Ni Supported on Urea‐Modified LaFeO 3 Perovskite for Efficient Hydrogenolysis of Polyethylene Plastics

ABSTRACT Hydrogenolysis of polyolefin plastics represents a promising strategy for their chemical recycling into liquid/wax fuels. However, the development of efficient non‐noble metal catalysts remains a major challenge. Herein, we report Ni catalysts supported on urea‐modified LaFeO 3 perovskites with systematically controlled La‐vacancy (V La ) concentrations (Ni/ x U‐LFO, x = 0, 1, 2, and 4) for polyethylene (PE) hydrogenolysis. Controlled modulation of V La effectively tunes the electronic structure of Ni, oxygen vacancy (V O ) formation, and hydrogen spillover behavior. Among the catalysts, Ni/2U‐LFO exhibits the most oxidic Ni electronic structure and the strongest hydrogen spillover capability. As a result, Ni/2U‐LFO delivers the highest PE conversion and liquid/wax yield. These results highlight A‐site defect engineering in perovskite supports as a powerful strategy to optimize the hydrogen behavior and electronic structure of non‐noble metal catalysts, enabling highly efficient and stable polyolefin hydrogenolysis.