Promoting the Transformation of Li₂S₂ to Li₂S: Significantly Increasing Utilization of Active Materials for High‐Sulfur‐Loading Li–S Batteries

Abstract

Lithium-sulfur (Li-S) batteries with high sulfur loading are urgently required in order to take advantage of their high theoretical energy density. Ether-based Li-S batteries involve sophisticated multistep solid-liquid-solid-solid electrochemical reaction mechanisms. Recently, studies on Li-S batteries have widely focused on the initial solid (sulfur)-liquid (soluble polysulfide)-solid (Li₂ S₂ ) conversion reactions, which contribute to the first 50% of the theoretical capacity of the Li-S batteries. Nonetheless, the sluggish kinetics of the solid-solid conversion from solid-state intermediate product Li₂ S₂ to the final discharge product Li₂ S (corresponding to the last 50% of the theoretical capacity) leads to the premature end of discharge, resulting in low discharge capacity output and low sulfur utilization. To tackle the aforementioned issue, a catalyst of amorphous cobalt sulfide (CoS₃ ) is proposed to decrease the dissociation energy of Li₂ S₂ and propel the electrochemical transformation of Li₂ S₂ to Li₂ S. The CoS₃ catalyst plays a critical role in improving the sulfur utilization, especially in high-loading sulfur cathodes (3-10 mg cm^-2 ). Accordingly, the Li₂ S/Li₂ S₂ ratio in the discharge products increased to 5.60/1 from 1/1.63 with CoS₃ catalyst, resulting in a sulfur utilization increase of 20% (335 mAh g^-1 ) compared to the counterpart sulfur electrode without CoS₃ .