Metal-Acid Balance Enables Earth-Abundant Metal Upcycling of Polyolefins to Jet Fuel

Abstract Hydrocracking over bifunctional metal–acid catalysts offers a promising route for converting polyolefin waste into liquid fuels, but highly active and economically viable non-noble-metal catalysts remain scarce. Here we show that such catalysts can be developed by independently tuning metal and acid sites to balance the tandem reactions occurring on them. Using inert zirconia as the support, we introduced atomically dispersed Ni and sulfate species to create independently tunable metal and acid functions. This design balances the rates of (de)hydrogenation and C–C bond cleavage of the substrate, enabling efficient polyolefin conversion. The optimized Ni–ZrO2/SO42– catalyst converted 200 g of postconsumer plastics into 187 g of methane-free fuels (C3–C20), including 117 g in the jet-fuel range (C8–C16). A volcano relationship between catalytic performance and the metal-to-acid ratio reveals a narrow optimum, underscoring the need for precise control of metal–acid balance. Extension of this strategy to Co- and Mo-based systems further demonstrates its generality and potential for scaled-up polyolefin upcycling.