Operando video microscopy of Li plating and re-intercalation on graphite anodes during fast charging

Chen, Yuxin; Chen, Kuan-Hung; Sanchez, Adrian J.; Kazyak, Eric; Goel, Vishwas; Gorlin, Yelena; Christensen, Jake; Thornton, Katsuyo; Dasgupta, Neil P.

doi:10.1039/d1ta06023f

Title: Operando video microscopy of Li plating and re-intercalation on graphite anodes during fast charging

Journal Article · Mon Oct 18 00:00:00 EDT 2021 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/d1ta06023f· OSTI ID:1924793

Chen, Yuxin ^[1]; Chen, Kuan-Hung ^[1]; Sanchez, Adrian J. ^[1];

^[1]; Goel, Vishwas ^[1];

^[2];

^[2]; Thornton, Katsuyo ^[1];

^[1]

Univ. of Michigan, Ann Arbor, MI (United States)
Robert Bosch LLC, Sunnyvale, CA (United States)

Despite the demand for fast-charging lithium (Li)-ion batteries, high-energy-density batteries with thick graphite anodes are limited by Li plating when charging at >4C rates. In this work, plan-view operando video microscopy is applied on >3 mA h cm^–2 calendared graphite electrodes to study the dynamic evolution of local state-of-charge (SoC) and Li plating during fast charging. This technique allows for visualization of the spatial heterogeneity in SoC across the electrode, nucleation and growth of Li filaments, Li re-intercalation into graphite, “dead Li” formation, and SoC equilibration. The operando microscopy analysis is complemented by ex situ imaging of through-plane gradients in SoC to gain a three-dimensional visualization of spatial heterogeneity. We demonstrate that (1) Li plating preferentially nucleates on the graphite particles that lithiate fastest during fast charging; (2) the onset of Li plating correlates with the local minimum of the graphite electrode potential; (3) galvanic corrosion currents are responsible for Li re-intercalation, dead Li formation, and SoC re-equilibration after fast charging; and (4) electrochemical signatures during OCV rest or discharge are associated with Li re-intercalation into graphite. Furthermore, this work provides insight into the Li–graphite interactions at the composite electrode level and can be used to inform strategies to diagnose and mitigate Li plating during fast charging.

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Research Organization:: Univ. of Michigan, Ann Arbor, MI (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0008362

OSTI ID:: 1924793

Alternate ID(s):: OSTI ID: 1826403

Journal Information:: Journal of Materials Chemistry. A, Vol. 9, Issue 41; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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