Tuning functional two-dimensional MXene nanosheets to enable efficient sulfur utilization in lithium-sulfur batteries

Practicality of lithium-sulfur batteries is severely hindered by the notorious polysulfide-shuttle phenomenon, leading to rapid capacity fade. This issue is aggravated with increase in sulfur loading, causing low-coulombic efficiency and cycle life. Herein, we present a facile strategy to combine hydrophobic sulfur and hydrophilic, conductive Ti₃C₂T_z-MXene via one-step surface functionalization using di(hydrogenated tallow)benzylmethyl ammonium chloride (DHT). The latter renders the Ti₃C₂T_z surface hydrophobic, making it readily dispersible in sulfur dissolved in a carbon disulfide (CS₂) solvent. By evaporating the solvent, we conformally coat the DHT-Ti₃C₂T_z (DMX) with sulfur. The developed composite, with higher available active area, enables effective trapping of lithium polysulfides (LiPs) on the electroactive sites within the cathode, leading to improvement in electrochemical performance at higher sulfur loadings. The DMX/S cathodes function with high sulfur loading of ∼10.7 mg·cm⁻² and deliver a stable areal capacity of ∼7 mAh·cm⁻² for 150 cycles. Moreover, a DMX/S cathode in a pouch-cell configuration retains ∼770 mAh·g⁻¹ after ∼200 cycles at 0.2C (85.5% retention). Ex situ studies elucidate the nature of the LiPs-MXene interaction and the effect of surface functionalization towards improved performance.