Phase separation technology has attracted extensive scientific
interest because of its intriguing structure changes during the phase
separation process. Phase separation inside emulsion droplets in continuous
surroundings has been well studied in recent years. Many investigations
have also been conducted to study the droplet phase separation phenomena
in noncontinuous surroundings. However, studies on the phase separation
phenomena and the spreading behavior of suspended droplets at the
air–liquid interface were rarely reported. In this study, PEGDA-glycerol
suspended Janus droplets with a patchy structure were produced by
utilizing solvent evaporation-induced droplet phase separation at
the air–liquid interface. By altering the glycerol/PEGDA volume
ratio, the initial proportion of ethanol, and the concentration of
surfactants, suspended droplets with different morphologies can be
achieved, which include filbert-shaped droplets (FSDs), half lotus
seedpod single-phase Janus droplets (HLSDs), lotus seedpod single-phase
Janus droplets (LSDs), lotus seedpod-shaped droplets (LSSDs), multiple-bulge
droplets (MBDs), and half gourd-shaped droplets (HGSDs). A patchy
structure was generated at the air–droplet interface, which
was attributed to the Marangoni stresses induced by nonuniform evaporation.
Furthermore, a modified spreading coefficient theory was constructed
and verified to illustrate the phase separation at the air–droplet
interface, which was the first research to predict the phase separation
phenomena at the air–liquid interface via spreading coefficients
theory. Moreover, we studied the factors that led to the droplets
being able to float by designing the combined parameters, including
three interfacial tensions and the equilibrium contact angles. Therefore,
a simple and versatile strategy for creating suspended Janus droplets
has been developed for the first time, which holds significant potential
in a variety of applications for material synthesis, such as the electrospinning
solution behavior when sprayed from the nozzle into the air.