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.

Abstract

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 PF₆^- 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^-1 at power densities of 0.225 and 22.5 kW kg^-1, 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^-1.