especially the sluggish dissociation kinetics of Li 2 O 2 , which lead to high charge overpotential and undesirable parasitic reactions. [12][13][14][15] Considerable parasitic reactions are largely detrimental to the reversible Li 2 O 2 formation/decomposition, which in turn results in low round-trip efficiency and inferior rechargeability for Li-O 2 batteries. [16][17][18][19] Therefore, a rational design of efficient electrocatalysts toward decreasing overpotential, enhancing round-trip efficiency, and improving cycling stability is one of the significant strategies to solve the problems for Li-O 2 batteries.To facilitate the reversible decomposition of Li 2 O 2 , numerous efforts have been devoted to explore the cathode catalysts, including carbons, [20][21][22][23] precious metals, [24][25][26][27][28] and nonprecious metal oxides. [29][30][31][32] Among all the candidates explored, palladium [12,33,34] and its oxides [35] have shown some promise in decreasing charge overpotential and enhancing round-trip efficiency for Li-O 2 batteries. A common problem of these studies is that excessive palladium is used among solid catalysts, which leads to low utilization of active sites. The scarcity and high cost of palladium, however, have severely restricted its practical applications as a cathode catalyst for Li-O 2 batteries. Therefore, it is of crucial importance to maximize its accessible active sites to improve the catalytic activity by regulating the inherent properties of the catalysts. Owing to the utmost utilization efficiency of atoms and unique electronic properties, single-atom catalysts have exhibited superior catalytic activity in the fields of catalysis, including fuel cells, [36,37] water electrolysis [38,39] and O 2 /CO 2 /N 2 reduction reactions, [40][41][42][43] and so on. Nevertheless, relatively only a few studies involving single-atom catalysts in aprotic Li-O 2 batteries were reported. [44][45][46] For example, Hu et al. lowered the overpotential using Ru single-atoms anchored on nitrogen-doped porous carbon (Ru SAs-NC) as a cathode catalyst for Li−O 2 batteries. [44] Xu et al tuned Li 2 O 2 formation and decomposition routes with a single atom Co catalyst. [45] Yin et al fabricated isolated cobalt atoms embedded in ultrathin nitrogen-rich carbon (Co-SAs/N-C) and the redox kinetics is enhanced. [46] Single-atom catalysts have indeed exhibited some prospects in aprotic Li-O 2 batteries, but the overpotential is still not low enough, especially the charge potential is not stable. The charge potential usually demonstrates an obvious decrease in the initial charge state but it rises a lot with the increase of capacity or the charge-discharge cycles. Therefore, how to further effectively reduce the charge potentialThe critical challenge for Li-O 2 batteries lies in the large charge overpotential, leading to undesirable side reactions and inferior cycle stability. Singleatom catalysts have shown promising prospects in expediting the kinetics of oxygen evolution reaction (OER) for Li-O 2 batteries. Ho...