Ti₃C₂T_x nanosheet@Cu/Fe-MOF separators for high-performance lithium-sulfur batteries: an experimental and density functional theory study

Lithium-sulfur (Li-S) batteries have attracted much attention due to their superior theoretical specific capacity and high theoretical energy density. However, rapid capacity fading originating from the shuttle effect, insulating the S cathode and the dendrite formation on the Li anode restrict the practical applications of Li-S batteries. Herein, we suggest novel coatings on glass fiber separators to satisfy all high-performance Li-S battery requirements. A conductive Ti3C2Tx (MXene) nanosheet/Fe-MOF or Ti3C2Tx (MXene) nanosheet/Cu-MOF layer was coated on a glass fiber separator to act as a polysulfide trapping layer. The MXene layer with high conductivity and polar surface functional groups could confine polysulfides and accelerate the redox conversions. The porous MOF layer acts as a Li ion sieve, thereby leading to the interception of polysulfides and mitigation of Li dendrite growth. The cells with the Cu-MOF/MXenes and Fe-MOF/MXene separators display superior capacities of 1100 and 1131 mA h g(-1 )after 300 cycles, respectively, whereas the cell with a pure glass fiber separator delivers a very low capacity of 309 mA h g(-1 ) after 300 cycles. With Fe-MOF/MXene and Cu-MOF/MXene configurations, the discharge capacity, coulombic efficiency, cycling stability, and electrochemical conversion reactions are significantly improved. Our ab initio calculations demonstrate that the MXene layer dissociates lithium polysulfides into adsorbed S and mobile Li ions, which explains the experimental findings.