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dc.contributor.authorBazaga García, Montse
dc.contributor.authorColodrero, Rosario M.P.
dc.contributor.authorPapadaki, M.
dc.contributor.authorGarczarek, Piotr
dc.contributor.authorZon, Jerzy
dc.contributor.authorOlivera-Pastor, Pascual 
dc.contributor.authorLosilla, Enrique R.
dc.contributor.authorLeón-Reina, Laura
dc.contributor.authorG. Aranda, Miguel Ángel
dc.contributor.authorChoquesillo-Lazarte, Duane
dc.contributor.authorDemadis, Konstantinos D.
dc.contributor.authorCabeza-Diaz, Aurelio 
dc.date.accessioned2021-03-08T08:48:15Z
dc.date.available2021-03-08T08:48:15Z
dc.date.issued2014-03-18
dc.identifier.citationJ. Am. Chem. Soc. 2014, 136, 5731−5739es_ES
dc.identifier.urihttps://hdl.handle.net/10630/21042
dc.description.abstractWe report the synthesis, structural characterization, and functionality of an open-framework hybrid that combines Ca2+ ions and the rigid polyfunctional ligand 5-(dihydroxyphosphoryl) isophthalic acid (PiPhtA). Ca-PiPhtA-I is obtained by slow crystallization at ambient conditions from acidic (pH≈3) aqueous solutions. It possesses a high water content (both Ca coordinated and in the lattice), and importantly, it exhibits water-filled 1D channels. At 75 °C, Ca-PiPhtA-I is partially dehydrated and exhibits a crystalline diffraction pattern that can be indexed in a monoclinic cell with parameters close to the pristine phase. Rietveld refinement was carried out for the sample heated at 75 °C, Ca-PiPhtA-II, using synchrotron powder X-ray diffraction data.All connectivity modes of the “parent” Ca-PiPhtA-I framework are retained in Ca-PiPhtA-II. Upon Ca-PiPhtA-I exposure to ammonia vapors (28% aqueous NH3) a new derivative is obtained (Ca-PiPhtA-NH3) containing 7 NH3 and 16 H2O molecules according to elemental and thermal analyses. Ca-PiPhtA-NH3 exhibits a complex X-ray diffraction pattern with peaks at 15.3 and 13.0 Å that suggest partial breaking and transformation of the parent pillared structure. Although detailed structural identification of Ca-PiPhtA-NH3 was not possible, due in part to nonequilibrium adsorption conditions and the lack of crystallinity, FT-IR spectra and DTA-TG analysis indicate profound structural changes compared to the pristine Ca-PiPhtA-I. At 98% RH and T = 24 °C, proton conductivity, σ, for Ca PiPhtA-I is 5.7 ×10−4 S·cm−1. It increases to 1.3 × 10−3 S·cm−1 upon activation by preheating the sample at 40 °C for 2 h followed by water equilibration at room temperature under controlled conditions. Ca-PiPhtA-NH3 exhibits the highest proton conductivity, 6.6 × 10−3 S·cm−1, measured at 98% RH and T = 24 °C. Ea for proton transfer in the above-mentioned frameworks range between 0.23 and 0.4 eV, typical of a Grothuss mechanism of proton conduction.es_ES
dc.description.sponsorshipProyecto nacional MAT2010-15175es_ES
dc.language.isoenges_ES
dc.publisherAmerican Chemical Societyes_ES
dc.rightsinfo:eu-repo/semantics/openAccesses_ES
dc.subjectQuímicaes_ES
dc.subject.otherCalcium Phosphonatees_ES
dc.subject.otherGuest Moleculees_ES
dc.subject.otherX-ray diffractiones_ES
dc.subject.otherSynchrotron powder diffractiones_ES
dc.subject.otherAmmoniaes_ES
dc.subject.other5-(dihydroxyphosphoryl)isophthalic acides_ES
dc.subject.otherPiPhtAes_ES
dc.subject.otherCa-PiPhtAes_ES
dc.subject.otherMetal phosphonateses_ES
dc.subject.otherProton conductivityes_ES
dc.titleGuest Molecule-Responsive Functional Calcium Phosphonate Frameworks for Tuned Proton Conductivityes_ES
dc.typeinfo:eu-repo/semantics/articlees_ES
dc.centroFacultad de Cienciases_ES
dc.identifier.doidx.doi.org/10.1021/ja500356z
dc.type.hasVersioninfo:eu-repo/semantics/publishedVersiones_ES


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