The charge/discharge capabilities of Li-ion cathodes are influenced by the meso-scale geometry, transport properties, and morphological parameters of the constituent phases in the cathode: active material, binder, conductive additive, and pore. Electrode processing influences the structure and attendant properties of these constituents. Thus, performance of the battery can be enhanced by correlating various electrode processing techniques with the charge/discharge behavior in the lithium-ion cathodes. X-ray microtomography was used to image samples obtained from pristine Li(Ni 1/3 Mn 1/3 Co 1/3 )O 2 (NMC) cathodes subjected to distinct processing approaches. Two sample preparation approaches were applied to the samples prior to microtomography. Casting the samples in epoxy yielded only the cathode active material domain. Encapsulating the sample with Kapton tape yielded phase contrast data that permitted segmentation of the active material and combined carbon/binder and pore regions. Geometrical and morphological details of the active material and the secondary phases were characterized and compared between the varied processing approaches. Calendered and ball-milled samples exhibited distinct differences in both geometry and morphology. Drying modes demonstrated variation in the distribution of the secondary and pore phases. Applying phase contrast capabilities, the processing−morphology relationship can be better understood to enhance overall battery performance across multiple scales.
Advancement of lithium-ion batteries for transportation applications requires addressing two key challenges: increasing energy density and providing fast charging capabilities. The first of these challenges can be met using thicker electrodes. However, the implementation of thick electrodes inherently presents a trade-off with respect to fast charging. As the thickness is increased, transport limitations reduce the ability of the battery to meet aggressive charge conditions. At the particle scale, interactions between solid diffusion and reaction kinetics influence the effective storage of lithium. At the electrode scale, diffusion limitations can lead to local variations in salt concentrations and electric potential. These short-range and long-range effects can combine to influence local current and heat generation. In the present work, a pseudo-2D lithium-ion battery model is applied to understand how active material particle size, porosity, and electrode thickness impact local field variables, current, heat generation, and cell capacity within a single-cell stack. The model was built assuming that the active particles are representative spherical particles. The governing equations and boundary conditions were set following the common Newman model. Cell response under varied combinations of charge and discharge cycling is assessed for rates of 1 C and 5 C. Aggressive charge and discharge conditions lead to locally elevated C-rates and attendant increases in local heat generation. These variations can be impacted in part by tailoring electrode structures. To this end, results for parametric studies of active material particle size, porosity, and electrode thickness are presented and discussed.
The continued advancement of lithium ion batteries for transportation applications requires addressing two key challenges: increasing energy density and providing fast charging capabilities. The first of these challenges can be met in part through the use of thicker electrodes, which reduce the electrochemically inactive mass of the cell. However, implementation of thick electrodes inherently presents a trade-off with respect to fast charging capabilities. As thickness is increased, transport limitations exert greater influence on battery performance and reduce the ability of the battery to meet aggressive charge conditions. This trade-off can manifest over multiple length scales. At the particle-scale, interactions between solid diffusion and reaction kinetics influence the effective storage of lithium within the active material. At the electrode scale, diffusion limitations can lead to local variations in salt concentrations and electric potential. These short-range and long-range effects can combine to influence local current and heat generation. In the present work, a pseudo-2D lithium ion battery model is applied to understand how active material particle size, porosity, and electrode thickness impact local field variables, current, heat generation, and cell capacity within a single cell stack. COMSOL Multiphysics 5.2 is used to implement the pseudo-2D model of a lithium ion battery consisting of a graphite negative electrode, polymer separator, and lithium transition metal oxide positive electrode. Lithium hexafluorophosphate (LiPF6) in 1:1 ethylene carbonate (EC) and diethylene carbonate (DEC) was used as the electrolyte. The model was built assuming that the active particles are representative spherical particles. The governing equations and boundary conditions were set following the common Newman model. Cell response under varied combinations of charge and discharge cycling is assessed for rates of 1C and 5C. Aggressive charge and discharge conditions lead to locally elevated C-rates and attendant increases in local heat generation. These variations can be impacted in part by tailoring electrode structures. To this end, results for parametric studies of active material particle size, porosity, and electrode thickness are presented and discussed.
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