Operando Investigation into Dynamic Evolution of Cathode-Electrolyte Interfaces in a Li-Ion Battery

Dongchang Chen, Mahmoud A. Mahmoud, Jeng Han Wang, Gordon H. Waller, Bote Zhao, Chong Qu, Mostafa A. El-Sayed, Meilin Liu*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

88 Citations (Scopus)


While Li-ion battery cathode-electrolyte interfaces (CEIs) have been extensively investigated in recent decades, accurately identifying the chemical nature and tracking the dynamics of the CEIs during electrochemical cycling still remain a grand challenge. Here we report our findings in the investigation into the dynamic evolution of the interface between a LiNi 0.33 Co 0.33 Mn 0.33 O 2 (LNMC) cathode and an ethylene carbonate/dimethyl carbonate (EC/DMC)-based electrolyte using surface-enhanced Raman spectroscopy (SERS) performed on a model cell under typical battery operating conditions. In particular, the strong SERS activity provided by a monolayer of Au nanocubes deposited on a model LNMC electrode (additive-free) enables quasi-quantitative assessment of the CEI evolution during cycling, proving information vital to revealing the dynamics of the species adsorbed on the LNMC surface as a function of cell potential. Furthermore, our theoretical calculation, which is based on the interaction between a model interface-bound molecule and a model LNMC surface, agrees with our experimental observation. The carefully designed operando SERS platform has demonstrated high sensitivity, good surface specificity, and excellent compatibility with extensive electrochemical measurements; it is also applicable to fundamental studies of dynamic interfaces in other electrochemical energy storage and conversion systems.

Original languageEnglish
Pages (from-to)2037-2043
Number of pages7
JournalNano Letters
Issue number3
Publication statusPublished - 2019 Mar 13


  • Raman spectroscopy
  • cathode-electrolyte interface (CEI)
  • lithium-ion battery
  • surface-enhanced Raman spectroscopy (SERS)

ASJC Scopus subject areas

  • Bioengineering
  • General Chemistry
  • General Materials Science
  • Condensed Matter Physics
  • Mechanical Engineering


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