A quantitative analysis method of complex sulfide components for understanding initial capacity degradation mechanism in lithium-sulfur batteries

Abstract

Lithium-sulfur (Li-S) batteries are a strong contender for the new-generation battery system to meet the growing energy demand due to their significantly high energy density (2600 Wh/kg) and cost-effectiveness. However, the practical operating conditions yield an initial capacity of less than 80 % of the theoretical capacity, resulting in a limited lifespan and hindering broader application. What's worse, current mechanism, especially the evolution process of sulfides for the initial capacity degradation is not clear due to the practical difficulties of effective separation and detection of sulfur-containing components. Herein, we have developed an instrumental analysis method enabling graded leaching and quantitative determination of sulfur-containing components. This technology achieves a detection precision surpassing 99.11 %, addressing the inherent deficiency in calculating sulfur-containing components using the decrement method. Applying this method reveals that the presence of lithium polysulfides in the electrolyte (26.34 wt%) after discharging is the primary factor causing insufficient capacity utilization in Li-S batteries. This work not only demonstrates the unique behavior of Li-S batteries at high sulfur loading but also provides a systematic evaluation method to guide further research on high-energy-density batteries, and provides theoretical and technical support to promote the development of high-energy, long-life Li-S batteries.