On the molecular mechanisms for the H2/CO2 separation performance of zeolite imidazolate framework two-layered membranes

Fernando Cacho-Bailo; Ismael Matito-Martos; Julio Perez-Carbajo; Miren Etxeberría-Benavides; Oğuz Karvan; Víctor Sebastián; Sofía Calero; Carlos Téllez; Joaquín Coronas

doi:10.1039/c6sc02411d

On the molecular mechanisms for the H₂/CO₂ separation performance of zeolite imidazolate framework two-layered membranes

Fernando Cacho-Bailo
, Ismael Matito-Martos
, Julio Perez-Carbajo
, Miren Etxeberría-Benavides
, Oğuz Karvan
, Víctor Sebastián
, Sofía Calero
, Carlos Téllez
, Joaquín Coronas

Research output: Contribution to journal › Article › Academic › peer-review

104 Citations (Scopus)

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 H₂/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 H₂/CO₂ separation selectivity of 9.6 together with a 250 GPU H₂ permeance at 150 °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.

Original language	English
Pages (from-to)	325-333
Number of pages	9
Journal	Chemical Science
Volume	8
Issue number	1
DOIs	https://doi.org/10.1039/c6sc02411d
Publication status	Published - 1 Jul 2017
Externally published	Yes

Funding

Financial support (MAT2013-40556-R) from the Spanish MINECO, the Arag?n Government (DGA, T05) and the European Social Fund is gratefully acknowledged. We also acknowledge the use of the Servicio General de Apoyo a la Investigaci?n-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 Microscop?as Avanzadas at the Instituto de Nanociencia de Arag?n (LMA-INA). The authors acknowledge the LMA-INA for offering access to their instruments and expertise.

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title = "On the molecular mechanisms for the H2/CO2 separation performance of zeolite imidazolate framework two-layered membranes",

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 H2/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 H2/CO2 separation selectivity of 9.6 together with a 250 GPU H2 permeance at 150 °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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AU - Cacho-Bailo, Fernando

AU - Matito-Martos, Ismael

AU - Perez-Carbajo, Julio

AU - Etxeberría-Benavides, Miren

AU - Karvan, Oğuz

AU - Sebastián, Víctor

AU - Calero, Sofía

AU - Téllez, Carlos

AU - Coronas, Joaquín

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N2 - 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 H2/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 H2/CO2 separation selectivity of 9.6 together with a 250 GPU H2 permeance at 150 °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.

AB - 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 H2/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 H2/CO2 separation selectivity of 9.6 together with a 250 GPU H2 permeance at 150 °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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On the molecular mechanisms for the H₂/CO₂ separation performance of zeolite imidazolate framework two-layered membranes

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