Reductive Photocatalysis Unlocks the Hydrodeoxygenation of Polycarbonate Plastic Into Fuel‐Range Hydrocarbons

Polycarbonate (PC) is among the most challenging plastics to recycle because its robust aromatic C─O linkages resist conventional depolymerization strategies. Here, we report the first visible-light-driven photocatalytic system for the reductive depolymerization and hydrodeoxygenation of PC under ambient conditions, selectively producing propane-2,2-diyldicyclohexane (DCHP), a saturated hydrocarbon relevant to jet fuel applications. A multifunctional Ru@P-CHS(g-C₃N₄) catalyst integrates light harvesting, electron mediation, acidity, and hydrogen activation, enabling near-quantitative conversion of bisphenol A with ∼94% molar selectivity toward DCHP. The catalyst also efficiently depolymerizes a range of real-world PC waste. Mechanistic investigations, including in situ UPS, kinetic isotope effect measurements, H₂─D₂ scrambling experiments, and DRIFT-IR spectroscopy, reveal light-driven electron accumulation at Ru sites and the formation of Ru─H intermediates, confirming illumination-induced H₂ activation at Ru that drives C─O bond cleavage. This work establishes a sustainable strategy for converting end-of-life plastics into fuel-range hydrocarbons and introduces reductive photocatalysis as a new paradigm for plastic upcycling.