Fabrication of Holey Graphene: Catalytic Oxidation by Metalloporphyrin‐Based Covalent Organic Framework Immobilized on Highly Ordered Pyrolytic Graphite

We report a facile chemical method for fabricating holey graphene by catalytic oxidation of highly ordered pyrolytic graphite (HOPG) using an FeIII porphyrin complex‐based covalent organic framework (COF) as a bifunctional surface catalyst–template. We demonstrate regular hole formation after oxidation with H2O2 and NaOCl, COF removal, and HOPG exfoliation. An organometallic honeycomb: Arrays of holes are patterned on highly ordered pyrolytic graphite (HOPG) by catalytic oxidation using an FeIII porphyrin covalent organic framework surface catalyst template and H2O2/NaOCl. The oxidation localizes in the vicinity of FeIII ions immobilized on the surface of HOPG, facilitating hole formation near the metal catalytic center and generating patterned holes. Subsequent exfoliation conveniently provides multiple holey graphene sheets.