Publication: Auto-ensamblaje supramolecular de nanopartículas plasmódicas de oro
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2017-11-28
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Universidad Complutense de Madrid
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Abstract
La ciencia de nanomateriales, conocida como nanociencia, ha emergido como un área de investigación muy prolífica en las últimas dos décadas, permitiendo avances importantes en el desarrollo y manipulación de materiales en la nanoescala (1−100 × 10-9 nm).1 En esta escala, los materiales presentan propiedades químico-físicas inusuales que difieren significativamente de sus correspondientes propiedades en la escala micro y macroscópica, como es por ejemplo la excitación de los plasmones de superficie. Esencialmente, este comportamiento dependiente del tamaño puede ser explicado a través de fenómenos físicos complejos entre los cuales caben destacar efectos cuánticos, propiedades magnéticas o electrónicas de superficie.2 De acuerdo a estas funcionalidades, e inspirados por los fenómenos que transcurren en la naturaleza, los químicos se han enfocado en el diseño de nanomateriales auto-ensamblados con la idea de mejorar o incluso generar nuevas propiedades (metamateriales). Para lograr tales objetivos, estas investigaciones se han centrado fundamentalmente en diseñar sistemas de síntesis basados en nanomateriales híbridos orgánicos e inorgánicos. Como ejemplo relevante de esta evolución, la nanoplasmónica ha surgido como un área importante de la nanociencia, dónde las propiedades ópticas de las nanopartículas plasmónicas metálicas pueden ser combinadas con componentes moleculares, obteniéndose materiales híbridos con nuevas propiedades y una amplia aplicabilidad...
Our contribution to tackle the transfer of information encoded by molecular subcomponents has focused on the design of a thiolated π-conjugated linking unit, whose cooperative self-assembly can be efficiently transferred from the molecular to gold nanoparticles (AuNPs). The transfer of supramolecular information by the linking π-system can take place when a cooperative nucleation-elongation mechanism is operative. We report an artificial AuNP–discrete π-conjugated molecule hybrid system that mimics the mechanical behavior of biological membranes and is able to self-assemble into colloidal gold nanoclusters or membranes in a controlled and reversible fashion by changing the concentration or the mechanical force (pressure) applied. This has been achieved by rational design of a small π-conjugated thiolated molecule that controls, to a great extent, the hierarchy levels involved in AuNP clustering by enabling reversible, cooperative non-covalent (π–π, solvophobic, and hydrogen bonding) interactions. The use of a thiol-functionalized nonionic surfactant to stabilize spherical gold nanoparticles in water induces the spontaneous formation of polyrotaxanes at the nanoparticle surface in the presence of the macrocycle α-cyclodextrin. Under controlled drying conditions the self-assembly between the surface supramolecules provides large and homogenous supercrystals with hexagonal close packing of nanoparticles. Once formed, the self-assembled supercrystals can be fully redispersable in water...
Our contribution to tackle the transfer of information encoded by molecular subcomponents has focused on the design of a thiolated π-conjugated linking unit, whose cooperative self-assembly can be efficiently transferred from the molecular to gold nanoparticles (AuNPs). The transfer of supramolecular information by the linking π-system can take place when a cooperative nucleation-elongation mechanism is operative. We report an artificial AuNP–discrete π-conjugated molecule hybrid system that mimics the mechanical behavior of biological membranes and is able to self-assemble into colloidal gold nanoclusters or membranes in a controlled and reversible fashion by changing the concentration or the mechanical force (pressure) applied. This has been achieved by rational design of a small π-conjugated thiolated molecule that controls, to a great extent, the hierarchy levels involved in AuNP clustering by enabling reversible, cooperative non-covalent (π–π, solvophobic, and hydrogen bonding) interactions. The use of a thiol-functionalized nonionic surfactant to stabilize spherical gold nanoparticles in water induces the spontaneous formation of polyrotaxanes at the nanoparticle surface in the presence of the macrocycle α-cyclodextrin. Under controlled drying conditions the self-assembly between the surface supramolecules provides large and homogenous supercrystals with hexagonal close packing of nanoparticles. Once formed, the self-assembled supercrystals can be fully redispersable in water...
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Tesis inédita de la Universidad Complutense de Madrid, Facultad de Ciencias Químicas, Departamento de Química Física I, leída el 31-03-2017