Abstract Upcycling waste plastics into liquid fuels presents significant potential for advancing the circular economy but is hindered by poo
Abstract Upcycling waste plastics into liquid fuels presents significant potential for advancing the circular economy but is hindered by poor selectivity and low-value methane byproduct formation. In this work, we report that atomic Ru-doped ZrO2 can selectively convert 100 grams of post-consumer polyethylene and polypropylene, yielding 85 mL of liquid in a solvent-free hydrocracking. The liquid (C5-C20) comprises ~70% jet-fuel-ranged branched hydrocarbons (C8-C16), while the gas product is liquefied-petroleum-gas (C3-C6) without methane and ethane. We found that the atomic Ru dopant in the Ru-O-Zr moiety functionalizes its neighboring O atom, originally inert, to create a Brønsted acid site. This Brønsted acid site, rather than the atomic Ru dopant itself, selectively governs the internal C−C bond cleavage in polyolefins through a carbonium ion mechanism, thereby enhancing the yield of jet-fuel-ranged hydrocarbons and suppressing methane formation. This oxide modulation strategy provides a paradigm shift in catalyst design for hydrocracking waste plastics and holds potential for a broad spectrum of applications.