Data for: Insights into the Overcharge-Induced Failure Mechanism of Lithium–Sulfur Batteries

In the pursuit of durable lithium–sulfur (Li–S) batteries, consider-able research has been devoted to extending cycle life by devel-oping advanced cathode materials. However, there exists acommon overcharging problem which leads to the disfunctionof Li–S batteries but has been largely overlooked. This studysystematically investigates the overcharging failure and its under-lying mechanisms. Experimental results reveal that failure comesfrom a soft internal short circuit (ISCs) caused by excessive lithiumdendrite growth, primarily driven by the sulfur cathode ratherthan the lithium anode. Electrochemical processes duringovercharging are examined, revealing the generation of a specificby-product. By analyzing the structural properties of the sulfurcathode such as topography and pore connectivity, and throughcombined experiments and theoretical simulations, the complexmechanisms through which the cathode influences lithium den-drite growth are elucidated. Finally, an effective "interlayer" strat-egy is proposed to mitigate the overcharging failure. This worksheds light on the overcharging mechanisms and emphasizesthe critical importance of cathode design in improving the safetyand reliability of Li–S batteries