The Unique Fe₃Mo₃N Structure Bestowed Efficient Fenton‐Like Performance of the Iron‐Based Catalysts: The Double Enhancement of Radicals and Nonradicals

Abstract Iron‐based catalysts are widely used in Fenton‐like water pollution control technology due to their high efficiency, but their practical applications are limited by complex preparation conditions and strong blockage of Fe²⁺/Fe³⁺ cycle during the reaction. Here, a new iron–molybdenum bimetallic carbon‐based catalyst is designed and synthesized using cellulose hydrogel for adsorption of Fe and Mo bimetals as a template, and the effective iron cycle in water treatment is realized. The integrated materials (Fe_2.5Mo@CNs) with “catalytic/cocatalytic” performance have higher Fenton‐like activation properties and universality than the equivalent quantity iron–carbon‐based composite catalysts (Fe@CNs). Through the different characterization methods, experimental verifications and theoretical calculations show that the unique Fe₃Mo₃N structure promotes the adsorption of persulfate and reduces the energy barrier of the reaction, further completing the double enhancement of radicals (such as SO₄·⁻) and nonradicals (¹O₂ and electron transport process). The integrated “catalytic/cocatalytic” combined material is expected to provide a new promotion strategy for Fenton‐like water pollution control.