Water-based synthesis and enhanced CO2 capture performance of perfluorinated cerium-based metal–organic frameworks with UiO-66 and MIL-140 topology

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dc.contributor.authorDonnadio, Anna
dc.contributor.authorCarta, Mariolino
dc.contributor.authorD'Amato, Roberto
dc.contributor.authorSangregorio, Claudio
dc.contributor.authorTiana, Davide
dc.contributor.authorVivani, Riccardo
dc.contributor.authorTaddei, Marco
dc.contributor.authorCostantino, Ferdinando
dc.contributor.funderHorizon 2020en
dc.contributor.funderH2020 Marie Skłodowska-Curie Actionsen
dc.contributor.funderUniversità degli Studi di Perugiaen
dc.date.accessioned2019-01-18T14:31:13Z
dc.date.available2019-01-18T14:31:13Z
dc.date.issued2019-11-23
dc.date.updated2019-01-18T12:53:17Z
dc.description.abstractReaction of cerium ammonium nitrate and tetrafluoroterephthalic acid in water afforded two new metal–organic frameworks with UiO-66 [F4_UiO-66(Ce)] and MIL-140 [F4_MIL-140A(Ce)] topologies. The two compounds can be obtained in the same experimental conditions, just by varying the amount of acetic acid used as crystallization modulator in the synthesis. Both F4_UiO-66(Ce) and F4_MIL-140A(Ce) feature pores with size <8 Å, which classifies them as ultramicroporous. Combination of X-ray photoelectron spectroscopy and magnetic susceptibility measurements revealed that both compounds contain a small amount of Ce(III), which is preferentially accumulated near the surface of the crystallites. The CO2 sorption properties of F4_UiO-66(Ce) and F4_MIL-140A(Ce) were investigated, finding that they perform better than their Zr-based analogues. F4_MIL-140A(Ce) displays an unusual S-shaped isotherm with steep uptake increase at pressure <0.2 bar at 298 K. This makes F4_MIL-140A(Ce) exceptionally selective for CO2 over N2: the calculated selectivity, according to the ideal adsorbed solution theory for a 0.15:0.85 mixture at 1 bar and 293 K, is higher than 1900, among the highest ever reported for metal–organic frameworks. The calculated isosteric heat of CO2 adsorption is in the range of 38–40 kJ mol–1, indicating a strong physisorptive character.en
dc.description.sponsorshipFondo Ricerca di Base FRB-2017 projecten
dc.description.statusPeer revieweden
dc.description.versionAccepted Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationD’Amato, R., Donnadio, A., Carta, M., Sangregorio, C., Tiana, D., Vivani, R., Taddei, M. and Costantino, F. (2019) 'Water-Based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal–Organic Frameworks with UiO-66 and MIL-140 Topology', ACS Sustainable Chemistry & Engineering, 7(1), pp. 394-402. doi: 10.1021/acssuschemeng.8b03765en
dc.identifier.doi10.1021/acssuschemeng.8b03765
dc.identifier.endpage402en
dc.identifier.issn2168-0485
dc.identifier.issued1en
dc.identifier.journaltitleAcs Sustainable Chemistry & Engineeringen
dc.identifier.startpage394en
dc.identifier.urihttps://hdl.handle.net/10468/7320
dc.identifier.volume7en
dc.language.isoenen
dc.publisherAmerican Chemical Society, ACSen
dc.relation.projectinfo:eu-repo/grantAgreement/EC/H2020::MSCA-COFUND-FP/663830/EU/Strengthening International Research Capacity in Wales/SIRCIWen
dc.relation.urihttps://pubs.acs.org/doi/10.1021/acssuschemeng.8b03765
dc.rights© 2018 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Sustainable Chemistry & Engineering, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acssuschemeng.8b03765en
dc.subjectCarbon dioxide captureen
dc.subjectGas separationsen
dc.subjectGreen synthesisen
dc.subjectPorous materialsen
dc.subjectMetal-organic frameworksen
dc.titleWater-based synthesis and enhanced CO2 capture performance of perfluorinated cerium-based metal–organic frameworks with UiO-66 and MIL-140 topologyen
dc.typeArticle (peer-reviewed)en
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