Dynamically crosslinked polyethylene-like materials with reversible self-reporting properties†

In alignment with circular economy principles, we have developed a reprocessable, self-reporting thermoset based on polyethylene. The self-reporting feature is achieved using a mechanophore as the crosslinking agent, which reversibly responds to applied stress while being quenched by thermal stimuli. This same heat trigger also facilitates the material's self-healing capability, ensuring efficient recovery and reusability. The chosen mechanophore is rhodamine, a widely recognized fluorescent dye known for its excellent stability, high absorption coefficient, and long-wavelength absorption and emission. For the covalent reversible bonds, we employ silylether exchange chemistry, as it enables the incorporation of crosslinker units without necessitating modifications to the polymer backbone.