A Li-rich layered oxide cathode with negligible voltage decay

Luo, Dong; Zhu, He; Xia, Yi; Yin, Zijia; Qin, Yan; Li, Tianyi; Zhang, Qinghua; Gu, Lin; Peng, Yong; Zhang, Junwei; Wiaderek, Kamila M.; Huang, Yalan; Yang, Tingting; Tang, Yu; Lan, Si; Ren, Yang; Lu, Wenquan; Wolverton, Christopher M.; Liu, Qi

doi:10.1038/s41560-023-01289-6

DOE OSTI · 2574847

A Li-rich layered oxide cathode with negligible voltage decay

Luo, Dong·Zhu, He·Xia, Yi·Yin, Zijia·Qin, Yan·Li, Tianyi·Zhang, Qinghua·Gu, Lin·Peng, Yong·Zhang, Junwei·Wiaderek, Kamila M.·Huang, Yalan·Yang, Tingting·Tang, Yu·Lan, Si·Ren, Yang·Lu, Wenquan·Wolverton, Christopher M.·Liu, Qi

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Abstract

With high capacity at low cost, Li- and Mn-rich (LMR) layered oxides are a promising class of cathodes for next generation Li-ion batteries. However, substantial voltage decay during cycling, due to the unstable Li 2 MnO 3 honeycomb structure, is still an obstacle for their practical deployment. Here we report a Co-free LMR Li-ion battery cathode without voltage decay. The material has a composite structure consisting of layered LiTMO 2 and various stacked Li 2 MnO 3 components, where transition metal (TM) ions partially reside in the Li layers of Li 2 MnO 3 , serving as a “cap” to strengthen the stability of the honeycomb structure. This unique capped-honeycomb structure is persistent after high-voltage cycling and prevents TM migration and oxygen loss, as shown by experimental and computational results. Furthermore, this work demonstrates that the long-standing voltage decay problem in LMRs can be effectively eliminated by internally pinning the honeycomb structure, which opens an avenue to developing nextgeneration high-energy cathode materials.

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Luo, Dong, Zhu, He, Xia, Yi, Yin, Zijia, Qin, Yan, Li, Tianyi, Zhang, Qinghua, Gu, Lin, Peng, Yong, Zhang, Junwei, Wiaderek, Kamila M., Huang, Yalan, Yang, Tingting, Tang, Yu, Lan, Si, Ren, Yang, Lu, Wenquan, Wolverton, Christopher M., Liu, Qi. 2023-07-06. A Li-rich layered oxide cathode with negligible voltage decay. https://doi.org/10.1038/s41560-023-01289-6

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