Chemomechanically Stable Ultrahigh-Ni Single-Crystalline Cathodes with Improved Oxygen Retention and Delayed Phase Degradations

Wang, Chunyang; Zhang, Rui; Siu, Carrie; Ge, Mingyuan; Kisslinger, Kim; Shin, Youngho; Xin, Huolin L.

doi:10.1021/acs.nanolett.1c03852

Chemomechanically Stable Ultrahigh-Ni Single-Crystalline Cathodes with Improved Oxygen Retention and Delayed Phase Degradations

Journal Article · Tue Nov 09 00:00:00 EST 2021 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.1c03852· OSTI ID:1835309

^[1]; Zhang, Rui ^[1]; Siu, Carrie ^[2]; Ge, Mingyuan ^[3]; Kisslinger, Kim ^[3]; Shin, Youngho ^[2]; ^[1]

Univ. of California, Irvine, CA (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)

The pressing demand in electrical vehicle (EV) markets for high-energy-density lithium-ion batteries (LIBs) requires further increasing the Ni content in high-Ni and low-Co cathodes. However, the commercialization of high-Ni cathodes is hindered by their intrinsic chemomechanical instabilities and fast capacity fade. The emerging single-crystalline strategy offers a promising solution, yet the operation and degradation mechanism of single-crystalline cathodes remain elusive, especially in the extremely challenging ultrahigh-Ni (Ni > 90%) regime whereby the phase transformation, oxygen loss, and mechanical instability are exacerbated with increased Ni content. Herein, we decipher the atomic-scale stabilization mechanism controlling the enhanced cycling performance of an ultrahigh-Ni single-crystalline cathode. We find that the charge/discharge inhomogeneity, the intergranular cracking, and oxygen-loss-related phase degradations that are prominent in ultrahigh-Ni polycrystalline cathodes are considerably suppressed in their single-crystalline counterparts, leading to improved chemomechanical and cycling stabilities of the single-crystalline cathodes. Furthermore, our work offers important guidance for designing next-generation single-crystalline cathodes for high-capacity, long-life LIBs.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; EE0008444; SC0012704; SC0021204

OSTI ID:: 1835309

Alternate ID(s):: OSTI ID: 1870393
OSTI ID: 1887546

Report Number(s):: BNL-223025-2022-JAAM; BNL-223311-2022-JAAM; 172322

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 22 Vol. 21; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Chemomechanically Stable Ultrahigh-Ni Single-Crystalline Cathodes with Improved Oxygen Retention and Delayed Phase Degradations

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