Multiphase Porous Electrode Theory
Name
J. Electrochem. Soc.-2017-Smith-E3291-310.pdf
Description
Published version
Size
1.04 MB
Format
Unknown
Checksum (MD5)
e0103f08a4b295cc4241c00da713c2fd
Author(s)
Smith, Raymond Barrett
Bazant, Martin Z
Date Issued
2017
Journal
Journal of The Electrochemical Society
Publisher
The Electrochemical Society
Version
Final published version
Abstract
© The Author(s) 2017. Porous electrode theory, pioneered by John Newman and collaborators, provides a macroscopic description of battery cycling behavior, rooted in microscopic physical models. Typically, the active materials are described as solid solution particles with transport and surface reactions driven by concentration fields, and the thermodynamics are incorporated through fitting of the open circuit potential. However, this approach does not apply to phase separating materials, for which the voltage is an emergent property of inhomogeneous concentration profiles, even in equilibrium. Here, we present a general framework, "multiphase porous electrode theory", based on nonequilibrium thermodynamics and implemented in an open-source software package called "MPET". Cahn-Hilliard-type phase field models are used to describe the active materials with suitably generalized models of interfacial reaction kinetics. Classical concentrated solution theory is implemented for the electrolyte phase, and Newman's porous electrode theory is recovered in the limit of solid solution active materials with Butler-Volmer kinetics. More general, quantum-mechanical models of faradaic reactions are also included, such as Marcus-Hush-Chidsey kinetics for electron transfer at electrodes, extended for concentrated solutions. The full model and implementation are described, and a variety of example calculations are presented to illustrate the novel features of the software compared to existing battery models.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Mathematics
Terms of Use
Creative Commons Attribution 4.0 International license
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1149/2.0171711JES
