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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.
This research was supported by Creative Materials Discovery Program (2017M3D1A1039558) and Nano-Material Technology Development Program (NRF-2016M3A7B4900119) through the National Research Foundation of Korea (NRF), funded by the Ministry of Science, ICT and Future Planning (MSIP). This work was also supported by the NRF of the Korea Government (MSIP) under Grant 2016R1E1A1A01943131.