thesis

Surface functionalisation techniques for colloidal inorganic nanocrystals

Abstract

Colloidally-stable inorganic nanocrystals have a wide range of envisaged applications in biological environments. To reach their potential, the nanocrystals need to be stable in aqueous environments and have pendant functionality available for attachment of biomolecules. In this thesis, new methods for the transfer of nanocrystals from organic to aqueous media are developed and the interaction of aqueous stabilised particles with serum proteins is investigated. In Chapter 3, a new method for the synthesis of a thin silica layer upon the surface of nanocrystals is demonstrated. The method uses the hydrophobic interaction between an amphiphilic polymer and nanocrystal ligands to provide a foundation for growth of a silica layer. The coated nanocrystals are characterised using a wide range of techniques confirming that the presence and location of the silica shell. In Chapter 4, custom-synthesised amphiphilic polymers for water transfer and functionalisation of nanocrystals are synthesised, characterised and tested. Commercially-available polymers used for this purpose are examined, leading to a rationale for custom-design. Partial water transfers were achieved using activated ester copolymers with styrene but no transfers were achieved the octadecylacrylate copolymers. Poly(ethylene glycol) containing monomers were also used but yielded no transfers. This suggests that behaviour of the polymer during the coating procedure is intimately linked to the structure of the polymer. In Chapter 5, small-angle neutron scattering is used to elucidate structural information for the protein corona formed on nanocrystals and silica nanoparticles. Information on the packing of ligands on colloidal nanocrystals without a amphiphilic polymer coating was determined. The fitting of the protein corona upon silica nanoparticles was explored using core-shell form factors but was hampered by complexities within the scattering profiles which were not accounted for using simple form factors

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