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In this work, the performance of new robust mixed matrix composite hollow fiber (MMCHF) membranes with a different selective layer composition is evaluated in the absence and presence of water vapor in CO2/N2 and CO2/CH4 separation. The selective layer of these membranes is made of highly permeable hydrophobic poly(trimethyl-1-silylpropine) (PTMSP) and hydrophilic chitosan-ionic liquid (IL-CS) hybrid matrices, respectively, filled with hydrophilic zeolite 4A particles in the first case and HKUST-1 nanoparticles in the second, coated over compatible supports. The effect of water vapor in the feed or using a commercial hydrophobic PDMSXA-10 HF membrane has also been studied for comparison. Mixed gas separation experiments were performed at values of 0 and 50% relative humidity (RH) in the feed and varying CO2 concentration in N2 and CH4, respectively. The performance has been validated by a simple mathematical model considering the effect of temperature and relative humidity on membrane permeability.
Clara Casado-Coterillo; Ana Fernández-Barquín; Angel Irabien. Effect of Humidity on CO2/N2 and CO2/CH4 Separation Using Novel Robust Mixed Matrix Composite Hollow Fiber Membranes: Experimental and Model Evaluation. Membranes 2019, 10, 6 .
AMA StyleClara Casado-Coterillo, Ana Fernández-Barquín, Angel Irabien. Effect of Humidity on CO2/N2 and CO2/CH4 Separation Using Novel Robust Mixed Matrix Composite Hollow Fiber Membranes: Experimental and Model Evaluation. Membranes. 2019; 10 (1):6.
Chicago/Turabian StyleClara Casado-Coterillo; Ana Fernández-Barquín; Angel Irabien. 2019. "Effect of Humidity on CO2/N2 and CO2/CH4 Separation Using Novel Robust Mixed Matrix Composite Hollow Fiber Membranes: Experimental and Model Evaluation." Membranes 10, no. 1: 6.
In the present work, the effect of zeolite type and topology on CO2 and N2 permeability using zeolites of different topology (CHA, RHO, and LTA) in the same Si/Al = 5, embedded in poly(trimethylsilyl-1-propyne) (PTMSP) is evaluated with temperature. Several models are compared on the prediction of CO2/N2 separation performance and then the modified Maxwell models are selected. The CO2 and N2 permeabilities through these membranes are predicted with an average absolute relative error (AARE) lower than 0.6% taking into account the temperature and zeolite loading and topology on non-idealities such as membrane rigidification, zeolite–polymer compatibility and sieve pore blockage. The evolution of this structure–performance relationship with temperature has also been predicted.
Clara Casado-Coterillo; Ana Fernández-Barquín; Susana Valencia; Angel Irabien. Estimating CO2/N2 Permselectivity through Si/Al = 5 Small-Pore Zeolites/PTMSP Mixed Matrix Membranes: Influence of Temperature and Topology. Membranes 2018, 8, 32 .
AMA StyleClara Casado-Coterillo, Ana Fernández-Barquín, Susana Valencia, Angel Irabien. Estimating CO2/N2 Permselectivity through Si/Al = 5 Small-Pore Zeolites/PTMSP Mixed Matrix Membranes: Influence of Temperature and Topology. Membranes. 2018; 8 (2):32.
Chicago/Turabian StyleClara Casado-Coterillo; Ana Fernández-Barquín; Susana Valencia; Angel Irabien. 2018. "Estimating CO2/N2 Permselectivity through Si/Al = 5 Small-Pore Zeolites/PTMSP Mixed Matrix Membranes: Influence of Temperature and Topology." Membranes 8, no. 2: 32.
CO2 permeability of zeolite A/PTMSP MMM increases with water content in the system, enhancing CO2/N2 and CO2/CH4 selectivities of PTMSP.
Ana Fernández-Barquín; Riccardo Rea; Davide Venturi; Marco Giacinti-Baschetti; Maria Grazia De Angelis; Clara Casado-Coterillo; Ángel Irabien. Effect of relative humidity on the gas transport properties of zeolite A/PTMSP mixed matrix membranes. RSC Advances 2018, 8, 3536 -3546.
AMA StyleAna Fernández-Barquín, Riccardo Rea, Davide Venturi, Marco Giacinti-Baschetti, Maria Grazia De Angelis, Clara Casado-Coterillo, Ángel Irabien. Effect of relative humidity on the gas transport properties of zeolite A/PTMSP mixed matrix membranes. RSC Advances. 2018; 8 (7):3536-3546.
Chicago/Turabian StyleAna Fernández-Barquín; Riccardo Rea; Davide Venturi; Marco Giacinti-Baschetti; Maria Grazia De Angelis; Clara Casado-Coterillo; Ángel Irabien. 2018. "Effect of relative humidity on the gas transport properties of zeolite A/PTMSP mixed matrix membranes." RSC Advances 8, no. 7: 3536-3546.
Novel mixed matrix membranes (MMM) with different characteristics are experimentally evaluated in a two-stage membranes-in-series bench-scale setup for the separation of CO2-N2 gas mixtures. For stage 1, a high permeability (higher than 1000 Barrer) and low selectivity (about 5–10) membrane is chosen: the [emim][Ac]-Chitosan (IL-CS) hybrid membrane developed in our laboratory and the Pervap 4060 (Sulzer) composite membrane. For stage 2, we chose our Zeolite A/PTMSP MMM, whose selectivity is higher than 20 even at up to 343 K, the CO2 permeability not lower than 5000 Barrer, which allows skipping the use of the intermediate compressor. The influence of membrane intrinsic properties (i.e. selective membrane material), number of modules in series, and feed concentration on separation performance is evaluated experimentally. In this system, a 10% CO2 feed is concentrated to 43%, 26 and 40% for the Zeolite A/PTMSP MMM – Zeolite A/PTMSP MMM, IL-CS – Zeolite A/PTMSP and Pervap 4060 – Zeolite A/PTMSP in stage 1 and stage 2, respectively. The agreement of the experimental results with a mathematical model at the low CO2 feed concentration of flue gas allows estimating the membrane area needed for each membrane material to achieve a given CO2 purity and removal efficiency. The very large membrane areas needed to reach the 90% CO2 purity and removal efficiency target are drastically reduced if the CO2 removal efficiency required is set to 70%, especially for the combinations with different membranes in each stage, which gives scope for attempting further development of novel membrane materials for CO2capture processes.This work is partially based on a concept from Eliot S. Gerber (U. S.A.), for which he is gratefully acknowledged. The authors are also grateful for the financial support from the Spanish Ministry of Economy and Competitiveness (MINECO) under project CTQ2012-31229. A.F.B. and C.C.C. also thank the MINECO for the Early Stage Researcher (BES2013-064266) and ‘‘Ramón y Cajal” (RYC2011-0855) contracts, respectively
Ana Fernández-Barquín; Clara Casado-Coterillo; Ángel Irabien. Separation of CO 2 -N 2 gas mixtures: Membrane combination and temperature influence. Separation and Purification Technology 2017, 188, 197 -205.
AMA StyleAna Fernández-Barquín, Clara Casado-Coterillo, Ángel Irabien. Separation of CO 2 -N 2 gas mixtures: Membrane combination and temperature influence. Separation and Purification Technology. 2017; 188 ():197-205.
Chicago/Turabian StyleAna Fernández-Barquín; Clara Casado-Coterillo; Ángel Irabien. 2017. "Separation of CO 2 -N 2 gas mixtures: Membrane combination and temperature influence." Separation and Purification Technology 188, no. : 197-205.
Zeolite A/poly (1-trimethylsilyl-1-propyne) (zeoliteA/PTMSP) and [emim][Ac]/chitosan (IL/CS) are mixed-matrix membrane (MMM) materials with enhanced CO2/N2 permselectivity even at higher temperature. The scalability to asymmetric flat and hollow-fiber geometry by a simple dip-coating method was analyzed. The CO2/N2 separation performance was evaluated at different temperatures. The resulting composite membranes exhibit a significantly enhanced CO2 permeation flux because the MMM layer thickness is reduced by 97 % from flat to hollow-fiber geometries in IL-CS composite membranes, while the selectivity is maintained similar to the self-standing membranes, thus proving that compatibility between the membrane component materials leads to a defect-free composite membrane, regardless the geometry and temperature.
Ana Fernández-Barquín; Clara Casado-Coterillo; Miren Etxeberria-Benavides; Jon Zuñiga; Angel Irabien. Comparison of Flat and Hollow-Fiber Mixed-Matrix Composite Membranes for CO 2 Separation with Temperature. Chemical Engineering & Technology 2017, 40, 997 -1007.
AMA StyleAna Fernández-Barquín, Clara Casado-Coterillo, Miren Etxeberria-Benavides, Jon Zuñiga, Angel Irabien. Comparison of Flat and Hollow-Fiber Mixed-Matrix Composite Membranes for CO 2 Separation with Temperature. Chemical Engineering & Technology. 2017; 40 (5):997-1007.
Chicago/Turabian StyleAna Fernández-Barquín; Clara Casado-Coterillo; Miren Etxeberria-Benavides; Jon Zuñiga; Angel Irabien. 2017. "Comparison of Flat and Hollow-Fiber Mixed-Matrix Composite Membranes for CO 2 Separation with Temperature." Chemical Engineering & Technology 40, no. 5: 997-1007.
In this work, mixed matrix membranes (MMMs) composed of small-pore zeolites with various topologies (CHA (Si/Al = 5), LTA (Si/Al = 1 and 5), and Rho (Si/Al = 5)) as dispersed phase, and the hugely permeable poly(1-trimethylsilyl-1-propyne) (PTMSP) as continuous phase, have been synthesized via solution casting, in order to obtain membranes that could be attractive for oxygen-enriched air production. The O2/N2 gas separation performance of the MMMs has been analyzed in terms of permeability, diffusivity, and solubility in the temperature range of 298–333 K. The higher the temperature of the oxygen-enriched stream, the lower the energy required for the combustion process. The effect of temperature on the gas permeability, diffusivity, and solubility of these MMMs is described in terms of the Arrhenius and Van’t Hoff relationships with acceptable accuracy. Moreover, the O2/N2 permselectivity of the MMMs increases with temperature, the O2/N2 selectivities being considerably higher than those of the pure PTMSP. In consequence, most of the MMMs prepared in this work exceeded the Robeson’s upper bound for the O2/N2 gas pair in the temperature range under study, with not much decrease in the O2 permeabilities, reaching O2/N2 selectivities of up to 8.43 and O2 permeabilities up to 4,800 Barrer at 333 K.
Ana Fernández-Barquín; Clara Casado-Coterillo; Susana Valencia Valencia; Angel Irabien. Mixed Matrix Membranes for O2/N2 Separation: The Influence of Temperature. Membranes 2016, 6, 28 .
AMA StyleAna Fernández-Barquín, Clara Casado-Coterillo, Susana Valencia Valencia, Angel Irabien. Mixed Matrix Membranes for O2/N2 Separation: The Influence of Temperature. Membranes. 2016; 6 (2):28.
Chicago/Turabian StyleAna Fernández-Barquín; Clara Casado-Coterillo; Susana Valencia Valencia; Angel Irabien. 2016. "Mixed Matrix Membranes for O2/N2 Separation: The Influence of Temperature." Membranes 6, no. 2: 28.
In this work, small-pore zeolites of different topology (CHA, LTA5, Rho), all with Si/Al ratio of 5, have been added to highly permeable poly(1-trimethylsilyl-1-propyne) (PTMSP) to increase its selectivity and thermal and mechanical stability. Membranes were characterized by TGA, XRD, SEM and CO2 and N2 single gas permeation measurements at different temperatures. TGA reveal that the thermal resistance of the mixed matrix membranes (MMM) is as good as that of pure PTMSP polymer membranes. XRD and SEM results reflect that there is good interaction between the fillers and the membrane matrix, at 5 and 10 wt.% zeolite loadings, while at 20 wt.% a dual layer structure is formed, when Rho zeolite is the filler, because the particle size of Rho is higher than those of LTA5 or CHA, and voids appear that limit the permselectivity performance. In single gas permeation of N2 and CO2, the influence of temperature, zeolite loading and type is analyzed. The selectivity of pure PTMSP is considerably enhanced with the addition of the zeolites and the increase of temperature, and the MMM loaded with 5 wt.% zeolite surpassed the Robeson's upper bound for CO2/N2 separation, without decreasing the permeability too much. Upon increasing temperature from 298 to 333 K, the permselectivity is enhanced even further without loss of permeability. The 5 wt.% loaded membranes were tested in CO2/N2 mixed gas separation experiments at 333 K and 12.5 wt.% CO2 in the feed, and the permselectivity of LTA5- and Rho-PTMSP membranes was further enhanced, compared with the single gas permeation experiments.Financial support from the Spanish Ministry of Economy and Competitiveness (MINECO) under project CTQ2012-31229 at the Universidad de Cantabria and MAT2012-38567-C02-01 and Severo Ochoa SEV-2012-0267 at the ITQ (UPV-CSIC) are gratefully acknowledged. A.F.B. and C.C.C. also thank the MINECO for the Early Stage Researcher (BES2013-064266) and ‘‘Ramón y Cajal’’ tenure-track (RYC2011-0855) contracts, respectively
Ana Fernández-Barquín; Clara Casado-Coterillo; Miguel Palomino; Susana Valencia; Angel Irabien. Permselectivity improvement in membranes for CO2/N2 separation. Separation and Purification Technology 2016, 157, 102 -111.
AMA StyleAna Fernández-Barquín, Clara Casado-Coterillo, Miguel Palomino, Susana Valencia, Angel Irabien. Permselectivity improvement in membranes for CO2/N2 separation. Separation and Purification Technology. 2016; 157 ():102-111.
Chicago/Turabian StyleAna Fernández-Barquín; Clara Casado-Coterillo; Miguel Palomino; Susana Valencia; Angel Irabien. 2016. "Permselectivity improvement in membranes for CO2/N2 separation." Separation and Purification Technology 157, no. : 102-111.
The CO2 permeability and CO2/N2 selectivity of IL–CS membranes is improved by adding nano-HKUST-1 and ZIF-8, and predicted accurately by Maxwell-derived model as a function of interfacial contact, crystallinity and pore blockage with temperature.
Clara Casado-Coterillo; Ana Fernández-Barquín; Beatriz Zornoza; Carlos Téllez; Joaquín Coronas; A Irabien. Synthesis and characterisation of MOF/ionic liquid/chitosan mixed matrix membranes for CO2/N2 separation. RSC Advances 2015, 5, 102350 -102361.
AMA StyleClara Casado-Coterillo, Ana Fernández-Barquín, Beatriz Zornoza, Carlos Téllez, Joaquín Coronas, A Irabien. Synthesis and characterisation of MOF/ionic liquid/chitosan mixed matrix membranes for CO2/N2 separation. RSC Advances. 2015; 5 (124):102350-102361.
Chicago/Turabian StyleClara Casado-Coterillo; Ana Fernández-Barquín; Beatriz Zornoza; Carlos Téllez; Joaquín Coronas; A Irabien. 2015. "Synthesis and characterisation of MOF/ionic liquid/chitosan mixed matrix membranes for CO2/N2 separation." RSC Advances 5, no. 124: 102350-102361.
Mixed‐matrix membranes (MMM) consisting of poly(1‐trimethylsilyl‐1‐propyne) (PTMSP) as continuous matrix and small‐pore LTA‐framework zeolites with Si/Al ratios from 1 (commercial zeolite A) to ∞ (ITQ‐29) as dispersed phase were prepared by solution casting. The thermal stability of the MMM is as high as that of glassy PTMSP polymer, whose high permeability is maintained even at increasing temperature. The effect of the Si/Al ratio in the zeolite fillers on the membrane performance is observed by the increasing CO2/N2 permselectivity of low‐Si/Al ratio zeolite A‐based membranes, in comparison with pure silica ITQ‐29. The performance of the LTA‐type zeolite‐PTMSP MMM was adjusted to the modified Maxwell model by estimating the chain immobilization factor and the interphase thickness as a function of temperature, Si/Al ratio, and zeolite loading.
Ana Fernández-Barquín; Clara Casado-Coterillo; Miguel Palomino; Susana Valencia; Angel Irabien. LTA/Poly(1-trimethylsilyl-1-propyne) Mixed-Matrix Membranes for High-Temperature CO2/N2Separation. Chemical Engineering & Technology 2015, 38, 658 -666.
AMA StyleAna Fernández-Barquín, Clara Casado-Coterillo, Miguel Palomino, Susana Valencia, Angel Irabien. LTA/Poly(1-trimethylsilyl-1-propyne) Mixed-Matrix Membranes for High-Temperature CO2/N2Separation. Chemical Engineering & Technology. 2015; 38 (4):658-666.
Chicago/Turabian StyleAna Fernández-Barquín; Clara Casado-Coterillo; Miguel Palomino; Susana Valencia; Angel Irabien. 2015. "LTA/Poly(1-trimethylsilyl-1-propyne) Mixed-Matrix Membranes for High-Temperature CO2/N2Separation." Chemical Engineering & Technology 38, no. 4: 658-666.