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Title: The Effect of Fluoroethylene Carbonate as an Additive on the Solid Electrolyte Interphase on Silicon Lithium-Ion Electrodes

Abstract

Fluoroethylene carbonate (FEC) has become a standard electrolyte additive for use with silicon negative electrodes, but how FEC affects solid electrolyte interphase (SEI) formation on the silicon anode’s surface is still not well understood. Herein, SEI formed from LiPF6-based carbonate electrolytes, with and without FEC, were investigated on 50 nm thick amorphous silicon thin film electrodes to understand the role of FEC on silicon electrode surface reactions. In contrast to previous work, anhydrous and anoxic techniques were used to prevent air and moisture contamination of prepared SEI films. This allowed for accurate characterization of the SEI structure and composition by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry depth profiling. These results show that FEC reduction leads to fluoride ion and LiF formation, consistent with previous computational and experimental results. Surprisingly, we also find that these species decrease lithium-ion solubility and increase the reactivity of the silicon surface. We conclude that the effectiveness of FEC at improving the Coulombic efficiency and capacity retention is due to fluoride ion formation from reduction of the electrolyte, which leads to the chemical attack of any silicon-oxide surface passivation layers and the formation of a kinetically stable SEI comprising predominately lithium fluoride andmore » lithium oxide.« less

Authors:
 [1];  [2];  [2];  [3];  [1];  [3]
+ Show Author Affiliations
  1. Univ. of Texas, Austin, TX (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Univ. of California, San Diego, CA (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Understanding Charge Separation and Transfer at Interfaces in Energy Materials (CST)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1261351
Grant/Contract Number:  
AC05-00OR22725; SC0001091
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 2015; Journal Issue: 27; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Schroder, Kjell, Li, Juchuan, Dudney, Nancy J., Meng, Ying Shirley, Stevenson, Keith J., and Alvarado, Judith. The Effect of Fluoroethylene Carbonate as an Additive on the Solid Electrolyte Interphase on Silicon Lithium-Ion Electrodes. United States: N. p., 2015. Web. doi:10.1021/acs.chemmater.5b01627.
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Schroder, Kjell, Li, Juchuan, Dudney, Nancy J., Meng, Ying Shirley, Stevenson, Keith J., & Alvarado, Judith. The Effect of Fluoroethylene Carbonate as an Additive on the Solid Electrolyte Interphase on Silicon Lithium-Ion Electrodes. United States. https://doi.org/10.1021/acs.chemmater.5b01627
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Schroder, Kjell, Li, Juchuan, Dudney, Nancy J., Meng, Ying Shirley, Stevenson, Keith J., and Alvarado, Judith. Mon . "The Effect of Fluoroethylene Carbonate as an Additive on the Solid Electrolyte Interphase on Silicon Lithium-Ion Electrodes". United States. https://doi.org/10.1021/acs.chemmater.5b01627. https://www.osti.gov/servlets/purl/1261351.
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@article{osti_1261351,
title = {The Effect of Fluoroethylene Carbonate as an Additive on the Solid Electrolyte Interphase on Silicon Lithium-Ion Electrodes},
author = {Schroder, Kjell and Li, Juchuan and Dudney, Nancy J. and Meng, Ying Shirley and Stevenson, Keith J. and Alvarado, Judith},
abstractNote = {Fluoroethylene carbonate (FEC) has become a standard electrolyte additive for use with silicon negative electrodes, but how FEC affects solid electrolyte interphase (SEI) formation on the silicon anode’s surface is still not well understood. Herein, SEI formed from LiPF6-based carbonate electrolytes, with and without FEC, were investigated on 50 nm thick amorphous silicon thin film electrodes to understand the role of FEC on silicon electrode surface reactions. In contrast to previous work, anhydrous and anoxic techniques were used to prevent air and moisture contamination of prepared SEI films. This allowed for accurate characterization of the SEI structure and composition by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry depth profiling. These results show that FEC reduction leads to fluoride ion and LiF formation, consistent with previous computational and experimental results. Surprisingly, we also find that these species decrease lithium-ion solubility and increase the reactivity of the silicon surface. We conclude that the effectiveness of FEC at improving the Coulombic efficiency and capacity retention is due to fluoride ion formation from reduction of the electrolyte, which leads to the chemical attack of any silicon-oxide surface passivation layers and the formation of a kinetically stable SEI comprising predominately lithium fluoride and lithium oxide.},
doi = {10.1021/acs.chemmater.5b01627},
journal = {Chemistry of Materials},
number = 27,
volume = 2015,
place = {United States},
year = {Mon Aug 03 00:00:00 EDT 2015},
month = {Mon Aug 03 00:00:00 EDT 2015}
}
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https://doi.org/10.1021/acs.chemmater.5b01627
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    • Angewandte Chemie International Edition, Vol. 57, Issue 14
    • DOI: 10.1002/anie.201712907

    Effect of Film-Forming Additive in Ionic Liquid Electrolyte on Electrochemical Performance of Si Negative-Electrode for LIBs
    journal, January 2019

    • Yamaguchi, Kazuki; Domi, Yasuhiro; Usui, Hiroyuki
    • Journal of The Electrochemical Society, Vol. 166, Issue 2
    • DOI: 10.1149/2.0971902jes

    Quantifying the Distribution of Electrolyte Decomposition Products in Silicon-Graphite Electrodes by Neutron Depth Profiling
    journal, January 2018

    • Wetjen, Morten; Trunk, Markus; Werner, Lukas
    • Journal of The Electrochemical Society, Vol. 165, Issue 10
    • DOI: 10.1149/2.1341810jes

    Morphological Changes of Silicon Nanoparticles and the Influence of Cutoff Potentials in Silicon-Graphite Electrodes
    journal, January 2018

    • Wetjen, Morten; Solchenbach, Sophie; Pritzl, Daniel
    • Journal of The Electrochemical Society, Vol. 165, Issue 7
    • DOI: 10.1149/2.1261807jes

    Embracing high performance potassium-ion batteries with phosphorus-based electrodes: a review
    journal, January 2019

    • Yang, Dan; Liu, Chuntai; Rui, Xianhong
    • Nanoscale, Vol. 11, Issue 33
    • DOI: 10.1039/c9nr05588f

    Impact of alginate and fluoroethylene carbonate on the electrochemical performance of SiO–SnCoC anode for lithium-ion batteries
    journal, November 2018

    • Luque, Guillermina L.; Li, Yan; Zeng, Xiaoqiao
    • Journal of Solid State Electrochemistry, Vol. 23, Issue 2
    • DOI: 10.1007/s10008-018-4145-2

    Quantitative Determination of Carbon Dioxide Content in Organic Electrolytes by Infrared Spectroscopy
    journal, January 2019

    • Yu, H.; Obrovac, M. N.
    • Journal of The Electrochemical Society, Vol. 166, Issue 12
    • DOI: 10.1149/2.0291912jes

    MOF derived ZnCo 2 O 4 porous hollow spheres functionalized with Ag nanoparticles for a long-cycle and high-capacity lithium ion battery anode
    journal, January 2017

    • Koo, Won-Tae; Jang, Hye-Yeon; Kim, Chanhoon
    • Journal of Materials Chemistry A, Vol. 5, Issue 43
    • DOI: 10.1039/c7ta07573a

    Towards maximized volumetric capacity via pore-coordinated design for large-volume-change lithium-ion battery anodes
    journal, January 2019

    A high-energy sulfur cathode in carbonate electrolyte by eliminating polysulfides via solid-phase lithium-sulfur transformation
    journal, October 2018

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