Delaying cyclization of polyacrylonitrile by boric acid for sulfurized poly(acrylonitrile) cathode materials

Abstract

Sulfurized poly(acrylonitrile) (SPAN) has become one of the most promising cathode materials in rechargeable Lithium-Sulfur (Li-S) batteries due to their inhibited polysulfide dissolution, high sulfur utilization and excellent electrochemical performance via unique solid–solid conversion mechanism. However, the sulfur content of SPAN (<50 %) is still one of the significant reasons that restrict the electrochemical performance and practical applicability. In this paper, a small amount of boric acid (HBO) was introduced into the precursor of SPAN cathode materials easily before heat-treating, to increase the sulfur content and improve the electrochemical performance. Meanwhile, the results of first principles calculation suggested that the increase of sulfur content of SPAN was derived from the delayed cyclization of polyacrylonitrile (PAN) by HBO. We also discovered when the additive amount of HBO was 1.5 % of PAN mass, the SPAN cathode material possessed high sulfur content up to 54.24 wt%, and delivered prominent reversible electrochemical performances of 714 mAh/g at 0.2C and 734 mAh/g at 0.1C with high Coulombic efficiency. In summary, we proposed a simple and easy method to improve sulfur content and introduced a new strategy for the design of high-sulfur content and high-performance SPAN cathode materials.