Rational Design of a High‐Loading Polysulfide Cathode and a Thin‐Lithium Anode for Developing Lean‐Electrolyte Lithium–Sulfur Full Cells

Lithium-sulfur cells are attractive energy-storage systems because of their high energy density and the electrochemical utilization rates of the high-capacity lithium-metal anode and the low-cost sulfur cathode. The commercialization of high-performance lithium-sulfur cells with high discharge capacity and cyclic stability requires the optimization of practical cell-design parameters. Herein, a carbon structural material composed of a carbon nanotube skeleton entrapping conductive graphene is synthesized as an electrode substrate. The carbon structural material is optimized to develop a high-loading polysulfide cathode with a high sulfur loading capacity (6-12 mg cm-2 ), rate performance (C/10-C/2), and cyclic stability for 200 cycles. A thin lithium anode based on the carbon structural material is developed and exhibits long lithium stripping/plating stability for ≈2500 h with a lithium-ion transference number of 0.68. A lean-electrolyte lithium-sulfur full cell with a low electrolyte-to-sulfur ratio of 6 µL mg-1 is constructed with the designed high-loading polysulfide cathode and the thin lithium anode. The integration of all the critical cell-design parameters endows the lithium-sulfur full cell with a low negative-to-positive capacity ratio of 2.4, while exhibiting stable cyclability with an initial discharge capacity of 550 mAh g-1 and 60% capacity retention after 200 cycles.