Graphdiyne-Modified Polyimide Separator: A Polysulfide-Immobilizing Net Hinders the Shuttling of Polysulfides in Lithium–Sulfur Battery

Graphdiyne (GDY), a new type of carbon material with an electron-rich conjugated structure, has been investigated as a separator coating layer to enhance the electrochemical performance of lithium–sulfur (Li–S) battery. Acetylenic bond (−CC–CC−) and benzene ring in the GDY coating layer are experimentally verified to reversibly attract the soluble lithium polysulfides by chemical adsorption during cycling. Meanwhile, the shuttle effect of soluble polysulfides is further physically restricted by the GDY coating layer due to the evenly distributed pores (5.42 Å) and a consistent interlayer spacing (3.65 Å) of GDY. Moreover, GDY is a conducting carbon skeleton with high Li⁺ mobility that can improve the rate performance. Hence, Li–S battery with an as-prepared GDY coating layer shows excellent electrochemical performances including superior specific capacity, excellent rate performance, and low capacity attenuation rate. The high initial discharge capacity of 1648.5 mA h g^–1 at 0.1C and 819.5 mA h g^–1 even at a high rate of 2C is achieved by this novel separator. The initial capacity of 1112.9 mA h g^–1 at 0.5C is retained to 816.7 mA h g^–1 after 200 cycles with a low attenuation rate of 0.13% per cycle. Compared with other coated separators, these results show that the GDY coating layer endows the separator with superior electrochemical performances for Li–S battery.