Journal
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
Volume 165, Issue 16, Pages A3878-A3890Publisher
ELECTROCHEMICAL SOC INC
DOI: 10.1149/2.0541816jes
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Funding
- Department of Energy, Office of Electricity's Energy Storage Program
- U.S. Department of Energy's National Nuclear Security Administration [DE-NA0003525]
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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 similar to 200 degrees 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. (C) The Author(s) 2018. Published by ECS.
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