Adhesion between Hydrophobic Elastomer and Hydrogel through Hydrophilic Modification and Interfacial Segregation

Recent progress in the printing of soft materials has made it possible to fabricate soft stretchable devices for a range of engineering applications. These devices tend to be heterogeneous systems, and their reliability depends to a large extent on the integrity of the interfaces between the various materials in the system. Previous studies on the printing of hydrogels have highlighted the need to investigate the adhesion between extrusion printable dielectric elastomers and hydrogels. Here we consider polydimethylsiloxane (PDMS) and a polyacrylamide hydrogel that contains lithium chloride and a nonionic rheological modifier. We show that the adhesion between oxygen plasma-treated PDMS and the hydrogel increases with time to reach a stable value of 15 J m^-2 after ∼6 days. During that time, the contact angle of water on the PDMS interface remains constant at ∼30°, suggesting that hydrophobic recovery of plasma-treated PDMS is suppressed by the presence of the hydrogel. It is further observed that a thin viscous layer develops at the interface between PDMS and hydrogel, which results in energy dissipation upon debonding and which allows full recovery of the adhesion after debonding and rejoining. This viscous layer develops only in the presence of the rheological modifier in the hydrogel and the hydrophilic surface treatment of the PDMS.