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Lithium-sulfur (Li-S) batteries have been recognized as promising substitutes for current energy-storage technologies owing to their exceptional advantage in energy density. The main challenge in developing highly efficient and long-life Li-S batteries is simultaneously suppressing the shuttle effect and improving the redox kinetics. Polar host materials have desirable chemisorptive properties to localize the mobile polysulfide intermediates; however, the role of their electrical conductivity in the redox kinetics of subsequent electrochemical reactions is not fully understood. Conductive polar titanium carbides (TiC) are shown to increase the intrinsic activity towards liquid-liquid polysulfide interconversion and liquid-solid precipitation of lithium sulfides more than non-polar carbon and semiconducting titanium dioxides. The enhanced electrochemical kinetics on a polar conductor guided the design of novel hybrid host materials of TiC nanoparticles grown within a porous graphene framework (TiC@G). With a high sulfur loading of 3.5 mg cm , the TiC@G/sulfur composite cathode exhibited a substantially enhanced electrochemical performance.

A cooperative interface constructed by "lithiophilic" nitrogen-doped graphene frameworks and "sulfiphilic" nickel-iron layered double hydroxides (LDH@NG) is proposed to synergistically afford bifunctional Li and S binding to polysulfides, suppression of polysulfide shuttles, and electrocatalytic activity toward formation of lithium sulfides for high-performance lithium-sulfur batteries. LDH@NG enables high rate capability, long lifespan, and efficient stabilization of both sulfur and lithium electrodes.

High‐dielectric solvents were explored for enhancing the sulfur utilization in lithium–sulfur (Li−S) batteries, but their applications have been impeded by low stability at the lithium metal anode. Now a radical‐directed, lithium‐compatible, and strongly polysulfide‐solvating high‐dielectric electrolyte based on tetramethylurea is presented. Over 200 hours of cycling was realized in Li|Li symmetric cells, showing good compatibility of the tetramethylurea‐based electrolyte with lithium metal. The high solubility of short‐chain polysulfides, as well as the presence of active S3.− radicals, enabled pouch cells to deliver a discharge capacity of 1524 mAh g−1 and an energy density of 324 Wh kg−1. This finding suggests an alternative recipe to ether‐based electrolytes for Li−S batteries.