Abstract
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.