A general and versatile procedure for coating of hydrophobic nanocrystals with a thin silica layer enabling facile biofunctionalization and dye incorporation

Abstract

Here we report a method for coating of hydrophobic nanocrystals (NCs) with a thin silica layer. By using this approach 11 nm NaGdF₄ NCs were coated with a mesoporous silica shell thinner than 20 nm resulting in highly monodisperse core–shell nanocomposite particles smaller than 50 nm. The synthetic protocol used here is based on the two-phase system that ensures high repeatability of the nanoparticle morphology and can be conveniently adapted for large-scale production. The use of an organic solvent as a diluent for tetraethoxysilane allows us to control not only the thickness, but also the porosity of the uniform silica shell. This procedure can be applied for coating NCs of various sizes and can be generalized to encapsulate other nanocrystals, e.g. semi-conductor quantum dots, into silica spheres. Furthermore, it allows facile surface modification with –NH₂ groups that can be then used to conjugate biomolecules to the nanoparticle surface, as well as straightforward incorporation of various organic molecules (e.g. dyes or drugs) into the silica shell during its growth. To demonstrate potential applications up-converting NaGd_0.80Yb_0.18Er_0.02F₄ NCs were used as cores and zinc phthalocyanine was incorporated into the silica shell as a photosensitizer. Under irradiation with a 980 nm laser diode efficient generation of singlet oxygen was observed indicating that such nanocomposite particles have the capability to be used for photodynamic therapy.