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Title: Thermal Decomposition of the Solid Electrolyte Interphase (SEI) on Silicon Electrodes for Lithium Ion Batteries

Abstract

Here, thermal behavior of the solid electrolyte interphase (SEI) on a silicon electrode for lithium ion batteries has been investigated by TGA. In order to provide a better understanding of the thermal decomposition of the SEI on silicon, the thermal decomposition behavior of independently synthesized lithium ethylene dicarbonate (LEDC) was investigated as a model SEI. The model SEI (LEDC) has three stages of thermal decomposition. Over the temperature range of 50–300 °C, LEDC decomposes to evolve CO2 and C2H4 gases leaving lithium propionate (CH3CH2CO2Li) and Li2CO3 as solid residues. The lithium propionate decomposes over the temperature range of 300–600 °C to evolve pentanone leaving Li2CO3 as a residual solid. Finally, the Li2CO3 decomposes over 600 °C to evolve CO2 leaving Li2O as a residual solid. A very similar thermal decomposition process is observed for the SEI generated on cycled silicon electrodes. However, two additional thermal decomposition reactions were observed characteristic of LixPOyFz at 300 °C and the polyimide binder at 550 °C. TGA measurements of Si electrodes after various numbers of cycles suggest that the LEDC on Si electrodes thermally decomposes during cycling to form lithium propionate and Li2CO3, resulting in increased complexity of the SEI.

Authors:
 [1];  [1];  [1]; ORCiD logo [1]
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  1. Univ. of Rhode Island, Kingston, RI (United States)
Publication Date:
Research Org.:
Brown Univ., Providence, RI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1534459
Grant/Contract Number:  
SC0007074
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 7; 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; 36 MATERIALS SCIENCE; Chemistry; Materials science; Degradation; Organic reactions; Electrodes; Surface chemistry; Silicon

Citation Formats

Yoon, Taeho, Milien, Mickdy S., Parimalam, Bharathy S., and Lucht, Brett L. Thermal Decomposition of the Solid Electrolyte Interphase (SEI) on Silicon Electrodes for Lithium Ion Batteries. United States: N. p., 2017. Web. doi:10.1021/acs.chemmater.7b00454.
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Yoon, Taeho, Milien, Mickdy S., Parimalam, Bharathy S., & Lucht, Brett L. Thermal Decomposition of the Solid Electrolyte Interphase (SEI) on Silicon Electrodes for Lithium Ion Batteries. United States. https://doi.org/10.1021/acs.chemmater.7b00454
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Yoon, Taeho, Milien, Mickdy S., Parimalam, Bharathy S., and Lucht, Brett L. Fri . "Thermal Decomposition of the Solid Electrolyte Interphase (SEI) on Silicon Electrodes for Lithium Ion Batteries". United States. https://doi.org/10.1021/acs.chemmater.7b00454. https://www.osti.gov/servlets/purl/1534459.
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@article{osti_1534459,
title = {Thermal Decomposition of the Solid Electrolyte Interphase (SEI) on Silicon Electrodes for Lithium Ion Batteries},
author = {Yoon, Taeho and Milien, Mickdy S. and Parimalam, Bharathy S. and Lucht, Brett L.},
abstractNote = {Here, thermal behavior of the solid electrolyte interphase (SEI) on a silicon electrode for lithium ion batteries has been investigated by TGA. In order to provide a better understanding of the thermal decomposition of the SEI on silicon, the thermal decomposition behavior of independently synthesized lithium ethylene dicarbonate (LEDC) was investigated as a model SEI. The model SEI (LEDC) has three stages of thermal decomposition. Over the temperature range of 50–300 °C, LEDC decomposes to evolve CO2 and C2H4 gases leaving lithium propionate (CH3CH2CO2Li) and Li2CO3 as solid residues. The lithium propionate decomposes over the temperature range of 300–600 °C to evolve pentanone leaving Li2CO3 as a residual solid. Finally, the Li2CO3 decomposes over 600 °C to evolve CO2 leaving Li2O as a residual solid. A very similar thermal decomposition process is observed for the SEI generated on cycled silicon electrodes. However, two additional thermal decomposition reactions were observed characteristic of LixPOyFz at 300 °C and the polyimide binder at 550 °C. TGA measurements of Si electrodes after various numbers of cycles suggest that the LEDC on Si electrodes thermally decomposes during cycling to form lithium propionate and Li2CO3, resulting in increased complexity of the SEI.},
doi = {10.1021/acs.chemmater.7b00454},
journal = {Chemistry of Materials},
number = 7,
volume = 29,
place = {United States},
year = {Fri Mar 17 00:00:00 EDT 2017},
month = {Fri Mar 17 00:00:00 EDT 2017}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/acs.chemmater.7b00454
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Cited by: 82 works
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Figures / Tables:

Figure 1 Figure 1: Cycling performances of the silicon/Li half-cell. Cy-cleability is displayed in upper panel in which lithiation/delithiation capacities are presented by white and black circles respectively. The lower panel is the corresponding Coulombic efficiency. Cut-off : 0.7~0.005 V (vs. Li/Li + ), Current : 1167 mA g -1 (1/3 C-rate,more » 0.76 mA cm -2 )« less
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    An in situ formed graphene oxide–polyacrylic acid composite cage on silicon microparticles for lithium ion batteries via an esterification reaction
    journal, January 2019

    • Jung, Chul-Ho; Kim, Kyeong-Ho; Hong, Seong-Hyeon
    • Journal of Materials Chemistry A, Vol. 7, Issue 20
    • DOI: 10.1039/c9ta02654a

    In situ combined analysis of gases and electrochemical signals of an activated carbon-based supercapacitor at 2.7–4 V
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