Light‐Driven Coupled Upcycling of Polyethylene and CO ₂ to Aromatics over Zeolite–Ni/CeO ₂ Composite Catalysts

Coupled upcycling of polyolefins and CO 2 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/CeO 2 for efficient coconversion of low‐density polyethylene (LDPE) and CO 2 . The highly dispersed Ni/CeO 2 component delivers strong light‐to‐heat conversion and abundant Ni–O–Ce interfacial oxygen vacancies for CO 2 activation. Under illumination, Zn/ZSM‐5 catalyzes LDPE C–C cleavage and aromatization, generating active hydrogen species. Simultaneously, Ni/CeO 2 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 CO 2 upcycling toward carbon‐neutral chemical recycling.