Coordinating Adsorption and Catalytic Activity of Polysulfide on Hierarchical Integrated Electrodes for High-Performance Flexible Li–S Batteries

Lithium–sulfur (Li–S) batteries have been known to be a promising substitute because of their much higher theoretical energy density than that of traditional Li-ion batteries. However, the low utilization of sulfur caused by the poor conductivity of sulfur and shuttle of lithium polysulfides (LiPSs) severely restrict the commercial application of Li–S batteries, especially in flexible wearable devices. Herein, a hierarchical nitrogen-doped carbon nanotube (NCNT)@Co–Co3O4 nanowire array (NWA)-integrated electrode was developed based on the rational design of density functional theory calculations, which shows simultaneous confinement adsorption and catalysis conversion of LiPSs. In situ Raman spectra further proved that the NCNT@Co–Co3O4 NWAs exhibit sufficient adsorption capacity and high catalytic conversion of LiPSs. As a result, the NCNT@Co–Co3O4@S electrode exhibited the desirable specific capacity and excellent cyclic stability at both low and high sulfur loadings. Moreover, pouch cells with the NCNT@Co–Co3O4@S cathode show higher capacity under flat or bending states and longer cycle stability than that of the reported results. This work provides a new approach for the development of high-performance Li–S batteries toward future wearable electronics.