Accelerated Degradation in a Quasi-Single-Crystalline Layered Oxide Cathode for Lithium-Ion Batteries Caused by Residual Grain Boundaries

Zhang, Rui; Wang, Chunyang; Ge, Mingyuan; Xin, Huolin L.

doi:10.1021/acs.nanolett.2c01103

Accelerated Degradation in a Quasi-Single-Crystalline Layered Oxide Cathode for Lithium-Ion Batteries Caused by Residual Grain Boundaries

Journal Article · Tue Apr 26 00:00:00 EDT 2022 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.2c01103· OSTI ID:1887535

Zhang, Rui ^[1]; ^[1]; Ge, Mingyuan ^[2]; ^[1]

Univ. of California, Irvine, CA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

The rapidly growing demand of electrical vehicle (EV) requires high-energy-density lithium-ion batteries (LIBs) with excellent cycling stability and safety performance. However, conventional polycrystalline high-Ni cathodes severely suffer from intrinsic chemo-mechanical degradation and fast capacity fade. The emerging single-crystallization strategy offers a promising pathway to improve the chemo-mechanical stability, however, the single-crystallinity of the cathode is not always guaranteed and residual grain boundaries (GBs) could persist in nonideal synthesis conditions, leading to the formation of ‘quasi’ single-crystalline (QSC) cathodes. So far, there is a lack of understanding of the influence of these residual GBs on the electrochemical performance and structural stability. Herein, we investigate the degradation pathway of a QSC high-Ni cathode through transmission electron microscopy and X-ray techniques. The residual GBs caused by insufficient calcination time, dramatically exacerbate the cathode’s chemo-mechanical instability and cycling performance. Our work offers important guidance for the next-generation cathodes for long-life LIBs.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: SC0012704; EE0008444; SC0021204

OSTI ID:: 1887535

Report Number(s):: BNL-223299-2022-JAAM

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 9 Vol. 22; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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