Combined enhanced redox kinetics and physiochemical confinement in three-dimensionally ordered macro/mesoporous TiN...

Lithium-sulfur (Li-S) batteries with tremendous energy density possess great promise for the next-generation energy storage devices. Even though, the shuttle effect and sluggish redox kinetics of lithium polysulfides (LiPSs) seriously restrict practical applications of Li-S batteries. Herein, a three-dimensionally ordered macro/mesoporous TiN (3DOM TiN) nanostructure is established via using poly (methyl methacrylate) PMMA spheres as template. The interconnected macro/mesoporous channels are constructed to effectively alleviate the stacking of composite materials and render a large portion of inherent active sites exposed on the surface region. Moreover, TiN exhibits high electrical conductivity, which efficiently enhances charge-transfer kinetics and guarantees the favorable electrochemical performance of sulfur cathode. More importantly, the as-prepared 3DOM TiN suppresses the shuttle effect and improves the redox kinetics significantly due to strong affinity toward LiPSs. Attributed to these unique features, the S/3DOM TiN electrode achieves an ultrahigh initial discharge capacity of 1187 mAh g^-1at 0.2 C, and stable cycling performance of 552 mAh g^-1over 500 cycles at 1 C. Meanwhile, the discharge capacity retention of 701 mAh g^-1(3.5 mAh cm^-2) can be endowed for the S/3DOM TiN electrode under high sulfur loading of 5 mg cm^-2after 100 cycles at 0.1 C. Therefore, the 3DOM TiN nanostructure electrocatalyst provides a promising path for developing practically useable Li-S batteries.