Electrocatalytically reducing the energy barrier for Li₂S deposition/dissociation is a promising strategy for high-rate Li-S batteries. However, the catalytic sites would be covered by the insulating Li₂S product during discharge, which deteriorates the catalytic activity. Here, suggested by first-principles calculations, single-atom copper (SA-Cu) was screened out to endow the insulator-to-metal transition of adsorbed Li₂S in view of the electronic structure. In addition to the thermodynamically reduced redox energy barrier, metallic Li₂S nuclei deposited on SA-Cu decorated nitrogen-doped carbon fiber foam (SA-Cu@NCNF) with favorable electronic transport present 3D spherical clusters rather than conventional 2D lateral morphology by continuous 3D nucleation and growth. The Li₂S deposition capacity and the catalytic efficiency of Li₂S-covered catalytic sites are thus greatly improved. As a result, SA-Cu@NCNF based Li-S cells with a sulfur loading of 4 mg cm⁻² retained an areal capacity of 1.60 mAh cm⁻² at 5 C after 500 cycles (0.038% decay per cycle). A competitive areal capacity of 8.44 mAh cm⁻² was obtained at 0.2 C with a sulfur loading of 10 mg cm⁻². The demonstration of the distinctive design of catalysts to adjust the electronic structure of adsorbed Li₂S paves the way for developing high-rate and long-life Li-S batteries.

电催化降低 Li ₂ S 沉积/解离的能垒是高倍率 Li-S 电池的一种有前途的策略。然而，在放电过程中，催化位点会被绝缘的Li ₂ S产物覆盖，从而降低催化活性。在这里，根据第一性原理计算，考虑到电子结构，筛选出单原子铜 (SA-Cu) 以赋予吸附的 Li ₂ S 的绝缘体到金属的转变。除了热力学降低的氧化还原能垒，金属 Li ₂沉积在 SA-Cu 装饰的氮掺杂碳纤维泡沫 (SA-Cu@NCNF) 上的 S 核具有良好的电子传输，呈现 3D 球形簇，而不是通过连续 3D 成核​​和生长的传统 2D 横向形态。从而大大提高了Li ₂ S 的沉积能力和Li _{2 S 覆盖的催化位点的催化效率。}结果，基于 SA-Cu@NCNF 的 Li-S 电池，硫负载量为 4 mg cm ^-2，在 5 C 时，在 500 次循环后（每循环衰减 0.038%）保持了 1.60 mAh cm ^-2的面积容量。^{在 0.2 C 和 10 mg cm -2}的硫负载下获得了 8.44 mAh cm ^-2的有竞争力的面积容量. 展示了用于调整吸附Li ₂ S电子结构的催化剂的独特设计，为开发高倍率和长寿命的Li-S电池铺平了道路。