Covalently Patterned Graphene Surfaces by a Force-Accelerated Diels–Alder Reaction

Cyclopentadienes (CPs) with Raman and electrochemically active tags were patterned covalently onto graphene surfaces using force-accelerated Diels–Alder (DA) reactions that were induced by an array of elastomeric tips mounted onto the piezoelectric actuators of an atomic force microscope. These force-accelerated cycloadditions are a feasible route to locally alter the chemical composition of graphene defects and edge sites under ambient atmosphere and temperature over large areas (∼1 cm2).