Thermally driven self-healing PEDOT conductive films relying on reversible and multiple Diels–Alder interaction

Thermally healing capability of cracks and defects is important and urgent for the safe operation and life extending of electric materials and devices. Here, by the combination of thermally driven reversible Diels–Alder (DA) interaction and in-situ chemical oxidative polymerization of 3,4-ethylenedioxythiophene (EDOT), a series of intrinsically conductive poly(3,4-ethylenedioxythiophene) (PEDOT)/DA composites possess intrinsically self-healing property under low-temperature (reverse DA reaction at 100°C; DA crosslinking at 60°C) stimulus were achieved. The crosslinking DA bonding reactions are multiple from the co-existence of pre-synthesized macromolecular polyurethane attached DA units (PU-DA) and 2,4-hexadiyne-1,6-diol (DADOL) in the films. PU-DA involved in the polymerization process of EDOT to endow PEDOT with outstanding solution-processability, uniform film making, and structural self-healing capability, while DADOL was added to enhance the cross bonding between polymer chains. This work will accelerate the research and application development of intrinsically self-healing conducting polymers for commercial capacitors, antistatic coatings, implantable, printable electronics, and so on.