ACS Applied Materials & Interfaces
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2022
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IF 10.383
Jinyin Lv,Yanwen Cui,Jianhua Yang,Liangqing Li,Xuerong Zhou,Jinming Lu,Gaohong He
Fluorinated metal–organic framework materials (NbOFFIVE-1-Ni, also referred to as KAUST-7) have attracted widespread attention because of their high chemical stability and thermal stability, outstanding tolerance with water and H2S, and high CO2-adsorption selectivity over H2 and CH4. KAUST-7 was expected to be a new membrane material candidate for H2/CO2 separation because of the hindered permeation of CO2 resulting from the interaction between CO2 and (NbOF5)2– of the KAUST-7 framework. A highly H2 perm-selective KAUST-7 membrane was first achieved using a novel strategy of inorganic pillar center-facilitated counterdiffusion (IPCFCD) proposed by us. The IPCFCD method not only effectively avoided the corrosion of hydrofluoric acid to α-Al2O3 tubes in the process of preparing KAUST-7 membranes, but also better reduced grain boundary defects because of the faster nucleation rate and resultant high crystallinity. The KAUST-7 membrane exhibited a high H2/CO2 separation factor (SF) of 27.30 for the 1:1 H2/CO2 binary gas mixture with a high H2 permeance of 5.30 × 10–7 mol m–2 s–1 Pa–1 under ambient conditions and a slight decrease of the H2/CO2 SF with increasing operation temperature and presence of steam. This study highlighted the importance of pre-synthesizing inorganic pillar centers (NiNbOF5 intermediate) and the innovation of a membrane formation process for synthesizing polycrystalline KAUST-7 membranes. Most important of all, our study provided a novel approach to overcome the challenge in fabricating metal–organic framework membranes containing corrosive reactants for the corresponding supports.
研究领域:
材料科学
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化学工程
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DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Ke Chen,Xin Guo,Linhan Ni,Junwen Qi,Jiansheng Li
Rational design and construction of fillers and polymers are crucial for the development of high-performance mixed matrix membranes (MMMs). In this work, amino-functionalized metal-organic frameworks KAUST-7 (KAUST-7-NH 2 ) with square-shaped sheet morphology were utilized as fillers to fabricate MMMs by physical blending with the polymer of intrinsic microporosity (PIM-1). The square-shaped KAUST-7-NH 2 sheets, prepared via in situ replacement of 2-aminopyrazine into the KAUST-7 framework, exhibited superior separation performance compared to the mono-ligand KAUST-7. Benefiting from the strong CO 2 affinity, high porosity and optimal pore sizes of KAUST-7-NH 2 , the outstanding CO 2 /CH 4 separation performance of the composite membrane was observed. The integration of square-shaped KAUST-7-NH 2 sheets provides a 2.5-fold improvement in CO 2 /CH 4 selectivity together with acceptable gas permeability as compared to the original PIM-1 membrane. Furthermore, a 100-h continuous permeation test validated the stability of the fabricated MMMs. Remarkably, the resulting MMM retained 92% of their initial CO 2 permeability after 150 days (drop of only 249 Barrer), indicating that the reduction in CO 2 permeability was approximately 10-fold lower than that of the pristine PIM-1 membrane. The prepared MMMs exhibit enhanced CO 2 /CH 4 selectivity and long-term stability, making it a highly promising candidate for practical application.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Ke Chen,Linhan Ni,Hao Zhang,Chengming Xiao,Li Li,Xin Guo,Junwen Qi,Chaohai Wang,Xiuyun Sun,Jiansheng Li
Rational design of fillers and polymers is of great importance to fabricate mixed matrix membranes (MMMs) with high performance. In this work, fluorinated metal-organic frameworks (KAUST-7 (also referred as NbOFFIVE-1-Ni)) were adopted as nanofillers to prepare MMMs through physically blending into the polymer of intrinsic microporosity (PIM-1). Benefiting from the features of porous KAUST-7, including well CO 2 affinity, distinctive pore characteristics (size, shape, and functionality) and strong intermolecular interactions with PIM-1, the achieved MMMs demonstrated increased CO 2 /CH 4 separation performance and improved anti-physical aging property. Specifically, with the assistance of KAUST-7, the CO 2 permeability and CO 2 /CH 4 (30:70 vol%) selectivity of the optimized MMMs increased up to 5928 Barrer and 23.5, corresponding to improvements of 50% of and 88% of the permeability and selectivity compared with the pristine membranes, respectively. Importantly, 100-h continuous separation test results confirmed the satisfying long-term stability of the prepared MMMs. Notably, the MMMs maintained 91% of the initial CO 2 permeability after 150 days (decreased only 539 Barrer), implying that the CO 2 permeability decrement is about 5-fold lower than that of the control PIM-1 membrane. These results suggest that the fabricated MMMs are promising candidates for CO 2 separation in practical applications.
研究领域:
材料科学
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环境工程
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Jinyin Lv,Xuerong Zhou,Jianhua Yang,Lei Wang,Jinming Lu,Gaohong He,Yingchao Dong
A well-intergrown and defect-free tubular KAUST-7 membrane was fabricated via in-situ synthesis assisted by fluorinated molecular building block using green solvent of water on coarse asymmetric α-Al 2 O 3 tubes. The strategy averted the serious corrosion of high-concentration hydrofluoric acid (HF) to α-Al 2 O 3 supports due to the substitution of HF with the pre-synthesized NiNbOF 5 , overcoming the difficulty of serious corrosion to supports compared to traditional one-pot synthesis. The pH manipulation of synthesis solution is proved crucial to the fabrication of defect-free KAUST-7 membranes. In addition, effects of reactant concentration, crystallization temperature and reaction solvents on the morphology and separation performance of KAUST-7 membrane were investigated. The optimized KAUST-7 membrane M4 exhibited a H 2 perm-selectivity of 17.7 over CO 2 for H 2 /CO 2 binary mixture with a H 2 permeance of 2.2 × 10 −7 mol m −2 s −1 Pa −1 at 25 °C and 1 bar, while the H 2 /CO 2 separation factor just had a slight decrease when test temperature increased to 120 °C. The formation mechanism of KAUST-7 membranes via in-situ method in this work was investigated by exposing a bare α-Al 2 O 3 tube into NiNbOF 5 aqueous solution at the pH of 4.0 at 130 °C for 12 h. XPS and FT-IR observations revealed the formation of AlF x O y or AlF x species, which were deduced to be acted as linkers to connect with 2D Ni (II)-pyrazine layers, promoting the heterogeneous nucleation of KAUST-7 crystals on the surface of Al 2 O 3 support.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2018
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IF 6.578
Ke Chen,Kai Xu,Long Xiang,Xiao Dong,Yue Han,Chongqing Wang,Lin-Bing Sun,Yichang Pan
Mixed matrix membranes (MMMs) derived from metal-organic frameworks (MOFs) nanocrystals represent a promising alternative for overcoming the trade-off between permeability and selectivity derived from the pristine polymeric membrane . The selection of MOFs fillers are mainly focused on their diffusion-selectivity property for gas-pairs. However, the improvement of both gas-permeability and selectivity through addition of sorption-selective MOFs are rarely reported. Herein, the incorporation of CO 2 -philic KAUST-7 (also referred to as NbOFFIVE-1-Ni) nanocrystals makes the neat 6FDA-Durene polyimide membrane more permeable and more selective, surpassing the state-of-the-art 2008 Robeson upper bound for CO 2 /CH 4 . Nano-sized (~ 80 nm) KAUST-7 crystals with sharp particle size distribution were first fabricated through a co-solvent synthesis method. The explored gas transportation mechanism indicates that the improvement of CO 2 /CH 4 selectivity on MMMs are attributed to the significant raise of the sorption-selectivity rather than the diffusion-selectivity. The favorable interfacial interaction between the imide groups of the 6FDA and the H of the pyrazine in the KAUST-7 enhances plasticization resistance of the neat polymer membrane. The developed MMMs exhibit a promising application in CO 2 capture from natural- and bio-gas.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
Advanced Materials Interfaces
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2023
·Vol. 10
·期 12
·2202524
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IF 5.4
Lei Wang,Xianying Bai,Yawei Gu,Xinxin Shi,Shilong Wang,Jingxian Hua,Rujing Hou,Chongqing Wang,Yichang Pan
2D metal–organic frameworks are attractive filler in mixed matrix membranes (MMMs) due to the high aspect ratio and contact opportunity at the filler–polymer interface. However, their alignment in polymer matrix remains a challenge to fully play their functions. Herein, to our best knowledge, for the first time, the facile synthesis of KAUST-7-NH 2 (KAUST, King University of Science and Technology) nanoplate is reported with 1D channels with an aspect ratio greater than 30. The nanoplates are incorporated and aligned in the 4,4′-(hexafluoroisopropylidene) diphthalic anhydride-2,4-diaminomesitylene (6FDA-DAM) polymer matrix under the shear force with a filler loading up to 50 wt%. The large difference in adsorption abilities between CO 2 and CH 4 from the (001)-oriented KAUST-7-NH 2 nanoplate-based MMMs and the favorable interaction at the filler–polymer interface contribute to the excellent CO 2 /CH 4 separation performance. The resultant membranes show CO 2 /CH 4 selectivity with 66.2% enhancement (surpassed 2008 Robeson upper bound), antiplasticization up to 17 bar, and long-term stability up to 240 h indicating its good potential for natural gas treatment.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Zeyu Chang,Xiaoxia Jia,Tong Li,Yong Wang,Libo Li
In the petrochemical industry, the separation of C4 olefins is crucial but a challenging and energy-intensive process. In this study, two fluorinated anion-pillared hybrid ultramicroporous materials (HUMs), namely KAUST-7 (NbOFFIVE-1-Ni) and KAUST-8 (AlFFIVE-1-Ni), were explored for the efficient separation of ternary C4 olefin mixtures (C 4 H 6 /n-C 4 H 8 / iso -C 4 H 8 ) via gate-opening and size-sieving effects. KAUST-7, with a narrow and flexible pore window that completely excludes iso -C 4 H 8 , but allows for the absorption of C 4 H 6 and n-C 4 H 8 through gate-opening effects, with a preferential adsorption of C 4 H 6 due to its easier access to the channel. KAUST-8, on the other hand, with a larger pore window size and the strong H-bond interactions between the electronegative fluorine atoms from inorganic anion pillar and the C4 olefin molecules, efficiently separates iso -C 4 H 8 from C4 olefins, as the adsorption of both C 4 H 6 and n-C 4 H 8 is significantly enhanced while iso -C 4 H 8 retains much lower adsorption capacity. The relationship between the structures and separation properties of these materials is discussed, providing insight into the development of efficient separation materials. Fixed bed breakthrough experiments verify the excellent separation performances of KAUST-7 and KAUST-8 for C 4 H 6 /n-C 4 H 8 / iso -C 4 H 8 , highlighting their potential for industrial applications.
研究领域:
材料科学
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石油化工
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吸附分离技术
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DOI
高影响因子
危险品化学品经营许可证（带存储）