Examining Performance Loss Mechanisms in Lithium-Ion Batteries with the High-Voltage Mn-Rich Spinel Positive Electrodes

Badami, Pavan P.; Trask, Stephen E.; Son, Seoung-Bum; Rodrigues, Marco-Tulio F.; Abraham, Daniel P.

doi:10.1149/1945-7111/ad3ad4

Title: Examining Performance Loss Mechanisms in Lithium-Ion Batteries with the High-Voltage Mn-Rich Spinel Positive Electrodes

Journal Article · 14 April 2024 · Journal of the Electrochemical Society

DOI: https://doi.org/10.1149/1945-7111/ad3ad4 · OSTI ID:2336818

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The high-voltage spinel, with the nominal composition of LiNi _0.5-x Mn _1.5+x O ₄ (LNMO), could be a sustainable alternative to the layered-oxide positive electrodes used in lithium-ion batteries. However, commercial acceptance has been limited as LNMO cells display rapid performance loss during cycling. To examine reasons for this loss we prepared cells with LNMO-based positive and either graphite or lithium titanate (LTO) based negative electrodes. Our initial cells displayed high impedance and rapid impedance rise during cycling. Adding single walled carbon nanotubes in the positive lowered initial cell impedance but impedance increased during cycling because of coating delamination from the Al foil. Using a primed Al current collector solved the delamination problem: cells with this current collector showed only a small impedance rise. Regarding capacity, cells with the LTO negative showed higher initial capacities and smaller fade. Our data indicate that cell capacity retention is determined by reduction reactions at the negative electrode that lower capacity and oxidation reactions at the positive electrode that increase capacity: both types of reactions deplete the cell electrolyte during extended cycling. All things considered, species generated at high voltages, either in the electrolyte or at the LNMO electrode, drive cell capacity fade.

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Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: NONE; AC02-06CH11357

OSTI ID:: 2336818

Alternate ID(s):: OSTI ID: 2333703; OSTI ID: 2497269

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 4 Vol. 171; ISSN 0013-4651

Publisher:: The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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