Unlocking Li‒S chemistry via acoustic-induced entropy-driven electrolyte

Abstract Li‒S batteries offer a transformative alternative to present energy storage technologies. However, their practical viability is impeded by polysulfide shuttling and lithium dendrite formation. Electrolyte engineering seeks to solve these thorny issues, yet conventional approaches rely on internal, static or invasive modifications. Here we report an acoustic-induced entropy-driven electrolyte design to steer Li‒S chemistry, realizing enhanced sulfur conversion kinetics and sustained lithium working interface. With the aid of comprehensive instrumental and computational toolbox, it is shown that the entropy-driven state of the electrolyte propels the homogeneous nucleation of both sulfur and lithium species, along with dictating Li-ion desolvation process. The designed electrolyte at a lean dosage of 2.9 µL mg –1 readily enables a 1.1 Ah-level pouch cell with a delivered specific energy of 404.1 Wh kg -1 without packaging. Our electrolyte formulation concept using external field modulation offers an appealing solution to overcome key hurdles in Li–S technology toward high-performance devices.