Embedding Cobalt Atom Clusters in CNT‐Wired MoS₂ Tube‐in‐Tube Nanostructures with Enhanced Sulfur Immobilization and Catalyzation for Li–S Batteries

Abstract

Lithium-sulfur batteries are one of the most promising next-generation energy storage systems. The efficient interconversion between sulfur/lithium polysulfides and lithium sulfide is a performance-determining factor for lithium-sulfur batteries. Herein, a novel strategy to synthesize a unique tube-in-tube CNT-wired sulfur-deficient MoS₂ nanostructure embedding cobalt atom clusters as an efficient polysulfide regulator is successfully conducted in Li-S batteries. It is confirmed that encapsulating MWCNTs into hollow porous sulfur-deficient MoS₂ nanotubes embedded with metal cobalt clusters not only can accelerate electron transport and confine the dissolution of lithium polysulfide by physical/chemical adsorption, but also can catalyze the kinetics of polysulfide redox reactions. Based on DFT calculations, in situ spectroscopic techniques, and various electrochemical studies, catalytic effects of CNT/MoS₂ -Co nanocomposite in Li-S battery are deeply investigated for the first time. The CNT/MoS₂ -Co composite cathode exhibits a very remarkable rate capability (641 mAh g^-1 at 5.0 C) and excellent cycling stability (capacity decay rate of 0.050% per cycle at 5.0 C) even at high sulfur mass loading of 3.6 mg cm^-2 . More crucially, CNT/MoS₂ -Co tube-in-tube nanostructures present a superior specific capacity of 650 mAh g^-1 in a Li-S pouch cell at 0.2 C (4.0 mg cm^-2 ).