A novel sulfur@void@hydrogel yolk-shell particle with a high sulfur content for volume-accommodable and...

High-energy-density secondary batteries are required for many applications such as electric vehicles. Lithium-sulfur (Li-S) batteries are receiving broad attention because of their high theoretical energy density. However, the large volume change of sulfur during cycling, poor conductivity, and the shuttle effect of sulfides severely restrict the Li-storage performance of Li-S batteries. Herein, we present a novel core-shell nanocomposite consisting of a sulfur core and a hydrogel polypyrrole (PPy) shell, enabling an ultra-high sulfur content of about 98.4% within the composite, which greatly exceeds many other conventional composites obtained by coating sulfur onto some hosts. In addition, the void inside the core-shell structure effectively accommodates the volume change; the conductive PPy shell improves the conductivity of the composite; and PPy is able to adsorb polysulfides, suppressing the shuttle effect. After cycling for 200 cycles, the prepared S@void@PPy composite retains a stable capacity of 650 mAh g^-1, which is higher than the bare sulfur particles. The composite also exhibits a fast Li ion diffusion coefficient. Furthermore, the density functional theory calculations show the PPy shell is able to adsorb polysulfides efficiently, with a large adsorption energy and charge density transfer.