Porous Carbon Cloth@CoSe2 as Kinetics‐Enhanced and High‐Loading Integrated Sulfur Host for Lithium–Sulfur Batteries

Abstract Carbon cloth (CC) possesses great potential as a sulfur host because of its excellent conductivity, flexibility, and easily modified free‐standing structure. However, the previous works do not take full advantage of CC except for the role of support and current collector. The smooth surface, small specific surface area, and poor binding force between coating materials and CC matrix are unfavorable for loading coating materials. The slow redox kinetics and low sulfur loading of sulfur cathodes still seriously restrict the development of Lithium–Sulfur (Li–S) batteries. Herein, the porous carbon cloth loading cobalt selenide (PCC@CoSe 2 ) is constructed as an integrated sulfur host through a pore‐creating and selenylation strategy. The pore‐creating engineering greatly optimizes the 3D pore structure of CC to raise the sulfur and catalyst loading and provides enough space to accommodate the volume change of sulfur species. In addition, CoSe 2 particles as nano‐catalyst units embedded in PCC can effectively adsorb‐catalyze polysulfides and improve the reaction kinetics. The resulting integrated sulfur cathode has realized the high‐efficiency polysulfide catalytic conversion and fast lithium ion migration, significantly enhancing redox kinetics and sulfur loading.