π-Conjugated Carbon Radicals at Graphene Oxide to Initiate Ultrastrong Chemiluminescence

Graphene oxide has widely been employed in various fields, but its structure and composition has still not been fully understood. Here we report that freshly prepared graphene oxide exhibits a large number of π‐conjugated carbon radicals at its π‐network plane, which result from the addition reaction of hydroxyl radicals from H2O2 onto the conjugated double bonds of graphene oxide. The π‐conjugated carbon radicals can directly initiate the long‐lasting visible chemiluminescence of luminol, which is even stronger than that obtained when horseradish peroxidase and H2O2 are used. Previously, graphene oxide was mainly reported to be a quencher of chemiluminescence instead. Remarkably, the reacted radicals can be regenerated, thereby enabling the repetitive initiation of chemiluminescence by re‐treatment of graphene oxide. The results reported here provide a new understanding of the structure, properties, and applications of graphene oxide. GO chemiluminescence: Freshly prepared graphene oxide exhibits a large number of π‐conjugated carbon radicals at its π‐network plane. These radicals result from the addition of hydroxyl radicals from hydrogen peroxide onto the conjugated double bonds of graphene oxide and can directly initiate a long‐lasting visible chemiluminescence of luminol.