Single O Hole Enables High Cycling Performance by Removing Thermodynamic and Kinetic Limitations

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.

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Publication Details

Journal
ACS Energy Letters
Published
2024-09-16
DOI
https://doi.org/10.1021/acsenergylett.4c02048
Citations
4
Primary Topic
Advanced Battery Technologies Research
Type
article
Field-Weighted Citation Impact
0.81

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Single O Hole Enables High Cycling Performance by Removing Thermodynamic and Kinetic Limitations

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Single O Hole Enables High Cycling Performance by Removing Thermodynamic and Kinetic Limitations

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article en
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Abstract

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.

ACS Energy LettersVol. 9(10)
Qingdao University (CN), University of Science and Technology of China (CN), Shanghai Jiao Tong University (CN), Chinese Academy of Sciences (CN), ShanghaiTech University (CN), Shanghai Advanced Research Institute (CN), Shanghai Institute of Microsystem and Information Technology (CN), National Synchrotron Radiation Laboratory (CN), University of Chinese Academy of Sciences (CN)
National Natural Science Foundation of China, National Key Research and Development Program of China
Affordable and clean energy
Openalex Percentile: Top 29%
Advanced Battery Technologies Research
0.81
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