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Electrocatalysts are an effective strategy to mitigate the shuttling effect of lithium polysulfides (LiPSs) and accelerate the redox kinetics of LiPSs in lithium-sulfur (Li-S) batteries. However, traditional electrocatalysts only have a single active site and often undergo structural collapse and aggregation during charging and discharging, resulting in reduced catalytic performance. Herein, the two-dimensional (2D) polar high-entropy La 0.71 Sr 0.29 Co 0.21 Ni 0.20 Fe 0.19 Cr 0.20 Cu 0.20 O 3 (LCO-HEO) nanosheets were rationally designed and successfully synthesized to address this issue. The distinct functional polar sites in LCO-HEOs were formed by the d - d orbital hybridization between spatially coupling adjacent transition metals, which can strengthen the dipole-dipole interaction between polar LCO-HEOs and polar LiPSs. 2D polar LCO-HEO nanosheets can efficiently capture and trigger the tandem catalysis of polar LiPSs during their sequential conversion. The S/LCO-HEO composite cathode exhibits a high specific capacity of 1161.1 mA h g −1 at 1.0 C, with an ultralow capacity attenuation rate of 0.036% per cycle over 1200 cycles, and achieves stable cycling for 1500 cycles even at 8.0 C. Furthermore, even with a high sulfur loading (5.5 mg cm −2 ) and a low electrolyte/sulfur (E/S) ratio (4.0 µL mg −1 ), the S/LCO-HEO composite cathode shows desirable sulfur utilization and good cycle stability. This work demonstrates the feasibility of high entropy-driven multiple distinct functional polar sites for high-rate and long-cycle Li-S batteries.
Wang et al. (Fri,) studied this question.