Highly Robust and Environment-Tolerant Conducting Polymer Organohydrogels through the Synergy of Salting-Out Effect and In Situ Polymerization

Conducting polymer hydrogels with high mechanical toughness and environmental stability are highly desirable for the long-term operation of flexible electronic devices. However, most existing conducting polymer hydrogels experience poor mechanical performance and limited environmental tolerance, severely restricting their practical applicability. Herein, we present a facile yet versatile strategy for fabricating conducting polymer organohydrogels with high mechanical robustness, good electrical conductivity, and excellent environmental stability, achieved through a synergistic salting-out effect coupled with in situ polymerization. Specifically, Fe2(SO4)3 is employed as a multifunctional oxidant to simultaneously induce the aggregation of poly(vinyl alcohol) (PVA) chains and initiate the in situ polymerization of pyrrole (Py) into a polypyrrole (PPy) conductive network within a dimethyl sulfoxide/water (DMSO/H2O) binary solvent system. The resultant conducting polymer organohydrogel achieves fracture stress (7.93 ± 0.56 MPa), ultrahigh toughness (22.64 ± 1.00 MJ/m3), and good conductivity up to 0.37 S/m. Additionally, the introduction of DMSO/H2O binary solvent endows the organohydrogel with extreme environmental stability (−45 to 65 °C). This robust organohydrogel can be readily engineered into highly sensitive, stable, and durable wearable sensors that maintain reliable performance even under extreme environmental conditions, enabling precise detection of a wide range of human motions. Importantly, the proposed strategy is generalizable to other polymer systems, offering a promising and scalable route for the design of high-performance conducting polymer gels for next-generation flexible and stretchable electronic applications.