Discrete Hollow Carbon Spheres Derived from Pyrolytic Copolymer Microspheres for Li-S Batteries

Discrete hollow carbon spheres (HCSs) with a high surface-to-volume ratio and distinct conducting shell have attracted immense attention as electrode materials for batteries and supercapacitors. In this study, we developed a novel and scalable method to synthesize well-defined HCSs. The HCSs were prepared using a pyrolytic soft template of styrene/acrylic acid copolymer microspheres. Sulfur could be effectively confined inside the pores of the uniform-sized HCSs (average diameter = 320 nm, shell thickness = 40–50 nm) to produce a S/HCS-65-IM (S content = 65 wt%) Li-S cathode using a modified sulfur-loading method involving solution impregnation followed by melt-diffusion (IM). S/HCS-65-IM delivered much higher capacity and greater cycling stability over 200 cycles and showed much lower impedance build up than S/HCS-65-PM prepared via the conventional melt-diffusion of a physical mixture of sulfur powder and HCSs. The sulfur utilization of S/HCS-65-IM was further improved by more than 20% by suppressing its lithium-polysulfide shuttle effect using a carbon-coated separator (CCS). The S/HCS-65-IM cathode (with CCS) also exhibited excellent cycling stability (capacity retention of >81% after 200 cycles at 0.5 C) and high rate capability with a reduced interfacial charge transfer resistance, suggesting that S/HCS-65-IM (with CCS) is a promising cathode for Li-S batteries.