Highly stretchable, self-adhesive, biocompatible, conductive hydrogels as fully polymeric strain sensors

Abstract

Development of highly stretchable and sensitive soft strain sensors is of great importance for broad applications in artificial intelligence, wearable devices, and soft robotics, but it proved to be a profound challenge to integrate the two seemingly opposite properties of high stretchability and sensitivity into a single material. Herein, we designed and synthesized a new fully polymeric conductive hydrogel with an interpenetrating polymer network (IPN) structure made of conductive PEDOT:PSS polymers and zwitterionic poly(HEAA-co-SBAA) polymers to achieve a combination of high mechanical, biocompatible, and sensing properties. The presence of hydrogen bonding, electrostatic interactions, and IPN structures enabled poly(HEAA-co-SBAA)/PEDOT:PSS hydrogels to achieve an ultra-high stretchability of 4000–5000%, a tensile strength of ∼0.5 MPa, a rapid mechanical recovery of 70–80% within 5 min, fast self-healing in 3 min, and a strong surface adhesion of ∼1700 J m⁻² on different hard and soft substrates. Moreover, the integration of zwitterionic polySBAA and conductive PEDOT:PSS facilitated charge transfer via optimal conductive pathways. Due to the unique combination of superior stretchable, self-adhesive, and conductive properties, the hydrogels were further designed into strain sensors with high sensing stability and robustness for rapidly and accurately detecting subtle strain- and pressure-induced deformation and human motions. Moreover, an in-house mechanosensing platform provides a new tool to real-time explore the changes and relationship between network structures, tensile stress, and electronic resistance. This new fully polymeric hydrogel strain sensor, without any conductive fillers, holds great promise for broad human-machine interface applications.