Unrecoverable lattice rotation governs structural degradation of single-crystalline cathodes

• 成果类型: Article
• 署名作者: Huang, Weiyuan; Liu, Tongchao; Yu, Lei; Wang, Jing; Zhou, Tao; Liu, Junxiang; Li, Tianyi; Amine, Rachid; Xiao, Xianghui; Ge, Mingyuan; Ma, Lu; Ehrlich, Steven N.; Holt, Martin V.; Wen, Jianguo; Amine, Khalil
• 署名单位: United States Department of Energy (DOE); Argonne National Laboratory; United States Department of Energy (DOE); Argonne National Laboratory; United States Department of Energy (DOE); Argonne National Laboratory; United States Department of Energy (DOE); Argonne National Laboratory; United States Department of Energy (DOE); Brookhaven National Laboratory
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-9197
• DOI: 10.1126/science.ado1675
• 发表日期: 2024-05-24
• 页码: 912-919
• 关键词: transition-metal oxide; rich

摘要

Transitioning from polycrystalline to single-crystalline nickel-rich cathodes has garnered considerable attention in both academia and industry, driven by advantages of high tap density and enhanced mechanical properties. However, cathodes with high nickel content (>70%) suffer from substantial capacity degradation, which poses a challenge to their commercial viability. Leveraging multiscale spatial resolution diffraction and imaging techniques, we observe that lattice rotations occur universally in single-crystalline cathodes and play a pivotal role in the structure degradation. These lattice rotations prove unrecoverable and govern the accumulation of adverse lattice distortions over repeated cycles, contributing to structural and mechanical degradation and fast capacity fade. These findings bridge the previous knowledge gap that exists in the mechanistic link between fast performance failure and atomic-scale structure degradation.