Effects of Intrinsic Pentagon Defects on Electrochemical Reactivity of Carbon Nanomaterials
Defect engineering is pivotal to the construction of high‐performance carbon nanomaterials toward many energy conversion and storage devices. In this work, theoretical calculations reveal that intrinsic pentagons in the basal plane can contribute to the local electronic redistribution and the contraction of bandgap, making the carbon matrix possess superior binding affinity and electrochemical reactivity. To experimentally verify this, pentagon defect‐rich carbon nanomaterial is first constructed by means of in situ etching of fullerene molecules (C60). The electrochemical tests show that, relative to common hexagons, such a carbon‐based material with abundant intrinsic pentagon defects makes much greater contribution to the electrocatalytic oxygen reduction activity and electric double layer capacitance. Especially, it shows a four‐electron‐reaction mechanism similar to that of commercial Pt/C and other transit metal‐based catalysts, and a higher specific capacitance than many reported metal‐free carbon materials. These mutually corroborative results confirm the profound influence of intrinsic pentagon defects for developing efficient and economical carbon‐based nanomaterials toward energy conversion and storage devices.