70693 20190709135531.0 doi 10.1039/c7ce00086c sideral 98452 ART-2017-98452 eng (orcid)0000-0002-0238-3127 Cacho-Bailo, Fernando Universidad de Zaragoza Sequential amine functionalization inducing structural transition in an aldehyde-containing zeolitic imidazolate framework: Application to gas separation membranes 2017 Access copy available to the general public Unrestricted A modification in the gas separation performance of zeolitic imidazolate framework (ZIF)-supported hollow fiber (HF) membranes by means of an imine-condensation functionalization reaction carried out by microfluidics is reported. The accommodation of voluminous amine molecules in the SIM-1, Zn(4-methyl-5-imidazolecarboxaldehyde)2, also known as ZIF-94, sod structure during the functionalization reaction caused the ZIF atoms to be rearranged in a less dense rho structure, with a wider pore diameter and a diminished CO2 affinity. These changes had effects on the membrane performance, resulting in an enhanced CO2 permeance while maintaining a good permeance-selectivity balance. ZIF aldehyde-containing SIM-1 membranes were earlier prepared on the inner side of polymeric P84® HF using a microfluidic approach. The SIM-1 membranes displayed very interesting results in the separation of gas mixtures of great relevance to the natural gas field. High selectivities in the separation of He/CH4 (160), H2/CH4 (136) and CO2/CH4 (38) mixtures were achieved, and these are the first SIM-1 membranes with such a high separation performance to the best of our knowledge. These SIM-1 membranes were in situ stepwise functionalized with long-chain amine solutions, namely, hexyl- and nonylamine. Microfluidics allowed the easy sequential implementation of this post-reaction step in the membrane fabrication procedure. An imine-condensation reaction took place between the aldehyde groups in the 4-methyl-5-imidazolecarboxaldehyde ligand forming SIM-1 and the corresponding amines. The extent of the reaction was analyzed by FTIR, TGA and XRD, together with the changes in the textural properties and the adsorption capacities. info:eu-repo/grantAgreement/ES/DGA/T05 info:eu-repo/grantAgreement/ES/MINECO/MAT2013-40566-R info:eu-repo/grantAgreement/ES/MINECO/MAT2016-77290-R info:eu-repo/semantics/openAccess All rights reserved http://www.europeana.eu/rights/rr-f/ 3.304 2017 CHEMISTRY, MULTIDISCIPLINARY 62 / 171 = 0.363 2017 Q2 T2 CRYSTALLOGRAPHY 8 / 26 = 0.308 2017 Q2 T1 0.998 2017 Chemistry (miscellaneous) 2017 Q1 Materials Science (miscellaneous) 2017 Q1 Condensed Matter Physics 2017 Q1 info:eu-repo/semantics/article info:eu-repo/semantics/acceptedVersion Etxeberría-Benavides, Miren Karvan, Oguz (orcid)0000-0002-4954-1188 Téllez, Carlos Universidad de Zaragoza (orcid)0000-0003-1512-4500 Coronas, Joaquín Universidad de Zaragoza 5005 555 Universidad de Zaragoza Dpto. Ing.Quím.Tecnol.Med.Amb. Área Ingeniería Química 19 (2017), [20 pp.] CrystEngComm CRYSTENGCOMM 1466-8033 1041491 http://zaguan.unizar.es/record/70693/files/texto_completo.pdf Postprint 74233 http://zaguan.unizar.es/record/70693/files/texto_completo.jpg?subformat=icon icon Postprint oai:zaguan.unizar.es:70693 articulos driver 2019-07-09-12:02:36 ARTICLE