Progress in the Understanding and Applications of the Intrinsic Reactivity of Graphene‐Based Materials

Enhancing the intrinsic reactivity of graphene materials is essential for the development of low‐cost materials such as catalysts for various applications. Although an increasing understanding of the intrinsic reactivity of these materials is being achieved, the mechanisms of these materials for catalyzing various reactions have not been fully understood. It is believed that the intrinsic reactivity of pristine graphene originates from its edge and defect sites, and unpaired electrons (radicals) particularly of graphene oxide have also been demonstrated to contribute to the reactivity. Herein, the various edges and defects, and radicals, as well as their influences on the electron structure, reactivity, and applications of graphene‐based materials are reviewed and analyzed. Knowledge gaps in advancing the understanding of the structure–property–reactivity correlations of these materials are discussed. The intrinsic reactivity of graphene materials can be enhanced by engineering its edge, defects, and free radicals, which enables fabrication of low‐cost carbon‐based metal‐free and dopant‐free catalysts for various applications.