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Dendrite-Free Lithium Deposition via Self-Healing Electrostatic Shield Mechanism

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† †Energy and Environment Directorate, ‡Fundamental and Computational Sciences Directorate, and §Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
∥ National Key Laboratory of Power Sources, Tianjin Institute of Power Sources, Tianjin 300381, People’s Republic of China
⊥ University College London, London WC1E 6BT, United Kingdom
[email protected]; [email protected]
Cite this: J. Am. Chem. Soc. 2013, 135, 11, 4450–4456
Publication Date (Web):February 28, 2013
https://doi.org/10.1021/ja312241y
Copyright © 2013 American Chemical Society
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Abstract

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Rechargeable lithium metal batteries are considered the “Holy Grail” of energy storage systems. Unfortunately, uncontrollable dendritic lithium growth inherent in these batteries (upon repeated charge/discharge cycling) has prevented their practical application over the past 40 years. We show a novel mechanism that can fundamentally alter dendrite formation. At low concentrations, selected cations (such as cesium or rubidium ions) exhibit an effective reduction potential below the standard reduction potential of lithium ions. During lithium deposition, these additive cations form a positively charged electrostatic shield around the initial growth tip of the protuberances without reduction and deposition of the additives. This forces further deposition of lithium to adjacent regions of the anode and eliminates dendrite formation in lithium metal batteries. This strategy may also prevent dendrite growth in lithium-ion batteries as well as other metal batteries and transform the surface uniformity of coatings deposited in many general electrodeposition processes.

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XPS spectra, EDX analysis, in situ optical observation of the deposited lithium film; simulation of the electrostatic potential and ion concentrations; and supplementary methods and movies. This material is available free of charge via the Internet at http://pubs.acs.org.

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