Uncovering the Relationship between Aging and Cycling on Lithium Metal Battery Self-Discharge

Journal Article · Tue Aug 10 00:00:00 EDT 2021 · ACS Applied Energy Materials

DOI:https://doi.org/10.1021/acsaem.1c00874· OSTI ID:1820405

Merrill, Laura C. ^[1]; Rosenberg, Samantha G. ^[1]; Jungjohann, Katherine L. ^[1]; Harrison, Katharine L. ^[1]

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1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Lithium metal is considered the “holy grail” material to replace typical Li-ion anodes due to the absence of a host structure coupled with a high theoretical capacity. The absence of a host structure results in large volumetric changes when lithium is electrodeposited/dissolved, making the lithium prone to stranding and parasitic reactions with the electrolyte. Lithium research is focused on enabling highly reversible lithium electrodeposition/dissolution, which is important to achieving long cycle life. Understanding the various mechanisms of self-discharge is also critical for realizing practical lithium metal batteries but is often overlooked. In contrast to previous work, it is shown here that self-discharge via galvanic corrosion is negligible, particularly when lithium is cycled to relevant capacities. Rather, the continued electrochemical cycling of lithium metal results in self-discharge when periodic rest is applied during cycling. The extent of self-discharge can be controlled by increasing the capacity of plated lithium, tuning electrolyte chemistry, incorporating regular rest, or introducing lithiophilic materials. Finally, the Coulombic losses that occur during periodic rest are largely reversible, suggesting that the dominant self-discharge mechanism in this work is not an irreversible chemical process but rather a morphological process.

• Research Organization: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
• Sponsoring Organization: USDOE National Nuclear Security Administration (NNSA)
• Grant/Contract Number: NA0003525
• OSTI ID: 1820405
• Report Number(s): SAND--2021-10435J; 698347
• Journal Information: ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 8 Vol. 4; ISSN 2574-0962
• Publisher: American Chemical Society (ACS)
• Country of Publication: United States
• Language: English

Related Subjects

25 ENERGY STORAGE
battery
deposition
electrochemical cells
electrodeposition
electrodes
electrolyte
lithium
self-discharge
solid electrolyte interphase
surface chemistry