In this work, we
unravel the role of surface properties of colloidal
particles on the formation of supraparticles (clusters of colloidal
particles) in a colloidal Ouzo droplet. Self-lubricating colloidal
Ouzo droplets are an efficient and simple approach to form supraparticles,
overcoming the challenge of the coffee stain effect
in situ
. Supraparticles are an efficient route to high-performance materials
in various fields, from catalysis to carriers for therapeutics. Yet,
the role of the surface of colloidal particles in the formation of
supraparticles using Ouzo droplets remains unknown. Therefore, we
used silica particles as a model system and compared sterically stabilized
versus electrostatically stabilized silica particles—positively
and negatively charged. Additionally, we studied the effect of hydration.
Hydrated negatively charged silica particles and sterically stabilized
silica particles form supraparticles. Conversely, dehydrated negatively
charged silica particles and positively charged amine-coated particles
form flat film-like deposits. Notably, the assembly process is different
for all the four types of particles. The surface modifications alter
(a) the contact line motion of the Ouzo droplet and (b) the particle–oil
and particle–substrate interactions. These alterations modify
the particle accumulation at the various interfaces, which ultimately
determines the shape of the final deposit. Thus, by modulating the
surface properties of the colloidal particles, we can tune the shape
of the final deposit, from a spheroidal supraparticle to a flat deposit.
In the future, this approach can be used to tailor the supraparticles
for applications such as optics and catalysis, where the shape affects
the functionality.