Coupling between oxygen redox and cation migration explains unusual electrochemistry in lithium-rich layered oxides
- Coupling between oxygen redox and cation migration explains unusual electrochemistry in lithium-rich layered oxides
- 홍지현; William E. Gent; 임기필; Yufeng Liang; Qinghao Li; Taylor Barnes; 안성진; Kevin H. Stone; Mitchell McIntire; Jay Hyok Song; Yiyang Li; Apurva Mehta; Stefano Ermon; Tolek Tyliszczak; David Kilcoyne; David Vine; 박진환; 두석광; Michael F. Toney; Wanli Yang; David Prendergast; William C. Chueh
- Issue Date
- Nature Communications
- VOL 8, 2091
- Lithium-rich layered transition metal oxide positive electrodes offer access to anion redox at high potentials, thereby promising high energy densities for lithium-ion batteries. However, anion redox is also associated with several unfavorable electrochemical properties, such as open-circuit voltage hysteresis. Here we reveal that in Li1.17-xNi0.21Co0.08Mn0.54O2, these properties arise from a strong coupling between anion redox and cation migration. We combine various X-ray spectroscopic, microscopic, and structural probes to show that partially reversible transition metal migration decreases the potential of the bulk oxygen redox couple by > 1 V, leading to a reordering in the anionic and cationic redox potentials during cycling. First principles calculations show that this is due to the drastic change in the local oxygen coordination environments associated with the transition metal migration. We propose that this mechanism is involved in stabilizing the oxygen redox couple, which we observe spectroscopically to persist for 500 charge/discharge cycles.
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