Hydrogel-Integrated Multimodal Response as a Wearable and Implantable Bidirectional Interface for Biosensor and Therapeutic Electrostimulation

A hydrogel that fuses long-term biologic integration, multimodal responsiveness, and therapeutic functions has received increasing interest as a wearable and implantable sensor but still faces great challenges as an all-in-one sensor by itself. Multiple bonding with stimuli response in a biocompatible hydrogel lights up the field of soft hydrogel interfaces suitable for both wearable and implantable applications. Given that, we proposed a strategy of combining chemical cross-linking and stimuli-responsive physical interactions to construct a biocompatible multifunctional hydrogel. In this hydrogel system, ureidopyrimidinone/tyramine (Upy/Tyr) difunctionalization of gelatin provides abundant dynamic physical interactions and stable covalent cross-linking; meanwhile, Tyr-doped poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) acts as a conductive filler to establish electrical percolation networks through enzymatic chemical cross-linking. Thus, the hydrogel is characterized with improved conductivity, conformal biointegration features (i.e., high stretchability, rapid self-healing, and excellent tissue adhesion), and multistimuli-responsive conductivity (i.e., temperature and urea). On the basis of these excellent performances, the prepared multifunctional hydrogel enables multimodal wearable sensing integration that can simultaneously track both physicochemical and electrophysiological attributes (i.e., motion, temperature, and urea), providing a more comprehensive monitoring of human health than current wearable monitors. In addition, the electroactive hydrogel here can serve as a bidirectional neural interface for both neural recording and therapeutic electrostimulation, bringing more opportunities for nonsurgical diagnosis and treatment of diseases.