Journal
ACS APPLIED ENERGY MATERIALS
Volume 4, Issue 8, Pages 7589-7598Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.1c00874
Keywords
lithium; electrolyte; solid electrolyte interphase; self-discharge; electrodeposition; battery
Funding
- Laboratory Directed Research and Development program at Sandia National Laboratories
- U.S. Department of Energy's National Nuclear Security Administration [DE-NA-0003525]
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Research on lithium metal is focused on achieving highly reversible lithium electrodeposition/dissolution for long cycle life. The extent of self-discharge can be controlled by increasing plated lithium capacity, tuning electrolyte chemistry, incorporating rest periods, or introducing lithiophilic materials. The dominant self-discharge mechanism is shown to be a morphological process rather than an irreversible chemical process.
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. 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.
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