A Nacre-Like Carbon Nanotube Sheet for High Performance Li-Polysulfide Batteries with High Sulfur Loading

Lithium-sulfur (Li-S) batteries are considered as one of the most promising energy storage systems for next-generation electric vehicles because of their high-energy density. However, the poor cyclic stability, especially at a high sulfur loading, is the major obstacles retarding their practical use. Inspired by the nacre structure of an abalone, a similar configuration consisting of layered carbon nanotube (CNT) matrix and compactly embedded sulfur is designed as the cathode for Li-S batteries, which are realized by a well-designed unidirectional freeze-drying approach. The compact and lamellar configuration with closely contacted neighboring CNT layers and the strong interaction between the highly conductive network and polysulfides have realized a high sulfur loading with significantly restrained polysulfide shuttling, resulting in a superior cyclic stability and an excellent rate performance for the produced Li-S batteries. Typically, with a sulfur loading of 5 mg cm⁻², the assembled batteries demonstrate discharge capacities of 1236 mAh g⁻¹ at 0.1 C, 498 mAh g⁻¹ at 2 C and moreover, when the sulfur loading is further increased to 10 mg cm⁻² coupling with a carbon-coated separator, a superhigh areal capacity of 11.0 mAh cm⁻² is achieved.