Selective Upcycling of Polycarbonate Waste to Cyclohexanol via RuLa Dual‐Atom Catalysis

Cyclohexanol is a key intermediate for nylon manufacture, yet its industrial synthesis relies on partial oxidation of cyclohexane at ∼2 MPa with <5% single‐pass conversion, an energetically wasteful and atom‐inefficient process that demands extensive recycle and generates substantial emissions. Here, we introduce an oxygen‐atom‐efficient synthetic strategy that transforms polycarbonate (PC) waste directly into cyclohexanol through a non‐oxidative catalytic route. The method leverages the intrinsic oxygen functionality of the polymer as a built‐in source of hydroxyl groups, thereby eliminating the conventional oxidation step. A RuLa dual‐atom (RuLa‐DA) catalyst anchored on CoAl oxide enables cooperative hydrogen activation and spillover through moderated Ru–H binding, driving selective aromatic‐ring hydrogenation under mild gas‐phase conditions. Operating at 0.25 MPa and a 4.2 s residence time, the tandem hydropyrolysis–hydrogenation process affords a 69.9% yield and 95.4% selectivity for cyclohexanol, maintaining >95% selectivity for post‐consumer PC over 100 feed cycles. Life‐cycle and techno‐economic analyses indicate the potential environmental and economic advantages, showing a 35% cost reduction and a threefold lower carbon footprint relative to the fossil route. This oxygen‐retentive hydrogenation paradigm establishes a general approach for valorizing oxygen‐rich substrates and suggests a conceptually viable pathway toward atom‐economical synthesis and circular chemical manufacturing.