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Reversible MOF-Based mixed matrix membranes for SO2/N2 separation: A photo-responsive approach 用于分离 SO2/N2 的可逆 MOF 基混合基质膜:光响应方法
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-18 DOI: 10.1016/j.memsci.2024.123431
Qingping Xin , Jiakang Dong , Wei Shao , Xiaoli Ding , Ningning Gao , Lei Zhang , Huimin Jin , Hao Chen , Yuzhong Zhang
Fuel consumption for industrial development, SO2 gas emissions are increasing year by year and have become a focal point of air pollution. Membrane separation method photo-responsive materials and MOFs have attracted more and more attention in a variety of fields. This is because the membrane separation method uses less energy and is an uncomplicated process; MOFs have superior gas adsorption capabilities; and the photo-responsive materials are controllable. In this study, mixed matrix membranes are prepared using Uio-66-NH2 and photo-responsive materials CE-Azo-Uio-66 as fillers and Pebax as base membranes. By improving the dissolution-diffusion mechanism for SO2 gas molecules, SO2/N2 gas separation is accomplished. More channels for the mass transport of SO2 gas through the membrane can be created by MOFs increased porosity and larger specific surface area. Secondly, the SO2 adsorption and dissolution-diffusion mechanism of the mixed matrix membrane are strengthened by the grafted SO2 affinity groups on the MOF. Moreover, Pebax/CE-Azo-Uio-66 membranes is not only significantly more permeation selective than Pebax/Uio-66-NH2 membranes, but also shows photo-responsive characteristic. The SO2 permeability and selectivity of Pebax/CE-Azo-Uio-66 mixed matrix membranes at CE-Azo-Uio-66 content of 20 % are increased by 191 % and 179 %, respectively, compared to pure Pebax membranes. It is also found that the SO2 permeability and SO2/N2 selectivity of the membranes show regularly reversible changes at the UV–Vis photoconversion conditions of Pebax/CE-Azo-Uio-66-20 % membranes, indicating the photo-responsive characteristics of mixed matrix membranes that include Azo groups. The SO2 permeability of the Pebax/CE-Azo-Uio-66 membrane is increased by 1300 Barrer and the SO2/N2 selectivity is increased by 350 when the light source is changed from UV to Vis light, achieving a controlled separation of SO2/N2. Besides, the addition of MOF particles significantly enhances the mechanical properties and stability of the membrane.
工业发展消耗燃料,二氧化硫气体排放量逐年增加,已成为大气污染的焦点。膜分离法中的光响应材料和 MOFs 在各个领域受到越来越多的关注。这是因为膜分离法耗能少、工艺简单;MOFs 具有优异的气体吸附能力;光响应材料具有可控性。本研究以 Uio-66-NH2 和光响应材料 CE-Azo-Uio-66 为填料,以 Pebax 为基膜,制备了混合基膜。通过改善 SO2 气体分子的溶解-扩散机制,实现了 SO2/N2 气体分离。通过增加 MOF 的孔隙率和比表面积,可为 SO2 气体通过膜的质量传输创造更多的通道。其次,MOF 上接枝的 SO2 亲和基团加强了混合基质膜的 SO2 吸附和溶解扩散机制。此外,与 Pebax/Uio-66-NH2 膜相比,Pebax/CE-Azo-Uio-66 膜不仅具有更高的渗透选择性,而且还具有光响应特性。与纯 Pebax 膜相比,当 CE-Azo-Uio-66 的含量为 20% 时,Pebax/CE-Azo-Uio-66 混合基质膜的二氧化硫渗透性和选择性分别提高了 191% 和 179%。研究还发现,在 Pebax/CE-Azo-Uio-66-20 % 膜的紫外可见光光电转换条件下,膜的 SO2 渗透性和 SO2/N2 选择性呈现出有规律的可逆变化,这表明含有偶氮基团的混合基质膜具有光响应特性。当光源从紫外光转变为可见光时,Pebax/CE-偶氮-Uio-66 膜的二氧化硫渗透率提高了 1300 巴,二氧化硫/氮选择性提高了 350,实现了二氧化硫/氮的可控分离。此外,MOF 颗粒的加入还显著提高了膜的机械性能和稳定性。
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引用次数: 0
Impact of filtration at elevated temperature and solvent pre-treatment on crosslinked polyvinylidene difluoride and polyimide solvent-resistant nanofiltration membranes 高温过滤和溶剂预处理对交联聚偏二氟乙烯和聚酰亚胺耐溶剂纳滤膜的影响
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-18 DOI: 10.1016/j.memsci.2024.123409
Sareh Rezaei Hosseinabadi , Sutapa Roy Swarna , Laurens A.J. Rutgeerts , Jianjun Huang , Ivo F.J. Vankelecom
The high temperature filtration performance of crosslinked polyvinylidene difluoride (XL-PVDF) and polyimide (XL-PI) membranes in solvent-resistant nanofiltration (SRNF) applications was studied. The membranes were tested in four industry-relevant, apolar solvents (toluene, xylene, chloroform, and n-butyl acetate) over a temperature range from 25 °C to 80 °C. The temperature effect on membrane performance was evaluated using a polar probe molecule (5,10,15,20-tetrakis(3,5-di-tert-butyl phenyl)porphyrin (TBPP), 1064 Da), showing that permeance increased with rising temperature due to the anticipating reduced solvent viscosity and enhanced flexibility of the membrane polymer chains. This effect varied clearly between the two polymer systems. After the high-temperature filtration, room-temperature (RT) filtrations demonstrated stable retention in xylene, BuOAc, and toluene, but a decrease in chloroform The membranes exhibited excellent long-term stability, retaining their quasi-intact filtration performance over a full week of operation. To investigate the impact of a pre-filtration solvent treatment, Sudan black (SB)/chloroform filtrations were done before and after exposure to toluene, xylene, BuOAc, and chloroform. Quite surprisingly, such solvent treatment resulted in a polymer-specific impact: an increased permeation for XL-PVDF and a decreased permeation for XL-PI. Retentions were constant for XL-PVDF but slightly increased for XL-PI. Overall, both membrane types showed excellent thermal and solvent stability, but the impact was very different.
研究了交联聚偏二氟乙烯(XL-PVDF)和聚酰亚胺(XL-PI)膜在耐溶剂纳滤(SRNF)应用中的高温过滤性能。在 25 °C 至 80 °C 的温度范围内,在四种与工业相关的极性溶剂(甲苯、二甲苯、氯仿和乙酸正丁酯)中对膜进行了测试。使用极性探针分子(5,10,15,20-四(3,5-二叔丁基苯基)卟啉(TBPP,1064 Da))评估了温度对膜性能的影响,结果表明,随着温度的升高,渗透率会增加,这是由于溶剂粘度会降低,膜聚合物链的柔韧性会增强。这种效应在两种聚合物体系之间存在明显差异。高温过滤后,室温(RT)过滤显示在二甲苯、BuOAc 和甲苯中的保留率稳定,但在氯仿中的保留率下降。为了研究过滤前溶剂处理的影响,在接触甲苯、二甲苯、BuOAc 和氯仿前后进行了苏丹黑 (SB) / 氯仿过滤。令人惊讶的是,这种溶剂处理会对聚合物产生特定的影响:XL-PVDF 的渗透率增加,而 XL-PI 的渗透率降低。XL-PVDF 的保留率保持不变,但 XL-PI 的保留率略有增加。总的来说,这两种膜都表现出卓越的热稳定性和溶剂稳定性,但影响却大不相同。
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引用次数: 0
Highly efficient separation of Li+/Mg2+ via nanofiltration membranes with conductive substrates under an electric field 在电场下通过带有导电基底的纳滤膜高效分离 Li+/Mg2+
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-17 DOI: 10.1016/j.memsci.2024.123413
Junjie Lv , Yuwei Wang , Boyang Hui , Yanhong Ji , Hong Wang , Mohammad Younas , Benqiao He
Electro-nanofiltration (ENF) achieved efficient separation of Li⁺/Mg2⁺. The conductivity of an NF membrane had a notable impact on the ENF process. In this work, an NF membrane was prepared by interface polymerization on a conductive polyether sulfone (PES)/MXene@CNT membrane, which was used in an ENF process to enable the highly efficient and precise separation of Li⁺/Mg2⁺. It was found that the PES/MXene@CNT membranes had fairly good electrical conductivity (>0.5 S/m) and hydrophilicity after the addition of MXene and CNT into PES membranes. The ENF membrane with a conductive substrate exhibited extremely excellent Li⁺/Mg2⁺ separation performance even at a low voltage. It was because the conductive substrate of the NF membrane could be directly considered as a cathode to enhance electric field strength and current density during ENF process, which was more suitable for surface charge reconstruction and Li+ transport. When the voltage was 2.5 V, Mg2+ was nearly completely rejected; while Li+ rejection was up to −100.6 %. The Li⁺/Mg2⁺ separation factor (SLi,Mg) was as high as 1164.6, which was far higher than that (SLi,Mg = 25.7) based on the common NFmembrane with a non-conductive support membrane at 2.5 V. The ENF showed a stable separation performance at 2.5 V. The results suggested that the NF membrane a with conductive substrate possessed obvious advantages in the preparation and performance of ENF membrane compared with the NF membranes with non-conductive substrates. This work offered a viable way for the efficient separation of Li+/Mg2+ and possessed tremendous potential in extracting high-purity Li+ salts from salt lakes.
电纳滤(ENF)实现了锂⁺/Mg2⁺的高效分离。纳滤膜的导电性对 ENF 过程有显著影响。本研究通过界面聚合法制备了导电聚醚砜(PES)/MXene@CNT膜,并将其用于ENF工艺中,实现了锂⁺/Mg2⁺的高效、精确分离。研究发现,在 PES 膜中添加 MXene 和 CNT 后,PES/MXene@CNT 膜具有相当好的导电性(>0.5 S/m)和亲水性。即使在低电压下,带有导电基底的 ENF 膜也能表现出极其出色的 Li⁺/Mg2⁺ 分离性能。这是因为在ENF过程中,NF膜的导电基底可直接被视为阴极,从而增强电场强度和电流密度,更适合表面电荷重构和Li+传输。当电压为 2.5 V 时,Mg2+ 几乎被完全排斥;而 Li+ 的排斥率高达 -100.6%。在 2.5 V 电压下,Li⁺/Mg2⁺ 分离因子(SLi,Mg)高达 1164.6,远高于采用非导电支撑膜的普通 NF 膜(SLi,Mg = 25.7)。ENF 在 2.5 V 下显示出稳定的分离性能。结果表明,与非导电基底的 NF 膜相比,导电基底的 NF 膜在 ENF 膜的制备和性能方面具有明显优势。这项工作为高效分离 Li+/Mg2+ 提供了一条可行的途径,在从盐湖中提取高纯度 Li+ 盐方面具有巨大的潜力。
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引用次数: 0
Poly-(aminoethyl piperazine) membranes with ultra-thin selective layers prepared via a rate-retarded interfacial polymerization method 通过缓速界面聚合法制备具有超薄选择层的聚(氨基乙基哌嗪)膜
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-17 DOI: 10.1016/j.memsci.2024.123415
PanPan Su , Man Xu , Cunwen Wang , Yanbo Li
New monomers have been exploring to fabricate interfacial polymerized thin film composite membranes for decades. N-aminoethyl piperazine (AEP), an aliphatic amine with a heterocyclic structure, was used in this work as an amine monomer to synthesize nanofiltration membranes. Due to the high reactivity nature of AEP, a rate-retarded interfacial polymerization method was applied, which was realized by applying ultra-low AEP concentration (0.07 wt%), low reaction temperature (4 °C monomer solutions), and ice-water quench. The resulting AEP membrane had much better performance (3–4 times permeance and closed rejections) compared with the membranes prepared by the hot water post-treatment and the oven heat treatment. At lower monomer concentrations, an NF membrane with a selective layer thickness of only around 20 nm was prepared by the rate-retarded interfacial polymerization method. The membranes had a negatively charged surface with "willow leaf" like morphology. The MWCO was around 200 g mol−1, and the water permeance was up to 22.8 L m−2 h−1 bar−1, which is comparable with the commercial polyamide membrane NF270. Therefore, AEP is a very competitive alternative monomer for NF membrane synthesis.
几十年来,人们一直在探索制造界面聚合薄膜复合膜的新单体。N-aminoethyl piperazine (AEP)是一种具有杂环结构的脂肪族胺,本研究采用它作为胺单体来合成纳滤膜。由于 AEP 具有高反应活性,因此采用了一种速率延缓的界面聚合方法,通过超低的 AEP 浓度(0.07 wt%)、低反应温度(4 °C单体溶液)和冰水淬火来实现。与通过热水后处理和烘箱热处理制备的膜相比,所制备的 AEP 膜性能要好得多(渗透率是其 3-4 倍,并具有封闭的排斥功能)。在单体浓度较低的情况下,通过速率滞后界面聚合法制备出了选择性层厚度仅为 20 纳米左右的 NF 膜。膜表面带负电荷,形态类似 "柳叶"。其截留分子量约为 200 g mol-1,透水率高达 22.8 L m-2 h-1 bar-1,与商用聚酰胺膜 NF270 不相上下。因此,AEP 是一种极具竞争力的 NF 膜合成替代单体。
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引用次数: 0
Biochar-driven fouling mitigation in sustainable microalgal-bacterial membrane bioreactors 生物炭驱动的可持续微藻-细菌膜生物反应器污垢缓解技术
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-16 DOI: 10.1016/j.memsci.2024.123427
Fei Huang , Jiaheng Teng , Yu Zhao , Shangfei Li , Hongjun Lin , Xiang Cai , Meijia Zhang
Microalgal-bacterial membrane bioreactor (MB-MBR) have emerged as a crucial technology for sustainable wastewater treatment. However, membrane fouling caused by free microalgae remains a major obstacle to their cost-effective operation. This study investigated the impact of biochar addition on membrane fouling in MB-MBR. The findings indicated that biochar significantly reduced membrane fouling, primarily due to the enlargement of floc size and the reduction of soluble microbial products (SMP). Detailed analyses suggested that biochar's adsorptive properties and its effect on decreasing the abundance of algae and bacteria species, such as Proteobacteria and Leptolyngbya, which promote fouling, are key factors. This alteration enhanced specific amino acid metabolic pathways, thereby reducing SMP production and fouling potential. Consequently, adhesion interaction energy of the flocs and membrane fouling were both diminished. This study demonstrated that biochar addition is an effective strategy for mitigating membrane fouling in MB-MBR systems, providing a theoretical foundation for their stable and sustainable operation.
微藻-细菌膜生物反应器(MBR)已成为可持续废水处理的一项重要技术。然而,游离微藻造成的膜堵塞仍然是其经济高效运行的主要障碍。本研究调查了生物炭的添加对 MB-MBR 膜堵塞的影响。研究结果表明,生物炭能显著减少膜堵塞,这主要是由于絮凝物尺寸增大和可溶性微生物产物(SMP)减少。详细的分析表明,生物炭的吸附特性及其对减少藻类和细菌(如变形杆菌和鳞状杆菌)数量的影响是造成污垢的关键因素。这种改变增强了特定的氨基酸代谢途径,从而减少了 SMP 的产生,降低了产生污垢的可能性。因此,絮凝体的粘附相互作用能和膜污垢都减少了。这项研究表明,添加生物炭是减轻 MB-MBR 系统膜污垢的有效策略,为其稳定和可持续运行提供了理论基础。
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引用次数: 0
Synthesis of poly(terphenyl-co-dibenzo-18-crown-6 methylimidazole) copolymers for high-performance high temperature polymer electrolyte membrane fuel cells 用于高性能高温聚合物电解质膜燃料电池的聚(三联苯-共二苯并-18-冠-6 甲基咪唑)共聚物的合成
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-16 DOI: 10.1016/j.memsci.2024.123416
Lele Wang, Qian Wang, Peiru Lv, Zhen Peng, Jingshuai Yang
This study focuses on the development of high temperature polymer electrolyte membranes (HT-PEMs), which are essential components for HT-PEM fuel cells (HT-PEMFCs). While phosphoric acid (PA) doped polybenzimidazole (PBI) has been recognized as a successful HT-PEM, it faces several challenges, including the use of carcinogenic monomer, complex synthesis processes, and poor solubility in organic solvents. To produce more cost-effective, easily synthesized, and high-performance alternatives, this study utilizes a straightforward superacid-catalyzed Friedel-Crafts reaction to synthesize a series of poly(terphenyl-co-dibenzo-18-crown-6 methylimidazole) copolymers, referred to as Co-x%TP-y%CE-Im, using p-terphenyl, dibenzo-18-crown-6 and 1-methyl-1H-imidazole-2-formaldehyde as monomers. The copolymerized hydrophilic and bulky crown ether units introduce substantial free volume and multiple interaction sites with PA molecules, as indicated by theoretical calculations. Additionally, the formation of microphase separation structures, confirmed by atomic force microscope (AFM) and transmission electron microscope (TEM), contributes to the enhanced performance of these membranes. For instance, after immersion in 85 wt% and 75 wt% PA solutions, the Co-90%TP-10%CE membrane achieves PA doping contents of 200 % and 169 %, achieving high conductivities of 0.092 S cm−1 and 0.054 S cm−1 at 180 °C, while maintaining tensile strengths of 6.5 MPa and 7.5 MPa at room temperature. Without the need for humidification or backpressure, the peak power density of an H2-O2 cell equipped with Co-90%TP-10%CE/169%PA membrane with a thickness of 79 μm reaches an impressive 1018 mW cm−2 at 210 °C. These results demonstrate new materials and insights for the development of high-performance HT-PEMs.
本研究的重点是高温聚合物电解质膜(HT-PEM)的开发,它是高温聚合物电解质燃料电池(HT-PEMFC)的重要组成部分。虽然掺杂磷酸(PA)的聚苯并咪唑(PBI)已被公认为是一种成功的高温聚合物电解质膜,但它也面临着一些挑战,包括使用致癌单体、复杂的合成工艺以及在有机溶剂中溶解性差等。为了生产出更具成本效益、更易合成和更高性能的替代品,本研究利用简单的超酸催化 Friedel-Crafts 反应,以对三联苯、二苯并-18-冠醚-6 和 1-甲基-1H-咪唑-2-甲醛为单体,合成了一系列聚(三联苯-共二苯并-18-冠醚-6 甲基咪唑)共聚物,称为 Co-x%TP-y%CE-Im。理论计算表明,共聚的亲水性和大体积冠醚单元引入了大量的自由体积以及与 PA 分子的多个相互作用位点。此外,经原子力显微镜(AFM)和透射电子显微镜(TEM)证实,微相分离结构的形成也有助于提高这些膜的性能。例如,在 85 wt% 和 75 wt% PA 溶液中浸泡后,Co-90%TP-10%CE 膜的 PA 掺杂含量分别达到 200 % 和 169 %,在 180 °C 时分别达到 0.092 S cm-1 和 0.054 S cm-1 的高电导率,同时在室温下保持 6.5 MPa 和 7.5 MPa 的抗拉强度。无需加湿或背压,配备了厚度为 79 μm 的 Co-90%TP-10%CE/169%PA 膜的 H2-O2 电池在 210 °C 时的峰值功率密度达到了惊人的 1018 mW cm-2。这些结果展示了开发高性能 HT-PEM 的新材料和新见解。
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引用次数: 0
Direct-through channels of ZIF-8 composite membranes via in-situ PolyBMA sealing: Radical-induced phase transformation and dye removal efficiency 通过原位 PolyBMA 密封实现 ZIF-8 复合膜的直通通道:辐射诱导的相变和染料去除效率
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-16 DOI: 10.1016/j.memsci.2024.123412
Jiali Tang , Viatcheslav Freger , Lu Shao , Xuezhong He
Metal-organic frameworks (MOFs)-based hybrid composite membranes are promising candidates for achieving highly efficient water purification. In this study, a facile, novel pressure-induced filtration method involving in-situ polymerization of butyl methacrylate (BMA) was proposed for sealing ZIF-8 nanoparticles on top of polyethersulfone (PES) ultrafiltration membrane support. The developed (ZIF-8+polyBMA)/PES composite membranes with thin toplayers of <1 μm present attractive water permeance (up to 31 LMH/bar) and good rejection of Congo red (99.2 %) and Methylene blue (99.1 %). The ZIF-8 particles served as direct-through channels with superior separation performance due to their high porosity and tunable pore structure, while the interstices were successfully sealed with polyBMA by in-situ polymerization, as demonstrated by SEM and dye removal experiments. It was found that the morphology of ZIF-8 transformed from a rhombic dodecahedron to two-dimensional hexagonal nanosheets during the fabrication process. We hypothesize that this surprising phenomenon is caused by the reaction of the initiators (Na2S2O5 and K2S2O8) that generate the hydroxyl and sulfate radicals attacking and transforming the Zn-MIM bond network of ZIF-8. However, insights into the structural changes need to be further investigated to understand the mechanism involved.
基于金属有机框架(MOFs)的混合复合膜是实现高效水净化的理想候选材料。本研究提出了一种简便、新颖的压力诱导过滤方法,该方法涉及甲基丙烯酸丁酯(BMA)的原位聚合,用于将 ZIF-8 纳米颗粒密封在聚醚砜(PES)超滤膜支架之上。所开发的(ZIF-8+聚 BMA)/聚醚砜复合膜具有 1 μm 薄的表层,透水性极佳(高达 31 LMH/bar),对刚果红(99.2%)和亚甲蓝(99.1%)有良好的抑制作用。ZIF-8 颗粒具有高孔隙率和可调节的孔隙结构,因此可用作具有优异分离性能的直通通道,同时通过原位聚合,成功地用聚 BMA 封住了间隙,这一点已在扫描电镜和染料去除实验中得到证实。我们发现,在制造过程中,ZIF-8 的形态从菱形十二面体转变为二维六边形纳米片。我们推测这一令人惊讶的现象是由引发剂(Na2S2O5 和 K2S2O8)的反应引起的,引发剂产生的羟基和硫酸根自由基攻击并改变了 ZIF-8 的 Zn-MIM 键网络。不过,要深入了解结构变化的机理,还需要进一步研究。
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引用次数: 0
Conductivity-enhanced Poly(biphenyl piperidine) anion exchange membranes with organic tubes 带有机管的电导增强型聚(联苯哌啶)阴离子交换膜
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-16 DOI: 10.1016/j.memsci.2024.123414
Dingting Yang , Xiuyang Zou , Meisheng Li , Yan Zhang , Shouyong Zhou , Dawei Yang , Yijiang Zhao
Anion exchange membrane fuel cells (AEMFCs) present an economically efficient alternative to proton exchange membrane fuel cells because of the use of non-precious metals. The development of high-performance and durable AEMFCs necessitates the use of highly conductive and robust anion exchange membranes (AEMs). In this study, a novel organic-organic composite AEM was synthesized by preparing poly(arylene piperidinium) polymer through Friedel-Crafts acid condensation and incorporating one-dimensional organic tubes as reinforcing materials. The composite AEM exhibits high conductivity (235 mS cm−1 at 80 °C) due to the chain orientation within the organic tubes and the availability of abundant transport sites. Furthermore, in contrast to the incompatibility of inorganic materials with polymers, the flexible nature of organic tubes enhanced polymer entanglement, significantly boosting the mechanical strength (120 MPa) of the AEM. Crosslinking the polymer backbone with the organic tubes facilitated simultaneous swelling, effectively mitigating interfacial compatibility issues, result in high dimensional stability. The H2–O2 fuel cell employing the developed AEM demonstrated a peak power density of 1018 mW cm−2 at 80 °C. This study provides a comprehensive synthetic strategy for producing stable AEMs with high hydroxide ion conductivity and outstanding mechanical properties tailored for alkaline membrane fuel cell applications.
阴离子交换膜燃料电池(AEMFC)由于使用非贵金属,因此是质子交换膜燃料电池的一种经济高效的替代品。要开发高性能和耐用的 AEMFC,就必须使用高导电性和坚固耐用的阴离子交换膜(AEM)。本研究通过 Friedel-Crafts 酸缩合法制备了聚(芳基哌啶)聚合物,并加入一维有机管作为增强材料,从而合成了一种新型有机-有机复合 AEM。由于有机管内的链取向和丰富的传输位点,复合 AEM 表现出很高的电导率(80 °C 时为 235 mS cm-1)。此外,与无机材料与聚合物不相容相反,有机管的柔性增强了聚合物的缠结,从而显著提高了 AEM 的机械强度(120 兆帕)。聚合物骨架与有机管交联可促进同时溶胀,有效缓解界面兼容性问题,从而实现高尺寸稳定性。采用所开发的 AEM 的 H2-O2 燃料电池在 80 °C 时的峰值功率密度为 1018 mW cm-2。这项研究为生产稳定的 AEM 提供了全面的合成策略,AEM 具有高氢氧根离子电导率和出色的机械性能,适合碱性膜燃料电池应用。
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引用次数: 0
Ligand content and driving force effects on ion-ion permselectivity in ligand-functionalized membranes 配体含量和驱动力对配体功能化膜中离子-离子过选择性的影响
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-16 DOI: 10.1016/j.memsci.2024.123418
Kristen Abels , Amilton Barbosa Botelho Junior , Xi Chen , William A. Tarpeh
Ion-selective membranes could enable sustainable critical material separations processes because of their scalability, low energy consumption, and low chemical input. The effects of membrane water content and incorporation of ion-coordinating ligands have been studied via computation and experiment to develop structure-performance relationships. However, few studies systematically investigate the effects of membrane composition beyond monomer chemical identity or the balance of driving forces such as diffusion and electromigration. Here we synthesized a library of poly(ethylene glycol) acrylate membranes with varying percentages of ion-coordinating monomers (acrylic acid, 4-vinylpyridine) to investigate the influence of ligand content on cation permeabilities and permselectivities. Trends in membrane performance under electrodialysis and diffusion were compared to elucidate the relative effects of separation driving forces and to inform electrochemical operation. We observed order-of-magnitude permeability reductions with ligand content for ions capable of multidentate ligand complexation, especially for nickel in the pyridine-containing membranes. As a result, lithium/nickel permselectivity gradually increased by a factor of 1.65 × from 10 to 50 mol% pyridine membranes. We further demonstrated simultaneous improvements in lithium/nickel separation productivity (1.75 ×) and selectivity (2.99 ×) with increasing electric potential driving force. Ultimately, results from this study provide design insights for ligand-functionalized membranes in electrified ion-ion separations processes.
离子选择性膜因其可扩展性、低能耗和低化学投入,可实现可持续的关键材料分离过程。人们已经通过计算和实验研究了膜含水量和离子配位体结合的影响,以建立结构-性能关系。然而,除了单体化学特性或扩散和电迁移等驱动力的平衡之外,很少有研究系统地调查膜组成的影响。在这里,我们合成了一个具有不同比例离子配位单体(丙烯酸、4-乙烯基吡啶)的聚(乙二醇)丙烯酸酯膜库,以研究配体含量对阳离子渗透性和过选择性的影响。我们比较了电渗析和扩散条件下膜性能的变化趋势,以阐明分离驱动力的相对影响,并为电化学操作提供参考。我们观察到,对于能与多叉配体络合的离子,特别是含吡啶膜中的镍,随着配体含量的增加,渗透率会出现数量级的降低。因此,从 10 摩尔到 50 摩尔吡啶膜,锂/镍的过选择性逐渐增加了 1.65 倍。我们进一步证明,随着电势驱动力的增加,锂/镍分离的生产率(1.75 倍)和选择性(2.99 倍)也同时提高。最终,这项研究的结果为电化离子-离子分离过程中配体功能化膜的设计提供了启示。
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引用次数: 0
Ultrafast and energy-efficient flowthrough capture of antibiotics through a reusable MOF@wood membrane adsorbent 通过可重复使用的 MOF@wood 膜吸附剂超快、高效地捕获抗生素
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-16 DOI: 10.1016/j.memsci.2024.123411
Yaqin Zhu , Gaigai Duan , Weijie Wu , Yanbo Liu , Shiyi Zeng , Haoqi Yang , Xiaoshuai Han , Shuijian He , Chunmei Zhang , Jingquan Han , Shaohua Jiang
The accumulation of antibiotics in aquatic environments poses escalating risks to both ecosystems and human health. However, current water remediation strategies are hampered by numerous limitations, especially in operating costs and processing efficiency. Herein, the MIL-100(Fe)@wood membrane with high metal-organic frameworks (MOFs) loading is prepared by a simple flow-based fabrication technique. The presented integrated water purification system comprising membrane preparation, antibiotic removal and membrane regeneration allows for the sequential and continuous execution of the individual processes, thereby improving the sustainability, time efficiency and energy efficiency of the system. The highly efficient and flowthrough capturing membranes (MIL-100(Fe)@wood) are reported to remove numerous common antibiotics from water: tetracycline (TC), ciprofloxacin (CIP), amoxicillin (AMX), roxithromycin (RXM), and sulfamethazine (SMT). The stability and excellent long-term performance under different pH environmental conditions of MIL-100(Fe)@wood are demonstrated. Furthermore, the removal mechanisms of the multimolecular interactions occurring between antibiotic and MIL-100(Fe)@wood have also been explored. The unique advantage of MIL-100(Fe)@wood is employed in sustainable, cost-effective, and facile strategies for the removal of antibiotics.
抗生素在水生环境中的积累对生态系统和人类健康都构成了不断升级的风险。然而,目前的水处理策略受到诸多限制,尤其是在运营成本和处理效率方面。本文通过一种简单的流式制备技术,制备了具有高金属有机框架(MOFs)负载的 MIL-100(Fe)@wood 膜。所介绍的集成水纯化系统包括膜制备、抗生素去除和膜再生,可按顺序连续执行各个过程,从而提高系统的可持续性、时间效率和能源效率。据报道,这种高效的穿流捕捉膜(MIL-100(Fe)@wood)可以去除水中的多种常见抗生素:四环素(TC)、环丙沙星(CIP)、阿莫西林(AMX)、罗红霉素(RXM)和磺胺甲基嘧啶(SMT)。结果表明,MIL-100(Fe)@wood 在不同 pH 值的环境条件下具有稳定性和出色的长期性能。此外,还探讨了抗生素与 MIL-100(Fe)@wood 之间发生的多分子相互作用的去除机制。MIL-100(Fe)@wood的独特优势可用于可持续、经济高效、简便易行的抗生素去除策略。
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引用次数: 0
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Journal of Membrane Science
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