Multicycling of Epoxy Thermoset Through a Two‐Step Strategy of Alcoholysis and Hydrolysis using a Self‐Separating Catalysis System

Plastic has now become a contradiction between civilization and pollution that human society has to resolve. The recycling of thermosetting plastics in waste plastics is a huge challenge since they are difficult to remold like thermoplastic plastics due to their high crosslinking density. Here, a new strategy was developed to achieve multicycling of anhydride-cured epoxy thermosets. The process consisted of mild and high-efficiency alcoholysis catalyzed by potassium phosphate/low-boiling alcohol system, and subsequent fast hydrolysis to obtain degradation products rich of carboxyl groups. The degradation products were reused as curing agent to prepare new anhydride-cured epoxy thermosets without sacrifice of high strength and stability. Moreover, the new epoxy thermosets could still be repeatedly recycled using the same protocol. The insolubility of potassium phosphate in ethanol at room temperature made the separation and reuse of the catalyst more convenient. The use of low-boiling alcohol not only allowed high-efficiency degradation but also enabled easy separation from the degradation products. The excellent degradation performance was attributed to the improved swelling of the thermoset and the increased solubility of potassium phosphate induced by small amounts of water in the alcohol. This research provides a recycling method that can reintegrate thermoset waste plastics into remodeling ones under the background of circular economy.