Multi-redox phenazine/non-oxidized graphene/cellulose nanohybrids as ultrathick cathodes for high-energy organic batteries

Various redox-active organic molecules can serve as ideal electrode materials to realize sustainable energy storage systems. Yet, to be more appropriate for practical use, considerable architectural engineering of an ultrathick, high-loaded organic electrode with reliable electrochemical performance is of crucial importance. Here, by utilizing the synergetic effect of the non-covalent functionalization of highly conductive non-oxidized graphene flakes (NOGFs) and introduction of mechanically robust cellulose nanofiber (CNF)-intermingled structure, a very thick (≈ 1 mm), freestanding organic nanohybrid electrode which ensures the superiority in cycle stability and areal capacity is reported. The well-developed ion/electron pathways throughout the entire thickness and the enhanced kinetics of electrochemical reactions in the ultrathick 5,10-dihydro-5,10-dimethylphenazine/NOGF/CNF (DMPZ-NC) cathodes lead to the high areal energy of 9.4 mWh·cm^-2 (= 864 Wh·kg^-1 at 158 W·kg^-1). This novel ultrathick electrode architecture provides a general platform for the development of the high-performance organic battery electrodes.