PARTICLES 2025

A Lattice-Particle Model for the Simulation of Calendering Process and Characterization of Na-ion Battery Electrodes

  • Valverde-González, Ángel (Universidad Loyola Andalucía)
  • Gonzalez, David (Universidad Loyola Andalucía)
  • Montero-Chacón, Francisco (Universidad Loyola Andalucía)

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Sodium-ion batteries (NIBs) have gained attention as they represent an alternative to sustainability-related issues inherent to Lithium-ion batteries (LIBs), among others. In contrast to Lithium, Sodium is a safer, more sustainable and scalable option, especially in stationary and grid integration. The electrochemical performance of NIBs is strongly influenced by the microstructural features resulting from the manufacturing process such as the slurry preparation, coating, drying, or calendering, which affect the ionic transport, porosity, or the mechanical integrity. Among them, the calendering process is critical in determining the porosity, tortuosity, and connectivity between the active particles, which define important properties such as the conductivity, storage capacity, and the cyclability of the electrodes. In this work, we present a lattice-particle modeling framework [1] that integrates both the diffusive and mechanical implications of the calendering process in NIBs. The microstructural features of the electrodes are modeled by means of Representative Volume Elements (RVE), that accounts for the main phases, namely, active material, additives, binder, and pores. The particles are placed following the take-and-place method meeting the mix design in terms of volume fractions and sieve curves of the phases. Once the RVE is virtually generated, it is subjected to uniaxial compression with a prescribed pressure until the target thickness is obtained, and a new microstructure (i.e., new particle positions, porosity, tortuosity) is achieved. The lattice-particle model is then adapted to solve the mechanical deformation and ionic diffusion problems [2], in a sequential analysis. The mechanical problem is solved via continuum damage formulation on the one-dimensional network obtained from the particle interactions, allowing different cases (i.e., particle separation, contact, or crushing). The evaluation of the electrochemical properties is tackled by means of Fickean diffusion of ionic species (i.e., Na+) within the compressed RVEs. The results obtained exhibit the effect of calendering process parameters, such as the compaction pressure, on the microstructural evolution (e.g., porosity, tortuosity) and electrochemical performance of graphite electrodes. The results are compared to empirical models existing in the literature, adapting these to NIBs, which is fundamental to improve the manufacturing process of these type of batteries.