High-entropy alloys (HEAs), as a special heterostructure, possesses many exclusive advantages, including the inherited merits from each component and the synergistic regulation of electronic properties, which has a great potential for catalyzing complicated redox conversions. Herein, we reveal that the synthesized nano-HEA plays a unique role in the multi-electron and multiphase conversions of lithium polysulfides (LiPSs) in lithium-sulfur batteries (Li-S). Owing to the strong affinity with LiPSs, nano-HEA enriches the activity of LiPSs around the electrode more than 17 times higher than that of the control sample (without nano-HEA addition), significantly reducing the concentration polarization. In addition, the activation polarization was greatly suppressed by the nano-HEA catalyst, which is demonstrated by the lower Tafel slope, higher exchange current density, and the larger current response from the scanning electrochemical microscopy (SECM). Besides, the smooth and continuous redistribution of surface charge is further revealed by DFT calculation, benefiting the multi-electron reactions of LiPSs. As a result, Li-S batteries assembled with nano-HEA modified separators delivered outstanding capacity retention rates of 83.3% (2 C after 500 cycles in coin cell) and 82% (0.1 C 150 cycles in pouch cell), respectively.

高熵合金（HEAs）作为一种特殊的异质结构，具有许多独特的优势，包括各组分的遗传优点和电子特性的协同调节，在催化复杂的氧化还原转化方面具有巨大潜力。在此，我们揭示了合成的纳米 HEA 在锂硫电池 (Li-S) 中多硫化锂 (LiPS) 的多电子和多相转换中起着独特的作用。由于与LiPSs的强亲和力，nano-HEA使电极周围LiPSs的活性比对照样品（未添加nano-HEA）高17倍以上，显着降低了浓度极化。此外，纳米 HEA 催化剂极大地抑制了活化极化，这由较低的 Tafel 斜率证明，更高的交换电流密度，以及来自扫描电化学显微镜 (SECM) 的更大电流响应。此外，DFT计算进一步揭示了表面电荷平滑连续的重新分布，有利于LiPS的多电子反应。因此，采用纳米 HEA 改性隔膜组装的 Li-S 电池分别具有 83.3%（纽扣电池 500 次循环后 2 C）和 82%（软包电池 0.1 C 150 次循环）的出色容量保持率。