Unveiling the Electrocatalytic Activity of 1T'-MoSe₂ on Lithium-Polysulfide Conversion Reactions

The dissolution of intermediate lithium polysulfides (LiPS) into an electrolyte and their shuttling between the electrodes have been the primary bottlenecks for the commercialization of high-energy density lithium-sulfur (Li-S) batteries. While several two-dimensional (2D) materials have been deployed in recent years to mitigate these issues, their activity is strictly restricted to their edge-plane-based active sites. Herein, for the first time, we have explored a phase transformation phenomenon in a 2D material to enhance the number of active sites and electrocatalytic activity toward LiPS redox reactions. Detailed theoretical calculations demonstrate that phase transformation from the 2H to 1T' phase in a MoSe₂ material activates the basal planes that allow for LiPS adsorption. The corresponding transformation mechanism and LiPS adsorption capabilities of the as-formed 1T'-MoSe₂ were elucidated experimentally using microscopic and spectroscopic techniques. Further, the electrochemical evaluation of phase-transformed MoSe₂ revealed its strong electrocatalytic activity toward LiPS reduction and their oxidation reactions. The 1T'-MoSe₂-based cathode hosts for sulfur later provide a superior cycling performance of over 250 cycles with a capacity loss of only 0.15% per cycle along with an excellent Coulombic efficiency of 99.6%.