Mono‐Atomic Fe Centers in Nitrogen/Carbon Monolayers for Liquid‐Phase Selective Oxidation Reaction

Abstract Two‐dimensional catalyst supports with mono‐atomic transition metals stabilized in special surface pockets conceptually promise excellent catalytic activity. Similar heterogenized mono‐atomic metal‐based catalysts usually suffer from poor stability in liquid‐phase reaction system, whilst highly ligand‐stabilized metal‐centers are less accessible for reactions. We report a two‐dimensional mono‐atomic Fe/N/C layered nanostructure (2D‐FeNC), generated through the direct polycondensation of C,N‐containing molecules and Fe salts. With a 2D structure similar to graphene, the ultrathin CN support act as a solid ligand, leaving the z‐direction open at molecular scale. This approach significantly promotes reactivity and the mass transfer to the Fe centers, here exemplified by the selective oxidation of alcohols using molecular oxygen. The catalysts show also high mechanical and chemical stability for good to excellent reusability.