CHEMISTRY-A EUROPEAN JOURNAL
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2020
·Vol. 26
·期 35
·7918-7922
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IF 4.857
Yichen Zhou,Mingmin Jia,Xiongfei Zhang,Jianfeng Yao
Graphical Filling the voids : Etched ZIF-8 (ZIF-8-E) crystals permeated by open through pores of size about 100 nm have been introduced into a polyethersulfone membrane matrix. The resulting material shows enhanced CO 2 /N 2 separation performance (see scheme). Zeolite ZIF-8 has been etched with acid to form microporous ZIF-8-E crystals. These were then introduced into a polyethersulfone (PES) membrane matrix to enhance its CO 2 /N 2 separation performance. Open through pores of size about 100 nm formed in the ZIF-8 crystals allow the ingrowth of polyethersulfone chains, ensuring a reduction in the number of nonselective voids, thereby achieving better interaction between ZIF-8-E and PES. As a result, the CO 2 /N 2 separation performance of the ZIF-8-E/PES membrane increased significantly, showing a CO 2 permeability of 15.7 Barrer and a CO 2 /N 2 ideal selectivity of 6.5.
研究领域:
材料科学
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环境工程
✓ 已验证
DOI
高影响因子
Membranes
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2021
·Vol. 11
·期 9
·693
·
IF 4.106
Fei Guo,Bingzhang Li,Rui Ding,Dongsheng Li,Xiaobin Jiang,Gaohong He,Wu Xiao
Mixing a polymer matrix and nanofiller to prepare a mixed matrix membrane (MMM) is an effective method for enhancing gas separation performance. In this work, a unique UiO-66-decorated halloysite nanotubes composite material (UiO-66@HNT) was successfully synthesized via a solvothermal method and dispersed into the Pebax-1657 matrix to prepare MMMs for CO2/N2separation. A remarkable characteristic of this MMM was that the HNT lumen provided the highway for CO2diffusion due to the unique affinity of UiO-66 for CO2. Simultaneously, the close connection of the UiO-66 layer on the external surface of HNTs created relatively continuous pathways for gas permeation. A suite of microscopy, diffraction, and thermal techniques was used to characterize the morphology and structure of UiO-66@HNT and the membranes. As expected, the embedding UiO-66@HNT composite materials significantly improved the separation performances of the membranes. Impressively, the as-obtained membrane acquired a high CO2permeability of 119.08 Barrer and CO2/N2selectivity of 76.26. Additionally, the presence of UiO-66@HNT conferred good long-term stability and excellent interfacial compatibility on the MMMs. The results demonstrated that the composite filler with fast transport pathways designed in this study was an effective strategy to enhance gas separation performance of MMMs, verifying its application potential in the gas purification industry.Keywords:composite material;UiO-66;HNT;mixed matrix membrane;CO2/N2separation
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Membranes
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2022
·Vol. 12
·期 8
·786
·
IF 4.562
Xingqian Wang,Yuping Zhang,Xinwei Chen,Yifei Wang,Mingliang He,Yongjiang Shan,Yuqin Li,Fei Zhang,Xiangshu Chen,Hidetoshi Kita
Fillers play a critical role in the performance of mixed matrix membranes (MMMs). Microporous metal azolate frameworks (MAFs) are a subclass material of metal–organic frameworks (MOFs). Due to the uncoordinated nitrogen of the organic ligands, MAF-7 (SOD-[Zn(mtz)2], Hmtz = 3-methyl-1,2,4-triazole, window: d = 0.34 nm) shows excellent CO2adsorption performance. In this work, Pebax 1657/MAF-7 MMMs were prepared by a sample solution casting method with MAF-7 particles as fillers for the first time. By means of X-ray diffraction (XRD), scanning electron microscope (SEM), infrared radiation (IR), and thermogravimetry (TG), the compositional and structural properties of the mixed matrix membrane with different filler content were analyzed. The results show that the compatibility of MAF-7 and Pebax is good with a filler content of 5 wt.%. The pure gas testing showed that mixed matrix membrane has a high ideal CO2/N2selectivity of 124.84 together with a better CO2permeability of 76.15 Barrer with the optimized filler content of 5 wt.%. The obtained membrane showed 323.04% enhancement in selectivity of CO2/N2and 27.74% increase in the permeability of CO2compared to the pristine membrane at 25 °C and 3 bar. The excellent separation performance may be due to the ligands that can afford a Lewis base active site for CO2binding with the uniform dispersion of MAF-7 particles in Pebax and the favorable interface compatibility. The obtained membrane overcomes the Robeson’s upper bound in 2008 for CO2/N2separation. This work provides a new strategy by utilizing MAFs as fillers with triazole ligand to enhance the gas separation performance of mixed matrix membranes.
研究领域:
材料科学
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气体分离
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膜技术
✓ 已验证
DOI
高影响因子
FUEL
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2023
·
IF 7.4
Hongxia Fang,Chuncai Zhou,Shihai Xu,Jiaqian Shi,Yunhu Hu,Guijian Liu,Lei Wu
Metal-organic frameworks (MOFs) are considered one of the promising adsorbents for CH 4 /N 2 separation. However, MOFs commercialization is a big challenge since their synthetic materials are expensive and not environmentally friendly. Herein, the dealumination solution obtained from coal fly ash (CFA) using sulfuric acid as an extracting agent through direct leaching and roasting technologies was applied as metal feedstock to prepare CFAx-FumMOF-y and compared to aluminum fumarate MOF (Al-FumMOF) in morphology, surface area, micropore volume, and CH 4 /N 2 selective separation. The results indicated that CFAx-FumMOF-y exhibited closely similar surface area (1164.94–1073.08 m 2 /g) and micropore volume (0.40–0.36 cm 3 /g) to Al-FumMOF (1287.55 m 2 /g, 0.42 cm 3 /g), even there were no detectable differences in CH 4 uptakes (CFAx-FumMOF-y, 21.93–20.69 cm 3 /g; Al-FumMOF, 22.13 cm 3 /g) at 298 K and 1.0 bar, suggesting that the impurity metal species in dealumination solution hardly affect textural properties and gas uptakes. Moreover, the isosteric heat of adsorption (Q st ) and IAST CH 4 /N 2 selectivity of CFAs-FumMOF-1 (19.25–17.84 kJ/mol) and CFAb-FumMOF-1 (18.83–18.64 kJ/mol) were slightly superior to Al-FumMOF (17.83.64–16.86 kJ/mol, 4.87), suggesting that CFAx-FumMOF-1 played an identical role as Al-FumMOF in gases separation. The cyclic regeneration experiments and binary breakthrough tests further confirmed that CFAx-FumMOF-y was feasible for practical application. This study provides a new perspective for reducing the production cost of MOFs as well as realizing high-value utilization of CFA.
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Zhiwei Zhao,Yating Wang,Yuhao Tang,Xiaoqing Wang,Feifei Zhang,Jiangfeng Yang
Unconventional natural gas has become an important supplement to conventional energy sources, and the process of enrichment and purification of methane from low concentration coalbed methane is crucial. To this end, we report a copper-based metal–organic framework (MOF), ZJNU-119Cu, featuring two methane traps constructed with uncoordinated carboxylic acid oxygens and open metal sites. ZJNU-119Cu exhibits a high methane adsorption capacity (58.2 cm 3 ·g –1 ) at 298 K and 0.1 MPa and excellent CH 4 /N 2 separation performance under dynamic conditions. Density-functional theory calculations combined with grand canonical Monte Carlo simulation theory reveal the interaction mechanism for the uncoordinated carboxylic acid oxygen atoms and open metal sites in ZJNU-119Cu with CH 4 . The gas adsorption isotherms, heat of adsorption calculations, and breakthrough separation experiments indicate that this MOF is a very promising adsorbent for CH 4 /N 2 separation.
研究领域:
材料科学
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能源化学
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理论计算
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2018
·
IF 6.578
Xiong-Fei Zhang,Yi Feng,Zhongguo Wang,Mingmin Jia,Jianfeng Yao
Incorporating metal-organic frameworks into cellulose matrix to prepare composite membranes is promising in gas-separation applications. In this study, UiO-66-NH 2 (Zr-based MOF) nanoparticles are wrapped into the densely packed cellulose nanofibrils (CNF-COOH) via a facile vacuum filtration process. The existence of acid-base interactions and electrostatic forces between UiO-66-NH 2 and CNF-COOH renders ideal interfacial morphology. Results show that UiO-66-NH 2 is cross-linked by -COOH groups and well-dispersed in the CNF matrix. The porous UiO-66-NH 2 strengthens the diffusion process of CO 2 molecules, thus elevating the permeation flux and separation factor simultaneously. The optimum separation performance is achieved over CM-1 membrane with a CO 2 permeability of 139 Barrer and a CO 2 /N 2 selectivity ratio of 46.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Membranes
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2023
·Vol. 13
·期 9
·781
·
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
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2018
·
IF 3.927
Shumin Wang,Qingping Guo,Shujun Liang,Peng Li,Jujie Luo
A series of mixed matrix membranes (MMMs) were fabricated with Ni-MOF-74 as filler and poly (styrene-b-butadiene-b-styrene) (SBS) polymer as matrix materials for CH 4 /N 2 separation. MMMs were characterized by Fourier transform infrared (FTIR) spectra, X-ray diffraction (XRD), scanning electron microscopy (SEM), and thermogravimetric analysis (TGA). Gas separation behavior was investigated by measuring single and mixed gases. For the single gas, the CH 4 permeability of the MMMs incorporated with 15 wt% Ni-MOF-74 (Ni-MOF-74/SBS-15) reached 83.5 Barrer, which was 116% higher than that of SBS (38.6 Barrer), while its ideal selectivity remained the same. CH 4 permeability can further increase to 176.6 Barrer with the increase in temperature to 55 °C. For the CH 4 /N 2 (50/50 vol%) mixed gas, the Ni-MOF-74/SBS-15 sample exhibited increasing CH 4 permeability (74.7 vs 36.7 Barrer), while selectivity remained unchanged relative to that of the pure SBS membrane.
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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2025
·
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
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Kunpeng Liu,Yixuan Yu,Qi Wang,Lingtong Kong,Tianjun Sun
A comprehensive investigation was conducted to explore the adsorption behaviors of CH 4 over N 2 on ultra-microporous Al/Zr-FDCA frameworks, which were synthesized specifically using the eco-friendly and bio-sourced 2,5-furandicarboxylic acid (FDCA). Characterization results revealed that both Al-FDCA and Zr-FDCA exhibited similar specific surface area and surface groups, leading to comparable methane uptake per-unit mass at atmospheric pressure. However, the presence of Zr nodes generated ultra-micropores around 0.43 nm in size, leading to a pronounced affinity for CH 4 . Zr-FDCA demonstrated a higher CH 4 /N 2 selectivity (8.90) calculated from the isotherms compared to Al-FDCA (3.86). Furthermore, breakthrough experiments indicated that under the same dynamic conditions, Zr-FDCA exhibited 1.5 times higher CH 4 uptake per unit volume and 2.5 times higher CH 4 /N 2 selectivity when compared to Al-FDCA. Initially, a four-step VPSA process was simulated to investigate the separation of CH 4 /N 2 mixture, in which the effects of feed-gas flow rate, adsorption time, adsorption pressure, and desorption pressure in VPSA cycle were extensively evaluated to enhance the purity and recovery of methane. Subsequently, a six-step process was employed for further optimization, achieving a purity of 95.9 % and a recovery of 99.1 %. The obtained results demonstrated the reliability of the established model and highlighted the significant potential of Zr-FDCA for CH 4 /N 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
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2023
·
IF 9.5
Zhihong Lin,Ziyi Yuan,Kaifang Wang,Xuezhong He
Novel mixed matrix membranes (MMMs) with superior CO 2 /N 2 separation properties are of great importance for post-combustion CO 2 capture from flue gas . Metal-organic frameworks (MOFs) as one of the most attractive porous fillers for MMMs fabrication, are considered to provide a solid molecular sieving mechanism for enhancing CO 2 /N 2 selectivity. However, it causes the reduction in gas permeability and limits its further industrialization. Herein, we proposed a new strategy for filler functionalization by doping silver ions (Ag + ) into UiO-66-NH 2 nanoparticles through the double-solvent method and used for the preparation of advanced MMMs. The double-solvent method is benefits for the enrichment of Ag + in the hydrophilic pores of UiO-66-NH 2 . As a result, the prepared novel MMMs called Ag + @UiO@PIM-1 with the polymers of intrinsic microporosity (PIMs) as polymer matrix , show outstanding CO 2 permeability. According to the mixed gases (CO 2 /N 2 = 10:90) permeation experiments under 25 °C and 2 bar, the membrane with 30%Ag + @10%UiO loading achieves more than 65% increase in CO 2 /N 2 selectivity (∼30) and 120% in CO 2 permeability (>15,000 Barrer) compared to the pristine PIM-1 membrane. By optimizing the Ag + doping amount and Ag + @UiO loading content, the separation performance exceeds the 2019 CO 2 /N 2 upper bound. To figure out the separation mechanism, the pore texture properties and CO 2 affinity of the functional filler (Ag + @UiO) together with the membrane structure were characterized by XPS , PXRD , SEM, gas sorption , etc. The synergistic mechanisms by combing CO 2 facilitated transport and molecular sieving from pore regulation were identified to enable advanced CO 2 /N 2 membrane separation .
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2015
·
IF 2.587
Song Zhao,Xiaochang Cao,Zijian Ma,Zhi Wang,Zhihua Qiao,Jixiao Wang,Shichang Wang
In this work, imidazolate framework ZIF-8 nanoparticles were synthesized and incorporated into a poly(vinylamine) (PVAm) coating solution. The chemical structure of a PVAm/ZIF-8 film was characterized by X-ray diffraction and attenuated total reflectance Fourier transform infrared spectroscopy techniques. Mixed-matrix membranes (MMMs) were developed by coating the PVAm/ZIF-8 mixed dispersion on a polysulfone (PSf) support membrane. Surface and cross-sectional scanning electron microscopy images of the MMMs were employed to observe the dispersion of nanoparticles in the polymer matrix. The CO2 permeance and CO2/N2 selectivity of the MMMs were evaluated by using a CO2/N2 mixture gas. Optimal preparation parameters for the MMMs were achieved by varying the incorporated ZIF-8 contents in the coating solution and the wet coating thickness. The effect of incorporated ZIF-8 on improving the gas permselectivity was revealed, and the mechanism of CO2-facilitated transport in the PVAm/ZIF-8/PSf membrane was analyzed. The CO2/N2 separation performance of PVAm/ZIF-8/PSf membranes with different wet coating thicknesses was also evaluated at 22–60 °C to analyze the changes of the gas permselectivity with increasing temperature.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）