Lithium-rich layered oxides involving both transition metal and oxygen redox have received widespread attention due to their high energy density. However, the participation of oxygen redox in charge compensation generally leads to significant voltage decay and capacity fade, largely because of the dimerization of lattice oxygen. Therefore, tunability and stabilization of O redox configuration become crucial. In this study, the stability of the multiple forms of oxygen redox and the resulting role in cycling performance have been comparatively studied. A stabilized single O hole state has been identified experimentally for the first time not only in the first cycle but also in the long term cycle, in sharp contrast to the case of O dimer. Moreover, the superiority of the O hole can also be reflected in removing kinetic limitations. These findings may open new horizons for offering stable and high capacity via regulation of specific oxygen-redox forms.

中文翻译：

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单 O 孔消除热力学和动力学限制，实现高循环性能


涉及过渡金属和氧氧化还原的富锂层状氧化物由于其高能量密度而受到广泛关注。然而，氧氧化还原参与电荷补偿通常会导致显着的电压衰减和容量衰减，这主要是由于晶格氧的二聚化。因此，O氧化还原构型的可调性和稳定性变得至关重要。在本研究中，对多种形式的氧氧化还原的稳定性及其对循环性能的作用进行了比较研究。首次通过实验鉴定出稳定的单 O 空穴状态，不仅在第一个循环中，而且在长期循环中，与 O 二聚体的情况形成鲜明对比。此外，O孔的优越性还可以体现在消除动力学限制上。这些发现可能为通过调节特定的氧氧化还原形式提供稳定和高容量开辟新的视野。