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Batteries, Volume 10, Issue 2 (February 2024) – 28 articles

Cover Story (view full-size image): With a rapidly growing number of EV traction batteries, there is a rising demand for classifying their usability, particularly for second-life applications and recycling. In this article, a novel approach is introduced named the State of Usability (SOU) for rating batteries that have reached the end of their primary life. Two comprehensive methods for the practical implementation of the approach are presented. View this paper
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24 pages, 15497 KiB  
Review
Could Commercially Available Aqueous Binders Allow for the Fabrication of Highly Loaded Sulfur Cathodes with a Stable Cycling Performance?
by Wenli Wei, Marzi Barghamadi, Anthony F. Hollenkamp and Peter J. Mahon
Batteries 2024, 10(2), 67; https://doi.org/10.3390/batteries10020067 - 19 Feb 2024
Viewed by 1534
Abstract
In this review, the application of five commercially available aqueous-based binders including sodium carboxyl methyl cellulose (CMC), polyacrylic acid (PAA), polyvinyl alcohol (PVA), polyethylene oxide (PEO), and polyethyleneimine (PEI) as well as some representative custom (or purpose) synthesized functional binders used in lithium [...] Read more.
In this review, the application of five commercially available aqueous-based binders including sodium carboxyl methyl cellulose (CMC), polyacrylic acid (PAA), polyvinyl alcohol (PVA), polyethylene oxide (PEO), and polyethyleneimine (PEI) as well as some representative custom (or purpose) synthesized functional binders used in lithium sulfur (Li-S) batteries is summarized based on the main evaluation criteria of cycling capacity, battery lifetime, and areal sulfur loading (and, consequently, energy density of the battery). CMC with SBR (styrene butadiene rubber) has been reported with promising results in highly loaded sulfur cathodes (>5 mg cm−2 sulfur loading). PVA and PEI were confirmed to provide an enhanced adsorption of lithium polysulfides due to the interaction with hydroxyl and amine groups. No competitive advantage in electrochemical performance was demonstrated through the use of PAA and PEO. Water-based binders modified with polysulfide-trapping functional groups have complex fabrication processes, which hinders their commercial application. In general, achieving a high capacity and long cycling stability for highly loaded sulfur cathodes using commercial aqueous-based binders remains a significant challenge. Additionally, the scalability of these reported sulfur cathodes, in terms of complexity, cost, and stable electrochemical cycling, should be evaluated through further battery testing, particularly targeting pouch cell performance. Full article
(This article belongs to the Special Issue Functional Binders and Additives for Rechargeable Batteries)
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22 pages, 6542 KiB  
Article
Equivalent Minimum Hydrogen Consumption of Fuzzy Control-Based Fuel Cells: Exploration of Energy Management Strategies for Ships
by Yubo Sun, Qianming Shang and Wanying Jiang
Batteries 2024, 10(2), 66; https://doi.org/10.3390/batteries10020066 - 18 Feb 2024
Viewed by 1245
Abstract
Aiming to solve the problems of insufficient dynamic responses, the large loss of energy storage life of a single power cell, and the large fluctuation in DC (direct current) bus voltage in fuel cell vessels, this study takes a certain type of fuel [...] Read more.
Aiming to solve the problems of insufficient dynamic responses, the large loss of energy storage life of a single power cell, and the large fluctuation in DC (direct current) bus voltage in fuel cell vessels, this study takes a certain type of fuel cell ferry as the research object and proposes an improved equivalent minimum hydrogen consumption energy management strategy, based on fuzzy logic control. First, a hybrid power system including a fuel cell, a lithium–iron–phosphate battery, and a supercapacitor is proposed, with the simulation of the power system of the modified mother ship. Second, a power system simulation model and a double-closed-loop PI (proportion integration) control model are established in MATLAB/Simulink to design the equivalent hydrogen consumption model and fuzzy logic control strategy. The simulation results show that, under the premise of meeting the load requirements, the control strategy designed in this paper improves the Li-ion battery’s power, the Li-ion battery’s SOC (state of charge), the bus voltage stability, and the equivalent hydrogen consumption significantly, compared with those before optimization, which improves the stability and economy of the power system and has certain practical engineering value. Full article
(This article belongs to the Special Issue Modeling, Reliability and Health Management of Lithium-Ion Batteries)
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22 pages, 3125 KiB  
Article
Modelling Binder Degradation in the Thermal Treatment of Spent Lithium-Ion Batteries by Coupling Discrete Element Method and Isoconversional Kinetics
by Christian Nobis, Marco Mancini and Michael Fischlschweiger
Batteries 2024, 10(2), 63; https://doi.org/10.3390/batteries10020063 - 18 Feb 2024
Viewed by 1303
Abstract
Developing efficient recycling processes with high recycling quotas for the recovery of graphite and other critical raw materials contained in LIBs is essential and prudent. This action holds the potential to substantially diminish the supply risk of raw materials for LIBs and enhance [...] Read more.
Developing efficient recycling processes with high recycling quotas for the recovery of graphite and other critical raw materials contained in LIBs is essential and prudent. This action holds the potential to substantially diminish the supply risk of raw materials for LIBs and enhance the sustainability of their production. An essential processing step in LIB recycling involves the thermal treatment of black mass to degrade the binder. This step is crucial as it enhances the recycling efficiency in subsequent processes, such as flotation and leaching-based processing. Therefore, this paper introduces a Representative Black Mass Model (RBMM) and develops a computational framework for the simulation of the thermal degradation of polymer-based binders in black mass (BM). The models utilize the discrete element method (DEM) with a coarse-graining (CG) scheme and the isoconversional method to predict binder degradation and the required heat. Thermogravimetric analysis (TGA) of the binder polyvinylidene fluoride (PVDF) is utilized to determine the model parameters. The model simulates a specific thermal treatment case on a laboratory scale and investigates the relationship between the scale factor and heating rate. The findings reveal that, for a particular BM system, a scaling factor of 100 regarding the particle diameter is applicable within a heating rate range of 2 to 22 K/min. Full article
(This article belongs to the Section Battery Processing, Manufacturing and Recycling)
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26 pages, 6055 KiB  
Review
Critical Review on High-Safety Lithium-Ion Batteries Modified by Self-Terminated Oligomers with Hyperbranched Architectures
by Debabrata Mohanty, I-Ming Hung, Chien-Te Hsieh, Jing-Pin Pan and Wei-Ren Liu
Batteries 2024, 10(2), 65; https://doi.org/10.3390/batteries10020065 - 16 Feb 2024
Viewed by 1448
Abstract
In recent years, the evolution of lithium-ion batteries (LIB) has been propelled by the growing demand for energy storage systems that are lightweight, have high energy density, and are long-lasting. This review article examines the use of self-terminated oligomers with hyperbranched architecture (STOBA) [...] Read more.
In recent years, the evolution of lithium-ion batteries (LIB) has been propelled by the growing demand for energy storage systems that are lightweight, have high energy density, and are long-lasting. This review article examines the use of self-terminated oligomers with hyperbranched architecture (STOBA) as a key electrode additive for the superior performance of LIBs. STOBA has been found to have excellent electrochemical properties, including high specific capacity, low impedance, and good cycling stability when used as an additive in electrode materials. The article discusses the process of synthesis and characterization of STOBA materials, including their potential applications in LIBs as electrode material additives. The article also discusses current research on the optimization of STOBA materials for LIBs, including the use of different solvents, monomers, and initiators. Overall, the review concludes that STOBA materials possess huge potential as a next-generation additive for LIB safety. Full article
(This article belongs to the Special Issue Review of Advanced Batteries: Electrode Materials)
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16 pages, 1643 KiB  
Article
Reducing Energy Consumption and Greenhouse Gas Emissions of Industrial Drying Processes in Lithium-Ion Battery Cell Production: A Qualitative Technology Benchmark
by Marius Schütte, Florian Degen and Hendrik Walter
Batteries 2024, 10(2), 64; https://doi.org/10.3390/batteries10020064 - 16 Feb 2024
Viewed by 1387
Abstract
As the world’s automotive battery cell production capacity expands, so too does the demand for sustainable production. Much of the industry’s efforts are aimed at reducing the high energy consumption in battery cell production. A key driver is electrode drying, which is currently [...] Read more.
As the world’s automotive battery cell production capacity expands, so too does the demand for sustainable production. Much of the industry’s efforts are aimed at reducing the high energy consumption in battery cell production. A key driver is electrode drying, which is currently performed in long ovens using large volumes of hot air. Several drying technologies from other industries could reduce energy consumption and greenhouse gas emissions if successfully applied to battery cell production. High process and quality requirements must be met when adapting these technologies for battery cell production. Evaluating the technologies against these requirements is difficult due to the technological novelty of this industry and the associated lack of data. Furthermore, the significant differences in drying technologies render a comparison even more challenging. One objective of this study was to evaluate drying technologies and identify those that could be best adapted to lithium-ion battery cell production. Near-infrared and laser drying were found to be the best in terms of energy efficiency, cost savings and other parameters. Another aim was to analyse, in more detail, the technological challenges and the advantages and disadvantages of the top-ranked drying technologies. Finally, the saving potential for greenhouse gas emissions of near-infrared and laser drying was calculated for a global production scenario of LIB cells in 2030. The saving potential in this scenario would amount to 2.63 million metric tonnes (Mt) CO2eq per year if near-infrared drying was applied in all global LIB cell production facilities within the mentioned scenario and 1.47 million Mt CO2eq per year for laser drying. Full article
(This article belongs to the Section Battery Processing, Manufacturing and Recycling)
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16 pages, 1273 KiB  
Review
Intrinsic Safety Risk Control and Early Warning Methods for Lithium-Ion Power Batteries
by Yi Cui, Xueling Shen, Hang Zhang, Yanping Yin, Zhanglong Yu, Dong Shi, Yanyan Fang and Ran Xu
Batteries 2024, 10(2), 62; https://doi.org/10.3390/batteries10020062 - 15 Feb 2024
Viewed by 1818
Abstract
Since 2014, the electric vehicle industry in China has flourished and has been accompanied by rapid growth in the power battery industry led by lithium-ion battery (LIB) development. Due to a variety of factors, LIBs have been widely used, but user abuse and [...] Read more.
Since 2014, the electric vehicle industry in China has flourished and has been accompanied by rapid growth in the power battery industry led by lithium-ion battery (LIB) development. Due to a variety of factors, LIBs have been widely used, but user abuse and battery quality issues have led to explosion accidents that have caused loss of life and property. Current strategies to address battery safety concerns mainly involve enhancing the intrinsic safety of batteries and strengthening safety controls with approaches such as early warning systems to alert users before thermal runaway and ensure user safety. In this paper, we discuss the current research status and trends in two areas, intrinsic battery safety risk control and early warning methods, with the goal of promoting the development of safe LIB solutions in new energy applications. Full article
(This article belongs to the Section Battery Performance, Ageing, Reliability and Safety)
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13 pages, 5092 KiB  
Article
A Low-Cost and High-Efficiency Active Cell-Balancing Circuit for the Reuse of EV Batteries
by Minh-Chau Dinh, Thi-Tinh Le and Minwon Park
Batteries 2024, 10(2), 61; https://doi.org/10.3390/batteries10020061 - 15 Feb 2024
Viewed by 1620
Abstract
In this paper, a high-efficiency and low-cost active cell-to-cell balancing circuit for the reuse of electric vehicle (EV) batteries is proposed. In the proposed method, a battery string is divided into two legs to transfer the charge from each cell in one leg [...] Read more.
In this paper, a high-efficiency and low-cost active cell-to-cell balancing circuit for the reuse of electric vehicle (EV) batteries is proposed. In the proposed method, a battery string is divided into two legs to transfer the charge from each cell in one leg to that in the other and a bidirectional CLLC resonant converter is used to transfer energy between the selected cells. Thanks to the proposed structure, the number of bidirectional switches and gate drivers can be reduced by half compared to the conventional direct cell-to-cell topologies, thereby achieving lower cost for the system. The CLLC converter is used to transfer the charge, and it is designed to work at resonant frequencies to achieve zero-voltage zero-current switching (ZVZCS) for all the switches and diodes. Consequently, the system’s efficiency can be enhanced, and hence, the fuel economy of the system can also be improved significantly. To verify the performance of the proposed active cell-balancing system, a prototype is implemented for balancing the three EV battery modules that contain twelve lithium-ion batteries from xEV. The maximum efficiency achieved for the charge transfer is 89.4%, and the balancing efficiency is 96.3%. Full article
(This article belongs to the Section Battery Modelling, Simulation, Management and Application)
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19 pages, 2601 KiB  
Article
Charge Scheduling of Electric Vehicle Fleets: Maximizing Battery Remaining Useful Life Using Machine Learning Models
by David Geerts, Róbinson Medina, Wilfried van Sark and Steven Wilkins
Batteries 2024, 10(2), 60; https://doi.org/10.3390/batteries10020060 - 15 Feb 2024
Viewed by 1233
Abstract
Reducing greenhouse emissions can be done via the electrification of the transport industry. However, there are challenges related to the electrification such as the lifetime of vehicle batteries as well as limitations on the charging possibilities. To cope with some of these challenges, [...] Read more.
Reducing greenhouse emissions can be done via the electrification of the transport industry. However, there are challenges related to the electrification such as the lifetime of vehicle batteries as well as limitations on the charging possibilities. To cope with some of these challenges, a charge scheduling method for fleets of electric vehicles is presented. Such a method assigns the charging moments (i.e., schedules) of fleets that have more vehicles than chargers. While doing the assignation, the method also maximizes the total Remaining Useful Life (RUL) of all the vehicle batteries. The method consists of two optimization algorithms. The first optimization algorithm determines charging profiles (i.e., charging current vs time) for individual vehicles. The second algorithm finds the charging schedule (i.e., the order in which vehicles are connected to a charger) that maximizes the RUL in the batteries of the entire fleet. To reduce the computational effort of predicting the battery RUL, the method uses a Machine Learning (ML) model. Such a model predicts the RUL of an individual battery while taking into account common stress factors and fabrication-related differences per battery. Simulation results show that charging a single vehicle as late as possible maximizes the RUL of that single vehicle, due to the lower battery degradation. Simulations also show that the ML model accurately predicts the RUL, while taking into account fabrication-related variability in the battery. Additionally, it was shown that this method schedules the charging moments of a fleet, leading to an increased total RUL of all the batteries in the vehicle fleet. Full article
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26 pages, 14951 KiB  
Article
Adaptive Integrated Thermal Management System for a Stable Driving Environment in Battery Electric Vehicles
by Jaehyun Bae, Daeil Hyun and Jaeyoung Han
Batteries 2024, 10(2), 59; https://doi.org/10.3390/batteries10020059 - 15 Feb 2024
Viewed by 1185
Abstract
With an increase in global warming, battery electric vehicles (BEVs), which are environmentally friendly, have been rapidly commercialized to replace conventional vehicles with internal combustion engines. Unlike traditional internal combustion engine vehicles, the powertrain system of BEVs operates with high efficiency, resulting in [...] Read more.
With an increase in global warming, battery electric vehicles (BEVs), which are environmentally friendly, have been rapidly commercialized to replace conventional vehicles with internal combustion engines. Unlike traditional internal combustion engine vehicles, the powertrain system of BEVs operates with high efficiency, resulting in lower heat generation. This poses a challenge for cabin heating under low-temperature conditions. Conversely, under high-temperature conditions, the operating temperature of a high-voltage battery (HVB) is lower than the ambient air temperature, which makes cooling through ambient air challenging. To overcome these challenges, in this study, we proposed an integrated thermal management system (ITMS) based on a heat pump system capable of stable thermal management under diverse climatic conditions. Furthermore, to assess the ability of the proposed ITMS to perform thermal management under various climatic conditions, we integrated a detailed powertrain system model incorporating BEV specifications and the proposed ITMS model based on the heat pump system. The ITMS model was evaluated under high-load-driving conditions, specifically the HWFET scenario, demonstrating its capability to perform stable thermal management not only under high-temperature conditions, such as at 36 °C, but also under low-temperature conditions, such as at −10 °C, through the designated thermal management modes. Full article
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21 pages, 6549 KiB  
Article
The Impact of Structural Pattern Types on the Electrochemical Performance of Ultra-Thick NMC 622 Electrodes for Lithium-Ion Batteries
by Penghui Zhu, Benjamin Ebert, Peter Smyrek and Wilhelm Pfleging
Batteries 2024, 10(2), 58; https://doi.org/10.3390/batteries10020058 - 08 Feb 2024
Viewed by 1729
Abstract
An increase in the energy density on the cell level while maintaining a high power density can be realized by combining thick-film electrodes and the 3D battery concept. The effect of laser structuring using different pattern types on the electrochemical performance was studied. [...] Read more.
An increase in the energy density on the cell level while maintaining a high power density can be realized by combining thick-film electrodes and the 3D battery concept. The effect of laser structuring using different pattern types on the electrochemical performance was studied. For this purpose, LiNi0.6Mn0.2Co0.2O2 (NMC 622) thick-film cathodes were prepared with a PVDF binder and were afterward structured using ultrafast laser ablation. Eight different pattern types were realized, which are lines, grids, holes, hexagonal structures, and their respective combinations. In addition, the mass loss caused by laser ablation was kept the same regardless of the pattern type. The laser-structured electrodes were assembled in coin cells and subsequently electrochemically characterized. It was found that when discharging the cells for durations of less than 2 h, a significant, positive impact of laser patterning on the electrochemical cell performance was observed. For example, when discharging was performed for one hour, cells containing laser-patterned electrodes with different structure types exhibited a specific capacity increase of up to 70 mAh/g in contrast to the reference ones. Although cells with a hole-patterned electrode exhibited a minimum capacity increase in the rate capability analysis, the combination of holes with lines, grids, or hexagons led to further capacity increases. In addition, long-term cycle analyses demonstrated the benefits of laser patterning on the cell lifetime, while cyclic voltammetry highlighted an increase in the Li-ion diffusion kinetics in cells containing hexagonal-patterned electrodes. Full article
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13 pages, 1713 KiB  
Article
On the State of Usability for Lithium–Ion Batteries
by Christopher Wett, Jörg Lampe, Jan Haß, Thomas Seeger and Bugra Turan
Batteries 2024, 10(2), 57; https://doi.org/10.3390/batteries10020057 - 04 Feb 2024
Viewed by 1833
Abstract
Lithium–ion batteries are well established as traction batteries for electric vehicles. This has led to a growing market for second-life batteries that can be used in applications like home energy storage systems. Moreover, the recyclability and safe handling of aged or damaged cells [...] Read more.
Lithium–ion batteries are well established as traction batteries for electric vehicles. This has led to a growing market for second-life batteries that can be used in applications like home energy storage systems. Moreover, the recyclability and safe handling of aged or damaged cells and packs has become more important. While there are several indicators, like state of health (SOH), state of power (SOP), or state of safety (SOS), which describe the state of a battery before its defined end of life (EOL), there is no consistent classification methodology by which to describe the usability of a cell or pack after its EOL is reached. The proposed state of usability (SOU) provides a new indicator that accounts for the usability for second life, recyclability, and possible required safety handling of a lithium–ion battery after its first intended life cycle. This work presents a decision tree method, which in turn leads to five discrete usability levels enabling a fast and rough determination of the SOU for practical use. Further, a calculation methodology for reasonable continuous regions of the SOU is proposed. Both methods are based on a literature-based rating of all of the relevant defect and aging mechanisms displayed in a risk matrix. Finally, some experimental methods that can be used for SOU determination are proposed. The developed methodology and the hands-on approach using a decision tree are well-suited for real world application in recycling companies and battery test laboratories. Full article
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27 pages, 5866 KiB  
Review
Phosphorus-Containing Polymer Electrolytes for Li Batteries
by Narcis Varan, Petru Merghes, Nicoleta Plesu, Lavinia Macarie, Gheorghe Ilia and Vasile Simulescu
Batteries 2024, 10(2), 56; https://doi.org/10.3390/batteries10020056 - 04 Feb 2024
Viewed by 1483
Abstract
Lithium-ion polymer batteries, also known as lithium-polymer, abbreviated Li-po, are one of the main research topics nowadays in the field of energy storage. This review focuses on the use of the phosphorus containing compounds in Li-po batteries, such as polyphosphonates and polyphosphazenes. Li-po [...] Read more.
Lithium-ion polymer batteries, also known as lithium-polymer, abbreviated Li-po, are one of the main research topics nowadays in the field of energy storage. This review focuses on the use of the phosphorus containing compounds in Li-po batteries, such as polyphosphonates and polyphosphazenes. Li-po batteries are mini-devices, capable of providing power for any portable gadget. From a constructive point of view, Li-po batteries contain an anode (carbon), a cathode (metal oxide), and a polymer electrolyte, which could be liquid electrolytes or solid electrolytes. In general, a divider is used to keep the anode and cathode from touching each other directly. Since liquid electrolytes have a generally high ionic conductivity, they are frequently employed in Li-ion batteries. In the last decade, the research in this field has also focused on solving safety issues, such as the leakage of electrolytes and risk of ignition due to volatile and flammable organic solvents. The research topics in the field of Li-po remain focused on solving safety problems and improving performance. Full article
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50 pages, 104911 KiB  
Article
Influence of the Arrangement of the Cells/Modules of a Traction Battery on the Spread of Fire in Case of Thermal Runaway
by Ana Olona and Luis Castejón
Batteries 2024, 10(2), 55; https://doi.org/10.3390/batteries10020055 - 03 Feb 2024
Viewed by 1996
Abstract
When designing the battery of an electric vehicle, different parameters must be considered to obtain the safest arrangement of the battery/modules/cells from the mechanical and thermal points of view. In this study, the thermal runaway propagation mechanism of lithium-ion cells is analyzed as [...] Read more.
When designing the battery of an electric vehicle, different parameters must be considered to obtain the safest arrangement of the battery/modules/cells from the mechanical and thermal points of view. In this study, the thermal runaway propagation mechanism of lithium-ion cells is analyzed as a function of their arrangement within a battery pack in case of a fire propagation of a battery pack in which a thermal runaway has occurred. The objective is to identify which cell/module arrangement is most critical within the battery pack, using microscopic analysis of the structure and chemical composition of the most damaged cells, both horizontally and vertically, of a battery belonging to a burnt vehicle. And their final condition was compared with the condition of new cells of the same type. In this way, the structure and chemical composition of the cathode, anode, and separator after thermal runaway were compared. This research was carried out to obtain information to understand the mechanical properties of lithium-ion cells and their behavior after thermal runaway heating leading to the propagation of a fire. Through the analysis carried out, it is concluded that cells placed in a vertical arrangement have worse behavior than cells in a horizontal arrangement. Regarding the safety of the battery, the results of this study will allow us to determine which arrangement and structure of the cells in the battery pack is safer against thermal runaway due to thermal failure. Full article
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20 pages, 3650 KiB  
Review
Tuning of Ionic Liquid–Solvent Electrolytes for High-Voltage Electrochemical Double Layer Capacitors: A Review
by Yan Wang, Kaiyuan Xue, Changzeng Yan, Yuehui Li, Xingyun Zhang, Kailimai Su, Pengjun Ma, Shanhong Wan and Junwei Lang
Batteries 2024, 10(2), 54; https://doi.org/10.3390/batteries10020054 - 02 Feb 2024
Viewed by 1700
Abstract
Electrochemical double-layer capacitors (EDLCs) possess extremely high-power density and a long cycle lifespan, but they have been long constrained by a low energy density. Since the electrochemical stability of electrolytes is essential to the operating voltage of EDLCs, and thus to their energy [...] Read more.
Electrochemical double-layer capacitors (EDLCs) possess extremely high-power density and a long cycle lifespan, but they have been long constrained by a low energy density. Since the electrochemical stability of electrolytes is essential to the operating voltage of EDLCs, and thus to their energy density, the tuning of electrolyte components towards a high-voltage window has been a research focus for a long time. Organic electrolytes based on ionic liquids (ILs) are recognized as the most commercially promising owing to their moderate operating voltage and excellent conductivity. Despite impressive progress, the working voltage of IL–solvent electrolytes needs to be improved to meet the growing demand. In this review, the recent progress in the tuning of IL- based organic electrolyte components for higher-voltage EDLCs is comprehensively summarized and the advantages and limitations of these innovative components are outlined. Furthermore, future trends of IL–solvent electrolytes in this field are highlighted. Full article
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31 pages, 9269 KiB  
Article
Bubble Wrap-like Carbon-Coated Rattle-Type silica@silicon Nanoparticles as Hybrid Anode Materials for Lithium-Ion Batteries via Surface-Protected Etching
by Angelica Martino, Jiyun Jeon, Hyun-Ho Park, Hochun Lee and Chang-Seop Lee
Batteries 2024, 10(2), 53; https://doi.org/10.3390/batteries10020053 - 01 Feb 2024
Viewed by 1634
Abstract
Severe volumetric expansion (~400%) limits practical application of silicon nanoparticles as anode materials for next-generation lithium-ion batteries (LIBs). Here, we describe the fabrication and characterization of a conformal polydopamine carbon shell encapsulating rattle-type silica@silicon nanoparticles (PDA–PEI@PVP–SiO2@Si) with a tunable void structure [...] Read more.
Severe volumetric expansion (~400%) limits practical application of silicon nanoparticles as anode materials for next-generation lithium-ion batteries (LIBs). Here, we describe the fabrication and characterization of a conformal polydopamine carbon shell encapsulating rattle-type silica@silicon nanoparticles (PDA–PEI@PVP–SiO2@Si) with a tunable void structure using a dual template strategy with TEOS and (3-aminopropyl)triethoxysilane (APTES) pretreated with polyvinylpyrrolidone (PVP K30) as SiO2 sacrificial template via a modified Stöber process. Polyethylene imine (PEI) crosslinking facilitated the construction of an interconnected three-dimensional bubble wrap-like carbon matrix structure through hydrothermal treatment, pyrolysis, and subsequent surface-protected etching. The composite anode material delivered satisfactory capacities of 539 mAh g−1 after 100 cycles at 0.1 A g−1, 512.76 mAh g−1 after 200 cycles at 1 A g−1, and 453 mAh g−1 rate performance at 5 A g−1, respectively. The electrochemical performance of PDA–PEI@PVP–SiO2@Si was attributed to the rattle-type structure providing void space for Si volume expansion, PVP K30-pretreated APTES/TEOS SiO2 seeds via catalyst-free, hydrothermal-assisted Stöber protecting Si/C spheres upon etching, carbon coating strategy increasing Si conductivity while stabilizing the solid electrolyte interface (SEI), and PEI carbon crosslinks providing continuous conductive pathways across the electrode structure. The present work describes a promising strategy to synthesize tunable yolk shell C@void@Si composite anode materials for high power/energy-density LIBs applications. Full article
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21 pages, 154686 KiB  
Article
Design Optimisation of Metastructure Configuration for Lithium-Ion Battery Protection Using Machine Learning Methodology
by Indira Cahyani Fatiha, Sigit Puji Santosa, Djarot Widagdo and Arief Nur Pratomo
Batteries 2024, 10(2), 52; https://doi.org/10.3390/batteries10020052 - 01 Feb 2024
Viewed by 1648
Abstract
The market for electric vehicles (EVs) has been growing in popularity, and by 2027, it is predicted that the market valuation will reach $869 billion. To support the growth of EVs in public road safety, advances in battery safety research for EV application [...] Read more.
The market for electric vehicles (EVs) has been growing in popularity, and by 2027, it is predicted that the market valuation will reach $869 billion. To support the growth of EVs in public road safety, advances in battery safety research for EV application should achieve low-cost, lightweight, and high safety protection. In this research, the development of a lightweight, crashworthy battery protection system using an excellent energy absorption capability is carried out. The lightweight structure was developed by using metastructure constructions with an arrangement of repeated lattice cellular structures. Three metastructure configurations (bi-stable, star-shaped, double-U) with their geometrical variables (thickness, inner spacing, cell stack) and material types (stainless steel, aluminium, and carbon steel) were evaluated until the maximum Specific Energy Absorptions (SEA) value was attained. The Finite Element Method (FEM) is utilised to simulate the mechanics of impact and calculate the optimum SEA of the various designs using machine learning methodology. Latin Hypercube Sampling (LHS) was used to derive the design variation by dividing the variables into 100 samples. The machine learning optimisation method utilises the Artificial Neural Networks (ANN) and Non-dominated Sorting Genetic Algorithm-II (NSGA-II) to forecast the design that produces maximum SEA. The optimum control variables are star-shaped cells consisting of one vertical unit cell using aluminium material with a cross-section thickness of 2.9 mm. The optimum design increased the SEA by 5577% compared to the baseline design. The accuracy of the machine learning prediction is also verified using numerical simulation with a 2.83% error. Four different sandwich structure configurations are then constructed using the optimal geometry for prismatic battery protection subjected to ground impact loading conditions. An optimum configuration of 6×4×1 core cells arrangement results in a maximum displacement of 7.33 mm for the prismatic battery in the ground impact simulation, which is still less than the deformation threshold for prismatic battery safety of 10.423 mm. It is shown that the lightweight metastructure is very efficient for prismatic battery protection subjected to ground impact loading conditions. Full article
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13 pages, 6159 KiB  
Article
AI-Based Nano-Scale Material Property Prediction for Li-Ion Batteries
by Mohit Anil Lal, Akashdeep Singh, Ryan Mzik, Amirmasoud Lanjan and Seshasai Srinivasan
Batteries 2024, 10(2), 51; https://doi.org/10.3390/batteries10020051 - 29 Jan 2024
Viewed by 1507
Abstract
In this work, we propose a machine learning (ML)-based technique that can learn interatomic potential parameters for various particle–particle interactions employing quantum mechanics (QM) calculations. This ML model can be used as an alternative for QM calculations for predicting non-bonded interactions in a [...] Read more.
In this work, we propose a machine learning (ML)-based technique that can learn interatomic potential parameters for various particle–particle interactions employing quantum mechanics (QM) calculations. This ML model can be used as an alternative for QM calculations for predicting non-bonded interactions in a computationally efficient manner. Using these parameters as input to molecular dynamics simulations, we can predict a diverse range of properties, enabling researchers to design new and novel materials suitable for various applications in the absence of experimental data. We employ our ML-based technique to learn the Buckingham potential, a non-bonded interatomic potential. Subsequently, we utilize these predicted values to compute the densities of four distinct molecules, achieving an accuracy exceeding 93%. This serves as a strong demonstration of the efficacy of our proposed approach. Full article
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45 pages, 13074 KiB  
Review
Review of Thermal Management Strategies for Cylindrical Lithium-Ion Battery Packs
by Mohammad Ahmadian-Elmi and Peng Zhao
Batteries 2024, 10(2), 50; https://doi.org/10.3390/batteries10020050 - 28 Jan 2024
Cited by 2 | Viewed by 2721
Abstract
This paper presents a comprehensive review of the thermal management strategies employed in cylindrical lithium-ion battery packs, with a focus on enhancing performance, safety, and lifespan. Effective thermal management is critical to retain battery cycle life and mitigate safety issues such as thermal [...] Read more.
This paper presents a comprehensive review of the thermal management strategies employed in cylindrical lithium-ion battery packs, with a focus on enhancing performance, safety, and lifespan. Effective thermal management is critical to retain battery cycle life and mitigate safety issues such as thermal runaway. This review covers four major thermal management techniques: air cooling, liquid cooling, phase-change materials (PCM), and hybrid methods. Air-cooling strategies are analyzed for their simplicity and cost-effectiveness, while liquid-cooling systems are explored for their superior heat dissipation capabilities. Phase-change materials, with their latent heat absorption and release properties, are evaluated as potential passive cooling solutions. Additionally, hybrid methods, such as combining two or more strategies, are discussed for their synergistic effects in achieving optimal thermal management. Each strategy is assessed in terms of its thermal performance, energy efficiency, cost implications, and applicability to cylindrical lithium-ion battery packs. The paper provides valuable insights into the strengths and limitations of each technique, offering a comprehensive guide for researchers, engineers, and policymakers in the field of energy storage. The findings contribute to the ongoing efforts to develop efficient and sustainable thermal management solutions for cylindrical lithium-ion battery packs in various applications. Full article
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13 pages, 4916 KiB  
Article
Graphite Felt as an Innovative Electrode Material for Alkaline Water Electrolysis and Zinc–Air Batteries
by Yejin Lee, Seung-hee Park and Sung Hoon Ahn
Batteries 2024, 10(2), 49; https://doi.org/10.3390/batteries10020049 - 28 Jan 2024
Viewed by 1714
Abstract
Recent advancements in energy conversion and storage systems have placed a spotlight on the role of multi-functional electrodes employing conductive substrates. These substrates, however, often face obstacles due to intricate and expensive production methods, as well as limitations in thickness. This research introduces [...] Read more.
Recent advancements in energy conversion and storage systems have placed a spotlight on the role of multi-functional electrodes employing conductive substrates. These substrates, however, often face obstacles due to intricate and expensive production methods, as well as limitations in thickness. This research introduces a novel, economical approach using graphite felt as a versatile electrode. A method to enhance the typically low conductivity of graphite felt was devised, incorporating interfacial chemical tuning and the electrodeposition of a highly conductive nickel layer. This technique facilitates the integration of diverse transition metal-based active sites, aiming to refine the catalytic activity for specific electrochemical reactions. A key finding is that a combination of a nickel-rich cathode and an iron-rich anode can effectively optimize alkaline water electrolysis for hydrogen production at the ampere scale. Furthermore, the addition of sulfur improves the bi-functional oxygen-related redox reactions, rendering it ideal for air cathodes in solid-state zinc–air batteries. The assembled battery exhibits impressive performance, including a peak power density of 62.9 mW cm−2, a minimal voltage gap in discharge–charge polarization, and a lifecycle surpassing 70 h. This advancement in electrode technology signifies a significant leap in energy storage and conversion, offering a sustainable and efficient solution for future energy systems. Full article
(This article belongs to the Special Issue Zinc-Based Batteries: Recent Progress and Future Perspectives)
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13 pages, 3286 KiB  
Article
Effect of Mn Substitution on GeFe2O4 as an Anode for Sodium Ion Batteries
by Marco Ambrosetti, Walter Rocchetta, Irene Quinzeni, Chiara Milanese, Vittorio Berbenni and Marcella Bini
Batteries 2024, 10(2), 48; https://doi.org/10.3390/batteries10020048 - 27 Jan 2024
Viewed by 1464
Abstract
GeFe2O4 (GFO), with its intriguing intercalation mechanism based on alloying–conversion reactions, was recently proposed as an anode material for sodium ion batteries (SIBs). However, drawbacks related to excessive volume expansion during intercalation/deintercalation and poor electronic conductivity enormously hinder its practical [...] Read more.
GeFe2O4 (GFO), with its intriguing intercalation mechanism based on alloying–conversion reactions, was recently proposed as an anode material for sodium ion batteries (SIBs). However, drawbacks related to excessive volume expansion during intercalation/deintercalation and poor electronic conductivity enormously hinder its practical application in batteries. In this regard, some experimental strategies such as cation substitutions and proper architectures/carbon coatings can be adopted. In this paper, pure and Mn-doped GFO samples were prepared by hydrothermal synthesis. The doped samples maintained the spinel cubic structure and the morphology of pure GFO. The electrochemical tests of the samples, performed after proper carbon coating, showed the expected redox processes involving both Ge and Fe ions. The Mn doping had a positive effect on the capacity values at a low current density (about 350 mAh/g at C/5 for the Mn 5% doping in comparison to 300 mAh/g for the pure sample). Concerning the cycling stability, the doped samples were able to provide 129 mAh/g (Mn 10%) and 150 mAh/g (Mn 5%) at C/10 after 60 cycles. Full article
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46 pages, 12754 KiB  
Review
N-Doped Graphene (N-G)/MOF(ZIF-8)-Based/Derived Materials for Electrochemical Energy Applications: Synthesis, Characteristics, and Functionality
by Niladri Talukder, Yudong Wang, Bharath Babu Nunna and Eon Soo Lee
Batteries 2024, 10(2), 47; https://doi.org/10.3390/batteries10020047 - 27 Jan 2024
Cited by 1 | Viewed by 2527
Abstract
In recent years, graphene-type materials originating from metal–organic frameworks (MOFs) or integrated with MOFs have exhibited notable performances across various applications. However, a comprehensive understanding of these complex materials and their functionalities remains obscure. While some studies have reviewed graphene/MOF composites from different [...] Read more.
In recent years, graphene-type materials originating from metal–organic frameworks (MOFs) or integrated with MOFs have exhibited notable performances across various applications. However, a comprehensive understanding of these complex materials and their functionalities remains obscure. While some studies have reviewed graphene/MOF composites from different perspectives, due to their structural–functional intricacies, it is crucial to conduct more in-depth reviews focusing on specific sets of graphene/MOF composites designed for particular applications. In this review, we thoroughly investigate the syntheses, characteristics, and performances of N-G/MOF(ZIF-8)-based/derived materials employed in electrochemical energy conversion and storage systems. Special attention is given to realizing their fundamental functionalities. The discussions are divided into three segments based on the application of N-G/ZIF-8-based/derived materials as electrode materials for batteries, electrodes for electrochemical capacitors, and electrocatalysts. As electrodes for batteries, N-G/MOF(ZIF-8) materials can mitigate issues like an electrode volume expansion for Li-ion batteries and the ‘shuttle effect’ for Li-S batteries. As electrodes for electrochemical capacitors, these materials can considerably improve the ion transfer rate and electronic conductivity, thereby enhancing the specific capacitance while maintaining the structural stability. Also, it was observed that these materials could occasionally outperform standard platinum-based catalysts for the electrochemical oxygen reduction reaction (ORR). The reported electrochemical performances and structural parameters of these materials were carefully tabulated in uniform units and scales. Through a critical analysis of the present synthesis trends, characteristics, and functionalities of these materials, specific aspects were identified that required further exploration to fully utilize their inherent capabilities. Full article
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15 pages, 2546 KiB  
Article
Impact of Mixing Shear on Polymer Binder Molecular Weight and Battery Electrode Reproducibility
by Samantha L. Morelly, Renee M. Saraka, Nicolas J. Alvarez and Maureen Tang
Batteries 2024, 10(2), 46; https://doi.org/10.3390/batteries10020046 - 27 Jan 2024
Viewed by 1573
Abstract
The viscosity and microstructure of Li-ion battery slurries and the performance of the resulting electrodes have been shown to depend on the mixing protocol. This work applies rheology to understand the impact of shear during mixing and polymer molecular weight on slurry microstructure [...] Read more.
The viscosity and microstructure of Li-ion battery slurries and the performance of the resulting electrodes have been shown to depend on the mixing protocol. This work applies rheology to understand the impact of shear during mixing and polymer molecular weight on slurry microstructure and electrode performance. Mixing protocols of different shear intensity are applied to slurries of LiNi0.33Mn0.33Co0.33O2 (NMC), carbon black (CB), and polyvinyldiene difluoride (PVDF) in N-methyl-2-pyrrolidinone (NMP), using both high-molecular-weight (HMW) and low-molecular-weight (LMW) PVDF. Slurries of both polymers are observed to form colloidal gels under high-shear mixing, even though unfavorable interactions between high molecular weight PVDF and CB should prevent this microstructure from forming. Theoretical analysis and experimental results show that increasing shear rate during the polymer and particle mixing steps causes polymer scission to decrease the polymer molecular weight and allow colloidal gelation. In general, electrodes made from high molecular weight PVDF generally show increased rate capability. However, high shear rates lead to increased cell variability, possibly due to the heterogeneities introduced by polymer scission. Full article
(This article belongs to the Special Issue Design and Processing for High Performance Li-Ion Battery Electrodes)
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26 pages, 5200 KiB  
Review
Recent Progress of Urea-Based Deep Eutectic Solvents as Electrolytes in Battery Technology: A Critical Review
by Mohamed Ammar, Sherif Ashraf, Diego Alexander Gonzalez-casamachin, Damilola Tomi Awotoye and Jonas Baltrusaitis
Batteries 2024, 10(2), 45; https://doi.org/10.3390/batteries10020045 - 27 Jan 2024
Cited by 1 | Viewed by 1977
Abstract
Urea, a basic chemical compound, holds diverse applications across numerous domains, ranging from agriculture to energy storage. Of particular interest is its role as a hydrogen bond donor (HBD). This specific characteristic has propelled its utilization as an essential component in crafting deep [...] Read more.
Urea, a basic chemical compound, holds diverse applications across numerous domains, ranging from agriculture to energy storage. Of particular interest is its role as a hydrogen bond donor (HBD). This specific characteristic has propelled its utilization as an essential component in crafting deep eutectic solvents (DESs) for battery electrolytes. Incorporating urea into DESs presents a promising avenue to address environmental concerns associated with traditional electrolytes, thereby advancing battery technology. Conventional electrolytes, often composed of hazardous and combustible solvents, pose significant environmental risks upon improper disposal potentially contaminating soil and water and threatening both human health and ecosystems. Consequently, there is a pressing need for eco-friendly alternatives capable of upholding high performance and safety standards. DESs, categorized as organic salts resulting from the blending of two or more compounds, have emerged as promising contenders for the next generation of electrolytes. Urea stands out among DES electrolytes by enhancing ion transport, widening the electrochemical window stability (ESW), and prolonging battery cycle life. Further, its non-toxic nature, limited flammability, and elevated thermal stability play pivotal roles in mitigating environmental concerns and safety issues associated with traditional electrolytes. Laboratory testing of urea-based DES electrolytes across various battery systems, including Al-ion, Na-ion, and Zn-ion batteries, has already been demonstrated. This review examines the evolution of urea-based DES electrolytes by elucidating their structure, molecular interaction mechanisms, performance attributes, and preparation methodologies. Full article
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13 pages, 5344 KiB  
Article
Effect of Partial Cation Replacement on Anode Performance of Sodium-Ion Batteries
by Shijiang He, Zidong Wang, Wenbo Qiu, Huaping Zhao and Yong Lei
Batteries 2024, 10(2), 44; https://doi.org/10.3390/batteries10020044 - 26 Jan 2024
Viewed by 1560
Abstract
Due to their high specific capacity and long cycle life, bimetallic sulfides are the preferred choice of researchers as anodes in sodium-ion batteries (SIBs). However, studies indicate that this class of materials often requires expensive elements such as Co, Sb, Sn, etc., and [...] Read more.
Due to their high specific capacity and long cycle life, bimetallic sulfides are the preferred choice of researchers as anodes in sodium-ion batteries (SIBs). However, studies indicate that this class of materials often requires expensive elements such as Co, Sb, Sn, etc., and their performance is insufficient with the use of inexpensive Fe, V alone. Therefore, there is a need to explore the relationship between metal cations and anode performance so that the requirements of cost reduction and performance enhancement can be met simultaneously. In this work, a series of partially replaced sulfides with different cation ratios have been prepared by a hydrothermal method followed by heat treatment. By partially replacing Co in NiCo sulfides, all samples show improved capacity and stability over the original NiCo sulfides. As a result, the metal elements have different oxidation states, which leads to a higher capacity through their synergistic effects on each other. Mn-NiCoS with 10% replacement showed satisfactory capacity (721.09 mAh g−1 at 300 mA g−1, 662.58 mAh g−1 after 20 cycles) and excellent cycle life (85.41% capacity retention after 1000 cycles at 2000 mA g−1). Full article
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29 pages, 13112 KiB  
Article
Comparative Analysis of Energy Storage and Buffer Units for Electric Military Vehicle: Survey of Experimental Results
by Ngoc Nam Pham, Radim Bloudicek, Jan Leuchter, Stanislav Rydlo and Quang Huy Dong
Batteries 2024, 10(2), 43; https://doi.org/10.3390/batteries10020043 - 23 Jan 2024
Viewed by 1822
Abstract
This paper deals with the analyses of batteries used in current military systems to power the electric drives of military vehicles. The article focuses on battery analyses based on operational data obtained from measurements rather than analyses of the chemical composition of the [...] Read more.
This paper deals with the analyses of batteries used in current military systems to power the electric drives of military vehicles. The article focuses on battery analyses based on operational data obtained from measurements rather than analyses of the chemical composition of the tested batteries. The authors of the article used their experience from the development test-laboratory of military technology. This article presents a comparative analysis of existing and promising technologies in the field of energy storage and buffering for military electric vehicles. The overview of these technologies, including the design, operating principles, advantages, and disadvantages, are briefly presented to produce theoretical comparative analyses. However, this article mainly focuses on the experimental verification of operational ability in varied conditions, as well as the comparison and analysis of these results. The main part of the article provides more experimental studies on technologies of energy storage and buffering using the results of several experiments conducted to demonstrate the behavior of each technology in different working conditions. The output parameters, as well as the state of charge of each technology’s samples, were surveyed in various temperatures and loading characteristics. The results presented in this paper are expected to be useful for optimizing the selection of energy storage and buffering solutions for military electric vehicles in different applications and functional environments. Full article
(This article belongs to the Section Battery Modelling, Simulation, Management and Application)
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20 pages, 15224 KiB  
Article
Lithium-Ion Supercapacitors and Batteries for Off-Grid PV Applications: Lifetime and Sizing
by Tarek Ibrahim, Tamas Kerekes, Dezso Sera, Abderezak Lashab and Daniel-Ioan Stroe
Batteries 2024, 10(2), 42; https://doi.org/10.3390/batteries10020042 - 23 Jan 2024
Cited by 1 | Viewed by 1702
Abstract
The intermittent nature of power generation from photovoltaics (PV) requires reliable energy storage solutions. Using the storage system outdoors exposes it to variable temperatures, affecting both its storage capacity and lifespan. Utilizing and optimizing energy storage considering climatic variations and new storage technologies [...] Read more.
The intermittent nature of power generation from photovoltaics (PV) requires reliable energy storage solutions. Using the storage system outdoors exposes it to variable temperatures, affecting both its storage capacity and lifespan. Utilizing and optimizing energy storage considering climatic variations and new storage technologies is still a research gap. Therefore, this paper presents a modified sizing algorithm based on the Golden Section Search method, aimed at optimizing the number of cells in an energy storage unit, with a specific focus on the unique conditions of Denmark. The considered energy storage solutions are Lithium-ion capacitors (LiCs) and Lithium-ion batteries (LiBs), which are tested under different temperatures and C-rates rates. The algorithm aims to maximize the number of autonomy cycles—defined as periods during which the system operates independently of the grid, marked by intervals between two consecutive 0% State of Charge (SoC) occurrences. Testing scenarios include dynamic temperature and dynamic load, constant temperature at 25 °C, and constant load, considering irradiation and temperature effects and cell capacity fading over a decade. A comparative analysis reveals that, on average, the LiC storage is sized at 70–80% of the LiB storage across various scenarios. Notably, under a constant-temperature scenario, the degradation rate accelerates, particularly for LiBs. By leveraging the modified Golden Section Search algorithm, this study provides an efficient approach to the sizing problem, optimizing the number of cells and thus offering a potential solution for energy storage in off-grid PV systems. Full article
(This article belongs to the Special Issue Advances in Battery Status Estimation and Prediction)
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12 pages, 2965 KiB  
Article
Monitoring of Thermal Runaway in Commercial Prismatic High-Energy Lithium-Ion Battery Cells via Internal Temperature Sensing
by Niklas Kisseler, Fabian Hoheisel, Christian Offermanns, Moritz Frieges, Heiner Heimes and Achim Kampker
Batteries 2024, 10(2), 41; https://doi.org/10.3390/batteries10020041 - 23 Jan 2024
Viewed by 2268
Abstract
The temperature of a lithium-ion battery is a crucial parameter for understanding the internal processes during various operating and failure scenarios, including thermal runaway. However, the internal temperature is comparatively higher than the surface temperature. This particularly affects cells with a large cross-section, [...] Read more.
The temperature of a lithium-ion battery is a crucial parameter for understanding the internal processes during various operating and failure scenarios, including thermal runaway. However, the internal temperature is comparatively higher than the surface temperature. This particularly affects cells with a large cross-section, which is due to heat development within the cell and lower heat dissipation due to a poorer ratio of volume to surface area. This paper presents an approach that enables real-time monitoring of the behavior of a commercial prismatic high-energy battery cell (NMC811/C, 95 Ah, Contemporary Amperex Technology Co., Limited (Ningde, China)) in the event of thermal runaway induced by overcharging. The internal cell temperature is investigated by the subsequent integration of two hard sensors between the two jelly rolls and additional sensors on the surface of the aluminum housing of the battery cell. The sensor’s signals show a significant increase in the temperature gradient between the temperature in the core of the cell and the cell casing surface until the onset of venting and thermal runaway of the battery. The data enable a detailed investigation of the behavior of the battery cell and the comparatively earlier detection of the point of no return in the event of thermal runaway. Full article
(This article belongs to the Special Issue Thermal Safety of Lithium Ion Batteries)
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18 pages, 4251 KiB  
Article
Spherical Graphite Anodes: Influence of Particle Size Distribution and Multilayer Structuring in Lithium-Ion Battery Cells
by Laura Gottschalk, Jannes Müller, Alexander Schoo, Ernesto Baasch and Arno Kwade
Batteries 2024, 10(2), 40; https://doi.org/10.3390/batteries10020040 - 23 Jan 2024
Viewed by 2358
Abstract
Current research focuses on lithium-ion battery cells with a high energy density and efficient fast-charging capabilities. However, transport limitations, and, therefore, the uniform diffusion of lithium-ions across the electrode layers, remain a challenge and could lead to reduced cell performance. One approach to [...] Read more.
Current research focuses on lithium-ion battery cells with a high energy density and efficient fast-charging capabilities. However, transport limitations, and, therefore, the uniform diffusion of lithium-ions across the electrode layers, remain a challenge and could lead to reduced cell performance. One approach to overcome these transport challenges is the use of subsequently produced two-layer anodes with the particle size variation of spherical graphite (x50 = 18 µm; x50 = 11 µm). Thereby, a defined pore network is created, which reduces the ionic resistance and ensuring improved fast charging capabilities. The analysis focuses on the evaluation of electrode properties and the electrochemical performance. By examining the pore size distribution of the anodes, it has been found that during the manufacturing of the two-layer anodes, carbon black and binder particles are transported into the existing microstructure of the lower layer, resulting in localized densification between the anode layers. This could also be supported by color measurements. This effect also extends to electrochemical investigations, with electrochemical impedance spectroscopy showing significantly lower ionic resistances in all two-layer anodes. Reduced ionic resistance and tortuosity near the separator due to absorption effects enhance the ion diffusion and have a direct impact on anode performance. Cell ageing analysis showed a significant capacity decrease of almost 15 mAh g −1 in the single-layer references only, in contrast to the stability of the two-layer anodes. This could also be attributed to the reduced ionic resistance and active counteraction of binder migration. In conclusion, this study highlights how subsequently produced two-layer anodes significantly shape the electrode properties and cell performance of lithium-ion batteries. Full article
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