Single-Atomic Dispersion of Fe and Co Supported on Reduced Graphene Oxide for High-Performance Lithium-Sulfur Batteries.

High theoretical energy density and low cost make lithium-sulfur (LSB) batteries a promising system for next-generation energy storage. LSB performance largely depends on efficient reversible conversion of elemental sulfur to LiS. Here, well-designed sulfur host materials including Fe or Co single atoms embedded on N-doped reduced graphene oxide (MNC/G with M = Fe or Co) are proposed to tackle the LSB challenges and enhance the electrochemical performance. Using a combination of Mössbauer spectroscopy and high-resolution scanning electron microscopy, the atomic dispersion of Co and Fe was revealed up to relatively high mass loadings. After optimization of the electrolyte/sulfur (E/S) ratio, FeNC/G shows the most promising cycle performance combining a constant high discharge capacity at low E/S values with the lowest polarization. In particular, the material FeNC/G@S with a high sulfur loading (9.4 mg cm) delivers a high area capacity of 7.7 mAh cm under lean electrolyte conditions (6 mL g).