Lithium–oxygen (Li–O₂) batteries have attracted tremendous attention due to their high specific energy density. However, their sluggish conversion kinetics and detrimental parasitic reactions would deteriorate the lifespan of batteries. Herein, a combined density functional theory (DFT) calculation and experimental approach is carried out to design an efficient cathode electrocatalyst for Li–O₂ batteries. A self-supporting film of Ru clusters anchored on Magnéli phase Ti₄O₇ enriched with oxygen vacancy (Ru/Ti₄O₇) is fabricated upon electrospinning and carbothermal reduction. In such a synergistic configuration of Ru/Ti₄O₇ hybrid film, the strong metal-support interaction (SMSI) between Ru and Ti₄O₇ can improve the charge transfer at the interface and enhance the adsorption energy of intermediates, accelerating the reaction kinetics of the formation/decomposition of Li₂O₂. Benefitting from this SMSI, the electrochemical stability of Ru/Ti₄O₇ over cycling is also enhanced. As a result, as-prepared Ru/Ti₄O₇ cathodes could realize excellent electrochemical performance, including high specific capacity (11000 mAh g^–1), low discharge/charge polarization (0.36 V), long lifespan (> 100 cycles) and superior rate capability. Furthermore, a flexible Li–O₂ pouch cell, constructed with as-fabricated Ru/Ti₄O₇ film cathode, lithium foil anode and GPE, can exert an impressive areal capacity of 5 mAh cm^–2 with a low voltage gap of 0.82 V in ambient air. This work suggests that the activity of catalysts can be significantly enhanced with interfacial modification, offering an efficient approach for rational designing of electrocatalysts for use in Li–air batteries and beyond.

锂-氧（Li-O ₂）电池由于其高比能量密度而引起了极大的关注。然而，它们缓慢的转换动力学和有害的寄生反应会缩短电池的寿命。在此，采用组合密度泛函理论 (DFT) 计算和实验方法来设计用于 Li-O ₂电池的高效正极电催化剂。通过静电纺丝和碳热还原制备了锚定在富含氧空位的 Magnéli 相 Ti ₄ O _{7 (Ru/Ti 4} O ₇ )上的 Ru 簇自支撑薄膜。_{在这样的Ru/Ti 4} O ₇协同构型中_{杂化薄膜中，Ru和Ti 4} O ₇之间的强金属-载体相互作用（SMSI）可以改善界面处的电荷转移，提高中间体的吸附能，加速Li ₂ O ₂形成/分解的反应动力学。受益于这种 SMSI，Ru/Ti ₄ O ₇的循环电化学稳定性也得到了增强。因此，所制备的 Ru/Ti ₄ O ₇正极可以实现优异的电化学性能，包括高比容量（11000 mAh g ^–1)、低放电/充电极化 (0.36 V)、长寿命 (> 100 次循环) 和卓越的倍率能力。此外，由预制的 Ru/Ti ₄ O ₇薄膜阴极、锂箔阳极和 GPE构成的柔性 Li-O _{2软包电池可以发挥令人印象深刻的 5 mAh cm} ^-2的面积容量和 0.82 的低电压间隙。环境空气中的 V。这项工作表明，通过界面改性可以显着提高催化剂的活性，为合理设计用于锂空气电池及其他领域的电催化剂提供了一种有效的方法。