Boron Carbonitride Lithium-Ion Capacitors with an Electrostatically Expanded Operating Voltage Window

Lithium-ion capacitors (LICs) have emerged as attractive energy storage devices to bridge the gap between lithium-ion batteries and supercapacitors. While the distinct charge storage kinetics between the anode and the cathode is still a challenge to the widespread application of LICs, the key to improving the energy density of these devices is to widen the operating voltage window and balance the mismatch of the electrode kinetics. To this end, we propose a strategy based on electrostatic attraction by adjusting the B and N atom contents of boron carbonitride (BCN) electrode materials to alter their electronegativities and successfully prepared B-rich and N-rich BCN nanotubes (BCNNTs) via a facile solid-phase synthesis approach. The B-rich BCN (B-BCN) cathode and N-rich BCN (N-BCN) anode noticeably enhance the adsorption of anions and cations, promoting a matching degree between the anode and cathode. In particular, the rationally designed B-BCN//N-BCN LIC achieves a maximum voltage range of 4.8 V, setting a new record for LICs. Furthermore, the energy density reaches up to 200 Wh kg^-1 (based on the total mass of cathodic and anodic active materials). Density functional theory calculations provided insight into the mechanism underlying our strategy of widening the voltage range. Our philosophy provides new design guidelines and alternatives for identifying and optimizing high-performance electrodes for energy storage devices.