Lithium-ion Battery Degradation Research Articles

Failure analysis of ternary lithium-ion batteries throughout the entire life cycling at high temperature

The operation life is a key factor affecting the cost and application of lithium-ion batteries. This article investigates the changes in discharge capacity, median voltage, and full charge DC internal resistance of the 25Ah ternary (LiNi0.5Mn0.3Co0.2O2/graphite) lithium-ion battery during full life cycles at 45 °C and 2000 cycles at 25 °C for comparison. The batteries before and after cycling were disassembled, and the structure, morphology, interface characteristics, element content of the cathode and anode plates of the battery were characterized. By analyzing the failure factors of the performance of the ternary batteries during the 45 °C cycling, a reaction mechanism for the rapid decline of high-temperature cycling performance of ternary batteries has been proposed. The results show that the performance degradation of the ternary lithium-ion batteries in the whole life operated at high temperature is characterized by slow decline in the initial stage and rapid drop in the latter stage. Further analysis of physical and chemical performance revealed irreversible damage to both the cathode and anode. The dissolution of transition metal ions from the cathode and their deposition on the anode surface catalyze the decomposition of electrolyte solvents to produce a large amount of gas. Gassing, accompanied by the deposition of Li2CO3 and the thickening of SEI, leads to an increase in the internal resistance of the battery. The coupling between gassing and increased internal resistance is responsible for the rapid drop in the performance of the ternary batteries during high-temperature cycling.

Enhancing Electrochemical Performance of Si@CNT Anode by Integrating SrTiO3 Material for High-Capacity Lithium-Ion Batteries

Silicon (Si) has attracted worldwide attention for its ultrahigh theoretical storage capacity (4200 mA h g−1), low mass density (2.33 g cm−3), low operating potential (0.4 V vs. Li/Li+), abundant reserves, environmentally benign nature, and low cost. It is a promising high-energy-density anode material for next-generation lithium-ion batteries (LIBs), offering a replacement for graphite anodes owing to the escalating energy demands in booming automobile and energy storage applications. Unfortunately, the commercialization of silicon anodes is stringently hindered by large volume expansion during lithiation–delithiation, the unstable and detrimental growth of electrode/electrolyte interface layers, sluggish Li-ion diffusion, poor rate performance, and inherently low ion/electron conductivity. These present major safety challenges lead to quick capacity degradation in LIBs. Herein, we present the synergistic effects of nanostructured silicon and SrTiO3 (STO) for use as anodes in Li-ion batteries. Si and STO nanoparticles were incorporated into a multiwalled carbon nanotube (CNT) matrix using a planetary ball-milling process. The mechanical stress resulting from the expansion of Si was transferred via the CNT matrix to the STO. We discovered that the introduction of STO can improve the electrochemical performance of Si/CNT nanocomposite anodes. Experimental measurements and electrochemical impedance spectroscopy provide evidence for the enhanced mobility of Li-ions facilitated by STO. Hence, incorporating STO into the Si@CNT anode yields promising results, exhibiting a high initial Coulombic efficiency of approximately 85%, a reversible specific capacity of ~800 mA h g−1 after 100 cycles at 100 mA g−1, and a high-rate capability of 1400 mA g−1 with a capacity of 800 mA h g−1. Interestingly, it exhibits a capacity of 350 mAh g−1 after 1000 lithiation and delithiation cycles at a high rate of 600 mA hg−1. This result unveils and sheds light on the design of a scalable method for manufacturing Si anodes for next-generation LIBs.

Diagnosis of lithium-ion batteries degradation with P2D model parameters identification: a case study on low temperature charging

The estimation of the state of health (SoH) of a lithium-ion battery is still a hot topic in the scientific research. This publication deals with the combined use of optimized tests, also involving impedance spectroscopy, and physical models to investigate lithium-ion batteries degradation. As a case study, this method is firstly applied on a low-temperature charging degradation campaign, in order to expectedly generate a lithium plating-dominated ageing state. Degradation tests, performed under previously selected combinations of operating conditions, are performed down to 75% SoH on commercial samples, determining severe ageing rate up to 1.5% capacity loss per equivalent full cycle. The proposed interpretation methodology identifies the ageing to be dominated by the loss of lithium inventory, consistently with the expected degradation mechanism. Large electrolyte consumption is also detected, which induces a strongly anisotropic utilization of the electrodes during discharge, as confirmed by pseudo-two-dimensional (P2D) model simulations.This activity contributes to verify the reliability of the methodology, elucidate the effect of lithium plating on the performance and underline the effect of the operating conditions at low temperature, paving the way to the application on real-world conditions.

Life Degradation of Lithium-Ion Batteries Under Vehicle-to-Grid Operations Based on a Multi-physics Model

Life Degradation of Lithium-Ion Batteries Under Vehicle-to-Grid Operations Based on a Multi-physics Model

Effect of fast charging on degradation and safety characteristics of lithium-ion batteries with LiFePO4 cathodes

Fast charging compatibility is a desirable feature for batteries to shape a promising future in our rechargeable world. Enabling fast charging of advanced energy-dense Li-ion batteries for growing electric vehicle (EV) markets depends on the breakthrough of material chemistry and optimization of charging strategy. Lithium iron phosphate (LiFePO4, or LFP) is a pivotal cathode material in state-of-the-art EV batteries due to the merits of high thermal stability, long cycle lifetime, and high-temperature performance. However, degradation-safety interactions of LFP-based Li-ion batteries under fast charging conditions and low temperatures remain elusive. In this study, we cycle LFP cells under different fast charging strategies and thermal environments to understand their effects on degradation pathways, where the capacity, voltage, temperature, coulombic inefficiency, internal resistance, and impedance spectroscopy are evaluated. Half-cell studies are implemented to assess electrode-level capacity retentions. Post-mortem analyses are conducted to reveal physicochemical changes in electrodes. Accelerating rate calorimeter tests are carried out to measure evolutions of cell-level thermal instabilities after fast charging tests. This research article highlights the significant roles of graphite-centric lithium plating and LFP-centric transition metal dissolution in driving substantial electrochemical degradations, suggesting that a mild low temperature does not necessarily reduce the LFP cell lifetime.

Evolution of aging mechanisms and performance degradation of lithium-ion battery from moderate to severe capacity loss scenarios

The aging mechanisms of Nickel-Manganese-Cobalt-Oxide (NMC)/Graphite lithium-ion batteries are divided into stages from the beginning-of-life (BOL) to the end-of-life (EOL) of the battery. The corresponding changes in the battery performance across these stages have been analyzed, and a digital twin model is established to quantify the primary parameters that influence these aging mechanisms. Post-mortem analysis is applied to validate the results. This paper compares the aging mechanisms from BOL to EOL using two charging protocols: a multi-step fast charge protocol and a common constant-current fast charge protocol that applies the average current of multi-step currents. Notably, a transition from a linear to a non-linear degradation trend in capacity fade is observed, beginning from a 10% capacity reduction to EOL. From BOL to 10% degradation, the resistance of solid electrolyte interphase (SEI) grows steadily. The graphite anode’s crack depth exhibits a significant increase, accompanied by an evident collapse of cathode materials in all the test cases following a 10% degradation until EOL. This phenomenon can be attributed to one primary reason—the expansion of the corresponding simulated resistance of charge transfer (Rct). Post-mortem analysis revealed the change in morphology, structure, and composition of various degradation conditions. This analysis proved that the primary driver of the linear aging stage is the SEI growth. Furthermore, it is evident that the transition to a non-linear aging degradation is dominated by electrode defects resulting from continuous mechanical stress during long-term aging.

Modeling Particle Versus SEI Cracking in Lithium-Ion Battery Degradation: Why Calendar and Cycle Aging Cannot Simply be Added

Degradation models are important tools for understanding and mitigating lithium-ion battery aging, yet a universal model that can predict degradation under all operating conditions remains elusive. One challenge is the coupled influence of calendar and cycle aging phases on degradation mechanisms, such as solid electrolyte interphase (SEI) formation. In this work, we identify and systematically compare three different SEI interaction theories found in the literature, and apply them to experimental degradation data from a commercial lithium-ion cell. In a step-by-step process, and after careful data selection, we show that SEI delamination without any cracking of the active particles, and SEI microcracking, where cycling only affects SEI growth during the cycle itself, are both unlikely candidates. Instead, the results indicate that upon cycling, both the SEI and the active particle crack, and we provide a simple, 4-parameter equation that can predict the particle crack rate. Contrary to the widely-accepted Paris’ law, the particle crack rate decreases with increasing cycles, potentially due to changing intercalation dynamics resulting from the increasing surface-to-volume ratio of the active particles. The proposed model predicts SEI formation accurately at different storage conditions, while simply adding the degradation from pure calendar and cycle aging underestimates the total degradation.

Predictive analytics for prolonging lithium-ion battery lifespan through informed storage conditions

The capacity degradation of lithium-ion batteries occurs both during storage and operational usage. This paper investigates the capacity degradation of lithium-ion batteries during storage (calendar ageing) by analysing the interplay of storage temperature, state-of-charge (SOC), and time. Leveraging the machine learning techniques of Gaussian process regression and extreme gradient boosting (XGBoost), a predictive model is developed to characterize the degradation patterns. The study includes a sensitivity analysis of stress factors to identify their relative impact on degradation. The insights gained from this analysis are utilized to recommend optimal storage conditions, offering practical guidance for enhancing the durability and performance of lithium-ion batteries in real-world applications.

Reduced artifacts in dynamic electrochemical impedance spectroscopy applied to battery degradation analysis

Lithium-ion batteries (LIBs) degradation can be classified into capacity reduction and increase of the internal resistance. Accurate estimation of degradation is important to determine the economic value and the remaining useful life of the battery. This paper adopts dynamic electrochemical impedance spectroscopy (EIS) to evaluate degradation while charging the battery, without requiring additional time for the analysis. A new method is proposed to remove the artifacts arising from the time-variance of the system during the measurement. The validity of the method is confirmed by comparing it with the results obtained by static EIS measurements at equilibrium. The spectra are fitted to an equivalent circuit containing three resistances (R0, R1, R2). The method is applied to data obtained before and after aging cycles performed at 1.4C charge and 2.0C discharge rates, at 25 °C, 10 °C and −5 °C. The resistance of the films (R1), which is obtained from the semicircle at high frequencies in the EIS spectrum, has proved to be the key indicator of aging, and linearly depends on the SoC. The increase of R1 dominates among all the resistances, particularly at higher temperatures. Dynamic EIS is considered a powerful tool to diagnose LIBs in practical applications.

Differential pulse voltammetry analytics for lithium-ion battery degradation

Differential pulse voltammetry analytics for lithium-ion battery degradation

Decomposition of Electrolyte Solutions at Positive Electrodes

Preventing the decomposition reactions of electrolyte solutions is essential for extending the lifetime of lithium-ion batteries. However, the high voltage (>4.5 V) reactivity of commonly used electrolyte solutions is still poorly understood; electrolyte decomposition at the positive electrode is generally believed to proceed via electrochemical oxidation of the organic carbonate solvent,1 while more recent work has revealed an alternative pathway involving reactive lattice oxygen species originating from the positive electrode (i.e., singlet oxygen).2 Unfortunately, we still have a limited understanding of these reactions, the products that form, and which chemical structural units in the electrolyte solution make them reactive - all of which make it challenging to assess and mitigate the impact of electrolyte decomposition on the battery’s lifetime.In this work, operando gas measurements and solution NMR were combined to study the electrochemical and chemical decomposition of widely used electrolyte salts, solvents, and additives. First, the electrochemical stability of the electrolyte components was reviewed against C65 electrodes in a standard H-cell setup: all solvents reveal little decomposition up to 5.5 V (vs Li/Li+), consistent with previous electrochemical measurements.3,4 Based on the experimentally detected soluble and gaseous products, the electrochemical decomposition mechanism is inferred. Subsequently, the chemical stability against reactive oxygen species (i.e., singlet oxygen; 1O2, peroxide anion; O2 2 −, and superoxide radical anion, O2 −) was explored. All carbonate solvents demonstrated instability against reactive oxygen species. As before, the experimentally detected gaseous and soluble products were used to infer the decomposition mechanisms. The proposed mechanisms were verified using 17O and 18O isotopic labeling for NMR spectroscopy and mass spectrometry measurements, respectively. The findings on the reactivity between the electrolyte components and reactive oxygen species provide a deeper understanding of electrolyte decomposition processes occurring at high voltage positive electrodes (e.g., Li-rich layered and disordered rocksalt oxides, high-voltage spinels, and polyanionic materials). Moreover, these insights will support the development of more stable electrolyte formulations, further extending the lifetime of lithium-ion batteries.(1) Imhof, R.; Novak, P. Oxidative Electrolyte Solvent Degradation in Lithium-Ion Batteries: An In Situ Differential Electrochemical Mass Spectrometry Investigation. J Electrochem Soc 1999, 146 (5), 1702–1706.(2) Jung, R.; Metzger, M.; Maglia, F.; Stinner, C.; Gasteiger, H. A. Oxygen Release and Its Effect on the Cycling Stability of LiNi x Mn y Co z O 2 (NMC) Cathode Materials for Li-Ion Batteries. J Electrochem Soc 2017, 164 (7), A1361–A1377. https://doi.org/10.1149/2.0021707jes.(3) Zhang, X.; Soc, J. E.; Zhang, X.; Kostecki, R.; Richardson, T. J.; Pugh, J. K.; Ross, P. N. Electrochemical and Infrared Studies of the Reduction of Organic Carbonates Electrochemical and Infrared Studies of the Reduction of Organic Carbonates. Journal of The Electrochemical Society 2001, 148 (12), A1341–A1345. https://doi.org/10.1149/1.1415547.(4) Moshkovich, M.; Cojocaru, M.; Gottlieb, H. E.; Aurbach, D. The Study of the Anodic Stability of Alkyl Carbonate Solutions by in Situ FTIR Spectroscopy, EQCM, NMR and MS. Journal of Electroanalytical Chemistry 2001, 497, 84–96. https://doi.org/http://dx.doi.org/10.1016/S0022-0728(00)00457-5.

Profile of Round-Trip Efficiency of Lithium-Ion Battery Energy Storage System

Lithium-ion battery energy storage systems (Li-BESSs) are expected to adjust variable renewable energies such as photovoltaic energy. In the viewpoint of the energy management cost, profiles of round-trip efficiency (RTE) are important characteristics of Li-BESSs. The profiles of RTE are related to the characteristics of both LIBs and inverters installed on Li-BESSs. The characteristics of Li-BESSs would be various because of reusing and degradation of lithium-ion batteries (LIBs). And inverters made by a lot of manufacturers would be so on. Accordingly, it could be said that the understanding of the profile of each Li-BESS’s RTE is complex and difficult. Therefore, we studied the time series analysis of operation data and tried to estimate the characteristics of both LIBs and inverters. The important ones of LIB are full-charge capacity (FCC), open-circuit voltage (OCV), and internal resistance (R). In addition, characteristics of OCV and R can be expressed as function profiles with state of charge (SOC) as elements. Similarly, the important one of inverter is the typical efficiency curve. In this study, we proposed the estimation method of the profiles of OCV and R and inverter efficiency curve. On the other hand, FCC was given as assuming that general diagnosis results would be provided. Then, a RTE profile of Li-BESS (including 9.94kWh LIB and 10kW inverter) was tried to establish from the results of it. The profiles of OCV and R were estimated by the method called MGFFD (Modified Gaussian Free-Form Deformation) that we have been established [1]. The novelty of this study could be described as: Development of the estimation method of an efficiency curve of inverter installed on BESS during operation (Fig.1). Quantitatively visualized profile of RTE of Li-BESS by combining results of MGFFD estimation applied for LIBs and inverter (Fig.2). The profile described on Fig.2 is the relationship between SOC, input-output power rate of inverter, and RTE of Li-BESS. To understand Li-BESS’s charge-discharge efficiency of from state at that time to the end of an operation plan, it would be necessary information. This proposed method could clarify various RTE of Li-BESSs, consequently, be useful for its efficient operation by information communication technology.Reference[1] M. Arima, L. Lin, and M. Fukui, "Kalman-Filter-Based Learning of Characteristic Profiles of Lithium-Ion Batteries", Sensors, vol. 22, no. 14, 5156. Figure 1

Mechano-Electro-Chemical Impedance Spectroscopy (MeIS): Concept, Theory and Experiment

Electrochemical impedance spectroscopy (EIS) is a widely used non-invasive method for characterizing and diagnosing lithium-ion batteries (LIBs)1. The key to utilizing EIS lies in interpreting the measured impedance spectrum. This involves fitting the experimental data to an impedance model to understand the internal states of the battery. However, due to the multiscale and multiphysical nature of LIBs, impedance models can be complex and have many parameters. As a result, there is a high risk of over-fitting the experimental data, making the interpretation of the EIS data challenging2. In addition to electrical signals, the mechanical responses of a LIB, such as pressure and thickness change during charge/discharge, provides valuable information for characterization and diagnosis3-5. Most existing analyses of mechanical signals focus on the time domain. Recently, von Kessel et al6 introduced Mechanical Impedance Spectroscopy (MIS) as a frequency-analyzing tool for characterizing LIBs. The MIS spectrum (the displacement response subject to a cyclic pressure trigger) turned out to vary with the state of the batteries, demonstrating the great potential of using mechanical responses in the frequency domain to characterize and diagnosis the LIBs. Nevertheless, measuring displacement for LIBs in real-world applications is challenging, as it requires a customized testing machine to measure the micrometer-level displacement while exerting a sinusoidal pressure input. This requirement for customized testing equipment limits the application scope of the MIS method.A free LIB cell cyclic changes its dimensions during charge/discharge. Under confinements where dimension change constricted, cyclic pressure change will be generated, which could be used for frequency analysis. This observation led us to propose a new method called mechano-electro-chemical impedance spectroscopy (MeIS). An MeIS spectrum is defined as the ratio of pressure perturbation to the input current, denoted as . Measurements can be obtained by perturbating the battery with sinusoidal current and recording the resulting pressure or displacement response. The basic transfer function for MeIS is derived from the electro-chemo-mechanical coupling of the porous electrode. The MeIS consists of two parts, the MIS term and an electrochemical term resulting from the insertion/extraction deformation of the electroactive particles. The great advantage of MeIS is that it requires only a pressure or displacement sensor and a charger capable of providing sinusoidal current, making it potentially applicable in in-field scenarios such as management of EV batteries or real-time monitoring of a battery-based energy storage facility. Sensitivity analysis reveals that MeIS is highly sensitive to changes in the structure of porous electrodes, thus providing valuable insights into the internal structural integrity and degradation of LIBs. In addition, the experimental design and demonstrational results are also provided. We believe that MeIS could serve as a convenient and useful complement to EIS, enhancing the non-invasive diagnostic toolbox for LIBs.Reference: K. Mc Carthy, H. Gullapalli, K. M. Ryan, and T. Kennedy, Journal of The Electrochemical Society, 168 (8), (2021).F. Ciucci, Current Opinion in Electrochemistry, 13 132-139 (2019).J. Zhu, T. Wierzbicki, and W. Li, Journal of Power Sources, 378 153-168 (2018).B. Rieger, S. Schlueter, S. V. Erhard, J. Schmalz, G. Reinhart, and A. Jossen, Journal of Energy Storage, 6 213-221 (2016).Z. J. Schiffer, J. Cannarella, and C. B. Arnold, Journal of The Electrochemical Society, 163 (3), A427-A433 (2015).O. von Kessel, T. Deich, S. Hahn, F. Brauchle, D. Vrankovic, T. Soczka-Guth, and K. P. Birke, Journal of Power Sources, 508 (2021). Figure 1

Investigating Temperature-Dependent Dynamics of SEI Growth and Battery Degradation

Several studies have contributed to the current understanding of the temperature-dependent behavior of solid-electrolyte interphase (SEI) formation in lithium-ion batteries and its impact on battery capacity and lifespan. Liu et al. developed a thermal-electrochemical model that revealed the complex interplay between diffusivity, reaction kinetics, and temperature on SEI growth1. Leng et al. presented an electrochemistry-based electrical model to examine the temperature's effect on battery aging2. Alipour et al. reviewed temperature-dependent electrochemical properties3, while Lubhani Mishra et al. provided a detailed physics-based analysis of battery degradation and temperature inhomogeneities4. These studies collectively indicate higher temperatures accelerating and promoting growth of compact and less permeable SEI structures leading to an increase in capacity loss and cell resistance, and lower temperatures resulting in slow ionic transport through the SEI also causing higher ohmic loss. In the present work, we study SEI growth and resulting effect on battery capacity fade using continuum scale modeling under the assumption of constant battery cell temperature as well as considering actual dynamically changing temperature data from experiments. SEI growth under these two considerations is compared and the comparison is used in determining scenarios where considering dynamically varying temperature is crucial for accuracy. The detailed analysis of the internal states from the simulation results contributes to the understanding of the effect of the thermal dynamics on battery cell degradation due to SEI growth. To achieve these objectives, a physics-based model, specifically the Single Particle Model (SPM), is utilized. The model uses temporal temperature data obtained from past experimental studies as well as temperature dependent properties of SEI provided in the literature as inputs for this investigation. The ultimate aim of this study is to better understand how temperature influences SEI characteristics, thereby contributing to improved battery performance and longevity across diverse thermal environments. References Liu, L., Park, J., Lin, X., Sastry, A. M., & Lu, W. (2014). A thermal-electrochemical model that gives spatial-dependent growth of solid electrolyte interphase in a Li-ion battery. Journal of power sources, 268, 482-490.Leng, F., Tan, C. M., & Pecht, M. (2015). Effect of temperature on the aging rate of Li-ion battery operating above room temperature. Scientific reports, 5(1), 12967.Alipour, M., Ziebert, C., Conte, F. V., & Kizilel, R. (2020). A review on temperature-dependent electrochemical properties, aging, and performance of lithium-ion cells. Batteries, 6(3), 35.Mishra, L., Subramaniam, A., Jang, T., Garrick, T. R., & Subramanian, V. R. (2022, October). Model Development for Temperature-Dependent Degradation in Large Format Lithium-Ion Batteries. In Electrochemical Society Meeting s 242 (No. 28, pp. 1075-1075). The Electrochemical Society, Inc.

Impact of Pretension and Cycling Window on Degradation of Graphite/Silicon Composite Anodes

Challenges such as mechanical degradation and limited cycle life persist for high energy density lithium-ion batteries with silicon/graphite composite anodes. In this research work, the patterns of degradation of cells with silicon/graphite composite and NMC622 cathode are examined at varied cycling conditions and applied external pressure or pretension. The most notable outcome of this analysis is that cells cycled between 0 and 100 State-of-Charge (SoC) exhibit the most accelerated aging process. Increasing the pretension force effectively restrains the irreversible expansion of the cells, and has a positive effect on capacity retention.In this research, a comprehensive experiment was conducted involving 46 cells subjected to diverse cycling conditions, voltage windows, pretension forces, and temperatures. Reference performance tests (e.g. HPPC and 1/20 C-rate charge tests) are conducted regularly for analysis of degradation mechanisms. The capacity fade, resistance growth, and thickness increase are correspondingly shown in Figures 1, 2, and 3 with ampere hour throughput as the x-axis. The legend columns indicate test conditions, including C-rate, SoC window during cycling, temperature (in degrees Celsius), and pretension force (in psi). As is shown in all figures, there is a substantial dependence on the SoC window for cycling. To be specific, a rapid rate of capacity loss, resistance increase, and thickness increase occurs in the cell group cycled over the full SoC window (plotted in blue). Cells cycled under full SoC windows also exhibit an early accelerated fading (knee [1]) of capacity and accelerated increase (elbows [2]) of resistance and thickness. According to [3], this accelerated aging could be a consequence of side reactions and increased mechanical stress within the silicon particle when operating across a broad potential range.Meanwhile, for the cell group with restrained cycle windows (plotted in gray) the cells have not yet reached any knee, and have a relatively linear capacity loss. It should be noted that, within the range of partial cycling windows examined, cells subjected to a cycling range of 50-100 exhibit the most rapid degradation, which aligns with the conclusions presented in [4] due to the time at elevated potential. In Figure 2, the elevated temperature (depicted in red) exhibits a significant influence on the increase in resistance, potentially attributed to the growth of the solid electrolyte interface (SEI), but minimal impact on capacity loss. Maintaining other conditions constant and comparing cells under 25 psi and 15 psi (marked with hollow circles and filled circles, respectively), it is evident that a higher pretension force has a positive effect on cell capacity loss. Simultaneously, in Figure 3, the pretension force at 25 psi (marked with hollow circles) effectively restrains the irreversible expansion of the cells. The results are similar to the degradation pattern outlined in [5], it is observed that employing a high pretension force facilitates the mitigation of both degradation and expansion. As highlighted in [6], heightened temperatures lead to accelerated resistance growth. Nevertheless, the impact of various C-rates on degradation remains inconclusive [6].This research systematically analyzed cell-level degradation through an extensive array of experiments, providing valuable insights into the intricate dynamics of capacity fade, resistance increase, and thickness growth. The study's revelation that the cycle window exerts a pronounced impact on battery health could offer crucial guidance for the design of Battery Management Systems (BMS). Moreover, the work establishes a foundational basis for future research, particularly in exploring electrode-level degradation patterns. These contributions collectively enhance the understanding of energy storage systems, offering practical implications for optimizing battery performance and longevity in various applications.[1]Attia, Peter M., et al. "“Knees” in lithium-ion battery aging trajectories." Journal of The Electrochemical Society 169.6 (2022): 060517.[2] Strange, Calum, et al. "Elbows of internal resistance rise curves in Li-ion cells." Energies 14.4 (2021): 1206.[3] Verbrugge, Mark, et al. "Fabrication and characterization of lithium-silicon thick-film electrodes for high-energy-density batteries." Journal of The Electrochemical Society 164.2 (2016): A156.[4] Xu, Bolun, et al. "Modeling of lithium-ion battery degradation for cell life assessment." IEEE Transactions on Smart Grid 9.2 (2016): 1131-1140.[5] Mohtat, Peyman, et al. "Reversible and irreversible expansion of lithium-ion batteries under a wide range of stress factors." Journal of The Electrochemical Society 168.10 (2021): 100520.[6] Pannala, Sravan, et al. "An Experimental Correlation of Degradation with Cell Reversible and Irreversible Expansion Measurement in Pouch Cells." Electrochemical Society Meeting s 243. No. 2. The Electrochemical Society, Inc., 2023. Figure 1

Characterization of Processes Occurring at Various Interfaces By Scanning Electrochemical Microscopy (SECM)

Scanning electrochemical microscopy (SECM) is an in-situ probe technique that can directly monitor the electrochemical processes occurring at different interfaces. SECM has been proven as a powerful characterization tool with a wide variety of applications in redox processes, near-surface reactions, reaction kinetics, and electrochemical imaging. In this work, we focused on the use of SECM measurement methods to detect electrochemically active materials formed at the cathode electrolyte interface (CEI) and study the cathode degradation process of lithium-ion batteries (LIBs). We demonstrated the direct electron transfer between the cathode and the electrolyte, and the evolution of reactive species released during CEI formation by applying the SECM generation/collection mode. Our work highlights the application of SECM in characterizing cathode–electrolyte interphase of LIBs, providing a deeper fundamental understanding of LIB degradation mechanisms and new perspectives for future rational design of stable cathode-electrolyte interfaces for LIBs.

Degradation Processes in Current Commercialized Li-Ion Batteries and Strategies to Mitigate Them

Lithium-ion batteries (LIBs) are now widely exploited for multiple applications, from portable electronics to electric vehicles and storage of renewable energy. Along with improving battery performance, current research efforts are focused on diminishing the levelized cost of energy storage (LCOS), which has become increasingly important in light of the development of LIBs for large transport vehicles and power grid energy storage applications. Since LCOS depends on the battery's lifetime, understanding the mechanisms responsible for battery degradation and developing strategies to increase the lifetime of LIBs is very important. In this review, the latest developments related to the performance and degradation of the most common LIBs on the market are reviewed. The numerous processes underlying LIB degradation are described in terms of three degradation loss modes: loss of lithium inventory (LLI), active positive electrode material loss and degradation, and active negative electrode material loss and degradation. A strong emphasis is placed on the most recent strategies and tactics for LIB degradation mitigation.

Review of Lithium-Ion Battery Internal Changes Due to Mechanical Loading

The growth of electric vehicles (EVs) has prompted the need to enhance the technology of lithium-ion batteries (LIBs) in order to improve their response when subjected to external factors that can alter their performance, thereby affecting their safety and efficiency. Mechanical abuse has been considered one of the major sources of LIB failure due to the changes it provokes in the structural integrity of cells. Therefore, this article aims to review the main factors that aggravate the effects of mechanical loading based on the results of different laboratory tests that subjected LIBs to abusive testing. The results of different cell types tested under different mechanical loadings have been gathered in order to assess the changes in LIB properties and the main mechanisms responsible for their failure and permanent damage. The main consequences of mechanical abuse are the increase in LIB degradation and the formation of events such as internal short circuits (ISCs) and thermal runways (TRs). Then, a set of standards and regulations that evaluate the LIB under mechanical abuse conditions are also reviewed.

Correction: Tasnim Mowri et al. Assessing the Impact of First-Life Lithium-Ion Battery Degradation on Second-Life Performance. Energies 2024, 17, 501

Error in Table [...]

Unraveling the Degradation Mechanisms of Lithium-Ion Batteries

Lithium-Ion Batteries (LIBs) usually present several degradation processes, which include their complex Solid-Electrolyte Interphase (SEI) formation process, which can result in mechanical, thermal, and chemical failures. The SEI layer is a protective layer that forms on the anode surface. The SEI layer allows the movement of lithium ions while blocking electrons, which is necessary to prevent short circuits in the battery and ensure safe operation. However, the SEI formation mechanisms reduce battery capacity and power as they consume electrolyte species, resulting in irreversible material loss. Furthermore, it is important to understand the degradation reactions of the LIBs used in Electric Vehicles (EVs), aiming to establish the battery lifespan, predict and minimise material losses, and establish an adequate time for replacement. Moreover, LIBs applied in EVs suffer from two main categories of degradation, which are, specifically, calendar degradation and cycling degradation. There are several studies about battery degradation available in the literature, including different degradation phenomena, but the degradation mechanisms of large-format LIBs have rarely been investigated. Therefore, this review aims to present a systematic review of the existing literature about LIB degradation, providing insight into the complex parameters that affect battery degradation mechanisms. Furthermore, this review has investigated the influence of time, C-rate, depth of discharge, working voltage window, thermal and mechanical stresses, and side reactions in the degradation of LIBs.