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

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. We report 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.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States). Materials and Chemical Science and Technology Directorate
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1592392
Report Number(s):
NREL/JA-5900-75341
Journal ID: ISSN 1948-7185
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 30 DIRECT ENERGY CONVERSION; silicon-electrolyte interphase; SiEI; in-situ surface-enhanced Raman spectroscopy; SERS; reversible evolution of silicon; alkyl carboxylates

Citation Formats

Ha, Yeyoung, Tremolet de Villers, Bertrand J., Li, Zhifei, Xu, Yun, Stradins, Paul, Zakutayev, Andriy, Burrell, Anthony, and Han, Sang-Don. Probing the Evolution of Surface Chemistry at the Silicon–Electrolyte Interphase via In Situ Surface-Enhanced Raman Spectroscopy. United States: N. p., 2019. Web. doi:10.1021/acs.jpclett.9b03284.
Ha, Yeyoung, Tremolet de Villers, Bertrand J., Li, Zhifei, Xu, Yun, Stradins, Paul, Zakutayev, Andriy, Burrell, Anthony, & Han, Sang-Don. Probing the Evolution of Surface Chemistry at the Silicon–Electrolyte Interphase via In Situ Surface-Enhanced Raman Spectroscopy. United States. https://doi.org/10.1021/acs.jpclett.9b03284
Ha, Yeyoung, Tremolet de Villers, Bertrand J., Li, Zhifei, Xu, Yun, Stradins, Paul, Zakutayev, Andriy, Burrell, Anthony, and Han, Sang-Don. Tue . "Probing the Evolution of Surface Chemistry at the Silicon–Electrolyte Interphase via In Situ Surface-Enhanced Raman Spectroscopy". United States. https://doi.org/10.1021/acs.jpclett.9b03284. https://www.osti.gov/servlets/purl/1592392.
@article{osti_1592392,
title = {Probing the Evolution of Surface Chemistry at the Silicon–Electrolyte Interphase via In Situ Surface-Enhanced Raman Spectroscopy},
author = {Ha, Yeyoung and Tremolet de Villers, Bertrand J. and Li, Zhifei and Xu, Yun and Stradins, Paul and Zakutayev, Andriy and Burrell, Anthony and Han, Sang-Don},
abstractNote = {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. We report 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.},
doi = {10.1021/acs.jpclett.9b03284},
journal = {Journal of Physical Chemistry Letters},
number = 1,
volume = 11,
place = {United States},
year = {2019},
month = {12}
}

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