Self‐templated covalent functionalization of graphitic surfaces with a quasi‐periodic pattern

Patterned covalent functionalization of graphitic surfaces (GSs) is of interest in the development of devices and nanocomposite materials. In contrast to the strategies using external templates or control for realizing patterned covalent functionalization of GSs, here, we present a self‐templated strategy by exploiting the synergistic effects of chemical and physical functionalization of GSs. Therefore, a diazonium salt is reduced by potassium iodide (KI) in dimethyl sulfoxide while the solution is in contact with a GS, resulting in its spatially heterogeneous, that is, chemical and physical, functionalization. This heterogeneous functionalization leads to a quasi‐periodic pattern of striped corrals with three equivalent orientations in the covalent layer. The formation of the striped corrals is ascribed to physisorbed domains formed by self‐assembled N 2 , which is produced in situ during the reduction of the diazonium salt, preventing the covalent functionalization.