作者
Xin He, Jue Wu, Zhuoying Zhu, Haodong Liu, Ning Li, Dong Zhou, Xu Hou, Jun Wang, Haowei Zhang, Dominic Bresser, Yanbao Fu, Matthew J Crafton, Bryan D McCloskey, Yan Chen, Ke An, Ping Liu, Anubhav Jain, Jie Li, Wanli Yang, Yong Yang, Martin Winter, Robert Kostecki
发表日期
2022
期刊
Energy & Environmental Science
卷号
15
期号
10
页码范围
4137-4147
出版商
Royal Society of Chemistry
简介
Although the two active redox centers in Li-rich cathodes, including the anionic and cationic contributions, can enable Li-ion batteries to achieve outstanding specific energy, their behaviors at different current densities have not been clarified. Here, we provide a comparative study of transition metals (TMs) and oxygen redox activities by directly accessing their oxidation states in Li-rich materials operated at very different current rates. Our data reveal that the oxidation of oxygen in the near-surface region is at the same level for electrodes cycled with a wide range of current rates, indicating a reaction gradient of lattice oxygen redox reactions. The oxidation process of lattice oxygen is found to be dynamically compatible with that of the TMs. Combining the results of first principles calculations and complementary experimental findings, we propose a detailed mechanism of structural distortion from octahedral Li to …
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