Lithium-oxygen (Li-O₂) battery is considered as one of the most promising alternatives because of its ultrahigh theoretical energy density. However, their cycling stability is severely restricted by the uncontrollable dendrite growth and serious oxygen corrosion issue on Li surface. Herein, a sulfur-modified Li surface can be successfully constructed via chemical reaction of guanylthiourea (GTU) molecule on Li, which can induce the selectively fast decomposition of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) to form a smooth and stable inorganics-rich solid-electrolyte interphase (IR-SEI) during the subsequent electrochemical process. Such an IR-SEI cannot only offer a highly reversible and stable Li plating/stripping chemistry with dendrite-free property (10 mA cm⁻²-10 mAh cm⁻², > 0.5 years; 3 mA cm⁻²-3 mAh cm⁻², > 1 year) but also endows the Li metal an anti-oxygen corrosion function, thereby significantly improving the cycling stability of Li-O₂ batteries. This work provides a new idea for constructing functional solid-electrolyte interphase (SEI) to achieve highly stable Li metal anode.

锂氧（Li - O 2 _）电池因其超高的理论能量密度而被认为是最有前途的替代品之一。然而，锂表面上不可控的枝晶生长和严重的氧腐蚀问题严重限制了它们的循环稳定性。本文通过脒基硫脲（GTU）分子在锂上的化学反应成功构建硫修饰的锂表面，从而诱导双（三氟甲磺酰）亚胺锂（ LiTFSI ）的选择性快速分解。在随后的电化学过程中形成光滑稳定的富含无机物的固体电解质界面（IR-SEI）。这样的 IR-SEI 不仅可以提供高度可逆和稳定的锂电镀/剥离化学，而且具有无枝晶特性（10 mA cm ^-2 -10 mAh cm ^-2，> 0.5 年；3 mA cm ^-2 -3 mAh cm ^{- 2} , > 1 year) 还赋予Li金属抗氧腐蚀功能，从而显着提高Li-O ₂电池的循环稳定性。这项工作为构建功能性固体电解质界面（SEI）以实现高度稳定的锂金属负极提供了新思路。