Myth and Reality of a Universal Lithium‐Ion Battery Electrode Design Optimum: A Perspective and Case Study

Abstract

The quest toward optimal electrode design for energy‐ and power‐demanding applications involves besides experimental effort also less resource‐intensive model‐based studies. The diversity of optimization objectives and benchmark systems complicates the practical utilization of available methods and gained knowledge. Despite the increasing importance of fast charging, electrode design studies commonly focus only on discharge characteristics. This paper features, besides an overview and perspective of electrode structuring concepts and optimization pathways, a model‐based full cell parameter screening of two‐layered electrodes for charge and discharge. The small fraction of cells with superior performance among the evaluated configurations underlines the importance of a joint experimental and model‐based electrode design optimization. The results further indicate that the performance of cell designs tailored for fast charge or fast discharge differs substantially; the gap widens if charging is terminated below 0 V versus Li/Li+ to prevent lithium plating. The broad parameter screening is complemented by a high‐resolution half cell parameter study. Their comparison underlines that the benefit of electrode structuring depends heavily on the study extent and the chosen benchmark. Furthermore, the importance of the parameter space surrounding an optimal electrode design for production with process tolerances is highlighted.

Digitalization Platform for Mechanistic Modeling of Battery Cell Production

“…The Doyle-Fuller-Newman-model type, also known as the Pseudo-2-Dimensional (P2D) model, represents a widespread solution since it allows a detailed investigation of the physico-chemical mechanisms inside the battery cell with a reasonable computational effort. These models can then be used to identify optimal electrode and cell structures by rigorous mathematical optimization [18]. They may further be connected to production models.…”

“…The chemical and electrochemical kinetics are also incorporated in the model. Consideration of various physical processes leads to more accurate predictions in terms of battery operation and consequently enables design optimization of the battery cell [18]. However, homogenization of the electrode volume simplifies the various processes, and local effects, like lithium plating, cannot be considered in detail.…”

The ARTISTIC Online Calculator: Exploring the Impact of Lithium‐Ion Battery Electrode Manufacturing Parameters Interactively Through Your Browser

“…Alternatively, the dataset constitued of the results already available in the platform can be utilized. Concerning iii), the electrode microstructures obtained by the online calculator can be either analyzed in terms of their averaged properties, as their tortuosity factor, [43] and use these properties as input of homogenized models, [44,45] or they can be used as direct input for 3D or 4D electrochemical models. For the latter, these structures should be meshed at first, which can be done through our recently released INNOV App, [46] accessible through the ARTISTIC computational portal as well [39] .…”

“…Alternatively, the dataset constitued of the results already available in the platform can be utilized. Concerning iii), the electrode microstructures obtained by the online calculator can be either analyzed in terms of their averaged properties, as their tortuosity factor, [43] and use these properties as input of homogenized models, [44,45] or they can be Figure 2. A schematic of the working principle behind the ARTISTIC online calculator, allowing to reproduce LIB electrode manufacturing, from the slurry to the calendered electrode, through a user-friendly web interface.…”

Analysis of Lithium‐Ion Battery State and Degradation via Physicochemical Cell and SEI Modeling

“…Simulation studies can be used proactively to develop cell designs with reduced mechanical stress in the active material, [3] to identify the impact of electrode manufacturing uncertainties on cell performance, [4] and to recommend application-specific electrode configurations, e. g., to prevent detrimental lithium plating during fast charging. [5] The prediction of the actual cell degradation remains an intricate challenge of lithium-ion battery technology, which is still too complex for predictive first principle aging models without extensive experimental data. [6,7] Advanced model-based cell diagnostics can help to improve the understanding of fundamental degradation-related and performance-limiting processes.…”