Current and future lithium-ion battery manufacturing

Conventional nickel-rich cathode materials suffer from reaction heterogeneity during electrochemical cycling particularly at high temperature, because of their polycrystalline properties and secondary particle morphology. Despite intensive research on the morphological evolution of polycrystalline nickel-rich materials, its practical investigation at the electrode and cell levels is still rarely discussed. Herein, an intrinsic limitation of polycrystalline nickel-rich cathode materials in high-energy full-cells is discovered under industrial electrode-fabrication conditions. Owing to their highly unstable chemo-mechanical properties, even after the first cycle, nickel-rich materials are degraded in the longitudinal direction of the high-energy electrode. This inhomogeneous degradation behavior of nickel-rich materials at the electrode level originates from the overutilization of active materials on the surface side, causing a severe non-uniform potential distribution during long-term cycling. In addition, this phenomenon continuously lowers the reversibility of lithium ions. Consequently, considering the degradation of polycrystalline nickel-rich materials, this study suggests the adoption of a robust single-crystalline LiNi0.8 Co0.1 Mn0.1 O2 as a feasible alternative, to effectively suppress the localized overutilization of active materials. Such an adoption can stabilize the electrochemical performance of high-energy lithium-ion cells, in which superior capacity retention above ≈80% after 1000 cycles at 45 °C is demonstrated.

Boosting Reaction Homogeneity in High-Energy Lithium-Ion Battery Cathode Materials.

All-solid-state lithium batteries are promising next-generation energy storage devices that have gained increasing attention in the past decades due to their huge potential towards higher energy density and safety. As a key component, solid electrolytes have also attracted significant attention and have experienced major breakthroughs, especially in terms of Li-ion conductivity. However, the poor electrode compatibility of solid electrolytes can lead to the degradation of electrolyte/electrode interfaces, which is the major cause for failure in all-solid-state lithium batteries. To address this, this review will summarize the in-depth understanding of physical and chemical interactions between electrolytes and electrodes with a focus on the contact, charge transfer and Li dendrite formation occurring at electrolyte/electrode interfaces. Based on mechanistic analyses, this review will also briefly present corresponding strategies to enhance electrolyte/electrode interfaces through compositional modifications and structural designs. Overall, the comprehensive insights into electrolyte/electrode interfaces provided by this review can guide the future investigation of all-solid-state lithium batteries.

Electrolyte/Electrode Interfaces in All-Solid-State Lithium Batteries: A Review

Investigating electrode calendering and its impact on electrochemical performance by means of a new discrete element method model: Towards a digital twin of Li-Ion battery manufacturing

Microstructural Evolution of Battery Electrodes During Calendering

Numerical simulation of the behavior of lithium-ion battery electrodes during the calendaring process via the discrete element method

Structural and mechanical characterization of lithium-ion battery electrodes via DEM simulations

Mechanical, Electrical, and Ionic Behavior of Lithium-Ion Battery Electrodes via Discrete Element Method Simulations

https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceat.201900501

Modeling the electrical conductive paths within all‐solid‐state battery electrodes

In this paper, a widely mechanistic model was developed to depict the rheological behaviour of nanoparticulate suspensions with solids contents up to 20 wt.%, based on the increase in shear stress caused by surface interaction forces among particles. The rheological behaviour is connected to drag forces arising from an altered particle movement with respect to the surrounding fluid. In order to represent this relationship and to model the viscosity, a hybrid modelling approach was followed, in which mechanistic relationships were paired with heuristic expressions. A genetic algorithm was utilized during model development, by enabling the algorithm to choose among several hard-to-assess model options. By the combination of the newly developed model with existing models for the various physical phenomena affecting viscosity, it can be applied to model the viscosity over a broad range of solids contents, shear rates, temperatures and particle sizes. Due to its mechanistic nature, the model even allows an extrapolation beyond the limits of the data points used for calibration, allowing a prediction of the viscosity in this area. Only two parameters are required for this purpose. Experimental data of an epoxy resin filled with boehmite nanoparticles were used for calibration and comparison with modelled values.

https://www.mdpi.com/1996-1944/14/11/2752/pdf

Clara Sangrós Giménez

Papers

Numerical simulation of the behavior of lithium-ion battery electrodes during the calendaring process via the discrete element method

Structural and mechanical characterization of lithium-ion battery electrodes via DEM simulations

Mechanical, Electrical, and Ionic Behavior of Lithium-Ion Battery Electrodes via Discrete Element Method Simulations

Modeling the electrical conductive paths within all‐solid‐state battery electrodes

Viscosity Model for Nanoparticulate Suspensions Based on Surface Interactions