CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Yan-Mei Zhang,Li-Hao Xu,Xiao-Xue Hu,Bing-Hong Chen,Xin-Ru Chen,Qian-Qian Li,Heng Mao,Zhi-Ping Zhao
Metal-organic framework (MOF) membranes, by virtue of their high selectivity and low diffusion resistance, make a significant contribution to energy conservation and CO 2 emission reduction via separation technology. Despite possessing substantial potential for propelling the production of high-performance membranes, hurdles persist in the process of constructing MOF membranes that are both highly integrated and structurally sound on flexible polymer substrates. We propose a strategy for constructing highly stable cobalt zeolitic imidazolate framework (ZIF-67) composite membranes on seeded polyacrylonitrile (PAN) substrate. Through a timed-interrupted in-situ growth process, the amino-modified polycrystalline ZIF-67 as a CO 2 affinity layer is precisely and completely confined within the “top sites” and partial “face sites” of the vertical layered double hydroxide (LDH) precursor layer, creating a barrier-low passage for CO 2 as a fast diffusion layer. The substrate and the hybrid ZIF-67@LDH layer were robustly anchored together by the pre-embedded LDH seeds, thereby producing an appealing membrane-multilayer interlocked-support (MMIS) composite architecture. This fast diffusion-CO 2 affinity Pebax/ZIF-67@LDH/PAN membranes with MMIS architecture show average CO 2 permeability of 1487 Barrer and CO 2 /N 2 selectivity of above 55.1 after the surface repair coating of polyether-block-amide (Pebax), maintaining stable performance over 150 h, surpassing the Robeson upper bound. The Pebax/ZIF-67@LDH/PAN membranes also exhibit the durability and mechanical robustness, because of the highly inducible activity of LDH precursor layer serving as a linker between the membrane and substrate. These results promote the development of MOF-based membranes in practical separation applications.
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Hongxu Tao,Haiqian Lian,Jingxian Hua,Shengui Ju,Yichang Pan
The MOF membrane has shown great promise for the gases or organic solvent mixtures separation. However, the implementation of MOF membranes remains challenged by defect formation during membrane fabrication. Herein, we reveal that the activation solvent plays a critical role in governing the degree of defect and separation performance in secondary-growth-derived ZIF-8 membranes. The isopropanol activation process exerts excellent membrane structure protection through a synergistic dual mechanism to limit the generation of ZIF-8 membrane defects during drying: (a) The isopropanol inhibits the ZIF-8 seed layer recrystallization and maintains its porous architecture to mitigate interfacial stress during drying through its elastic deformation. (b) The low surface tension of isopropanol minimizes the capillary force during solvent removal to reduce the risk of structural damage. While methanol activation and n-propanol activation have no such structure control. The optimized isopropanol-activated membrane achieves a C 3 H 6 /C 3 H 8 selectivity of 141 to show a 4.8-fold and a 4.4-fold compared to n-propanol- and methanol-activated membranes at room temperature and 1 bar. This study highlights low-surface-tension as an effective strategy for defect suppression in MOF membranes, advancing their potential for industrial hydrocarbon separations.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
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IF 6.7
Chongchong Chen,Hexiang Gao,Hui Li,Mingchao Wang,Jie Zhang,Tengfei Li,Wenjia Wu,Zhirong Yang,Jingtao Wang
The poor water-stability and cross-layer proton transfer property pose a challenge to the lamellar metal–organic frameworks (MOFs) membrane when acting as a promising proton exchange membrane. Herein, we report an adipic acid-mediated strategy to improve the water-stability and the cross-layer proton conductivity of CuTCPP lamellar MOF membrane, which achieves a maximum power density and current density of 112.6 mW cm −2 and 424.4 mA cm −2 , respectively. Adipic acid with extra functional groups (–PO 3 H 2 , –COOH) stably bridges the adjacent crystal layers via the terminal carboxylic acid anchoring Cu sites. In particular, the extra functional groups introduced into the adipic acid regulate the allocation of hydrogen bonding networks in an umbrella-shape around adipic acid with copper-porphyrin structures as external margin, enriching the coherence of hydrogen bonding network on the proton transport path. Benefiting from the regular pore structure of MOF, the optimized hydrogen bonding networks in adjacent crystal layers construct a more abundant through-plane transfer pathway. The resultant through-plane proton conductivities of CuTCPP-PO 3 H 2 /–COOH membranes are up to 108/89 mS cm −1 at 80 °C and 100 % RH, which is ∼ 6-fold higher than that of the pristine CuTCPP membrane (13 mS cm −1 ), with a conductivity attenuation of < 5 % during a humidity cycling test for 12 times.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Qian Wang,Changchao Zhou,Li Shen,Eryue Song,Yu Yang,Haiqian Lian,Rujing Hou,Yichang Pan
The pervaporation (PV) technology is attractive for azeotrope component separation of the MeOH/MTBE mixture due to the reduced energy and cost relative to the traditional ternary distillation process. However, the membrane separation performance is largely affected by its microstructure including pore size and shape as well as its surface properties such as hydrophilicity. Herein, we report a Co-gallate MOF membrane that features preferential adsorption and diffusion of methanol (MeOH) relative to the methyl tert -butyl ether (MTBE) molecules during the PV separation process. The high-quality Co-gallate MOF membrane has been prepared by introducing a regulator of KOH. The MeOH flux of the Co-gallate MOF membrane was 0.565 kg m −2 h −1 and the separation factor was up to 721 at 15 wt% MeOH/MTBE feed composition. It is worth noting that the separation performance exceeds most of the reported membrane materials for MeOH/MTBE separation in the PV process. Furthermore, the separation performance of the Co-gallate MOF membrane for MeOH/MTBE mixtures remained almost unchanged over 70 h, indicating the reliable long-term stability of the membrane. Thus, the Co-gallate MOF membrane demonstrated a potential practical application for MeOH/MTBE separation.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Yongjiang Shan,Mingliang He,Fei Zhang,Yifei Wang,Yuxin Liu,Yingdong Yang,Xingqian Wang,Xinkang Zhang,Yuqin Li,Zhipeng Wang,Xiangshu Chen
Well-intergrown MOF membranes were challenging to construct using the in-situ approach, due to the poor heterogeneous nucleation of MOF on the supports. Here, we described a technique to manufacture ZIF-8 membranes devoid of induced seeds using support modified by O 2 plasma for the first time. O 2 plasma can increase the number of oxygen-containing functional groups (–OH) on the support surface that could absorb zinc ions from synthesizing solution and offer heterogeneous nucleation sites for the formation of ZIF-8 membranes. The as-synthesized membrane exhibits outstanding gas permeation performance with a high hydrogen permeance of about 2.22 × 10 −7 mol·m −2 ·s −1 ·Pa −1 and a high H 2 /CH 4 ideal selectivity of 25.91. The separation factor of the equimolar H 2 /CO 2 and H 2 /CH 4 mixtures reached 8.72 and 31.03 at 298 K and 0.1 MPa, respectively. In addition, this new technique also allowed for the synthesis of ZIF-67 membranes, and the prepared membrane had an H 2 /CH 4 ideal selectivity of 14.92. This work develops a new route for the efficient fabrication of MOF membranes.
研究领域:
材料科学
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化学工程
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Yueyao Liang,Ruquan Zhang,Zhihua Qiao,Chongli Zhong
Supported metal–organic framework (MOF) membranes are promising candidates for energy-efficient natural gas purification, but the preparation of ultrathin MOF membranes supported by polymer substrates remains challenging. Herein, we proposed a polymer collaboration method for preparing ultrathin two-dimensional MOF membranes on polymer support layers. Cu(II) meso-tetra (4-carboxyphenyl) porphyrin (CuTCPP) membranes having thicknesses as low as <10 nm were formed in situ because of the high density of heterogeneous nucleation sites in a polyvinyl alcohol-Cu 2+ interface layer and the controlled anisotropic growth of nanocrystals enabled by a polyvinylpyrrolidone (PVP) surfactant. The prepared CuTCPP membranes showed excellent CO 2 /CH 4 separation performance, yielding a high permeance of 4560 GPU and a moderate selectivity of 31.8. Furthermore, the prepared CuTCPP membranes also displayed good CO 2 /N 2 separation performance, having a CO 2 permeance of 3200 GPU and a CO 2 /N 2 selectivity of 36. The thickness of CuTCPP membranes can be controlled by varying the concentration of metal ions in the organic interface layer. This preparation method can not only fix the active sites for membrane formation but also control the morphology of crystal growth and is applicable to membrane fabrication using other porous MOFs.
研究领域:
材料科学
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化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Yinghui Xu,Xuan Zhao,Ran Chang,Hongqiang Qu,Jianzhong Xu,Jing Ma
Rationally regulating the separation pores is an effective way to achieve efficient separation membrane . However, the developed metal-organic framework (MOF) membranes for water treatment are all formed by one kind of MOF, which can only provide rigid pores, makes it difficult to achieve high flux and excellent rejection ratio simultaneity. Here, we proposed a facile strategy for the synthesis of heterogeneous MOF-on-MOF membrane with hierarchical pores, by site-specific grown ZIF-8 layer on UiO-66-NH 2 layer. Thus unique architecture of the obtained double-layered MOF membrane (UiO-66-NH 2 @ZIF-8) endows multidimensional separation pores: (i) the large pores of UiO-66-NH 2 can facilitate water transportation, (ii) the molecular-sieving pores of ZIF-8 can intercept dyes, (iii) UiO-66-NH 2 acting as active sites can promote the growth of ZIF-8. As a result, the optimized UiO-66-NH 2 @ZIF-8 membrane exhibits high flux (36.7 L m −2 h −1 bar −1 ) and excellent dye rejections (>97.0%). Through analysis and comparison, the regulated multi-type pores play an important role in membrane performance. Coupled with the facile membrane preparing method, this work can used as a potential approach of designing other advanced MOF membrane for water treatment.
研究领域:
材料科学
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环境工程
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化学工程
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Siyuan Qiao,Pei Nian,Guisen Yang,Yingfei He,Xingrui Li,Yibin Wei
Vapor-phase deposition for the preparation of metal–organic framework (MOF) membranes is of great interest in its scalable and sustainable manufacturing. Nevertheless, there remains no report on vapor-assisted conversion (VAC) for preparation of zirconium-based MOF membranes to date. Here, we established a VAC protocol for preparing UiO-66 membranes on the porous α-Al 2 O 3 tube. It was found that the substrate surface modification, metal-to-ligand ratio and concentration of the modulator are crucial parameters to control the quality of the resulting membrane microstructure. The obtained UiO-66 membrane exhibited excellent dye rejection rates (>99.5 %) and reliable operation stability (no reduction in separation performance during 96 h). In addition, the VAC approach also can be adopted to synthesis of high-performance UiO-66-NH 2 and MOF-801 membranes. Therefore, the VAC protocol might open new horizons in sustainable production of water-stable MOF membranes for practical applications.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
Advanced Materials Interfaces
·
2022
·Vol. 9
·期 7
·2101908
·
IF 6.389
Meng Miao,Zhipeng Wang,Zhiming Guo,Jinfeng Xing
A quasi solid–liquid reaction strategy is proposed that is based on the instantaneous transformation of structured solid ligand aggregation into insoluble Cu 3 (HITP) 2 metal–organic framework (MOF) aggregation without morphologic change (HITP = 2,3,6,7,10,11-hexaiminotriphenylene). The initial 3D ordered submicron macropores (TOM) in ligand aggregation can be maintained during the transformation due to the extremely rapid rate of coordination reaction. In this case, the in situ synthesis of the Cu 3 (HITP) 2 MOF film with large-scale TOM structure (TOM-Cu 3 (HITP) 2 film) on ceramic-based gold interdigital electrode (IDE) is achieved. Scanning electron microscope is used to confirm the morphology in each stage of synthetic process. Spectroscopic characterizations prove that there is no essential difference between TOM-Cu 3 (HITP) 2 film and ordinary Cu 3 (HITP) 2 MOF, except for slight differences in the contents of individual surface functional group and integral crystallinities, respectively. Notably, TOM structure endows the TOM-Cu 3 (HITP) 2 film with a dramatic promotion in sensitivity to H 2 S gas. The resistive response of the IDE loaded with TOM-Cu 3 (HITP) 2 film to the 80 ppm H 2 S gas reaches 78.5 at room temperature, which is 6.7× more than that of the Cu 3 (HITP) 2 film without TOM structure. The method of obvious universality allows the authors to perform in situ synthesis directly on the desired substrate without transfer process.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xingxing Wang,Jian Gao,Shuaichuan Cui,Shihan Liu,Yifan Huang,Yifan Zhang,Pengyang Deng
Separation membranes with high solvent permeation and rejection are attractive for energy conservation in waste solvents separation. Herein, ultra-high flux dye separation membrane was firstly obtained by in situ growing continuous thin MOF membranes on commercial non woven fabrics, which overcome the “trade-off” effect of traditional separation membranes. The continuity of MOF membrane is closely related to the grafting density of maleic anhydride (MAH), and the thickness and surface morphology of continuous thin UiO-66-NH 2 membrane (CTUM) can be controlled by tuning reaction time. The CTUM exhibits a molecule weight cut-off of 950 Da and organic solvents permeation of > 2200 L m −2 h −1 bar −1 with the rose bengal (RB) rejection of 99.39 %. The selectivity of CTUM depends on the size screening and electrorepulsion effect, and the permeation of CTUM is at least 10 times higher than conventional separation membranes. Meanwhile, the CTUM is durable under mechanical friction and during filtration. Our work represent a reliable way to make durable MOF membranes for ultra-high permeation organic solvent filtration, which lay a foundation for further exploration of high performance separating membranes.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Guoshu Gao,Yumeng Zhao,Peng Zhu,Haiou Liu,Xiongfu Zhang,Yu Guo,Guohui Yang
The Co-gallate MOF membrane exhibits great potential for separating MeOH/MTBE mixtures due to its regular pore size, exceptional stability, and high hydrophilicity. Nevertheless, the rapid nucleation and growth rate of the Co-gallate crystals in the synthesis solution cause poor nucleation on the substrate surface, which presents a significant challenge for the preparation of continuous Co-gallate membranes. In this study, we presented a cobalt carbonate hydroxide nanowire array (Co-NWA)-induced strategy that enabled the rapid and defect-free synthesis of tubular Co-gallate membranes within just 1 h. The presynthesized Co-NWAs on the substrate played as nucleation centers and anchoring sites, facilitating robust membrane formation. The effects of various synthesis parameters on the crystal morphology and membrane compactness were systematically examined. The optimized Co-gallate membrane demonstrated excellent pervaporation performance, with a permeation flux of 2.03 kg m–2 h–1 and a separation factor of 6711 for a 14.3/85.7 wt % MeOH/MTBE mixture, maintaining high performance for over 100 h, indicative of its remarkable long-term stability. This Co-NWA-induced synthesis strategy presents a promising approach for the industrial-scale application of Co-gallate MOF membranes and the design of other MOF membranes, thereby advancing their utility in requisite liquid separation processes.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Rong Rong,Yanwei Sun,Taotao Ji,Yi Liu
Zirconium-based MOF (Zr-MOF) membranes have attracted widespread attention due to their highly tailorable pore aperture and adsorption behavior achieved by functional group decoration and ligand/cluster-missing defect regulation as well as extraordinary chemical/thermal stability. Nevertheless, it has remained a great challenge to further improve the separation performance of Zr-MOF membranes due to very limited available zirconium sources and heating modes. In this study, we prepared polycrystalline UiO-66 membranes exhibiting unprecedented CO 2 /N 2 selectivity (31.3). The use of layered ZrS 2 , a representative of transition-metal dichalcogenides (TMDCs), as zirconium source during tertiary solvothermal growth was found to be indispensable for improving the separation performance of UiO-66 membranes. As far as we know, the CO 2 /N 2 selectivity reported in this study was the highest among all pristine polycrystalline MOF membranes measured under ambient conditions. More importantly, our study highlighted the importance of concurrent metal source and fabrication process innovation in performance enhancement of polycrystalline MOF membranes.
研究领域:
材料科学
·
化学工程
·
膜技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）