Structural Design of Electrocatalyst-Decorated MXenes on Sulfur Spheres for Lithium–Sulfur Batteries

Lithium-sulfur batteries (LSBs) are known to be potential next-generation energy storage devices. Recently, our group reported an LSB cathode made using sulfur spheres that has been spherically templated by MXene nanosheets decorated with CoSe2 nanoparticles, forming a "loose-templating" configuration. It was postulated that the minimal restacking of the outer nanoparticle-decorated MXene layer helps to enable facile ionic transport. However, as the nanosheets do not adhere conformally to the internal sphere's surface, such a configuration can be controversial, thus requiring a more systematic understanding. In this work, we report and quantify for the first time the independent and dependent variables involved in this morphology, allowing us to identify that having smaller nanoparticles resulted in better Li+ ion transport and enhanced electrochemical performances. The optimized cathode structure exhibited an initial specific capacity of 1274 mAh/g and a 0.06% decay rate per cycle at 0.5 C over 1000 cycles in LSBs.