MICROPOROUS AND MESOPOROUS MATERIALS
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2018
·
IF 3.649
Yunzhe Jiang,Chuanyao Liu,Jürgen Caro,Aisheng Huang
A new UiO-66-NH 2 based MOF named UiO-66-NH 2 @ICA has been prepared by grafting imidazole-2-carbaldehyde (ICA) to UiO-66-NH 2 through a post-synthesis reaction via amine condensation. FESEM , XRD , 1 H NMR, FT-IR and N 2 adsorption were used to characterize the morphology and structure of UiO-66-NH 2 @ICA. The grafted ICA mainly reduces the pore volume of UiO-66-NH 2 but increases the number of nitrogen atom as binding site of CO 2 . The UiO-66-NH 2 @ICA showed less BET surface area but a higher CO 2 /CH 4 adsorption selectivity in comparison with UiO-66-NH 2 . UiO-66-NH 2 @ICA and UiO-66-NH 2 crystals were dispersed in Matrimid ® 5218 to form mixed-matrix membranes (MMMs). Single gas permeation and mixed gas separation was carried out to investigate the effects of filler loading and feed gas pressure on the separation performances of the MMMs. The UiO-66-NH 2 @ICA/Matrimid ® MMM with 10 wt % filler showed a high CO 2 /CH 4 selectivity with a separation factor of 64.7, which is an increase by 40% in comparison with UiO-66-NH 2 /Matrimid ® MMM.
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xue Yang,Yuxuan Wang,Jingxian Hua,Rujing Hou,Jinfeng Chen,Qihan Gong,Chongqing Wang,Yichang Pan
Plate-like or sheet-like porous materials with nanometer thickness have been considered as the preferred fillers to improve mixed-matrix membranes (mmms)-based separation. Herein, hexagonal Co-fa (HG-Co-fa) nanoplates were simply synthesized without the addition of any modifier and used as fillers to construct 6FDA-DAM-based MMMs for efficient CO 2 /CH 4 separation. HG-Co-fa nanoplates exhibit high dispersion and interface compatibility in 6FDA-DAM matrix. The results demonstrated that the CO 2 /CH 4 separation performance of 6FDA-DAM was obviously improved after the incorporation of HG-Co-fa nanoplates. The resultant MMMs with nanoplate loading of 10 wt% showed CO 2 /CH 4 selectivity of 27 and CO 2 permeability of 1419 Barrer at 25 ℃ and 0.2 MPa, surpassing 2008 Robeson upper bound. Meanwhile, the high lattice integrity and structural stability of HG-Co-fa nanoplates contribute to the excellent thermal and mechanical stability of MMMs, contributing to their anti-plasticization property up to 14 bar and long-term stability up to 240 h, indicating their potential for natural gas separation.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2019
·
IF 5.107
Meidi Wang,Kaidong Quan,Xiaohong Zheng,Yu Cao,Xiangyu Cui,Ming Xue,Fusheng Pan
Two-dimensional (2D) covalent organic nanosheets (CONs) present versatile 2D materials, which hold great promise in mixed matrix membranes. The facile synthesis of CONs for the fabrication of mixed matrix membranes represents the development trend. Herein, mixed matrix membranes with facilitated transport ability were prepared based on self-exfoliated covalent organic nanosheets (CONs) and poly(ether-block-amide) (Pebax® MH 1657) matrix. The self-exfoliated TpDT CONs were facilely synthesized via Schiff base condensation reaction between 1,3,5-Triformylphloroglucinol (Tp) and 3, 5-diamino-1,2,4-triazole (DT). Abundant amine groups on TpDT CONs skeleton served as facilitated transport carriers to promote the transport of CO 2 by reversible nucleophilic addition reactions. And the highly ordered channels of TpDT CONs allowed the rapid transportation of CO 2 molecules to reach the facilitated transport carriers. Moreover, the incorporated TpDT CONs disturbed the packing of the Pebax chains by the intervention effects and increased the chain mobility. The facilitated transport carriers from TpDT CONs and the optimized structure endowed the as-prepared membranes with elevated permeance and selectivity. Specially, the Pebax-TpDT/PVDF membranes with 1 wt% TpDT CONs achieved an optimum CO 2 /CH 4 separation performance with a separation factor of 36.0 and a CO 2 permeance of 142.3 GPU, which were increased by 68% and 131%, respectively, compared with the pristine Pebax membrane.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
Advanced Materials Interfaces
·
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
ACS Sustainable Chemistry & Engineering
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2019
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IF 6.97
Chunyu Li,Chao Wu,Baoquan Zhang
Blending porous inorganic fillers into polymers to fabricate mixed matrix membranes (MMMs) is an efficient method to acquire good-quality membranes for CO2 separation and purification. The poor interface coupling between bulky filling particles and polymer phase in MMMs results in reduced mechanical strengths with low separation performances. The novel two-dimensional (2D) and ultrathin α-Ni(im)2 nanosheets with high aspect ratios are herein synthesized and blended with Pebax MH 1657 to prepare MMMs. The larger contacting area and strong hydrogen bonding between α-Ni(im)2 nanosheets and Pebax improve their compatibility to form defect-free MMMs. The ultrathin α-Ni(im)2 nanosheets in MMMs can effectively enhance CO2/CH4 selectivity based on molecular sieving. With the addition of 2 wt % of α-Ni(im)2 nanosheets, the as-prepared MMMs exhibit CO2/CH4 selectivity up to 33.4 with a permeability of 100.6 Barrer. Compared with pure Pebax membrane, the separation selectivity shows a 72% increase with no significant change in CO2 permeability.
研究领域:
材料科学
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化学工程
·
膜技术
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DOI
高影响因子
HIGH PERFORMANCE POLYMERS
·
2022
·
IF 1.73
Shuo Yan,Haibin Yu,Zan Chen
Membranes with both good permeation and selectivity are highly desired for gas separations. In this study, we synthesized a new 6FDA-type polyimide copolymer 6FDA-BDTA-ODA, and then an organic polymer of poly (N-vinylimidazole) was doped into the polyimide to prepare mixed matrix membranes (MMMs). We also studied the effect of poly (N-vinylimidazole) contents on the separation performance of MMMs. The results showed that the ideal selectivity for CO2/CH4 was improved by adding the poly (N-vinylimidazole) filler. The ideal selectivity reached 63.5 with 6 wt% poly (N-vinylimidazole) loading with the permeability of 29.2 Barrer. The highly permeable MMMs showed a considerably enhanced performance for CO2/CH4 that close to the 2008 Robeson upper-bound. The gas separation performance of the prepared MMMs for CO2/CH4 was improved compared to that of the pure polymer membrane, indicating that the copolyimide/poly (N-vinylimidazole) MMMs have promising applications in CO2/CH4 gas separation.
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
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Chengli Jiao,Xiangju Song,Xiaoqian Zhang,Lixian Sun,Heqing Jiang
Control of the surface morphology of polyamide membranes fabricated by interfacial polymerization is of great importance in dictating the separation performance. Herein, polyamide membranes with a specific nanoscale striped Turing structure are generated through facile addition of Zr-based metal–organic framework UiO-66-NH2 in the aqueous triethylenetetramine phase. Interestingly, accompanied by the degradation of UiO-66-NH2 in aqueous solution, an intermediate complex is in situ formed through the strong interaction between the Zr metal center and the amine group from triethylenetetramine, which can lower amine diffusion and induce a local interfacial reaction, contributing to the generation of a homogeneous nanoscale striped Turing structure. The resulting membranes are used for CO2/CH4 gas separation. Compared with the parent polyamide membrane displaying a CO2/CH4 selectivity of 43.1 and a CO2 permeance of 31.5 GPU, the membrane with 0.02 wt % of UiO-66-NH2 introduced into the aqueous phase shows a higher CO2/CH4 selectivity of 58.3, along with a CO2 permeance of 27.1 GPU. Additionally, when 0.1 wt % of UiO-66-NH2 is incorporated into the aqueous phase, the membrane exhibits a combination of a higher CO2/CH4 selectivity and an enhanced CO2 permeance in contrast with the parent polyamide membrane.
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
PubMed
高影响因子
Journal of Materials Chemistry A
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2022
·Vol. 10
·期 47
·24975-24984
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IF 14.511
Lili Gong,Zhili Cai,Qi Wu,Lu Liu,Can Wang,Linglong Shan,Xianghai Meng,Shuangjiang Luo,Zhichang Liu,Suojiang Zhang
Mixed matrix membranes (MMMs) are highly promising for natural gas sweetening due to their high microporosity and outstanding gas separation performance. However, MMMs are frequently challenged by the polymer/filler interfacial incompatibility, leading to the deterioration of gas separation performance. In this study, the mixed-linker ZIF-7-8 was employed as a filler by finely tuning the molecular sieving for CO2/CH4 separation. An amino-functionalized ionic liquid ([C3NH2Mim][Cl]) was introduced for constructing the interface connection between the ZIF-7-8 filler and polymer matrix through coordination and hydrogen bonding, which was verified by extended X-ray absorption fine structure (EXAFS) and electron paramagnetic resonance (EPR). The design of interface interaction through an IL is crucial to improve the interface compatibility and the CO2/CH4 separation performance. The newly developed 20% ZIF-7-8-IL (1%)/PI and 25% ZIF-7-8-IL (1%)/PI MMMs displayed a dramatic improvement of CO2 permeability by 244.2% and 291.6%, from 308 to 1060 and 1206 barrer, respectively, for pure-gas separation, compared to the pristine polyimide matrix. Moreover, the 25% ZIF-7-8-IL (1%)/PI MMM also demonstrated outstanding low-temperature mixed-gas CO2/CH4 separation performance in the temperature range of −45–35 °C, far beyond the 2018 mixed-gas CO2/CH4 upper bound.
研究领域:
材料科学
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环境工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jiawu Huang,Cuiting Yang,Shengjun Du,Lin Zhu,Zhenglin Du,Guang Miao,Chunshan Song,Jing Xiao
Adsorption-based capture of carbon dioxide (CO 2 ) to upgrade natural gas offer a promising solution for energy crisis and the reduction of CO 2 emission. However, trade-off between high adsorption selectivity and rapid kinetic is an inherent shortcoming of size-sieving based adsorptive separation of gas molecules at similar sizes, hindering the launch of sieving adsorbent for practical challenging selective gas capture. Herein, a gradiently porous carbon nanofiber PCF-800 with interconnected sieving ultramicropores and low-proportion surficial mesopores is tailor-made to simultaneously realize the exclusive and rapid capture of CO 2 from CH 4 . Arising from the unique interconnected micro-mesoporous structure, the as-prepared PCF-800 not only achieves remarkable uptake ratio of 45 (298 K, 1 bar) for CO 2 /CH 4 separation via size-sieving effect but also shows fast kinetic with diffusion rate of 1.35 × 10 -3 s −1 , outperforming the conventional ultramicroporous counterpart. Moreover, the impressive dynamic CO 2 /CH 4 separation factor up to 21.7 and satisfying cycling durability revealed by the breakthrough experiments further imply the industrial potential of PCF-800 in practical CH 4 purification. This work may shed light on the design of gradient sieving carbonaceous adsorbent with high selectivity and fast kinetic for extensive high-performance small gas separation.
研究领域:
材料科学
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环境工程
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产品关联
DOI
高影响因子
Membranes
·
2025
·Vol. 15
·期 5
·128
·
IF 3.6
Yingxiu Wu,Haiyan Guo,Bingyu Zhao,Yuxiu Yu,Yaodong Liu,Shouchun Zhang
Carbon molecular sieve (CMS) membranes demonstrate considerable advantages and significant potential in the separation of CO2and CH4. Nevertheless, current research predominantly emphasizes the enhancement of CMS membranes through the incorporation of rigid structures and chain spatial stacking. The role of flexible structures in this context remains inadequately understood. To address this gap, we introduced long-chain polydimethylsiloxane (PDMS) and copolymerized it to synthesize polyimide that combines rigid and flexible frameworks. This approach enabled us to investigate the impact of flexible structures on the structure and properties of carbon membranes by varying the PDMS content. The findings indicated that flexible PDMS significantly influenced the thermal decomposition behavior of polyimide and facilitated in situ silicon doping within the carbon membranes, thereby modifying the pore characteristics of the carbon film. Specifically, with a 10% addition of PDMS, the CO2permeability of the CMS membrane reached 9556 Barrer, representing an enhancement of 103.9% and surpassing the 2019 upper bound for CO2/CH4separation. Furthermore, the effect of pyrolysis temperature was also examined. Ultimately, this study offers a novel perspective on regulating the structural and performance characteristics of carbon membranes through the integration of long-chain flexible structures.
研究领域:
材料科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Peng Hu,Hao Wang,Chao Xiong,Hao Liu,Jun Han,Jie Zhou,Zhenxia Zhao,Yongqing Wang,Hongbing Ji
We demonstrate a novel microwave-assisted strategy to in situ functionalize the node chemistry of Zr-based metal–organic frameworks (Zr-MOFs) with a 2-aminobenzimidazole (2-AMI) agent. The novel strategy can concomitantly weaken the Lewis acidity of Zr6O8 nodes of Zr-MOFs through bonding with 2-AMI, contributing to admirable surface hydrophobicity with an ultrahigh water contact angle of 151.7° and enhanced stability. The successful coordination process was jointly verified by thermogravimetry analysis, 1H nuclear magnetic resonance spectroscopy , and X-ray photoelectron spectroscopy analyses. Meanwhile, the tailor-made pore microenvironment enabled highly efficient CO2/CH4 separation via a synergetic equilibrium-kinetic effect. Gas adsorption isotherms and time-dependent kinetic profiles cooperatively reveal that UiO-66(N10%-Zr) exhibits an advanced ideal adsorbed solution theory selectivity of 326, an excellent diffusion selectivity of 60.7, and a dynamic selectivity of 195 for CO2/CH4 separation, confirming the unwanted equilibrium-kinetic effect. Breakthrough experiments and modeling simulations further confirm the enhanced hydrophobic nature and high CO2/CH4 separation performance of UiO-66(N10%-Zr) even under humid conditions. The node-based engineering strategy is here demonstrated to be highly effective for CO2/CH4 separation, providing a new direction to achieve advanced MOF structures with sustainable advantages including high adsorption capacity, high selectivity, and hydrophobicity, which are of crucial significance for industrial applications.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
Journal of Natural Gas Science and Engineering
·
2018
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IF 2.803
Tengyang Zhu,Xing Yang,Yi Zhang,Yayun Zheng,Xiaoqi He,Jujie Luo
Air pollution gradually aggravated, which accelerates the demand of clean energy (in particular clean natural gas) because of its abundant storage worldwide. However, raw natural gas commonly contains impurity gases, such as CO 2 and N 2 , which reduce the heat of its combustion. Here, we reported new polyamide-poly(propylefne glycol) (PA-PPG) random and block copolymer materials with excellent CO 2 /CH 4 separation performance. These copolymers were characterised by Fourier-transform infrared spectroscopy (FTIR), nuclear magnetic resonance spectroscopy ( 1 H NMR), UV–vis absorption spectrum and X-ray diffraction (XRD). The gas permeation properties of these copolymers were investigated by using five single gases (CO 2 , H 2 , O 2 , CH 4 and N 2 ) at different temperatures (298–328 K) and a feed pressure of 76 cmHg. The effects of chemical structure, PPG content and operating temperature on the gas permeation properties of these copolymers were also further discussed. Results showed that PA-PPG random copolymer membranes exhibited better gas permeation properties than those of PA-PPG block copolymer membranes. PA-PPG random copolymer membrane with 20 wt% PPG exhibited the highest selectivity (CO 2 /CH 4 = 37.31 and H 2 /CH 4 = 33.44) at 298 K and 76 cmHg. The CO 2 and H 2 permeability values were 5.97 Barrer and 5.19 Barrer, respectively.
研究领域:
材料科学
·
环境科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）