Mesoscale Elucidation of Surface Passivation in the Li–Sulfur Battery Cathode
We report the cathode surface passivation caused by Li 2 S precipitation adversely affects the performance of lithium-sulfur (Li-S) batteries. Li 2 S precipitation is a complicated mesoscale process involving adsorption, desorption and diffusion kinetics, which are affected profoundly by the reactant concentration and operating temperature. In this work, a mesoscale interfacial model is presented to study the growth of Li 2 S film on carbon cathode surface. Li 2 S film growth experiences nucleation, isolated Li 2 S island growth and island coalescence. The slow adsorption rate at small S 2- concentration inhibits the formation of nucleation seeds and the lateral growth of Li 2 S islands, which deters surface passivation. An appropriate operating temperature, especially in the medium-to-high temperature range, can also defer surface passivation. Fewer Li 2 S nucleation seeds form in such an operating temperature range, which facilitates heterogeneous growth and thereby inhibits the lateral growth of the Li 2 S film, which may also result in reduced surface passivation. Finally, the high specific surface area of the cathode microstructure is expected to mitigate the surface passivation.