Probing the Evolution of Surface Chemistry at the Silicon-Electrolyte Interphase via In Situ Surface-Enhanced Raman Spectroscopy.

Yeyoung Ha, Bertrand J Tremolet de Villers, Zhifei Li, Yun Xu, Paul Stradins, Andriy Zakutayev, Anthony Burrell, Sang-Don Han
Author Information
  1. Yeyoung Ha: Materials and Chemical Science and Technology Directorate , National Renewable Energy Laboratory , 15013 Denver West Parkway , Golden , Colorado 80401 , United States. ORCID
  2. Bertrand J Tremolet de Villers: Materials and Chemical Science and Technology Directorate , National Renewable Energy Laboratory , 15013 Denver West Parkway , Golden , Colorado 80401 , United States. ORCID
  3. Zhifei Li: Materials and Chemical Science and Technology Directorate , National Renewable Energy Laboratory , 15013 Denver West Parkway , Golden , Colorado 80401 , United States. ORCID
  4. Yun Xu: Materials and Chemical Science and Technology Directorate , National Renewable Energy Laboratory , 15013 Denver West Parkway , Golden , Colorado 80401 , United States. ORCID
  5. Paul Stradins: Materials and Chemical Science and Technology Directorate , National Renewable Energy Laboratory , 15013 Denver West Parkway , Golden , Colorado 80401 , United States.
  6. Andriy Zakutayev: Materials and Chemical Science and Technology Directorate , National Renewable Energy Laboratory , 15013 Denver West Parkway , Golden , Colorado 80401 , United States. ORCID
  7. Anthony Burrell: Materials and Chemical Science and Technology Directorate , National Renewable Energy Laboratory , 15013 Denver West Parkway , Golden , Colorado 80401 , United States.
  8. Sang-Don Han: Materials and Chemical Science and Technology Directorate , National Renewable Energy Laboratory , 15013 Denver West Parkway , Golden , Colorado 80401 , United States. ORCID

Abstract

We present a novel spectroscopic technique for in situ Raman microscopy studies of battery electrodes. By creating nanostructures on a copper mesh current collector, we were able to utilize surface-enhanced Raman spectroscopy (SERS) to monitor the evolution of the Silicon anode-electrolyte interphase. The spectra show reversible Si peak intensity changes upon lithiation and delithiation. Moreover, an alkyl carboxylate species, lithium propionate, was detected as a significant SiEI component. Our experimental setup showed reproducible and stable performance over multiple cycles in terms of both electrochemistry and spectroscopy.

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