Reduced graphene oxide (RGO) is an ideal material as an electrode used in the electrochemical energy storage field. However, the serious aggregation of graphene sheets and fewer chemically active sites limit it from exhibiting higher performance. Herein, we introduce a facile solvothermal reaction method to simultaneously regulate the functional groups on RGO, balance the aggregation and connection of graphene sheets, and dope the nitrogen element in a graphene network. The obtained electrode (RGO-N(DMF)) has a high content of carbonyl and nitrogen functional groups, and shows a fluffy structure as well as good electron conductivity, exhibiting both high chemically and physically actives sites. Benefiting from these advantages, RGO-N(DMF) shows a high specific capacity of 135 mA h g−1 at 0.2 A g−1 and favorable rate performance of maintaining 53% capacity at 50 A g−1, which are both higher than those of the normal hydrothermally obtained RGO electrodes. More interestingly, RGO-N(DMF) can maintain the high electrochemical performance at a high mass loading of 5.1 mg cm−2. In addition, when the RGO-N(DMF) electrode is used in the flexible Zn-ion hybrid supercapacitor (ZHS), the capacity retention remains at 100% after 500-time bending, showing excellent mechanical flexibility. This study not only provides an effective strategy for constructing carbon-based cathode materials with excellent properties, but also provides prospects and enlightenment for the practical application of aqueous ZHSs.
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