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Title: 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.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Electricity Delivery and Energy Reliability (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; 670885
Grant/Contract Number:  
AC04-94AL85000; NA0003525
Resource Type:
Published Article
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
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, 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, Engerer, Jeffrey D., & Hewson, John C. Predicting High-Temperature Decomposition of Lithiated Graphite: Part I. Review of Phenomena and a Comprehensive Model. United States. doi:10.1149/2.0541816jes.
Shurtz, Randy, 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. doi: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 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 = {2018},
month = {12}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.1149/2.0541816jes

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Cited by: 2 works
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