Synergistic effect of nitrogen and oxygen dopants in 3D hierarchical porous carbon cathodes for ultra-fast zinc ion hybrid supercapacitors

Zinc-ion hybrid supercapacitor is one of the most promising electrochemical energy storage devices for the applications needing both high energy densities and power densities. Nitrogen doping is an effective way to enhance the capacitive performance of porous carbon cathodes in zinc-ion hybrid supercapacitor. However, accurate evidence is yet needed to demonstrate how nitrogen dopants influence the charge storage of Zn2+ and H+ cations. Herein, we prepared 3D interconnected hierarchical porous carbon nanosheets by a one-step explosion method. The effect of nitrogen dopants on pseudocapacitance was analyzed by the electrochemical behaviors of as-prepared porous carbon samples with similar morphology and pore structure but different nitrogen and oxygen doping levels. Ex-situ XPS and DFT calculation demonstrate that nitrogen dopants promote the pseudocapacitive reactions by lowering the energy barrier for the change of oxidation states of carbonyl moieties. Owing to the improved pseudocapacitance by nitrogen/oxygen dopants and fast diffusion of Zn2+ ions in 3D interconnected hierarchical porous carbon matrix, the as-constructed ZIHCs show both high gravimetric capacitance (301 F g-1 at 0.1 A g-1) and excellent rate capability (a capacitance retention of 30% at 200 A g-1).