Pushing Lithium–Sulfur Batteries towards Practical Working Conditions through a Cathode–Electrolyte Synergy

摘要

Abstract The commercialization of lithium–sulfur (Li?S) batteries is still hindered by the unsatisfactory cell performance under practical working conditions, which is mainly caused by the sluggish cathode redox kinetics, severe polysulfide shuttling, and poor Li stripping/plating reversibility. Herein, we report an effective strategy by combining Se‐doped S hosted in an ordered macroporous framework with a highly fluorinated ether (HFE)‐based electrolyte to simultaneously address the aforementioned issues in both cathode and anode. A reversible and stable high areal capacity of >5.4?mAh?cm?2 with high Coulombic efficiency >99.2?% can be achieved under high areal Se/S loading (5.8?mg?cm?2), while the underlying mechanism was further revealed through synchrotron X‐ray probes and Time‐of‐Flight Secondary Ion Mass Spectrometry (ToF‐SIMS). The practical application potential was further evaluated at low (0?°C) and high (55?°C) temperatures under high areal Se/S loading (>5.0?mg?cm?2) and thin Li metal (40?μm).