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Abstract

The abundant surface chemical information and edge structures of carbon materials have attracted tremendous interest in catalysis. For the oxygen evolution reaction (OER), edge effects of carbon materials have been rarely studied in detail due to the complexity of various coexisting edge configurations and the controversy between carbon corrosion and carbon catalysis. In the present work, the exact roles of common carbon active edge sites in OER using polycyclic aromatic hydrocarbons (PAHs) with designated configurations (zigzag and armchair) as model probe molecules were interrogated with the focus on structure‐function relationships. Zigzag configurations of PAHs were determined to show high activity for OER while also showing a remarkable stability at a reasonable potential. It performs with a TOF value of 0.276 s^‐1 in 0.1 M KOH. The catalytic activity of carbon edge sites could be further effectively regulated by extending their π conjugation structure at a molecular level.