Jia Wang, Dongxian Li, Zedong Zhang, Zechao Zhuang, Jiarui Yang, Shule Wang, Tao Gan, Dingsheng Wang, Jianchun Jiang
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.