SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Zhenggang Wang,Jianwei Yuan,Renhao Li,Haipeng Zhu,Jingui Duan,Yanan Guo,Gongping Liu,Wanqin Jin
Compared with traditional separation methods, membrane-based technology shows advantages in energy efficiency for natural gas purification. To overcome the performance trade-off of conventional polymeric membranes, in this study, ZIF-301 MOF was employed as novel filler to fabricate 6FDA-DAM polyimide mixed-matrix membranes (MMMs) for CO 2 /CH 4 separation. A solvent exchange approach was proposed to remove the high-boiling-point solvent used for fabricating the MMMs. The microstructures and physico-chemical properties of the ZIF-301 fillers and ZIF-301/6FDA-DAM MMMs were characterized by SEM, EDX, XRD, IR, TGA, DSC and high-pressure sorption isotherms. The CO 2 /CH 4 transport properties through the MMMs were evaluated by permeation measurement at various feed pressures and analyzed by solution-diffusion model. The results showed that the incorporation of ZIF-301 into 6FDA-DAM enhanced both the CO 2 permeability and CO 2 /CH 4 selectivity, attributing to the preferential CO 2 sorption and aperture molecular sieving effect of the ZIF-301 filler. The MMM with optimal ZIF-301 loading of 20 wt% exhibited CO 2 permeability of 891 barrer and CO 2 /CH 4 of 29.3 that surpassed the 2008 Robeson upper-bound, suggesting that ZIF-301 based membrane could be a potential candidate for natural gas purification.
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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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Yi Wang,Liang Li,Fangli Zhang,Huajiang Wang,Zhaoliang Cui,Zhaohui Wang,Xiaozu Wang
Mixed matrix membranes (MMMs) can significantly improve gas separation performance, but the type and state of the filler in the membrane matrix are key indicators for the development of MMMs. Therefore, in this work, 6FDA-DAM/ODA (1:1), metal–organic frameworks (MOFs) with different particle sizes (UiO-66 and UiO-66-NH2) were synthesized, and then MOFs were doped into 6FDA-DAM/ODA to prepare MMMs. The effects of the dopant materials and their particle sizes on the gas separation performance of the membranes were investigated by testing the permeability of the MMMs to H2, CO2, CH4, and N2. When the dopant material was UIO-66, the permeability and selectivity of MMMs for each gas were significantly improved compared with that of the original membrane; when the dopant material was 300 nm UIO-66-NH2 with a loading of 10 wt %, the permeability performance and the CO2/CH4 selectivity increased from 44.1 to 57.2 compared with that of the original membrane. The permeation performance for CO2, N2, and H2 and the selectivity for CO2/N2, H2/N2, and H2/CH4 were also significantly improved. In terms of comprehensive separation performance, doping 300 nm UiO-66-NH2 was better than doping 70 and 400 nm UiO-66-NH2 and also showed excellent performance in 50:50 (vol/vol) CO2/CH4 binary mixed gas separation. This work provides an idea for the fabrication of MMMs for high-performance gas separation.
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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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
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Xiuling Chen,Lei Wu,Cong Xie,Shan Xu,Yanfang Fan,Nanwen Li
Carbon molecular sieve (CMS), as the gas separation membrane materials, still faces challenges for regulation pore diameter precisely. In this work, we propose to reconstruct the 6FDA-DAM-Br-85% polyimide CMS membranes by introducing 6,6'-(1,4-phenylenebis(((4-hydroxyphenyl)amino)methylene))bis(dibenzo[c,e][1,2] oxaphosphinine6-oxide) small molecule compound (DOPO- p -DP) as crosslinking agent to regulate the pore distribution. The crosslinked precursors were obtained via the reaction between C–Br bond in 6FDA-DAM-Br-85% polyimide and N–H bond in DOPO- p -DP compound, the precursors and CMS membranes (550 °C- 2 h) were characterized with ATR-TFIR, XRD and XPS. The pore size distribution of crosslinked CMS membranes was range in 4.5–8.0 Å from the N 2 adsorption data. The crosslinked CMS membranes exhibited excellent gas separation performance, which was strongly dependent on the mass fraction of DOPO- p -DP, an increasing mass fraction of DOPO- p -DP leaded to improve in gas selectivity, while reduced its permeability. The 6FDA-DAM-Br-85%/DOPO- p -DP-20% CMS membrane showed the impressive permeability and superior gas selectivity, the permeabilities of O 2 , CO 2 , and H 2 are 798, 3018, and 13560 Barrer combined with the O 2 /N 2 , CO 2 /CH 4 , and H 2 /CH 4 selectivities of 7.8, 65.6, and 294.8 respectively, the separation performances surpassed the latest trade-off relationship. In addition, the 20% of the DOPO- p -DP crosslinked CMS membrane revealed the superior aging behaviour than that of the 6FDA-DAM-Br-85% CMS membrane over 480 h aging under vacuum conditions.
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
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2021
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IF 8.742
Shan Xu,Xiaolong Ren,Ning Zhao,Lei Wu,Zhiguang Zhang,Yanfang Fan,Nanwen Li
The CO 2 -induced plasticization effects impose detrimental effects on polymeric membranes separation performance. To address this issue, a high-performance crosslinked brominated 6FDA-based polyimide (BMPI) is developed in this work, exhibiting highly suppressed plasticizing effects. The permeability and selectivity of polyimide precursor membranes are tuned by introducing bromine atoms into the polyimide structure, creating a best performing membrane with bromination degree of 60%. The membrane CO 2 permeability reaches 395 Barrer, and the selectivity of CO 2 /CH 4 increases from 22.0 for a non-brominated analogue to 26.0. The debromination induced crosslinked BMPI membranes are achieved upon thermal treatment within the temperature range of 150 °C–350 °C with varied crosslinking degree, resulting in large differences for the membrane separation performance. The completely crosslinked BMPI treated at 350 °C for 10 h demonstrates high CO 2 permeability of 483.6 Barrer and the CO 2 /CH 4 selectivity of 26.0. Most importantly, the crosslinking reaction greatly stabilizes the membrane performance against plasticization under high CO 2 feed pressure. Compared with the non-crosslinked membranes with a plasticizing pressure of 150 psia, the plasticization for the crosslinked membrane occurs at high CO 2 pressure of 600 psia. This study provides a facile approach for the preparation of high-performance gas separation polymeric membranes with enhanced plasticization resistance.
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
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2022
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IF 10.53
Shan Xu,Ning Zhao,Lei Wu,Shuanyan Kang,Zhiguang Zhang,Guolong Huo,Zhongde Dai,Nanwen Li
Tuning the relationship between the microporous structure of carbon molecular sieve (CMS) membranes and the corresponding gas permeability performance enables optimization for gas separation applications. The pre-crosslinked structure of the precursor plays a key role in improving the performance of the CMS membrane. Herein, the thermally crosslinkable brominated 6FDA-based polyimide (BMPI) by debromination is prepared and selected as the precursor to fabricate high performance CMS gas separation membranes . By heat-treating the BMPI membrane at 350 °C for 10 h, the debromination-induced crosslinking exhibited higher permeability over the uncrosslinked precursors, as it forms a pre-crosslinked structure that is more stable at 550 °C. A representative BMPI-350/10h-550 °C CMS membranes pyrolyzed at 550 °C had CO 2 and O 2 permeabilities of 11169 and 2182 Barrer with a CO 2 /CH 4 and O 2 /N 2 ideal selectivity of 26.5 and 5.4. These values are much higher than that of the un-crosslinkable precursor (6FDA-DAM) derived CMS membrane (P CO2 = 3465, α CO2/CH4 = 21.1). Even at the high carbonization temperature of 800 °C, the as-obtained CMS membrane still show a promising CO 2 permeability of 1119 Barrer and a CO 2 /CH 4 ideal gas selectivity of 41.2. Importantly, the excellent gas separation performance of CMS membranes obtained in this work exceeds the Robeson's upper-bound. This work outlines a new protocol to tailor CMS membrane microstructures to meet high permeability performance needs. These CMS membrane materials hold great potential in corrosive natural gas purification applications.
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Xiaobing Wang,Qi Ding,Rimin You,Cong Yu,Yujia Li,Junjie Zhao,Xili Cui,Huabin Xing
The development of efficient membranes for ethylene/ethane (C2H4/C2H6) separation is highly important. Here, we report the development of a series of new mixed matrix membranes (ZnAtzPO4/6FDA-DAM MMMs) based on a microporous material with phosphate anion pillar ZnAtzPO4 (Atz = 3-amino-1, 2, 4-triazole) and 6FDA-DAM polymer matrix. Compared with the pure 6FDA-DAM membranes, the C2H4 permeability and the C2H4/C2H6 selectivity of 10 wt % ZnAtzPO4/6FDA-DAM MMMs were simultaneously increased by 46 and 6%, breaking the trade-off between permeability and selectivity. Interestingly, the separation performance of ZnAtzPO4/6FDA-DAM MMMs at 10 wt % for the equimolar C2H4/C2H6 gas mixture was 105.0 Barrer and 3.90, which surpassed the 2013 upper bound of C2H4/C2H6. For ZnAtzPO4/6FDA-DAM MMMs with 10 wt % filler loading, both the solubility selectivity and the diffusion selectivity continued to rise concurrently, enhancing the C2H4/C2H6 separation performance of ZnAtzPO4/6FDA-DAM MMMs. This work generates a useful concept for the design and fabrication of high-performance MMMs.
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
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IF 8.6
Guozhen Liu,Renhao Li,Xi Chen,Long Cheng,Yu Liu,Gongping Liu,Wanqin Jin
Carbon molecular sieve (CMS) membranes with exceptional separation performance and scalable processing are promising for precise gas separation. However, their broad applicability is hampered owing to stability issues, mainly resulting from physical aging. Herein, we manipulate the pyrolysis temperature (550 °C, 650 °C and 750 °C) to regulate the gas transport properties and control the physical aging of CMS membranes derived from 6FDA-DAM polyimide. The morphology, chemical composition and pore size of the membranes were characterized using SEM, IR, XPS and XRD. Results demonstrated that the pore structure of CMS membranes shows densification with increasing the pyrolysis temperature, affording enhanced separation efficiency for gas pairs: H 2 /N 2 , H 2 /CH 4 , and CO 2 /CH 4 pairs based on the size-sieving effect. Moreover, the effect of aging is more considerable for membranes pyrolyzed at a higher temperature. In addition, the membrane subjected to pre-aging treatment via vacuum storage exhibit better, stable gas separation performance beyond the upper-bond for polymeric membranes. The separation mechanism of the CMS membranes reveals that gas permeation behavior is dominated by diffusion. Tailoring gas permeation and physical aging can provide an alternative approach to tune the gas transport properties of CMS membranes.
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
ACS Applied Engineering Materials
·
2026
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IF 3.5
Zehui Yao,Xinhai Zhang,Yi Wang,Xiaozu Wang,Zhaohui Wang,Zhaoliang Cui
Polyimide (PI) membranes face a trade-off between permeability and selectivity, limiting their gas separation applications. To address this, we synthesized 6FDA-DAM/DABA(DAM:DABA = 3:2) PI and two-dimensional COF-1 nanofillers, fabricating hollow fiber mixed matrix membranes (MMMs) via dry-jet wet-spinning. Under optimized conditions (25 cm air gap, 50 °C spinneret temperature, 30 °C NMP coagulation bath), the 10 wt % COF-1 incorporated membranes achieved optimal performance: tensile strength of 15.34 MPa; H2 and CO2 permeances of 79.3 GPU and 54.3 GPU, and ideal selectivities of 187.9 for H2/CH4 and 128.7 for CO2/CH4, respectively. The results demonstrate that the incorporation of COF-1 modifies solvent exchange during spinning, necessitating targeted optimization of spinning parameters to coordinate membrane structure and performance.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）