Nitrogen-enriched graphene framework from a large-scale magnesiothermic conversion of CO2 with synergistic kinetics for high-power lithium-ion capacitors

Lithium-ion capacitors are envisaged as promising energy-storage devices to simultaneously achieve a large energy density and high-power output at quick charge and discharge rates. However, the mismatched kinetics between capacitive cathodes and faradaic anodes still hinder their practical application for high-power purposes. To tackle this problem, the electron and ion transport of both electrodes should be substantially improved by targeted structural design and controllable chemical doping. Herein, nitrogen-enriched graphene frameworks are prepared via a large-scale and ultrafast magnesiothermic combustion synthesis using CO2 and melamine as precursors, which exhibit a crosslinked porous structure, abundant functional groups and high electrical conductivity (10524 S m−1). The material essentially delivers upgraded kinetics due to enhanced ion diffusion and electron transport. Excellent capacities of 1361 mA h g−1 and 827 mA h g−1 can be achieved at current densities of 0.1 A g−1 and 3 A g−1, respectively, demonstrating its outstanding lithium storage performance at both low and high rates. Moreover, the lithium-ion capacitor based on these nitrogen-enriched graphene frameworks displays a high energy density of 151 Wh kg−1, and still retains 86 Wh kg−1 even at an ultrahigh power output of 49 kW kg−1. This study reveals an effective pathway to achieve synergistic kinetics in carbon electrode materials for achieving high-power lithium-ion capacitors. A large-scale and ultrafast combustion synthesis using CO2 as feedstock is demonstrated for the fabrication of nitrogen-enriched graphene frameworks (NGF) with high electrical conductivity, which delivers an upgraded kinetics due to the enhanced ion diffusion and electron transport. Lithium-ion capacitors based on NGF as both cathode and anode exhibit a high gravimetric energy density of 151 Wh kg−1 and power output of 49 kW kg−1. This study reveals an effective pathway to achieve synergistic kinetics in electrode materials for high-performance electrochemical energy storage.