Nanorecettori autoorganizzati per la rilevazione di metaboliti

Gold nanoparticles, or, more in general, metal nanoparticles functionalized with a monolayer of organic ligands, provide a straightforward way to implement and exploit cooperativity mechanisms between the functional groups present in attached ligands, which are kept in close proximity by the monolayer arrangement. A good variety of different species can be easily attached to the nanoparticle surface with different methods and interligand cooperation can be exploited, among the possible applications, for molecular recognition. In this way, monolayer protected metal nanoparticles ca be easily turned in self-organized supramolecular receptors.1,2 It is still difficult, however, to precisely design and control the recognition properties of the monolayers as these depend not only on the chemical structure of the species bound on the surface, but also on the ligands conformation and dynamics. In this work, new approaches to the design of the monolayers were investigated, introducing combinatorial and potentially automatable computer aided synthetic approaches, capable to predict and the properties of the nanoparticles and quickly prepare them. Pre-synthesized and pre-organized binding pockets were also used for the post-synthetic functionalization of gold nanoparticles. Novel nanoreceptors for the detection of biomedically relevant metabolites were developed, which offered several advantages with respect to the previous generation, such as an increased sensitivity and an extended concentration window for the analyte detection via NMR-chemosensing. A new hyperpolarization-based strategy to further enhance the sensitivity of this analytical technique was also conceived and explored.