Multifunctional Ultrathin Ti₃C₂T_x MXene@CuCo₂O₄ /PE Separator for Ultra‐High‐Energy‐Density and Large‐Capacity Lithium‐Sulfur Pouch Cells

Abstract The shuttling of lithium polysulfides (LiPSs), sluggish reaction kinetics, and uncontrolled lithium deposition/stripping remain the main challenges in lithium‐sulfur batteries (LSBs), which are aggravated under practical working conditions, i.e., high sulfur loading and lean electrolyte in large‐capacity pouch cells. This study introduces a Ti₃C₂T_x MXene@CuCo₂O₄ (MCC) composite on a polyethylene (PE) separator to construct an ultrathin MXene@CuCo₂O₄/PE (MCCP) film. The MCCP functional separator can deliver superior LiPSs adsorption/catalysis capabilities via the MCC composite and regulate the Li⁺ deposition through a conductive Ti₃C₂T_x MXene framework, enhancing redox kinetics and cycling lifetime. When paired with sulfur/carbon (S/C) cathode and lithium metal anode, the resultant 10 Ah‐level pouch cell with the ultrathin MCCP separator achieves an energy density of 417 Wh kg⁻¹ based on the whole cell and a stable running of 100 cycles under practical operation conditions (cathode loading = 10.0 mg cm⁻², negative/positive areal capacity ratio (N/P ratio) = 2, and electrolyte/sulfur weight ratio (E/S ratio) = 2.6 µL mg⁻¹). Furthermore, through a systematic evaluation of the as‐prepared Li‐S pouch cell, the study unveils the operational and failure mechanisms of LSBs under practical conditions. The achievement of ultrahigh energy density in such a large‐capacity lithium‐sulfur pouch cell will accelerate the commercialization of LSBs.