Single Atom Array Mimic on Ultrathin MOF Nanosheets Boosts the Safety and Life of Lithium–Sulfur Batteries

The development of Li-S batteries is largely impeded by the growth of Li dendrites and polysulfide shuttling. To solve these two problems simultaneously, herein the study reports a "single atom array mimic" on ultrathin metal organic framework (MOF) nanosheet-based bifunctional separator for achieving the highly safe and long life Li-S batteries. In the designed separator, the periodically arranged cobalt atoms coordinated with oxygen atoms (CoO4 moieties) exposed on the surface of ultrathin MOF nanosheets, "single atom array mimic", can greatly homogenize Li ion flux through the strong Li ion adsorption with O atoms at the interface between anode and separator, leading to stable Li striping/plating. Meantime, at the cathode side, the Co single atom array mimic serves as "traps" to suppress polysulfide shuttling by Lewis acid-base interaction. As a result, the Li-S coin cells with the bifunctional separator exhibit a long cycle life with an ultralow capacity decay of 0.07% per cycle over 600 cycles. Even with a high sulfur loading of 7.8 mg cm-2 , an areal capacity of 5.0 mAh cm-2 can be remained after 200 cycles. Moreover, the assembled Li-S pouch cell displays stable cycling performance under various bending angles, demonstrating the potential for practical applications.