Tuning Water-Resistant Networks in Mussel-Inspired Hydrogels for Robust Wet Tissue and Bioelectronic Adhesion

Hydrogels with robust wet adhesion are desirable for applications in aqueous environments. Wet adhesion arising from synergy between hydrophobic and catechol components in mussel foot proteins has been highlighted. However, optimizing hydrogels with multiple components is challenging because of their complex structure–property relationships. Herein, high-throughput screening of a series of hydrophobic alkyl monomers and adhesive catechol derivatives was used to systematically develop wet adhesive hydrogels. Short alkyl chains promote wet adhesion by repelling water at the adhesive interface, whereas long alkyl chains form strong hydrophobic interactions inside the hydrogel network that impede or dissipate energy for wet adhesion. The optimized wet adhesive hydrogel, containing short alkyl chain, was applied for rapid hemostasis and wound healing because of the synergistic effect of catechol and alkyl groups and its immunomodulation ability, which is revealed through a transcriptomic analysis. Conductive nanocomponents were incorporated into the optimized hydrogel to produce a wearable device, which was used for continuous monitoring human electrocardiogram (ECG) during swimming, and in situ epicardial ECG on a porcine living and beating heart. This study demonstrated an efficient and generalized molecular design strategy for multifunctional wet adhesive hydrogels.