Degradable and Fully Recyclable Dynamic Thermoset Elastomer for 3D-Printed Wearable Electronics

Wearable electronics have become an important part of daily lives. However, its rapid development results in the problem of electronic waste (e-waste). Consequently, recyclable materials suitable for wearable electronics are highly sought after. In this study, a conductive recyclable composite (PFBC) is designed based on a dynamic covalently cross-linked elastomer and hierarchical hybrid nanofillers. The PFBC shows excellent wide-ranging properties including processability, elasticity, conductivity, and stability, which are superior to previous materials used for recyclable electronics, and exhibits outstanding mechanical properties and environmental tolerance including high temperature, high humidity, brine, and ethanol owing to its covalent cross-linking. Reversible dissociation of Diels–Alder networks allows for convenient processing and recycling. After three recycles, the toughness of the PFBC remained at 10.1 MJ m⁻³, which is conspicuous among the reported recyclable electronic materials. Three types of PFBC-based wearable electronics including a triboelectric nanogenerator, a capacitive pressure sensor, and a flexible keyboard, are successfully 3D printed with excellent performance. The PFBC possessed both recyclability and degradability, the combination of which provides a new way to reduce e-waste. This is the first work to recycle electronics using direct 3D printing and presents promising new design principles and materials for wearable electronics.