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Guest Molecule-Responsive Functional Calcium Phosphonate Frameworks for Tuned Proton Conductivity
dc.contributor.author | Bazaga-García, Montse | |
dc.contributor.author | Pérez-Colodrero, Rosario Mercedes | |
dc.contributor.author | Papadaki, M. | |
dc.contributor.author | Garczarek, Piotr | |
dc.contributor.author | Zon, Jerzy | |
dc.contributor.author | Olivera-Pastor, Pascual | |
dc.contributor.author | Losilla, Enrique R. | |
dc.contributor.author | León-Reina, Laura | |
dc.contributor.author | García-Aranda, Miguel Ángel | |
dc.contributor.author | Choquesillo-Lazarte, Duane | |
dc.contributor.author | Demadis, Konstantinos D. | |
dc.contributor.author | Cabeza-Díaz, Aurelio | |
dc.date.accessioned | 2021-03-08T08:48:15Z | |
dc.date.available | 2021-03-08T08:48:15Z | |
dc.date.issued | 2014-03-18 | |
dc.identifier.citation | J. Am. Chem. Soc. 2014, 136, 5731−5739 | es_ES |
dc.identifier.uri | https://hdl.handle.net/10630/21042 | |
dc.description.abstract | We 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.sponsorship | Proyecto nacional MAT2010-15175 | es_ES |
dc.language.iso | eng | es_ES |
dc.publisher | American Chemical Society | es_ES |
dc.rights | info:eu-repo/semantics/openAccess | es_ES |
dc.subject | Química | es_ES |
dc.subject.other | Calcium Phosphonate | es_ES |
dc.subject.other | Guest Molecule | es_ES |
dc.subject.other | X-ray diffraction | es_ES |
dc.subject.other | Synchrotron powder diffraction | es_ES |
dc.subject.other | Ammonia | es_ES |
dc.subject.other | 5-(dihydroxyphosphoryl)isophthalic acid | es_ES |
dc.subject.other | PiPhtA | es_ES |
dc.subject.other | Ca-PiPhtA | es_ES |
dc.subject.other | Metal phosphonates | es_ES |
dc.subject.other | Proton conductivity | es_ES |
dc.title | Guest Molecule-Responsive Functional Calcium Phosphonate Frameworks for Tuned Proton Conductivity | es_ES |
dc.type | info:eu-repo/semantics/article | es_ES |
dc.centro | Facultad de Ciencias | es_ES |
dc.identifier.doi | dx.doi.org/10.1021/ja500356z | |
dc.type.hasVersion | info:eu-repo/semantics/publishedVersion | es_ES |