Journal of Environmental Chemical Engineering
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2020
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IF 4.3
Junwen Xu,Shujuan Ma,Ya Li,Xiaowei Li,Junjie Ou,Mingliang Ye
Polymers of intrinsic microporosity (PIMs) are a class of microporous polymers with rigid and contorted molecular structures. The special structures lead to incomplete space occupation, and the pores of PIMs originate from the formed void. In this work, we made attempts to expand the applications of PIMs to the aspect of heavy metal removal. First, PIM-1 was synthesized using tetrafluoroterephthalonitrile (TFTPN) and 5,5′,6,6′-tetrahydroxy-3,3,3′,3′-tetramethyl-1,1′-spirobisindane (TTSBI) as precursors. The primary PIM-1 was quite hydrophobic, and thus could not be evenly dispersed in water, resulting in low adsorption capacity for mercury ions (Hg 2+ ). A conversion of nitrile group in PIM-1 to thiol group was then carried out by two steps, namely carboxylation and introduction of thiol groups. The carboxylation made the polymers more active, and the final thiol-functionalization provided the polymers with hydrophilicity and affinity for Hg 2+ . The thiolethyl modified PIM-1 (assigned as PIM-G) and thiophenyl modified (assigned as PIM-B) possessed maximum Hg 2+ adsorption capacity of 136 mg g −1 and127 mg g −1 at pH 5, respectively. Besides, the thiol-functionalized PIMs had fluorescence property and showed potential in sensing for Hg 2+ .
研究领域:
材料科学
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环境科学
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DOI
高影响因子
INORGANIC CHEMISTRY
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2024
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IF 4.3
Jing-ran Yu,Pan-pan Zhang,Jia-yu Ding,Yue-bin Liu,Wei-hai Lin,Wei Shao,Jia-jia He,Qihan Gong,Ming Xue
The separation of high-octane dibranched alkanes from naphtha is critical in the refining of gasoline. To date, research on the membrane-based separation of alkane isomers has been limited, with a particular paucity of investigations into mixed-matrix membranes. Herein, the continuous and dense UiO-66/PIM-1 mixed-matrix membrane, which was prepared through precise control of the interfacial structure, was first applied to the differentiation of C6 alkane isomers. Due to the synergistic combination of UiO-66 with differential adsorption capabilities for alkanes and PIM-1 that possesses a cross-linkable structure, the resulting UiO-66/PIM-1-(20) membrane demonstrated remarkable separation performance and high stability. Pervaporation measurements showed that the mass fraction of 2,2-dimethylbutane in the feed side was increased from 50.0 to 75.8 wt % while an excellent flux of 1700 g m–2 h–1 was maintained over a continuous 40 h period. The UiO-66/PIM-1-(20) membrane, characterized by its facile replication and processing, shows potential for large-scale fabrication. This study offers a new approach to the membrane separation of alkane isomers.
研究领域:
化学工程
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材料科学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Zewen Xu,Pei Li,Hao Guo,Shengchao Zhao,Kuo Chen,Xinliang Liu,Ming Wang,Yingfei Hou
Excessive carbon emission leads to global warming, threatening human survival. Membrane-based carbon capture technology is an important component of carbon capture, utilization, and storage (CCUS) technology and one of the main upstream technologies for achieving carbon neutrality. PIM-1 materials exhibit high CO 2 permeability but lower CO 2 /N 2 selectivity, making it a significant focus to improve CO 2 /N 2 selectivity without sacrificing CO 2 permeability. In this work, Noria was introduced as a block through the bottom-up approach into the PIM-1 molecular chain, forming Noria-based porous organic polymer (NPOP) microregions with excellent CO 2 affinity. Additionally, the presence of NPOP increases the interchain gaps, resulting in a higher free volume. Consequently, the separation membrane prepared under optimal conditions broke the 2008 upper bound, with a 43.6 % increase in CO 2 permeability and a 41.7 % increase in CO 2 /N 2 selectivity. Furthermore, NPOP could form colloidal networks and provide rigidity to the separation membrane, endowing it with excellent aging resistance. After 6 months of aging, the CO 2 permeability of 0.5 %Noria decreased by only 33.4 % (67.4 % for pure PIM-1), indicating its strong potential for widespread applications.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Gas Science and Engineering
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2024
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IF 0
Xuebi Du,Dawei Shao,Yinhua Wan
Metal-organic frameworks (MOFs) have shown potential as nanofillers for the selective capture of specific gases in mixed matrix membranes (MMMs). This study introduces an efficient method, utilizing a mild (100 °C) reaction condition and a short reaction time (20 min), for the synthesis of MOF-808(Ce) nanocrystals. The MOF-808(Ce) that is obtained exhibits porous characteristics, a notable affinity for CO 2 , and robust intermolecular interactions with PIM-1. Furthermore, this study pioneers the incorporation of MOF-808(Ce) as a filler into PIM-1, with varying loadings, to create PIM/MOF-808 MMMs for the purpose of CO 2 separation. Consequently, the MMMs containing 2 wt% MOF-808(Ce) demonstrate high CO 2 permeability of 6854 Barrer and CO 2 /N 2 selectivity of 23.2, which is far surpasses 2008 upper bound from Robeson and approaches the refined 2019 upper bound from MeKenow. A comparative analysis demonstrates the efficacy of MOF-808(Ce) as a filler in PIM-1 for the purpose of CO 2 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
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jian Guan,Xiangzeng Wang,Jingcheng Du,Quansheng Liang,Wen He,Ying Liu,Ji Ma,Chunwei Zhang,Jiangtao Liu
Polymers of intrinsic microporosity (PIMs) are promising candidates for carbon dioxide (CO 2 ) separation and capture from flue gas or natural gas. PIM-1, which has excellent gas permeation properties over the Robeson upper bound (1991), has been widely functionalized to further enhance the CO 2 permeability or selectivity. In this work, a simple and readily processive surface modification method has been proposed via hydrolysis of the PIM-1 membrane. The two hydrolysis processes by the acid method, amidation and carboxylation processes, have been conducted to functionalize the surface of PIM-1 membranes forming N A -PIM-1 and C A -PIM-1 membranes. The TGA, FT-IR spectra and NMR results verify that the composition and structure inside the PIM-1 membrane remain unchanged. XPS and NMR spectra demonstrate that the nitrile group at the surface was successfully functionalized with an amine group or carboxyl group. The CO 2 permeability and CO 2 /N 2 selectivity of the N A -PIM-1 membrane both increased to 4593.2 Barrer and 28.5, respectively. Another advantage of N A -PIM-1 membranes is the coordination site from introduced nitrogen atoms with zinc ions to form N A -PIM-1-Zn, which could further react with PEI to introduce amine-rich groups on the surface of the PIM-1 membrane. The CO 2 /N 2 selectivity of the N A -PIM-1-Zn-PEI membrane coated with PEI on the surface increases 45.4% compared to the unmodified PIM-1 membranes, with CO 2 permeability decreasing only 15.5% compared to the unmodified PIM-1 membrane. The N A -PIM-1 and N A -PIM-1-Zn-PEI membranes both surpass the Robeson upper bound (2008) even under mixed gas feeding, suggesting that surface modification of PIM-1 is a promising approach for CO 2 capture from natural gas and flue gas.
研究领域:
材料科学
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环境工程
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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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2020
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IF 7.183
Jiaqi Li,Mengxiao Zhang,Weilin Feng,Liping Zhu,Lin Zhang
Herein, a novel thin film composite (TFC) membrane pore-filled with polymer of intrinsic microporosity, PIM-1, has been developed for organic solvent nanofiltration (OSN). The TFC membranes were facilely prepared by dip-coating of PIM-1/chloroform solution onto polyacrylonitrile support membranes followed by a solvent vapor annealing (SVA) process. The relationship between preparation conditions, selective layer morphologies and OSN performances of the prepared TFC membranes were studied systematically. It was found PIM-1 was evidently filled into the near surface pores of support membranes due to the infiltration of PIM-1 solution. With the elongation of SVA time, the thickness of the PIM-1 layer decreased and the PIM-1/PAN interface gradually disappeared, which is advantageous to enhance the interfacial bonding. The prepared TFC membranes were used to reject organic molecules in organic solvents and exhibited tunable solvent permeability and solute rejection. Especially, the membranes were suitable for the removal of neutral molecules and anionic dyes from ethanol. The typical membrane demonstrated an ethanol permeance of 4.3 L m −2 h −1 bar −1 with a rejection of 93.7% towards Methyl Orange (327 Da). By comparing the permeance of various solvents, it is found that the closer the Hansen solubility parameter of solvent is to that of PIM-1, the higher the solvent permeance. This indicates the affinity between solvent and membrane plays an important role in solvent permeability. This work offers a novel and convenient strategy to prepare highly permeable membranes with controllable microstructures and tunable permselectivity to meet the diverse demands of molecular separation in organic solvents.
研究领域:
材料科学
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分离工程
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Kaifang Wang,Danlin Chen,Jiali Tang,Zihao Hong,Zhongtai Zhu,Ziyi Yuan,Zhihong Lin,Yuqi Liu,Raphael Semiat,Xuezhong He
Membrane gas separation technologies have emerged as highly prospective avenues for the selective separation of CO 2 . In this research, a novel array of mixed-matrix membranes (MMMs) was engineered, integrating two-dimensional nanosheets of MXene, specifically Ti 3 C 2 T x , into polymers of intrinsic microporosity (PIMs) to selectively separate CO 2 from N 2 . The inclusion of Ti 3 C 2 T x nanosheets, rich in polar functional groups, significantly increases the affinity between CO 2 molecules and the fabricated MMMs. Additionally, the precise modulation of the molecular diffusion channels for CO 2 and N 2 is achievable due to the interlayer spacing between MXene layers (∼0.35 nm) within the PIM-1 matrix. This innovation is predicated on the synergistic effect of solution-diffusion and molecular sieving mechanisms that underpin the gas separation process, leading to a marked improvement in both selectivity for CO 2 over N 2 and the permeability of CO 2 . Among the series, the MMMs with a 0.5 wt% MXene display exceptional separation efficiency, achieving a CO 2 permeability of 12475.3 barrer and a CO 2 /N 2 selectivity of 32.7. Notably, all the PIM-1/MXene membranes prepared with different compositions in this study exceed the Robeson upper bound defined in 2019, indicating their substantial promise for CO 2 separation and capture in industrial applications.
研究领域:
材料科学
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环境工程
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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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2025
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IF 9
Shuangqi Song,Hong Li,Jingde Li,Yanqin Yang
Mixed-matrix membranes (MMMs), developed through the combination of solid fillers with polymer matrices, represent an effective approach addressing the persistent challenge of balancing permeability and selectivity in polymer membrane. Diethylenetriamine-functionalized porous material of PP-DETA, which is synthesized from porous organic polymer of PP via one-step diethylenetriamine grafting, is an ideal material for MMMs production. However, designing and optimizing PP-DETA for high-performance CO 2 separation membranes remains a challenge. Herein, we develop an improved PP-DETA material, designated as PP-DETA-cPIM-1, by covalently attaching a carboxylated polymer of intrinsic microporosity (cPIM-1) network layer onto the PP-DETA surface. Membranes prepared from this PP-DETA-cPIM-1 filler and PIM-1 matrix demonstrate enhanced interfacial adhesion and stronger mechanical properties in comparison to the counterparts with the same loading of PP-DETA. The incorporation of PP-DETA-cPIM-1 into MMMs establishes an enhanced filler/polymer interface that facilitates the selective transport of CO 2 through the filler, while simultaneously improving membrane stability and suppressing physical aging. Specifically, with 5 wt% loading of PP-DETA-cPIM-1 filler, the MMM is able to enhance the CO 2 /N 2 selectivity and CO 2 permeability by 52.3 % and 25.3 %, respectively, exceeding the upper bound established in 2008. Furthermore, PP-DETA-cPIM-1/PIM-1 MMMs display superior anti-aging ability for 180 days of aging.
研究领域:
材料科学
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环境科学
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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
Keming Zhang,Xianye Luo,Sihui Li,Xiaohe Tian,Qingnan Wang,Chenlu Liu,Yanting Tang,Xiaoting Feng,Rui Zhang,Shuangfeng Yin,Shaofei Wang
Developing high-performance H 2 /CH 4 separation membranes is of great potential for H 2 production in the petroleum industry. Incorporating nanofillers into a polymer matrix to form mixed matrix membranes (MMMs) can elevate selectivity and permeability, but poor polymer-filler interfacial compatibility and filler aggregation are formidable problems. Targeting this, we propose a novel approach by incorporating a metal–organic framework (MOF) gel, ZIF-8 gel, as the versatile filler to a high free volume polymer PIM-1 and investigate the H 2 /CH 4 separation capabilities of the MMMs. Benefiting from the gel network morphology of ZIF-8, they were dispersed evenly in the PIM-1 matrix. The interconnected gel network structure of ZIF-8 gel helped to construct continuous gas transport pathways in the polymer. As a result, the H 2 /CH 4 separation performance was notably improved, demonstrating a substantial increase in H 2 permeability by 78.9% (exceeding 6800 Barrer) and a 38.0% enhancement in H 2 /CH 4 selectivity at a ZIF-8 gel loading of 31.0 wt%. These improvements surpassed the upper bound established in 2008. The Maxwell and Lewis-Nielsen models were developed to clarify gas transport mechanisms across membranes, and the experimental data of ZIF-8 gel/PIM-1 was well-matched with the calculated results of the Lewis-Nielsen models. Adopting MOF gel as fillers may pave a new approach to design high-performance MMMs with interconnected transport pathways.
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
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2020
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IF 5.774
Lei Hou,Zhe Wang,Zhaoyu Chen,Wenbo Chen,Cancan Yang
PIM-1 and poly(arylene fluorene ether ketone) (Am-PAFEK) were synthesized by polycondensation . Their structures were characterized by 1 H NMR and FT-IR spectral analyses. A series of flexible and transparent blend membranes were prepared by solution blending with different ratios of PIM-1 and Am-PAFEK. DSC and SEM analyses showed good compatibility between them. PIM-1 and Am-PAFEK in the blend membrane perform their respective functions. The former provides excellent permeability; the latter provides high selectivity for CO 2 . Addition of 20% Am-PAFEK into the blend membrane increased the gas separation selectivity of CO 2 /CH 4 and CO 2 /N 2 by 75% and 65%, respectively. The optimum separation performance was achieved with blend membrane with a CO 2 permeability of 752.4 Barrer and a CO 2 /N 2 selectivity ratio of 26.7, extremely close to the Robeson upper bound (2008). After 140-days aging test, the blend membranes still maintained above 70% CO 2 permeability, indicating that it has good antiaging properties. Consequently, the new type of membranes have great potential in industrial applications.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Membranes
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2023
·Vol. 13
·期 9
·781
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IF 4.2
Jiaming Gao,Yongchao Sun,Feifei Kang,Fei Guo,Gaohong He,Hanli Wang,Zhendong Yang,Canghai Ma,Xiaobin Jiang,Wu Xiao
Mixed matrix membranes (MMMs) generally have some fatal defects, such as poor compatibility between the two phases leading to non-selective pores. In this work, PIM-1 was chosen as the polymer matrix, and UiO-66 modified with amidoxime (UiO-66-AO) was used as the filler to prepare the MMMs. In the MMMs, the amino and hydroxyl groups on UO-66-AO form a rich hydrogen bond network with the N and O atoms in the polymer PIM-1 chain to improve the compatibility between the polymer matrix and the filler. In addition, the selective adsorption of CO2by the amidoxime group can promote the transport of CO2in the membrane, which enhances the gas selectivity. The CO2permeability and CO2/N2selectivity of UiO-66-AO@PIM-1 MMMs are increased by 35.2% and 45.2% compared to pure PIM-1 membranes, reaching 7535.5 Barrer and 26.9, surpassing the Robeson Upper Bound (2008) and close to the 2019 Upper Bound. After 38 days of the aging experiment, the CO2permeability is approximately 74% of the original. The results show that the addition of UiO-66-AO has an obvious effect on improving the aging properties of the membrane. The UiO-66-AO@PIM-1 MMMs have a bright prospect for CO2separation in the future.Keywords:amidoxime;UiO-66-AO;mixed matrix membrane;PIM-1;CO2/N2separation
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
PubMed
高影响因子
MACROMOLECULAR RAPID COMMUNICATIONS
·
2022
·Vol. 44
·期 6
·2200826
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IF 5.006
Jiaqi Li,Weilin Feng,Mengxiao Zhang,Xiaohe Wang,Chuanjie Fang,Jianyu Wang,Lin Zhang,Liping Zhu
Polymers of intrinsic microporosity (PIMs) are a class of microporous organic materials that contain interconnected pores of less than 2 nm in diameter. Such materials are of great potential used in membranes for molecular separation, such as drug fractionation in pharmaceutical industry. However, the PIMs membranes are often susceptible to low separation selectivity toward different molecules due to their wide pore size distribution. Herein, a linear polyimide, Matrimid, is incorporated with PIM-1 (a typical member of PIMs) by solution blending, and the blends are dip-coated onto a polyimide P84 support membrane to prepare thin-film composite (TFC) membranes to control pore size distribution while keep high microporosity. The component miscibility, pore characteristics, and molecular separation performances of the Matrimid/PIM-1 TFC membranes are investigated in detail. The Matrimid and PIM-1 are partially miscible due to their similar Hansen solubility parameters. The Matrimid endows the selective layers (coatings) with narrower pore size distribution due to more compact chain packing. The prepared Matrimid/PIM-1 TFC membranes show high selectivity for separation of riboflavin (80% of retention) and isatin (only 5% of retention). The developed membranes exhibit great potential for separating molecules with different molecular weights.
研究领域:
材料科学
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化学工程
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生物医学工程
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DOI
高影响因子
危险品化学品经营许可证（带存储）