Utilizing Crystal Phase‐Specific Interactions to Regulate Catalysts for Boosting Fenton‐Like Nonradical Reaction Activity and Stability

Abstract A notable challenge persists in understanding how crystal phase‐site interactions govern the activity and stability of catalytic materials. A series of FeNC@C composites is fabricated, and the universal principles in precisely controlling crystal composition are proposed for leveraging the interactions among FeN x , Fe 3 C, Fe, and graphite to regulate the generation of ROS and electron transfer in the Fenton‐like reaction. The crystal interactions restrict the spin state of Fe to intermediate‐low levels, ensuring that the reaction remains a non‐radical process. The non‐radical pathway is not singular; the dominance of single or two‐electron transfer processes depends on the potential difference between the contaminants and the catalyst. A matrix equation is constructed to conclusively describe the roles of sites‐specific interactions in catalytic activity. The catalytic reaction showed pH independence due to the stabilization of the interactions, which nearly completely suppresses iron leaching during the reaction. This finding provides guidance for the efficient utilization of crystal phase‐specific interactions to regulate the heterogeneous Fenton‐like reaction.