Structural Distortion Induced by Manganese Activation in a Lithium-Rich Layered Cathode

作者：Liguang Wang, Alvin Dai, Wenqian Xu, Sungsik Lee, Wonsuk Cha, Ross Harder, Tongchao Liu, Yang Ren, Geping Yin, Pengjian Zuo, Jun Wang, Jun Lü, Jiajun Wang · 发表于：Journal of the American Chemical Society · 年份：2020 · DOI：10.1021/jacs.0c05498 · 被引用次数：143 · 研究领域：Advancements in Battery Materials、Advanced Battery Materials and Technologies、Supercapacitor Materials and Fabrication

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 Li 2 MnO 3 -like phase during anionic redox and its role in battery performance and structural stability are still not fully understood. Here, we systematically probe microstructural evolution using spatially resolved synchrotron X-ray measurements and reveal an underlying interaction between the Li 2 MnO 3 -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 Li 2 MnO 3 -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.