Core–shell
structures containing active materials can be
fabricated using almost infinite reactant combinations. A mechanism
to describe their formation is therefore useful. In this work, nanoscale
all-silica shell capsules with an aqueous core were fabricated by
the HCl-catalyzed condensation of tetraethyl orthosilicate (TEOS),
using Pickering emulsion templates. Pickering emulsions were fabricated
using modified commercial silica (LUDOX TMA) nanoparticles as stabilizers.
By following the reaction over a 24 h period, a general mechanism
for their formation is suggested. The interfacial activity of the
Pickering emulsifiers heavily influenced the final capsule products.
Fully stable Pickering emulsion templates with interfacially active
particles allowed a highly stable sub-micrometer (500–600 nm)
core–shell structure to form. Unstable Pickering emulsions,
i.e., where interfacially inactive silica nanoparticles do not adsorb
effectively to the interface and produce only partially stable emulsion
droplets, resulted in capsule diameter increasing markedly (1+ μm).
Scanning electron microscope (SEM) and transmission electron microscope
(TEM) measurements revealed the layered silica “colloidosome”
structure: a thin yet robust inner silica shell with modified silica
nanoparticles anchored to the outer interface. Varying the composition
of emulsion phases also affected the size of capsule products, allowing
size tuning of the capsules. Silica capsules are promising protective
nanocarriers for hydrophilic active materials in applications such
as heat storage, sensors, and drug delivery.