Catalytic and Dual-Conductive Matrix Regulating the Kinetic Behaviors of Polysulfides in Flexible Li-S Batteries

The main challenge in developing foldable Li-S batteries (LSB) lies in developing an electrode that is ultraflexible, conductive, and catalytic for dissolved lithium polysulfides (LiPSs). In this paper, lightweight macromolecule graphitic carbon nitride (g-C3N4) film and a conductive polymer (CP) of poly(3,4-ethylenedioxythiophene) shell are introduced into flexible LSBs by compositing with carbon cloth (CC). In the designed hybrid of CP/g-C3N4@CC, 2D g-C(3)N(4)is used in the form of an effective trapper and functions as a continuous catalytic layer for LiPSs via the formation of pyridinic-N-Li bonds. This is revealed by both experimental investigations and theoretical analysis. The sandwich-like CC and CP simultaneously bring an omnidirectional conductive network for fast interfacial reaction kinetics. With these benefits, the self-supported CP/g-C3N4@CC forms a powerful interaction system to fully in situ lock LiPSs in the commercial CC matrix. Thus, a substantially enhanced electrochemical performance is obtained at a high sulfur loading (4.7 mg cm(-2)) even operating in a pouch cell. This work may provide a potential avenue for practical use of high-performance LSBs toward flexible energy-storage devices.