High-Entropy Oxide Heterostructure-Boosted Bidirectional Electrocatalysis in Lithium-Sulfur Batteries

Despite the advantageous features of high theoretical specific capacity (1675 mA h g^-1) and low production costs, lithium-sulfur batteries have faced obstacles in achieving commercial fabrication, primarily due to sluggish reaction kinetics and the challenging shuttle effect. To address these issues, a novel high-entropy heterojunction interlayer, HEO@CC, was developed, which controllably grew homogeneous FeCoNiO-MnCrO (HEO) heterojunction particles onto carbon cloth. Consequently, HEO@CC generates multimetal active sites and a structure with low intrinsic resistance, enhancing the polysulfide anchoring capacity, accelerating the redox kinetics of Li₂S, and physically impeding polysulfide shuttling. As analyzed by differential radial transmission (DRT) techniques, HEO@CC facilitates rapid anchoring ability and conversion capability of soluble polysulfides. This integration leads to a reduction in charge transfer impedance, improves sulfur utilization, and enhances Li⁺ diffusion. During the rate capability tests, the HEO@CC battery exhibited a substantial capacity retention of 622.79 mA h g^-1 even after 500 cycles, demonstrating an average weekly capacity decay rate of only 0.029%. This research introduces innovative perspectives on the design of high-entropy heterostructured bidirectional catalytic interlayers and their catalytic mechanism, promoting the progress of high-capacity energy storage technologies.