Hydrogels consist of hydrophilic polymer networks dispersed in water. Many applications of hydrogels rely on their unique combination of solid-like mechanical behavior and water-like transport properties. If the temperature is lowered below 0 °C, however, hydrogels freeze and become rigid, brittle, and non-conductive. Here, a general class of hydrogels that do not freeze at temperatures far below 0 °C, while retaining high stretchability and fracture toughness, is demonstrated. These hydrogels are synthesized by adding a suitable amount of an ionic compound to the hydrogel. The present study focuses on tough polyacrylamide-alginate double network hydrogels equilibrated with aqueous solutions of calcium chloride. The resulting hydrogels can be cooled to temperatures as low as -57 °C without freezing. In this temperature range, the hydrogels can still be stretched more than four times their initial length and have a fracture toughness of 5000 J m . It is anticipated that this new class of hydrogels will prove useful in developing new applications operating under a broad range of environmental and atmospheric conditions.

A hydrogel–dielectric‐elastomer system, polyacrylamide and poly(dimethylsiloxane) (PDMS), is adapted for extrusion printing for integrated device fabrication. A lithium‐chloride‐containing hydrogel printing ink is developed and printed onto treated PDMS with no visible signs of delamination and geometrically scaling resistance under moderate uniaxial tension and fatigue. A variety of designs are demonstrated, including a resistive strain gauge and an ionic cable.

In vitro cell culture and animal models are the most heavily relied upon tools of the pharmaceutical industry. When these tools fail, the results are costly and have at times, proven deadly. One promising new tool to enhance preclinical development of drugs is Organs on Chips (OOCs), proposed as a clinically and physiologically relevant means of modeling health and disease. Bringing the patient from bedside to bench in this form requires that the design, build, and test of OOCs be founded in clinical observations and methods. By creating OOCs as models of the patient, the industry may be better positioned to evaluate medicinal therapeutics

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.

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.