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.