Cryo-EM of Li Metal Battery Aging and Failure Mechanisms.
Abstract not provided.
Jungjohann, Katherine Leigh↗
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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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Cryogenic EM Imaging of Li Metal Battery Aging and Failure Mechanisms.
Abstract not provided.
Jungjohann, Katherine Leigh↗
4D insights into lithium-ion battery sidewall rupture during thermal runaway
Thermal runaway (TR), characterized by rapid exothermic reactions, presents a serious safety risk in lithium-ion batteries (LiBs). External triggers such as high temperatures, mechanical abuse, or internal short circuits (ISCs) can initiate TR, often resulting in sidewall rupture, which may escalate to catastrophic battery pack failure. In this study, we developed and applied high-speed synchrotron imaging techniques to investigate sidewall rupture mechanisms in LiBs subjected to different triggering scenarios. Using in situ 4D tomographic imaging, we visualized the dynamic evolution of sidewall rupture with high spatial and temporal resolution. The results revealed distinct failure behaviors linked to each trigger, underscoring the complex and condition-specific nature of sidewall breach and battery failure. These insights highlight the critical importance of implementing tailored safety strategies across diverse applications. Our findings demonstrate the powerful potential of synchrotron high-speed tomography as a diagnostic tool for advanced safety testing and cell qualification.
25 ENERGY STORAGE↗
Numerical and experimental analysis of mechanically induced failure in electric vehicle battery modules
Mitigating thermal runaway and cell-to-cell propagation is essential for improving the safety of electric and hybrid vehicles. Enhancing digital twin capabilities to predict battery mechanical abuse is particularly critical for automotive and aerospace applications, where crashworthiness is a key concern. Understanding failure conditions and propagation in battery modules during mechanical abuse is complex due to interactions between structural deformation, heat transfer, electrochemical processes, exothermic reactions and mechanical fracture. While prior studies have focused on modeling cell-level behavior, extending these models to module or pack level is necessary for a system level understating of electric vehicle safety. This study develops coupled large deformation finite element models that simultaneously solve for electrochemistry, material failure, internal short circuit and thermal runaway propagation. The models account for mechanical and thermal interactions between lithium-ion cells and other battery components while the contact interfaces are evolving with time. Model-predicted voltage, temperature and force responses are compared with experimental data for validation. The results demonstrate that the approach captures key failure mechanisms, including thermal propagation through heat transfer, electrical propagation from short circuits in parallel-connected cells, and mechanical propagation via penetration and crack formation. These findings show that computational models are valuable tools for understanding battery module failure and providing insight that can reduce the need for extensive experimental testing.
25 ENERGY STORAGE↗
Fundamental Investigations of Mechanical and Chemical Degradation Mechanisms in Lithium Ion Battery Materials (Final Technical Report)
The objective of our effort under the DOE EPSCoR Implementation grant is to establish a comprehensive and internationally recognized research program at Brown University and University of Rhode Island in understanding degradation mechanisms and to improve the cycle and calendar life of lithium ion battery (LIB) materials. A series of basic investigations are undertaken to characterize the mechanical and chemical degradation mechanisms, which can help enable new higher capacity and longer lasting electrode designs. Controlling mechanical and chemical degradation is the primary challenge in developing the next generation of higher energy density batteries. The development of failure resistant battery microstructures will require a fundamental understanding of the evolution of stress, deformation, damage, and electrochemistry in battery materials during cyclic charging and discharging. In addition, controlling the reactions at the electrode/electrolyte interface is critical for the formation of a stable SEI layer. We address these issues through a combination of controlled experiments on model battery materials and practical composite electrodes, together with multi-scale computations. Our effort is organized into three focus areas that encompass many critical challenges in Lithium Ion Battery Technologies: (i) Mechanical properties, fracture and damage in electrode materials; (ii) Chemistry and Mechanics of Solid Electrolyte Interphase (SEI); (iii) Mechanical and Chemical Integrity of Solid-Solid Interfaces in Practical Electrodes.
25 ENERGY STORAGE↗
The Effect of Artificial SEIs on Lithium Metal Anode Morphology and Conductivity
Lithium metal has often been termed the “holy grail” of battery technology, due to its high capacity (2,061 mAh/cm3) and low electrochemical potential (-3.04 V vs. SHE). However, lithium’s beneficially low potential also causes it to be highly reactive in the presence of organic solvents, making it difficult to harness the high energy capabilities for rechargeable batteries. Common failure of lithium metal batteries occurs by rapid dendrite growth leading to a hazardous short-circuit. Various methods have been brought forth to better understand the fundamental mechanisms of lithium metal batteries, as well as modifications made to better stabilize lithium metal. A common route of modification is done through interface engineering, with attempts to artificially provide a stable, homogeneous solid-electrolyte interface (SEI). The stability of the SEI has direct effects on the heterogeneity of the electrode surface, which initiates a waterfall effect of for progressive reactions such as dendrite growth, dead lithium accumulation, and electrolyte consumption. This work aims to produce a mixed LiI-LiF artificial SEI to improve ionic conductivity while retaining a high elastic modulus.
25 ENERGY STORAGE↗
Early Failure of Lithium–Sulfur Batteries at Practical Conditions: Crosstalk between Sulfur Cathode and Lithium Anode
Lithium–sulfur (Li–S) batteries are one of the most promising next-generation energy storage technologies due to their high theoretical energy and low cost. However, Li–S cells with practically high energy still suffer from a very limited cycle life with reasons which remain unclear. Here, through cell study under practical conditions, it is proved that an internal short circuit (ISC) is a root cause of early cell failure and is ascribed to the crosstalk between the S cathode and Li anode. The cathode topography affects S reactions through influencing the local resistance and electrolyte distribution, particularly under lean electrolyte conditions. The inhomogeneous reactions of S cathodes are easily mirrored by the Li anodes, resulting in exaggerated localized Li plating/stripping, Li filament formation, and eventually cell ISC. Manipulating cathode topography is proven effective to extend the cell cycle life under practical conditions. The findings of this work shed new light on the electrode design for extending cycle life of high-energy Li–S cells, which are also applicable for other rechargeable Li or metal batteries.
25 ENERGY STORAGE↗
Modeling strategy for progressive failure prediction in lithium-ion batteries under mechanical abuse
The prediction for the internal failure of lithium-ion batteries (LIBs) under external mechanical abuse loading remains a challenge for safe design. This paper systematically studies the modeling approach for progressive failure simulation and short-circuit prediction. Hemispherical indentation experiments are conducted on a battery specimen containing 5 representative sandwich (RS) layers to examine the deformation and progressive failure behavior of battery components. Three different models, viz, a high-fidelity detailed model, an intermediate homogenized model and a fully homogenized model, are developed and employed to simulate the progressive failure in a multi-layer battery specimen. The simulation results obtained using the three models all correlate well with experimental phenomena, capturing the overall stress-strain response and ultimate failure of the battery structure. The numerical results can help us understand the failure behavior and the mechanism for mechanical abuse-induced short circuit in LIBs. The feasibility of the three models for use in progressive failure prediction is compared by analyzing the capability of the models in predicting the critical failure events, the computational efficiency of the models, and the feasibility to implement coupled mechanical-electrochemical-thermal simulations. The results of this work provide useful insights on practical choices for the modeling strategy and safety design of LIBs under mechanical abuse conditions.
25 ENERGY STORAGE↗
Methods and systems for diagnosis of failure mechanisms and for prediction of lifetime of metal batteries
Methods for diagnosing failure mechanisms and for predicting lifetime of metal batteries include monitoring rest voltage and Coulombic Efficiency over relatively few cycles to provide profiles that indicate, by the trends thereof, a particular failure mechanism (e.g., electrolyte depletion, loss of metal inventory, increased cell impedance). The methods also include cycling over relatively few cycles an anode-free cell, having the same cathode and electrolyte as the metal battery, but with a current collector instead of the anode. Discharge capacity is monitored and profiled, and a discharge capacity curve is fitted to the discharge capacity profile to discern a capacity retention per cycle. The lifetime of the metal battery is determined using the capacity retention per cycle discerned from the anode-free cell. Related systems include a metal-based battery and an anode-free cell or a battery cell reconfigurable between a metal-based and an anode-free cell.
Li, Bin↗
Deconvoluting sources of failure in lithium metal batteries containing NMC and PEO-based electrolytes
Solid-state lithium metal batteries (SSLMBs) containing polyethylene oxide (PEO)-derived polymer electrolytes and high-voltage (> 4 V vs. Li/Li + ) cathode materials suffer from three sources of failure: (1) instability between the polymer electrolyte and cathode at high voltage, (2) instability of the polymer electrolyte with Li metal, and (3) poorly-designed cathodes. In this study, these three sources of failure are deconvoluted by studying Ni-rich LiNi x Mn y Co 1-x-y O 2 (NMC, x ≥ 0.6) cathodes and a gel polymer electrolyte (GPE) derived from PEO. Initial cycling data reveals that rapid capacity fade occurs regardless of whether soft short circuits form due to Li dendrites. Cyclic voltammetry scans on cells featuring a Li metal electrode, GPE, and a NMC811 electrode free of additives suggest that there are no runaway reactions between the GPE and NMC811 up to 4.5 V vs. Li/Li + . Cathode/cathode symmetric cell cycling demonstrates that Li metal reactivity is a prime source of failure, though a poorly-designed cathode leads to subpar performance. A cathode with single-crystal NMC particles was demonstrated to achieve better initial capacity and longer cycle life, indicating room for improvement in SSLMB cathode design. Therefore, the sources of failure as enumerated may be ranked as follows from most to least concerning: 2 > 3 > 1.
25 ENERGY STORAGE↗
Spatiotemporal mapping of microscopic strains and defects to reveal Li-dendrite-induced failure in all-solid-state batteries
Solid-state electrolytes (SSEs) are key to the success and reliability of all-solid-state lithium batteries, potentially enabling improvements in terms of safety and energy density over state-of-the-art lithium-ion batteries. However, there are several critical challenges to their implementation, including the interfacial instability stemming from the dynamic interaction of as-formed dendritic lithium during cycling. Here, we emphasize the importance of studying the spatial distribution and temporal evolution of strains and defects in crystalline solid-state electrolytes at the micro-scale, and how this affects dendrite growth. A proof-of-principle study is demonstrated using the synchrotron radiation based micro Laue X-ray diffraction method, and a custom-developed in-situ cycling device. Defects and residual strains are mapped, and the evolution of intragranular misorientation is observed. The feasibility of using this technique is discussed, and recommendations for micro-strain engineering to address the Li/SSEs interfacial issues are given. Additionally, work directions are pointed out with the consideration of combining multi-techniques for “poly-therapy”.
36 MATERIALS SCIENCE↗
Bayesian learning for rapid prediction of lithium-ion battery-cycling protocols
Advancing lithium-ion battery technology requires the optimization of cycling protocols. A new data-driven methodology is demonstrated for rapid, accurate prediction of the cycle life obtained by new cycling protocols using a single test lasting only 3 cycles, enabling rapid exploration of cycling protocol design spaces with orders of magnitude reduction in testing time. We achieve this by combining lifetime early prediction with a hierarchical Bayesian model (HBM) to rapidly predict performance distributions without the need for extensive repetitive testing. The methodology is applied to a comprehensive dataset of lithium-iron-phosphate/graphite comprising 29 different fast-charging protocols. HBM alone provides high protocol-lifetime prediction performance, with 6.5% of overall test average percent error, after cycling only one battery to failure. Here, by combining HBM with a battery lifetime prediction model, we achieve a test error of 8.8% using a single 3-cycle test. In addition, the generalizability of the HBM approach is demonstrated for lithium-manganese-cobalt-oxide/graphite cells.
25 ENERGY STORAGE↗
Dispersion of stored energy within a battery system at risk of failure
A method and system for dispersing stored energy in an energy storage system to delay or arrest propagation of thermal runaway and thermally-induced cascading failures. The system includes a plurality of battery sub-assemblies and DC-DC converters connected to a shared DC bus through which energy may be exchanged. The system may be interfaced to an AC power grid or DC power system through an additional power converter. The method of dispersing stored energy uses this system to charge and discharge sub-assemblies such that the system is less susceptible to propagation of thermal runaway. The method determines, based on awareness of current system state, battery types, and electrical and thermal structure, the sequence of charging and discharging actions to best inhibit thermal runaway while preserving the system's ability to perform subsequent energy redistribution.
Mueller, Jacob↗
Avoiding thermal runaway in lithium-ion batteries using ultrasound detection of early failure mechanisms
Thermal runaway leading to catastrophic failure has slowed the adoption of lithium-ion batteries, highlighting the need for early warning systems. In this work, ultrasound is used to detect physical changes in 0.950 Ah Li-ion battery cells by inducing conditions associated with thermal runaway. Ultrasound signal features are extracted as the batteries are cycled under baseline conditions and subsequently subjected to constant current and voltage overcharges. Two conditions identifying failure are defined: a warning to detect the start of overcharge and an emergency stop (E-stop), to immediately take the battery out of service. Using changes in ultrasound signal features, consistent warning and stopping classifications are applied to all failure experiments. On average, a warning notification was issued after 15% of the overcharge time and an E-stop was triggered after 35% of total overcharge duration before failure. Further testing suggests that it is possible to avoid thermal runaway by reacting to intermediate, warning notifications prior to an immediate E-stop. In other words, not only can detection derived by ultrasound identify battery failure before a catastrophic event, but can also provide early, actionable warnings so that overcharges can be detected and corrected quickly enough so the battery does not need to be decommissioned.
25 ENERGY STORAGE↗
Dynamics of Intra-Cell Thermal Front Propagation in Lithium-Ion Battery Safety Issues
Thermal runaway (TR), a critical failure mode in lithium-ion batteries (LIBs), poses significant safety risks and hinders wider application of LIBs. TR typically begins at a localized heat source and spreads across the cell. Understanding thermal front propagation (TFP) characteristics, such as front and velocity, is crucial for assessing energy release and temperature distribution for battery hazardous estimation. Recent studies assume that TR within cells propagates at a near-constant velocity, based on the reaction kinetics and thermal properties. Here, in this study, an intra-battery TR model is further proposed and it indicates that TFP velocity stabilizes when the front is distanced from the heat source. Theoretical estimates for propagation velocity and front are developed and validated through numerical simulations and experimental tests from the NREL Battery Failure Databank. The energy release rate during TFP and the impact of preheating based on a point heat source are explored. This work clarifies the long-standing clouds of the thermal font propagation behaviors within the single cell, highlights the power and beauty of mathematics modeling to describe the complicated thermal behaviors, and provides important guidelines for thermal hazardous understanding for next-generation batteries.
25 ENERGY STORAGE↗
Non-destructive electrochemical diagnosis of failure mechanisms in aqueous zinc batteries
The early detection of secondary reactions that affect the life and performance of zinc manganese oxide batteries requires a shift from conventional time-consuming and often destructive procedures to rapid lifetime-predictive techniques. In this work, an electrochemical approach is employed to elucidate independent signatures for four common types of failure mechanisms in zinc manganese dioxide (Zn||MnO2) batteries—namely, the loss of zinc inventory, the loss of active material at the cathode, electrolyte depletion, and increased cell impedance. Our findings, specific to coin cell configurations, reveal that each induced failure mechanism can be distinctively modeled and identified based on responses from the rest voltage and columbic-efficiency data for prompt detection. For instance, electrolyte depletion response manifests a distinctive abrupt (>80 %) decrease in columbic efficiency (CE) and charge-rest voltage (Vc) while the discharge-rest voltage remained constant at ~1.3 V. Furthermore, electrolyte rejuvenation of the cell increased the CE to >95 % and restored Vc from ~0.3 to >1.7 V. Recovery experiments and reference performance tests demonstrated consistency between electrochemical descriptors and their associated failure mechanisms. Further, the outcomes of this work provide valuable insights and data models for some of the dominant failure mechanisms present in zinc manganese battery chemistries, which are beneficial to accelerated early-lifetime diagnosis and advancement of Zn batteries development.
25 ENERGY STORAGE↗
Techno-Economic Impact of Partial String Failurein Multi-string Energy Storage Systems
Electric utilities and large industrial/commercial customers, which integrate multi-MW multi-string energy storage systems (ESS), are typically at a significant risk of string failure. This results in loss of system performance and capacity. In order to evaluate the accurate costs and benefits associated with a particular battery system, it is essential to incorporate the costs associated with battery string failure and, as a result, reduced capacity. This report analyzes how the economic losses can be estimated based on market rules and ESS availability. A framework for calculation of economic losses is developed and implemented with an illustrative string failure case for Independent System Operator (ISO-NE) forward capacity market. Further scenarios and case studies are analyzed by varying the probability of string failure as well as the capacity bid into the market. These scenarios are used to assess the variability of economic losses and the impact of string failure on final realized benefits from the battery's market participation.
Fotedar, Vanshika↗
Development of 3D Printing Techniques for Solid-State Lithium Batteries: Energy Storage Internship (Final Report)
The goal of this internship was to develop a solid polymer electrolyte with a suitable ionic conductivity and mechanical properties and integrate it with 3D printed cathode for solid state lithium batteries. While liquid electrolytes will have much higher conductivities and therefore higher power densities than solid electrolytes, batteries with such electrolytes suffer from extreme dendritic growth, short-circuiting, and general failure. Typically, batteries prevent this by including a solid yet porous separator somewhere between the anode and cathode to suppress dendritic growth. Solid polymer electrolyte acts as the conductive medium between electrodes as well as the separator that prevents failure from short-circuiting. The specific system explored is a vinyl ethylene carbonate (VEC) and polyethylene glycol diacrylate (PEGDA) mixed polymer solution using both 2,2’-azobis(2-methylpropionitrile) (AIBN) and Irgacure 819, respectively as thermal and photo- initiators. Electrochemical and rheological techniques were used to determine the optimal polymer solution and curing conditions. Through this research, multiple new pathways of exploration have been determined to create a usable solid polymer electrolyte through a combination of varying cure intensities and initiator concentrations.
25 ENERGY STORAGE↗