The Chemistry of Electrolyte Reduction on Silicon Electrodes Revealed by in Situ ATR-FTIR Spectroscopy

Feifei Shi, Philip N. Ross, Gabor A. Somorjai, Kyriakos Komvopoulos

Research output: Contribution to journalArticle

15 Citations (Scopus)

Abstract

While silicon is the most promising next-generation anode material for lithium-ion batteries (LIBs), silicon electrodes exhibit significant capacity fade with cycling. A common hypothesis is that the capacity loss is due to the solid electrolyte interphase (SEI) forming in the first cycle and becoming destabilized by large cyclic volume changes. A cell for in situ attenuated total reflection-Fourier transform infrared spectroscopy with controllable penetration depth was used to study the chemistry at the electrode-electrolyte interface. The SEI product precursors at the interface were successfully identified and differentiated from free or solvated solvent molecules in the bulk electrolyte. Intriguingly, for the most common electrolyte consisting of ethylene carbonate and diethyl carbonate, ethylene carbonate was found to directly reduce to lithium ethylene dicarbonate on the lithiated silicon surface and diethyl carbonate to selectively reduce to diethyl 2,5-dioxahexane dicarboxylate on the surface of the native silicon-oxide film. Understanding this surface dependence of the SEI composition is critical to tuning the silicon electrode surface condition and, ultimately, enhancing the performance of future LIBs. (Figure Presented).

Original languageEnglish (US)
Pages (from-to)14476-14483
Number of pages8
JournalJournal of Physical Chemistry C
Volume121
Issue number27
DOIs
StatePublished - Jul 13 2017

Fingerprint

Silicon
Electrolytes
Carbonates
carbonates
Solid electrolytes
solid electrolytes
electrolytes
Spectroscopy
chemistry
Ethylene
Electrodes
ethylene
electrodes
lithium
silicon
spectroscopy
electric batteries
cycles
Silicon oxides
silicon oxides

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Cite this

Shi, Feifei ; Ross, Philip N. ; Somorjai, Gabor A. ; Komvopoulos, Kyriakos. / The Chemistry of Electrolyte Reduction on Silicon Electrodes Revealed by in Situ ATR-FTIR Spectroscopy. In: Journal of Physical Chemistry C. 2017 ; Vol. 121, No. 27. pp. 14476-14483.
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The Chemistry of Electrolyte Reduction on Silicon Electrodes Revealed by in Situ ATR-FTIR Spectroscopy. / Shi, Feifei; Ross, Philip N.; Somorjai, Gabor A.; Komvopoulos, Kyriakos.

In: Journal of Physical Chemistry C, Vol. 121, No. 27, 13.07.2017, p. 14476-14483.

Research output: Contribution to journalArticle

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