Collection of codes for the multiphase-smoothed-boundary method and the corresponding publication "Simulation of intercalation and phase transitions in nano-porous, polycrystalline agglomerates"
The abstract reads:
Optimal microstructure design of battery materials is critical to enhance the performance of batteries for tailored applications such as high power cells. Accurate simulation of the thermodynamics, transport, and electrochemical reaction kinetics in commonly used polycrystalline battery materials remains a challenge. Here, we combine state-of-the-art multiphase field modelling with the smoothed boundary method to accurately simulate complex battery microstructures and multiphase physics. The phase-field method is employed to parameterize complex open pore cathode microstructures and we present a formulation to impose galvanostatic charging conditions on the diffuse boundary representation. By extending the smoothed boundary method to the multiphasefield method, we build a simulation framework which is capable of simulating the coupled effects of intercalation, anisotropic diffusion, and phase transitions in arbitrary complex polycrystalline agglomerates. This method is directly compatible with voxel-based data, e.g. from X-ray tomography. The simulation framework is used to study the reversible phase transitions in LiXNiO2 in dense and nanoporous agglomerates. Based on the thermodynamic consistency of phase-field approaches with ab-initio simulations and the open circuit potential, we reconstruct the Gibbs free energies of four individual phases (H1, M, H2 and H3) from experimental cycling data. The results show remarkable agreement with previously published DFT results. From charge simulations, we discover a strong influence of particle morphology on the phase transition behaviour, in particular a shrinking core-like behaviour in dense polycrystalline structures and a particle-by-particle mosaic behavior in nanoporous samples. Overall, the proposed simulation framework enables the detailed study of phase transitions in intercalation materials to enhance microstructure design and fast charging protocols.
The code is based on python including the following libraries
- numpy
- scipy
- matplotlib
- pyvista
SD conceptualized the work and carried out the implementation and validation of the simulation code. SD, MR, DS and QH all contributed to the formulation and validation of the MP-SBM method. SD, AEC and MZB formulated the electrochemical model; simulation studies and data visualization were carried out by SD and MW. DS and BN provided funding for the project. SD, AEC, QH, MZB and BN wrote the manuscript. All authors read and approved the final manuscript.
This work contributes to the research performed at CELEST (Center for Electrochemical Energy Storage Ulm-Karlsruhe) and was funded by the German Research Foundation (DFG) under Project ID 390874152 (POLiS Cluster of Excellence). Support by the Helmholtz association though the MTET programme (no. 38.02.01) is gratefully acknowledged.
This code has been published under the MIT licence.