Suppression of Structural Heterogeneity in High‐Entropy Intermetallics for Electrocatalytic Upgrading of Waste Plastics

Abstract The key to fully realizing the potential of high‐entropy alloys (HEAs) lies in balancing their inherent local chemical disordering with the long‐range ordering required for electrochemical applications. Herein, we synthesized a distinctive L1 0 ‐(PtIr)(FeMoBi) high‐entropy intermetallics (HEIs) exhibiting nanoscale long‐range order and atomic scale short‐range disorder via a lattice compensation strategy to mitigate the entropy reduction tendency. The (PtIr)(FeMoBi) catalyst exhibited remarkable activity and selectivity of glycollic acid (GA) production via electrocatalytic waste polymer‐derived ethylene glycol oxidation reaction (EGOR). With a mass activity of 5.2 A mg Pt −1 and a Faradaic efficiency (FE) for GA of 95 %, it outperformed most previously reported electrocatalysts for selective GA production. The lattice‐compensation effect promotes the homogeneity of Pt and Fe actives sites, facilitating co‐adsorption of EG and OH and reducing the energy barriers for dehydrogenation and OH‐combination processes. This approach effectively avoids the formation of low‐active sites commonly encountered in HEA solid solutions, offering a promising avenue for exploring the complex interplay between catalytic activity and HEI structures.