Functionalization and Crosslinking of Reduced Graphene Oxide Sheets by Multiple Tetrazine Units to Improve the Energy Storage in Supercapacitors

A multi‐tetrazine compound tailored for grafting on graphene sheets has been designed and investigated. It is composed of hydrogen substituted tetrazines involved in inverse Diels‐Alder demand cycloaddition reactions for grafting and a central dialkoxytetrazine to confer redox properties to the final material. The successful incorporation of this compound in reduced graphene oxide was demonstrated by elemental analysis, XPS, Raman spectroscopy, AFM, SEM and XRD. Cyclic voltammetry shows the redox activity of the remaining central tetrazine unit in graphene and allows to assess the specific capacity of the material. A significant increase in the specific capacity was found compared to pristine graphene and another tetrazine model compound bearing only one grafting unit. This result was assigned to an increase in the specific area in relation to bridges created between graphene sheets, as evidenced by AFM and XRD. The performance in energy storage were assessed in symmetrical Swagelok cells confirming the high impact of the functionalization on capacitance values.