Short-Chain Polyselenosulfide Copolymers as Cathode Materials for Lithium-Sulfur Batteries

Copolymerization of sulfur, which forms sulfur-rich polymers, has recently opened a new era in the lithium-sulfur (Li-S) battery research as improved battery performances could be achieved compared to pure sulfur (S₈). By means of organic chemistry, sulfur copolymers with desired features and chemical structures could be rationally designed and synthesized. In this study, sulfur-rich polymers consisting of short-chain tetrasulfide (R-S₄-R) (PTS) and selenotrisulfide (R-SeS₃-R) (PTSeS) bonds are suggested as cathode materials for Li-S batteries. Intrinsically short poly(seleno)sulfide bonds along with covalent anchoring effect effectively suppress the parasitic shuttle effect originating from soluble long-chain lithium polysulfides formed from pure S₈. Furthermore, a comparative study demonstrates the indisputable advantage of the selenium doping, which enhances the electrical conductivity of the polymer and following battery performances. In terms of cycling performance, both PTSeS and PTS with ∼2 mg cm^-2 polymer loading exhibit small capacity decays of 0.078 and 0.052% per cycle until 500 cycles at 0.5C, respectively. However, active material utilization and high rate performance are substantially superior in PTSeS due to the enhanced electron transfer kinetics. This work would provide useful design principles for fabrication of sulfur-based polymers with even greater applicability in future Li-S batteries.