Chemically Coupled Interfacial Adhesion in Multimaterial Printing of Hydrogels and Elastomers

Functional devices that use hydrogels as ionic conductors and elastomers as dielectrics have the advantage of being soft, stretchable, transparent, and biocompatible, making them ideal for biomedical applications. These devices are typically fabricated by manual assembly. Techniques for the manufacturing of soft materials have generally not looked at integrating multiple dissimilar materials. Silane coupling agents have recently shown promise for creating strong bonds between hydrogels and elastomers but have yet to be used in the extrusion printing of complex devices that integrate both hydrogels and elastomers. Here, we demonstrate the viability of silane coupling agents in a system with the rheology and functional composition necessary for three-dimensional (3D) extrusion printing of hydrogel-elastomer materials, specifically polyacrylamide (PAAm) hydrogel and poly(dimethylsiloxane) (PDMS) hydrophobic elastomer. By introducing a charge-neutral surfactant in the PDMS and adjusting silane concentrations in the PAAm, cast material samples demonstrate strong adhesion. We were also able to achieve an interfacial toughness of up to Γ = 193 ± 6.3 J/m² for a fully extrusion printed PAAm hydrogel-on-PDMS bilayer. This result demonstrates that an integration strategy based on silane coupling agents makes it possible for extrusion printing of a wide variety of hydrogel and silicone elastomers.