Manufacturing process modeling of bilayer cathode for graded thick electrode design
Abstract
The energy density and rate capability of lithium-ion batteries can be improved through the design of bilayer and compositionally graded architectures for thick electrodes. For this, manufacturing steps such as drying and calendering are key considerations, since they determine the final electrode microstructure and therefore affect its electrochemical performance. Here, we extend our previously developed processcoupled coarse-grained molecular dynamics and discrete element method manufacturing computational workflow from single-layer LiNi0.33Co0.33Mn0.33O2 cathodes to bilayer cathode architectures. The model accounts for active material particles with realistic shapes obtained from X-ray micro-computed tomography. We use bilayer cathodes with different layer formulations as study cases. The Our simulation results show that the initial through-thickness heterogeneity can be preserved after slurry drying but is progressively reshaped during calendering. The layer-averaged porosity contrast can be weakened or even reversed under compression. This indicates a transition from porosity heterogeneity arising from slurry drying to residual porosity governed more by formulation-dependent particle packing. Meanwhile, the interfacial mixing region between the two layers broadens and the effective tortuosity factor increases sharply in the low-porosity regime. These results demonstrate that bilayer electrode design should be treated as a process-history-dependent engineering problem rather than as a static layer stacking one.
Related
- Manufacturing-conditioned hierarchical generation of cathode active-material microstructures with global electrode context
- Fiber-Scale Discrete Element Modeling Approach for Microstructural Evolution in Carbon Felt Electrode Manufacturing
- Battery Electrode Design Process Using Deep Neural Network
- Mathematical Modeling of Coupled Electronic and Ionic Transport Mechanics in Flow-Electrode Capacitive Deionization
- From Top to Bottom: Manufacturing Process‐Context Aware Resolution of Energy Device Electrodes Through a 3D Diffusion Generative Model
BibTeX
@misc{qin2026manufacturing,
title = {{Manufacturing process modeling of bilayer cathode for graded thick electrode design}},
author = {Lei Qin and Francisco Fernandez and Rares-George Scurtu and Margret Wohlfahrt-Mehrens and Alejandro A. Franco},
howpublished = {ChemRxiv},
year = {2026},
month = sep,
doi = {10.26434/chemrxiv.15009237/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009237/v1},
note = {CC BY},
}
RIS
TY - UNPB
TI - Manufacturing process modeling of bilayer cathode for graded thick electrode design
AU - Lei Qin
AU - Francisco Fernandez
AU - Rares-George Scurtu
AU - Margret Wohlfahrt-Mehrens
AU - Alejandro A. Franco
PY - 2026
DA - 2026/09/22
PB - ChemRxiv
DO - 10.26434/chemrxiv.15009237/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009237/v1
AB - The energy density and rate capability of lithium-ion batteries can be improved through the design of bilayer and compositionally graded architectures for thick electrodes. For this, manufacturing steps such as drying and calendering are key considerations, since they determine the final electrode microstructure and therefore affect its electrochemical performance. Here, we extend our previously developed processcoupled coarse-grained molecular dynamics and discrete element method manufacturing computational workflow from single-layer LiNi0.33Co0.33Mn0.33O2 cathodes to bilayer cathode architectures. The model accounts for active material particles with realistic shapes obtained from X-ray micro-computed tomography. We use bilayer cathodes with different layer formulations as study cases. The Our simulation results show that the initial through-thickness heterogeneity can be preserved after slurry drying but is progressively reshaped during calendering. The layer-averaged porosity contrast can be weakened or even reversed under compression. This indicates a transition from porosity heterogeneity arising from slurry drying to residual porosity governed more by formulation-dependent particle packing. Meanwhile, the interfacial mixing region between the two layers broadens and the effective tortuosity factor increases sharply in the low-porosity regime. These results demonstrate that bilayer electrode design should be treated as a process-history-dependent engineering problem rather than as a static layer stacking one.
ER -