To meet the growing demand for global electrical energy storage, high‐energy‐density electrode materials are required for Li‐ion batteries. To overcome the limit of the theoretical energy density in conventional electrode materials based solely on the transition metal redox reaction, the oxygen redox reaction in electrode materials has become an essential component because it can further increase the energy density by providing additional available electrons. However, the increase in the contribution of the oxygen redox reaction in a material is still limited due to the lack of understanding its controlled parameters. Here, it is first proposed that Li‐transition metals (TMs) inter‐diffusion between the phases in Li‐rich materials can be a key parameter for controlling the oxygen redox reaction in Li‐rich materials. The resulting Li‐rich materials can achieve fully exploited oxygen redox reaction and thereby can deliver the highest reversible capacity leading to the highest energy density, ≈1100 Wh kg⁻¹ among Co‐free Li‐rich materials. The strategy of controlling Li/transition metals (TMs) inter‐diffusion between the phases in Li‐rich materials will provide feasible way for further achieving high‐energy‐density electrode materials via enhancing the oxygen redox reaction for high‐performance Li‐ion batteries.

中文翻译：

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不含钴的富锂材料中互扩散阳离子对高性能锂离子电池的充分利用氧还原反应

为了满足全球不断增长的电能存储需求，锂离子电池需要高能量密度的电极材料。为了克服仅基于过渡金属氧化还原反应的常规电极材料中理论能量密度的限制，电极材料中的氧氧化还原反应已成为必不可少的组成部分，因为它可以通过提供额外的可用电子来进一步提高能量密度。但是，由于缺乏对材料的控制参数的了解，材料中氧氧化还原反应的贡献增加仍然受到限制。在此，首次提出，富锂材料中各相之间的锂过渡金属（TMs）相互扩散可以作为控制富锂材料中氧还原反应的关键参数。不含钴的富锂材料中的^-1。控制富锂材料中各相之间锂/过渡金属（TMs）相互扩散的策略将通过增强高性能锂离子电池的氧还原反应，为进一步实现高能量密度电极材料提供可行的途径。