Plasma and magnetron sputtering constructed dual-functional polysulfides barrier separator for high-performance lithium-sulfur batteries.

ABSTRACT

In order to fundamentally suppress the shuttle effect, N2 Plasma & Al2O3 magnetron sputtered separators (Al2O3@N-PP) are proposed for lithium-sulfur batteries (LSBs). Such a dual-functional polysulfides (LiPSs) barrier separator greatly inhibits the shuttle effect from the perspective of physical and chemical interaction. Physically, the inherently electronegative amorphous Al2O3 first achieves the repulsion of LiPSs to the sulfur cathode through the electrostatic repulsive effect, effectively preventing a large amount of soluble LiPSs from accumulating at the separator. At the same time, the Al2O3 film seals the shuttle channel of LiPSs to a certain extent. Chemically, N2 plasma-doped N heteroatoms form a lithium bond with Li+ in LiPSs to achieve the first step chemical adsorption and anchoring of LiPSs. When the LiPSs reaches the amorphous Al2O3 film, more stable chemical bonds are formed between Al3+ and S2-, Li+ and O2- to achieve more effective adsorption and anchoring of LiPSs. At 1C with a high sulfur loading up to 3-5 mg cm-2 the LSB contributes a specific charge capacity of 717.4 mAh g-1, with high retention rate up to 75.49 % after 450 cycles. The U-shaped electrolytic cell experiment and ultraviolet-visible spectrum experiment confirmed the LiPSs barrier function of the functional separator.