Decoding Synergistic Pathways in Bimetallic MOFs for Advanced Oxidation Processes

ABSTRACT Bimetallic metal–organic frameworks (BMOFs) offer a versatile platform for advanced oxidation processes (AOPs) because paired metal centers can regulate framework structure, charge distribution, redox cycling, oxidant activation, and reactive‐species generation. This review presents a mechanism‐oriented analysis of BMOF‐based AOPs for wastewater remediation, covering material design, synthesis, purification, activation, structural validation, and catalytic applications. Particular attention is given to validating genuine BMOF formation through phase, compositional, spatial, and local‐structural analyses, and to establishing bimetallic synergy through appropriate controls, leaching tests, spectroscopic evidence, and theoretical calculations. Cooperative pathways are compared across photocatalysis, H 2 O 2 activation, peroxymonosulfate and peroxydisulfate activation, catalytic ozonation, and peracetic acid activation, with emphasis on how metal chemistry and local coordination regulate electronic structure, oxidant selectivity, reactive‐species generation, and catalytic performance. Cross‐study comparisons, metal leaching, aqueous stability, and performance in real‐water matrices are critically assessed, while catalyst recovery and long‐term operation are identified as key practical gaps. Finally, design principles and future priorities are proposed for developing stable, scalable, and mechanistically validated BMOFs for practical wastewater treatment. By integrating structural validation, mechanistic analysis, design principles, and engineering considerations, this review provides a basis for developing stable and scalable BMOF‐AOP systems for practical wastewater treatment.