Batteries — Open Access Journal

The economic value of high-capacity battery systems, being used in a wide variety of automotive and energy storage applications, is strongly affected by the duration of their service lifetime. Because many battery systems now feature a very large number of individual cells, it is necessary to understand how cell-to-cell interactions can affect durability, and how to best replace poorly performing cells to extend the lifetime of the entire battery pack. This paper first examines the baseline results of aging individual cells, then aging of cells in a representative 3S3P battery pack, and compares them to the results of repaired packs. The baseline results indicate nearly the same rate of capacity fade for single cells and those aged in a pack; however, the capacity variation due to a few degrees changes in room temperature (≃±3 ${}^{\circ }$ C) is significant (≃±1.5% of capacity of new cell) compared to the percent change of capacity over the battery life cycle in primary applications (≃20–30%). The cell replacement strategies investigation considers two scenarios: early life failure, where one cell in a pack fails prematurely, and building a pack from used cells for less demanding applications. Early life failure replacement found that, despite mismatches in impedance and capacity, a new cell can perform adequately within a pack of moderately aged cells. The second scenario for reuse of lithium ion battery packs examines the problem of assembling a pack for less-demanding applications from a set of aged cells, which exhibit more variation in capacity and impedance than their new counterparts. The cells used in the aging comparison part of the study were deeply discharged, recovered, assembled in a new pack, and cycled. We discuss the criteria for selecting the aged cells for building a secondary pack and compare the performance and coulombic efficiency of the secondary pack to the pack built from new cells and the repaired pack. The pack that employed aged cells performed well, but its efficiency was reduced. Full article

Common issues aqueous-based vanadium redox flow batteries (VRFBs) face include low cell voltage due to water electrolysis side reactions and highly corrosive and environmentally unfriendly electrolytes (3 to 5 M sulfuric acid). Therefore, this investigation looks into the comparison of a highly conductive ionic liquid with a well-studied deep eutectic solvent (DES) as electrolytes for non-aqueous VRFBs. The latter solvent gives 50% higher efficiency and capacity utilization than the former. These figures of merit increase by 10% when nitrogen-doped graphene (N-G)-modified carbon papers, via a one-step binder-free electrophoretic deposition process, are used as electrodes. X-ray computed tomography confirms the enhancement of electrochemical surface area of the carbon electrodes due to N-G while electrochemical impedance spectra show the effect of its higher conductivity on improving RFB performance. Finally, potential strategies for the scaling-up of DES-based VRFBs using a simple economical model are also briefly discussed. From this study, it is deduced that more investigations on applying DESs as non-aqueous electrolytes to replace the commonly used acetonitrile may be a positive step forward because DESs are not only cheaper but also safer to handle, far less toxic, non-flammable, and less volatile than acetonitrile. Full article

This paper introduces a physical–chemical model that governs the lithium ion (Li-ion) battery performance. It starts from the model of battery life and moves forward with simplifications based on the single-particle model (SPM), until arriving at a more simplified and computationally fast model. On the other hand, the implementation of this model is developed through MATLAB. The goal is to characterize an Li-ion cell and obtain its charging and discharging curves with different current rates and different cycle depths, as well as its transitory response. In addition, the results provided are represented and compared, and different methods of estimating the state of the batteries are applied. They include the dynamics of the electrolyte and the effects of aging caused by a high number of charging and discharging cycles of the batteries. A complete comparison with the three-parameter method (TPM) is represented in order to demonstrate the superiority of the applied methodology. Full article

Lithium–oxygen (Li-O₂) batteries require scalable air electrode concepts and a sensible choice of operation parameters to achieve their promised energy densities. Furthermore, different test parameters are often investigated individually, but rarely brought together in order to optimize the discharge process and unlock the full discharge capability of an air electrode. In this work, we present a highly porous electrode based on graphite nanosheets (GNS) and discuss the impact of the discharge current density and the oxygen pressure as battery test parameters, as well as the electrolyte salt and volume, on the discharge behavior. In particular, changing the electrolyte salt from LiNO₃ to LiTFSI proved to be an important step towards better cell performance, because synergistic effects of the electrolyte and GNS greatly enhance the carbon-specific capacity. The optimized combination of the aforementioned parameters enabled a remarkably high discharge capacity of 56.3 mAh/cm² (5860 mAh/g_carbon) obtained at 150 µA/cm² (15.6 mA/g_carbon), resulting in the almost complete conversion of the lithium anode. These experimental results are an important step towards practical high-capacity air electrodes for Li-O₂ batteries. Full article

Temperature heavily affects the behavior of any energy storage chemistries. In particular, lithium-ion batteries (LIBs) play a significant role in almost all storage application fields, including Electric Vehicles (EVs). Therefore, a full comprehension of the influence of the temperature on the key cell components and their governing equations is mandatory for the effective integration of LIBs into the application. If the battery is exposed to extreme thermal environments or the desired temperature cannot be maintained, the rates of chemical reactions and/or the mobility of the active species may change drastically. The alteration of properties of LIBs with temperature may create at best a performance problem and at worst a safety problem. Despite the presence of many reports on LIBs in the literature, their industrial realization has still been difficult, as the technologies developed in different labs have not been standardized yet. Thus, the field requires a systematic analysis of the effect of temperature on the critical properties of LIBs. In this paper, we report a comprehensive review of the effect of temperature on the properties of LIBs such as performance, cycle life, and safety. In addition, we focus on the alterations in resistances, energy losses, physicochemical properties, and aging mechanism when the temperature of LIBs are not under control. Full article

Lithium-ion cells with a silicon-graphite (SiC) anode and a nickel-rich cathode are potential candidates for use in electric vehicles (EVs) as this material combination offers high energy densities and low costs. Another desired cell specification that results from an intended short charging time for EVs is the robustness against high charge rates. However, high charge rates can lead to the critical aging mechanism of lithium plating, especially at low temperatures. Investigating this issue, this paper presents a test series on cyclic aging with varying charge rates from 0.2C to 1.5C at ambient temperatures of 0 °C and 10 °C applied to a nickel-rich SiC cell candidate. The resulting effects on cell aging are analyzed with a stripping method, whereby reversible lithium plating can be detected, and a differential voltage analysis (DVA), whereby the overall loss of capacity can be attributed to changes in individual characteristic capacities. The results indicate a degradation sensitivity of SiC anodes at elevated charge rates, evidenced by the loss in the silicon-related characteristic capacity, and question the aging robustness of this material combination. Full article

Cycling Li-ion cells with large capacities requires high currents and hence an expensive measurement setup. Aging the Li-ion cell material in coin cells offers an orders-of-magnitude-lower power requirement to the battery tester. The preparation procedure used in this work allows one to build coin cells in a reproducible manner. The original 40 Ah pouch cells and the corresponding 4.3 mAh coin cells (PAT-Cell) utilizing electrode material from the original cells are cycled with 1C at different temperatures. The results show the same basic aging mechanisms in both cell types: loss of lithium inventory at room temperature but an increasing proportion of loss of active material toward higher temperatures. This is confirmed by similar activation energies in capacity degradation of the 40 Ah cells and the averaged coin cells. However, the capacity of the coin cells decreases faster over time. This is caused by diffusion of moisture into the coin cell housing. Nonetheless, the increasing water contamination over measurement time is not directly linked to the loss of capacity of the coin cells. Thus, the observed aging mechanisms of the 40 Ah cells can be qualitatively transferred to coin cell level. Full article

Internal resistance is one of the important parameters in the Li-Ion battery. This paper identifies it using two different methods: electrochemical impedance spectroscopy (EIS) and parameter estimation based on equivalent circuit model (ECM). Comparing internal resistance, the conventional parameter estimation method yields a different value than EIS. Therefore, a hysteresis-free parameter identification method based on ECM is proposed. The proposed technique separates hysteresis resistance from the effective resistance. It precisely estimated actual internal resistance, which matches the internal resistance obtained from EIS. In addition, state of charge, open circuit voltage, and different internal equivalent circuit components were identified. The least square method was used to identify the parameters based on ECM. A parameter extraction algorithm to interpret impedance spectrum obtained from the EIS. The algorithm is based on the properties of Nyquist plot, phasor algebra, and resonances. Experiments were conducted using a cellphone pouch battery and a cylindrical 18650 battery. Full article

Lithium-ion batteries are extensively used for electric vehicles, owing to their great power and energy density. A battery thermal management system is essential for lithium-ion batteries. With the extensive utilization of liquid-cooling approaches for lithium-ion batteries’ thermal management, temperature homogeneity is considerably influenced by coolant distribution. A lower temperature of the cooling fluid brings about a lower temperature of the cell, but the relation and the amount are important to be analyzed. The cooling efficiency is considerably influenced by the flowing conduit arrangement in the cooling plate. Different parameters are affected by the cooling performance of the battery pack. Consequently, the effect of entrance temperature of coolant fluid, current rate, environment temperature, entrance velocity of the coolant fluid, and plate material on the performance and efficiency of a battery thermal management system were investigated. In this investigation, the program ANSYS/FLUENT was employed as the numerical solver to solve the problem. The simulation was accomplished after the end of the discharge. It was seen that the temperature distributions were the most sensitive to the entrance velocity of coolant fluid. It was concluded that the entrance velocity of coolant fluid has the greatest impact on the cooling efficiency and performance of the cold plate. Full article

Lithium-ion batteries (LIBs) are gaining importance in the automotive sector because of the potential of electric vehicles (EVs) to reduce greenhouse gas emissions and air pollution. However, there are serious hazards resulting from failing battery cells leading to exothermic chemical reactions inside the cell, called thermal runaway (TR). Literature of quantifying the failing behavior of modern automotive high capacity cells is rare and focusing on single hazard categories such as heat generation. Thus, the aim of this study is to quantify several hazard relevant parameters of a failing currently used battery cell extracted from a modern mass-produced EV: the temperature response of the cell, the maximum reached cell surface temperature, the amount of produced vent gas, the gas venting rate, the composition of the produced gases including electrolyte vapor and the size and composition of the produced particles at TR. For this purpose, overtemperature experiments with fresh 41 Ah automotive lithium NMC/LMO—graphite pouch cells at different state-of-charge (SOC) 100%, 30% and 0% are performed. The results are valuable for firefighters, battery pack designers, cell recyclers, cell transportation and all who deal with batteries. Full article

The phase-field model based on the Cahn-Hilliard equation is employed to simulate lithium intercalation dynamics in a cathode with particles of distributed size. We start with a simplified phase-field model for a single submicron particle under galvanostatic condition. We observe two stages associated with single-phase and double-phase patterns typical for both charging and discharging processes. The single-phase stage takes approximately 10–15% of the process and plays an important role in the intercalation dynamics. We establish the laws for speed of front propagation and evolution of single-phase concentration valid for different sizes of electrode particles and a wide range of temperatures and C-rates. The universality of these laws allows us to formulate the boundary condition with time-dependent flux density for the Cahn-Hilliard equation and analyze the phase-field intercalation in a heterogeneous cathode characterized by the particle size distribution. Full article

The adhesion between electrode and separator is a key feature in cell assembly. Nafion™-coated separators for water-processed LiNi_0.5Mn_1.5O₄ (LNMO) electrodes are here proposed as an alternative to the polyolefin separators. Specifically, polyolefin separators are modified with Nafion™ solutions and their adhesion to high-potential LNMO electrodes is investigated. The physicochemical properties of the Nafion™-coated separator and its electrochemical performance in Li/LNMO cells are discussed and compared to those obtained with polyolefin Celgard^® (Charlotte, NC, USA) PP2075 separator. Improved adhesion and cycling stability, which could be further enhanced by a mild lamination process, were demonstrated with a thin layer of Nafion™ (0.1 mg cm⁻²). Full article

We describe a ZnBr₂ single cell which has a highly modular symmetrical structure. With designed polyethylene shell frames, membrane frame and composite titanium-carbon felt electrodes, it has a higher energy density and is more flexible compared with traditional flow batteries. We repeatedly tested its performance, which showed good tightness, high reliability and a high energy efficiency of 75%. Due to the special symmetrical structure and modular design, it is easy to assemble and disassemble, which makes it suitable as a test platform for electrodes, membranes and electrolyte performance testing. The designed modular flow cell has low cost and high energy density, and can provide good guidance for flow battery research. Full article

As electric mobility becomes more important every day, scientific research brings us new solutions that increase performance, reduce financial and economic impacts and increase the market share of electric vehicles. Therefore, there is a necessity to compare technical and economic aspects of different technologies for each transport application. This article presents a comparison of three bus prototypes in terms of dynamic performance. The analysis is based on the collection of real data (acceleration, maximum speed and energy consumption) under different settings. Each developed prototype uses the same bus chassis but relies on different energy storage systems. Results show that the dynamic bus performance is independent on the three energy storage technologies, whereas technologies affect the management costs, charging time and available range. An extensive experimental analysis reveals that the bus equipped with a hybrid storage (lithium-ion batteries and supercapacitors) had the most favorable net present value, in comparison with storage composed of only lead–acid or lithium-ion batteries. This result is due to the greater life of lithium-ion batteries and to the capability of supercapacitors, which reduce both batteries depth of discharge and discharge rate. Full article

Lithium-Ion batteries are used in ever more demanding applications regarding operating range and safety requirements. This work presents a series of high-temperature abuse experiments on a nickel-manganese-cobalt oxide (NMC)/graphite lithium-ion battery cell, using advanced in-operando measurement techniques like fast impedance spectroscopy and ultrasonic waves, as well as strain-gauges. the presented results show, that by using these methods degradation effects at elevated temperature can be observed in real-time. These methods have the potential to be integrated into a battery management system in the future. Therefore they make it possible to achieve higher battery safety even under the most demanding operating conditions. Full article

The growing electrification of vehicles and tools increases the demand for low resistance contacts. Today’s batteries for electric vehicles consist of large quantities of single battery cells to reach the desired nominal voltage and energy. Each single cell needs a contacting of its cell terminals, which raises the necessity of an automated contacting process with low joint resistances to reduce the energy loss in the cell transitions. A capable joining process suitable for highly electrically conductive materials like copper or aluminium is the laser beam welding. This study contains the theoretical examination of the joint resistance and a simulation of the current flow dependent on the contacting welds’ position in an overlap configuration. The results are verified by examinations of laser-welded joints in a test bench environment. The investigations are analysing the influence of the shape and position of the weld seams as well as the influence of the laser welding parameters. The investigation identifies a tendency for current to flow predominantly through a contact’s edges. The use of a double weld seam with the largest possible distance greatly increases the joint’s conductivity, by leveraging this tendency and implementing a parallel connection. A simplistic increase of welded contact area does not only have a significantly smaller effect on the overall conductivity, but can eventually also reduce it. Full article

The range of electrode porosity, electrode internal void volume, cell capacity, and capacity ratio that result from electrode coating and calendering tolerance can play a considerable role in cell-to-cell and lot-to-lot performance variation. Based on a coating loading tolerance of ±0.4 mg/cm² and calender tolerance of ±3.0 μm, the resulting theoretical range of physical properties was investigated. For a target positive electrode porosity of 30%, the resulting porosity can range from 19.6% to 38.6%. To account for this variation during the manufacturing process, as much as 41% excess or as little as 59% of the target electrolyte quantity should be added to cells to match the positive electrode void volume. Similar results are reported for a negative electrode of 40% target porosity, where a range from 30.8% to 48.0% porosity is possible. For the negative electrode as little as 72% up to 28% excess electrolyte should be added to fill the internal void space. Although the results are specific to each electrode composition, density, chemistry, and loading the presented process highlight the possible variability of the produced parts. These results are further magnified as cell design moves toward higher power applications with thinner electrode coatings. Full article

Activated carbon (AC) with a very high specific surface area of >3000 m² g⁻¹ and a number of course particles (average size: 75 µm) was pulverized by means of planetary ball milling under different conditions to find its greatest performances as the active material of an electric double-layer capacitor (EDLC) using a nonaqueous electrolyte. The variations in textural properties and particle morphology of the AC during the ball milling were investigated. The electrochemical performance (specific capacitance, rate and cyclic stabilities, and Ragone plot, both from gravimetric and volumetric viewpoints) was also evaluated for the ACs milled with different particle size distributions. A trade-off relation between the pulverization and the porosity maintenance of the AC was observed within the limited milling time. However, prolonged milling led to a degeneration of pores within the AC and a saturation of pulverization degree. The appropriate milling time provided the AC a high volumetric specific capacitance, as well as the greatest maintenance of both the gravimetric and volumetric specific capacitance. A high volumetric energy density of 6.6 Wh L⁻¹ was attained at the high-power density of 1 kW L⁻¹, which was a 35% increment compared with the nonmilled AC. The electrode densification (decreased interparticle gap) and the enhanced ion-transportation within the AC pores, which were attributed to the pulverization, were responsible for those excellent performances. It was also shown that excessive milling could degrade the EDLC performances because of the lowered micro- and meso-porosity and the excessive electrode densification to restrict the ion-transportation within the pores. Full article

The accumulation of solid electrolyte interphases (SEI) in graphite anodes related to elevated formation rates (0.1C, 1C and 2C), cycling rates (1C and 2C), and electrode-separator lamination is investigated. As shown previously, the lamination technique is beneficial for the capacity aging in graphite-LiNi_1/3Mn_1/3Co_1/3O₂ cells. Here, surface resistance growth phenomena are quantified using electrochemical impedance spectroscopy (EIS). The graphite anodes were extracted from the graphite NMC cells in their fully discharged state and irreversible accumulations of lithium in the SEI are revealed using neutron depth profiling (NDP). In this post-mortem study, NDP reveals uniform lithium accumulations as a function of depth with lithium situated at the surface of the graphite particles thus forming the SEI. The SEI was found to grow logarithmically with cycle number starting with the main formation in the initial cycles. Furthermore, the EIS measurements indicate that benefits from lamination arise from surface resistance growth phenomena aside from SEI growth in superior anode fractions. Full article