Mixed plastics encountered in automotive or packaging sectors represent a real challenge for recycling at end-of-life. Here, we provide a circular system for the recycling of mixed-polymers by controlling the hydrolysis rates of polydiketoenamines (PDKs) with the molecular tuning of the polymer microstructure and a regulation of the temperature (Figure 1). Spatio-temporal control on PDK chemical recycling was realized on mixed-PDK laminates, composites and bonded assemblies, enabling the recovery of pure monomers and additives at every step of the process. We show by using small molecule analogues of the polymer, we may understand acid-catalyzed PDK depolymerization through (1) a computational study of the energetic barrier of the rate limiting step and (2) an experimental validation of the diketoenamine bond hydrolysis rates. The temperature dependency of the hydrolysis of different PDK variants opens new opportunities for associating mixed reusable feedstocks and sustainable manufacturing.

Circular polydiketoenamines enabling mixed plastic recycling through variable rates of hydroysis

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