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Design principles for self-forming interfaces enabling stable lithium-metal anodes
Edited by Alexis T. Bell, University of California, Berkeley, CA, and approved September 15, 2020 (received for review February 1, 2020)

Significance
It is possible to nearly double the energy density of existing lithium-ion batteries by using lithium metal anodes. However, it has been known for decades that the lithium dendrites and mossy lithium formed during charging (electrodeposition) limit the cycle life of the batteries. It is important to change the growth behavior of lithium metal, which is closely related to the properties of the solid–electrolyte interface (SEI) formed via spontaneous reactions between the lithium metal and the electrolyte. In this experimental-modeling integrated study, we reveal the design principles of the SEI that facilitates the dendrite-free and dense deposition of lithium and demonstrate one of the best cycling performances of lithium metal anode to date under practically relevant conditions.
Abstract
The path toward Li-ion batteries with higher energy densities will likely involve use of thin lithium (Li)-metal anode (<50 µm thickness), whose cyclability today remains limited by dendrite formation and low coulombic efficiency (CE). Previous studies have shown that the solid–electrolyte interface (SEI) of the Li metal plays a crucial role in Li-electrodeposition and -stripping behavior. However, design rules for optimal SEIs are not well established. Here, using integrated experimental and modeling studies on a series of structurally similar SEI-modifying model compounds, we reveal the relationship between SEI compositions, Li deposition morphology, and CE and identify two key descriptors for the fraction of ionic compounds and compactness, leading to high-performance SEIs. We further demonstrate one of the longest cycle lives to date (350 cycles for 80% capacity retention) for a high specific-energy Li||LiCoO2 full cell (projected >350 watt hours [Wh]/kg) at practical current densities. Our results provide guidance for rational design of the SEI to further improve Li-metal anodes.
Footnotes
↵1Y.Z. and V.P. contributed equally to the work.
- ↵2To whom correspondence may be addressed. Email: linsenli{at}sjtu.edu.cn, venkvis{at}cmu.edu, or ychiang{at}mit.edu.
Author contributions: L.L., V.V., and Y.-M.C. conceived and supervised the research; Y.Z. and L.L. performed the experiments with assistance from B.W., M.S.P., D.W., and Z.-F.M.; V.P. carried out the DFT simulations and analysis; and V.P., L.L., V.V., and Y.-M.C. wrote the manuscript with assistance from all authors.
Competing interest statement: V.P., L.L., V.V., and Y.-M.C. are inventors on US provisional patent application 15/480,235 submitted by the Massachusetts Institute of Technology that relates to electrolyte additives and self-formed separators enabling lithium metal anodes.
This article is a PNAS Direct Submission.
This article contains supporting information online at https://www.pnas.org/lookup/suppl/doi:10.1073/pnas.2001923117/-/DCSupplemental.
Data Availability.
All study data are included in the article and supporting information.
Published under the PNAS license.
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