Multivariate CuBTC Metal–Organic Framework with Enhanced Selectivity, Stability, Compatibility, and Processability

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dc.contributor.authorPeterson, Gregory W.
dc.contributor.authorAu, Kathleen
dc.contributor.authorTovar, Trenton M.
dc.contributor.authorEpps, Thomas H. III
dc.date.accessioned2019-11-04T17:39:53Z
dc.date.available2019-11-04T17:39:53Z
dc.date.issued2019-09-27
dc.description.abstractA novel, mixed-linker metal−organic framework (MOF) was synthesized, and the resulting macromolecular assembly had enhanced activity and stability in comparison to the isostructural CuBTC (aka HKUST-1). Mixtures of 5-aminoisophthalic acid (AIA) and 1,3,5-benzenetricarboxylic acid (BTC) were combined at different ratios to incorporate aryl amine groups into the MOF that were readily amenable to postsynthetic modification. As one example, the amine groups were reacted with decanoyl chloride (DC) through the formation of amide linkages, which overcame a major shortcoming of CuBTC by stabilizing the MOF toward ammonia vapor during breakthrough experiments and to liquid water for over 24 h. Furthermore, the MOF modified with DC exhibited ∼70% increases in CO₂/N₂ and CO₂/H₂O selectivity at flue gas relevant conditions relative to CuBTC. The modified MOFs had increased compatibility with polyacrylonitrile, poly(styrene-block-isoprene-block-styrene), and poly(styrene-block-ethylene-ranbutylene-block-styrene) polymers, which made them ideal for incorporation in polymer fibers and composite films and reduced defects generally associated with polymer−nanoparticle systems. Finally, the AIA and DC-modified MOFs had significantly enhanced moisture stability relative to unmodified CuBTC. Overall, this facile modification route provides the framework for higher-performance materials in applications such as filtration, gas storage, and flue gas scrubbing, among many others.en_US
dc.description.sponsorshipThe authors thank the U.S. Army for funding through CCDC Chemical Biological Center’s Individual Laboratory Independent Research program (PE 0601101A 91A). The opinions, interpretations, conclusions, and recommendations are those of the authors and are not necessarily endorsed by the United States Government. G.W.P. thanks John Mahle and Jim Buchanan for measuring water isotherms, Matt Browe for measuring breakthrough capacities, Hui Wang for conducting NMR experiments, and Erin Durke and Monica McEntee for conducting TIR experiments. T.H.E. acknowledges the Thomas & Kipp Gutshall Professorship at the University of Delaware for supporting this research effort.en_US
dc.description.urihttps://pubs.acs.org/doi/10.1021/acs.chemmater.9b02756en_US
dc.format.extent7 pagesen_US
dc.genrejournal articlesen_US
dc.identifierdoi:10.13016/m2iruc-ml6z
dc.identifier.citationPeterson, Gregory W.; Au, Kathleen; Tovar, Trenton M.; Epps, Thomas H. III; Multivariate CuBTC Metal–Organic Framework with Enhanced Selectivity, Stability, Compatibility, and Processability; Chemistry of Materials 31,20; https://doi.org/10.1021/acs.chemmater.9b02756en_US
dc.identifier.urihttps://doi.org/10.1021/acs.chemmater.9b02756
dc.identifier.urihttp://hdl.handle.net/11603/16030
dc.language.isoen_USen_US
dc.publisherAmerican Chemical Societyen_US
dc.relation.isAvailableAtThe University of Maryland, Baltimore County (UMBC)
dc.relation.ispartofUMBC Chemical, Biochemical & Environmental Engineering Department Collection
dc.relation.ispartofUMBC Faculty Collection
dc.rightsThis item is likely protected under Title 17 of the U.S. Copyright Law. Unless on a Creative Commons license, for uses protected by Copyright Law, contact the copyright holder or the author.
dc.rightsPublic Domain Mark 1.0*
dc.rightsThis work was written as part of one of the author's official duties as an Employee of the United States Government and is therefore a work of the United States Government. In accordance with 17 U.S.C. 105, no copyright protection is available for such works under U.S. Law.
dc.rights.urihttp://creativecommons.org/publicdomain/mark/1.0/*
dc.subjectmetal−organic frameworken_US
dc.subjectisostructural CuBTCen_US
dc.subjectCompatibilityen_US
dc.subjectProcessabilityen_US
dc.subjectStabilityen_US
dc.subjectSelectivityen_US
dc.titleMultivariate CuBTC Metal–Organic Framework with Enhanced Selectivity, Stability, Compatibility, and Processabilityen_US
dc.typeTexten_US

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