Deconvoluting sources of failure in lithium metal batteries containing NMC and PEO-based electrolytes

Hawley, William; Du, Zhijia; Kukay, Alexander; Dudney, Nancy; Westover, Andrew; Li, Jianlin

doi:10.1016/j.electacta.2021.139579

Title: Deconvoluting sources of failure in lithium metal batteries containing NMC and PEO-based electrolytes

Journal Article · 01 February 2022 · Electrochimica Acta

DOI: https://doi.org/10.1016/j.electacta.2021.139579 · OSTI ID:1840192

Hawley, William ^[1];

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center for Interdisciplinary Research and Graduate Education
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Solid-state lithium metal batteries (SSLMBs) containing polyethylene oxide (PEO)-derived polymer electrolytes and high-voltage (> 4 V vs. Li/Li⁺) cathode materials suffer from three sources of failure: (1) instability between the polymer electrolyte and cathode at high voltage, (2) instability of the polymer electrolyte with Li metal, and (3) poorly-designed cathodes. In this study, these three sources of failure are deconvoluted by studying Ni-rich LiNi_xMn_yCo_1-x-yO₂ (NMC, x ≥ 0.6) cathodes and a gel polymer electrolyte (GPE) derived from PEO. Initial cycling data reveals that rapid capacity fade occurs regardless of whether soft short circuits form due to Li dendrites. Cyclic voltammetry scans on cells featuring a Li metal electrode, GPE, and a NMC811 electrode free of additives suggest that there are no runaway reactions between the GPE and NMC811 up to 4.5 V vs. Li/Li⁺. Cathode/cathode symmetric cell cycling demonstrates that Li metal reactivity is a prime source of failure, though a poorly-designed cathode leads to subpar performance. A cathode with single-crystal NMC particles was demonstrated to achieve better initial capacity and longer cycle life, indicating room for improvement in SSLMB cathode design. Therefore, the sources of failure as enumerated may be ranked as follows from most to least concerning: 2 > 3 > 1.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1840192

Journal Information:: Electrochimica Acta, Journal Name: Electrochimica Acta Vol. 404; ISSN 0013-4686

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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