Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 35, Pages 14966-14973Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c05498
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Funding
- Harbin Institute of Technology
- Natural Science Funds of Heilongjiang Province [ZD2019B001]
- DOE Office of Science [DE-AC02-06CH11357]
- National Synchrotron Light Source II, Brookhaven National Laboratory, under DOE [DESC0012704]
- National Natural Science Foundation of China [U1932205]
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The search for batteries with high energy density has highlighted lithium-rich manganese-based layered oxides due to their exceptionally high capacity. Although it is clear that both cationic and anionic redox are present in the charge compensation mechanism, the microstructural evolution of the Li2MnO3-like phase during anionic redox and its role in battery performance and structural stability are still not fully understood. Her; we systematically probe microstructural evolution using spatially resolved synchrotron X-ray measurements and reveal an underlying interaction between the Li2MnO3-like domains and bulk rhombohedral structure. Mn ion activation and a previously unobserved structural distortion are discovered at high voltages, and can be related to structural strain present in the Li2MnO3-like phase upon substantial lithium ion extraction. Moreover, we elucidate a correlation between this structural distortion and irreversible phase transitions by thermally perturbing delithiated samples. These insights highlight a pathway toward achieving high capacity cathode materials required for future commercial applications.
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