RSC Advances
·
2021
·Vol. 11
·期 46
·28863-28875
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IF 3.361
Yu Qin,Li Xu,Liying Liu,Xiaoyu Deng,Yucheng Gao,Zhongwei Ding
A novel gas separation approach is proposed in this work by combining an amine-based solid adsorbent with a zeolitic imidazolate framework-8 (ZIF-8) membrane. This was achieved by incorporating the amine-based solid adsorbent during the fabrication of the ZIF-8 membrane on a macroporous substrate. An amine-based solid adsorbent was prepared using porous ZIF-8-3-isocyanatopropyltrimethoxysilane (IPTMS) and N-[(3-trimethoxysilyl)propyl]diethylenetriamine (3N-APS) amine compounds. The as-prepared porous amine-based solid adsorbent (denoted as ZIF-8-IPTMS-3N-APS) possessed excellent adsorptive CO2/N2 and CO2/CH4 separation performances. As the adsorbent needs to be regenerated, this could indicate that the CO2 adsorption separation process cannot be continuously operated. In this work, an amine-based solid adsorbent was applied during the preparation of the ZIF-8 membranes owing to the following reasons: (i) gas separation by the membrane can be operated continuously; (ii) the amino group provides a heterogeneous nucleation site for ZIF-8 to grow; and (iii) the reparation of surface defects on the macroporous substrate can be performed prior to the growth of the ZIF-8 membrane. Herein, the ZIF-8 membrane was successfully fabricated, and it possessed excellent CO2/CH4, CO2/N2, and H2/CH4 separation performances. The 0.6 μm ultrathin ZIF-8 membrane demonstrated a high CO2 permeance of 4.75 × 10−6 mol m−2 s−1 Pa−1 at 35 °C and 0.1 MPa, and ideal CO2/N2 and CO2/CH4 selectivities of 4.67 and 6.02, respectively. Furthermore, at 35 °C and 0.1 MPa, the ideal H2/CH4 selectivity of the ZIF-8 membrane reached 31.2, and a significantly high H2 permeance of 2.45 × 10−5 mol m−2 s−1 Pa−1.
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
MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Peng Yan,Jucai Yang,Deyun Ma,Siyun Zhang,Shigong Zeng,Liting Feng,Sihui Zhan,Qiaquan Lin
A water-stable porous cobalt(II)–organic framework functionalized by ethoxyl groups with a chemical formula, {[Co 6 (5-EIA) 5 (tmbpy)(OH) 2 (H 2 O) 2 ]∙4(H 2 O)} n ( 1 ) (5-H 2 EIA = 5-ethoxy-isophthalic acid; tmbpy = 3,3′-dimethyl-4,4′-bipyridine) has been constructed and studied in terms of structure and performance. 1 shows a 3D framework, and has a 1D channel of 8.1 × 6.0 Å 2 along the a axis. The framework 1 exhibits high humid and thermal stability according to PXRD and TGA results. The C 2 H 2 and CO 2 uptakes of the activated 1 ( 1a ) were up to 2.07 mmol g −1 and 1.89 mmol g −1 at 273 K (100 kPa), respectively. More importantly, 1a shows excellent C 2 H 2 /CH 4 (1:1) and CO 2 /CH 4 (1:1) separations with IAST selectivity of 23.7 and 11.4 at 298 K (100 kPa), respectively. Furthermore, 1a showed good reuse performance, suggesting that 1a could be applied to the separation of C 2 H 2 /CH 4 or CO 2 /CH 4 .
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 POROUS MATERIALS
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2025
·
IF 3.2
Qian Yi,Jiang Qingqing,Xiang Shimeng,Lu Zhenhao,Xu Xiaowen,Yang Jing,Dai Guoliang,Song Ruifeng,Jiang Ji
Separating CO 2 and N 2 from CH 4 is crucial for energy production and environmental protection. This study showed the rapid synthesis of CHA zeolites with different morphologies using an in situ growth method, without the assistance of organic structure directing agents (OSDA) or fluoride media. The crystallization behavior of CHA zeolites was studied in terms of synthesis gel composition (including water content, silicon and aluminum content, alkalinity and Sr 2+ concentration), synthesis temperature and duration. The results suggested that pure phase CHA zeolite nano-aggregates could be synthesized with broad precursor conditions at 150 °C for only 4 h. Then, K-CHA zeolite was ion-exchanged to Na-CHA and Ca-CHA and the adsorption properties of CHA zeolites with different morphologies and ions were studied. The results suggested that Na-CHA exhibited highest CH 4 , CO 2 and N 2 adsorption capacity and showed higher ideal selectivity for N 2 /H 2 ; Although Ca-CHA zeolites exhibited relative lower CO 2 and CH 4 adsorption capacity, it exhibited the highest ideal selectivity for CO 2 /CH 4 ; Simultaneously, K-CHA zeolite exhibited high CH 4 adsorption capacity and high adsorption separation ability of CH 4 /N 2 . Furthermore, breakthrough experiments have confirmed the practical feasibility of separating CO 2 from CH 4 .
研究领域:
材料科学
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化学工程
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吸附与分离
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分子筛合成
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气体分离
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2024
·
IF 4.4
Wei Li,Jingyun Wang,Mengmeng Han,Shanshan Xu
Obtaining pure clean energy methane (CH 4 , 3.80 Å) from natural gas is a great challenge task at present due to the similar kinetic diameter with nitrogen (N 2 , 3.64 Å). Herein, a well-defined rod-like bimetallic MOF (Cu 0.5 Ca 0.5 -SBMOF) with an excellent adsorption performance for CH 4 was successfully prepared and blended as filler with Matrimid® 5218 (PI) for preparing mixed matrix membranes (Cu 0.5 Ca 0.5 -SBMOF@PI MMMs). In the separation experiment of N 2 /CH 4 binary gas mixture, both filler loadings and trans -membrane pressure have significant effects on the separation performance of MMMs. When the filler loading is 20 wt%, Cu 0.5 Ca 0.5 -SBMOF@PI MMMs exhibits an excellent separation performance with a separation factor of CH 4 /N 2 up to 17.03, and the permeability of 22.57 barrer for N 2 , which significantly preceded the most reported MMMs. Moreover, the prepared MMMs also show excellent stability. This work has taken an important step towards practical application in the field of separating N 2 /CH 4 gas mixture using MMMs method.
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 MEMBRANE SCIENCE
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2022
·
IF 10.53
Ruoxing Liao,Yumin Guo,Liqiu Yang,Haoli Zhou,Wanqin Jin
Membrane technology , a successful technology for separating gases such as CO 2 /CH 4 mixture, has attracted much attention because of its low energy consumption, and membrane performance is an important factor affecting its industrial application. Herein, the solvent-induced microstructure of a polyimide membrane was employed to enhance its CO2/CH4 separation performance. The effect of solvents on the membrane structure and gas separation performance was investigated by using different solvents (such as tetrahydrofuran, N,N-dimethylacetamide) to dissolve a newly synthesized polyimide polymer, which was fabricated into a membrane. Various characterization methods, such as positron annihilation lifetime spectroscopy (PALs) and X-ray diffractometry (XRD), were conducted to reveal changes in the microstructure of membranes prepared with different solvents. The interaction of solvents with groups of polymer backbones was also analyzed for the explanation of the effect of solvents on the membrane performance for the separation of different gas pairs, such as CO2/CH4 mixture. The results showed that a membrane with optimal separation performance was obtained by optimizing the solvent composition, which exceeded the 2018 mixed-gas CO2/CH4 upper bound. The induced effect of solvents on the polymer membrane structure provides a new research path for the optimization of polymer membranes to enhance separation performance.
研究领域:
材料科学
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化学工程
·
气体分离技术
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产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2022
·
IF 5.876
Yanyong Sun,Minmin Gou
Based on the one-dimensional tubular structure of halloysite nanotubes (HNTs), plant polyphenols and polyamines were used for in situ polymerization on the surface of HNTs to form amino-rich polymers, which were then removed as templates to synthesize polymer nanotubes. These nanotubes were then incorporated into a Pebax matrix to prepare mixed-matrix membranes (MMMs) for CO 2 /CH 4 gas separation. The removal of the HNT template increased the lumen diameter of the filler and significantly improved its gas permeability . And the amino groups on the inner surface of the polymer nanotubes were exposed. Further, the number of CO 2 reaction sites increased, which improved the reaction selectivity of CO 2 . In addition, the presence of amine groups on the inner and outer surfaces of the polymer nanotubes provided various transfer channels for CO 2 , which were conducive for CO 2 gas transfer in the membrane. When the CC-PEINT content was 8 wt%, the CO 2 permeability was 710 Barrer and CO 2 /CH 4 selectivity was 60. The CO 2 permeability and CO 2 /CH 4 selectivity of the Pebax/CC-PEINTs membranes increased by 163% and 132%, respectively, compared with those of the pure Pebax membrane.
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
Carbon Capture Science & Technology
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2023
·
IF 0
Wufeng Wu,Jiang Fan,Dongyue Wang,Yali Zhao,Xinglei Zhao,Yanying Wei
MOF membranes exhibit impressive performance in gas separation due to their large surface area, controllable pore size and unique affinity. Here, the ultrathin UiO-66-NH 2 polycrystalline membranes with thickness of ∼320 nm are successfully prepared within 1 h using a combination of ultrasound-assisted and microwave synthesis strategies. During the reaction, high-density small MOF nuclei are produced by sodium formate ultrasound-assisted, which act as sufficient nucleation sites for heterogeneous nucleation during membrane growth, aiming for development of a continuous MOF membrane on the porous substrate. The obtained UiO-66-NH 2 membrane shows an ideal CO 2 /CH 4 selectivity of 40 due to the enhanced the interaction between CO 2 molecules and the membrane. Moreover, the narrowed pore structure further hinders the diffusion of larger-sized molecules owing to -NH 2 occupying the pore channels, resulting in elevated CO 2 /CH 4 selectivity. Compared to many other MOF membranes, the UiO-66-NH 2 polycrystalline membranes exhibit a well balance of gas permeance and CO 2 /CH 4 selectivity, which presents a new route for CO 2 capture.
研究领域:
材料科学
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化学工程
·
环境科学
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DOI
JOURNAL OF MEMBRANE SCIENCE
·
2017
·
IF 6.035
Ning Zhang,Dongdong Peng,Hong Wu,Yanxiong Ren,Leixin Yang,Xingyu Wu,Yingzhen Wu,Zihan Qu,Zhongyi Jiang,Xingzhong Cao
For high-performance hybrid membranes, it is crucial to design multi-functional filler to rationally manipulate the structure-property relationship. In this study, a novel kind of hybrid membrane was fabricated by incorporating zinc ion loaded sulfonated pitch (SP-Zn 2+ ) nanofillers into poly (ether-block-amide) (Pebax) matrix for CO 2 /CH 4 separation. Sulfonated pitch (SP) with high sulfonate content was functionalized by zinc ion (Zn 2+ ) via complexation reaction to synthesize SP-Zn 2+ nanofillers with high Zn 2+ loading. Mixed gas separation performances of membranes with different SP-Zn 2+ loading were conducted. Meanwhile, the effect of operating pressure on separation performance and long-term operation stability were investigated. The hybrid membranes displayed significantly enhanced permeability and CO 2 /CH 4 selectivity. First, the hydrophilic sulfonate group in SP had good compatibility with Pebax matrix and effectively suppressed interfacial defects. Second, zinc ions and sulfonate group could form zinc-sulfonate complex network. The sulfonated moiety afforded strong affinity toward CO 2 due to multiple interactions whereas the Zn 2+ moiety afforded a transport highway for CO 2 . Third, the incorporation of SP-Zn 2+ nanofillers could disturb the Pebax chain packing and optimize the free volume characteristics. Particularly, Pebax/SP-Zn 2+ (2) membrane exhibited an increment of 104% and 70.2% in CO 2 permeability and CO 2 /CH 4 selectivity respectively, much higher than that of Pebax 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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产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Xiaoli Ding,Yongfu Tang,Hongyong Zhao,Qingping Xin,Yuzhong Zhang
Hollow SAPO-34 with an average particle size of ca .370 nm was synthesized by selective etching its precursor under the controlled alkaline condition. Subsequently, freestanding mixed matrix membranes were synthesized by UV-induced in-situ polymerization of the mixture of hollow SAPO-34, the fluorinated monomer , and the trifunctional cross-linker. The structure and the physical characteristic of hollow SAPO-34 and membranes were characterized by scan electron microscope, wide-angle X-ray diffraction, etc. The effect of the hollow SAPO-34 loading amount on the gas permeation-separation performance of mixed matrix membranes was investigated. The results showed that hollowing out SAPO-34 improved the N 2 /CH 4 sorption selectivity and converted the crystals from preferential adsorption of N 2 to preferential adsorption of CH 4 , the incorporation of hollow SAPO-34 into membranes increased the N 2 /CH 4 solubility selectivity and the permeability. The optimal membrane exhibited a 39-fold increase in N 2 permeability from 6.9 × 10 −13 to 2.7 × 10 −11 cm 3 (STP)cm·cm −2 ·s −1 ·Pa −1 at 0.2 MPa and 35 °C without the loss of N 2 /CH 4 permselectivity, which exceeded the 2008 Robeson upper bound.
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
·
2022
·
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
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
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
✓ 已验证
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
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
危险品化学品经营许可证（带存储）