Cooperative behavior in functionalized graphene: Explaining the occurrence of 1,3 cycloaddition of azomethine ylides onto graphene

► Cooperative behavior is responsible for the occurrence of 1,3 dipolar cycloadditions and other organic reactions. ► Reaction energies are increased up to 30 kcal/mol per functional group. ► Functionalization forming infinite armchair lines is the avenue to heavily functionalize graphene. ► The band gap can be varied from 0 to 2 eV!.