Installing a Trigger to Upcycle High-Density Polyethylene

Creating C═C bonds as “weak” sites in the stable C–C chains of polyethylene (PE) is an appealing strategy to promote sustainable development of the polyolefin industry. Compared to methods, such as dehydrogenation and postpolymerization modification, the copolymerization of ethylene (E) and butadiene (BD) should be a convenient and direct approach to introduce C═C bonds in PE, whereas it encounters problems in controlling the composition and regularity of the copolymer due to the mismatched activities and mechanisms between the two monomers. Herein, we report by employing the amidinate gadolinium complex, controllable E/BD copolymerization was achieved, where BD was incorporated in the uniformly discrete 1,4 mode. The obtained copolymer possesses the same physical, mechanical, processing, and antioxygen (aging at 100 °C for 28 days) properties as commercial high-density-PE, which, strikingly, were degraded by C═C bonds into α,ω-telechelic oligomers with narrow distribution. These degraded functional products were transferred to compatibilizers via atom-transfer radical polymerization or immortal ring-opening polymerization, achieving upcycling.