High-voltage lithium-metal batteries (LMBs) with LiCoO₂ (LCO) as the cathode have high volumetric and gravimetric energy densities. However, it remains a challenge for stable cycling of LCO >4.5 V_Li. Here we demonstrate that a rationally designed sulfonamide-based electrolyte can greatly improve the cycling stability at high voltages up to 4.7 V_Li by stabilizing the electrode–electrolyte interfaces (EEIs) on both the Li-metal anode (LMA) and high-voltage LCO cathode. With the sulfonamide-based electrolyte, commercial LCO cathodes retain 89% and 85% of their capacities after 200 and 100 cycles under high charging voltages of 4.55 V_Li and 4.6 V_Li, respectively, significantly outperforming traditional carbonate-based electrolytes. The surface degradation, impedance growth, and detrimental side reactions in terms of gas evolution and Co dissolution are well suppressed. Our work demonstrates a promising strategy for designing new electrolytes to realize high-energy Li||LCO batteries.

中文翻译：

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通过磺酰胺基电解质稳定电极-电解质界面以实现高压Li||LiCoO2电池

以 LiCoO ₂ (LCO) 作为阴极的高压锂金属电池 (LMB)具有高体积和重量能量密度。然而，LCO > 4.5 V _{Li 的}稳定循环仍然是一个挑战。在这里，我们证明了一种合理设计的磺酰胺基电解质可以通过稳定锂金属负极 (LMA) 和高压 LCO 上的电极-电解质界面 (EEIs)来大大提高高达 4.7 V _Li的高压循环稳定性阴极。使用基于磺酰胺的电解质，在 4.55 V _Li和 4.6 V _{Li 的}高充电电压下，商业 LCO 正极在 200 和 100 次循环后保持其容量的 89% 和 85%，分别显着优于传统的碳酸盐基电解质。表面降解、阻抗增长和气体逸出和 Co 溶解方面的有害副反应得到了很好的抑制。我们的工作展示了一种设计新电解质以实现高能 Li||LCO 电池的有前景的策略。