Lithium metal stripping beneath the solid electrolyte interphase

Feifei Shi, Allen Pei, David Thomas Boyle, Jin Xie, Xiaoyun Yu, Xiaokun Zhang, Yi Cui

Research output: Contribution to journalArticle

15 Citations (Scopus)

Abstract

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. The deeper understanding of this buried interface stripping process provides beneficial clues for future lithium anode and electrolyte design.

Original languageEnglish (US)
Pages (from-to)8529-8534
Number of pages6
JournalProceedings of the National Academy of Sciences of the United States of America
Volume115
Issue number34
DOIs
StatePublished - Aug 21 2018

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Interphase
Lithium
Electrolytes
Metals
Cations
Electrodes

All Science Journal Classification (ASJC) codes

  • General

Cite this

Shi, Feifei ; Pei, Allen ; Boyle, David Thomas ; Xie, Jin ; Yu, Xiaoyun ; Zhang, Xiaokun ; Cui, Yi. / Lithium metal stripping beneath the solid electrolyte interphase. In: Proceedings of the National Academy of Sciences of the United States of America. 2018 ; Vol. 115, No. 34. pp. 8529-8534.
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Lithium metal stripping beneath the solid electrolyte interphase. / Shi, Feifei; Pei, Allen; Boyle, David Thomas; Xie, Jin; Yu, Xiaoyun; Zhang, Xiaokun; Cui, Yi.

In: Proceedings of the National Academy of Sciences of the United States of America, Vol. 115, No. 34, 21.08.2018, p. 8529-8534.

Research output: Contribution to journalArticle

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AU - Shi, Feifei

AU - Pei, Allen

AU - Boyle, David Thomas

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AB - 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. The deeper understanding of this buried interface stripping process provides beneficial clues for future lithium anode and electrolyte design.

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