Closing the loop for poly(butylene-adipate-co-terephthalate) recycling: depolymerization, monomers separation, and upcycling

Efficient recycling and upcycling strategies to retain the material in the economy and away from the ecosystems are important to achieve a sustainable plastic system. Poly(butylene adipate-co-terephthalate) (PBAT) is a biodegradable polyester that has gained considerable interest for various applications. Here, we report a study on enzymatic depolymerization of PBAT, recovery and purification of its monomers, and feasible routes for their recycling/upcycling. PBAT films (15 g L⁻¹) were completely hydrolysed employing a leaf-branch compost cutinase variant (LCC-WCCG, 1.4 mg per gram polymer) to its monomers at a rate of 0.49 g L⁻¹ h⁻¹. LCC-WCCG kinetics were superior to that of other enzymes engineered for PBAT hydrolysis; the data were supported by in silico investigations. The released monomers were separated using membrane filtration and precipitation techniques and recovered with purity exceeding 95%. To close the loop, the monomers were re-polymerized and successfully cast into PBAT films. Moreover, adipic acid was reacted with hexamethylene diamine using Novozym®435 to form a polyamide, while 1,4-butanediol was oxidized to 4-hydroxybutyrate using Gluconobacter oxydans cells. The current study exemplifies a high-impact scientific approach toward a circular plastics economy.