Constructing Bimetallic Ruthenium–Nickel Alloy Toward High‐Efficiency Selective Hydrogenolysis of Polyethylene Terephthalate Plastic Waste

The upcycling of plastic waste into renewable chemicals offers a pathway toward carbon resource recovery and reduced environmental pollution. Polyethylene terephthalate (PET) hydrogenolysis can produce aromatic hydrocarbons, cycloalkanes, or a mixture of both, while achieving selective control over the reaction pathway remains challenging. Herein, we report a TiO 2 (P25)‐supported bimetallic Ru─Ni alloy catalyst (RuNi/P25) that can directly upgrade PET into cycloalkanes in 84.9% yield with 100% selectivity among the liquid products under mild reaction conditions (230 °C, 1.5 MPa H 2 ). The outstanding performance of RuNi/P25 mainly originates from the electron‐rich Ru species, which play a key role in activating hydrogen and C─O bonds. The formation of the RuNi alloy facilitates electron transfer from Ni to Ru, thereby accelerating the hydrogenation rate of the benzene ring and promoting the catalytic activity for converting PET to cycloalkanes. The strategy of constructing a RuNi alloy presented in this work affords a promising approach for the development of highly effective catalysts, which can be applied in the valorization of aromatic plastic wastes and biomass‐derived feedstocks.