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Title: Design principles for self-forming interfaces enabling stable lithium-metal anodes

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||LiCoO 2 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.

Authors:
; ; ORCiD logo; ORCiD logo; ; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
OSTI Identifier:
1690296
Grant/Contract Number:  
EE0007810
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 117 Journal Issue: 44; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English

Citation Formats

Zhu, Yingying, Pande, Vikram, Li, Linsen, Wen, Bohua, Pan, Menghsuan Sam, Wang, David, Ma, Zi-Feng, Viswanathan, Venkatasubramanian, and Chiang, Yet-Ming. Design principles for self-forming interfaces enabling stable lithium-metal anodes. United States: N. p., 2020. Web. https://doi.org/10.1073/pnas.2001923117.
Zhu, Yingying, Pande, Vikram, Li, Linsen, Wen, Bohua, Pan, Menghsuan Sam, Wang, David, Ma, Zi-Feng, Viswanathan, Venkatasubramanian, & Chiang, Yet-Ming. Design principles for self-forming interfaces enabling stable lithium-metal anodes. United States. https://doi.org/10.1073/pnas.2001923117
Zhu, Yingying, Pande, Vikram, Li, Linsen, Wen, Bohua, Pan, Menghsuan Sam, Wang, David, Ma, Zi-Feng, Viswanathan, Venkatasubramanian, and Chiang, Yet-Ming. Thu . "Design principles for self-forming interfaces enabling stable lithium-metal anodes". United States. https://doi.org/10.1073/pnas.2001923117.
@article{osti_1690296,
title = {Design principles for self-forming interfaces enabling stable lithium-metal anodes},
author = {Zhu, Yingying and Pande, Vikram and Li, Linsen and Wen, Bohua and Pan, Menghsuan Sam and Wang, David and Ma, Zi-Feng and Viswanathan, Venkatasubramanian and Chiang, Yet-Ming},
abstractNote = {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||LiCoO 2 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.},
doi = {10.1073/pnas.2001923117},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 44,
volume = 117,
place = {United States},
year = {2020},
month = {10}
}

Journal Article:
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https://doi.org/10.1073/pnas.2001923117

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