Vertical Graphene Growth on LDH Nanosheets and Carbon Cloth Nanofibers with NiCo Nanoparticles as a Freestanding Host for High-Performance Lithium–Sulfur Batteries

Lithium–sulfur batteries have been recognized as one of the excellent candidates for next-generation energy storage batteries because of their high energy density and low cost and low pollution. However, lithium–sulfur batteries have been challenged by low conductivity, low sulfur utilization, poor cycle life, and the shuttle effect of polysulfides. To address these problems, we report here an independent mixed sulfur host. First, NiCoAl-layered double hydroxide (LDH) nanosheets were uniformly grown on carbon cloth (CC) by a hydrothermal method. Then, vertical graphene (VG) was uniformly vertically grown on the composite structures to form VG@LDH/CC by a plasma enhanced chemical vapor deposition (PECVD) method. Graphene and LDH nanosheets forming a three-dimensional mesh structure can effectively physically block lithium polysulfides, store singlet sulfur, and improve the conductivity of the cathode. In addition, during the growth of graphene, the Ni and Co ions in the LDH nanosheets are reduced to NiCo nanoparticles, which can enhance the chemical adsorption of polysulfides, thus effectively mitigating the “shuttle effect” and improving the electrical conductivity of the material. The lithium sulfur batteries with derived sulfur anodes (VG@LDH/CC-S) exhibited excellent electrochemical properties, including excellent rate performance (780.8 mAh g^–1 at 3C) and impressive cycling stability (capacity decay of about 0.0755% per cycle after 750 cycles at 0.5C).