Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 117, Issue 44, Pages 27195-27203Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.2001923117
Keywords
batteries; lithium metal anode; solid-electrolyte interface; electrolytes
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Funding
- Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US DOE through Advanced Battery Materials Research Program [DE-EE0007810]
- Shanghai Jiao Tong University
- Natural Science Foundation of Shanghai, the Science and Technology Commission Shanghai Municipality [19ZR1475100]
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The path toward Li-ion batteries with higher energy densities will likely involve use of thin lithium (Li)-metal anode (<50 mu m 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 parallel to 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.
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