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

© 2020 National Academy of Sciences. All rights reserved. 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). Pre...

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Main Authors: Zhu, Yingying, Pande, Vikram, Li, Linsen, Wen, Bohua, Pan, Menghsuan Sam, Wang, David, Ma, Zi-Feng, Viswanathan, Venkatasubramanian, Chiang, Yet-Ming
Other Authors: Massachusetts Institute of Technology. Department of Materials Science and Engineering
Format: Article
Language:English
Published: Proceedings of the National Academy of Sciences 2022
Online Access:https://hdl.handle.net/1721.1/142491
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author Zhu, Yingying
Pande, Vikram
Li, Linsen
Wen, Bohua
Pan, Menghsuan Sam
Wang, David
Ma, Zi-Feng
Viswanathan, Venkatasubramanian
Chiang, Yet-Ming
author2 Massachusetts Institute of Technology. Department of Materials Science and Engineering
author_facet Massachusetts Institute of Technology. Department of Materials Science and Engineering
Zhu, Yingying
Pande, Vikram
Li, Linsen
Wen, Bohua
Pan, Menghsuan Sam
Wang, David
Ma, Zi-Feng
Viswanathan, Venkatasubramanian
Chiang, Yet-Ming
author_sort Zhu, Yingying
collection MIT
description © 2020 National Academy of Sciences. All rights reserved. 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 LijjLiCoO2 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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spelling mit-1721.1/1424912023-04-14T15:39:19Z Design principles for self-forming interfaces enabling stable lithium-metal anodes Zhu, Yingying Pande, Vikram Li, Linsen Wen, Bohua Pan, Menghsuan Sam Wang, David Ma, Zi-Feng Viswanathan, Venkatasubramanian Chiang, Yet-Ming Massachusetts Institute of Technology. Department of Materials Science and Engineering © 2020 National Academy of Sciences. All rights reserved. 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 LijjLiCoO2 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. 2022-05-11T18:05:36Z 2022-05-11T18:05:36Z 2020 2022-05-11T17:56:22Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/142491 Zhu, Yingying, Pande, Vikram, Li, Linsen, Wen, Bohua, Pan, Menghsuan Sam et al. 2020. "Design principles for self-forming interfaces enabling stable lithium-metal anodes." Proceedings of the National Academy of Sciences of the United States of America, 117 (44). en 10.1073/PNAS.2001923117 Proceedings of the National Academy of Sciences of the United States of America Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf Proceedings of the National Academy of Sciences PNAS
spellingShingle 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
title Design principles for self-forming interfaces enabling stable lithium-metal anodes
title_full Design principles for self-forming interfaces enabling stable lithium-metal anodes
title_fullStr Design principles for self-forming interfaces enabling stable lithium-metal anodes
title_full_unstemmed Design principles for self-forming interfaces enabling stable lithium-metal anodes
title_short Design principles for self-forming interfaces enabling stable lithium-metal anodes
title_sort design principles for self forming interfaces enabling stable lithium metal anodes
url https://hdl.handle.net/1721.1/142491
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