and can adversely affect separation performance. In this study, 4-(trifluoromethyl) benzoic acid (4-TFMBA) was introduced in situ to grow synchronously with polyvinyl pyrrolidone (PVP) on UiO-66-NH2, forming a hydrophobic bifunctional nanoparticle composite, PVP-Zr-MOF-F. Furthermore, in situ loading of PVP-Zr-MOF-F onto a PVDF polymer matrix was achieved using a wet method and the NIPS technique to prepare PVP-Zr-MOF-F@PVDF. The introduction of 4-TFMBA, with highly electronegative F atoms, enhances hydrophobicity and increases H2 affinity through polarization and hydrogen bonding induced by C–F bonds. PVP promotes the formation of smaller Zr-MOF particles, increases the proportion of small pores, prevents aggregation, and acts as a pore-forming agent, facilitating the in situ loading and dispersion of PVP-Zr-MOF-F within PVDF chains. This bifunctionalization not only improves the compatibility and dispersion of the nanofillers but also increases the number of small pores, enhancing van der Waals forces and confinement effects on H2 molecules, making it suitable for gas separation under humid conditions. The results indicate that the H2 permeance of PVP2–Zr-MOF-F@PVDF can reach 114,735 GPU, with selectivities of 19, 21, 24, and 120 for H2/CO2, H2/CH4, H2/C2H4, and H2/n-C6H14, respectively, surpassing the 2008 Robeson's upper bound. Notably, under high humidity conditions, the selectivities for H2/CO2, H2/CH4, and H2/n-C6H14 are 1566 %, 1891 %, and 3264 % higher than those of the original PVDF membrane, achieving high selectivity separation. Additionally, after repetitive experiments with varying humidity, the membrane's selectivity remained almost unchanged, demonstrating the high hydrothermal stability of PVP2–Zr-MOF-F@PVDF. This research provides a new reference for hydrogen purification and holds significant implications for the sustainable development of green energy.
由于制氢过程中经常会产生二氧化碳、甲烷、水和烷烃等杂质,因此氢气纯化对全球绿色能源应用至关重要。使用金属有机框架(MOF)材料的混合基质膜(MMM)为氢气纯化提供了一种非热、高能效的方法。这些膜具有可控结构,促进了环境的可持续发展。然而,在制备 MOF-MMMs 的过程中,填料聚集和基质-填料不相容等难题难以避免,并可能对分离性能产生不利影响。本研究在 UiO-66-NH2 上原位引入 4-(三氟甲基)苯甲酸(4-TFMBA)与聚乙烯吡咯烷酮(PVP)同步生长,形成疏水双功能纳米粒子复合材料 PVP-Zr-MOF-F。此外,还采用湿法和 NIPS 技术将 PVP-Zr-MOF-F 原位负载到 PVDF 聚合物基体上,制备出 PVP-Zr-MOF-F@PVDF。4-TFMBA 具有高电负性的 F 原子,它的引入增强了疏水性,并通过 C-F 键引起的极化和氢键增加了 H2 亲和力。PVP 可促进形成更小的 Zr-MOF 颗粒,增加小孔的比例,防止聚集,并作为孔形成剂,促进 PVP-Zr-MOF-F 在 PVDF 链中的原位装载和分散。这种双官能化不仅提高了纳米填料的相容性和分散性,还增加了小孔的数量,增强了对 H2 分子的范德华力和约束效应,使其适用于潮湿条件下的气体分离。结果表明,PVP2-Zr-MOF-F@PVDF 的 H2 渗透率可达 114,735 GPU,对 H2/CO2、H2/CH4、H2/C2H4 和 H2/n-C6H14 的选择性分别为 19、21、24 和 120,超过了 2008 年 Robeson 的上限。值得注意的是,在高湿度条件下,H2/CO2、H2/CH4 和 H2/n-C6H14 的选择性分别比原来的 PVDF 膜高出 1566 %、1891 % 和 3264 %,实现了高选择性分离。此外,在不同湿度下重复实验后,膜的选择性几乎保持不变,这表明 PVP2-Zr-MOF-F@PVDF 具有很高的水热稳定性。这项研究为氢气提纯提供了新的参考,对绿色能源的可持续发展具有重要意义。
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引用次数: 0
Interfacial demulsification and antifouling of oil/water separation membrane by dynamically self-releasing hydroxide ions 动态自释放氢氧根离子对油水分离膜的界面破乳和防污作用
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-21 DOI: 10.1016/j.memsci.2024.123341
Hui Li , Shaopeng Gan , Jianqiang Zhang , Kangxing Wei , Xu Zhu , Xilu Liu , Lei Zhu , Hongbo Zeng , Qingzhong Xue
Advanced membranes are urgently needed in concentration, purification and separation of various industrial emulsions. However, their performance is impeded by issues such as membrane fouling and the inherent trade-off between separation efficiency and permeation flux. In this work, an interfacial demulsification and antifouling membrane was achieved through self-releasing high concentration of hydroxide ions on the membrane surface in a dynamic manner. These hydroxide ions can facilitate the emulsified oil droplets on the membrane surface to demulsify by greatly decreasing their Debye length and suppressing their electric double layer repulsion. In this way, the emulsified oil droplets could aggregate into large ones and rapidly detach from the membrane surface, mitigating the challenges of membrane fouling and trade-off. Thus, the membrane exhibits outstanding antifouling ability, achieving high efficiency (99.79 %) and flux (3046 L m−2 h−1 bar−1) in long-term oil/water emulsion separation. This ionic self-releasing membrane is easy to manage, requires no reagent consumption, and causes no pollution. This work provides a promising solution and valuable insights into membrane separation and emulsion-related systems.
各种工业乳液的浓缩、净化和分离迫切需要先进的膜。然而,膜污垢和分离效率与渗透通量之间的固有权衡等问题阻碍了膜的性能。在这项工作中,通过以动态方式在膜表面自释放高浓度氢氧根离子,实现了界面破乳和防污膜。这些氢氧根离子可大大降低膜表面乳化油滴的德拜长度,抑制其双电层斥力,从而促进乳化油滴的破乳化。这样,乳化油液滴就能聚集成大液滴,并迅速从膜表面脱离,从而减轻膜堵塞和折衷的难题。因此,该膜具有出色的防污能力,在长期油/水乳液分离中实现了高效率(99.79 %)和高通量(3046 L m-2 h-1 bar-1)。这种离子自释放膜易于管理,无需消耗试剂,不会造成污染。这项研究为膜分离和乳化液相关系统提供了一种前景广阔的解决方案和宝贵的见解。
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引用次数: 0
Real-time non-destructive monitoring of supported liquid membranes using electrochemical impedance spectroscopy 利用电化学阻抗谱对支撑液体膜进行实时无损监测
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-21 DOI: 10.1016/j.memsci.2024.123360
Hiroki Fukuda, Jongho Lee
The degradation of supported liquid membranes (SLMs) due to membrane liquid leaching has been a hurdle for their implementation in resource recovery from waste streams. We present a novel approach utilizing four-electrode mode electrochemical impedance spectroscopy (EIS) for real-time, non-destructive monitoring of SLM degradation, providing detailed analysis of SLM's structural changes. We first showed that SLMs may be depicted as an electrical circuit of resistors and capacitors by EIS. The EIS then revealed that SLM degradation progressed over four different phases as a result of varying rates of thickness and area reduction of the SLM. To demonstrate the effectiveness of EIS-based diagnosis, we prepared SLMs designed for selective medium-chain fatty acid (MCFA) extraction in intact, partially, and completely degraded states, determined by the EIS. The intact SLM showed a high selectivity (∼50) for MCFAs over short-chain fatty acids. The selectivity decreased to ∼22 in the partially degraded SLMs, and less than 1 in the completely degraded SLM, indicating the clear linkage between the degree of degradation and the separation performance. Our four-electrode mode EIS method is expected to serve as a key tool for efficient SLM operation and stable SLM development.
膜液浸出导致的支撑液体膜(SLMs)降解一直是其从废物流中进行资源回收的障碍。我们提出了一种新方法,利用四电极模式电化学阻抗光谱(EIS)对 SLM 降解进行实时、无损监测,提供 SLM 结构变化的详细分析。我们首先通过 EIS 发现 SLM 可被描述为电阻器和电容器组成的电路。然后,通过 EIS 发现,由于 SLM 的厚度和面积减小的速度不同,SLM 退化经历了四个不同的阶段。为了证明基于 EIS 诊断的有效性,我们制备了用于选择性提取中链脂肪酸 (MCFA) 的 SLM,并通过 EIS 确定了其完整、部分和完全降解的状态。与短链脂肪酸相比,完整的 SLM 对 MCFA 具有较高的选择性(50 ∼ 50)。在部分降解的 SLM 中,选择性降至 ∼22,而在完全降解的 SLM 中,选择性低于 1,这表明降解程度与分离性能之间存在明显的联系。我们的四电极模式 EIS 方法有望成为高效 SLM 运行和稳定 SLM 开发的关键工具。
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引用次数: 0
Facile and controlled dual-step modification with enhanced anti-fouling performance in polyvinylidene fluoride membranes 简便、可控的双步改性,增强聚偏氟乙烯膜的防污性能
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-21 DOI: 10.1016/j.memsci.2024.123358
Mingfu Gao , Yang Liu , Hai Huang , Sanchuan Yu , Doufeng Wu , Congjie Gao
Water scarcity and pollution pose significant challenges, necessitating advancements in water treatment technologies. Among various solutions, ultrafiltration membranes, especially those crafted from polyvinylidene fluoride (PVDF), are favored for their mechanical robustness and chemical stability. However, their practical application is often limited by severe membrane fouling due to the inherent hydrophobicity of PVDF. This project introduces a straightforward, controlled method to enhance the anti-fouling properties of PVDF membranes, utilizing a blend of cellulose acetate (CA). The process involves a two-step modification of hydrolysis followed by quaternization, effectively increasing hydroxyl group presence and facilitating subsequent chemical reactions. The optimized membranes achieve a dynamic water contact angle of 0° within 30 s and maintain an electroneutral surface at pH 7.1. With a mean pore size reduction from 28.6 nm to 23.9 nm and an impressive drop in the irreversible fouling ratio from 36.9 % to 0.3 %, these modifications markedly improve the anti-fouling performance. This research demonstrates significant potential for enhancing the functionality of PVDF ultrafiltration membranes through post-fabrication modifications, offering significant benefits for water treatment applications.
水资源匮乏和污染带来了巨大挑战,因此有必要改进水处理技术。在各种解决方案中,超滤膜,尤其是由聚偏二氟乙烯(PVDF)制成的超滤膜,因其机械坚固性和化学稳定性而备受青睐。然而,由于聚偏二氟乙烯固有的疏水性,其实际应用往往受到严重的膜堵塞限制。本项目介绍了一种直接、可控的方法,利用醋酸纤维素(CA)混合物增强 PVDF 膜的防污性能。该工艺包括水解和季铵化两步改性,可有效增加羟基的存在并促进后续化学反应。优化后的膜可在 30 秒内达到 0° 的动态水接触角,并在 pH 值为 7.1 时保持电中性表面。平均孔径从 28.6 nm 减小到 23.9 nm,不可逆污垢率从 36.9 % 显著下降到 0.3 %,这些改性显著提高了防污性能。这项研究证明了通过制造后改性来增强 PVDF 超滤膜功能的巨大潜力,可为水处理应用带来显著效益。
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引用次数: 0
Micropollutant removal via nanofiltration: The effect of salt concentration — Theory and experimental validation 通过纳滤去除微污染物:盐浓度的影响--理论与实验验证
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-21 DOI: 10.1016/j.memsci.2024.123347
S. Castaño Osorio , I.I. Ryzhkov , E. Spruijt , A. van der Wal , P.M. Biesheuvel , J.E. Dykstra
Nanofiltration guarantees high water recovery and low energy consumption in removing micropollutants (MPs). In this study, we derive a concise model to describe MP removal with nanofiltration membranes. We compare the results from the model with experimental data for the removal of 7 MPs with 5 salt concentrations using the NF270 membrane. Our findings indicate that the model accurately describes MP transport through nanofiltration membranes. Furthermore, we evaluate the effect of salt concentration on MP rejection. The results show that salt concentration impacts MP rejection differently based on MP charge and size. Increasing salt concentration decreases the rejection of counter-charged MPs that are small and increases the rejection of counter-charged MP that are large.
纳滤膜在去除微污染物(MPs)时可保证高水回收率和低能耗。在本研究中,我们推导出一个简明模型来描述纳滤膜去除 MP 的情况。我们将模型结果与使用 NF270 膜去除 7 种 MPs 和 5 种盐浓度的实验数据进行了比较。我们的研究结果表明,该模型准确地描述了 MP 通过纳滤膜的传输。此外,我们还评估了盐浓度对 MP 排斥的影响。结果表明,根据 MP 电荷和大小的不同,盐浓度对 MP 阻隔的影响也不同。增加盐浓度会降低对反电荷小的 MP 的排斥,增加对反电荷大的 MP 的排斥。
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引用次数: 0
Open and FAIR data for nanofiltration in organic media: A unified approach 有机介质纳滤的开放和 FAIR 数据:统一方法
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-21 DOI: 10.1016/j.memsci.2024.123356
Simon Van Buggenhout , Gergo Ignacz , Scout Caspers , Robin Dhondt , Marie Lenaerts , Nathalie Lenaerts , Sareh Rezaei Hosseinabadi , Ines Nulens , Guy Koeckelberghs , Yi Ren , Ryan P. Lively , Murielle Rabiller-Baudry , Ki Min Lim , Nazlee Ghazali , Joaquin Coronas , Milan Abel , Matthias Wessling , Mirko Skiborowski , Adam Oxley , Seok Ju Han , Rhea Verbeke
Organic solvent nanofiltration (OSN), also called solvent-resistant nanofiltration (SRNF), has emerged as a promising technology for the removal of impurities, recovery of solutes, and the regeneration of solvents in various industries, such as the pharmaceutical and the (petro)chemical industries. Despite the widespread use of OSN/SRNF, the presence of scattered, non-standardized data, and the absence of openly accessible data pose critical challenges to the development of new membrane materials and processes, their comparison to the state-of-the-art materials, and their fundamental understanding. To overcome these hurdles, data from peer-reviewed research articles and commercial datasheets were curated via a standardized procedure to obtain an extensive dataset on the membrane materials, synthesis parameters, operational conditions, physicochemical properties, and performance of OSN/SRNF membranes. Thanks to a truly impressive joint effort of the OSN/SRNF community, the dataset contains, as per April 2024, 5006 unique membrane filtrations from 294 publications for 42 solvents under several process parameters. This findable, accessible, interoperable, reproducible, and open (FAIR/O) dataset is available on both the OSN Database and the newly inaugurated Open Membrane Database for SRNF (OMD4SRNF). These databases provide multiple visualization and data exploration tools. Here, the standardized procedure applied to curate the data and the functionality of the databases are outlined, as well as the online user interface to deposit new data by external users on the OMD4SRNF. This community-led project has been supported by all the co-authors of this work. Most importantly, they additionally agreed to systematically deposit their future peer-reviewed data on OSN/SRNF into the databases. We thereby pave the road for FAIR/O data in the field of OSN/SRNF to increase transparency, enable more accurate data analysis, and foster collaboration and innovation.
有机溶剂纳滤(OSN),又称耐溶剂纳滤(SRNF),已成为制药和(石油)化学工业等各种工业中去除杂质、回收溶质和溶剂再生的一项很有前途的技术。尽管 OSN/SRNF 的使用非常广泛,但由于数据分散、非标准化,以及缺乏可公开获取的数据,对开发新的膜材料和工艺、将其与最先进的材料进行比较以及对其进行基本了解构成了严峻的挑战。为了克服这些障碍,我们通过标准化程序对同行评审的研究文章和商业数据表中的数据进行了整理,从而获得了关于膜材料、合成参数、操作条件、物理化学特性和 OSN/SRNF 膜性能的大量数据集。在 OSN/SRNF 社区的共同努力下,截至 2024 年 4 月,该数据集包含了来自 294 份出版物的 5006 个独特的膜过滤数据,涉及 42 种溶剂和多个工艺参数。这个可查找、可访问、可互操作、可重现和开放(FAIR/O)的数据集可在 OSN 数据库和新启用的 SRNF 开放式膜数据库(OMD4SRNF)中找到。这些数据库提供多种可视化和数据探索工具。在此,我们将简要介绍整理数据的标准化程序和数据库的功能,以及外部用户在 OMD4SRNF 上存放新数据的在线用户界面。这个由社区主导的项目得到了这项工作所有共同作者的支持。最重要的是,他们还同意今后将其在 OSN/SRNF 上经过同行评审的数据系统地存入数据库。因此,我们为 OSN/SRNF 领域的 FAIR/O 数据铺平了道路,以提高透明度,实现更准确的数据分析,促进合作与创新。
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引用次数: 0
Optimized ceramic membrane-based method for efficient and acid-free rice protein preparation from alkaline extracts 基于陶瓷膜的高效无酸制备碱性提取物中大米蛋白质的优化方法
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-21 DOI: 10.1016/j.memsci.2024.123355
Yulong Xie , Maosong Wang , Xianfu Chen , Wei Ke , Kaiyun Fu , Minghui Qiu , Tao Wang , Yiqun Fan
Rice protein, stands out as a high-quality plant-based protein, suitable for dietary supplementation and food processing. Traditional methods, involving alkaline extraction and acid precipitation, are challenged by the extensive use of chemicals and the difficulty in desalination. This study proposed a novel separation method that utilizes ceramic membranes for direct alkali filtration, eliminating the formation of salts by acid neutralization. The membrane pore size and the operating parameters such as transmembrane pressure, cross-flow velocity, and pH were optimized to enable a high flux (>80 L m−2·h−1) and favorable protein rejection (>95 %) while permitting the removal of excess alkali. Additionally, the effects of non-protein substances, e.g., starch, present in the alkaline extract on the separation performance were explored. Subsequently, an optimized strategy for starch removal was proposed, involving the concentration of the alkali extract using an ultrafiltration membrane, followed by enzymatic hydrolysis of starch and diafiltration to eliminate the residuals of starch hydrolysates and alkali. Under stabilization of protein particles by carboxymethyl cellulose, rice protein with a uniform particle size of 25 nm and a purity of over 80 % was produced. The direct removal of alkali from alkali extracts of rice by ceramic membranes presents a promising strategy for producing rice protein with high purity and reduced aggregation degree, enabling better functionalities such as solubility than the conventional alkali-extraction and acid-precipitation method.
大米蛋白质是一种优质的植物性蛋白质,适用于膳食补充和食品加工。传统的方法包括碱提取和酸沉淀,但由于大量使用化学品和脱盐困难而面临挑战。本研究提出了一种新型分离方法,利用陶瓷膜直接进行碱过滤,消除了酸中和形成的盐分。通过优化膜孔径和操作参数,如跨膜压力、横流速度和 pH 值,实现了高通量(80 L m-2-h-1)和良好的蛋白质去除率(95%),同时允许去除过量的碱。此外,还探讨了碱性提取物中的非蛋白质物质(如淀粉)对分离性能的影响。随后,提出了去除淀粉的优化策略,包括使用超滤膜浓缩碱提取物,然后对淀粉进行酶水解和重过滤,以去除残留的淀粉水解物和碱。在羧甲基纤维素稳定蛋白质颗粒的情况下,生产出粒度均匀的 25 纳米大米蛋白质,纯度超过 80%。与传统的碱提取和酸沉淀法相比,用陶瓷膜直接去除大米碱提取物中的碱,是生产高纯度和低聚集度大米蛋白质的一种有前途的策略,能使蛋白质具有更好的功能,如溶解性。
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引用次数: 0
Mechanism underlying anion-sieving in poly(ionic liquid)-based membrane: Effective acid recovery from engineering waste 聚(离子液体)膜中的阴离子筛分机理:从工程废料中有效回收酸
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-21 DOI: 10.1016/j.memsci.2024.123349
Nagaraj S. Naik , Usha Nellur , K.K. Nagaraja , Mahesh Padaki
Anion exchange membranes (AEMs) are promising for recovering acid from different engineering effluent due to their lower energy consumption, positive environmental impact, and potential for providing clean water resources. Utilizing the diffusion dialysis (DD) process, AEMs effectively retain metal ions while selectively allowing fast proton permeation. Achieving high hydrophilicity, proton conductivity, and ion exchange capacity through exact control of polymeric structure and chemical composition is crucial for enhancing the efficiency of the acid recovery process. This study presents the findings on the impact of novel Poly(ionic liquid) on cellulose acetate-based AEMs for acid recovery through DD application. In this study, interconnected nanochannel AEMs with high acid permeability are engineered using a straightforward blending technique. Poly(3-butyl-1-vinylimidazolium bromide-co-methyl methacrylate-co-styrene) (poly([BVIM]-[Br]–co–MMA-co-Styrene, PIL) is blended with cellulose acetate to achieve ionic crosslinking, resulting in a mechanically stable membrane. The dosage of PIL within the membrane matrix plays a vital role in determining the prepared membranes' physicochemical properties and ion exchange capabilities, which exhibit excellent thermal stability. Remarkably, the optimal AEM (7.5 % PILM) exhibits a high acid dialysis coefficient (UH+) of 1.05 m/h and a separation factor (S) of 802, outperforming previously reported state-of-the-art AEMs and commercial membranes. These findings indicate that the prepared AEMs are highly effective for acid recovery through DD. Notably, our work stands out by introducing new AEMs with superior acid dialysis performance and selectivity.
阴离子交换膜(AEM)能耗较低、对环境有积极影响,而且具有提供清洁水资源的潜力,因此有望从不同的工程废水中回收酸。利用扩散透析(DD)工艺,阴离子交换膜可有效截留金属离子,同时选择性地允许质子快速渗透。通过精确控制聚合物结构和化学成分来实现高亲水性、质子传导性和离子交换能力,对于提高酸回收工艺的效率至关重要。本研究介绍了新型聚(离子液体)对醋酸纤维素基 AEMs 通过 DD 应用进行酸回收的影响。在这项研究中,采用一种简单的混合技术,设计出了具有高酸渗透性的互连纳米通道 AEM。聚(3-丁基-1-乙烯基溴化咪唑-甲基丙烯酸甲酯-苯乙烯)(Poly([BVIM]-[Br]-co-MMA-co-Styrene, PIL)与醋酸纤维素混合,实现离子交联,从而形成机械稳定的膜。膜基质中 PIL 的用量在决定制备的膜的理化性质和离子交换能力方面起着至关重要的作用,这种膜具有出色的热稳定性。值得注意的是,最佳 AEM(7.5% PILM)的酸透析系数(UH+)高达 1.05 m/h,分离因子(S)达 802,优于之前报道的最先进的 AEM 和商用膜。这些研究结果表明,所制备的 AEM 在通过 DD 进行酸回收方面非常有效。值得注意的是,我们的工作通过引入具有卓越酸透析性能和选择性的新型 AEM 而脱颖而出。
{"title":"Mechanism underlying anion-sieving in poly(ionic liquid)-based membrane: Effective acid recovery from engineering waste","authors":"Nagaraj S. Naik ,&nbsp;Usha Nellur ,&nbsp;K.K. Nagaraja ,&nbsp;Mahesh Padaki","doi":"10.1016/j.memsci.2024.123349","DOIUrl":"10.1016/j.memsci.2024.123349","url":null,"abstract":"<div><div>Anion exchange membranes (AEMs) are promising for recovering acid from different engineering effluent due to their lower energy consumption, positive environmental impact, and potential for providing clean water resources. Utilizing the diffusion dialysis (DD) process, AEMs effectively retain metal ions while selectively allowing fast proton permeation. Achieving high hydrophilicity, proton conductivity, and ion exchange capacity through exact control of polymeric structure and chemical composition is crucial for enhancing the efficiency of the acid recovery process. This study presents the findings on the impact of novel Poly(ionic liquid) on cellulose acetate-based AEMs for acid recovery through DD application. In this study, interconnected nanochannel AEMs with high acid permeability are engineered using a straightforward blending technique. Poly(3-butyl-1-vinylimidazolium bromide-co-methyl methacrylate-co-styrene) (poly([BVIM]-[Br]–co–MMA-co-Styrene, PIL) is blended with cellulose acetate to achieve ionic crosslinking, resulting in a mechanically stable membrane. The dosage of PIL within the membrane matrix plays a vital role in determining the prepared membranes' physicochemical properties and ion exchange capabilities, which exhibit excellent thermal stability. Remarkably, the optimal AEM (7.5 % PILM) exhibits a high acid dialysis coefficient (U<sub>H</sub><sup>+</sup>) of 1.05 m/h and a separation factor (S) of 802, outperforming previously reported state-of-the-art AEMs and commercial membranes. These findings indicate that the prepared AEMs are highly effective for acid recovery through DD. Notably, our work stands out by introducing new AEMs with superior acid dialysis performance and selectivity.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"713 ","pages":"Article 123349"},"PeriodicalIF":8.4,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142315953","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
High-performance carbon molecular sieve membrane derived from PEK-N polymer for CO2 separation 用于二氧化碳分离的 PEK-N 聚合物衍生高性能碳分子筛膜
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-20 DOI: 10.1016/j.memsci.2024.123337
Li Yin , Shuai Wang , Tao Shen , Fangyuan Gai , Zhixuan Ma , Gengbo Liu , Jing Li , Hao Wang
Carbon molecular sieve (CMS) membranes demonstrate promising economic and environmental advantages in gas separation applications. In this work, we synthesized a novel polymer precursor of PEK-N and utilized it to fabricate a series of PEK-N derived CMS membranes. With varying carbonization temperature and time, the pore structures and gas separation performance were finely tuned. The gas separation properties of membranes with different carbonization temperature were comprehensively evaluated. In particular, by carbonizing the sample at 650 °C for 1 h, PEK-N derived CMS membranes (CMS-650-1) achieved the highest CO2 permeability around 2176 Barrer, and selectivities of 48.2 for CO2/N2 and 57.8 for CO2/CH4 in their gas mixtures. Our study suggests that the use of rationally designed polymers has the potential to bring about high gas separation performance for polymer-derived carbon molecular sieve membranes.
碳分子筛(CMS)膜在气体分离应用中展现出了良好的经济和环境优势。在这项工作中,我们合成了 PEK-N 的新型聚合物前体,并利用它制造了一系列 PEK-N 衍生的 CMS 膜。随着碳化温度和时间的变化,孔隙结构和气体分离性能得到了微调。对不同碳化温度下膜的气体分离性能进行了全面评估。其中,通过在 650 °C 下碳化样品 1 小时,PEK-N 衍生的 CMS 膜(CMS-650-1)获得了最高的二氧化碳渗透率,约为 2176 巴雷尔,其气体混合物中 CO2/N2 和 CO2/CH4 的选择性分别为 48.2 和 57.8。我们的研究表明,使用合理设计的聚合物有可能为聚合物衍生碳分子筛膜带来较高的气体分离性能。
{"title":"High-performance carbon molecular sieve membrane derived from PEK-N polymer for CO2 separation","authors":"Li Yin ,&nbsp;Shuai Wang ,&nbsp;Tao Shen ,&nbsp;Fangyuan Gai ,&nbsp;Zhixuan Ma ,&nbsp;Gengbo Liu ,&nbsp;Jing Li ,&nbsp;Hao Wang","doi":"10.1016/j.memsci.2024.123337","DOIUrl":"10.1016/j.memsci.2024.123337","url":null,"abstract":"<div><div>Carbon molecular sieve (CMS) membranes demonstrate promising economic and environmental advantages in gas separation applications. In this work, we synthesized a novel polymer precursor of PEK-N and utilized it to fabricate a series of PEK-N derived CMS membranes. With varying carbonization temperature and time, the pore structures and gas separation performance were finely tuned. The gas separation properties of membranes with different carbonization temperature were comprehensively evaluated. In particular, by carbonizing the sample at 650 °C for 1 h, PEK-N derived CMS membranes (CMS-650-1) achieved the highest CO<sub>2</sub> permeability around 2176 Barrer, and selectivities of 48.2 for CO<sub>2</sub>/N<sub>2</sub> and 57.8 for CO<sub>2</sub>/CH<sub>4</sub> in their gas mixtures. Our study suggests that the use of rationally designed polymers has the potential to bring about high gas separation performance for polymer-derived carbon molecular sieve membranes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"713 ","pages":"Article 123337"},"PeriodicalIF":8.4,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142316008","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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