SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Peng Li,Yuxiu Sun,Zhengqing Zhang,Zhenjie Gu,Zhihua Qiao,Chongli Zhong
Metal-organic frameworks (MOFs) have driven the development of polycrystalline membranes in the field of gas separation owing to the strong adsorption-desorption behavior and stable framework structure. However, the poor heterogeneous bonding ability between crystals and the substrate leads to the unsatisfactory gas separation as well as low stability of MOF membranes, especially in the humid environment . Herein, we prepared a thin and defect-free UiO-66 membrane by a crystal heterogeneous nucleation assisted growth strategy for efficient CO 2 /N 2 separation. The addition of small amount of water in the precursor solution promoted the crystal nucleation process on the substrate surface. Meanwhile, the smooth PDMS interlayer guaranteed the heterogeneous well-intergrown of crystals into thin UiO-66 membranes, and provided a hydrophobic environment. Therefore, the dense UiO-66 membrane with a small thickness exhibited a high CO 2 permeance (177.4 × 10 −9 mol·m −2 ·s −1 ·Pa −1 ) with moderate CO 2 /N 2 selectivity (24.3) under humid conditions. Furthermore, the prepared membrane demonstrated excellent renewable performance after dehumidification at high temperature, and maintained good hydrothermal stability during long-term operation under the humid environment. This work provides a new insight for the design of high-quality MOF membranes and promotes the development of MOF membranes in practical gas separation process.
研究领域:
材料科学
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化学工程
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气体分离技术
✓ 已验证
产品关联
DOI
高影响因子
Science Advances
·
2024
·Vol. 10
·期 19
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IF 11.7
Tingting Xu,Bin Wu,Wenmin Li,Yifan Li,Yanran Zhu,Fangmeng Sheng,Qiuhua Li,Liang Ge,Xingya Li,Huanting Wang,Tongwen Xu
Fast transport of monovalent ions is imperative in selective monovalent ion separation based on membranes. Here, we report the in situ growth of crown ether@UiO-66 membranes at a mild condition, where dibenzo-18-crown-6 (DB18C6) or dibenzo-15-crown-5 is perfectly confined in the UiO-66 cavity. Crown ether@UiO-66 membranes exhibit enhanced monovalent ion transport rates and mono-/divalent ion selectivity, due to the combination of size sieving and interaction screening effects toward the complete monovalent ion dehydration. Specifically, the DB18C6@UiO-66 membrane shows a permeation rate (e.g., K+) of 1.2 mol per square meter per hour and a mono-/divalent ion selectivity (e.g., K+/Mg2+) of 57. Theoretical calculations and simulations illustrate that, presumably, ions are completely dehydrated while transporting through the DB18C6@UiO-66 cavity with a lower energy barrier than that of the UiO-66 cavity. This work provides a strategy to develop efficient ion separation membranes via integrating size sieving and interaction screening and to illuminate the effect of ion dehydration on fast ion transport.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yanwei Sun,Chunshan Song,Xinwen Guo,Yi Liu
Preferred orientation has proven to exert a significant impact on the gas separation performance of metal–organic framework membranes. Nevertheless, realizing three-dimensional orientation control remains a challenging issue. In this study, well-intergrown NH2-UiO-66 membranes with both (111) out-of-plane and regional in-plane orientations were prepared by combining oriented deposition of seeds and solvothermal epitaxial growth. Dynamic air–liquid interface-assisted self-assembly method was employed to organize uniform octahedral-shaped NH2-UiO-66 seeds into closely packed monolayers with (111) out-of-plane and regional in-plane orientations, whereas the use of ZrS2 as the zirconium precursor during the solvothermal epitaxial growth was found indispensible for sealing the intercrystalline gaps while preserving the preferred orientation inherited from seed layers. In addition, compared with solvothermal heating, employing microwave heating led to poor intergrowth between neighboring NH2-UiO-66 crystals because of a lower dielectric loss factor of the reaction medium. Gas permeation results indicated that the prepared NH2-UiO-66 membranes exhibited H2/CO2 selectivity up to 5.5 times higher than their counterparts with random and/or mere out-of-plane orientations as well as H2 permeability 14.5 times higher than NH2-MIL-125(Ti) membranes with mere out-of-plane orientation under similar operating conditions.
研究领域:
材料科学
·
化学工程
·
膜技术
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Wenmin Li,Tingting Xu,Fangmeng Sheng,Yue Wang,Yifan Li,Yuan Xia,Bin Wu,Xingya Li,Tongwen Xu
The selective separation of monovalent ions remains a challenge because of the similar sub-nanometer sizes. Metal-organic frameworks (MOFs) are promising candidate membranes for ion selective separation based on the angstrom sized windows for size sieving. Here, to further enhance the monovalent ion selectivity , 1, 5-naphthalenedisulfonic acid tetrahydrate (NTDS) molecules with sulfonate groups are incorporated to offer a binding affinity, generating a UiO-66@NTDS membrane via the window-cavity structure confinement. In addition to the size sieving effect, the charge and affinity interaction can compensate the energy loss induced by the ion dehydration. Thus, the UiO-66@NTDS membranes exhibit elevated separation performance compared to the original UiO-66 membranes under the concentration gradient driven, accompanied by high monovalent cation permeation rates (i.e., 0.3–0.7 mol m −2 h −1 ) and mono-/divalent cation selectivities (i.e., ∼73 for K + /Mg 2+ , ∼57 for Na + /Mg 2+ , and ∼46 for Li + /Mg 2+ ). This work provides guidelines for the development of efficient ion-selective MOF membranes via the combination of size sieving and interaction attraction.
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Shenyi Tang,Chenglian Luo,Zhi Wang,Xinlei Liu
A defect-free and stable metal–organic framework (MOF) membrane is a promising candidate for the separation of methanol/methyl tertiary butyl ether (MeOH/MTBE) mixtures. In this work, a structural-integrity and low-thickness (∼400 nm) UiO-66 membrane was fabricated by regulating the metal ion/ligand molar ratio in the synthesis solution and optimizing the preparation process using the secondary growth method with safer and more environment-friendly Zr(n-OPr)4 metal source. Based on the effective pore size and inherent amphiphilic structure of UiO-66, the membrane exhibits exceptional pervaporation (PV) performance. For the separation of MeOH/MTBE (5:95 wt/wt %) mixtures, the membrane displays an outstanding separation performance with an average separation factor of 2.23 × 104 and an average total flux of 3.61 kg·m–2·h–1 at 40 °C, which is superior to most membranes reported for the PV separation of MeOH/MTBE mixtures. In addition, a 72 h PV process was used to further confirm the structural stability of the membrane.
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）