Constructing monolithic sulfur cathodes with multifunctional N,P dual-doped carbon nanocages to achieve high-areal-capacity lithium-sulfur batteries

Despite the great progress achieved, lithium-sulfur (Li-S) batteries still suffer unsatisfactory performance at high sulfur loading (>5 mg cm⁻²), which results from the impeded kinetics in charge transfer and polysulfides conversion with increasing electrode thickness. Herein, we have constructed a high-sulfur-loading monolithic cathode by in-situ reducing graphene oxide (GO) in the aqueous solution with dispersed sulfur-filled N,P dual-doped carbon nanocages (NPCNC). The Li-S battery with the areal sulfur loading of 6 mg cm⁻² exhibits a high areal capacity of 6.7 mAh cm⁻² and a retention of 4.2 mAh cm⁻² after 250 cycles. The excellent performance is attributed to the synergism of the facilitated charge transfer and alleviated polysulfide diffusion by the reduced GO-framed 3D network, and the suppressed shuttle and polarization effects by the confinement and electrocatalysis of NPCNC. In addition, the monolithic sulfur electrode is free from binder, conductive agent and current collector, much beneficial to gravimetric performance. This study demonstrates an efficient strategy to increase the areal performance of Li-S batteries.