9 research outputs found
Metal-Organic Frameworks and their composites for water remediation
347 p.La contaminación del agua es una preocupación global creciente, ya como consecuencia de los avances económicos del siglo XXI, cada día aumenta el número y tipo de productos químicos, fármacos y materiales que entran en contacto con las fuentes de agua, y por ende, con la cadena trófica completa. Entre las múltiples estrategias para abordar este problema, la adsorción y la fotocatálisis han atraído una atención considerable debido a su simplicidad, rentabilidad, fácil portabilidad y el hecho de que no necesite la adición de productos secundarios dañinos. En este sentido, las estructuras metal-orgánicas (MOF por sus siglas en inglés) se han perfilado como materiales muy prometedores ya que pueden fusionar adsorción y fotocatálisis en un mismo material.Los MOF son sólidos cristalinos construidos a partir de iones metálicos o grupos conectados por ligandos orgánicos en redes extendidas, ordenadas y altamente porosas. Estos materiales han sido ampliamente estudiados para la remediación de agua debido a la buena estabilidad química y térmica que muestran. Sin embargo, la mayoría de estos MOF muestran una baja selectividad por la mayoría de los iones metálicos, por lo que se deben realizar diferentes estrategias de funcionalización en ellos para mejorar sus capacidades de adsorción respecto a los metales pesados. Esta tesis se centra en explorar diferentes estrategias de funcionalización con el objetivo de mejorar la capacidad de adsorción hacia iones metálicos o potenciar otras funcionalidades, como la capacidad de fotorreducción de los metales o la actividad catalítica para degradar contaminantes fenólicos
Chitin/Metal‐Organic Framework Composites as Wide‐Range Adsorbent
Composites based on chitin (CH) biopolymer and metal-organic framework (MOF) microporous nanoparticles have been developed as broad-scope pollutant absorbent. Detailed characterization of the CH/MOF composites revealed that the MOF nanoparticles interacted through electrostatic forces with the CH matrix, inducing compartmentalization of the CH macropores that led to an overall surface area increase in the composites. This created a micro-, meso-, and macroporous structure that efficiently retained pollutants with a broad spectrum of different chemical natures, charges, and sizes. The unique prospect of this approach is the combination of the chemical diversity of MOFs with the simple processability and biocompatibility of CH that opens application fields beyond water remediation.Fil: Tovar Jimenez, Gabriel Ibrahin. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Houssay. Instituto de Química y Metabolismo del Fármaco. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Instituto de Química y Metabolismo del Fármaco; ArgentinaFil: Valverde, Ainara. Universidad del País Vasco; EspañaFil: Mendes Felipe, Cristian. Universidad del País Vasco; EspañaFil: Wuttke, Stefan. Universidad del País Vasco; EspañaFil: Fidalgo Marijuan, Arkaitz. University of the Basque Country ; EspañaFil: Larrea, Edurne S.. Loire Valley Institute for Advanced Studies, ; FranciaFil: Lezama, Luis. Universidad del País Vasco; EspañaFil: Zheng, Fangyuan. Universidad del País Vasco; EspañaFil: Reguera, Javier. Universidad del País Vasco; EspañaFil: Lanceros Méndez, Senentxu. Universidad del País Vasco; EspañaFil: Arriortua, María. Universidad del País Vasco; EspañaFil: Copello, Guillermo Javier. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Houssay. Instituto de Química y Metabolismo del Fármaco. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Instituto de Química y Metabolismo del Fármaco; ArgentinaFil: Luis, Roberto Fernández. Universidad del País Vasco; Españ
Multigeruza polimerikoak: mediku-protesietarako materialen ezaugarriak hobetzeko bidea
Biomedikuntza arloan inplante moduan erabiltzeko material berrien es-kaera handia dago, baina errefus arazoak sortzen dituzte biobateragarritasun kontuak direla eta.Lan honetan azalduko dugu nola eraldatu dugun bi substratu motaren gainazala. Bat ezorganikoa izango da eta bestea polimerikoa. Geruzaz geruzako ("layer by layer") estrategiaz baliatuta, azido hialuroniko eta kitosanozko multigeruzak sortuko dira.Kitosanoa fluoreszenteki markatu eta mikroskopio konfokalean fluoreszentzia-haz kun dea behatu ondoren, ondorioztatu da geruzak modu arrakastatsu batean sortu direla. Honi esker, materialaren hidrofilitatea areagotzea lortu da, eta horrela, bakte-rioen aurkako gainazala lortzeaz gainera materialaren biobateragarritasuna handituko da modu merke eta sinple batean.; There is a great demand for new materials in the field of biomedicine to be used as implants, however they cause rejection problems due to their lack of biocom-patibility. In this work two substrates (inorganic and polymeric) will be surface modi-fied using the layer by layer strategy (LbL), in order to construct hyaluronic and chi-tosan multilayers. It has been proven that the layers were successfully built by fluorescent confocal microscopy by means of the increase of fluorescence along layers deposition after fluorescent labelling of chitosan. Thanks to this, it has been possible to increase the hydrophilicity of the surfaces enhancing antibacterial properties and get-ting more biocompatible materials in a simple and inexpensive way
Metal organic framework based PVDF separators for high rate cycling lithium-ion batteries
Poly(vinylidene fluoride) (PVDF) and MOF-808-based separators for lithium-ion batteries (LIBs) have been prepared and fully characterized in terms of morphological and thermal properties, electrolyte uptake, and retention, and surface hydrophilic characteristics. The effect of PVDF/MOF-808 separators on the electrochemical performance of LIBs has been evaluated. The PVDF/MOF-808 membranes exhibit a well-defined porous structure with a uniform distribution of interconnected macro- to mesopores. The inclusion of the Zr-based MOF nanoparticles increases the porosity and surface area of the separator, enhancing the electrolyte uptake and the ionic conductivity. Finally, the presence of MOF-808 fillers improves the liquid electrolyte retention, which prevents the capacity fading at high C-rates cycling. Indeed, charge–discharge tests performed in Li/C-LiFePO4 half-cells reveal a discharge capacity of 68 mAh·.g–1 at 2C-rate for PVDF/MOF-808 membranes, in comparison with the 0 mAh·g–1 obtained for pure PVDF. The PVDF/10 wt % MOF-808 sample shows a long-term stable cycling behavior with a Coulombic efficiency close to 100%. Thus, it is shown that the composite membranes represent an improvement with respect to conventional separators for lithium ion battery applications, since they coupled the polymer meso- and macroporous structure with the well-ordered microporous system of the MOFs, which improve significantly the electrolyte affinityFCT (Fundação para a Ciência e Tecnologia) for financial support under the framework of Strategic Funding grants UID/FIS/04650/2019, and UID/QUI/0686/2019 and project PTDC/FIS-MAC/28157/2017. The author also thanks the FCT for financial support under grant SFRH/BPD/112547/2015 (C.M.C.) and Investigator FCT contract CEECIND/00833/2017 (R.G.). A.V. thanks to the Basque Government Education department for her pre-doctoral grant. The European Commission Research & Innovation H2020-MSCA-RISE-2017 (Ref.: 778412) INDESMOF project is also acknowledged. Financial support from the Basque Government Industry and Education Departments under the ELKARTEK (ACTIMAT and LION), HAZITEK (SIMAM) and PIBA (PIBA-2018-06- LIMOFILM)
New clues to the evolutionary history of the main European paternal lineage M269:dissection of the Y-SNP S116 in Atlantic Europe and Iberia
The dissection of S116 in more than 1500 individuals from Atlantic Europe and the Iberian Peninsula has provided important clues about the controversial evolutionary history of M269. First, the results do not point to an origin of M269 in the Franco–Cantabrian refuge, owing to the lack of sublineage diversity within M269, which supports the new theories proposing its origin in Eastern Europe. Second, S116 shows frequency peaks and spatial distribution that differ from those previously proposed, indicating an origin farther west, and it also shows a high frequency in the Atlantic coastline. Third, an outstanding frequency of the DF27 sublineage has been found in Iberia, with a restricted distribution pattern inside this peninsula and a frequency maximum in the area of the Franco–Cantabrian refuge. This entire panorama indicates an old arrival of M269 into Western Europe, because it has generated at least two episodes of expansion in the Franco–Cantabrian area. This study demonstrates the importance of continuing the dissection of the M269 lineage in different European populations because the discovery and study of new sublineages can adjust or even completely revise the theories about European peopling, as has been the case for the place of origin of M269
Designing Metal-Chelator-like Traps by Encoding Amino Acids in Zirconium-Based Metal-Organic Frameworks
Metal chelators and porous sorbents are two of the forefront technologies applied for the recovery and separation of hazardous and/or valuable metal ions from aqueous solutions (i.e., polluted water sources, metal-rich mining wastewaters, acid leachates, and so forth). The transfer of the metal coordination functions of metal chelators to chemically stable host materials had only limited success so far. Here, we report the installation of natural acids (i.e., malic acid, mercaptosuccinic acid, succinic acid, fumaric acid, and citric acid) and amino acids (i.e., histidine, cysteine, and asparagine) within a porous zirconium-based trimesate metal-organic framework (MOF), namely, MOF-808. Applying this strategy, we were able to produce a pore environment spatially decorated with multiple functional groups usually found in commercial chelator molecules. The chemical stability of the amino acid molecules installed by the solvent-assisted ligand exchange has been studied to delimitate the applicability window of these materials. The adsorption affinity of MOF-808@(amino)acids in static and column-bed configurations can be fine-tuned as a function of the amino acid residues installed in the framework. MOF-808(amino)acid columns can be applied efficiently both for water remediation of heavy metals and for the separation of metal ions with different acidities. For instance, the initial trends for the dispersion of rare-earth elements have been identified. Electron paramagnetic resonance and inelastic neutron scattering spectroscopy reveal that MOF-808@(amino)acids stabilize metal centers as isolated and clustered species in a coordination fashion that involves both the amine and thiol functionals and that affects the vibrational freedom of some of the chemical groups of the amino acid molecules. The metal-ion stabilization within amino acid-decorated MOFs opens the avenue for application for pseudo biocatalysis purposes in the near future.Fil: Valverde, Ainara. Universidad del País Vasco; EspañaFil: Tovar, Gabriel I.. Universidad de Buenos Aires; ArgentinaFil: Rio López, Natalia A.. No especifíca;Fil: Torres, Dimas Ignacio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaFil: Rosales, Maibelin. Advanced Mining Technology Center; ChileFil: Wuttke, Stefan. No especifíca;Fil: Fidalgo Marijuan, Arkaitz. No especifíca;Fil: Porro, José María. No especifíca;Fil: Jiménez Ruiz, Mónica. Institut Laue Langevin; FranciaFil: García Sakai, Victoria. No especifíca;Fil: García, Andreina. No especifíca;Fil: Laza, José Manuel. Universidad del País Vasco; EspañaFil: Vilas Vilela, José Luis. Universidad del País Vasco; EspañaFil: Lezama, Luis. Universidad del País Vasco; EspañaFil: Arriortua, María I.. Universidad del País Vasco; EspañaFil: Copello, Guillermo Javier. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Houssay. Instituto de Química y Metabolismo del Fármaco. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Instituto de Química y Metabolismo del Fármaco; ArgentinaFil: Fernández De Luis, Roberto. No especifíca