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Non-aqueous Electrode Processing and Construction of Lithium-ion Coin Cells

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Localized Recrystallization of a Lithium-Metal Anode during Fast Stripping in High-Activity Liquid Electrolytes.

Shang Zhu¹, Zijian Hong^1,2, Zeeshan Ahmad^3,4

¹Department of Mechanical Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania15213, United States.

ACS Applied Materials & Interfaces

|January 30, 2023

Summary

Researchers used a phase-field model to study lithium-metal anode morphology during battery cycling. They discovered a localized recrystallization phenomenon at high discharging rates that improves morphological stability.

Keywords:

electrolyte nonidealities fast stripping lithium-metal anode localized recrystallization phase-field model

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Area of Science:

Materials Science
Electrochemistry
Computational Modeling

Background:

Lithium-metal anodes offer high capacity for next-generation batteries.
Electrode-electrolyte interface instability limits lithium-metal anode commercialization.
Morphological evolution during plating/stripping impacts battery cycling performance.

Purpose of the Study:

To computationally characterize morphological evolution dynamics at the lithium-metal-electrolyte interface.
To investigate the influence of electrolyte nonidealities on interfacial reaction kinetics.
To explore strategies for enhancing lithium-metal anode stability.

Main Methods:

Phase-field modeling of lithium plating and stripping.
Incorporation of electrolyte solution nonidealities into interfacial reaction kinetics.
Systematic investigation of lithium-ion activity and overpotential effects.

Main Results:

Observed an unexpected localized recrystallization phenomenon during fast lithium stripping at high discharging overpotentials.
Demonstrated that this recrystallization occurs in high-lithium-ion-concentration valley regions.
Showed that recrystallization mitigates reaction rate heterogeneity, improving morphological stability.

Conclusions:

Localized recrystallization is a key phenomenon for improving lithium-metal anode morphological stability.
The study provides a potential approach to enhance battery cycling performance.
A simplified phase diagram for overpotential-dependent recrystallization was developed.