Abstract
Single-use polyolefins are widely used in our daily life and industrial production due to their light weight, low cost, superior stability, and durability. However, the rapid accumulation of plastic waste and low-profit recycling methods resulted in a global plastic crisis. Catalytic hydrogenolysis is regarded as a promising technique, which can effectively and selectively convert polyolefin plastic waste to value-added products. In this perspective, we focus on the design and synthesis of structurally well-defined hydrogenolysis catalysts across mesoscopic, nanoscopic, and atomic scales, accompanied by our insights into future directions in catalyst design for further enhancing catalytic performance. These design principles can also be applied to the depolymerization of other polymers and ultimately realize the chemical upcycling of waste plastics.