In Situ Mass Spectrometric Determination of Molecular Structural Evolution at the Solid Electrolyte Interphase in Lithium-Ion Batteries

Zihua Zhu, Yufan Zhou, Pengfei Yan, Rama Sesha Vemuri, Wu Xu, Rui Zhao, Xuelin Wang, Suntharampillai Thevuthasan, Donald R. Baer, Chong Min Wang

Research output: Contribution to journalArticle

28 Citations (Scopus)

Abstract

Dynamic structural and chemical evolution at solid-liquid electrolyte interface is always a mystery for a rechargeable battery due to the challenge to directly probe a solid-liquid interface under reaction conditions. We describe the creation and usage of in situ liquid secondary ion mass spectroscopy (SIMS) for the first time to directly observe the molecular structural evolution at the solid-liquid electrolyte interface for a lithium (Li)-ion battery under dynamic operating conditions. We have discovered that the deposition of Li metal on copper electrode leads to the condensation of solvent molecules around the electrode. Chemically, this layer of solvent condensate tends to be depleted of the salt anions and with reduced concentration of Li<sup>+</sup> ions, essentially leading to the formation of a lean electrolyte layer adjacent to the electrode and therefore contributing to the overpotential of the cell. This observation provides unprecedented molecular level dynamic information on the initial formation of the solid electrolyte interphase (SEI) layer. The present work also ultimately opens new avenues for implanting the in situ liquid SIMS concept to probe the chemical reaction process that intimately involves solid-liquid interface, such as electrocatalysis, electrodeposition, biofuel conversion, biofilm, and biomineralization.

Original languageEnglish
Pages (from-to)6170-6176
Number of pages7
JournalNano Letters
Volume15
Issue number9
DOIs
Publication statusPublished - 9 Sep 2015
Externally publishedYes

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Keywords

  • In situ liquid SIMS
  • lithium ion battery
  • molecular structural evolution
  • SEI layers
  • solid-liquid interface

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Mechanical Engineering

Cite this

Zhu, Z., Zhou, Y., Yan, P., Vemuri, R. S., Xu, W., Zhao, R., Wang, X., Thevuthasan, S., Baer, D. R., & Wang, C. M. (2015). In Situ Mass Spectrometric Determination of Molecular Structural Evolution at the Solid Electrolyte Interphase in Lithium-Ion Batteries. Nano Letters, 15(9), 6170-6176. https://doi.org/10.1021/acs.nanolett.5b02479