A Bottom-Up Formation Mechanism of Solid Electrolyte Interphase Revealed by Isotope-Assisted Time-of-Flight Secondary Ion Mass Spectrometry

Zhe Liu, Peng Lu, Qinglin Zhang, Xingcheng Xiao, Yue Qi, Long-qing Chen

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

Understanding the solid electrolyte interphase (SEI) formation mechanism is critically important for the performance and durability of lithium-ion batteries. However, the details of how SEI builds up into a nanometer-thick layer from molecular level reduction reactions on negative electrodes are missing. Here, isotope-assisted time-of-flight secondary ion mass spectrometry analyses were designed to answer this fundamental question. By investigating the isotope ratio profile in SEI during the initial SEI formation cycle, it is discovered that the topmost SEI near the electrolyte formed first and the SEI near the electrode formed later. This new "bottom-up" SEI growth mechanism was then correlated to the electrolyte one-electron and two-electron reduction reaction dynamics, which in turn explains the formation of the two-layered organic-inorganic SEI composite structure.

Original languageEnglish (US)
Pages (from-to)5508-5514
Number of pages7
JournalJournal of Physical Chemistry Letters
Volume9
Issue number18
DOIs
StatePublished - Sep 20 2018

Fingerprint

Solid electrolytes
solid electrolytes
Secondary ion mass spectrometry
Isotopes
secondary ion mass spectrometry
isotopes
Electrolytes
electrolytes
Electrodes
electrodes
Electrons
isotope ratios
composite structures
Composite structures
durability
electric batteries
Durability
electrons
lithium
cycles

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Physical and Theoretical Chemistry

Cite this

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title = "A Bottom-Up Formation Mechanism of Solid Electrolyte Interphase Revealed by Isotope-Assisted Time-of-Flight Secondary Ion Mass Spectrometry",
abstract = "Understanding the solid electrolyte interphase (SEI) formation mechanism is critically important for the performance and durability of lithium-ion batteries. However, the details of how SEI builds up into a nanometer-thick layer from molecular level reduction reactions on negative electrodes are missing. Here, isotope-assisted time-of-flight secondary ion mass spectrometry analyses were designed to answer this fundamental question. By investigating the isotope ratio profile in SEI during the initial SEI formation cycle, it is discovered that the topmost SEI near the electrolyte formed first and the SEI near the electrode formed later. This new {"}bottom-up{"} SEI growth mechanism was then correlated to the electrolyte one-electron and two-electron reduction reaction dynamics, which in turn explains the formation of the two-layered organic-inorganic SEI composite structure.",
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A Bottom-Up Formation Mechanism of Solid Electrolyte Interphase Revealed by Isotope-Assisted Time-of-Flight Secondary Ion Mass Spectrometry. / Liu, Zhe; Lu, Peng; Zhang, Qinglin; Xiao, Xingcheng; Qi, Yue; Chen, Long-qing.

In: Journal of Physical Chemistry Letters, Vol. 9, No. 18, 20.09.2018, p. 5508-5514.

Research output: Contribution to journalArticle

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T1 - A Bottom-Up Formation Mechanism of Solid Electrolyte Interphase Revealed by Isotope-Assisted Time-of-Flight Secondary Ion Mass Spectrometry

AU - Liu, Zhe

AU - Lu, Peng

AU - Zhang, Qinglin

AU - Xiao, Xingcheng

AU - Qi, Yue

AU - Chen, Long-qing

PY - 2018/9/20

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AB - Understanding the solid electrolyte interphase (SEI) formation mechanism is critically important for the performance and durability of lithium-ion batteries. However, the details of how SEI builds up into a nanometer-thick layer from molecular level reduction reactions on negative electrodes are missing. Here, isotope-assisted time-of-flight secondary ion mass spectrometry analyses were designed to answer this fundamental question. By investigating the isotope ratio profile in SEI during the initial SEI formation cycle, it is discovered that the topmost SEI near the electrolyte formed first and the SEI near the electrode formed later. This new "bottom-up" SEI growth mechanism was then correlated to the electrolyte one-electron and two-electron reduction reaction dynamics, which in turn explains the formation of the two-layered organic-inorganic SEI composite structure.

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