Enhancing Waste Plastic Hydrogenolysis on Ru/CeO ₂ Through Concurrent Incorporation of Fe Single Atoms and FeO _x Nanoclusters

Abstract Ru‐based catalysts have exhibited significant promise in converting waste plastics into valuable long‐carbon chain products. However, their efficiency is hindered by the uncontrollable cascade hydrogenation, which stems from their exceptional reactivity for C─C cleavage. Herein, we reported a multi‐scale regulation strategy by selectively anchoring Fe single atoms (SAs) and FeO x nanoclusters (NCs) by Ru NCs‐decorated CeO 2 substrates. This catalyst demonstrates an extraordinary performance, achieving nearly 100% low density polyethylene (LDPE) conversion under the conditions of 250 °C and 2 MPa hydrogen after 1 h, along with remarkably‐improved liquid product selectivity of 86.4% compared to that of bare Ru/CeO 2 (59.8%). Through a variety of spectroscopic studies, we revealed the unique interactions between FeO x NCs and Ru NCs, which leads to an increased Ru° content. More significantly, we also confirmed the crucial role of Fe SAs in adsorbing active hydrogen species, thereby increasing the hydrogen coverage. Such precise regulations towards both the intrinsic surface state of Ru and its adjacent chemical environment successfully inhibited the cascade hydrogenation, ultimately resulting in a significant enhancement in the selectivity of liquid products.