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Local pH oscillations witness autocatalytic self-organization of biomorphic nanostructures
Bottom-up self-assembly of simple molecular compounds is a prime pathway to complex materials with interesting structures and functions. Coupled reaction systems are known to spontaneously produce highly ordered patterns, so far observed in soft matter. Here we show that similar phenomena can occur during silica-carbonate crystallization, the emerging order being preserved. The resulting materials, called silica biomorphs, exhibit non-crystallographic curved morphologies and hierarchical textures, much reminiscent of structural principles found in natural biominerals. We have used a fluorescent chemosensor to probe local conditions during the growth of such self-organized nanostructures. We demonstrate that the pH oscillates in the local microenvironment near the growth front due to chemical coupling, which becomes manifest in the final mineralized architectures as intrinsic banding patterns with the same periodicity. A better understanding of dynamic autocatalytic crystallization processes in such simple model systems is key to the rational development of advanced materials and to unravel the mechanisms of biomineralization. ; This work was funded by the European Research Council (European Union's Seventh Framework Programme (FP7/2007-2013, grant no. 340863) and the Spanish MINECO grant CGL2010-16882 (co-funded by FEDER) ; Peer reviewed
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Interconvertible Hydrochlorothiazide–Caffeine Multicomponent Pharmaceutical Materials: A Solvent Issue
The design of new multicomponent pharmaceutical materials that involve different active pharmaceutical ingredients (APIs), e.g., drug-drug cocrystals, is a novel and interesting approach to address new therapeutic challenges. In this work, the hydrochlorothiazide-caffeine (HCT–CAF) codrug and its methanol solvate have been synthesized by mechanochemical methods and thoroughly characterized in the solid state by powder and single crystal X-ray diffraction, respectively, as well as differential scanning calorimetry, thermogravimetric analyses and infrared spectroscopy. In addition, solubility and stability studies have also been performed looking for improved physicochemical properties of the codrug. Interestingly, the two reported structures show great similarity, which allows conversion between them. The desolvated HCT–CAF cocrystal shows great stability at 24 h and an enhancement of solubility with respect to the reference HCT API. Furthermore, the contribution of intermolecular forces on the improved physicochemical properties was evaluated by computational methods showing strong and diverse H-bond and π–π stacking interactions. ; Spanish Agencia Estatal de Investigacion of the Ministerio de Ciencia, Innovacion y Universidades (MICIU) ; European Union (EU) PGC2018-102047-B-I00 ; MICIU/AEI from SPAIN CTQ2017-85821-R
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Role of CaCO3° neutral pair in calcium carbonate crystallization
The molecular structure of the units that get incorporated into the nuclei of the crystalline phase and sustain their growth is a fundamental issue in the pathway from a supersaturated solution to the formation of crystals. Using a fluorescent dye we have recorded the variation of the pH value in time along a gel where CaCl2 and NaHCO3 counter-diffuse to crystallize CaCO3. The same pH–space–time distribution maps were also computationally obtained using a chemical speciation code (phreeqc). Using data arising from this model we investigated the space-time evolution of the activity of the single species (ions and ion pairs) involved in the crystallization process. Our combined results suggest that, whatever the pathway from solution to crystals, the neutral pair CaCO3° is a key species in the CaCO3 precipitation system. ; European Research Council (European Union's Seventh Framework Programme (FP7/2007-2013) grant agreement no 340863, and Spanish MINECO grants MAT2014-60533-R and CGL2010-16882 cofounded with FEDER ; Peer reviewed
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Reflexiones sobre la diversidad religiosa, el pluralismo y la interculturalidad
In: Serie teológica número 27
Fluoride-doped amorphous calcium phosphate nanoparticles as a promising biomimetic material for dental remineralization
Demineralization of dental hard tissue is a widespread problem and the main responsible for dental caries and dentin hypersensitivity. The most promising strategies to induce the precipitation of new mineral phase are the application of materials releasing gradually Ca and PO ions or mimicking the mineral phase of the host tissue. However, the design of formulations covering both processes is so far a challenge in preventive dentistry. In this work, we have synthesized innovative biomimetic amorphous calcium phosphate (ACP), which has been, for the first time, doped with fluoride ions (FACP) to obtain materials with enhanced anti-caries and remineralizing properties. Significantly, the doping with fluoride (F) did not vary the physico-chemical features of ACP but resulted in a faster conversion to the crystalline apatite phase in water, as observed by in-situ time-dependent Raman experiments. The efficacy of the as synthesized ACP and FACP samples to occlude dentinal tubules and induce enamel remineralization has been tested in vitro in human molar teeth. The samples showed good ability to partially occlude the tubules of acid-etched dentin and to restore demineralized enamel into its native structure. Results demonstrate that ACP and FACP are promising biomimetic materials in preventive dentistry to hinder demineralization of dental hard tissues. ; M.I. acknowledges support by National Research Program -National Research Council (PNRCNR) Aging Program 2012–2014. J.M.D.-L. was partially supported by the Andalucía Talent Hub fellowship BioBone (cofunded by the Spanish Junta de Andalucía and EU-FP7 within the Marie Skłodowska-Curie Actions) and the Ramón y Cajal contract (NanoSmart, RYC-2016-21042) of the Spanish Government (Ministerio de Economía y Competividad). J.G.-M. acknowledges support from MAT2014-60533-R co-funded by FEDER.
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