Evaporation driven buckling of a drop laden with graphene oxide nanosheets†

The time-dependent shape of an evaporating spherical water drop containing graphene oxide (GO) nanosheets is measured for varying solid concentration, humidity level, and pH. The drop is sitting on a superhydrophobic surface, depinned from it. Three different stages of evaporation are identified: isotropic retraction of the drop interface, buckling of the shell of particles accumulated at the fluid interface, and shrinking of the buckled shell at constant shell shape. Marked differences between acidic and basic drops are reported. It is argued that this feature is caused by the pH-dependent interfacial adsorption of the GO particles. For intermediate values of GO concentration, dried capsules with remarkably repeatable folding patterns could be obtained, whose mode numbers are compatible with those predicted by an inertialess, linear elastic shell model. When redispersed in water, the dried capsules from acidic drops retain their shape better than capsules from basic drops.