LiCoO2 electrodes contain three phases, or domains, each having specific‐intended functions: ion‐conducting pore space, lithium‐ion‐reacting active material, and electron conducting carbon‐binder domain (CBD). Transport processes take place in all domains on different characteristic length scales: from the micrometer scale in the active material grains through to the nanopores in the carbon‐binder phase. Consequently, more than one imaging approach must be utilized to obtain a hierarchical geometric representation of the electrode. An approach incorporating information from the micro‐ and nanoscale to calculate 3D transport‐relevant properties in a large‐reconstructed active domain is presented. Advantages of focused ion beam/scanning electron microscopy imaging and X‐ray tomography combined by a spatial stochastic model, validated with an artificially produced reference structure are used. This novel approach leads to significantly different transport relevant properties compared with previous tomographic approaches: nanoporosity of the CBD leads to up to 42% additional contact area between active material and pore space and increases ionic conduction by a factor of up to 3.6. The results show that nanoporosity within the CBD cannot be neglected.
The fabrication process of Li-ion battery electrodes plays a prominent role in the microstructure and corresponding cell performance. Here, a mesoscale particle dynamics simulation is developed to relate the manufacturing process of a cathode containing Toda NCM-523 active material to physical and structural properties of the dried film. Particle interactions are simulated with shifted-force Lennard-Jones and granular Hertzian functions. LAMMPS, a freely available particle simulator, is used to generate particle trajectories and resulting predicted properties. To make simulations of the full film thickness feasible, the carbon binder domain (CBD) is approximated with μm-scale particles, each representing about 1000 carbon black particles and associated binder. Metrics for model parameterization and validation are measured experimentally and include the following: slurry viscosity, elasticity of the dried film, shrinkage ratio during drying, volume fraction of phases, slurry and dried film densities, and microstructure cross sections. Simulation results are in substantial agreement with experiment, showing that the simulations reasonably reproduce the relevant physics of particle arrangement during fabrication.
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