Engineering Interfacial Compatibility and Dynamic Active Hydrogen Pools to Accelerate Polyolefin Hydrogenolysis

The chemical inertness of polyolefin plastics poses a significant challenge to their efficient recycling. In this work, a Ru/TiO2-CNT catalyst is developed by engineering interfacial compatibility and dynamic active hydrogen pools to accelerate polyolefin hydrogenolysis. Enhanced interfacial compatibility between Ru and TiO2 optimizes the electronic state of Ru, thereby facilitating effective C−C bond cleavage. Meanwhile, dynamic active hydrogen pools, enabled by a reversible hydrogen spillover pathway mediated by CNTs as a hydrogen-transfer channel, promote efficient hydrogenation and desorption of reaction intermediates. Under mild conditions, the catalyst exhibits broad applicability toward a variety of real-world polypropylene (PP) and polyethylene (PE) wastes. This work presents an effective catalyst construction strategy and offers fundamental insights into the hydrogenolysis of waste polyolefins.