Probing the atomic interaction between zinc clusters and defective carbon in promoting the wide temperature applications of lithium-sulfur battery

Abstract Suppressing the dissolution and accelerating conversion kinetics of intermediate polysulfides are central to the practical usage of lithium−sulfur (Li–S) battery in a wide temperature range. Herein, an atomic engineering strategy is innovatively proposed to constructing a sulfur host consisting of chemical-anchoring zinc atomic cluster within double layer N-doped carbon matrix (ZnAC CM@CL) for addressing concerns. The as-prepared ZnAC CM@CL@S can deliver capacity as high as 1451 mAh g−1 at 0.2 C with electrolyte/sulfur ratio (E/S ratio) of 5.5 μL mg−1 and maintain 749 mAh g−1 after 1200 cycles (fading rate of 0.021% per cycle) at 5 C. Remarkably, the reversible capacity holds 627 mAh g−1 at 0.2 C at the −25 ℃. By a further combination analysis of electron holography (EH) and geometry phase analysis (GPA), the outstanding performance is revealed to be mainly traced to synergistic effect of the polarity N-doped multi-layer carbon matrix and internal periodical charge field induced by atomic strain, greatly enhancing the capability towards on the immobilization and conversion of intermediate polysulfides. More importantly, such an interplay also renders the strongly coupled cathode achieve a high area specific capacity of 8.71 mAh cm−2 even the area sulfur loading obtain to 7.34 mg cm−2. This atomic-level engineering strategy might shed light on the novel insights on the design of high performance for sulfur hosts.