Physics-based battery models are important tools in battery research, development, and control. To obtain useful information from the models, accurate parametrization is essential. A complex model structure and many unknown and hard-to-measure parameters make parametrization challenging. Furthermore, numerous applications require non-invasive parametrization relying on parameter estimation from measurements of current and voltage. Parametrization of physics-based battery models from input-output data is a growing research area with many recent publications. This paper aims to bridge the gap between researchers from different fields that work with battery model parametrization, since successful parametrization requires both knowledge of the underlying physical system as well as understanding of theory and concepts behind parameter estimation. The review encompasses sensitivity analyses, methods for parameter optimization, structural and practical identifiability analyses, design of experiments and methods for validation as well as the use of machine learning in parametrization. We highlight that not all model parameters can accurately be identified nor are all relevant for model performance. Nonetheless, no consensus on parameter importance could be shown. Local methods are commonly chosen because of their computational advantages. However, we find that the implications of local methods for analysis of non-linear models are often not sufficiently considered in reviewed literature.

Li-ion batteries are a key enabling technology for electric vehicles and determining their properties precisely is an essential step in improving utilization and performance. Batteries are highly complex electrochemical sys-tems, with processes occurring in parallel on many time-and length-scales. Models describing these mechanisms require extensive parametrization efforts, conventionally using a combination of ex-situ characterization and systems identification. We present a methodology that algorithmically designs current input signals to optimize parameter identifiability from voltage measurements. Our approach uses global sensitivity analysis based on the generalized polynomial chaos expansion to map the entire parameter uncertainty space, relying on minimal prior knowledge of the system. Parameter specific optimal experiments are designed to maximize sensitivity and simultaneously minimize interactions and unwanted contributions by other parameters. Experiments are defined using only three design variables making our approach computationally efficient. The methodology is demon-strated using the Doyle-Fuller-Newman battery model for eight parameters of a 2.6 Ah 18,650 cell. Validation confirms that the proposed approach significantly improves model performance and parameter accuracy, while lowering experimental burden.

Lithium-ion battery degradation is complex, and many mechanisms occur concurrently. In-depth degradation is traditionally investigated by post-mortem characterization in lab-settings. If mechanisms could instead be identified in-operando, utilization could be adjusted, and battery lifetime extended. We investigate changes in electrochemical model parameters during battery testing and their correlation with degradation observed in a traditional post-mortem characterization. Commercial batteries are cycle-aged using different stationary storage service cycles and a novel reference performance test is applied intermittently. This test is based on current profiles optimally designed with respect to maximized sensitivity for individual electrochemical parameters and embedded within a charging procedure. Usage dependency of parameter trajectories over the course of ageing is demonstrated and coupled to observed micro-structural changes. Subsequently, the parameter trajectories are extrapolated using Gaussian Process Regression for physics-based state-of-health estimation and remaininguseful-life prediction. We demonstrate and validate estimation of full cell performance under constant load at a later state in life.

Li-ion batteries in electric vehicles must be utilized more efficiently to lower their economic and environmental cost. To achieve this increase in efficiency, it is of large interest to develop more thorough battery management that can predict internal states in online settings and update usage and control accordingly. Electrochemical models are an important tool in achieving this, and their implementation in battery management systems is the topic of ongoing research. However, electrochemical battery management relies on accurate parametrization and thus requires re-parametrization as a battery ages. We therefore studied viability of re-parametrization for electrochemical model-based battery management. To this end, we performed global sensitivity analysis on selected Doyle-Fuller-Newman model parameters using on-board current measurements. Representative driving data was collected from several types of heavy-duty vehicles. This elucidated which model parameters should be updated periodically to conserve model accuracy and which parameters are sensitive enough to be estimated from the on-board data. Additionally, we studied how parameter uncertainty affects estimation of internal states and highlight how model-based state estimation relying on a beginning-of-life parametrization degrades as electrochemical parameters change with aging.

Fast charging of electric vehicles remains a compromise between charging time and degradation penalty. Conventional battery management systems use experience-based charging protocols that are expected to meet vehicle lifetime goals. Novel electrochemical model-based battery fast charging uses a model to observe internal battery states. This enables control of charging rates based on states such as the lithium-plating potential but relies on an accurate model as well as accurate model parameters. However, the impact of battery degradation on the model’s accuracy and therefore the fitness of the estimated optimal charging procedure is often not considered. In this work, we therefore investigate electrochemical model-based aging-adaptive fast charging of automotive lithium-ion cells. First, an electrochemical model is identified at the beginning of life for 6 automotive prototype cells and the electrochemically constrained fast-charge is designed. The model parameters are then periodically re-evaluated during a cycling study and the charging procedure is updated to account for cell degradation. The proposed method is compared with two reference protocols to investigate both the effectiveness of selected electrochemical constraints as well as the benefit of aging-adaptive usage. Finally, post-mortem characterization is presented to highlight the benefit of aging-adaptive battery utilization.

The effects of electrochemical aging on the mechanical properties of electrodes in lithium-ion batteries are challenging to measure and are largely unknown. Mechanochemical degradation processes occur at different scales within an electrode and understanding the correlation between the degradation of mechanical properties, electrochemical aging, and morphological changes is crucial for mitigating battery performance degradation. This paper explores the evolution of mechanical and electrochemical properties at the layer level in a Ni-rich positive electrode during the initial stages of electrochemical cycling. The investigation involves complementary cross-section analyses aimed at unraveling the connection between observed changes on both macroscopic and microscopic scales. The macroscopic constitutive properties were assessed using a U-shaped bending test method that had been previously developed. The compressive modulus exhibited substantial dependency on both the porous structure and binder properties. It experienced a notable reduction with electrolyte wetting but demonstrated an increase with cycling and aging. During the initial stages of aging, electrochemical impedance spectra revealed increased local resistance near the particle–electrolyte interface. This is likely attributable to factors such as secondary particle grain separation and the redistribution of carbon black. The swelling of particles, compression of the binder phase, and enhanced particle contact were identified as probable factors adding to the elevation of the elastic modulus within the porous layer as a result of cycling.