Unraveling the Nanoscale Heterogeneity of Solid Electrolyte Interphase Using Tip-Enhanced Raman Spectroscopy
We employ tip-enhanced Raman spectroscopy (TERS) to study model amorphous silicon (a-Si) thin film anodes galvanostatically cycled for different numbers. For the 1× cycled a-Si, TERS shows good correlation between solid electrolyte interphase (SEI) topography and chemical mapping, corresponding to distribution of lithium ethylene dicarbonate (LEDC) and poly (ethylene oxide) (PEO)-like oligomer species. Subsequent electrochemical cycling makes the SEI relatively thick and rough with the chemical composition heavily dominated by LEDC monomer-dimer for 5× cycled a-Si. For 20× cycled a-Si, the TERS signal is dominated by carboxylate (RCO2Li) compounds of various conformations and fluorinated species (LixPOyFz). A nanomosaic-multilayer hybrid SEI model on top of the a-Si anode is proposed. Here, the significance of this work is applicable not only to silicon, where SEI plays a dominant role in determining the cycle life performance and reversibility, but also for a number of other relevant battery chemistries such as Na-ion and multivalent redox systems.
- Research Organization:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Organization:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- Grant/Contract Number:
- AC05-00OR22725
- OSTI ID:
- 1648567
- Alternate ID(s):
- OSTI ID: 1557528; OSTI ID: 1564449
- Journal Information:
- Joule, Journal Name: Joule Vol. 3 Journal Issue: 8; ISSN 2542-4351
- Publisher:
- ElsevierCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
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