Biomimetic Electronic Communication of Iodine Doped Single‐Atom Fe Site for Highly Active and Stable Dopamine Oxidation

Abstract Rational design of highly active and stable catalysts for dopamine oxidation is still a great challenge. Herein, inspired by the catalytic pocket of natural enzymes, an iodine (I)‐doped single Fe‐site catalyst (I/Fe SA NC) is synthesized to mimic the catalytic center of heme enzymes in both geometrical and electronic structures, aiming to enhance dopamine (DA) oxidation. Experimental studies and theoretical calculations show that electronic communication between I and FeN 5 effectively modulates the electronic structure of the active site, greatly optimizing the overlap of Fe 3d and O 2p orbitals, thereby enhancing OH adsorption. In addition, the electronic communication induced by iodine doping attenuates the attack of proton hydrogen on the active center, thereby enhancing the stability of I/Fe SA NC. This work provides new insights into the design of highly active and stable single‐atom catalysts and enhances the understanding of catalytic mechanisms for DA oxidation at the atomic scale.