The pursuit of new negative electrode materials for redox supercapacitors with a high capacitance, boosted energy, and high rate capability is still a tremendous challenge. Herein, we report a Nile Blue conjugated graphene aerogel (NB-GA) as a negative electrode material with excellent pseudocapacitive performance (with specific capacitance of up to 483 F g at 1 A g) in all acidic, neutral, and alkaline aqueous electrolytes. The contribution from capacitive charge storage represents 93.4% of the total charge, surpassing the best pseudocapacitors known. To assess the feasibility of NB-GA as a negative electrode material across the full pH range, we fabricated three devices, namely, a symmetric NB-GA||NB-GA device in an acidic (1.0 M HSO) electrolyte, an NB-GA||MnO device in a pH-neutral (1.0 M NaSO) electrolyte, and an NB-GA||LDH (LDH = Ni-Co-Fe layered double hydroxide) device in an alkaline (1.0 M KOH) electrolyte. The NB-GA||NB-GA device exhibits a maximum specific energy of 22.1 Wh kg and a specific power of up to 8.1 kW kg; the NB-GA||MnO device displays a maximum specific energy of 55.5 Wh kg and a specific power of up to 14.9 kW kg, and the NB-GA||LDH device shows a maximum specific energy of 108.5 Wh kg and a specific power of up to 25.1 kW kg. All the devices maintain excellent stability over 5000 charge-discharge cycles. The outstanding pseudocapacitive performances of the NB-GA nanocomposites render them a highly promising negative electrode material across the entire pH range.
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