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Title: Intrinsic Properties of Individual Inorganic Silicon–Electrolyte Interphase Constituents

Abstract

Because of the complexity, high reactivity, and continuous evolution of the silicon-electrolyte interphase (SiEI), 'individual' constituents of the SiEI were investigated to understand their physical, electrochemical, and mechanical properties. For the analysis of these intrinsic properties, known SiEI components (i.e., SiO 2, Li 2Si 2O 5, Li 2SiO 3, Li 3SiO x, Li 2O, and LiF) were selected and prepared as amorphous thin films. The chemical composition, purity, morphology, roughness, and thickness of prepared samples were characterized using a variety of analytical techniques. On the basis of subsequent analysis we found, LiF shows the lowest ionic conductivity and relatively weak, brittle mechanical properties, while lithium silicates demonstrate higher ionic conductivities and greater mechanical hardness. This research establishes a framework for identifying components critical for stabilization of the SiEI, thus enabling rational design of new electrolyte additives and functional binders for the development of next-generation advanced Li-ion batteries utilizing Si anodes.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2];  [1];  [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States). Materials and Chemical Science and Technology Directorate
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States). Materials and Chemical Science and Technology Directorate; Colorado School of Mines, Golden, CO (United States)
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Materials Characterization and Performance
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:
1580097
Report Number(s):
NREL/JA-5900-74658
Journal ID: ISSN 1944-8244
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 11; Journal Issue: 50; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; silicon-electrolyte interphase (SiEI); individual constituents; amorphous thin films; chemical composition; intrinsic properties

Citation Formats

Han, Sang-Don, Wood, Kevin N., Stetson, Caleb, Norman, Andrew G., Brumbach, Michael T., Coyle, Jaclyn, Xu, Yun, Harvey, Steven P., Teeter, Glenn, Zakutayev, Andriy, and Burrell, Anthony K. Intrinsic Properties of Individual Inorganic Silicon–Electrolyte Interphase Constituents. United States: N. p., 2019. Web. doi:10.1021/acsami.9b18252.
Han, Sang-Don, Wood, Kevin N., Stetson, Caleb, Norman, Andrew G., Brumbach, Michael T., Coyle, Jaclyn, Xu, Yun, Harvey, Steven P., Teeter, Glenn, Zakutayev, Andriy, & Burrell, Anthony K. Intrinsic Properties of Individual Inorganic Silicon–Electrolyte Interphase Constituents. United States. doi:10.1021/acsami.9b18252.
Han, Sang-Don, Wood, Kevin N., Stetson, Caleb, Norman, Andrew G., Brumbach, Michael T., Coyle, Jaclyn, Xu, Yun, Harvey, Steven P., Teeter, Glenn, Zakutayev, Andriy, and Burrell, Anthony K. Mon . "Intrinsic Properties of Individual Inorganic Silicon–Electrolyte Interphase Constituents". United States. doi:10.1021/acsami.9b18252.
@article{osti_1580097,
title = {Intrinsic Properties of Individual Inorganic Silicon–Electrolyte Interphase Constituents},
author = {Han, Sang-Don and Wood, Kevin N. and Stetson, Caleb and Norman, Andrew G. and Brumbach, Michael T. and Coyle, Jaclyn and Xu, Yun and Harvey, Steven P. and Teeter, Glenn and Zakutayev, Andriy and Burrell, Anthony K.},
abstractNote = {Because of the complexity, high reactivity, and continuous evolution of the silicon-electrolyte interphase (SiEI), 'individual' constituents of the SiEI were investigated to understand their physical, electrochemical, and mechanical properties. For the analysis of these intrinsic properties, known SiEI components (i.e., SiO2, Li2Si2O5, Li2SiO3, Li3SiOx, Li2O, and LiF) were selected and prepared as amorphous thin films. The chemical composition, purity, morphology, roughness, and thickness of prepared samples were characterized using a variety of analytical techniques. On the basis of subsequent analysis we found, LiF shows the lowest ionic conductivity and relatively weak, brittle mechanical properties, while lithium silicates demonstrate higher ionic conductivities and greater mechanical hardness. This research establishes a framework for identifying components critical for stabilization of the SiEI, thus enabling rational design of new electrolyte additives and functional binders for the development of next-generation advanced Li-ion batteries utilizing Si anodes.},
doi = {10.1021/acsami.9b18252},
journal = {ACS Applied Materials and Interfaces},
number = 50,
volume = 11,
place = {United States},
year = {2019},
month = {11}
}

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This content will become publicly available on November 18, 2020
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