skip to main content

DOE PAGESDOE PAGES

This content will become publicly available on August 6, 2019

Title: Lithium metal stripping beneath the solid electrolyte interphase

Lithium stripping is a crucial process coupled with lithium deposition during the cycling of Li metal batteries. Lithium deposition has been widely studied, whereas stripping as a subsurface process has rarely been investigated. Here we reveal the fundamental mechanism of stripping on lithium by visualizing the interface between stripped lithium and the solid electrolyte interphase (SEI). We observed nanovoids formed between lithium and the SEI layer after stripping, which are attributed to the accumulation of lithium metal vacancies. High-rate dissolution of lithium causes vigorous growth and subsequent aggregation of voids, followed by the collapse of the SEI layer, i.e., pitting. We systematically measured the lithium polarization behavior during stripping and find that the lithium cation diffusion through the SEI layer is the rate-determining step. Nonuniform sites on typical lithium surfaces, such as grain boundaries and slip lines, greatly accelerated the local dissolution of lithium. As a result, the deeper understanding of this buried interface stripping process provides beneficial clues for future lithium anode and electrolyte design.
Authors:
 [1] ; ORCiD logo [1] ;  [1] ; ORCiD logo [1] ;  [1] ;  [2] ;  [3]
  1. Stanford Univ., Stanford, CA (United States)
  2. Univ. of Electronic Science and Technology of China, Sichuan (People's Republic of China)
  3. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-76SF00515
Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 115; Journal Issue: 34; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; lithium metal; stripping; solid electrolyte interphase; pitting; battery
OSTI Identifier:
1476112

Shi, Feifei, Pei, Allen, Boyle, David Thomas, Xie, Jin, Yu, Xiaoyun, Zhang, Xiaokun, and Cui, Yi. Lithium metal stripping beneath the solid electrolyte interphase. United States: N. p., Web. doi:10.1073/pnas.1806878115.
Shi, Feifei, Pei, Allen, Boyle, David Thomas, Xie, Jin, Yu, Xiaoyun, Zhang, Xiaokun, & Cui, Yi. Lithium metal stripping beneath the solid electrolyte interphase. United States. doi:10.1073/pnas.1806878115.
Shi, Feifei, Pei, Allen, Boyle, David Thomas, Xie, Jin, Yu, Xiaoyun, Zhang, Xiaokun, and Cui, Yi. 2018. "Lithium metal stripping beneath the solid electrolyte interphase". United States. doi:10.1073/pnas.1806878115.
@article{osti_1476112,
title = {Lithium metal stripping beneath the solid electrolyte interphase},
author = {Shi, Feifei and Pei, Allen and Boyle, David Thomas and Xie, Jin and Yu, Xiaoyun and Zhang, Xiaokun and Cui, Yi},
abstractNote = {Lithium stripping is a crucial process coupled with lithium deposition during the cycling of Li metal batteries. Lithium deposition has been widely studied, whereas stripping as a subsurface process has rarely been investigated. Here we reveal the fundamental mechanism of stripping on lithium by visualizing the interface between stripped lithium and the solid electrolyte interphase (SEI). We observed nanovoids formed between lithium and the SEI layer after stripping, which are attributed to the accumulation of lithium metal vacancies. High-rate dissolution of lithium causes vigorous growth and subsequent aggregation of voids, followed by the collapse of the SEI layer, i.e., pitting. We systematically measured the lithium polarization behavior during stripping and find that the lithium cation diffusion through the SEI layer is the rate-determining step. Nonuniform sites on typical lithium surfaces, such as grain boundaries and slip lines, greatly accelerated the local dissolution of lithium. As a result, the deeper understanding of this buried interface stripping process provides beneficial clues for future lithium anode and electrolyte design.},
doi = {10.1073/pnas.1806878115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 34,
volume = 115,
place = {United States},
year = {2018},
month = {8}
}

Works referenced in this record:

Lithium metal stripping/plating mechanisms studies: A metallurgical approach
journal, October 2006

Aprotic and Aqueous Li–O2 Batteries
journal, April 2014
  • Lu, Jun; Li, Li; Park, Jin-Bum
  • Chemical Reviews, Vol. 114, Issue 11, p. 5611-5640
  • DOI: 10.1021/cr400573b

Selective deposition and stable encapsulation of lithium through heterogeneous seeded growth
journal, February 2016
  • Yan, Kai; Lu, Zhenda; Lee, Hyun-Wook
  • Nature Energy, Vol. 1, Issue 3, Article No. 16010
  • DOI: 10.1038/nenergy.2016.10

Li–O2 and Li–S batteries with high energy storage
journal, January 2012
  • Bruce, Peter G.; Freunberger, Stefan A.; Hardwick, Laurence J.
  • Nature Materials, Vol. 11, Issue 1, p. 19-29
  • DOI: 10.1038/nmat3191