Conductive hydrogels are a promising class of materials to design bioelectronics for new technological interfaces with human body, which are required to work for a long-term or under extreme environment. Traditional hydrogels are limited in short-term usage under room temperature, as it is difficult to retain water under cold or hot environment. Inspired by the antifreezing/antiheating behaviors from nature, and based on mussel chemistry, an adhesive and conductive hydrogel is developed with long-lasting moisture lock-in capability and extreme temperature tolerance, which is formed in a binary-solvent system composed of water and glycerol. Polydopamine (PDA)-decorated carbon nanotubes (CNTs) are incorporated into the hydrogel, which assign conductivity to the hydrogel and serve as nanoreinforcements to enhance the mechanical properties of the hydrogel. The catechol groups on PDA and viscous glycerol endow the hydrogel with high tissue adhesiveness. Particularly, the hydrogel is thermal tolerant to maintain all the properties under extreme wide tempreature spectrum (−20 or 60 °C) or stored for a long term. In summary, this mussel-inspired hydrogel is a promising material for self-adhesive bioelectronics to detect biosignals in cold or hot environments, and also as a dressing to protect skin from injuries related to frostbites or burns.

Adhesive hydrogels are attractive biomaterials for various applications, such as electronic skin, wound dressing, and wearable devices. However, fabricating a hydrogel with both adequate adhesiveness and excellent mechanical properties remains a challenge. Inspired by the adhesion mechanism of mussels, we used a two-step process to develop an adhesive and tough polydopamine-clay-polyacrylamide (PDA-clay-PAM) hydrogel. Dopamine was intercalated into clay nanosheets and limitedly oxidized between the layers, resulting in PDA-intercalated clay nanosheets containing free catechol groups. Acrylamide monomers were then added and in situ polymerized to form the hydrogel. Unlike previous single-use adhesive hydrogels, our hydrogel showed repeatable and durable adhesiveness. It adhered directly on human skin without causing an inflammatory response and was easily removed without causing damage. The adhesiveness of this hydrogel was attributed to the presence of enough free catechol groups in the hydrogel, which were created by controlling the oxidation process of the PDA in the confined nanolayers of clay. This mimicked the adhesion mechanism of the mussels, which maintain a high concentration of catechol groups in the confined nanospace of their byssal plaque. The hydrogel also displayed superior toughness, which resulted from nanoreinforcement by clay and PDA-induced cooperative interactions with the hydrogel networks. Moreover, the hydrogel favored cell attachment and proliferation, owning to the high cell affinity of PDA. Rat full-thickness skin defect experiments demonstrated that the hydrogel was an excellent dressing. This free-standing, adhesive, tough, and biocompatible hydrogel may be more convenient for surgical applications than adhesives that involve in situ gelation and extra agents.

Adhesive hydrogels have gained popularity in biomedical applications, however, traditional adhesive hydrogels often exhibit short-term adhesiveness, poor mechanical properties and lack of antibacterial ability. Here, a plant-inspired adhesive hydrogel has been developed based on Ag-Lignin nanoparticles (NPs)triggered dynamic redox catechol chemistry. Ag-Lignin NPs construct the dynamic catechol redox system, which creates long-lasting reductive-oxidative environment inner hydrogel networks. This redox system, generating catechol groups continuously, endows the hydrogel with long-term and repeatable adhesiveness. Furthermore, Ag-Lignin NPs generate free radicals and trigger self-gelation of the hydrogel under ambient environment. This hydrogel presents high toughness for the existence of covalent and non-covalent interaction in the hydrogel networks. The hydrogel also possesses good cell affinity and high antibacterial activity due to the catechol groups and bactericidal ability of Ag-Lignin NPs. This study proposes a strategy to design tough and adhesive hydrogels based on dynamic plant catechol chemistry.

A graphene oxide conductive hydrogel is reported that simultaneously possesses high toughness, self-healability, and self-adhesiveness. Inspired by the adhesion behaviors of mussels, our conductive hydrogel shows self-adhesiveness on various surfaces and soft tissues. The hydrogel can be used as self-adhesive bioelectronics, such as electrical stimulators to regulate cell activity and implantable electrodes for recording in vivo signals.

An ideal hydrogel for biomedical engineering should mimic the intrinsic properties of natural tissue, especially high toughness and self-healing ability, in order to withstand cyclic loading and repair skin and muscle damage. In addition, excellent cell affinity and tissue adhesiveness enable integration with the surrounding tissue after implantation. Inspired by the natural mussel adhesive mechanism, we designed a polydopamine-polyacrylamide (PDA-PAM) single network hydrogel by preventing the overoxidation of dopamine to maintain enough free catechol groups in the hydrogel. Therefore, the hydrogel possesses super stretchability, high toughness, stimuli-free self-healing ability, cell affinity and tissue adhesiveness. More remarkably, the current hydrogel can repeatedly be adhered on/stripped from a variety of surfaces for many cycles without loss of adhesion strength. Furthermore, the hydrogel can serve as an excellent platform to host various nano-building blocks, in which multiple functionalities are integrated to achieve versatile potential applications, such as magnetic and electrical therapies.