Predicting High-Temperature Decomposition of Lithiated Graphite: Part I. Review of Phenomena and a Comprehensive Model
Abstract
Heat release that leads to thermal runaway of lithium-ion batteries begins with decomposition reactions associated with lithiated graphite. We broadly review the observed phenomena related to lithiated graphite electrodes and develop a comprehensive model that predicts with a single parameter set and with reasonable accuracy measurements over the available temperature range with a range of graphite particle sizes. The model developed in this work uses a standardized total heat release and takes advantage of a revised dependence of reaction rates and the tunneling barrier on specific surface area. The reaction extent is limited by inadequate electrolyte or lithium. Calorimetry measurements show that heat release from the reaction between lithiated graphite and electrolyte accelerates above ~200°C, and the model addresses this without introducing additional chemical reactions. This method assumes that the electron-tunneling barrier through the solid electrolyte interphase (SEI) grows initially and then becomes constant at some critical magnitude, which allows the reaction to accelerate as the temperature rises by means of its activation energy. Phenomena that could result in the upper limit on the tunneling barrier are discussed. The model predictions with two candidate activation energies are evaluated through comparisons to calorimetry data, and recommendations are made for optimal parameters.
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Sponsoring Org.:
- USDOE Office of Electricity (OE); USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1487161
- Alternate Identifier(s):
- OSTI ID: 1492360
- Report Number(s):
- SAND-2018-13764J
Journal ID: ISSN 0013-4651; /jes/165/16/A3878.atom
- Grant/Contract Number:
- AC04-94AL85000; NA0003525
- Resource Type:
- Published Article
- Journal Name:
- Journal of the Electrochemical Society
- Additional Journal Information:
- Journal Name: Journal of the Electrochemical Society Journal Volume: 165 Journal Issue: 16; Journal ID: ISSN 0013-4651
- Publisher:
- The Electrochemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; 36 MATERIALS SCIENCE; Batteries; Batteries - Lithium; Lithiated Graphite; Solid Electrolyte Interphase; Thermal Runaway
Citation Formats
Shurtz, Randy C., Engerer, Jeffrey D., and Hewson, John C. Predicting High-Temperature Decomposition of Lithiated Graphite: Part I. Review of Phenomena and a Comprehensive Model. United States: N. p., 2018.
Web. doi:10.1149/2.0541816jes.
Shurtz, Randy C., Engerer, Jeffrey D., & Hewson, John C. Predicting High-Temperature Decomposition of Lithiated Graphite: Part I. Review of Phenomena and a Comprehensive Model. United States. https://doi.org/10.1149/2.0541816jes
Shurtz, Randy C., Engerer, Jeffrey D., and Hewson, John C. Fri .
"Predicting High-Temperature Decomposition of Lithiated Graphite: Part I. Review of Phenomena and a Comprehensive Model". United States. https://doi.org/10.1149/2.0541816jes.
@article{osti_1487161,
title = {Predicting High-Temperature Decomposition of Lithiated Graphite: Part I. Review of Phenomena and a Comprehensive Model},
author = {Shurtz, Randy C. and Engerer, Jeffrey D. and Hewson, John C.},
abstractNote = {Heat release that leads to thermal runaway of lithium-ion batteries begins with decomposition reactions associated with lithiated graphite. We broadly review the observed phenomena related to lithiated graphite electrodes and develop a comprehensive model that predicts with a single parameter set and with reasonable accuracy measurements over the available temperature range with a range of graphite particle sizes. The model developed in this work uses a standardized total heat release and takes advantage of a revised dependence of reaction rates and the tunneling barrier on specific surface area. The reaction extent is limited by inadequate electrolyte or lithium. Calorimetry measurements show that heat release from the reaction between lithiated graphite and electrolyte accelerates above ~200°C, and the model addresses this without introducing additional chemical reactions. This method assumes that the electron-tunneling barrier through the solid electrolyte interphase (SEI) grows initially and then becomes constant at some critical magnitude, which allows the reaction to accelerate as the temperature rises by means of its activation energy. Phenomena that could result in the upper limit on the tunneling barrier are discussed. The model predictions with two candidate activation energies are evaluated through comparisons to calorimetry data, and recommendations are made for optimal parameters.},
doi = {10.1149/2.0541816jes},
journal = {Journal of the Electrochemical Society},
number = 16,
volume = 165,
place = {United States},
year = {Fri Dec 14 00:00:00 EST 2018},
month = {Fri Dec 14 00:00:00 EST 2018}
}
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