Implantable electronics have recently been attracting attention because of the promising advances in personalized healthcare. They can be used to diagnose and treat chronic diseases by monitoring and applying bioelectrical signals to various organs. However, there are challenges regarding the rigidity and hardness of typical electronic devices that can trigger inflammatory reactions in tissues. In an effort to improve the physicochemical properties of conventional implantable electronics, soft hydrogel-based platforms have emerged as components of implantable electronics. It is important that they meet functional criteria, such as stretchability, biocompatibility, and self-healing. Herein, plant-inspired conductive alginate hydrogels composed of “boronic acid modified alginate” and “oligomerized epigallocatechin gallate,” which are extracted from plant compounds, are proposed. The conductive hydrogels show great stretchability up to 500% and self-healing properties because of the boronic acid-cis-diol dynamic covalent bonds. In addition, as a simple strategy to increase the electrical conductivity of the hydrogels, ionically crosslinked shells with cations (e.g., sodium) were generated on the hydrogel under physiological salt conditions. This decreased the resistance of the conductive hydrogel down to 900 ohm without trading off the original properties of stretchability and self-healing. The hydrogels were used for “electrophysiological bridging” to transfer electromyographic signals in an ex vivo muscle defect model, showing a great bridging effect comparable to that of a muscle-to-muscle contact model. The use of plant-inspired ionically conductive hydrogels is a promising strategy for designing implantable and self-healable bioelectronics.

The development of flexible and stretchable materials has led to advances in implantable bio-integrated electronic devices that can sense physiological signals or deliver electrical stimulation to various organs in the human body. Such devices are particularly useful for neural interfacing systems that monitor neurodegenerative diseases such as Parkinson’s disease or epilepsy in real time. However, coupling current brain-interfacing devices with magnetic resonance imaging (MRI) remains a practical challenge due to resonance frequency variations from inorganic metal-based devices. Thus, organic conductive materials, such as poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS), have recently been considered as promising candidates. Nonetheless, their conformability on curvilinear tissues remains questionable. In this study, we developed an injectable conductive hydrogel (ICH) composed of tyramine-conjugated hyaluronic acid (HATYR) and PEDOT:PSS for MRI-compatible brain-interfacing electrodes. Our ICH produced low impedance around 5 kΩ even under 10 Hz, demonstrating high confidence volumetric capacitance. Due to HATYR’s biocompatibility, histological and cytotoxicity assays showed almost no inflammation and toxicity, respectively; in addition, ICH was able to degrade into 40% of its original volume within four weeks in vivo. An electrocorticogram (ECoG) array was also patternable by syringe injections of ICH on a stretchable and flexible elastomeric substrate layer that conformed to curvy brain tissues and successfully recorded ECoG signals under light stimulation. Furthermore, MRI imaging of implanted devices did not show any artifacts, indicating the potential of the MRI-compatible hydrogel electrodes for advanced ECoG arrays. This study provides a promising solution for MRI-compatible neural electrodes, enabling the advancement of chronic neural interfacing systems for monitoring neurodegenerative diseases.

Hydrogels that have a capability to provide mechanical modulus matching between time-dynamic curvilinear tissues and bioelectronic devices have been considered tissue-interfacing ionic materials for stably sensing physiological signals and delivering feedback actuation in skin-inspired healthcare systems. These functionalities are totally different from those of elastomers with low ionic conductivity and higher stiffness. Despite such remarkable progress, their low conductivity remains limited in transporting electrical charges to internal or external terminals without undesired information loss, potentially leading to an unstable biotic–abiotic interfaces in the wearable electronics. Here, we report a soft stretchable conductive hydrogel composite consisting of alginate, carboxymethyl cellulose, polyacrylamide, and silver flakes. This composite was fabricated via sol–gel transition. In particular, the phase stability and low dynamic modulus rates of the conductive hydrogel were confirmed through an oscillatory rheological characterization. In addition, our conductive hydrogel showed maximal tensile strain (≈400%), a low deformations of cyclic loading (over 100 times), low resistance (≈8.4 Ω), and a high gauge factor (≈241). These stable electrical and mechanical properties allowed our composite hydrogel to fully support the operation of a light-emitting diode demonstration under mechanical deformation. Based on such durable performance, we successfully measured the electromyogram signals without electrical malfunction even in various motions.

Soft bioelectronic systems with a unique mechanical property, namely modulus matching between human skin (or tissue) and the device, have gained widespread attention. This is because of their closed-loop strain-insensitive electrical performance ranging from application in the long-term stable measurements of physiological signals and feedback modulation to human skin (or organs). Various materials and integration/fabrication strategies such as buckled, rigid islands, and wavy designs addressed for soft bioelectronic systems require complex device fabrication with time-consuming packaging and integration processes. In this study, we developed a soft bio-integrated multifunctional device (SBMD) fabricated through the simple thermal evaporation and transfer processes. The intrinsically stretchable Au–SEBS film composed of thermally evaporated gold (Au) nanomembranes and an elastomeric substrate was applied to various functional modules that are capable of sensing the strain (up to ~300%), temperature (with a thermal sensitivity of ~0.6 Ω/°C), chemicals (at a concentration of NaCl of ~0.5 wt%), and even electrophysiological cardiac/muscle signals and showing thermal actuations (80 °C at 9 V). Specifically, such multifunctions of the SBMD were stably performed even on skin. Thus, we believe the SBMD would be a promising candidate for realizing soft bioelectronic systems.