The polysulfide shuttle phenomenon substantially deterioratesthe electrochemical performance of lithium?sulfur (Li?S) batteries, resultingin continued self-discharge and capacity fade during cycling. In this study, amesoscale analysis is presented to explore the mechanisms of self-dischargebehavior in the Li?S battery during the resting state. It is found that the self-discharge rate is determined by the sulfur solubility, desorption capability,diffusion kinetics, and reaction rate on the anode surface. Three regimes havebeen identified: desorption control, diffusion control, and charge transfercontrol. Correspondingly, strategies are suggested to increase the capacityretention, such as enhancing the binding of sulfur molecules to the host,reducing dissolved sulfur diffusivity, and improving the chemical stability ofactive materials with a Li metal anode. Furthermore, the use of an interlayerwith high diffusion barriers can effectively suppress the self-discharge rate due to the confinement effect.
Perpustakaan Digital ITB