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At least 145 records · Page 8

Advanced diagnostics to evaluate heterogeneity in lithium-ion battery modules

Battery packs for electric and stationary applications experience varied operating conditions, including abuse—e.g., fast charging, overcharging, thermal, vibration, shock, etc.—throughout their lifetimes. Innovative diagnostic tools and algorithms that go beyond single cells and deal with modules and packs are essential for early detection of off-normal issues. High-resolution tools with known detection limits are key to developing appropriate mitigation strategies. With the advent of rapid impedance spectroscopy that can generate a broadband impedance spectrum in ~10 sec, the case for impedance-based diagnostics that can be readily aligned with other methods, such as incremental capacity or dQ.dV -1 , has become promising. This study used the aforementioned diagnostic methods to identify realistic in-vehicle battery abnormalities (e.g., localized self-discharge and non-uniform aging), in series (up to 10S) and parallel (4P) strings, using 16 Ah graphite/NMC cells. The impedance-based diagnostic is found to be sensitive to the string size and state. Depending on the type of abnormality, detection frequency varied. The dQ.dV -1 method showed the potential to detect long-term aging-related heterogeneity in modules. In general, both the impedance and dQ.dV -1 methods were able to detect series strings’ abnormalities, but struggled to find those issues within parallel modules.

25 ENERGY STORAGE↗

Multiscale Understanding of Surface Structural Effects on High-Temperature Operational Resiliency of Layered Oxide Cathodes

The worldwide energy demand in electric vehicles and the increasing global temperature have called for development of high-energy and long-life lithium-ion batteries (LIBs) with improved high temperature operational resiliency. However, current attention has been mostly focused on cycling aging at elevated temperature, leaving considerable gaps of knowledge in the failure mechanism and practical control of abusive calendar aging and thermal runaway that are highly related to the eventual operational lifetime and safety performance of LIBs. Herein, using a combination of various in situ synchrotron X-ray and electron microscopy techniques, we report a multiscale understanding of surface structure effects involved in regulating the high temperature operational tolerance of polycrystalline Ni-rich layered cathodes. Our results collectively show that an ultraconformal poly (3,4-ethylenedioxythiophene) coating can effectively prevent LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode from undesired phase transformation and transition metal dissolution on the surface, atomic displacement and dislocations within primary particles, intergranular cracking along the grain boundaries within secondary particles, and intensive bulk oxygen release during high state-of-charge and high temperature aging. As a result, the present work highlights the essential role of surface structure controls in overcoming the multiscale degradation pathways of high-energy battery materials at extreme temperature.

25 ENERGY STORAGE↗

Thermal management challenges in lithium-ion batteries: understanding heat generation mechanisms

This paper investigates heat generation in commercial 18 650 lithium-ion battery cells and the thermal management challenges from their high energy density and electrochemical processes. Thermal effects can degrade performance, accelerate aging, and increase thermal runaway risk. Using isothermal calorimetry and EIS, the study emphasizes optimizing thermal behavior to improve battery efficiency, safety, and durability.

25 ENERGY STORAGE↗

Bridging Additive Manufacturing and Electronics Printing in the Age of AI

Printing techniques have been instrumental in developing flexible and stretchable electronics, including organic light-emitting diode displays, organic thin film transistor arrays, electronic skins, organic electrochemical transistors for biosensors and neuromorphic computing, as well as flexible solar cells with low-cost processes such as inkjet printing, ultrasonic nozzle, roll-to-roll coating. The rise of additive manufacturing provides even more opportunities to print electronics in automated and customizable ways. In this work, we will review the current technologies of printing electronics (including printed batteries, supercapacitors, fuel cells, and sensors), especially with 3D printing. In this age of ongoing AI revolution, the application of AI algorithms is discussed in terms of combining them with 3D printing and electronics printing for a future with automated optimization, sustainable design, and customizable and scalable manufacturing.

Chemistry↗

Endpoint Slippage Analysis in the Presence of Impedance Rise and Loss of Active Material

Endpoint slippage analysis can be used to quantify the reduction and oxidation side-reactions occurring in rechargeable batteries. Application of this technique often disregards the interference of additional aging modes, such as impedance rise and loss of active material (LAM). Here, we show that these modes can themselves induce slippage of endpoints, making the direct determination of parasitic reactions more difficult. We provide equations that describe the slippages caused by LAM and impedance rise. We show that these equations can, in principle, account for the contribution of these additional modes to endpoint slippage, enabling “correction” of testing data to quantify the side-reactions of interest. However, the challenge with this approach is that it requires information about the average Li+ content of disconnected active material domains, which is, in many cases, unknowable. The present work explores mathematical connections between measurable quantities (such as capacity fade and endpoint slippages) and the extent of LAM or impedance rise endured by the cell, and discuss how the tracking of endpoints can better serve battery diagnostics.

Rodrigues, Marco-Tulio F. [Argonne National Labora↗

Characterization of Cycle-Aged Commercial NMC and NCA Lithium-ion Cells: I. Temperature-Dependent Degradation

Lithium-ion batteries are widely used in applications from consumer electronic devices to stationary energy storage. Appropriate management of batteries is challenging due to limited data on their performance and materials degradation. Previous studies have focused on characterization of single cells under specific operating conditions. In the present work, commercial 18650 lithium-ion cells with LiNi x Mn y Co 1-x-y O 2 (NMC) and LiNi x Co y Al 1-x-y O 2 (NCA) positive electrodes were characterized by a wide range of electrochemical and materials techniques after cycling at 15, 25, or 35 °C to ∼80% capacity. The NCA cells exhibit weak temperature dependence in their cycle aging and materials degradation. The NMC cells exhibited increased capacity fade and materials degradation as ambient temperature decreased. All cells exhibited loss of lithium inventory as their primary degradation mode. However, the NCA cells only showed evidence of solid electrolyte interphase (SEI) growth whereas the NMC cells showed signs of Li plating at 15 °C, transitioning to SEI growth at 35 °C. The NMC cells displayed signs of loss of active material at the positive electrode at lower temperatures, suggesting that Li plating is correlated to additional processes that increase the rate of degradation. These results highlight the importance of avoiding broad generalizations about Li-ion battery temperature dependence.

25 ENERGY STORAGE↗

Field-Aging Test Bed for Behind-the-Meter PV + Energy Storage

Small DC-coupled battery test systems are deployed at the National Renewable Energy Laboratory to evaluate capacity fade models and report on performance parameters such as round-trip efficiency under indoor and outdoor deployment scenarios. Initial commercial battery products include LG Chem RESU lithium-ion (Li-ion) and Avalon vanadium redox flow batteries. Adapting indoor lab-scale test methods to outdoor systems has challenges, including maintaining constant temperature and fully controlling batteries through standard discharge curves. Initial measurements show the Li-ion battery systems performing within expectations, near 85% round-trip efficiency. Initial lifetime modeling and measurements indicate that battery capacity could degrade by 20%-35% over 10 years at current rates.

14 SOLAR ENERGY↗

Lithium-Ion Battery Life Model with Electrode Cracking and Early-Life Break-in Processes

This paper develops a physically justified reduced-order capacity fade model from accelerated calendar- and cycle-aging data for 32 lithium-ion (Li-ion) graphite/nickel-manganese-cobalt (NMC) cells. The large data set reveals temperature-, charge C-rate-, depth-of-discharge-, and state of charge (SOC)-dependent degradation patterns that would be unobserved in a smaller test matrix. Model structure is informed by incremental capacity analysis that shows loss of lithium inventory and cathode-material loss as the dominant capacity fade mechanisms. The model includes terms attributable to solid-electrolyte interface (SEI) growth, electrode cracking, cycling-driven acceleration of SEI growth, and "break-in" mechanisms that slightly decrease or increase available Li inventory early in life. The study explores what mathematical couplings of these mechanisms best describe calendar aging, cycle aging, and mixed calendar/cycle aging. Various approaches are discussed for extracting relevant stress factors from complex cycling profiles to predict lifetime during real-world battery loads using models trained on constant-current laboratory test results. The complexity of the present human-driven model identification process motivates future work in machine learning to more widely search and statistically discern the optimal model that correctly extrapolates capacity fade based on physical knowledge.

25 ENERGY STORAGE↗

The influence of temperature on area-specific impedance and capacity of Li-ion cells with nickel-containing positive electrodes

The temperature-dependent behaviors of five nickel-containing positive electrodes (NCA, NMC811, NMC622, NMC532, and NMC111) in lithium-ion batteries are investigated using an electrochemical protocol involving rate studies, mild aging (~100 cycles), and hybrid pulse power characterization (HPPC). Tests are conducted using coin-cells with graphite negative electrodes at -20 °C, 0 °C, 20 °C, and 40 °C. Three techniques are compared for determining the area-specific impedance (ASI): i) fits to the rate study average voltages, ii) fitting to the entire voltage curves using a regularization scheme, and iii) HPPC. When fit to an Arrhenius-type equation, all methods yield similar apparent activation energies (±2 kJ/mol) for the impedance, which range from -20 to -31 kJ/mol for the electrodes. Impedance growth increases with temperature but remains at less than 0.2% per cycle for most electrodes and temperatures. NCA and NMC811 are the exceptions, which yield 0.5% and 1.5% increases in ASI per cycle, respectively, at 40 °C. For cells with the same electrodes, the capacities are similar at 20 and 40 °C but reduce at lower temperatures, with up to a 52% reduction at -20 °C and 2C. The fade in energy of the cells during C/3 cycling is attributed to decreasing capacity as opposed to increasing ASI.

25 ENERGY STORAGE↗

Forecasting battery capacity and power degradation with multi-task learning

Lithium-ion batteries degrade due to usage and exposure to environmental conditions, which affects their capability to store energy and supply power. Accurately predicting the capacity and power fade of lithium-ion battery cells is challenging due to intrinsic manufacturing variances and coupled nonlinear ageing mechanisms. In this paper, we propose a data-driven prognostics framework to predict both capacity and power fade simultaneously with multi-task learning. The model is able to predict the degradation trajectory of both capacity and internal resistance together with knee-points and end-of-life points accurately at early-life stage. The validation shows an average percentage error of 2.37% and 1.24% for the prediction of capacity fade and resistance rise, respectively. The model's ability to accurately predict the degradation, facing capacity and resistance estimation errors, further demonstrates the model's robustness and generalizability. Compared with single-task learning models for forecasting capacity and power degradation, the model shows a significant prediction accuracy improvement and computational cost reduction. This work presents the highlights of multi-task learning in the degradation prognostics for lithium-ion batteries.

25 ENERGY STORAGE↗

Predicting Si-Anode Calendar Life Using Machine Learning: Correlating Electrolyte Properties and Electrochemical Signals

This study evaluates novel electrolytes tailored for Si-containing anodes to promote calendar-life. Drawing inspiration from advancements in electrolytes for Li-metal cells, the work investigates correlations between predicted electrolyte properties and measured electrochemical performance using several machine-learning models. By leveraging machine learning and advanced modeling techniques, this study aims to establish predictive frameworks that accelerate calendar-aging experiments and inform rational electrolyte design for Si-containing cells. In the present study, fifteen different electrolytes are evaluated in a Si-containing cell using an accelerated calendar-life protocol. For each electrolyte considered, 87 properties (features) from the Advanced Electrolyte Model were produced to identify key property/performance relationships. In this study, the best performing electrolytes were generally those formulations that included non-coordinating fluoroether solvents, and the most predictive features for long-term calendar-life were features related to salt concentration and electrolyte viscosity as well as early capacity, ionic conductivity, and Coulombic efficiency measurements. The framework developed in this study correlating electrolyte properties to measured electrochemical performance is expected to accelerate electrolyte design for Si-containing anodes and ultimately enable high-energy-density, long-life Li-ion batteries.

25 - ENERGY STORAGE↗

Magnetohydrodynamic Control of Interfacial Degradation in Lithium-Ion Batteries for Fast Charging Applications

Interfacial anodic degradation in graphitic materials under fast charging conditions causes severe performance loss and safety hazard in lithium ion batteries. We present a novel method for minimizing the growth of these aging mechanism by application of an external magnetic field. Under magnetic field, paramagnetic lithium ions experience a magnetohydrodynamic force, which rotates the perpendicularly diffusing species and homogenizes the ionic transport. This phenomenon minimizes the overpotential hotspots at the anode/separator interface, consequently reducing SEI growth, lithium plating, and interfacial fracture. In situ electrochemical measurements indicate an improvement in capacity for lithium cobalt oxide/graphite pouch cell (20 mAh) charged from 1–5 C under an applied field of 1.8 kG, with a maximum capacity gain of 22% at 5C. Post-mortem FE-SEM and EDS mapping shows that samples charged with magnetic field have a reduced lithium deposition at 3C and a complete suppression of interfacial fracture at 5C. At 5C, a 24% reduction in the lithium content is observed by performing XPS on the anodic interfacial film. Finally, fast charging performance under variable magnetic field strengths indicate a saturation behavior in capacity at high fields (>2 kG), thereby limiting the field and consequent energy requirements to obtain maximum capacity gain under extreme conditions.

electromagnetism↗

Understanding the Nature of Capacity Decay and Interface Properties in Li//LiNi 0.5 Mn 1.5 O 4 Cells by Cycling Aging and Titration Techniques

The spinel structure LiNi 0.5 Mn 1.5 O 4 (LNMO) is a propitious cathode material for next-generation lithium-ion batteries for fast charge–discharge applications, but its capacity decay mechanism and rate-limiting process are not yet well understood. In this work, electrochemical impedance spectroscopy (EIS) with galvanostatic intermittent titration (GITT) and cycling aging techniques were employed to investigate the nature of capacity decay in disordered-phase LNMO. Different resistive components were separated after every 10 cycles. Cell overvoltages (ΔVs) due to ohmic conduction, charge transfer (CT), and concentration polarization (CP) were individually determined. Results revealed that the cell exhibited a higher ΔV at a higher discharged state. However, the ΔV value for CP was higher at a higher state of charge (SOC), and the overall LNMO/electrolyte interface played a major role in the rate-determining step. Battery life was estimated based on the results. Battery calendar life was found to be more vulnerable than cycle life. Furthermore, results also indicated that the working SOC range could be optimized based on the resistance analysis by avoiding those SOCs that have the most detrimental impact (e.g., heat generation and fire hazard).

25 ENERGY STORAGE↗

Solar and battery can reduce energy costs and provide affordable outage backup for US households

Distributed energy resources are promising solutions for household energy affordability and resilience as weather extremes and aging infrastructure intensify grid reliability risks. This study presents a comprehensive nationwide assessment of over 500,000 U.S. households, evaluating economic and backup viability of solar-battery systems. We find that 60% of households could reduce electricity costs with average savings of 15%, while 63% of households could achieve affordable backup power during power outages covering an average of 51% of their essential energy needs. However, these benefits show limited alignment with areas of greatest need, particularly in regions facing high outage risks. We also identify significant disparities in access to solar and battery, with less-populated and disadvantaged communities showing consistently lower viability. Furthermore, these findings demonstrate the need for targeted policy interventions to ensure equitable access to solar-battery benefits, especially as states transition from net energy metering to other electricity tariff policies.

14 SOLAR ENERGY↗

Isolation and conversion of electrolyte components into a value-added product

The overall objective of this work was to develop a process for effectively (i) recycling the electrolyte components from the end-of-life batteries and reduce the environmental hazard, (ii) understand the fundamental differences between pristine and recycled electrolyte components, (iii) electrochemically and analytically evaluate the recycled electrolyte components and (iv) establish deviations from the pristine electrolyte, and effectively separation of value-added product. We focused on determining scaling up the electrolyte recovery process by distillation of end-of-life batteries to get yield enough to use it for electrolyte formulation of reuse in the battery cell. The used cells from the ORNL battery manufacture facility (BMF)as well as received from the industry partner, Austin Elements Inc., was scaled to 10 used multilayered pouch cells in each batch of distillation and systematically separated and identified the electrolyte components of the used cells with FTIR and NMR studies. We were able to recovery 10g of solvent mass from the used pouch cells. NMR spectroscopy showed that the solvent was pure EMC,DMC and the sample was used to make a new battery cell. The end-of-life battery, it was noted that some cells were visually drier than the other cells and were more advanced in aged. In that case, even though the same distillation conditions were utilized, no usable mass of electrolyte solvent was recovered. It is expected that most of the solvent was decomposed during the battery charge-discharge cycling. The solid salt residue was separated by chemical and water treatment processes. Components of resulting solid product was analyzed by XRD and XPS measurements. The solid products are very much related to the salts used in the electrolyte solution.

25 ENERGY STORAGE↗

Isolation and Conversion of Electrolyte Components into a Value-Added Product

The overall objective of this work was to develop a process for effectively (i) recycling the electrolyte components from the end-of-life batteries and reduce the environmental hazard, (ii) understand the fundamental differences between pristine and recycled electrolyte components, (iii) electrochemically and analytically evaluate the recycled electrolyte components and (iv) establish deviations from the pristine electrolyte, and effectively separation of value-added product. We focused on determining scaling up the electrolyte recovery process by distillation of end-of-life batteries to get yield enough to use it for electrolyte formulation of reuse in the battery cell. The used cells from the ORNL battery manufacture facility (BMF) as well as received from the industry partner, Austin Elements Inc., was scaled to 10 used multilayered pouch cells in each batch of distillation and systematically separated and identified the electrolyte components of the used cells with FTIR and NMR studies. We were able to recovery 10g of solvent mass from the used pouch cells. NMR spectroscopy showed that the solvent was pure EMC, DMC and the sample was used to make a new battery cell. The end-of-life battery, it was noted that some cells were visually drier than the other cells and were more advanced in aged. In that case, even though the same distillation conditions were utilized, no usable mass of electrolyte solvent was recovered. It is expected that most of the solvent was decomposed during the battery charge-discharge cycling. The solid salt residue was separated by chemical and water treatment processes. Components of resulting solid product was analyzed by XRD and XPS measurements. The solid products are very much related to the salts used in the electrolyte solution.

25 ENERGY STORAGE↗

Origin of Phase Separation in Ni-Rich Layered Oxide Cathode Materials During Electrochemical Cycling

In intercalation materials, the kinetics and uniformity of mass transport across the nanocrystalline domains dictate the structural reversibility and transport capability at the macroscopic level. (De)intercalation-induced interlayer disintegrations exhibit anisotropic crystallite size change. Due to the anisotropic mass transport mechanism, separated phases are inherently crystallographically oriented. One such material is LiNi $1–x–y$ Mn $x$ Co $y$ O 2 , which plays a pivotal role in advanced Li-ion batteries but suffers from severe phase inhomogeneities under fast charge or electrochemical aging. Here, using operando synchrotron techniques, we probe the mechanistic origins of the compositional and orientational-dependent phase separations during the electrochemical cycling of LiNi 0.8 Mn 0.1 Co 0.1 O 2 by comprehensive analysis of both in-plane and out-of-plane reflections. In the H2/H3 phase regime, in-plane domain propagation occurs due to increased covalency despite the severe decay of interlayer crystallographic order, resulting in the change of crystalline domain shape from 3D spheres to two-dimensional nanosheets. The crystallographically selective XRD line splitting is linked to the geometry of the facets as mass transfers along the ab plane. In conclusion, this work provides mechanistic insights into crystallographic orientation-dependent phase inhomogeneity under fast charge and extended cycling.

36 MATERIALS SCIENCE↗