Developing single-site catalysts featuring maximum atom utilization efficiency is urgently desired to improve oxidation-reduction efficiency and cycling capability of lithium-oxygen batteries. Here, we report a green method to synthesize isolated cobalt atoms embedded ultrathin nitrogen-rich carbon as a dual-catalyst for lithium-oxygen batteries. The achieved electrode with maximized exposed atomic active sites is beneficial for tailoring formation/decomposition mechanisms of uniformly distributed nano-sized lithium peroxide during oxygen reduction/evolution reactions due to abundant cobalt-nitrogen coordinate catalytic sites, thus demonstrating greatly enhanced redox kinetics and efficiently ameliorated over-potentials. Critically, theoretical simulations disclose that rich cobalt-nitrogen moieties as the driving force centers can drastically enhance the intrinsic affinity of intermediate species and thus fundamentally tune the evolution mechanism of the size and distribution of final lithium peroxide. In the lithium-oxygen battery, the electrode affords remarkably decreased charge/discharge polarization (0.40 V) and long-term cyclability (260 cycles at 400 mA g⁻¹).

迫切需要开发具有最大原子利用效率的单中心催化剂来提高锂氧电池的氧化还原效率和循环能力。在这里，我们报告了一种绿色方法来合成嵌入超薄富氮碳的孤立钴原子作为锂氧电池的双催化剂。由于丰富的钴氮配位催化位​​点，所获得的具有最大化暴露原子活性位点的电极有利于在氧还原/放出反应过程中调整均匀分布的纳米尺寸过氧化锂的形成/分解机制，从而证明氧化还原动力学大大增强并有效改善超潜力。重要的是，理论模拟表明，丰富的钴氮部分作为驱动力中心可以极大地增强中间物质的内在亲和力，从而从根本上调整最终过氧化锂的尺寸和分布的演化机制。在锂氧电池中，该电极提供显着降低的充电/放电极化（0.40 V）和长期循环能力（400 mA g ^-1下260个循环）。