Sulfur/carbon cathode material chemistry and morphology optimisation for lithium-sulfur batteries

Lithium-sulfur batteries (LSBs) are a promising alternative to lithium-ion batteries because sulfur is highly abundant and exhibits a high theoretical capacity (1675 mA h g^-1). However, polysulfide shuttle and other challenges have made it difficult for LSBs to be commercialised. Here, a sulfur/carbon (S/C) composite was synthesised and cathodes were fabricated via scalable melt diffusion and slurry casting methods. Carbon nanoparticles (C65) were used as both sulfur host and electrical additive. Various carbon ratios between the melt-diffusion step and cathode slurry formulation step were investigated. An increased amount of C65 in melt-diffusion led to increased structural heterogeneity in the cathodes, more prominent cracks, and a lower mechanical strength. The best performance was exhibited by a cathode where 10.5 wt% C65 (TC10.5) was melt-diffused and 24.5 wt% C65 was externally added to the slurry. An initial discharge capacity of ∼1500 mA h g^-1 at 0.05C and 800 mA h g^-1 at 0.1C was obtained with a capacity retention of ∼50% after 100 cycles. The improved electrochemical performance is rationalised as an increased number of C-S bonds in the composite material, optimum surface area, pore size and pore volume, and more homogeneous cathode microstructure in the TC10.5 cathode.