Unraveling the Nanoscale Heterogeneity of Solid Electrolyte Interphase Using Tip-Enhanced Raman Spectroscopy

Unraveling the Nanoscale Heterogeneity of Solid Electrolyte Interphase Using Tip-Enhanced Raman Spectroscopy

TitleUnraveling the Nanoscale Heterogeneity of Solid Electrolyte Interphase Using Tip-Enhanced Raman Spectroscopy
Publication TypeJournal Article
Year of Publication2019
AuthorsJagjit Nanda, Guang Yang, Tingzheng Hou, Dmitry N Voylov, Xin Li, Rose E Ruther, Michael Naguib, Kristin A Persson, Gabriel M Veith, Alexei P Sokolov
JournalJoule
Date PublishedJan-06-2019
ISSN25424351
Abstract

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. 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.

DOI10.1016/j.joule.2019.05.026
Short TitleJoule
Refereed DesignationRefereed