In Situ High-Level Nitrogen Doping into Carbon Nanospheres and Boosting of Capacitive Charge Storage in Both Anode and Cathode for a High-Energy 4.5 V Full-Carbon Lithium-Ion Capacitor.

To circumvent the imbalances of electrochemical kinetics and capacity between Li storage anodes and capacitive cathodes for lithium-ion capacitors (LICs), we herein demonstrate an efficient solution by boosting the capacitive charge-storage contributions of carbon electrodes to construct a high-performance LIC. Such a strategy is achieved by the in situ and high-level doping of nitrogen atoms into carbon nanospheres (ANCS), which increases the carbon defects and active sites, inducing more rapidly capacitive charge-storage contributions for both Li storage anodes and PF storage cathodes. High-level nitrogen-doping-induced capacitive enhancement is successfully evidenced by the construction of a symmetric supercapacitor using commercial organic electrolytes. Coupling a pre-lithiated ANCS anode with a fresh ANCS cathode enables a full-carbon LIC with a high operating voltage of 4.5 V and high energy and power densities thereof. The assembled LIC device delivers high energy densities of 206.7 and 115.4 Wh kg at power densities of 0.225 and 22.5 kW kg, respectively, as well as an unprecedented high-power cycling stability with only 0.0013% capacitance decay per cycle within 10 000 cycles at a high power output of 9 kW kg.