Assembling Carbon Pores into Carbon Sheets: Rational Design of Three-Dimensional Carbon Networks for a Lithium–Sulfur Battery

The conversion reaction-based lithium-sulfur battery features an attractive energy density of 2600 W h/kg. Nevertheless, the unsatisfied performance in terms of poor discharge capacity and cycling stability still hinders its practical applications. Recently, porous carbon materials have been widely reported as promising sulfur reservoirs to promote the sluggish reaction kinetics of sulfur conversion, tolerate volume expansion of sulfur, and suppress polysulfide shuttling. However, porous carbon with a simply designed nanostructure is hard to satisfy all of these aspects simultaneously. Herein, we have applied a dual-template strategy that assembles carbon pores into carbon sheets to prepare three-dimensional (3D) nitrogen-doped porous carbon nanosheets (N-PCSs) as the multifunctional sulfur host for the Li-S battery. By arranging carbon pores within an interconnected 3D architecture, the porous carbon sheets enable rapid electron/ion transfer. Moreover, the micro/mesopores and nitrogen dopant in N-PCS provide both physical and chemical restrictions to polysulfide species. With these advances, the N-PCS/S cathode delivers a large initial discharge capacity of 1360 mA h/g at 0.1 C. When performed at 0.5 C for 1000 cycles, the cathode can still remain ∼50% of its capacity with a low decay rate of 0.05% per cycle, showing the important role of the 3D carbon material in the Li-S battery.