An Ultrahigh Capacity Graphite/Li(2)S Battery with Holey‐Li(2)S Nanoarchitectures

The pairing of high‐capacity Li(2)S cathode (1166 mAh g(−1)) and lithium‐free anode (LFA) provides an unparalleled potential in developing safe and energy‐dense next‐generation secondary batteries. However, the low utilization of the Li(2)S cathode and the lack of electrolytes compatible to both electrodes are impeding the development. Here, a novel graphite/Li(2)S battery system, which features a self‐assembled, holey‐Li(2)S nanoarchitecture and a stable solid electrolyte interface (SEI) on the graphite electrode, is reported. The holey structure on Li(2)S is beneficial in decomposing Li(2)S at the first charging process due to the enhanced Li ion extraction and transfer from the Li(2)S to the electrolyte. In addition, the concentrated dioxolane (DOL)‐rich electrolyte designed lowers the irreversible capacity loss for SEI formation. By using the combined strategies, the graphite/holey‐Li(2)S battery delivers an ultrahigh discharge capacity of 810 mAh g(−1) at 0.1 C (based on the mass of Li(2)S) and of 714 mAh g(−1) at 0.2 C. Moreover, it exhibits a reversible capacity of 300 mAh g(−1) after a record lifecycle of 600 cycles at 1 C. These results suggest the great potential of the designed LFA/holey‐Li(2)S batteries for practical use.