Alleviating the Polysulfide Shuttle Effect by Optimization of 3D Flower-Shaped Vanadium Dioxide for Lithium-Sulfur Batteries

Abstract

With the rapid development of portable devices and Energy Storage Systems (ESS), secondary batteries with high energy density and high capacity are in great demand. Among various candidates, Lithium-sulfur (Li-S) batteries have been considered for next-generation energy devices given their high theoretical capacity (1675 mAh g^-1) and energy density (2500 Wh kg^-1). However, the commercialization of Li-S batteries faces challenges due to sulfur’s low electrical conductivity and the shuttle effect, caused by the dissolution of lithium polysulfide intermediates in the electrolyte during the charge-discharge process. Herein, to resolve these problems, we report the fabrication of a vanadium dioxide (VO₂) composite via a simple hydrothermal method and optimize the structure of VO₂ for constructing an effective Multi-Walled Carbon Nano Tube (MWCNT) and 3D flower-shaped VO₂ (MWCNT@VO₂) binary sulfur host by a simple melt diffusion method. In particular, the polar VO₂ composite not only physically absorbs the soluble lithium polysulfides but also has strong chemical bonds with a higher affinity for lithium polysulfides, which act as a catalyst, enhancing electrochemical reversibility. Additionally, MWCNT improves sulfur’s poor electrical conductivity and buffers volume expansion during cycling. The designed S-MWCNT@VO₂ electrode also exhibits better capacity retention and cycling performance than a bare S-MWCNT electrode as a lithium polysulfide reservoir.