Traditional graphene-based electrode materials often can not have excellent gravimetric and volumetric electrochemical properties at the same time. Furthermore, the gel electrolyte widely used at present has the disadvantages of poor water retention, easy solidification, low ionic conductivity, and narrow working temperature range during the working process. In this paper, nanocellulose/N, P co-doped reduced graphene oxide composites (NC-NPrGOs) were synthesized via a simple approach using graphene oxide (GO), ammonium dihydrogen phosphate, and nanocellulose (NC) as raw materials. Meanwhile, a new type of gel electrolyte (SNG) with renewable, wide working temperature range and ultra-high water retention properties was prepared using sodium alginate (SA), NC, GO, and potassium hydroxide as precursors. Benefiting from the unique physical and chemical properties of NC-NPrGOs, the assembled aqueous symmetric supercapacitors assembled by NC-NPrGOs present high gravimetric (303.9 F/g) and volumetric specific capacitance (416.5 F cm−3), large gravimetric (10.5 Wh kg−1) and volumetric energy density (14.6 Wh/L). Due to the multiple interactions of several components in SNG, the flexible solid-state supercapacitors (ASSC) assembled by NC-NPrGO55 and SNG deliver high specific capacitance (240.0 F/g), ultra-long cycling life, excellent bending resistance, a wide range of operating temperatures, and good regenerative performance. In summary, NC-NPrGOs and SNGs are ideal for the investigation of new energy storage devices.
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