Li-O₂ batteries provide an attractive and potential strategy for energy conversion and storage with high specific energy densities. However, large over-potential in oxygen evolution reactions (OER) caused by the decomposition obstacles of Li₂O₂ seriously impedes its electrochemical performances. Herein, a novel N, O, S and F co-doping vesicular carbon was prepared by self-template pyrolysis method and used in Li-O₂ battery to tune the nucleation and decomposition of Li₂O₂. The introduction of F in the carbon matrix with suitable content can regulate the adsorption of intermediates, through which the morphology of Li₂O₂ can be controlled to film, favorable to its decomposition in charge process. The cathode based on the optimized F doped carbon vesicle exhibits improved electrochemical performances including a low over-potential, large capacity and a long-term stability. Density functional theory (DFT) results show that F and C in C–F bond has a strong interaction to Li and O in Li₂O₂, respectively, which can enhance the transfer of electrons from Li₂O₂ to the carbon matrix to generate hole polaron and thus accelerate the delithiation and decomposition of Li₂O₂. This work provides a new sight into understanding the mechanism of nucleation and decomposition of Li₂O₂ for the development of high-performance Li-O₂ batteries.

Li-O ₂电池为具有高比能量密度的能量转换和存储提供了一种有吸引力和潜在的策略。_{然而，Li 2} O ₂的分解障碍导致的析氧反应（OER）过电位严重阻碍了其电化学性能。在此，通过自模板热解法制备了一种新型的N、O、S和F共掺杂泡状碳，并用于Li-O ₂电池中以调节Li ₂ O ₂的成核和分解。在碳基体中引入合适含量的F可以调节中间体的吸附，从而改变Li ₂ O _{2的形貌。}可控制成膜，有利于其在充电过程中的分解。基于优化的 F 掺杂碳囊泡的正极表现出改善的电化学性能，包括低过电位、大容量和长期稳定性。密度泛函理论 (DFT) 结果表明，C-F 键中的 F 和 C 分别与 Li ₂ O ₂中的 Li 和 O 具有强相互作用，可以增强电子从 Li ₂ O ₂向碳基体的转移产生空穴极化子，从而加速Li ₂ O ₂的脱锂和分解。这项工作为理解 Li ₂ O的成核和分解机理提供了新的视角₂用于开发高性能Li-O ₂电池。