Lithium metal stripping beneath the solid electrolyte interphase

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

doi:10.1073/pnas.1806878115

Title: Lithium metal stripping beneath the solid electrolyte interphase

Journal Article · 06 August 2018 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.1806878115 · OSTI ID:1476112

Shi, Feifei ^[1];

^[1]; Boyle, David Thomas ^[1];

^[1]; Yu, Xiaoyun ^[1]; Zhang, Xiaokun ^[2]; Cui, Yi ^[3]

Stanford Univ., Stanford, CA (United States)
Univ. of Electronic Science and Technology of China, Sichuan (People's Republic of China)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1476112

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 34 Vol. 115; ISSN 0027-8424

Publisher:: National Academy of Sciences, Washington, DC (United States)Copyright Statement

Country of Publication:: United States

Language:: English

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