On the molecular mechanisms for the H2/CO2 separation performance of zeolite imidazolate framework two-layered membranes
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2017-07-01
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Abstract
Double-layered zeolitic imidazolate framework (ZIF) membranes were fabricated inside polyimide P84 hollow fibers by a step-synthesis conducted by microfluidic technology and applied to pre-combustion gas separation. Our hypothesis, based on the information provided by a combination of molecular simulation and experiments, is that a CO2 adsorption reduction on the surface of the ZIF-9 would enhance the molecular sieving effect of this ZIF-9 layer and therefore the selectivity in the H-2/CO2 mixture separation of the entire membrane. This reduction would be achieved by means of a less-CO2-adsorptive methylimidazolate-based ZIF-67 or ZIF-8 layer coating the ZIF-9. ZIF-8/ZIF-9 and ZIF-67/ZIF-9 double-layered membranes were prepared and characterized by XRD, FTIR, SEM, FIB, TEM and EDS. This unprecedented strategy led to a H-2/CO2 separation selectivity of 9.6 together with a 250 GPU H-2 permeance at 150 degrees C, showing a significant improvement with respect to the pure ZIF-9 membrane. Double-layered membranes also showed higher apparent CO2 activation energies than single-layered membranes, attributable to a diminished adsorption.
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Publisher Copyright: © The Royal Society of Chemistry.
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CARBON-DIOXIDE ADSORPTION , MIXED-MATRIX MEMBRANES , CO2 SEPARATION , HYDROGEN SELECTIVITY , COMPOSITE MEMBRANES , PHASE-TRANSITION , LINKER SYNTHESIS , ZIF-90 MEMBRANE , GAS SEPARATION , HOLLOW-FIBER , CARBON-DIOXIDE ADSORPTION , MIXED-MATRIX MEMBRANES , CO2 SEPARATION , HYDROGEN SELECTIVITY , COMPOSITE MEMBRANES , PHASE-TRANSITION , LINKER SYNTHESIS , ZIF-90 MEMBRANE , GAS SEPARATION , HOLLOW-FIBER , General Chemistry , SDG 13 - Climate Action , Funding Info , Financial support (MAT2013-40556-R) from the Spanish MINECO, the Aragon Government (DGA, T05) and the European Social Fund is gratefully acknowledged. We also acknowledge the use of the Servicio General de Apoyo a la Investigacion-SAI (Universidad de Zaragoza). F. C.-B. acknowledges his DGA predoctoral fellowship. V. S. acknowledges the support of the People Program (CIG-Marie Curie Actions, REA grant agreement no. 321642). I. M.-M. thanks the Spanish MINECO for his predoctoral fellowship. The European Research Council through an ERC Grant (ERC2011-StG-279520-RASPA) is also acknowledged. All the microscopy work was done in the Laboratorio de Microscopias Avanzadas at the Instituto de Nanociencia de Aragon (LMA-INA). The authors acknowledge the LMA-INA for offering access to their instruments and expertise. , Financial support (MAT2013-40556-R) from the Spanish MINECO, the Aragon Government (DGA, T05) and the European Social Fund is gratefully acknowledged. We also acknowledge the use of the Servicio General de Apoyo a la Investigacion-SAI (Universidad de Zaragoza). F. C.-B. acknowledges his DGA predoctoral fellowship. V. S. acknowledges the support of the People Program (CIG-Marie Curie Actions, REA grant agreement no. 321642). I. M.-M. thanks the Spanish MINECO for his predoctoral fellowship. The European Research Council through an ERC Grant (ERC2011-StG-279520-RASPA) is also acknowledged. All the microscopy work was done in the Laboratorio de Microscopias Avanzadas at the Instituto de Nanociencia de Aragon (LMA-INA). The authors acknowledge the LMA-INA for offering access to their instruments and expertise.
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Cacho-Bailo , F , Matito-Martos , I , Perez-Carbajo , J , Etxeberría-Benavides , M , Karvan , O , Sebastián , V , Calero , S , Téllez , C & Coronas , J 2017 , ' On the molecular mechanisms for the H2/CO2 separation performance of zeolite imidazolate framework two-layered membranes ' , Chemical Science , vol. 8 , no. 1 , pp. 325-333 . https://doi.org/10.1039/c6sc02411d