Atomically Engineered Transition Metal Dichalcogenides for Liquid Polysulfide Adsorption and Their Effective Conversion in Li-S Batteries

Curtailing the polysulfide shuttle by anchoring the intermediate lithium polysulfides (LiPS) within the electrode structure is essential to impede the rapid capacity fade in lithium-sulfur (Li-S) batteries. While most of the contemporary Li-S cathode surfaces are capable of entrapping certain LiPS, developing a unique electrode material that can adsorb all the intermediates of sulfur redox is imperative. Herein, we report doping of the MoS 2 atomic structure with nickel (Ni@1TMoS 2 ) to modulate its absorption capability toward all LiPS and function as an electrocatalyst for Li-S redox. Detailed in situ and ex situ spectroscopic analysis revealed that both Ni and Mo sites chemically anchor all the intermediate of LiPS. Electrochemical studies and detailed kinetics analysis suggested that the conversion of liquid LiPS to solid end products are facilitated on the Ni@1TMoS 2 electrocatalytic surface. Further, the employment of the Ni@1TMoS 2 electrocatalyst enhances the Li + diffusion coefficient, thus contributing to the realization of a high capacity of 1107 mA h g –1 at 0.2C with a very limited capacity fade of 0.19% per cycle for over 100 cycles. In addition, this cathode demonstrated an excellent high rate and long cycling performance for over 300 cycles at a 1C rate.