Unrecoverable lattice rotation governs structural degradation of single-crystalline cathodes

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

doi:10.1126/science.ado1675

Title: Unrecoverable lattice rotation governs structural degradation of single-crystalline cathodes

Journal Article · 23 May 2024 · Science

DOI: https://doi.org/10.1126/science.ado1675 · OSTI ID:2432580

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Argonne National Laboratory (ANL), Argonne, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

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. Here, 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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; SC0012704

OSTI ID:: 2432580

Report Number(s):: BNL--225960-2024-JAAM

Journal Information:: Science, Journal Name: Science Journal Issue: 6698 Vol. 384; ISSN 0036-8075

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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