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1.
Mixed matrix membranes (MMMs) made from inorganic fillers and polymers is a kind of promising candidate for gas separation. In this work, two‐dimensional MXene nanosheets were synthesized and incorporated into a polyether‐polyamide block copolymer (Pebax) matrix to fabricate MMM for CO2 capture. The physicochemical properties of MXene nanosheets and MXene/Pebax membranes were studied systematically. The introduction of MXene nanosheets provided additional molecular transport channels and meanwhile enhanced the CO2 adsorption capacity, thereby enhancing both the CO2 peremance and CO2/N2 selectivity of Pebax membrane. The optimized MXene/Pebax membrane with a MXene loading of 0.15 wt % displayed a high separation performance with a CO2 permeance of 21.6 GPU and a CO2/N2 selectivity of 72.5, showing potential application in CO2 capture.  相似文献   

2.
In this paper, poly(amide-6-b-ethylene oxide) (Pebax1657)/SAPO-34 mixed matrix membranes (MMMs) were prepared by solvent-evaporation method with acetic acid as a novel solvent. CO2, N2, CH4 and H2 permeation properties were investigated, and the physical properties of Pebax/SAPO-34 MMMs were characterized by XRD and SEM. At low SAPO-34 content, it was homogeneously distributed in the Pebax matrix, and then precipitated and agglomerated at high SAPO-34 content. The crystallinity of Pebax phase in Pebax/SAPO-34 MMMs decreased initially and then rebounded as a result of phase separation. With the increase of transmembrane pressure difference, CO2 permeability was enhanced due to the effect of pressure-induced plasticization. Owing to the happening of stratification, the CO2 permeability of Pebax/SAPO-34 MMMs (50 wt% SAPO-34) increased to 338 Barrer from 111 Barrer of pristine Pebax, while the selectivities of CO2/CH4 and CO2/N2 were almost unchanged. Compared with the pristine Pebax, the gas separation performances of Pebax/SAPO-34 MMMs were remarkably enhanced.  相似文献   

3.
Mixed matrix membranes (MMMs) containing graphene-based fillers have attracted considerable attention in the field of gas separation. In this study, two types of graphene derivatives (Graphene (G) and Graphene Oxide (GO)) were embedded into the poly-ether-block-amide (Pebax) based MMM to investigate and compare CO2/N2 separation at various filler loadings (0.3–1 wt%). The morphologies of the prepared neat Pebax and MMMs were characterized by SEM, XRD, FTIR and DSC. Compared with the neat Pebax, the permeability of all gases was increased by adding filler content in the MMMs due to the crystallinity decrement of the polyamide (PA) segment. The best separation performance of the Pebax/G MMMs occurred at 0.7 wt%, where the CO2 permeability increased from 26.51 to 44.78 Barrer (~1.7 times). Also, for the Pebax/GO MMMs, the CO2 permeability was increased up to 58.96 Barrer (~2.2 times) by adding 0.5 wt% filler. This further gas permeation increment for the Pebax/GO sample was attributed to the higher affinity of GO nanosheets to CO2 sorption, which can facilitate CO2 gas transition through the membrane matrix. Moreover, the CO2/N2 ideal selectivity increased from 74.26 for the neat Pebax to 111.95 (~1.5 times) and 120.72 (~1.62 times) by adding 0.7 wt% G (Pebax/G-0.7) and 1 wt% GO (Pebax/GO-1) into Pebax, respectively. As a consequence, graphene derivatives can be recognized as a promising developer of permselectivity (permeability and selectivity) of the MMMs.  相似文献   

4.
Graphene oxide nanoparticles (GO) were firstly functionalized using p-phenylenediamine and then utilized as nanofillers to prepare poly(ether-block-amide) (Pebax®-1657)/poly(vinyl alcohol) (PVA-60000)-based mixed-matrix membranes. The modified GO as well as the fabricated mixed matrix membranes underwent some characterization analyses, including FTIR, TGA, XRD, FESEM, and EDX. The influence of amine-modified nanoparticles content (2, 4, and 6 wt%), and feed pressure on CO2, CH4, and N2 permeabilitis and ideal CO2/CH4 and CO2/N2 selectivities values of the MMMs were investigated. The permeation experiments demonstrated that Pebax/PVA (10 and 15 wt%) blend membranes caused an increase in CO2 permeability owing to the high affinity of polar CO2 molecules to polar PVA segments. Moreover, the incorporation of 6 wt% amine-functionalized GO into the Pebax/PVA (10 wt%) and Pebax/PVA (15 wt%) blend polymer raised the CO2 permeability and CO2/CH4 and CO2/N2 selectivity by nearly 43%, 28%, and 37%, respectively, due to the higher CO2 adsorption capacity of the amine-functionalized GO.  相似文献   

5.
Mixed-matrix membranes (MMMs) with combination of two distinct dimensional nanofillers (such as 1D-3D, 2D-3D, or 3D-3D, etc.) have drawn special attention for gas separation applications due to their concerted effects on gas permeation and mechanical properties. An amine-functionalized 1D multiwalled carbon nanotube (NH2-MWCNT) with exceptional mechanical strength and rapid gas transport was crosslinked with an amine-functionalized 3D metal-organic framework (UiO-66-NH2) with high CO2 affinity in a Schiff base reaction. The resultant crosslinked mixed-dimensional nanostructure was used as a nanofiller in a polysulfone (PSf) polymer matrix to explore the underlying synergy between 1D and 3D nanostructures on the gas separation performance of MMMs. Cross-sectional scanning electron microscopy and mapping revealed the homogenous dispersion of UiO-66@MWCNT in the polymer matrix. The MMM containing 5.0 wt. % UiO-66@MWCNT demonstrated a superior permeability 8.3 Barrer as compared to the 4.2 Barrer of pure PSf membrane for CO2. Moreover, the selectivity (CO2/CH4) of this MMM was enhanced to 39.5 from the 28.0 observed for pure PSf under similar conditions of pressure and temperature.  相似文献   

6.
《先进技术聚合物》2018,29(4):1334-1343
The aminated graphene oxide (GO) was prepared by the functionalization of pristine GO with ethylenediamine and then dispersed into the poly(amic acid) (the precursor of polyimide [PI]) solution followed by the chemical imidization to successfully fabricate the PI/amine‐functionalized GO mixed matrix membranes (MMMs) using in‐situ polymerization method. Chemical structure and morphology of the GO before and after amine modification were characterized by scanning electron microscopy, Raman spectrum, Fourier transform infrared, and X‐ray photoelectron spectroscopy. Scanning electron microscopy indicated that fine dispersion of GO throughout PI matrix was achieved, which indicates that the in‐situ polymerization approach can enhance the interfacial interaction between the GO and the PI matrix, and then improve the dispersion of carbon material in the polymer matrix. Compared with the conventional solution mixture method, the MMMs prepared with in‐situ polymerization method showed excellent CO2 permeability and CO2/N2 selectivity. The MMMs doped with 3 wt.% aminated GO exhibited maximum gas separation performance with a CO2 permeability of 12.34 Barrer and a CO2/N2 selectivity of 38.56. These results suggest that the amino groups on GO have strong interaction with the CO2 molecules, which can significantly increase the solubility of polar gas. Our results provide an easy and efficient way to prepare MMMs with good mechanical behavior and excellent gas separation performance.  相似文献   

7.
Mixed‐matrix membranes (MMMs) comprising Matrimid and a microporous azine‐linked covalent organic frameworks (ACOF‐1) were prepared and tested in the separation of CO2 from an equimolar CO2/CH4 mixture. The COF‐based MMMs show a more than doubling of the CO2 permeability upon 16 wt % ACOF‐1 loading together with a slight increase in selectivity compared to the bare polymer. These results show the potential of COFs in the preparation of MMMs.  相似文献   

8.
In this work, the films of poly(ether-block-amide) (Pebax 1657) and hydrophilic/hydrophobic silica nanoparticles (0–10 wt%) were coated on a poly(vinyl chloride) (PVC) ultrafiltration membrane to form new mixed matrix composite membranes (MMCMs) for CO2/N2 separation. The membranes were characterized by SEM, FTIR, DSC and XRD. Successful formation of a non-porous defect-free dense top layer with ~4 μm of thickness and also uniform dispersion of silica nanoparticles up to 8 wt% loading in Pebax matrix were confirmed by SEM images. The gas permeation results showed an increase in the permeance of all gases and an increase in ideal CO2/N2 selectivity with the increase in silica nanoparticle contents. Comparison between the incorporation of hydrophilic and hydrophobic silica nanoparticle into Pebax matrix revealed that the great enhancement of CO2 solubility is the key factor for the performance improvement of Pebax + silica nanoparticle membranes. The best separation performance of the hydrophilic silica nanoparticle-incorporated Pebax/PVC membrane for pure gases (at 1 bar and 25 °C) was obtained with a CO2 permeability of 124 barrer and an ideal CO2/N2 selectivity of 76, i.e., 63 and 35% higher than those of neat Pebax membrane, respectively. The corresponding values for hydrophobic silica nanoparticle-incorporated Pebax/PVC membrane were 107 barrer for CO2 permeability and 61 for ideal CO2/N2 selectivity. Also the performances of MMCMs improved upon pressure increase (1–10 bar) owing to the shift in plasticizing effect of CO2 towards the higher pressures. In addition, an increase in permeabilities with a decrease in ideal selectivity was observed upon temperature increase (25–50 °C) due to the intensification of chain mobility.  相似文献   

9.
Poly (ether-b-amide) (PEBA) mixed matrix membranes (MMMs) filled by different amounts of nano ZnO (up to 1 wt %) were synthesized and their gas separation performance was evaluated for CO2, CH4 and N2 pure gas and their binary mixtures. The ZnO-filled PEBA MMMs were characterized using ATR-FTIR, FESEM, AFM, TGA, DMTA, XRD and Mechanical tensile strength analyses. Generally, it was revealed that 0.5 wt % loading of ZnO into the polymer matrix caused a ZnO−PEO interaction; while ZnO–ZnO self-association hindered the interaction for the MMMs with other loadings of ZnO. As a result, PEBA-ZnO 0.5 wt % MMM possessed a higher glass transition temperature (Tg). Therefore, the CO2 permeability through PEBA-ZnO 0.5 wt % enhanced 27% than simple PEBA membrane. Moreover, all the fabricated MMMs were simulated by molecular simulation. Grand Canonical Monte Carlo (GCMC) and Molecular Dynamics (MD) methods were also applied to simulate the structural and gas transport properties of the membranes. The RDF, XRD, Tg, FFV and density analysis were compared with experimental results. Also, a binary mixture of CO2:CH4 (10:90) was used to determine CO2 permeability and CO2/CH4 selectivity, which were considerably reduced compared to single gas experiments. Moreover, the solubility of the binary gas mixture, the energy distribution and density distribution of both gases within the simulated cell were calculated by molecular simulation.  相似文献   

10.
In this study a thin film composite (TFC) membrane with a Pebax/Task-specific ionic liquid (TSIL) blend selective layer was prepared. Defect-free Pebax/TSIL layers were coated successfully on a polysulfone ultrafiltration porous support with a polydimethylsiloxane (PDMS) gutter layer. Different parameters in the membrane preparation (e.g. concentration, coating time) were investigated and optimized. The morphology of the membranes was studied by scanning electron microscopy (SEM), while the thermal properties and chemical structures of the membrane materials were investigated by thermo-gravimetric analyzer (TGA), differential scanning calorimetry (DSC) and Fourier transform infrared spectroscopy (FTIR). The CO2 separation performance of the membrane was evaluated using a mixed gas permeation test. Experimental results show that the incorporation of TSIL into the Pebax matrix can significantly increase both CO2 permeance and CO2/N2 selectivity. With the presence of water vapor, the membrane exhibits the best CO2/N2 selectivity at a relative humidity of around 75%, where a CO2 permeance of around 500 GPU and a CO2/N2 selectivity of 46 were documented. A further increase in the relative humidity resulted in higher CO2 permeance but decreased CO2/N2 selectivity. Experiments also show that CO2 permeance decreases with a CO2 partial pressure increase, which is considered a characteristic in facilitated transport membranes.  相似文献   

11.
Mixed matrix membranes (MMMs) have received worldwide attention for natural gas purification due to their superior performance in terms of permeability and selectivity. The zeolitic imidazole framework-8 (ZIF-8) blended polysulfone (PSf) membranes have been fabricated for natural gas purification. ZIF-8 was selected due to its low cost, remarkable thermal and chemical stabilities, and tunable microporous structure. The neat PSf hollow fiber membrane and mixed matrix hollow fiber membranes incorporated with the various ZIF-8 loadings up to 1.25% were fabricated. The prepared membranes were evaluated using field emission scanning electron microscopy (FESEM), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), Fourier transform infrared spectroscopy (FTIR), atomic force microscopy (AFM), and gas separation performance. The low loading of ZIF-8 nanoparticles to the MMM improved thermal stability and glass transition temperature and yielded low surface roughness. MMMs were tested using pure gases with a significant improvement of 36% in CO2 permeability and 28% in CO2/CH4 selectivity compared to the neat membrane. However, the high ZIF-8 loading reduced the separation performances. Moreover, CO2/CH4 selectivity decreased at elevated pressure (8 and 10 bar) due to CO2-induced plasticization. Previously, the incorporation of ZIF-8 particles has primarily been subjected to the fabrication of flat sheet membranes, whereas this work focused on hollow fiber membranes which are rarely investigated. Hence, the promising results obtained at low feed pressure in this study demonstrated the potential of ZIF-8 based hollow fiber membrane for natural gas purification.  相似文献   

12.
Three phase Pebax~? MH 1657/PEG-ran-PPG/CuBTC(polymer/liquid/solid) was successfully deposited as a selective layer on a porous Polysulfone(PSF) support. In fact, the beneficial properties of PEG(high selectivity) with those of PPG(high permeability, amorphous) have been combined with superior properties of mixed matrix membrane(MMMs). The membranes were characterized by DSC, TGA and SEM, while CuBTC was characterized by CO_2 and CH_4adsorption test. Statistically based experimental design(central composite design, CCD) was applied to analyze and optimize the effect of PEG-ran-PPG(10–50 wt%) and CuBTC(0–20 wt%) mass contents on the CO_2 permeance and CO_2/CH_4 ideal selectivity. Based on the regression coefficients of the obtained models, the CO_2 permeance was notably influenced by PEG-ran-PPG,while CuBTC has the most significant effect on the CO_2/CH_4 ideal selectivity. Under the optimum conditions(PEG-ran-PPG: 32.76 wt% and CuBTC: 20 wt%), nearly 620% increase in the CO_2 permeance and43% enhancement in the CO_2/CH_4 ideal selectivity was observed compared to the neat Pebax. The effect of pressure(3, 9 and 15 bar) on the pure and mixed gas separation performance of the composite membranes was also investigated. The high solubility of CO_2 in the membranes resulted in the enhancement of CO_2 permeability with increase in gas pressure.  相似文献   

13.
In this paper, poly(amide-6-b-ethylene oxide) (Pebax1657)/SAPO-34 mixed matrix membranes (MMMs) were prepared by solvent-evaporation method with acetic acid as a novel solvent. CO2, N2, CH4 and H2 permeation properties were investigated, and the physical properties of Pebax/SAPO-34 MMMs were characterized by XRD and SEM. At low SAPO-34 content, it was homogeneously distributed in the Pebax ma- trix, and then precipitated and agglomerated at high SAPO-34 content. The crystallinity of Pebax phase in Pebax/SAPO-34 MMMs decreased initially and then rebounded as a result of phase separation. With the increase of transmembrane pressure difference, CO2 permeability was en- hanced due to the effect of pressure-induced plasticization. Owing to the happening of stratification, the CO2 permeability of Pebax/SAPO-34 MMMs (50 wt% SAPO-34) increased to 338 Barrer from 111 Barrer of pristine Pebax, while the selectivities of CO2/CH4 and CO2/N2 were almost unchanged. Compared with the pristine Pebax, the gas separation performances of Pebax/SAPO-34 MMMs were remarkably enhanced.  相似文献   

14.
A novel composite membrane consisting of an interconnected MOF scaffold coated with cross‐linked poly(ethylene glycol) (PEG) has been developed. As a result of its unique structure, the membrane shows an exceptional 18‐fold permeability enhancement as compared to pristine PEG membranes, without compromising the selectivity. This performance is unattainable with current mixed‐matrix membranes (MMMs). Our optimized membrane has a permeability of 2700 Barrer with a CO2/N2 selectivity of 35, which surpasses the latest Robeson upper bound.  相似文献   

15.
《Arabian Journal of Chemistry》2020,13(12):8979-8994
Mixed matrix membranes (MMMs) fabricated with porous metal organic frame works have enhanced the separation performance of polymer membranes. In this context microporous 3D Tb(BTC)(H2O).(DMF)1.1 MOF was incorporated into pristine Matrimid® with loadings of 10, 20 and 30 weight percentages. SEM micrographs indicated proper distribution of filler in the Matrimid and no interfacial voids were observed. Gas permeation studies evidenced the CO2 permeability to be 13.2 (82.32%) and 18.34 (153.31%) and 25.86 Barrer for 10, 20 and 30 wt% MMMs respectively. The 257.18% increase in CO2 permeability of 30 wt% MMM than methane was attributed to polar nature of CO2, its smaller kinetic diameter, condensability, and larger solubility within the Matrimid matrix than non – polar and larger CH4 molecules.Addition of filler influenced the pure gas selectivity of all MMMs positively. So, 30 wt% MMM exhibited the highest 58.04% increase in selectivity that was attributed to the molecular sieving property of the filler and the size exclusion phenomena as followed by CH4 and CO2. The high values of mixed and pure gas selectivity were obtained upon increasing filler concentration. The commercial applicability of these MMMs was tested by checking their selectivity under increased feed concentrations of CO2 and checking permeability and selectivities at high temperatures. The study depicted that, competitive sorption of gases, prevalence of size exclusion phenomena and polymer chains relaxation at higher temperature were responsible for low gas selectivity. MMM with 30 wt% of MOF lied close to Robson’s Upper bound 2008 that indicated its good separation potential.  相似文献   

16.
Mixed‐matrix membranes (MMMs) of Matrimid® and polyaniline/clay (PC) are investigated for CO2/CH4 separation and CO2‐induced plasticization. PC particles are synthesized through in‐situ polymerization of aniline in the presence of organophilic clay and then incorporated into Matrimid by solution casting method. Chemical structure and morphology of PC powder and fabricated membranes are analyzed by Fourier transform infrared (FTIR), X‐ray diffraction (XRD), differential scanning calorimetry/thermogravimetric analysis (DSC/TGA) and scanning electron microscopy (SEM). The XRD spectra of PC particles show the exfoliation of silicate layers throughout the polyaniline (PAni) matrix, and SEM images indicate flower‐petal morphology for PC particles. The permeability values of CO2 and CH4 increase 30–35% by incorporation of 10 wt% PC without any significant drop in selectivity. PC particles with flower‐petal morphology plays an important role in increasing the gas permeability values of both gases while Matrimid is the only phase that controls CO2/CH4 selectivity. The plasticization pressure was increased to 30 bar by incorporation of 10 wt% PC in the Matrimid matrix. CO2 permeability and pplast improved 35% and 200%, respectively, resulting in 300% enhancement in the capacity of MMM in the purification of natural gas with a selectivity of about 40. Copyright © 2016 John Wiley & Sons, Ltd.  相似文献   

17.
In this study, graphene nanosheets (GNs) were incorporated into polyethersulfone (PES) by phase inversion approach for preparing PES-GNs mixed matrix membranes (MMMs). To investigate the impact of filler content on membrane surface morphology, thermal stability, chemical composition, porosity and mechanical properties, MMMs were constructed with various GNs loadings (0.01, 0.02, 0.03, and 0.04 wt%). ?The performance of prepared MMMs was tested for separation and selectivity of CO2, N2, H2 and CH4 gases at various pressures from 1 to 6 bar and temperature varying from 20 to 60 °C. It was observed that, compared to the pristine PES membrane, the prepared MMMs significantly improved the gas separation and selectivity performance with adequate mechanical stability. The permeability of CO2, N2, H2 and CH4 for the PES + 0.04 wt% GNs increases from 9 to 2246, 11 to 2235, 9 to 7151, and 3 to 4176 Barrer respectively, as compared with pure PES membrane at 1 bar and 20 °C due to improving the membrane absorption and porosity. In addition, by increasing the pressure, the permeability and selectivity of CO2, N2, H2 and CH4 are increased due to the increased driving force for the transport of gas via membranes. Furthermore, the permeability of CO2, N2, H2 and CH4 increased by increasing the temperature from 20 to 60 °C due to the plasticization in the membranes and the improvement in polymer chain movement. This result proved that the prepared membranes can be used for gas separation applications.  相似文献   

18.
In the early stage of membrane technology development in gas separation, utilization of polymeric membranes has gained attention due to their robustness and ease of fabrication. However, the performance of polymeric membranes is limited by the trade-off between permeability and selectivity. Meanwhile, inorganic membrane is capable to exhibit great enhancement in separation performance but unfortunately its fabrication process is hard and costly. Thus, development of mixed matrix membranes (MMMs) by incorporating inorganic fillers into the polymer matrix has become a potential alternative to overcome the limitations of polymeric and inorganic membranes in gas separation. Nevertheless, fabrication of defect-free MMMs with improved separation performance and without compromising the mechanical and thermal stability is extremely difficult and challenging. In the current review paper, various types of inorganic fillers for MMMs fabrication and recent reported efforts to tailor the underlying problems on MMMs fabrication were discussed. The future outlook to advance the performance of MMMs in gas separation especially for CO2/CH4 separation was highlighted.  相似文献   

19.
Incompatibility between filler and polymer chains accompanied by particle agglomeration has a detrimental effect on the performance of mixed matrix membranes (MMMs). To obviate intermolecular forces of different additives, functional groups (-COOH, –NCO, and –NH2) were grafted on the surface of multi-walled carbon nanotubes (MWCNTs) which were then incorporated as fillers in the poly(ether-block-amide) (PEBA) polymeric matrix in the range of 0.1–1 wt% loading. CO2 permeability and ideal CO2/N2 and CO2/CH4 selectivity of MMMs was compared with the neat membrane, and the results revealed favorable enhancement and surpassed CO2/N2 Robeson's upper bound under 4–10 bar in the range of 15–55 °C. Mixed gas separation performance of MMMs, which is of vital importance in industrial applications, was also investigated. The results indicate that MWCNT-NCO created superior grafts with the polymer chains, and MMMs with this additive had a better gas separation performance with high mechanical and thermal stability.  相似文献   

20.
In the present work, membranes from commercially available Pebax® MH 1657 and its blends with low molecular weight poly(ethylene glycol) PEG were prepared by using a simple binary solvent (ethanol/water). Dense film membranes show excellent compatibility with PEG system up to 50 wt.% of content. Gas transport properties have been determined for four gases (H2, N2, CH4, CO2) and the obtained permeabilities were correlated with polymer properties and morphology of the membranes. The permeability of CO2 in Pebax®/PEG membrane (50 wt.% of PEG) was increased two fold regarding to the pristine Pebax®. Although CO2/N2 and CO2/CH4 selectivity remained constant, an enhancement of CO2/H2 selectivity (∼11) was observed. These results were attributed to the presence of EO units which increases CO2 permeability, and to a probable increase of fractional free-volume. Furthermore, for free-volume discussion and permeability of gases, additive and Maxwell models were used.  相似文献   

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