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

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 (Li2S2) 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 Li2S2 to the final discharge product Li2S (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 Li2S2 and propel the electrochemical transformation of Li2S2 to Li2S. 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 Li2S/Li2S2 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.