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Phase Transformation Dynamics in Porous Battery Electrodes

Author(s)
Ferguson, Todd Richard; Bazant, Martin Z
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Abstract
Porous electrodes composed of multiphase active materials are widely used in Li-ion batteries, but their dynamics are poorly understood. Two-phase models are largely empirical, and no models exist for three or more phases. Using a modified porous electrode theory based on non-equilibrium thermodynamics, we show that experimental phase behavior can be accurately predicted from free energy models, without artificially placing phase boundaries or fitting the open circuit voltage. First, we simulate lithium intercalation in porous iron phosphate, a popular two-phase cathode, and show that the zero-current voltage gap, sloping voltage plateau and under-estimated exchange currents all result from size-dependent nucleation and mosaic instability. Next, we simulate porous graphite, the standard anode with three stable phases, and reproduce experimentally observed fronts of color-changing phase transformations. These results provide a framework for physics-based design and control for electrochemical systems with complex thermodynamics.
Date issued
2014-09
URI
http://hdl.handle.net/1721.1/109043
Department
Massachusetts Institute of Technology. Department of Chemical Engineering; Massachusetts Institute of Technology. Department of Mathematics
Journal
Electrochimica Acta
Publisher
Elsevier
Citation
Ferguson, Todd R., and Martin Z. Bazant. “Phase Transformation Dynamics in Porous Battery Electrodes.” Electrochimica Acta 146 (November 2014): 89–97.
Version: Original manuscript
ISSN
00134686

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