Interfacial Engineering of Fe–Zr Bimetallic Oxides Boosts Phenolic Pollutants Removal in Heterogeneous Fenton–Like Process

Fenton technology has garnered significant attention for the deep removal of low‐concentration emerging contaminants due to its remarkable oxidation performance. However, the traditional mineralization process for emerging contaminants requires a substantial amount of hydroxyl radicals (HO˙), leading to excessive consumption of H 2 O 2 . Through interfacial engineering of Fe–Zr bimetallic catalysts (FeZrO x ), this study demonstrates synergistic enhancement of phenolic pollutant removal at heterojunction interfaces while achieving an 80% reduction in H 2 O 2 dosage compared to traditional Fe 2 O 3 systems. The chemical states of Fe and Zr at the (104)/(111) heterojunction interface in FeZrO x exhibit marked modifications relative to their monometallic Fe 2 O 3 and ZrO 2 counterparts. The elevated charge density at interfacial Fe sites in FeZrO x promotes HO˙ generation, while optimized antibonding orbital composition below the Fermi level in bisphenol A adsorbed on Zr sites enhances hydrogen abstraction and subsequent polymerization. This Fe–Zr synergy at the (104)/(111) heterojunction concurrently suppresses HO˙ diffusion losses and directs phenolic pollutant (e.g., phenol and bisphenol A) polymerization within the reactive interface, thereby reducing H 2 O 2 consumption compared to monometallic systems.