Manipulating Electrocatalytic Polysulfide Redox Kinetics by 1D Core–Shell Like Composite for Lithium–Sulfur Batteries

Abstract Although lithium–sulfur batteries have high theoretical energy density of 2600 Wh kg −1 , the sluggish redox kinetics of soluble liquid polysulfide intermediates during discharge and charge is one of the main reasons for their limited battery performance. Designing highly efficient electrocatalysts with a core–shell like structure for accelerating polysulfide conversion is vital for the development of Li–S batteries. Herein, core–shell MoSe 2 @C nanorods are proposed to manipulate electrocatalytic polysulfide redox kinetics, thereby improving the Li–S battery performance. The 1D MoSe 2 @C is synthesized via a facile hydrothermal and subsequent selenization reaction. The electrocatalysis of MoSe 2 is confirmed by the analysis of symmetric batteries, Tafel curves, changes of activation energy, and lithium‐ion diffusion. Density functional theory calculations also prove the low Gibbs free energy of the reaction pathway and the lithium‐ion diffusion barrier. Therefore, the Li–S batteries using MoSe 2 electrocatalyst exhibit an excellent rate performance of 560 mAh g −1 at 1 C with a high sulfur loading of 3.4 mg cm −2 and an areal capacity of 4.7 mAh cm −2 at a high sulfur loading of 4.7 mg cm −2 under lean electrolyte conditions. This work provides a deeper insight into regulation of polysulfide redox kinetics in electrocatalysts for Li–S batteries.