Three-Dimensional Graphene–Carbon Nanotube–Ni Hierarchical Architecture as a Polysulfide Trap for Lithium–Sulfur Batteries

Despite their high energy density and affordable cost compared to lithium-ion (Li-ion) batteries, lithium–sulfur (Li–S) batteries still endure from slow reaction kinetics and capacity loss induced by the insulating sulfur and severe polysulfide diffusion. To address these issues, we report here nickel nanoparticles filled in vertically grown carbon nanotubes (CNTs) on graphene sheets (graphene–CNT–nickel composite (Gr–CNT–Ni)) that are coated onto a polypropylene separator as a polysulfide trap for the construction of high-loading sulfur cathodes. The hierarchical porous framework of Gr–CNT physically entraps and immobilizes the active material sulfur, while the strong chemical interaction with Ni nanoparticles in Gr–CNT–Ni inhibits polysulfide diffusion. The covalently interconnected electron conduction channels and carbon shell-confined metal active sites provide feasible paths for the continual regeneration of active material during the charge–discharge process. Benefitting from these novel morphological and structural features, the Li–S cell with the Gr–CNT–Ni as a polysulfide trap demonstrates high specific capacity and good cycle life. This work provides new avenues for synergistically combining the advantages of hierarchical porous carbon architectures and metal active sites for the development of high-performance cathodes for Li–S batteries.