Printable, Self-Healing and Recyclable PEDOT:PSS/Polyurethane Composites for Durable Bioelectronics

Abstract

The development of self-healing conductors that are simultaneously printable, recyclable, and resilient to severe mechanical damage remains a key challenge for flexible bioelectronic technologies. Here, we report a multifunctional composite based on poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) blended with a custom-designed polyurethane (PU) incorporating dynamic disulfide bonds and hydrogen-bonding motifs. This materials design enables autonomous room-temperature healing from scratches, cuts, and punctures, without external stimuli, while preserving mechanical integrity and electrical continuity. The composite is processable from green solvents and can be spin-coated or printed into uniform, transparent, and highly stretchable films, as well as free-standing membranes transferable to diverse substrates. Optimized PEDOT:PSS/PU/Gly films exhibit a functional conductivity (~15 S cm⁻¹), high stretchability (>650 %), strong self-adhesion, and stable performance under repeated deformation. Importantly, the material supports both mechanical reuse and chemical recycling over at least 15 cycles, retaining more than 90 % of its mechanical strength and fully recovering its electrical conductivity. Mechanistic investigations reveal that reversible disulfide exchange and hydrogen bond reformation govern rapid network reorganization and efficient self-repair. Printed electronic tattoos and free-standing electrodes fabricated from this composite deliver low-impedance and high-fidelity electrocardiogram (ECG) recordings. Together, these results establish a sustainable and versatile materials platform that advances self-healing conductors beyond superficial damage, providing a practical pathway toward durable and recyclable bioelectronic materials and devices.