Polymeric materials have been accumulating in the environment for decades as a result of the linear way of consuming plastics. Unfortunately, the current approaches followed to treat such a large amount of plastic waste, mainly involving physical recycling or pyrolysis, are not efficient enough. Recently, chemical degradation has emerged as a long-term strategy towards reaching completely sustainable cycles where plastics are polymerised, depolymerised, and then re-polymerised with minimal changes in their quantity or final properties. Organocatalysts, which are promising “green” substitutes for traditional organometallic complexes, are able to catalyse depolymerisation reactions yielding highly pure small molecules that are adequate for subsequent polymerisations or other uses. Moreover, by varying several reaction parameters (e.g. solvent, temperature, concentration, co-catalyst, etc.), the depolymerisation products can be tuned in innumerable possibilities, which further evidences the versatility of depolymerisation. In this review, we highlight the recent advances made by applying organocatalysts, such as organic bases, organic acids, and ionic compounds, to chemically degrade the most commonly used commercial polymers. Indeed, organocatalysis is envisaged as a promising tool to reach a circular and environmentally friendly plastic economy.

Mechanical recycling of polymers downgrades them such that they are unusable after a few cycles. Alternatively, chemical recycling to monomer offers a means to recover the embodied chemical feedstocks for remanufacturing. However, only a limited number of commodity polymers may be chemically recycled, and the processes remain resource intensive. We use systems analysis to quantify the costs and life-cycle carbon footprints of virgin and chemically recycled polydiketoenamines (PDKs), next-generation polymers that depolymerize under ambient conditions in strong acid. The cost of producing virgin PDK resin using unoptimized processes is ~30-fold higher than recycling them, and the cost of recycled PDK resin ($1.5 kg⁻¹) is on par with PET and HDPE, and below that of polyurethanes. Virgin resin production is carbon intensive (86 kg CO₂e kg⁻¹), while chemical recycling emits only 2 kg CO₂e kg⁻¹. This cost and emissions disparity provides a strong incentive to recover and recycle future polymer waste.

We report the potential of thermally stable acid-base mixtures for the upcycling of PET in the presence of amines.