Beyond Chemistry: Tailoring Stiffness and Microarchitecture to Engineer Highly Sensitive Biphasic Elastomeric Piezoresistive Sensors

[Image: see text] Carbon-based nanoparticles and conductive polymers are two classes of materials widely used in the production of three-dimensional (3D) piezoresistive sensors. One conductive polymer, poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) has excellent stability and conductivity yet is limited in its application as a sensor, often existing upon a base, limiting its performance and potential. Despite much progress in the field of materials chemistry and polymer synthesis, one aspect we consider worthy of exploration is the impact that microstructure and stiffness may have on the sensitivity of 3D sensors. In this study, we report a strategy for fabricating biphasic electroactive sponges (EAS) that combine 3D porous PEDOT:PSS scaffolds possessing either an isotropic or anisotropic microarchitecture, infused with insulating elastomeric fillers of varying stiffness. When characterizing the electromechanical behavior of these EAS, a higher stiffness yields a higher strain gauge factor, with values as high as 387 for an isotropic microarchitecture infused with a stiff elastomer. The approach we describe is cost-effective and extremely versatile, by which one can fabricate piezoresistive sensors with adaptable sensitivity ranges and excellent high strain gauge factor with the underlying microarchitecture and insulant stiffness dictating this performance.