Batteries

19 pages, 7765 KiB

Open AccessEditor’s ChoiceArticle

High-Precision and Robust SOC Estimation of LiFePO₄ Blade Batteries Based on the BPNN-EKF Algorithm

by Zhihang Zhang, Siliang Chen, Languang Lu, Xuebing Han, Yalun Li, Siqi Chen, Hewu Wang, Yubo Lian and Minggao Ouyang

Batteries 2023, 9(6), 333; https://doi.org/10.3390/batteries9060333 - 20 Jun 2023

Cited by 2 | Viewed by 1937

Abstract

The lithium iron phosphate (LiFePO₄) blade battery is a long, rectangular-shaped cell that can be directly integrated into battery pack systems. It enhances volumetric power density, significantly reduces costs, and is widely utilized in electric vehicles. However, the flat open circuit [...] Read more.

The lithium iron phosphate (LiFePO₄) blade battery is a long, rectangular-shaped cell that can be directly integrated into battery pack systems. It enhances volumetric power density, significantly reduces costs, and is widely utilized in electric vehicles. However, the flat open circuit voltage and significant polarization differences under wide operational temperatures are challenging for accurate voltage modeling of battery management systems (BMSs). In particular, inaccurate state of charge (SOC) estimation may cause overcharging and over-discharging risks. To accurately perceive the SOC of LiFePO₄ blade batteries, a SOC estimation method based on the backpropagation neural network-extended Kalman filter (BPNN-EKF) algorithm is proposed. BPNN is a neural network model that utilizes the backpropagation algorithm to update model parameters, while EKF is an optimal estimation algorithm. Firstly, dynamic working condition tests, including the New European Driving Cycle (NEDC) and high-speed working (HSW) condition tests, are conducted under a wide temperature range (−25–43 °C). HSW conditions refer to a simulated operating condition that mimics the driving of an electric vehicle on a highway. The minimum voltage of the battery system is used as the output for training the BPNN model. We derive the Kalman gain by combining the BPNN output voltage. Additionally, the EKF algorithm is employed to correct the SOC value using voltage error information. Concerning long SOC calculation intervals, capacity errors, initial SOC errors, and current and voltage sampling errors, the maximum SOC estimation RMSE is 3.98% at −20 °C NEDC, 3.62% at 10 °C NEDC, and 1.68% at 35 °C HSW. The proposed algorithm can be applied to different temperatures and operations, demonstrating high robustness. This BPNN-EKF algorithm has the potential to be embedded in electric vehicle BMS systems for practical applications. Full article

(This article belongs to the Special Issue Battery Energy Storage in Advanced Power Systems)

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13 pages, 4406 KiB

Open AccessEditor’s ChoiceArticle

Modeling Anisotropic Transport in Polycrystalline Battery Materials

by Simon Daubner, Marcel Weichel, Paul W. Hoffrogge, Daniel Schneider and Britta Nestler

Batteries 2023, 9(6), 310; https://doi.org/10.3390/batteries9060310 - 05 Jun 2023

Cited by 1 | Viewed by 1885

Abstract

Hierarchical structures of many agglomerated primary crystals are often employed as cathode materials, especially for layered-oxide compounds. The anisotropic nature of these materials results in a strong correlation between particle morphology and ion transport. In this work, we present a multiphase-field framework that [...] Read more.

Hierarchical structures of many agglomerated primary crystals are often employed as cathode materials, especially for layered-oxide compounds. The anisotropic nature of these materials results in a strong correlation between particle morphology and ion transport. In this work, we present a multiphase-field framework that is able to account for strongly anisotropic diffusion in polycrystalline materials. Various secondary particle structures with random grain orientation as well as strongly textured samples are investigated. The observed ion distributions match well with the experimental observations. Furthermore, we show how these simulations can be used to mimic potentiostatic intermittent titration technique (PITT) measurements and compute effective diffusion coefficients for secondary particles. The results unravel the intrinsic relation between particle microstructure and the apparent diffusivity. Consequently, the modeling framework can be employed to guide the microstructure design of secondary battery particles. Furthermore, the phase-field method closes the gap between computation of diffusivities on the atomistic scale and the effective properties of secondary particles, which are a necessary input for Newman-type cell models. Full article

(This article belongs to the Special Issue Materials Design for Electrochemical Energy Storage)

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20 pages, 1400 KiB

Open AccessEditor’s ChoiceArticle

Maximizing Efficiency in Smart Adjustable DC Link Powertrains with IGBTs and SiC MOSFETs via Optimized DC-Link Voltage Control

by Yu Xu, Anton Kersten, Simon Klacar and David Sedarsky

Batteries 2023, 9(6), 302; https://doi.org/10.3390/batteries9060302 - 31 May 2023

Cited by 4 | Viewed by 1766

Abstract

In recent years, the push towards electrifying transportation has gained significant traction, with battery-electric vehicles (BEVs) emerging as a viable alternative. However, the widespread adoption of BEVs faces multiple challenges, such as limited driving range, making powertrain efficiency improvements crucial. One approach to [...] Read more.

In recent years, the push towards electrifying transportation has gained significant traction, with battery-electric vehicles (BEVs) emerging as a viable alternative. However, the widespread adoption of BEVs faces multiple challenges, such as limited driving range, making powertrain efficiency improvements crucial. One approach to improve powertrain energy efficiency is to adjust the DC-link voltage using a DC-DC converter between the battery and inverter. Here, it is necessary to address the losses introduced by the DC-DC converter. This paper presents a dynamic programming approach to optimize the DC-link voltage, taking into account the battery terminal voltage variation and its impact on the overall powertrain losses. We also examine the energy efficiency gains of IGBT-based and silicon carbide (SiC) MOSFET-based adjustable DC-link voltage powertrains during WLTC driving cycles through PLECS and Matlab/Simulink simulations. The findings indicate that both IGBT and MOSFET-based adjustable DC-link voltage powertrains can enhance the WLTC drive-cycle efficiency up to

2.51 %

and

3.25 %

compared to conventional IGBT and MOSFET-based powertrains, respectively. Full article

(This article belongs to the Special Issue Future Smart Battery Management Systems)

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19 pages, 5478 KiB

Open AccessEditor’s ChoiceArticle

Hybrid Modeling of Lithium-Ion Battery: Physics-Informed Neural Network for Battery State Estimation

by Soumya Singh, Yvonne Eboumbou Ebongue, Shahed Rezaei and Kai Peter Birke

Batteries 2023, 9(6), 301; https://doi.org/10.3390/batteries9060301 - 30 May 2023

Cited by 8 | Viewed by 5329

Abstract

Accurate forecasting of the lifetime and degradation mechanisms of lithium-ion batteries is crucial for their optimization, management, and safety while preventing latent failures. However, the typical state estimations are challenging due to complex and dynamic cell parameters and wide variations in usage conditions. [...] Read more.

Accurate forecasting of the lifetime and degradation mechanisms of lithium-ion batteries is crucial for their optimization, management, and safety while preventing latent failures. However, the typical state estimations are challenging due to complex and dynamic cell parameters and wide variations in usage conditions. Physics-based models need a tradeoff between accuracy and complexity due to vast parameter requirements, while machine-learning models require large training datasets and may fail when generalized to unseen scenarios. To address this issue, this paper aims to integrate the physics-based battery model and the machine learning model to leverage their respective strengths. This is achieved by applying the deep learning framework called physics-informed neural networks (PINN) to electrochemical battery modeling. The state of charge and state of health of lithium-ion cells are predicted by integrating the partial differential equation of Fick’s law of diffusion from a single particle model into the neural network training process. The results indicate that PINN can estimate the state of charge with a root mean square error in the range of 0.014% to 0.2%, while the state of health has a range of 1.1% to 2.3%, even with limited training data. Compared to conventional approaches, PINN is less complex while still incorporating the laws of physics into the training process, resulting in adequate predictions, even for unseen situations. Full article

(This article belongs to the Special Issue The Precise Battery—towards Digital Twins for Advanced Batteries)

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20 pages, 5215 KiB

Open AccessEditor’s ChoiceArticle

A Plating-Free Charging Scheme for Battery Module Based on Anode Potential Estimation to Prevent Lithium Plating

by Yaxing Ren, Dhammika Widanage and James Marco

Batteries 2023, 9(6), 294; https://doi.org/10.3390/batteries9060294 - 27 May 2023

Cited by 1 | Viewed by 1474

Abstract

Since fast charging schemes for lithium-ion batteries are known to lead to a reduction in battery capacity, there is a need to avoid lithium plating during the charging process. This paper designed an anode potential observer and a plating-free charging scheme for a [...] Read more.

Since fast charging schemes for lithium-ion batteries are known to lead to a reduction in battery capacity, there is a need to avoid lithium plating during the charging process. This paper designed an anode potential observer and a plating-free charging scheme for a battery module to avoid the risk of lithium plating for all cells in the module. The observer was designed using an electrochemical cell model and an electrical busbar model to estimate the anode potential of all cells within a parallel connected battery module. Due to its simplicity and low computational loads, the observer was easy to implement in a charge management system. The results demonstrated that the designed observer and charging scheme can accurately estimate the anode potential of all cells in the module. The estimation results of the observer were used in the plating-free charging scheme. Compared to conventional charging methods, the proposed scheme added an additional stage to estimate and control the anode potential, therefore reducing the risk of lithium plating during charging. It also reduced the peak temperature of the battery by approximately 9.8% and reduced the overall charging time by 18%. Full article

(This article belongs to the Section Battery Modelling, Simulation, Management and Application)

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20 pages, 6699 KiB

Open AccessEditor’s ChoiceArticle

Dynamic Charge Acceptance Compared to Electrochemical Impedance Spectroscopy Parameters: Dependencies on Additives, State of Charge, and Prior Usage

by Sophia Bauknecht, Julia Kowal, Jochen Settelein, Markus Föhlisch and Eckhard Karden

Batteries 2023, 9(5), 263; https://doi.org/10.3390/batteries9050263 - 08 May 2023

Cited by 1 | Viewed by 1678

Abstract

The goal of this work was to predict the dynamic charge acceptance (DCA) for cells using different additives on the negative electrode from the evaluation of small-signal measurements by electrochemical impedance spectroscopy (EIS). Thereby, various operating points were evaluated, such as state of [...] Read more.

The goal of this work was to predict the dynamic charge acceptance (DCA) for cells using different additives on the negative electrode from the evaluation of small-signal measurements by electrochemical impedance spectroscopy (EIS). Thereby, various operating points were evaluated, such as state of charge (SoC) and prior usage (charge or discharge). The 2V test cells under investigation utilized plates of enhanced flooded 3P2N battery cells (EFB). They contained three positive and two negative electrodes. The latter varied in their additive composition. In total, eight different negative electrodes were investigated, five including specially synthesized amorphous carbon as an additive, two with unknown additive mixes, and one including a commercially available carbon black. The best parameters for predicting the DCA were found within the first semicircle of the negative half-cell spectra measured during a superimposed charging current. Full article

(This article belongs to the Section Battery Mechanisms and Fundamental Electrochemistry Aspects)

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17 pages, 3781 KiB

Open AccessEditor’s ChoiceArticle

Sustainable Approach for the Development of TiO₂-Based 3D Electrodes for Microsupercapacitors

by Nathalie Poirot, Marie Gabard, Mohamed Boufnichel, Rachelle Omnée and Encarnacion Raymundo-Piñero

Batteries 2023, 9(5), 258; https://doi.org/10.3390/batteries9050258 - 29 Apr 2023

Viewed by 1502

Abstract

This study reports a sustainable approach for developing electrodes for microsupercapacitors. This approach includes the synthesis of TiO₂ nanoparticles via a green sol–gel method and the deposition of thin films of that electrochemically active material on three-dimensional (3D) Si substrates with a [...] Read more.

This study reports a sustainable approach for developing electrodes for microsupercapacitors. This approach includes the synthesis of TiO₂ nanoparticles via a green sol–gel method and the deposition of thin films of that electrochemically active material on three-dimensional (3D) Si substrates with a high area enlargement factor (AEF) via a simple, fast, and inexpensive spin-coating pathway. The thickness of the film was first optimized via its deposition over two-dimensional (2D) substrates to achieve high capacitances to provide high energy density but also to deliver a good rate capability to ensure the power density required for a supercapacitor device. A film thickness of ~120 nm realizes the best compromise between the electronic/ionic conductivity and capacitance in a supercapacitor device. Such layers of TiO₂ were successfully coated onto 3D microstructured substrates with different architectures, such as trenches and pillars, and different aspect ratios. The spin-coating-based route developed here has been established to be superior as, on the one hand, a conformal deposition can be achieved over high AEF subtracts, and on the other hand, the 3D electrodes present higher surface capacitances than those obtained using other deposition techniques. The rate capability and appreciable cyclability ensure a reliable supercapacitor behavior. Full article

(This article belongs to the Special Issue High-Performance and Sustainable Supercapacitors: Current Status and Perspective)

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36 pages, 5081 KiB

Open AccessEditor’s ChoiceReview

Lithium Niobate for Fast Cycling in Li-ion Batteries: Review and New Experimental Results

by Erwin Hüger, Lukas Riedel, Jing Zhu, Jochen Stahn, Paul Heitjans and Harald Schmidt

Batteries 2023, 9(5), 244; https://doi.org/10.3390/batteries9050244 - 25 Apr 2023

Cited by 8 | Viewed by 3639

Abstract

Li-Nb-O-based insertion layers between electrodes and electrolytes of Li-ion batteries (LIBs) are known to protect the electrodes and electrolytes from unwanted reactions and to enhance Li transport across interfaces. An improved operation of LIBs, including all-solid-state LIBs, is reached with Li-Nb-O-based insertion layers. [...] Read more.

Li-Nb-O-based insertion layers between electrodes and electrolytes of Li-ion batteries (LIBs) are known to protect the electrodes and electrolytes from unwanted reactions and to enhance Li transport across interfaces. An improved operation of LIBs, including all-solid-state LIBs, is reached with Li-Nb-O-based insertion layers. This work reviews the suitability of polymorphic Li-Nb-O-based compounds (e.g., crystalline, amorphous, and mesoporous bulk materials and films produced by various methodologies) for LIB operation. The literature survey on the benefits of niobium-oxide-based materials for LIBs, and additional experimental results obtained from neutron scattering and electrochemical experiments on amorphous LiNbO₃ films are the focus of the present work. Neutron reflectometry reveals a higher porosity in ion-beam sputtered amorphous LiNbO₃ films (22% free volume) than in other metal oxide films such as amorphous LiAlO₂ (8% free volume). The higher porosity explains the higher Li diffusivity reported in the literature for amorphous LiNbO₃ films compared to other similar Li-metal oxides. The higher porosity is interpreted to be the reason for the better suitability of LiNbO₃ compared to other metal oxides for improved LIB operation. New results are presented on gravimetric and volumetric capacity, potential-resolved Li⁺ uptake and release, pseudo-capacitive fractions, and Li diffusivities determined electrochemically during long-term cycling of LiNbO₃ film electrodes with thicknesses between 14 and 150 nm. The films allow long-term cycling even for fast cycling with rates of 240C possessing reversible capacities as high as 600 mAhg⁻¹. Electrochemical impedance spectroscopy (EIS) shows that the film atomic network is stable during cycling. The Li diffusivity estimated from the rate capability experiments is considerably lower than that obtained by EIS but coincides with that from secondary ion mass spectrometry. The mostly pseudo-capacitive behavior of the LiNbO₃ films explains their ability of fast cycling. The results anticipate that amorphous LiNbO₃ layers also contribute to the capacity of positive (LiNi_xMn_yCo_zO₂, NMC) and negative LIB electrode materials such as carbon and silicon. As an outlook, in addition to surface-engineering, the bulk-engineering of LIB electrodes may be possible with amorphous and porous LiNbO₃ for fast cycling with high reversible capacity. Full article

(This article belongs to the Section Battery Materials and Interfaces: Anode, Cathode, Separators and Electrolytes or Others)

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31 pages, 7355 KiB

Open AccessEditor’s ChoiceArticle

Thermal and Mechanical Safety Assessment of Type 21700 Lithium-Ion Batteries with NMC, NCA and LFP Cathodes–Investigation of Cell Abuse by Means of Accelerating Rate Calorimetry (ARC)

by Sebastian Ohneseit, Philipp Finster, Claire Floras, Niklas Lubenau, Nils Uhlmann, Hans Jürgen Seifert and Carlos Ziebert

Batteries 2023, 9(5), 237; https://doi.org/10.3390/batteries9050237 - 22 Apr 2023

Cited by 9 | Viewed by 4982

Abstract

In this experimental investigation, we studied the safety and thermal runaway behavior of commercial lithium-ion batteries of type 21700. The different cathode materials NMC, NCA and LFP were compared, as well as high power and high energy cells. After characterization of all relevant [...] Read more.

In this experimental investigation, we studied the safety and thermal runaway behavior of commercial lithium-ion batteries of type 21700. The different cathode materials NMC, NCA and LFP were compared, as well as high power and high energy cells. After characterization of all relevant components of the batteries to assure comparability, two abuse methods were applied: thermal abuse by the heat-wait-seek test and mechanical abuse by nail penetration, both in an accelerating rate calorimeter. Several critical temperatures and temperature rates, as well as exothermal data, were determined. Furthermore, the grade of destruction, mass loss and, for the thermal abuse scenario, activation energy and enthalpy, were calculated for critical points. It was found that NMC cells reacted first, but NCA cells went into thermal runaway a little earlier than NMC cells. LFP cells reacted, as expected, more slowly and at significantly higher temperatures, making the cell chemistry considerably safer. For mechanical abuse, no thermal runaway was observed for LFP cells, as well as at state of charge (SOC) zero for the other chemistries tested. For thermal abuse, at SOC 0 and SOC 30 for LFP cells and at SOC 0 for the other cell chemistries, no thermal runaway occurred until 350 °C. In this study, the experimental data are provided for further simulation approaches and system safety design. Full article

(This article belongs to the Special Issue Materials Design for Electrochemical Energy Storage)

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13 pages, 1218 KiB

Open AccessEditor’s ChoiceArticle

How Cell Design Affects the Aging Behavior: Comparing Electrode-Individual Aging Processes of High-Energy and High-Power Lithium-Ion Batteries Using High Precision Coulometry

by Sebastian Michael Peter Jagfeld, Kai Peter Birke, Alexander Fill and Peter Keil

Batteries 2023, 9(4), 232; https://doi.org/10.3390/batteries9040232 - 18 Apr 2023

Cited by 2 | Viewed by 1760

Abstract

The aging behavior of lithium-ion batteries is crucial for the development of electric vehicles and many other battery-powered devices. The cells can be generally classified into two types: high-energy (HE) and high-power (HP) cells. The cell type used depends on the field of [...] Read more.

The aging behavior of lithium-ion batteries is crucial for the development of electric vehicles and many other battery-powered devices. The cells can be generally classified into two types: high-energy (HE) and high-power (HP) cells. The cell type used depends on the field of application. As these cells differ in their electrical behavior, this work investigates whether both cell types also show different aging behavior. More precisely, the occurring capacity loss and internal side reactions are analyzed via the charge throughput. For comparison, aging tests are carried out with a high-precision battery tester, allowing the application of High Precision Coulometry (HPC). This enables early detection of aging effects and also allows us to break down the capacity loss into electrode-individual processes. A total of two sub-studies are performed: (1) a cyclic study focusing on lithium plating; and (2) an accelerated calendar aging study. It is found that HE cells exhibit stronger cyclic aging effects (lithium plating) and HP cells exhibit stronger calendar aging effects. The higher lithium plating can be explained by the higher diffusion resistance of the lithium ions within the electrodes of HE Cell. The higher calendar aging fits to the larger electrode surfaces of the HP cell. These results give deep insights into the proceeding aging in a novel way and are interesting for the selection of the appropriate cell type in the context of battery development. In a next step, the measured capacity losses could also be used for a simple parameterization of battery aging models. Full article

(This article belongs to the Special Issue The Precise Battery—towards Digital Twins for Advanced Batteries)

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18 pages, 4124 KiB

Open AccessEditor’s ChoiceArticle

Experimental Investigation on Reversible Swelling Mechanisms of Lithium-Ion Batteries under a Varying Preload Force

by Emanuele Michelini, Patrick Höschele, Simon Franz Heindl, Simon Erker and Christian Ellersdorfer

Batteries 2023, 9(4), 218; https://doi.org/10.3390/batteries9040218 - 04 Apr 2023

Cited by 8 | Viewed by 4157

Abstract

The safety of lithium-ion batteries has to be guaranteed over the complete lifetime considering geometry changes caused by reversible and irreversible swellings and degradation mechanisms. An understanding of the pressure distribution and gradients is necessary to optimize battery modules and avoid local degradation [...] Read more.

The safety of lithium-ion batteries has to be guaranteed over the complete lifetime considering geometry changes caused by reversible and irreversible swellings and degradation mechanisms. An understanding of the pressure distribution and gradients is necessary to optimize battery modules and avoid local degradation bearing the risk of safety-relevant battery changes. In this study, the pressure distribution of two fresh lithium-ion pouch cells was measured with an initial preload force of 300 or 4000

N

. Four identical cells were electrochemically aged with a 300 or 4000

N

preload force. The irreversible thickness change was measured during aging. After aging, the reversible swelling behavior was investigated to draw conclusions on how the pressure distribution affected the aging behavior. A novel test setup was developed to measure the local cell thickness without contact and with high precision. The results suggested that the applied preload force affected the pressure distribution and pressure gradients on the cell surface. The pressure gradients were found to affect the locality of the irreversible swelling. Positions suffering from large pressure variations and gradients increased strongly in thickness and were affected in terms of their reversible swelling behavior. In particular, the edges of the investigated cells showed a strong thickness increase caused by pressure peaks. Full article

(This article belongs to the Special Issue Battery Safety: Recent Advances and Perspective)

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20 pages, 3464 KiB

Open AccessEditor’s ChoiceArticle

Tragacanth, an Exudate Gum as Suitable Aqueous Binder for High Voltage Cathode Material

by Daniele Versaci, Oana D. Apostu, Davide Dessantis, Julia Amici, Carlotta Francia, Marco Minella and Silvia Bodoardo

Batteries 2023, 9(4), 199; https://doi.org/10.3390/batteries9040199 - 28 Mar 2023

Cited by 3 | Viewed by 1782

Abstract

The improvements in future-generation lithium-ion batteries cannot be exclusively focused on the performance. Other aspects, such as costs, processes, and environmental sustainability, must be considered. Research and development of new active materials allow some fundamental aspects of the batteries to be increased, such [...] Read more.

The improvements in future-generation lithium-ion batteries cannot be exclusively focused on the performance. Other aspects, such as costs, processes, and environmental sustainability, must be considered. Research and development of new active materials allow some fundamental aspects of the batteries to be increased, such as power and energy density. However, one of the main future challenges is the improvement of the batteries’ electrochemical performance by using “non-active” materials (binder, current collector, separators) with a lower cost, lower environmental impact, and easier recycling procedure. Focusing on the binder, the main goal is to replace the current fluorinated compounds with water-soluble materials. Starting from these considerations, in this study we evaluate, for the first time, tragacanth gum (TG) as a suitable aqueous binder for the manufacturing process of a cobalt-free, high-voltage lithium nickel manganese oxide (LNMO) cathode. TG-based LNMO cathodes with a low binder content (3 wt%) exhibited good thermal and mechanical properties, showing remarkably high cycling stability with 60% capacity retention after more than 500 cycles at 1 C and an outstanding rate capability of 72 mAh g⁻¹ at 15 C. In addition to the excellent electrochemical features, tragacanth gum also showed excellent recycling and recovery properties, making this polysaccharide a suitable and sustainable binder for next-generation lithium-ion batteries. Full article

(This article belongs to the Special Issue Green and Sustainable Materials for Li-Ion Batteries)

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19 pages, 6987 KiB

Open AccessEditor’s ChoiceArticle

Thermal Modelling and Simulation Studies of Containerised Vanadium Flow Battery Systems

by Bing Shu, Logan S. Weber, Maria Skyllas-Kazacos, Jie Bao and Ke Meng

Batteries 2023, 9(4), 196; https://doi.org/10.3390/batteries9040196 - 24 Mar 2023

Cited by 1 | Viewed by 1646

Abstract

With increasing commercial applications of vanadium flow batteries (VFB), containerised VFB systems are gaining attention as they can be mass produced and easily transported and configured for different energy storage applications. However, there are limited studies on the thermodynamic modelling of containerised vanadium [...] Read more.

With increasing commercial applications of vanadium flow batteries (VFB), containerised VFB systems are gaining attention as they can be mass produced and easily transported and configured for different energy storage applications. However, there are limited studies on the thermodynamic modelling of containerised vanadium redox flow battery systems, and thermal control designs. In this paper, a dynamic thermal model is developed for containerised VFB systems, based on which thermal design options are evaluated using simulation studies. Full article

(This article belongs to the Special Issue Feature Papers to Celebrate the First Impact Factor of Batteries)

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14 pages, 3783 KiB

Open AccessEditor’s ChoiceArticle

Optimisation of Industrially Relevant Electrode Formulations for LFP Cathodes in Lithium Ion Cells

by Geanina Apachitei, Marc Hidalgo, Daniela Dogaru, Michael Lain, Robert Heymer, James Marco and Mark Copley

Batteries 2023, 9(4), 192; https://doi.org/10.3390/batteries9040192 - 23 Mar 2023

Cited by 4 | Viewed by 3700

Abstract

The electrode formulation has a significant effect on the performance of lithium ion cells. The active material, binder, and conductive carbon all have different roles, and finding the optimum composition can be difficult using an iterative approach. In this study, a design of [...] Read more.

The electrode formulation has a significant effect on the performance of lithium ion cells. The active material, binder, and conductive carbon all have different roles, and finding the optimum composition can be difficult using an iterative approach. In this study, a design of experiment (DoE) methodology is applied to the optimisation of a cathode based on lithium iron phosphate (LFP). The minimum LFP content in the electrodes is 94 wt%. Seventeen mixes are used to evaluate adhesion, resistivity, and electrochemical performance. The coating adhesion increases with binder content, and the coating conductivity increases with carbon nano-tube content. The best coatings achieve 5C:0.2C capacity ratios above 50%, despite the relatively high coat weight. Models based on just the component mixture do not replicate the discharge capacities at high rates. However, a combined mixture + process model can fit the data, and is used to predict an optimum formulation. Full article

(This article belongs to the Section Battery Materials and Interfaces: Anode, Cathode, Separators and Electrolytes or Others)

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49 pages, 15657 KiB

Open AccessFeature PaperEditor’s ChoiceReview

All-Solid-State Thin Film Li-Ion Batteries: New Challenges, New Materials, and New Designs

by Baolin Wu, Chunguang Chen, Dmitri L. Danilov, Rüdiger-A. Eichel and Peter H. L. Notten

Batteries 2023, 9(3), 186; https://doi.org/10.3390/batteries9030186 - 21 Mar 2023

Cited by 9 | Viewed by 7219

Abstract

All-solid-state batteries (ASSBs) are among the remarkable next-generation energy storage technologies for a broad range of applications, including (implantable) medical devices, portable electronic devices, (hybrid) electric vehicles, and even large-scale grid storage. All-solid-state thin film Li-ion batteries (TFLIBs) with an extended cycle life, [...] Read more.

All-solid-state batteries (ASSBs) are among the remarkable next-generation energy storage technologies for a broad range of applications, including (implantable) medical devices, portable electronic devices, (hybrid) electric vehicles, and even large-scale grid storage. All-solid-state thin film Li-ion batteries (TFLIBs) with an extended cycle life, broad temperature operation range, and minimal self-discharge rate are superior to bulk-type ASSBs and have attracted considerable attention. Compared with conventional batteries, stacking dense thin films reduces the Li-ion diffusion length, thereby improving the rate capability. It is vital to develop TFLIBs with higher energy density and stability. However, multiple challenges, such as interfacial instability, low volumetric energy density, and high manufacturing cost, still hinder the widespread application of TFLIBs. At present, many approaches, such as materials optimization and novel architecture design, have been explored to enhance the stability and energy density of TFLIBs. An overview of these discoveries and developments in TFLIBs is presented in this review, together with new insights into the intrinsic mechanisms of operation; this is of great value to the batteries research community and facilitates further improvements in batteries in the near future. Full article

(This article belongs to the Special Issue Advancements towards Practical All-Solid-State Batteries)

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25 pages, 5437 KiB

Open AccessFeature PaperEditor’s ChoiceReview

Development of All-Solid-State Li-Ion Batteries: From Key Technical Areas to Commercial Use

by Constantin Bubulinca, Natalia E. Kazantseva, Viera Pechancova, Nikhitha Joseph, Haojie Fei, Mariana Venher, Anna Ivanichenko and Petr Saha

Batteries 2023, 9(3), 157; https://doi.org/10.3390/batteries9030157 - 01 Mar 2023

Cited by 9 | Viewed by 6132

Abstract

Innovation in the design of Li-ion rechargeable batteries is necessary to overcome safety concerns and meet energy demands. In this regard, a new generation of Li-ion batteries (LIBs) in the form of all-solid-state batteries (ASSBs) has been developed, attracting a great deal of [...] Read more.

Innovation in the design of Li-ion rechargeable batteries is necessary to overcome safety concerns and meet energy demands. In this regard, a new generation of Li-ion batteries (LIBs) in the form of all-solid-state batteries (ASSBs) has been developed, attracting a great deal of attention for their high-energy density and excellent mechanical-electrochemical stability. This review describes the current state of research and development on ASSB technology. To this end, study of the literature and patents as well as market analysis over the last two decades were carried out, highlighting how scientific achievements have informed the application of commercially profitable ASSBs. Analyzing the patents registered over the past 20 years revealed that the number of them had increased exponentially-from only few per year in early 2000 to more than 342 in 2020. Published literature and patents on the topic declare a solid-state electrolyte (SSE) to be the main component of ASSBs, and most patented examples are referred to as solid inorganic electrolytes (SIEs), followed by solid polymer electrolytes (SPEs) and solid hybrid electrolytes (SHEs) in popularity. Investigation of company websites, social media profiles, reports, and academic publications identified 93 companies associated with ASSBs. A list of leading businesses in the solid-state battery sector was compiled, out of which 36 provided information on the ASSB units in their product portfolio for detailed analysis. Full article

(This article belongs to the Section Battery Materials and Interfaces: Anode, Cathode, Separators and Electrolytes or Others)

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21 pages, 6660 KiB

Open AccessEditor’s ChoiceReview

Strategies and Challenge of Thick Electrodes for Energy Storage: A Review

by Junsheng Zheng, Guangguang Xing, Liming Jin, Yanyan Lu, Nan Qin, Shansong Gao and Jim P. Zheng

Batteries 2023, 9(3), 151; https://doi.org/10.3390/batteries9030151 - 27 Feb 2023

Cited by 11 | Viewed by 5815

Abstract

In past years, lithium-ion batteries (LIBs) can be found in every aspect of life, and batteries, as energy storage systems (ESSs), need to offer electric vehicles (EVs) more competition to be accepted in markets for automobiles. Thick electrode design can reduce the use [...] Read more.

In past years, lithium-ion batteries (LIBs) can be found in every aspect of life, and batteries, as energy storage systems (ESSs), need to offer electric vehicles (EVs) more competition to be accepted in markets for automobiles. Thick electrode design can reduce the use of non-active materials in batteries to improve the energy density of the batteries and reduce the cost of the batteries. However, thick electrodes are limited by their weak mechanical stability and poor electrochemical performance; these limitations could be classified as the critical cracking thickness (CCT) and the limited penetration depth (LPD). The understanding of the CCT and the LPD have been proposed and the recent works on breaking the CCT and improving the LPD are listed in this article. By comprising these attempts, some thick electrodes could not offer higher mass loading or higher accessible areal capacity that would defeat the purpose. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries and Li-Ion Capacitors: From Fundamentals to Practical Applications)

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17 pages, 6870 KiB

Open AccessEditor’s ChoiceArticle

High-Entropy Metal Oxide (NiMnCrCoFe)₃O₄ Anode Materials with Controlled Morphology for High-Performance Lithium-Ion Batteries

by Xuan Liang Wang, En Mei Jin, Gopinath Sahoo and Sang Mun Jeong

Batteries 2023, 9(3), 147; https://doi.org/10.3390/batteries9030147 - 24 Feb 2023

Cited by 10 | Viewed by 2630

Abstract

High-entropy metal oxides (HEMOs) with several functional properties, including high structural stability and superior conductivity, have been recently utilized in energy-storage devices. Morphology control is the key factor to optimizing HEMO performance for successful use in lithium-ion anode materials. Hence, in this study, [...] Read more.

High-entropy metal oxides (HEMOs) with several functional properties, including high structural stability and superior conductivity, have been recently utilized in energy-storage devices. Morphology control is the key factor to optimizing HEMO performance for successful use in lithium-ion anode materials. Hence, in this study, HEMO ((NiMnCrCoFe)₃O₄) was synthesized via a hydrothermal reaction and subsequent post-annealing process, where cetyltrimethylammonium bromide (CTAB) and urea were used to optimize the morphological structure of HEMO particles to ensure a bimodal distribution. A bimodal particle distribution of HEMO was observed and the electrochemical performance was also investigated for an anode in lithium-ion batteries (LIBs). The proposed bimodal HEMO manifests a superior electrochemical performance compared to existing HEMO, which is controlled by uniform nanoscale or micro-sized secondary particles. The present study shows that collective metal cations with different ionic radii, valence states, and reaction potentials, and a diversification of structures, enable a synergistic effect for the excellent performance of HEMOs in LIBs. The proposed HEMO shows an improved initial discharge capacity of 527 mAh g⁻¹ at a high current density of 5 A g⁻¹ compared to the other referred HEMO systems, and 99.8% cycle retention after 300 cycles. Further, this work allows a new approach for designing multi-element transition metal oxide anode materials using a high-entropy strategy, which can be employed in the development of advanced LIBs. Full article

(This article belongs to the Special Issue Advanced Cathode and Anode Materials for Lithium/Sodium-Ion Batteries)

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21 pages, 5681 KiB

Open AccessEditor’s ChoiceArticle

Ammonium and Tetraalkylammonium Salts as Additives for Li Metal Electrodes

by Dario Di Cillo, Luca Bargnesi, Giampaolo Lacarbonara and Catia Arbizzani

Batteries 2023, 9(2), 142; https://doi.org/10.3390/batteries9020142 - 20 Feb 2023

Cited by 1 | Viewed by 1919

Abstract

Lithium metal batteries are considered a promising technology to implement high energy density rechargeable systems beyond lithium-ion batteries. However, the development of dendritic morphology is the basis of safety and performance issues and represents the main limiting factor for using lithium anodes in [...] Read more.

Lithium metal batteries are considered a promising technology to implement high energy density rechargeable systems beyond lithium-ion batteries. However, the development of dendritic morphology is the basis of safety and performance issues and represents the main limiting factor for using lithium anodes in commercial rechargeable batteries. In this study, the electrochemical behaviour of Li metal has been investigated in organic carbonate-based electrolytes by electrochemical impedance spectroscopy measurements and deposition/stripping galvanostatic cycling. Low amounts of tetraalkylammonium hexafluorophosphate salts have been added to the electrolytes with the aim of regulating the lithium deposition/stripping process through the electrostatic shielding effect that improves the lithium deposition. The use of NH₄PF₆ also determined good lithium deposition/stripping performance due to the chemical modification of the native solid electrolyte interphase via direct reaction with lithium. Full article

(This article belongs to the Section Battery Materials and Interfaces: Anode, Cathode, Separators and Electrolytes or Others)

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25 pages, 3249 KiB

Open AccessEditor’s ChoiceReview

Renewable Electricity for Decarbonisation of Road Transport: Batteries or E-Fuels?

by Gianluca Pasini, Giovanni Lutzemberger and Lorenzo Ferrari

Batteries 2023, 9(2), 135; https://doi.org/10.3390/batteries9020135 - 14 Feb 2023

Cited by 11 | Viewed by 4497

Abstract

Road transport is one of the most energy-consuming and greenhouse gas (GHG) emitting sectors. Progressive decarbonisation of electricity generation could support the ambitious target of road vehicle climate neutrality in two different ways: direct electrification with onboard electrochemical storage or a change of [...] Read more.

Road transport is one of the most energy-consuming and greenhouse gas (GHG) emitting sectors. Progressive decarbonisation of electricity generation could support the ambitious target of road vehicle climate neutrality in two different ways: direct electrification with onboard electrochemical storage or a change of energy vector with e-fuels. The most promising, state-of-the-art electrochemical storages for road transport have been analysed considering current and future technologies (the most promising ones) whose use is assumed to occur within the next 10–15 years. Different e-fuels (e-hydrogen, e-methanol, e-diesel, e-ammonia, E-DME, and e-methane) and their production pathways have been reviewed and compared in terms of energy density, synthesis efficiency, and technology readiness level. A final energetic comparison between electrochemical storages and e-fuels has been carried out considering different powertrain architectures, highlighting the huge difference in efficiency for these competing solutions. E-fuels require 3–5 times more input energy and cause 3–5 times higher equivalent vehicle CO₂ emissions if the electricity is not entirely decarbonised. Full article

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27 pages, 25177 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Data-Driven Battery Aging Mechanism Analysis and Degradation Pathway Prediction

by Ruilong Xu, Yujie Wang and Zonghai Chen

Batteries 2023, 9(2), 129; https://doi.org/10.3390/batteries9020129 - 12 Feb 2023

Cited by 8 | Viewed by 2548

Abstract

Capacity decline is the focus of traditional battery health estimation as it is a significant external manifestation of battery aging. However, it is difficult to depict the internal aging information in depth. To achieve the goal of deeper online diagnosis and accurate prediction [...] Read more.

Capacity decline is the focus of traditional battery health estimation as it is a significant external manifestation of battery aging. However, it is difficult to depict the internal aging information in depth. To achieve the goal of deeper online diagnosis and accurate prediction of battery aging, this paper proposes a data-driven battery aging mechanism analysis and degradation pathway prediction approach. Firstly, a non-destructive aging mechanism analysis method based on the open-circuit voltage model is proposed, where the internal aging modes are quantified through the marine predator algorithm. Secondly, through the design of multi-factor and multi-level orthogonal aging experiments, the dominant aging modes and critical aging factors affecting the battery capacity decay at different life phases are determined using statistical analysis methods. Thirdly, a data-driven multi-factor coupled battery aging mechanism prediction model is developed. Specifically, the Transformer network is designed to establish nonlinear relationships between factors and aging modes, and the regression-based data enhancement is performed to enhance the model generalization capability. To enhance the adaptability to variations in aging conditions, the model outputs are set to the increments of the aging modes. Finally, the experimental results verify that the proposed approach can achieve satisfactory performances under different aging conditions. Full article

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13 pages, 5445 KiB

Open AccessEditor’s ChoiceArticle

Genetic Algorithm and Taguchi Method: An Approach for Better Li-Ion Cell Model Parameter Identification

by Taha Al Rafei, Nadia Yousfi Steiner and Daniela Chrenko

Batteries 2023, 9(2), 72; https://doi.org/10.3390/batteries9020072 - 20 Jan 2023

Cited by 4 | Viewed by 2475

Abstract

The genetic algorithm (GA) is one of the most used methods to identify the parameters of Li-ion battery models. However, the parametrization of the GA method is not straightforward and can lead to poor accuracy and/or long calculation times. The Taguchi design method [...] Read more.

The genetic algorithm (GA) is one of the most used methods to identify the parameters of Li-ion battery models. However, the parametrization of the GA method is not straightforward and can lead to poor accuracy and/or long calculation times. The Taguchi design method provides an approach to optimize GA parameters, achieving a good balance between accuracy and calculation time. The Taguchi design method is thus used to define the most adapted GA parameters to identify the parameters of model of Li-ion batteries for household applications based on static and dynamic tests in the time domain. The results show a good compromise between calculation time and accuracy (RMSE less than 0.6). This promising approach could be applied to other Li-ion battery applications, resulting from measurements in the frequency domain or different kinds of energy storage. Full article

(This article belongs to the Special Issue High Energy Rechargeable Batteries: Li-Ion and Beyond)

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14 pages, 27428 KiB

Open AccessEditor’s ChoiceArticle

Changes in the Mechanical Behavior of Electrically Aged Lithium-Ion Pouch Cells: In-Plane and Out-of-Plane Indentation Loads with Varying Testing Velocity and State of Charge

by Marvin Sprenger, Georgi Kovachev, Norbert Dölle, Florian Schauwecker, Wolfgang Sinz and Christian Ellersdorfer

Batteries 2023, 9(2), 67; https://doi.org/10.3390/batteries9020067 - 17 Jan 2023

Viewed by 2326

Abstract

The knowledge about the influence of electrical aging on the behavior of lithium-ion cells under mechanical loads is of high importance to ensure a safe use of batteries over the lifetime in electric vehicles. In order to describe the mechanical behavior in relation [...] Read more.

The knowledge about the influence of electrical aging on the behavior of lithium-ion cells under mechanical loads is of high importance to ensure a safe use of batteries over the lifetime in electric vehicles. In order to describe the mechanical behavior in relation to electrical aging, fresh and electrically aged NCM pouch cells were investigated under different mechanical crash loads. For the first time, the aged cells’ behavior under quasistatic lateral loading was taken into account. Aged cells showed lower maximum forces compared to the fresh cells. The reason of the changed mechanical cell behavior was explained with the different buckling behavior of fresh and aged cells by experimental images. Furthermore, quasistatic and dynamic crash tests in cell’s thickness direction were performed at varying state of charge (SOC) and compared to the results of a previously published study. Independently of the testing velocity, the electrically aged cells failed at increased deformation values. This observation was justified by an increased cell thickness due to an additional softer layer, formed on the aged graphite particle surface, which was observed by the means of scanning electron microscopy. Furthermore, the aged cells showed lower failure forces of up to −11% under quasistatic and dynamic loads at 0% SOC. It was also illustrated that electrical aging causes a deeper voltage drop after cell failure, which suggests a higher energy release after the internal short circuit. The investigations show that electrical aging has a significant influence on the mechanical properties of lithium-ion cells and must be taken into account in the safety assessment. Full article

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18 pages, 7783 KiB

Open AccessEditor’s ChoiceArticle

Fast Identification of Micro-Health Parameters for Retired Batteries Based on a Simplified P2D Model by Using Padé Approximation

by Jianing Xu, Chuanyu Sun, Yulong Ni, Chao Lyu, Chao Wu, He Zhang, Qingjun Yang and Fei Feng

Batteries 2023, 9(1), 64; https://doi.org/10.3390/batteries9010064 - 16 Jan 2023

Cited by 18 | Viewed by 3002

Abstract

Better performance consistency of regrouped batteries retired from electric vehicles can guarantee the residual value maximized, which greatly improves the second-use application economy of retired batteries. This paper develops a fast identification approach for micro-health parameters characterizing negative electrode material and electrolyte in [...] Read more.

Better performance consistency of regrouped batteries retired from electric vehicles can guarantee the residual value maximized, which greatly improves the second-use application economy of retired batteries. This paper develops a fast identification approach for micro-health parameters characterizing negative electrode material and electrolyte in LiFePO₄ batteries on the basis of a simplified pseudo two-dimensional model by using Padé approximation is developed. First, as the basis for accurately identifying micro-health parameters, the liquid-phase and solid-phase diffusion processes of pseudo two-dimensional model are simplified based on Padé approximation, especially according to enhanced boundary conditions of liquid-phase diffusion. Second, the reduced pseudo two-dimensional model with the lumped parameter is proposed, the target parameters characterizing negative electrode material (ε_n, D_s,n) and electrolyte (D_e, C_e) are grouped with other unknown but fixed parameters, which ensures that no matter whether the target parameters can be achieved, the corresponding varying traces is able to be effectively and independently monitored by lumped parameters. Third, the fast identification method for target micro-health parameters is developed based on the sensitivity of target parameters to constant-current charging voltage, which shortens the parameter identification time in comparison to that obtained by other approaches. Finally, the identification accuracy of the lumped micro-health parameters is verified under 1 C constant-current charging condition. Full article

(This article belongs to the Special Issue Battery Energy Storage in Advanced Power Systems)

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27 pages, 8163 KiB

Open AccessEditor’s ChoicePerspective

Use of Water-In-Salt Concentrated Liquid Electrolytes in Electrochemical Energy Storage: State of the Art and Perspectives

by Shahid Khalid, Nicolò Pianta, Piercarlo Mustarelli and Riccardo Ruffo

Batteries 2023, 9(1), 47; https://doi.org/10.3390/batteries9010047 - 07 Jan 2023

Cited by 8 | Viewed by 4430

Abstract

Batteries based on organic electrolytes have been raising safety concerns due to some associated fire/explosion accidents caused by the unusual combination of highly flammable organic electrolytes and high energy electrodes. Nonflammable aqueous batteries are a good alternative to the current energy storage systems. [...] Read more.

Batteries based on organic electrolytes have been raising safety concerns due to some associated fire/explosion accidents caused by the unusual combination of highly flammable organic electrolytes and high energy electrodes. Nonflammable aqueous batteries are a good alternative to the current energy storage systems. However, what makes aqueous batteries safe and viable turns out to be their main weakness, since water molecules are prone to decomposition because of a narrow electrochemical stability window (ESW). In this perspective we introduce aqueous batteries and then discuss the state-of-the-art of water-in-salt (WIS) electrolytes for aqueous energy storage systems. The main strategies to improve ESW are reviewed, including: (i) the use of fluorinated salts to make a solid electrolyte interphase (SEI); (ii) the use of cost-effective and highly soluble salts to reduce water activity through super concentration; and (iii) the use of hybrid electrolytes combining the advantages of both aqueous and non-aqueous phases. Then, we discuss different battery chemistries operated with different WIS electrolytes. Finally, we highlight the challenges and future technological perspectives for practical aqueous energy storage systems, including applications in stationary storage/grid, power backup, portable electronics, and automotive sectors. Full article

(This article belongs to the Topic Energy Storage Materials and Devices)

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14 pages, 2206 KiB

Open AccessEditor’s ChoiceArticle

Strain Compensation Methods for Fiber Bragg Grating Temperature Sensors Suitable for Integration into Lithium-Ion Battery Electrolyte

by Johanna Unterkofler, Gregor Glanz, Markus Koller, Reinhard Klambauer and Alexander Bergmann

Batteries 2023, 9(1), 34; https://doi.org/10.3390/batteries9010034 - 03 Jan 2023

Cited by 4 | Viewed by 2235

Abstract

Temperature is a crucial factor for the safe operation of lithium-ion batteries. During operation, the internal temperature rises above the external temperature due to poor inner thermal conductivity. Various sensors have been proposed to detect the internal temperature, including fiber Bragg grating sensors. [...] Read more.

Temperature is a crucial factor for the safe operation of lithium-ion batteries. During operation, the internal temperature rises above the external temperature due to poor inner thermal conductivity. Various sensors have been proposed to detect the internal temperature, including fiber Bragg grating sensors. However, to the authors’ knowledge, there is no detailed description of the encapsulation of the fiber Bragg grating sensor in the literature to shield it from strain. In this study, different encapsulation methods for strain compensation were compared to find the encapsulation material most compatible with the electrolyte. For this, we stored the proposed sensors with different encapsulation methods in ethylene carbonate:ethyl methyl carbonate (EC:EMC) 3:7 with LiPF₆ (lithium hexafluorophosphate) electrolyte and applied temperature changes. After evaluating the sensor encapsulation methods in terms of handling, diameter, uncertainty, usability, and hysteresis behavior, the most suitable sensor encapsulation was found to be a fused silica capillary with polyimide coating. Full article

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11 pages, 2877 KiB

Open AccessEditor’s ChoiceArticle

In Situ Solidified Gel Polymer Electrolytes for Stable Solid−State Lithium Batteries at High Temperatures

by Junfeng Ma, Zhiyan Wang, Jinghua Wu, Zhi Gu, Xing Xin and Xiayin Yao

Batteries 2023, 9(1), 28; https://doi.org/10.3390/batteries9010028 - 30 Dec 2022

Cited by 8 | Viewed by 3665

Abstract

Lithium metal batteries have attracted much attention due to their high energy density. However, the critical safety issues and chemical instability of conventional liquid electrolytes in lithium metal batteries significantly limit their practical application. Herein, we propose polyethylene (PE)−based gel polymer electrolytes by [...] Read more.

Lithium metal batteries have attracted much attention due to their high energy density. However, the critical safety issues and chemical instability of conventional liquid electrolytes in lithium metal batteries significantly limit their practical application. Herein, we propose polyethylene (PE)−based gel polymer electrolytes by in situ polymerization, which comprise a PE skeleton, polyethylene glycol and lithium bis(trifluoromethylsulfonyl)imide as well as liquid carbonate electrolytes. The obtained PE−based gel polymer electrolyte exhibits good interfacial compatibility with electrodes, high ion conductivity, and wide electrochemical window at high temperatures. Moreover, the assembled LiFePO₄//Li solid−state batteries employing PE−based gel polymer electrolyte with 50% liquid carbonate electrolytes deliver good rate performance and excellent cyclic life at both 60 °C and 80 °C. In particular, they achieve high specific capacities of 158.5 mA h g⁻¹ with a retention of 98.87% after 100 cycles under 80 °C at 0.5 C. The in situ solidified method for preparing PE−based gel polymer electrolytes proposes a feasible approach for the practical application of lithium metal batteries. Full article

(This article belongs to the Special Issue Solid State Batteries: From Materials Research to Design and Applications)

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57 pages, 19335 KiB

Open AccessFeature PaperEditor’s ChoiceReview

Progress and Prospect of Practical Lithium-Sulfur Batteries Based on Solid-Phase Conversion

by Yikun Yi, Feng Hai, Jingyu Guo, Xiaolu Tian, Shentuo Zheng, Zhendi Wu, Tao Wang and Mingtao Li

Batteries 2023, 9(1), 27; https://doi.org/10.3390/batteries9010027 - 29 Dec 2022

Cited by 5 | Viewed by 3206

Abstract

Lithium–sulfur (Li–S) batteries hold great promise in the field of power and energy storage due to their high theoretical capacity and energy density. However, the “shuttle effect” that originates from the dissolution of intermediate lithium polysulfides (LiPSs) during the charging and discharging process [...] Read more.

Lithium–sulfur (Li–S) batteries hold great promise in the field of power and energy storage due to their high theoretical capacity and energy density. However, the “shuttle effect” that originates from the dissolution of intermediate lithium polysulfides (LiPSs) during the charging and discharging process is prone to causing continuous irreversible capacity loss, which restricts the practical development. Beyond the traditional Li–S batteries based on the dissolution-diffusion mechanism, novel Li–S batteries based on solid-phase conversion exhibit superior cycling stability owing to the absolute prevention of polysulfides shuttling. Radically eliminating the formation of polysulfides in cathodes or cutting off their diffusion in electrolytes are the two main ways to achieve solid-phase conversion. Generally, direct transformation of sulfur to final Li₂S without polysulfides participation tends to occur in short-chain sulfur polymers or special molecular forms of sulfur substances, while specific regulations of liquid electrolytes with solvating structure or solid-state electrolytes can effectively suppressing the polysulfides dissolution. In this review, we systematically organized and summarized the structures and approaches to achieve solid-phase conversion, introduce their preparation methods, discuss their advantages and disadvantages, and analyze the factors and effects of different structures on battery performances. Finally, the problems demanding a prompt solution for the practical development of solid-phase conversion-based Li–S batteries, as well as their future development direction, are suggested. Full article

(This article belongs to the Special Issue Lithium-Sulfur Batteries: Research Progress of Key Materials)

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13 pages, 5677 KiB

Open AccessEditor’s ChoiceArticle

The Stabilizing of 1T-MoS₂ for All-Solid-State Lithium-Ion Batteries

by Peidian Chong, Ziwang Zhou, Kaihong Wang, Wenhao Zhai, Yafeng Li, Jianbiao Wang and Mingdeng Wei

Batteries 2023, 9(1), 26; https://doi.org/10.3390/batteries9010026 - 29 Dec 2022

Cited by 8 | Viewed by 2786

Abstract

All-solid-state batteries (SSBs) are prospective candidates for a range of energy accumulation systems, delivering higher energy densities compared to batteries which use liquid electrolytes. Amongst the numerous solid-state electrolytes (SEs), sulfide-based electrolytes in particular have received more attention given that they have a [...] Read more.

All-solid-state batteries (SSBs) are prospective candidates for a range of energy accumulation systems, delivering higher energy densities compared to batteries which use liquid electrolytes. Amongst the numerous solid-state electrolytes (SEs), sulfide-based electrolytes in particular have received more attention given that they have a high ionic conductivity. However, the incompatibility between the electrode and SEs is still an ongoing challenge that leads to poor electrochemical performance. In this work, we focus on 1T-MoS₂. It is well known that 1T metallic MoS₂ is unstable even at room temperature. However, we showed that 1T-MoS₂ can be stabilized at 600 °C for at least 2 h, and the 1T-MoS₂-600 interlayer spacing expanded to 0.95 nm. The high crystallinity of the 1T phase is highly compatible with solid electrolytes and coupled with the increased interlayer spacing, so in the all-solid-state lithium-ion battery (ALLLIB), we achieved outstanding cycling performance. At the current density of 0.2 C (1 C = 670 mA g⁻¹), this material delivered a capacity of 406 mA h g⁻¹ after 50 cycles. Full article

(This article belongs to the Special Issue Recent Progress of Electrochemical Performance and Interface Analysis of Batteries)

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13 pages, 2812 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Electrocatalytic and Conductive Vanadium Oxide on Carbonized Bacterial Cellulose Aerogel for the Sulfur Cathode in Li-S Batteries

by Xueyan Lin, Wenyue Li, Xuan Pan, Shu Wang and Zhaoyang Fan

Batteries 2023, 9(1), 14; https://doi.org/10.3390/batteries9010014 - 26 Dec 2022

Cited by 2 | Viewed by 2242

Abstract

Many transition-metal-oxide-based catalysts have been investigated to chemically bind soluble lithium polysulfides and accelerate their redox kinetics in lithium-sulfur (Li-S) battery chemistry. However, the intrinsic poor electrical conductivities of these oxides restrict their catalytic performance, consequently limiting the sulfur utilization and the rate [...] Read more.

Many transition-metal-oxide-based catalysts have been investigated to chemically bind soluble lithium polysulfides and accelerate their redox kinetics in lithium-sulfur (Li-S) battery chemistry. However, the intrinsic poor electrical conductivities of these oxides restrict their catalytic performance, consequently limiting the sulfur utilization and the rate performance of Li-S batteries. Herein, we report a freestanding electrocatalytic sulfur host consisting of hydrogen-treated VO₂ nanoparticles (H-VO₂) anchored on nitrogen-doped carbonized bacterial cellulose aerogels (N-CBC). The hydrogen treatment enables the formation and stabilization of the rutile VO₂(R) phase with metallic conductivity at room temperature, significantly enhancing its catalytic capability compared to the as-synthesized insulative VO₂(M) phase. Several measurements characterize the electrocatalytic performance of this unique H-VO₂@N-CBC structure. In particular, the two kinetic barriers between S₈, polysulfides, and Li₂S are largely reduced by 28.2 and 43.3 kJ/mol, respectively. Accordingly, the Li-S battery performance, in terms of sulfur utilization and charge/discharge rate, is greatly improved. This work suggests an effective strategy to develop conductive catalysts based on a typical transition metal oxide (VO₂) for Li-S batteries. Full article

(This article belongs to the Special Issue Feature Papers to Celebrate the First Impact Factor of Batteries)

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22 pages, 16816 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Particle Contamination in Commercial Lithium-Ion Cells—Risk Assessment with Focus on Internal Short Circuits and Replication by Currently Discussed Trigger Methods

by Jens Grabow, Jacob Klink, Ralf Benger, Ines Hauer and Hans-Peter Beck

Batteries 2023, 9(1), 9; https://doi.org/10.3390/batteries9010009 - 23 Dec 2022

Cited by 9 | Viewed by 3304

Abstract

A possible contamination with impurities or material weak points generated in cell production of lithium-ion batteries increases the risk of spontaneous internal short circuits (ISC). An ISC can lead to a sudden thermal runaway (TR) of the cell, thereby making these faults especially [...] Read more.

A possible contamination with impurities or material weak points generated in cell production of lithium-ion batteries increases the risk of spontaneous internal short circuits (ISC). An ISC can lead to a sudden thermal runaway (TR) of the cell, thereby making these faults especially dangerous. Evaluation regarding the criticality of an ISC, the development of detection methods for timely fault warning and possible protection concepts require a realistic failure replication for general validation. Various trigger methods are currently discussed to reproduce these ISC failure cases, but without considering a valid basis for the practice-relevant particle properties. In order to provide such a basis for the evaluation and further development of trigger methods, in this paper, the possibilities of detecting impurity particles in production were reviewed and real particles from pouch cells of an established cell manufacturer were analysed. The results indicate that several metallic particles with a significant size up to 1 mm × 1.7 mm could be found between the cell layers. This evidence shows that contamination with impurity particles cannot be completely prevented in cell production, as a result of which particle-induced ISC must be expected and the need for an application-oriented triggering method currently exists. The cause of TR events in the field often cannot be identified. However, it is noticeable that such faults often occur during the charging process. A new interesting hypothesis for this so-far unexplained phenomenon is presented here. Based on all findings, the current trigger methods for replicating an external particle-induced ISC were evaluated in significant detail and specific improvements are identified. Here, it is shown that all current trigger methods for ISC replication exhibit weaknesses regarding reproducibility, which results mainly from the scattering random ISC contact resistance. Full article

(This article belongs to the Topic Safety of Lithium-Ion Batteries)

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12 pages, 3043 KiB

Open AccessEditor’s ChoiceArticle

Defect Chemistry in Zn₃V₄(PO₄)₆

by Navaratnarajah Kuganathan

Batteries 2023, 9(1), 5; https://doi.org/10.3390/batteries9010005 - 22 Dec 2022

Viewed by 1520

Abstract

Zinc-ion batteries have attracted great interest for their low cost, safety, and high energy density. Recently, Zn₃V₄(PO₄)₆ has been reported to be a promising cathode material for zinc-ion batteries. The defect chemistry, diffusion of Zn-ions, and [...] Read more.

Zinc-ion batteries have attracted great interest for their low cost, safety, and high energy density. Recently, Zn₃V₄(PO₄)₆ has been reported to be a promising cathode material for zinc-ion batteries. The defect chemistry, diffusion of Zn-ions, and solution of dopants are examined by advanced simulation techniques. The simulation results show that the most favorable intrinsic defect is the Zn-V anti-site. A zig-zag pattern of long-range Zn²⁺ diffusion is observed and the activation energy of 1.88 eV indicates that the ionic conductivity of this material is low. The most promising isovalent dopants on the Zn site are Ca²⁺ and Fe²⁺. Although the solution of Ga³⁺, Sc³⁺, In³⁺, Y³⁺, Gd³⁺, and La³⁺ on the V site is exoergic, the most promising is In³⁺. Different reaction routes for the formation of Zn₃V₄(PO₄)₆ are considered and the most thermodynamically favorable reaction consists of binary oxides (ZnO, V₂O₃, and P₂O₅) as reactants. Full article

(This article belongs to the Special Issue Zinc-Ion Batteries: Issues and Opportunities)

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20 pages, 5598 KiB

Open AccessFeature PaperEditor’s ChoiceReview

Anode-Free Rechargeable Sodium-Metal Batteries

by Qiao Ni, Yuejiao Yang, Haoshen Du, Hao Deng, Jianbo Lin, Liu Lin, Mengwei Yuan, Zemin Sun and Genban Sun

Batteries 2022, 8(12), 272; https://doi.org/10.3390/batteries8120272 - 05 Dec 2022

Cited by 8 | Viewed by 5991

Abstract

Due to the advantages of rich resources, low cost, high energy conversion efficiency, long cycle life, and low maintenance fee, sodium–ion batteries have been regarded as a promising energy storage technology. However, their relatively low energy density compared with the commercialized lithium–ion batteries [...] Read more.

Due to the advantages of rich resources, low cost, high energy conversion efficiency, long cycle life, and low maintenance fee, sodium–ion batteries have been regarded as a promising energy storage technology. However, their relatively low energy density compared with the commercialized lithium–ion batteries still impedes their application for power systems. Anode–free rechargeable sodium–metal batteries (AFSMBs) pose a solution to boost energy density and tackle the safety problems of metal batteries. At present, researchers still lack a comprehensive understanding of the anode-free cells in terms of electrolytes, solid–electrolyte interphase (SEI), and current collectors. This review is devoted to the field of AFSMBs, and outlines the breakthroughs that have been accomplished along with our perspective on the direction of future development for AFSMBs and the areas that warrant further investigation. Full article

(This article belongs to the Special Issue Anode Materials for Sodium-Ion Batteries)

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21 pages, 3536 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Verification of the Modified Degradation Mode Identification Technique by Employing Electrochemical Impedance Spectroscopy and Differential Voltage Analysis

by Sadia Tasnim Mowri, Anup Barai, Aniruddha Gupta and James Marco

Batteries 2022, 8(12), 274; https://doi.org/10.3390/batteries8120274 - 05 Dec 2022

Cited by 2 | Viewed by 2241

Abstract

For retired automotive lithium-ion batteries, state of health (SoH) is currently utilised to grade them for a second-life application. However, researchers previously challenged this and expressed that, in addition to SoH, the actual degradation mechanism, also known as degradation mode (DM), should be [...] Read more.

For retired automotive lithium-ion batteries, state of health (SoH) is currently utilised to grade them for a second-life application. However, researchers previously challenged this and expressed that, in addition to SoH, the actual degradation mechanism, also known as degradation mode (DM), should be considered for grading, for efficient second-life operation. To date, there is little evidence to support this. A validated DM detection technique for cell/module grading does not exist. A modified DM detection technique by tracking and indexing the incremental capacity (IC) curves was previously proposed by the authors; nevertheless, it was difficult to validate. Researchers previously proposed DM identification using Electrochemical Impedance Spectroscopy (EIS) and Differential Voltage (DV) analysis. With a direct comparison of the techniques made exploiting IC, DV, and EIS, a correlation can be made, which is presented in this article. The correlation suggests that cells identified as having the same (or different) DM by the proposed technique also identified as having the same (or different) DM growth by EIS technique proposed by other researchers. Likewise, DV analysis suggests that the DV peak’s standard deviation of similar DM cells is smaller than that of the different DM cells. Full article

(This article belongs to the Section Battery Performance, Ageing, Reliability and Safety)

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16 pages, 9729 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Nanostructured Manganese Dioxide for Hybrid Supercapacitor Electrodes

by Jon Rodriguez-Romero, Idoia Ruiz de Larramendi and Eider Goikolea

Batteries 2022, 8(12), 263; https://doi.org/10.3390/batteries8120263 - 30 Nov 2022

Cited by 8 | Viewed by 3032

Abstract

Hybrid supercapacitors, as emerging energy storage devices, have gained much attention in recent years due to their high energy density, fast charge/discharge and long cyclabilities. Among the wide range of systems covered by this topic, low cost, environmental friendliness and high power provide [...] Read more.

Hybrid supercapacitors, as emerging energy storage devices, have gained much attention in recent years due to their high energy density, fast charge/discharge and long cyclabilities. Among the wide range of systems covered by this topic, low cost, environmental friendliness and high power provide MnO₂ with great characteristics to be a competitive candidate. The present work reports a hybrid aqueous supercapacitor system using a commercial activated carbon as the negative electrode and a synthesized manganese dioxide as the positive electrode. Two manganese dioxide polymorphs (α-MnO₂ and δ-MnO₂) were tested in different neutral and basic aqueous electrolytes. In this way, full cell systems that reached an energy density of 15.6 Wh kg⁻¹ at a power density of 1 kW kg⁻¹ were achieved. The electrode–electrolyte combination explored in this study exhibits excellent performance without losing capacity after 5000 charge/discharge cycles, leading to a promising approach towards more sustainable, high-performance energy storage systems. Full article

(This article belongs to the Special Issue Feature Papers to Celebrate the First Impact Factor of Batteries)

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14 pages, 4468 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Mitigating Polysulfide Shuttles with Upcycled Alkali Metal Terephthalate Decorated Separators

by Daniel A. Gribble, Zih-Yu Lin, Sourav Ghosh, Brett M. Savoie and Vilas G. Pol

Batteries 2022, 8(12), 253; https://doi.org/10.3390/batteries8120253 - 23 Nov 2022

Cited by 1 | Viewed by 2525

Abstract

High energy density lithium–sulfur batteries (LSBs) are a potential replacement for lithium-ion batteries (LIBs). However, practical lifetimes are inhibited by lithium polysulfide (LiPS) shuttling. Concurrently, plastic waste accumulation worldwide threatens our ecosystems. Herein, a fast and facile strategy to upcycle polyethylene terephthalate (PET) [...] Read more.

High energy density lithium–sulfur batteries (LSBs) are a potential replacement for lithium-ion batteries (LIBs). However, practical lifetimes are inhibited by lithium polysulfide (LiPS) shuttling. Concurrently, plastic waste accumulation worldwide threatens our ecosystems. Herein, a fast and facile strategy to upcycle polyethylene terephthalate (PET) waste into useful materials is investigated. Dilithium terephthalate (Li₂TP) and dipotassium terephthalate (K₂TP) salts were synthesized from waste soda bottles via microwave depolymerization and solution coated onto glass fiber paper (GFP) separators. Salt-functionalized separators with Li₂TP@GFP and K₂TP@GFP mitigated LiPS shuttling and improved electrochemical performance in cells. Pore analysis and density functional theory (DFT) calculations indicate the action mechanism is synergistic physical blocking of bulky LiPS anions in nanopores and diffusion inhibition via electrostatic interactions with abundant carboxylate groups. LSBs with K₂TP@GFP separator showing highest LiPS affinity and smallest pore size demonstrated enhanced initial capacity as compared to non-modified GFP by 5.4% to 648 mAh g⁻¹, and increased cycle 100 capacity by 23% to 551 mAh g⁻¹. Overall, K₂TP@GFP retained 85% of initial capacity after 100 cycles with an average capacity fading of 0.15% per cycle. By comparison, GFP retained only 73% of initial capacity after 100 cycles with 0.27% average capacity loss, demonstrating effective LiPS retention. Full article

(This article belongs to the Collection Advances in Battery Materials)

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28 pages, 4239 KiB

Open AccessEditor’s ChoiceReview

A Review of Lithium-Ion Battery Failure Hazards: Test Standards, Accident Analysis, and Safety Suggestions

by Xin Lai, Jian Yao, Changyong Jin, Xuning Feng, Huaibin Wang, Chengshan Xu and Yuejiu Zheng

Batteries 2022, 8(11), 248; https://doi.org/10.3390/batteries8110248 - 20 Nov 2022

Cited by 34 | Viewed by 11031

Abstract

The frequent safety accidents involving lithium-ion batteries (LIBs) have aroused widespread concern around the world. The safety standards of LIBs are of great significance in promoting usage safety, but they need to be constantly upgraded with the advancements in battery technology and the [...] Read more.

The frequent safety accidents involving lithium-ion batteries (LIBs) have aroused widespread concern around the world. The safety standards of LIBs are of great significance in promoting usage safety, but they need to be constantly upgraded with the advancements in battery technology and the extension of the application scenarios. This study comprehensively reviews the global safety standards and regulations of LIBs, including the status, characteristics, and application scope of each standard. A standardized test for thermal runaway triggering is also introduced. The recent fire accidents in electric vehicles and energy storage power stations are discussed in relation to the upgrading of the rational test standards. Finally, the following four suggestions for improving battery safety are proposed to optimize the safety standards: (1) early warning and cloud alarms for the battery’s thermal runaway; (2) an innovative structural design for a no-fire battery pack; (3) the design of a fire water injection interface for the battery pack; (4) the design of an immersive energy storage power station. This study provides insights for promoting the effectiveness of relevant safety standards for LIBs, thereby reducing the failure hazards. Full article

(This article belongs to the Collection Advances in Battery Energy Storage and Applications)

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24 pages, 12542 KiB

Open AccessEditor’s ChoiceReview

A Review of the Application of Carbon Materials for Lithium Metal Batteries

by Zeyu Wu, Kening Sun and Zhenhua Wang

Batteries 2022, 8(11), 246; https://doi.org/10.3390/batteries8110246 - 18 Nov 2022

Cited by 9 | Viewed by 4621

Abstract

Lithium secondary batteries have been the most successful energy storage devices for nearly 30 years. Until now, graphite was the most mainstream anode material for lithium secondary batteries. However, the lithium storage mechanism of the graphite anode limits the further improvement of the [...] Read more.

Lithium secondary batteries have been the most successful energy storage devices for nearly 30 years. Until now, graphite was the most mainstream anode material for lithium secondary batteries. However, the lithium storage mechanism of the graphite anode limits the further improvement of the specific capacity. The lithium metal anode, with the lowest electrochemical potential and extremely high specific capacity, is considered to be the optimal anode material for next-generation lithium batteries. However, the lifetime degradation and safety problems caused by dendrite growth have seriously hindered its commercialization. Carbon materials have good electrical conductivity and modifiability, and various carbon materials were designed and prepared for use in lithium metal batteries. Here, we will start by analyzing the problems and challenges faced by lithium metal. Then, the application progress and achievements of various carbon materials in lithium metal batteries are summarized. Finally, the research suggestions are given, and the application feasibility of carbon materials in metal lithium batteries is discussed. Full article

(This article belongs to the Special Issue Lithium-Ion Batteries and Li-Ion Capacitors: From Fundamentals to Practical Applications)

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10 pages, 1847 KiB

Open AccessEditor’s ChoiceArticle

An Exploratory Study of MoS₂ as Anode Material for Potassium Batteries

by Lucia Fagiolari, Daniele Versaci, Federica Di Berardino, Julia Amici, Carlotta Francia, Silvia Bodoardo and Federico Bella

Batteries 2022, 8(11), 242; https://doi.org/10.3390/batteries8110242 - 17 Nov 2022

Cited by 15 | Viewed by 2589

Abstract

Potassium-based batteries represent one of the emerging classes of post-lithium electrochemical energy storage systems in the international scene, due to both the abundance of raw materials and achievable cell potentials not far from those of lithium batteries. In this context, it is important [...] Read more.

Potassium-based batteries represent one of the emerging classes of post-lithium electrochemical energy storage systems in the international scene, due to both the abundance of raw materials and achievable cell potentials not far from those of lithium batteries. In this context, it is important to define electrodes and electrolytes that give reproducible performance and that can be used by different research groups as an internal standard when developing new materials. We propose molybdenum disulfide (MoS₂) as a valid anode choice, being a commercial and easily processable material, the 2D layered structure of which is promising for large potassium ions reversible storage. It has been proven to work for hundreds of cycles, keeping a constant specific capacity around 100 mAh g⁻¹ while also preserving its electrochemical interphase and morphology. Full article

(This article belongs to the Collection Advances in Battery Materials)

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15 pages, 3911 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Online Identification of VLRA Battery Model Parameters Using Electrochemical Impedance Spectroscopy

by Javier Olarte, Jaione Martinez de Ilarduya, Ekaitz Zulueta, Raquel Ferret, Joseba Garcia-Ortega and Jose Manuel Lopez-Guede

Batteries 2022, 8(11), 238; https://doi.org/10.3390/batteries8110238 - 14 Nov 2022

Cited by 5 | Viewed by 1970

Abstract

This paper introduces the use of a new low-computation cost algorithm combining neural networks with the Nelder–Mead simplex method to monitor the variations of the parameters of a previously selected equivalent circuit calculated from Electrochemical Impedance Spectroscopy (EIS) corresponding to a series of [...] Read more.

This paper introduces the use of a new low-computation cost algorithm combining neural networks with the Nelder–Mead simplex method to monitor the variations of the parameters of a previously selected equivalent circuit calculated from Electrochemical Impedance Spectroscopy (EIS) corresponding to a series of battery aging experiments. These variations could be correlated with variations in the battery state over time and, therefore, identify or predict battery degradation patterns or failure modes. The authors have benchmarked four different Electrical Equivalent Circuit (EEC) parameter identification algorithms: plain neural network mapping EIS raw data to EEC parameters, Particle Swarm Optimization, Zview, and the proposed new one. In order to improve the prediction accuracy of the neural network, a data augmentation method has been proposed to improve the neural network training error. The proposed parameter identification algorithms have been compared and validated through real data obtained from a six-month aging test experiment carried out with a set of six commercial 80 Ah VLRA batteries under different cycling and temperature operation conditions. Full article

(This article belongs to the Special Issue Feature Papers to Celebrate the First Impact Factor of Batteries)

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19 pages, 4953 KiB

Open AccessEditor’s ChoiceArticle

Deep Learning Classification of Li-Ion Battery Materials Targeting Accurate Composition Classification from Laser-Induced Breakdown Spectroscopy High-Speed Analyses

by Marie-Chloé Michaud Paradis, François R. Doucet, Steeve Rousselot, Alex Hernández-García, Kheireddine Rifai, Ouardia Touag, Lütfü Ç. Özcan, Nawfal Azami and Mickaël Dollé

Batteries 2022, 8(11), 231; https://doi.org/10.3390/batteries8110231 - 10 Nov 2022

Cited by 3 | Viewed by 2591

Abstract

Laser-induced breakdown spectroscopy (LIBS) is a valuable tool for the solid-state elemental analysis of battery materials. Key advantages include a high sensitivity for light elements (lithium included), complex emission patterns unique to individual elements through the full periodic table, and record speed analysis [...] Read more.

Laser-induced breakdown spectroscopy (LIBS) is a valuable tool for the solid-state elemental analysis of battery materials. Key advantages include a high sensitivity for light elements (lithium included), complex emission patterns unique to individual elements through the full periodic table, and record speed analysis reaching 1300 full spectra per second (1.3 kHz acquisition rate). This study investigates deep learning methods as an alternative tool to accurately recognize different compositions of similar battery materials regardless of their physical properties or manufacturer. Such applications are of interest for the real-time digitalization of battery components and identification in automated manufacturing and recycling plant designs. Full article

(This article belongs to the Collection Advances in Battery Materials)

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25 pages, 6215 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

What Differentiates Dielectric Oxides and Solid Electrolytes on the Pathway toward More Efficient Energy Storage?

by Antonio Nuno Guerreiro, Beatriz Arouca Maia, Hesham Khalifa, Manuela Carvalho Baptista and Maria Helena Braga

Batteries 2022, 8(11), 232; https://doi.org/10.3390/batteries8110232 - 10 Nov 2022

Cited by 7 | Viewed by 3122

Abstract

Taking advantage of electrode thicknesses well beyond conventional dimensions allowed us to follow the surface plasmonic THz frequency phenomenon with vacuum wavelengths of 100 μm to 1 mm, only to scrutinize them within millimeters-thicknesses insulators. Here, we analyze an Al/insulator/Cu cell in which [...] Read more.

Taking advantage of electrode thicknesses well beyond conventional dimensions allowed us to follow the surface plasmonic THz frequency phenomenon with vacuum wavelengths of 100 μm to 1 mm, only to scrutinize them within millimeters-thicknesses insulators. Here, we analyze an Al/insulator/Cu cell in which the metal electrodes-collectors were separated by a gap that was alternatively filled by SiO₂, MgO, Li₂O, Na₃Zr₂Si₂PO₁₂–NASICON, Li_1.5Al_0.5Ge_1.5(PO₄)₃–LAGP, and Li_2.99Ba_0.005ClO–Li⁺ glass. A comparison was drawn using experimental surface chemical potentials, cyclic voltammetry (I-V plots), impedance spectroscopy, and theoretical approaches such as structure optimization, simulation of the electronic band structures, and work functions. The analysis reveals an unexpected common emergency from the cell’s materials to align their surface chemical potential, even in operando when set to discharge under an external resistor of 1842 Ω.cm_insulator. A very high capability of the metal electrodes to vary their surface chemical potentials and specific behavior among dielectric oxides and solid electrolytes was identified. Whereas LAGP and Li₂O behaved as p-type semiconductors below 40 °C at OCV and while set to discharge with a resistor in agreement with the Li⁺ diffusion direction, NASICON behaved as a quasi n-type semiconductor at OCV, as MgO, and as a quasi p-type semiconductor while set to discharge. The capacity to behave as a p-type semiconductor may be related to the ionic conductivity of the mobile ion. The ferroelectric behavior of Li_2.99Ba_0.005ClO has shown surface plasmon polariton (SPP) waves in the form of surface propagating solitons, as in complex phenomena, as well as electrodes’ surface chemical potentials inversion capabilities (i.e., χ (Al) − χ (Cu) > 0 to χ (Al) − χ (Cu) < 0 vs. E_vacuum = 0 eV) and self-charge (ΔV_cell ≥ +0.04 V under a 1842 Ω.cm_insulator resistor). The multivalent 5.5 mm thick layer cell filled with Li_2.99Ba_0.005ClO was the only one to display a potential bulk difference of 1.1 V. The lessons learned in this work may pave the way to understanding and designing more efficient energy harvesting and storage devices. Full article

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14 pages, 3348 KiB

Open AccessEditor’s ChoiceArticle

High-Performance and Low-Cost Membranes Based on Poly(vinylpyrrolidone) and Cardo-Poly(etherketone) Blends for Vanadium Redox Flow Battery Applications

by Tong Mu, Shifan Leng, Weiqin Tang, Ning Shi, Guorui Wang and Jingshuai Yang

Batteries 2022, 8(11), 230; https://doi.org/10.3390/batteries8110230 - 10 Nov 2022

Cited by 5 | Viewed by 2068

Abstract

Energy storage systems have aroused public interest because of the blooming development of intermittent renewable energy sources. Vanadium redox flow batteries (VRFBs) are the typical candidates owing to their flexible operation and good cycle durability. However, due to the usage of perfluorinated separator [...] Read more.

Energy storage systems have aroused public interest because of the blooming development of intermittent renewable energy sources. Vanadium redox flow batteries (VRFBs) are the typical candidates owing to their flexible operation and good cycle durability. However, due to the usage of perfluorinated separator membranes, VRFBs suffer from both high cost and serious vanadium ions cross penetration. Herein, we fabricate a series of low-budget and high-performance blend membranes from polyvinylpyrrolidone (PVP) and cardo-poly(etherketone) (PEKC) for VFRB. A PEKC network gives the membrane excellent mechanical rigidity, while PVP endows the blend membranes with superior sulfonic acid uptake owing to the present N-heterocycle and carbonyl group in PVP, resulting in low area resistance. Meanwhile, blend membranes also display low vanadium ion permeability resulting from the electrostatic repulsion effect of protonated PVP polymer chains towards vanadium ions. Consequently, the 50%PVP-PEKC membrane has a high ionic selectivity of 1.03 × 10⁶ S min cm⁻³, while that of Nafion 115 is nearly 17 times lower (6.03 × 10⁴ S min cm⁻³). The VRFB equipped with 50%PVP-PEKC membrane has high coulombic efficiencies (99.3–99.7%), voltage efficiencies (84.6–67.0%) and energy efficiencies (83.9–66.8%) at current densities of 80–180 mA cm⁻², and possesses excellent cycle constancy, indicating that low-cost x%PVP-PEKC blend membranes have a great application potentiality for VRFBs. Full article

(This article belongs to the Special Issue Promising Redox Flow Batteries)

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13 pages, 3994 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Thermal Propagation Modelling of Abnormal Heat Generation in Various Battery Cell Locations

by Ao Li, Anthony Chun Yin Yuen, Wei Wang, Jingwen Weng, Chun Sing Lai, Sanghoon Kook and Guan Heng Yeoh

Batteries 2022, 8(11), 216; https://doi.org/10.3390/batteries8110216 - 04 Nov 2022

Cited by 8 | Viewed by 2827

Abstract

With the increasing demand for energy capacity and power density in battery systems, the thermal safety of lithium-ion batteries has become a major challenge for the upcoming decade. The heat transfer during the battery thermal runaway provides insight into thermal propagation. A better [...] Read more.

With the increasing demand for energy capacity and power density in battery systems, the thermal safety of lithium-ion batteries has become a major challenge for the upcoming decade. The heat transfer during the battery thermal runaway provides insight into thermal propagation. A better understanding of the heat exchange process improves a safer design and enhances battery thermal management performance. This work proposes a three-dimensional thermal model for the battery pack simulation by applying an in-house model to study the internal battery thermal propagation effect under the computational fluid dynamics (CFD) simulation framework. The simulation results were validated with the experimental data. The detailed temperature distribution and heat transfer behaviour were simulated and analyzed. The thermal behaviour and cooling performance were compared by changing the abnormal heat generation locations inside the battery pack. The results indicated that various abnormal heat locations disperse heat to the surrounding coolant and other cells. According to the current battery pack setups, the maximum temperature of Row 2 cases can be increased by 2.93%, and the temperature difference was also increased. Overall, a new analytical approach has been demonstrated to investigate several stipulating battery thermal propagation scenarios for enhancing battery thermal performances. Full article

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18 pages, 6797 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Characteristic Prediction and Temperature-Control Strategy under Constant Power Conditions for Lithium-Ion Batteries

by Junfu Li, Shaochun Xu, Changsong Dai, Ming Zhao and Zhenbo Wang

Batteries 2022, 8(11), 217; https://doi.org/10.3390/batteries8110217 - 04 Nov 2022

Cited by 3 | Viewed by 1588

Abstract

Accurate characteristic prediction under constant power conditions can accurately evaluate the capacity of lithium-ion battery output. It can also ensure safe use for new-energy vehicles and electrochemical energy storage. As the battery voltage continues to drop under constant power conditions, the battery current [...] Read more.

Accurate characteristic prediction under constant power conditions can accurately evaluate the capacity of lithium-ion battery output. It can also ensure safe use for new-energy vehicles and electrochemical energy storage. As the battery voltage continues to drop under constant power conditions, the battery current output will accordingly increase, which brings a risk of thermal runaway in instances of weak heat dissipation. Therefore, knowing how to control the battery temperature is very critical for safe use. At present, the model-based method for characteristic prediction and temperature control has been used by most scholars, and that is also the key to this method. This work firstly extends a cell model to a pack-based electrochemical two-dimensional thermal coupling model, considering the heterogeneity of different cells inside the pack, and obtains the model parameters for a prismatic lithium-ion battery with a rated capacity of 42 Ah. Characteristic prediction under constant power conditions is then conducted based on an iterative solution method. Validations of characteristic prediction indicate the convenience of the developed models, with average absolute errors of voltage and temperature less than 36 mV and 0.4 K, respectively, and power error less than 0.005%. Finally, two model-based temperature feed-forward control strategies with lower cooling costs and shorter prediction times were developed based on the battery characteristic predictions, which leaves room for further controller development. Full article

(This article belongs to the Section Battery Modelling, Simulation, Management and Application)

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12 pages, 2597 KiB

Open AccessEditor’s ChoiceArticle

“In Situ” Formation of Zn Anode from Bimetallic Cu-Zn Alloy (Brass) for Dendrite-Free Operation of Zn-Air Rechargeable Battery

by Tibor Nagy, Lajos Nagy, Zoltán Erdélyi, Eszter Baradács, György Deák, Miklós Zsuga and Sándor Kéki

Batteries 2022, 8(11), 212; https://doi.org/10.3390/batteries8110212 - 03 Nov 2022

Cited by 7 | Viewed by 2208

Abstract

In this article, the performance of brass electrode was investigated in a Zn-air (charcoal-based cathode) rechargeable battery. The construction of the battery was carried out with biodegradable materials, namely a cotton cloth diaphragm and carboxymethyl cellulose sodium salt (CMC-Na) viscosity modifier, while the [...] Read more.

In this article, the performance of brass electrode was investigated in a Zn-air (charcoal-based cathode) rechargeable battery. The construction of the battery was carried out with biodegradable materials, namely a cotton cloth diaphragm and carboxymethyl cellulose sodium salt (CMC-Na) viscosity modifier, while the battery skeleton was printed by 3D printing technology. The brass acted as a collector and a preferable surface for the metallic Zn deposition on the brass anode surface. The electrochemical behavior of the brass anode was investigated by cyclic voltammetry (CV). Cyclic performance tests were carried out, which showed stable cell operation even in the presence or absence of additives up to more than 100 cycles. Furthermore, high energy (E_eff) and Coulomb (C_eff) efficiencies, 80% (E_eff), 95% (C_eff), 75% (E_eff), and 95% (C_eff) were obtained, respectively. The Shepherd model was applied to describe the discharging processes of the Zn-air battery containing brass as anode in the presence of additive-free electrolyte or electrolyte with CMC-Na salt additive. It was found that the Shepherd equation described only approximately the resulting discharge curves. In order to attain a more precise mathematical description, stretched exponential function was implemented into the last term of the Shepherd equation. The need for such a correction shows the complexity of the electrochemical processes occurring in these systems. In addition, the surface of the brass anode was also investigated by scanning electron microscopy (SEM) and the composition of the brass alloys was determined by X-ray fluorescence spectroscopy (XRF). Importantly, the formation of dendritic deposition was successfully suppressed and a smooth and uniform surface was obtained after the cycling tests. Full article

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17 pages, 2930 KiB

Open AccessEditor’s ChoiceArticle

Effects of Excessive Prelithiation on Full-Cell Performance of Li-Ion Batteries with a Hard-Carbon/Nanosized-Si Composite Anode

by Yusuke Abe, Ippei Saito, Masahiro Tomioka, Mahmudul Kabir and Seiji Kumagai

Batteries 2022, 8(11), 210; https://doi.org/10.3390/batteries8110210 - 02 Nov 2022

Cited by 2 | Viewed by 2117

Abstract

The effects of excessive prelithiation on the full-cell performance of Li-ion batteries (LIBs) with a hard-carbon/nanosized-Si (HC/N-Si) composite anode were investigated; HC and N-Si simply mixed at mass ratios of 9:1 and 8:2 were analyzed. CR2032-type half- and full-cells were assembled to evaluate [...] Read more.

The effects of excessive prelithiation on the full-cell performance of Li-ion batteries (LIBs) with a hard-carbon/nanosized-Si (HC/N-Si) composite anode were investigated; HC and N-Si simply mixed at mass ratios of 9:1 and 8:2 were analyzed. CR2032-type half- and full-cells were assembled to evaluate the electrochemical LIB anode behavior. The galvanostatic measurements of half-cell configurations revealed that the composite anode with an 8:2 HC/N-Si mass ratio exhibited a high capacity (531 mAh g⁻¹) at 0.1 C and superior current-rate dependence (rate performance) at 0.1–10 C. To evaluate the practical LIB anode performance, the optimally performing composite anode was used in the full cell. Prior to full-cell assembly, the composite anodes were prelithiated via electrochemical Li doping at different cutoff anodic specific capacities (200–600 mAh g⁻¹). The composite anode was paired with a LiNi_0.5Co_0.2Mn_0.3O₂ cathode to construct full-cells, the performance of which was evaluated by conducting sequential rate and cycling performance tests. Prelithiation affected only the cycling performance, without affecting the rate performance. Excellent capacity retention was observed in the full-cells with prelithiation conducted at cutoff anodic specific capacities greater than or equal to 500 mAh g⁻¹. Full article

(This article belongs to the Special Issue Feature Papers to Celebrate the First Impact Factor of Batteries)

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18 pages, 6508 KiB

Open AccessEditor’s ChoiceArticle

Physics-Based SoH Estimation for Li-Ion Cells

by Pietro Iurilli, Claudio Brivio, Rafael E. Carrillo and Vanessa Wood

Batteries 2022, 8(11), 204; https://doi.org/10.3390/batteries8110204 - 01 Nov 2022

Cited by 11 | Viewed by 3849

Abstract

Accurate state of health (SoH) estimation is crucial to optimize the lifetime of Li-ion cells while ensuring safety during operations. This work introduces a methodology to track Li-ion cells degradation and estimate SoH based on electrochemical impedance spectroscopy (EIS) measurements. Distribution of relaxation [...] Read more.

Accurate state of health (SoH) estimation is crucial to optimize the lifetime of Li-ion cells while ensuring safety during operations. This work introduces a methodology to track Li-ion cells degradation and estimate SoH based on electrochemical impedance spectroscopy (EIS) measurements. Distribution of relaxation times (DRT) were exploited to derive indicators linked to the so-called degradation modes (DMs), which group the different aging mechanisms. The combination of these indicators was used to model the aging progression over the whole lifetime (both in the “pre-knee” and “after-knee” regions), enabling a physics-based SoH estimation. The methodology was applied to commercial cylindrical cells (NMC811|Graphite SiO_x). The results showed that loss of lithium inventory (LLI) is the main driving factor for cell degradation, followed by loss of cathode active material (LAM_C). SoH estimation was achievable with a mean absolute error lower than 0.75% for SoH values higher than 85% and lower than 3.70% SoH values between 85% and 80% (end of life). The analyses of the results will allow for guidelines to be defined to replicate the presented methodology, characterize new Li-ion cell types, and perform onboard SoH estimation in battery management system (BMS) solutions. Full article

(This article belongs to the Collection Recent Advances in Battery Management Systems)

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33 pages, 7304 KiB

Open AccessEditor’s ChoiceReview

Review of the Research Status of Cost-Effective Zinc–Iron Redox Flow Batteries

by Huan Zhang, Chuanyu Sun and Mingming Ge

Batteries 2022, 8(11), 202; https://doi.org/10.3390/batteries8110202 - 31 Oct 2022

Cited by 33 | Viewed by 5417

Abstract

Zinc–iron redox flow batteries (ZIRFBs) possess intrinsic safety and stability and have been the research focus of electrochemical energy storage technology due to their low electrolyte cost. This review introduces the characteristics of ZIRFBs which can be operated within a wide pH range, [...] Read more.

Zinc–iron redox flow batteries (ZIRFBs) possess intrinsic safety and stability and have been the research focus of electrochemical energy storage technology due to their low electrolyte cost. This review introduces the characteristics of ZIRFBs which can be operated within a wide pH range, including the acidic ZIRFB taking advantage of Fen+ with high solubility, the alkaline ZIRFB operating at a relatively high open-circuit potential and current densities, and the neutral ZIRFB providing a non-toxic, harmless, and mild environment. No matter what kind of ZIRFB, there are always zinc dendrites limiting areal capacity on the anode, which has become an obstacle that must be considered in zinc-based RFBs. Therefore, we focus on the current research progress, especially the summarizing and analysis of zinc dendrites, Fe(III) hydrolysis, and electrolytes. Given these challenges, this review reports the optimization of the electrolyte, electrode, membrane/separator, battery structure, and numerical simulations, aiming to promote the performance and development of ZIRFBs as a practical application technology. Based on these investigations, we also provide the prospects and development direction of ZIRFBs. Full article

(This article belongs to the Special Issue Redox Flow Batteries: Recent Advances and Perspectives)

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19 pages, 1972 KiB

Open AccessFeature PaperEditor’s ChoiceReview

Examining the Benefits of Using Boron Compounds in Lithium Batteries: A Comprehensive Review of Literature

by Changlin (Allen) Zheng

Batteries 2022, 8(10), 187; https://doi.org/10.3390/batteries8100187 - 17 Oct 2022

Cited by 8 | Viewed by 7026

Abstract

Boron and boron compounds have been extensively studied together in the history and development of lithium batteries, which are crucial to decarbonization in the automotive industry and beyond. With a wide examination of battery components, but a boron-centric approach to raw materials, this [...] Read more.

Boron and boron compounds have been extensively studied together in the history and development of lithium batteries, which are crucial to decarbonization in the automotive industry and beyond. With a wide examination of battery components, but a boron-centric approach to raw materials, this review attempts to summarize past and recent studies on the following: which boron compounds are studied in a lithium battery, in which parts of lithium batteries are they studied, what improvements are offered for battery performance, and what improvement mechanisms can be explained. The uniqueness of boron and its extensive application beyond batteries contextualizes the interesting similarity with some studies on batteries. At the end, the article aims to predict prospective trends for future studies that may lead to a more extensive use of boron compounds on a commercial scale. Full article

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