Highly Thermal-Wet Comfortable and Conformal Silk-Based Electrodes for On-Skin Sensors with Sweat Tolerance

Noninvasive and seamless interfacing between the sensors and human skin is highly desired for wearable healthcare. Thin-film-based soft and stretchable sensors can to some extent form conformal contact with skin even under dynamic movements for high-fidelity signals acquisition. However, sweat accumulation underneath these sensors for long-term monitoring would compromise the thermal-wet comfort, electrode adherence to the skin, and signal fidelity. Here, we report the fabrication of a highly thermal-wet comfortable and conformal silk-based electrode, which can be used for on-skin electrophysiological measurement under sweaty conditions. It is realized through incorporating conducting polymers poly(3,4-ethylenedioxythiophene): polystyrenesulfonate (PEDOT:PSS) into glycerol-plasticized silk fiber mats. Glycerol plays the role of tuning the mechanical properties of silk fiber mats and enhancing the conductivity of PEDOT:PSS. Our silk-based electrodes show high stretchability (>250%), low thermal insulation (∼0.13 °C·m²·W^-1), low evaporative resistance (∼23 Pa·m²·W^-1, 10 times lower than ∼1.3 mm thick commercial gel electrodes), and high water-vapor transmission rate (∼117 g·m^-2·h^-1 under sweaty conditions, 2 times higher than skin water loss). These features enable a better electrocardiography signal quality than that of commercial gel electrodes without disturbing the heat dissipation during sweat evaporation and provide possibilities for textile integration to monitor the muscle activities under large deformation. Our glycerol-plasticized silk-based electrodes possessing superior physiological comfortability may further engage progress in on-skin electronics with sweat tolerance.