Mechanical robustness of monolayer nanoparticle-covered liquid marbles

Powder-derived liquid marbles (LMs) are versatile nonwetting systems but are confronted with many limitations in application, as their surface particles are usually large and agglomerated. Recently, sol-gel film-derived LMs have come on the scene that are termed monolayer nanoparticle-covered (mNPc) LMs based on their unique characteristics, revealing great application potential but also generating many questions. Here, mechanical robustness, a very important yet to be addressed property, of mNPc LMs was systematically studied. Rolling, pendant contact, and compression experiments were designed using bare and coated glasses with water contact angles (WCAs) ranging from 23° to 157°. With rupture as a quality criteria, the mechanical robustness of mNPc LMs enhanced with the hydrophobicity of solid surfaces that exerted pressure on them, but maintained much weaker than typical powder LMs until the solid surface was superhydrophobic. In particular, when contacting hydrophilic surfaces of WCAs ≤53°, an mNPc LM did not have the capacity for nonwetting and ruptured immediately, even if the pressure approached zero. This was distinct from powder LMs and indicated that a particle shell as thin as ∼20 nm could not prevent intermolecular attractions between the internal liquid and external solid surface. An interface scenario consisting of solid surface microroughness was proposed to address this issue. On the other hand, mNPc LMs remained unruptured on superhydrophobic surfaces but presented degraded elasticity under extreme compression. Uncovering these properties could be of much help for developments of mNPc LMs and their counterparts, the mNPc liquid plasticines.