Alleviating polarization by designing ultrasmall Li2S nanocrystals encapsulated in N-rich carbon as a cathode material for high-capacity, long-life Li–S batteries.

Lithium sulfide (Li₂S), which has a high theoretical specific capacity of 1166 mA h g⁻¹, has potential application in cathode materials because of its high safety and compatibility with lithium-free anodes for Li–S batteries. However, its low electron conductivity and lithium transfer cause significant polarization in Li₂S electrodes. Here, we demonstrate the use of ultrasmall Li₂S nanocrystals encapsulated in N-rich carbon (NRC) as a cathode material for Li–S batteries. By evaporating a mixture of polyacrylonitrile (PAN) and Li₂S in dimethylformamide (DMF) solution and then subjecting the mixture to carbonization, a nano-Li₂S@NRC composite with ultrasmall Li₂S well dispersed in its carbon matrix was successfully synthesized. The obviously lower potential barriers and excellent cycling performance of nano-Li₂S@NRC electrodes confirm their improved polarization because of the size effect of Li₂S nanocrystals and the good electron transfer between Li₂S and N-doped carbon. The nano-Li₂S@NRC cathode delivers a high initial specific capacity of 1046 mA h g⁻¹ of Li₂S (∼1503 mA h g⁻¹ of S) at 0.25C and 958 mA h g⁻¹ of Li₂S (∼1376 mA h g⁻¹ of S) at 0.5C with a favorable cycling performance with an ∼0.041% decay rate per cycle over 1000 cycles. [ABSTRACT FROM AUTHOR]