Light-Driven Coupled Upcycling of Polyethylene and CO₂ to Aromatics over Zeolite-Ni/CeO₂ Composite Catalysts

Coupled upcycling of polyolefins and CO₂ into valuable chemicals is a promising waste management strategy, but conventional thermocatalysis requires harsh conditions and high energy input. Here, we report a light-driven photothermal tandem catalyst of Zn/ZSM-5 and Ni/CeO₂ for efficient coconversion of low-density polyethylene (LDPE) and CO₂. The highly dispersed Ni/CeO₂ component delivers strong light-to-heat conversion and abundant Ni-O-Ce interfacial oxygen vacancies for CO₂ activation. Under illumination, Zn/ZSM-5 catalyzes LDPE C-C cleavage and aromatization, generating active hydrogen species. Simultaneously, Ni/CeO₂ then consumes hydrogen via reverse water-gas shift, suppressing alkene hydrogenation and promoting aromatics formation. The photothermal catalytic system achieves 82.4% LDPE conversion and 34% aromatic selectivity. This work provides an energy-efficient, solar-driven route for plastic and CO₂ upcycling toward carbon-neutral chemical recycling.