Sandwich-type CoSe2-CNWs@NG as host for lithium-sulfur batteries with high sulfur loading, ultrahigh rate, and long lifespan

Abstract

While lithium-sulfur batteries (LSBs) have tremendous potential in capacity and energy, their application in practice is limited by short cycle life, slow reaction kinetics, and underutilization of sulfur. To tackle these challenges, we have developed a multifunctional host consisting of sandwich-type CoSe2-CNWs@NG that were hydrothermally synthesized through self-assembly of CoSe2-embedded carbon nanowires (CoSe2-CNWs) with N-doped graphene (NG). Through the implementation of CoSe2-CNWs@NG as a host material, active sulfur can be effectively intercalated within the interlayer spaces of neighboring NG layers. The extensive contact area between sulfur and NG sheets facilitates rapid electron transfer, thereby maximizing sulfur utilization. N-doped graphene and polar CoSe2 provide sufficient chemisorption sites for polysulfides, while the catalytic activity of CoSe2 promotes polysulfide conversion. In addition to building a good conductivity structure for fast carrier transport and electrolyte diffusion, the sandwich structure of CoSe2-CNWs@NG physically restricts polysulfides and buffers substantial sulfur volume changes during cycling. As a result, the CoSe2-CNWs@NG/S cathode possessing high-load sulfur capacity (4.06 mg cm−2) exhibits superior cell performance at an ultrahigh rate as well as low E/S ratio. After 1000 cycles at 10 C, it achieves a remarkable reversible capacity of 314.4 mAh g−1 with an impressively low average fading rate of 0.023 % per cycle. Even at a low E/S ratio of 5 μL mg−1, the cathode exhibits remarkable performance, retaining a reversible capacity of 628.2 mAh g−1 after 150 cycles at the rate of 1 C.