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Batteries, Volume 9, Issue 12 (December 2023) – 37 articles

Cover Story (view full-size image): The groundbreaking semi-dry process for LFP cathodes reduces solvent usage significantly, validated with a 1 wt.% PTFE binder to minimize inactive material. Extrusion screws with multiple kneading zones intensify PTFE stress, increasing fibrillation. The process yields a flexible cathode layer with a specific capacitance of 155 mAh g−1 at 0.1 C. Compared to conventional methods, it markedly enhances discharge capacity and overall energy output while reducing energy consumption. View this paper
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17 pages, 3331 KiB  
Article
Fabrication and Characterization of Plasma Sprayed TiO2 and Li4Ti5O12 Materials as All Active Material Lithium-Ion Battery Electrodes
Batteries 2023, 9(12), 598; https://doi.org/10.3390/batteries9120598 - 17 Dec 2023
Viewed by 1290
Abstract
Two strategies to increase battery energy density at the cell level are to increase electrode thickness and to reduce the amount of inactive electrode constituents. All active material (AAM) electrodes provide a route to achieve both of those aims toward high areal capacity [...] Read more.
Two strategies to increase battery energy density at the cell level are to increase electrode thickness and to reduce the amount of inactive electrode constituents. All active material (AAM) electrodes provide a route to achieve both of those aims toward high areal capacity electrodes. AAM electrodes are often fabricated using hydraulic compression processes followed by thermal treatment; however, additive manufacturing routes could provide opportunities for more time-efficient and geometry-flexible electrode fabrication. One possible route for additive manufacturing of AAM electrodes would be to employ plasma spray as a direct additive manufacturing technology, and AAM electrode fabrication using plasma spray will be the focus of the work herein. TiO2 and Li4Ti5O12 (LTO) powders were deposited onto stainless steel substrates via plasma spray processing to produce AAM battery electrodes, and evaluated with regards to material and electrochemical properties. The TiO2 electrodes delivered low electrochemical capacity, <12 mAh g−1, which was attributed to limitations of the initial feed powder. LTO plasma sprayed AAM electrodes had much higher capacity and were comparable in total capacity at a low rate of discharge to composite electrodes fabricated using the same raw powder feed material. LTO material and electrochemical properties were sensitive to the plasma spray conditions, suggesting that tuning the material microstructure and electrochemical properties is possible by controlling the plasma spray deposition parameters. Full article
(This article belongs to the Section Battery Processing, Manufacturing and Recycling)
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36 pages, 6313 KiB  
Article
Multiagent-Based Control for Plug-and-Play Batteries in DC Microgrids with Infrastructure Compensation
Batteries 2023, 9(12), 597; https://doi.org/10.3390/batteries9120597 - 15 Dec 2023
Viewed by 1471
Abstract
The influence of the DC infrastructure on the control of power-storage flow in micro- and smart grids has gained attention recently, particularly in dynamic vehicle-to-grid charging applications. Principal effects include the potential loss of the charge–discharge synchronization and the subsequent impact on the [...] Read more.
The influence of the DC infrastructure on the control of power-storage flow in micro- and smart grids has gained attention recently, particularly in dynamic vehicle-to-grid charging applications. Principal effects include the potential loss of the charge–discharge synchronization and the subsequent impact on the control stabilization, the increased degradation in batteries’ health/life, and resultant power- and energy-efficiency losses. This paper proposes and tests a candidate solution to compensate for the infrastructure effects in a DC microgrid with a varying number of heterogeneous battery storage systems in the context of a multiagent neighbor-to-neighbor control scheme. Specifically, the scheme regulates the balance of the batteries’ load-demand participation, with adaptive compensation for unknown and/or time-varying DC infrastructure influences. Simulation and hardware-in-the-loop studies in realistic conditions demonstrate the improved precision of the charge–discharge synchronization and the enhanced balance of the output voltage under 24 h excessively continuous variations in the load demand. In addition, immediate real-time compensation for the DC infrastructure influence can be attained with no need for initial estimates of key unknown parameters. The results provide both the validation and verification of the proposals under real operational conditions and expectations, including the dynamic switching of the heterogeneous batteries’ connection (plug-and-play) and the variable infrastructure influences of different dynamically switched branches. Key observed metrics include an average reduced convergence time (0.66–13.366%), enhanced output-voltage balance (2.637–3.24%), power-consumption reduction (3.569–4.93%), and power-flow-balance enhancement (2.755–6.468%), which can be achieved for the proposed scheme over a baseline for the experiments in question. Full article
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17 pages, 10873 KiB  
Article
A Two-State-Based Hybrid Model for Degradation and Capacity Prediction of Lithium-Ion Batteries with Capacity Recovery
Batteries 2023, 9(12), 596; https://doi.org/10.3390/batteries9120596 - 15 Dec 2023
Viewed by 1293
Abstract
The accurate prediction of Li-ion battery capacity is important because it ensures mission and personnel safety during operations. However, the phenomenon of capacity recovery (CR) may impede the progress of improving battery capacity prediction performance. Therefore, in this study, we focus on the [...] Read more.
The accurate prediction of Li-ion battery capacity is important because it ensures mission and personnel safety during operations. However, the phenomenon of capacity recovery (CR) may impede the progress of improving battery capacity prediction performance. Therefore, in this study, we focus on the phenomenon of capacity recovery during battery degradation and propose a hybrid lithium-ion battery capacity prediction framework based on two states. First, to improve the density of capacity-related information, the simultaneous Markov blanket discovery algorithm (STMB) is used to screen the causal features of capacity from the initial feature set. Then, the life-long cycle sequence of batteries is partitioned into global degradation regions and recovery regions, as part of the proposed prediction framework. The prediction branch for the global degradation region is implemented through a long short-term memory network (LSTM) and the other prediction branch for the recovery region is implemented through Gaussian process regression (GPR). A support vector machine (SVM) model is applied to identify recovery points to switch the branch of the prediction framework. The prediction results are integrated to obtain the final prediction results. Experimental studies based on NASA’s lithium battery aging data highlight the trustworthy capacity prediction ability of the proposed method considering the capacity recovery phenomenon. In contrast to the comparative methods, the mean absolute error and the root mean square error are reduced by up to 0.0013 Ah and 0.0043 Ah, which confirms the validity of the proposed method. Full article
(This article belongs to the Special Issue State-of-the-Art in Battery Management Systems)
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12 pages, 2695 KiB  
Article
Percolation Behavior of a Sulfide Electrolyte–Carbon Additive Matrix for Composite Cathodes in All-Solid-State Batteries
Batteries 2023, 9(12), 595; https://doi.org/10.3390/batteries9120595 - 15 Dec 2023
Viewed by 1487
Abstract
To achieve high energy densities with sufficient cycling performance in all-solid-state batteries, the fraction of active material has to be maximized while maintaining ionic and electronic conduction throughout the composite cathode. It is well known that low-surface-area carbon additives added to the composite [...] Read more.
To achieve high energy densities with sufficient cycling performance in all-solid-state batteries, the fraction of active material has to be maximized while maintaining ionic and electronic conduction throughout the composite cathode. It is well known that low-surface-area carbon additives added to the composite cathode enhance the rate capability; however, at the same time, they can lead to rapid decomposition of the solid electrolyte in thiophosphate-based cells. Thus, the fraction of such conductive additives has to be well balanced. Within this study we determined the electronic percolation threshold of a conducting matrix consisting of Li6PS5Cl and C65. Furthermore, we systematically investigated the microstructure and effective conductivity (σeff) of the conducting matrix. The percolation threshold pc was determined as ~4 wt.-% C65, and it is suggested that below pc, the ionic contribution is dominant, which can be seen in temperature-dependent σeff and blocked charge transport at low frequencies. Above pc, the impedance of the conducting matrix becomes frequency-independent, and the ohmic law applies. Thus, the conducting matrix in ASSB can be regarded as an electronic and ionic conducting phase between active material particles. Additionally, guidelines are provided to enable electronic conduction in the conducting matrix with minimal C65 content. Full article
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12 pages, 3656 KiB  
Article
Rational Design of a Cost-Effective Biomass Carbon Framework for High-Performance Lithium Sulfur Batteries
Batteries 2023, 9(12), 594; https://doi.org/10.3390/batteries9120594 - 15 Dec 2023
Viewed by 1538
Abstract
Lithium–sulfur (Li-S) batteries are the most attractive candidates for next-generation large-scale energy storage because of their high theoretical energy density and the affordability of sulfur. However, most of the reported research primarily concentrates on low sulfur loading (below 2 mgs cm−2 [...] Read more.
Lithium–sulfur (Li-S) batteries are the most attractive candidates for next-generation large-scale energy storage because of their high theoretical energy density and the affordability of sulfur. However, most of the reported research primarily concentrates on low sulfur loading (below 2 mgs cm−2) cathodes using binders and traditional collectors, thus undermining the expected energy density. Herein, a N, O co-doped carbon nanotube (N, O-CNT) decorated wood framework (WF), denoted as WF-CNT, was designed as a free-standing sulfur host, achieving high sulfur loading of 10 mgs cm−2. This unique cathode featured low tortuosity microchannels and a conductive framework, reducing the diffusion paths for both ions and electrons and accommodating the volume changes associated with sulfur. Moreover, the internal CNT forests effectively captured soluble lithium polysulfides (LiPSs) and catalyze their redox kinetic. Consequently, the S@WF-CNT-800 sample exhibited a high initial discharge capacity of 1438.2 mAh g−1 at a high current density of 0.5 A g−1. Furthermore, a reversible capacity of 404.5 mAh g−1 was obtained after 500 cycles with sulfur loading of 5 mgs cm−2 at 0.5 A g−1. This work may support the development of high sulfur loading cathodes utilizing cost-effective and sustainable biomass materials for Li-S batteries. Full article
(This article belongs to the Special Issue Lithium-Sulfur Batteries: Research Progress of Key Materials)
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16 pages, 2918 KiB  
Article
Qualitative Characterization of Lead–Acid Batteries Fabricated Using Different Technological Procedures: An EIS Approach
Batteries 2023, 9(12), 593; https://doi.org/10.3390/batteries9120593 - 14 Dec 2023
Viewed by 1168
Abstract
Electrochemical impedance spectroscopy techniques were applied in this work to nine industrially fabricated lead–acid battery prototypes, which were divided into three type/technology packages. Frequency-dependent impedance changes were interpreted during successive charge/discharge cycles in two distinct stages: (1) immediately after fabrication and (2) after [...] Read more.
Electrochemical impedance spectroscopy techniques were applied in this work to nine industrially fabricated lead–acid battery prototypes, which were divided into three type/technology packages. Frequency-dependent impedance changes were interpreted during successive charge/discharge cycles in two distinct stages: (1) immediately after fabrication and (2) after a controlled aging procedure to 50% depth of discharge following industrial standards. To investigate their state of health behavior vs. electrical response, three methods were employed, namely, the Q-Q0 total charge analysis, the decay values of the constant-phase element in the equivalent Randles circuits, and the resonance frequency of the circuit. A direct correlation was found for the prediction of the best-performing batteries in each package, thus allowing for a qualitative analysis that was capable of providing the decay of the batteries’ states of health. We found which parameters were directly connected with their lifetime performance in both stages and, as a consequence, which type/technology battery prototype displayed the best performance. Based on this methodology, industrial producers can further establish the quality of novel batteries in terms of performance vs. lifespan, allowing them to validate the novel technological innovations implemented in the current prototypes. Full article
(This article belongs to the Special Issue Electrochemistry of Lead-Acid Batteries)
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22 pages, 8659 KiB  
Article
Optimizing the Location of Frequency Regulation Energy Storage Systems for Improved Frequency Stability
Batteries 2023, 9(12), 592; https://doi.org/10.3390/batteries9120592 - 14 Dec 2023
Viewed by 1163
Abstract
The installation of battery energy storage systems (BESSs) with various shapes and capacities is increasing due to the continuously rising demand for renewable energy. To prepare for potential accidents, a study was conducted to select the optimal location for installing an input BESS [...] Read more.
The installation of battery energy storage systems (BESSs) with various shapes and capacities is increasing due to the continuously rising demand for renewable energy. To prepare for potential accidents, a study was conducted to select the optimal location for installing an input BESS in terms of frequency stability when the index assumes the backup input of the BESS. This study builds on the premise that installing a BESS on a bus in an area where active power absorption and transmission are the most active can significantly contribute to increasing the frequency recovery of the power system. Based on this premise, the magnitude of the active power flow and the proportional characteristics of the phase difference between buses were mathematically confirmed. This study also calculated the effective power sensitivity index of a bus with 13 FR-ESSs installed in a domestic system and reviewed the frequency output by establishing a table for each failure scenario. The results indicated that the effect of frequency rise can be estimated at the level of tidal current calculation. Thus, the study suggested a direction for subsequent studies to improve the sensitivity index. Full article
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18 pages, 13652 KiB  
Review
Traditional and Iterative Group-IV Material Batteries through Ion Migration
Batteries 2023, 9(12), 591; https://doi.org/10.3390/batteries9120591 - 14 Dec 2023
Viewed by 1400
Abstract
In this review, we emphasize the significant potential of carbon group element-based (Group-IV) electrochemical energy devices prepared on the basis of ion migration in the realm of high-efficiency batteries. Based primarily on our group research findings, we elucidate the key advantages of traditional [...] Read more.
In this review, we emphasize the significant potential of carbon group element-based (Group-IV) electrochemical energy devices prepared on the basis of ion migration in the realm of high-efficiency batteries. Based primarily on our group research findings, we elucidate the key advantages of traditional Group-IV materials as electrodes in ion batteries powered by metal ion migration. Subsequently, we delve into the operational principles and research progress of iterative Group-IV material moisture ion batteries, driven by ion migration through external moisture. Finally, considering the practical challenges and issues in real-world applications, we offer prospects for the development and commercialization of Group-IV materials utilizing ion migration in both conventional and next-generation battery technologies. Full article
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11 pages, 2262 KiB  
Article
Analysis of Ni-Rich Cathode Composite Electrode Performance According to the Conductive Additive Distribution for Application in Sulfide All-Solid-State Lithium-Ion Batteries
Batteries 2023, 9(12), 590; https://doi.org/10.3390/batteries9120590 - 14 Dec 2023
Viewed by 1366
Abstract
All-solid-state lithium-ion batteries (ASSLBs) represent a promising breakthrough in battery technology owing to their high energy density and exceptional stability. When crafting cathode electrodes for ASSLBs, the solid electrolyte/cathode material interface is physically hindered by the specific morphology of carbon additive materials. In [...] Read more.
All-solid-state lithium-ion batteries (ASSLBs) represent a promising breakthrough in battery technology owing to their high energy density and exceptional stability. When crafting cathode electrodes for ASSLBs, the solid electrolyte/cathode material interface is physically hindered by the specific morphology of carbon additive materials. In this paper, we examine the distribution of conductive additives within the electrode and its impact on the electrochemical performance of composites incorporating either nano-sized carbon black (CB) or micron-sized carbon nanofibers (CNF) into Ni-rich (LiNi0.8Co0.1Mn0.1O2) cathode material based composites. When nano-sized CB is employed as a conductive additive, it enhances the electrical conductivity of the composite by adopting a uniform distribution. However, its positioning between the solid electrolyte and cathode material leads to an increase in interfacial resistance during charge and discharge cycles, resulting in decreased electrochemical performance. In contrast, using micron-sized CNF as a conductive additive results in a reduction in the composite’s electrical conductivity compared to CB. Nevertheless, due to the comparatively uninterrupted interfaces between the solid electrolyte and cathode materials, it exhibits superior electrochemical characteristics. Our findings are expected to aid the fabrication of electrochemical-enhanced cathode composite electrodes for ASSLBs. Full article
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14 pages, 2280 KiB  
Article
Advances in the Separation of Graphite from Lithium Iron Phosphate from End-of-Life Batteries Shredded Fine Fraction Using Simple Froth Flotation
Batteries 2023, 9(12), 589; https://doi.org/10.3390/batteries9120589 - 13 Dec 2023
Viewed by 1644
Abstract
Olivine-type lithium iron phosphate (LiFePO4, LFP) lithium-ion batteries (LIBs) have become a popular choice for electric vehicles (EVs) and stationary energy storage systems. In the context of recycling, this study addresses the complex challenge of separating black mass of spent LFP [...] Read more.
Olivine-type lithium iron phosphate (LiFePO4, LFP) lithium-ion batteries (LIBs) have become a popular choice for electric vehicles (EVs) and stationary energy storage systems. In the context of recycling, this study addresses the complex challenge of separating black mass of spent LFP batteries from its main composing materials to allow for direct recycling. In this study, 71% copper and 81% aluminium foil impurities were removed by sieving black mass to <250 µm. Next, the application of froth flotation as a separation technique was explored, examining the influence of chemical agents, pre-treatment, and multi-step processes. Frother agent addition improved material recovery in the froth, while collector addition influenced the separation efficiency and enhanced graphite recovery. Pre-treatment, particularly sonication, was found to break down agglomerates and further improve separation. Multi-step flotation increased the purity of recovered fractions. The optimized process for a black mass < 250 µm, involving sonication pre-treatment and double flotation, resulted in enriched carbonaceous material (80.3 mol%) in froth fractions and high LFP concentration (81.9 mol%) in tailings fractions. The recovered spent LFP cathode material contained 37.20 wt% Fe2P2O7, a degradation product of LiFePO4. This research offers valuable insights for the development of efficient battery recycling methods for LFP batteries. Full article
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14 pages, 2964 KiB  
Article
Ionic Liquid-Laden Zn-MOF-74-Based Solid-State Electrolyte for Sodium Batteries
Batteries 2023, 9(12), 588; https://doi.org/10.3390/batteries9120588 - 12 Dec 2023
Viewed by 1379
Abstract
Sodium batteries are receiving increasing interest as an alternative to reduce dependence on lithium-based systems. Furthermore, the development of solid-state electrolytes will lead to higher-performing and safer devices. In this work, a Zn-based metal–organic framework (Zn-MOF-74) is combined as a physical barrier against [...] Read more.
Sodium batteries are receiving increasing interest as an alternative to reduce dependence on lithium-based systems. Furthermore, the development of solid-state electrolytes will lead to higher-performing and safer devices. In this work, a Zn-based metal–organic framework (Zn-MOF-74) is combined as a physical barrier against the growth of dendrites, together with 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMIm][TFSI]) ionic liquid, which provides improved mobility to sodium ions. It is demonstrated that the incorporation of the appropriate amount of ionic liquid within the pores of the MOF produces a considerable increase in ionic conductivity, achieving values as high as 5 × 10−4 S cm−1 at room temperature, in addition to an acceptable Na+ transference number. Furthermore, the developed Na[EMIm][TFSI]@Zn-MOF-74 hybrid solid electrolyte contributes to stable and dendrite-free sodium plating/stripping for more than 100 h. Finally, a more than notable extension of the electrochemical stability window of the electrolyte has been determined, being useful even above 7 V vs. Na+/Na. Overall, this work presents a suitable strategy for the next generation of solid-state sodium batteries. Full article
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22 pages, 3507 KiB  
Article
Multi-Method Model for the Investigation of Disassembly Scenarios for Electric Vehicle Batteries
Batteries 2023, 9(12), 587; https://doi.org/10.3390/batteries9120587 - 12 Dec 2023
Viewed by 1380
Abstract
Disassembly is a pivotal technology to enable the circularity of electric vehicle batteries through the application of circular economy strategies to extend the life cycle of battery components through solutions such as remanufacturng, repurposing, and efficient recycling, ultimately reintegrating gained materials into the [...] Read more.
Disassembly is a pivotal technology to enable the circularity of electric vehicle batteries through the application of circular economy strategies to extend the life cycle of battery components through solutions such as remanufacturng, repurposing, and efficient recycling, ultimately reintegrating gained materials into the production of new battery systems. This paper aims to develop a multi-method self-configuring simulation model to investigate disassembly scenarios, taking into account battery design as well as the configuration and layout of the disassembly station. We demonstrate the developed model in a case study using a Mercedes–Benz battery and the automated disassembly station of the DeMoBat project at Fraunhofer IPA. Furthermore, we introduce two disassembly scenarios: component-oriented and accessibility-oriented disassembly. These scenarios are compared using the simulation model to determine several indicators, including the frequency of tool change, the number and distribution of robot routes, tool utilization, and disassembly time. Full article
(This article belongs to the Special Issue Advances in Battery Electric Vehicles)
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10 pages, 4986 KiB  
Article
Hierarchical CaMn2O4/C Network Framework toward Aqueous Zn Ion Hybrid Capacitors as Competitive Cathodes
Batteries 2023, 9(12), 586; https://doi.org/10.3390/batteries9120586 - 12 Dec 2023
Viewed by 1134
Abstract
Manganese-based materials have received more attention as cathodes for aqueous zinc ion hybrid capacitors (AZIHCs) due to their advantages such as abundant reserves, low cost, and large theoretical capacity. However, manganese-based materials have the disadvantage of poor electrical conductivity. Herein, a solid-phase method [...] Read more.
Manganese-based materials have received more attention as cathodes for aqueous zinc ion hybrid capacitors (AZIHCs) due to their advantages such as abundant reserves, low cost, and large theoretical capacity. However, manganese-based materials have the disadvantage of poor electrical conductivity. Herein, a solid-phase method was used to synthesize a hierarchical carbon-coated calcium manganate (CaMn2O4/C) network framework as the cathode for AZIHCs. Thanks to the unique structural/componential merits including conductive carbon coating and hierarchical porous architecture, the achieved CaMn2O4/C cathode shows an exceptionally long life of close to 5000 cycles at 2.0 A g−1, with a reversible specific capacity of 195.6 mAh g−1. The assembled CaMn2O4/C-based AZIHCs also display excellent cycling stability with a capacity retention rate of 84.9% after 8000 cycles at 1.0 A g−1, and an energy density of 21.3 Wh kg−1 at an output power density of 180.0 W kg−1. Full article
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28 pages, 12894 KiB  
Article
A Novel Method for State of Health Estimation of Lithium-Ion Batteries Based on Deep Learning Neural Network and Transfer Learning
Batteries 2023, 9(12), 585; https://doi.org/10.3390/batteries9120585 - 12 Dec 2023
Viewed by 1398
Abstract
Accurate state of health (SOH) estimation of lithium-ion batteries is critical for maintaining reliable and safe working conditions for electric vehicles (EVs). The machine learning-based method with health features (HFs) is encouraging for health prognostics. However, the machine learning method assumes that the [...] Read more.
Accurate state of health (SOH) estimation of lithium-ion batteries is critical for maintaining reliable and safe working conditions for electric vehicles (EVs). The machine learning-based method with health features (HFs) is encouraging for health prognostics. However, the machine learning method assumes that the training and testing data have the same distribution, which restricts its application for different types of batteries. Thus, in this paper, a deep learning neural network and fine-tuning-based transfer learning strategy are proposed for accurate and robust SOH estimation toward different types of batteries. First, a universal HF extraction strategy is proposed to obtain four highly related HFs. Second, a deep learning neural network consisting of long short-term memory (LSTM) and fully connected layers is established to model the relationship between the HFs and SOH. Third, the fine-tuning-based transfer learning strategy is exploited for SOH estimation of various types of batteries. The proposed methods are comprehensively verified using three open-source datasets. Experimental results show that the proposed deep learning neural network with the HFs can estimate the SOH accurately in a single dataset without using the transfer learning strategy where the mean absolute error (MAE) and root mean square error (RMSE) are constrained to 1.21% and 1.83%. For the transfer learning between different aging datasets, the overall MAE and RMSE are limited to 1.09% and 1.41%, demonstrating the reliability of the fine-tuning strategy. Full article
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17 pages, 5358 KiB  
Article
Design of Hierarchical Nickel-Cobalt Phosphide/Nickel Oxide with Tunable Electronic Structure and Strong Chemical Interface for Advanced Supercapacitors
Batteries 2023, 9(12), 584; https://doi.org/10.3390/batteries9120584 - 12 Dec 2023
Viewed by 1218
Abstract
The design of a reasonable heterostructure electrode to achieve enhanced areal performance for supercapacitors remains a great challenge. Here, we constructed hierarchical porous NiCoP/NiO nanocomposites anchored on Ni foam with tunable electronic and structural properties, as well as robust interfacial interaction. In NiCoP/NiO, [...] Read more.
The design of a reasonable heterostructure electrode to achieve enhanced areal performance for supercapacitors remains a great challenge. Here, we constructed hierarchical porous NiCoP/NiO nanocomposites anchored on Ni foam with tunable electronic and structural properties, as well as robust interfacial interaction. In NiCoP/NiO, the interconnected NiO nanosheets serve as a carrier with enriched anchoring sites to confine the NiCoP and improve its stability. Meanwhile, the ultrathin NiCoP nanosheets with bimetallic centers are connected with porous NiO nanosheets to form a reliable heterojunction, enhancing the electrochemical reaction kinetics. Taking advantage of the synergistic contribution of bimetallic centers, phosphides and unique structure, the NiCoP/NiO delivers a high areal specific capacitance (1860 mF cm−2 at 5 mA cm−2), good rate performance of 78.5% at six times the increased current density, and remarkable durability (11.0% decrease after 10,000 cycles). Furthermore, the assembled hybrid supercapacitor NiCoP/NiO//porous-activated carbon (PAC) delivers a high areal energy density of 173.7 μWh cm−2 (116.4 μWh cm−2) at 1.6 mW cm−2 (32 mW cm−2). The results indicate that the design of the heterostructure interface with strong chemical interface and tunable electronic structure is an effective and promising approach to boost the electrochemical performance for advanced supercapacitors. Full article
(This article belongs to the Special Issue Transition Metal Complex for Electrochemical Energy Storage)
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15 pages, 3290 KiB  
Article
An Extended Kalman Filter Design for State-of-Charge Estimation Based on Variational Approach
Batteries 2023, 9(12), 583; https://doi.org/10.3390/batteries9120583 - 12 Dec 2023
Cited by 1 | Viewed by 1329
Abstract
State of charge (SOC) is a very important variable for using batteries safely and reliably. To improve the accuracy of SOC estimation, a novel variational extended Kalman filter (EKF) technique based on least square error method is herein provided by establishing [...] Read more.
State of charge (SOC) is a very important variable for using batteries safely and reliably. To improve the accuracy of SOC estimation, a novel variational extended Kalman filter (EKF) technique based on least square error method is herein provided by establishing a second-order equivalent circuit model for the battery. It was found that when SOC decreased, resistance polarization occurred in the electrochemical model, and the parameters in the equivalent RC model varied. To decrease the modeling error in the equivalent circuit model, the system parameters were identified online depending on the SOC’s estimated result. Through the SOC-estimation process, the variation theorem was introduced, which enabled the system parameters to track the real situations based on the output measured. The experiment results reveal the comparison of the SOC-estimation results of the variational EKF algorithm, the traditional EKF algorithm, the recursive least square (RLS) EKF algorithm, and the forgotten factor recursive least square (FFRLS) EKF algorithm based on different indices, including the mean square error (MSE) and the mean absolute error (MAE). The variational EKF algorithm provided in this paper has higher estimation accuracy and robustness than the traditional EKF, which verifies the superiority and effectiveness of the proposed method. Full article
(This article belongs to the Special Issue Advances in Battery Status Estimation and Prediction)
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18 pages, 1576 KiB  
Article
Aging and Homogenized Mechanical Character of Quasi-Statically Charged Gr-Si and NMC Based Electrodes Using Damage Material Modeling
Batteries 2023, 9(12), 582; https://doi.org/10.3390/batteries9120582 - 06 Dec 2023
Viewed by 1357
Abstract
Silicon-based, high-energy-density electrodes show severe microstructural degradation due to continuous expansion and contraction upon charging and discharging. This mechanical degradation behaviour affects the cell’s lifetime by changing the microstructure morphology, altering transport parameters, and active volume losses. Since direct experimental observations of mechanical [...] Read more.
Silicon-based, high-energy-density electrodes show severe microstructural degradation due to continuous expansion and contraction upon charging and discharging. This mechanical degradation behaviour affects the cell’s lifetime by changing the microstructure morphology, altering transport parameters, and active volume losses. Since direct experimental observations of mechanical degradation are challenging, we develop a computer simulation approach that is based on real three-dimensional electrode microstructures. By assuming quasi-static cycling and taking into account the mechanical properties of the electrode’s constituents we calculate the heterogeneous deformation and resulting morphological changes. Additionally, we implement an ageing model that allows us to compute a heterogeneously evolving damage field over multiple cycles. From the damage field, we infer the remaining electrode capacity. Using this technique, an anode blend of graphite particles and silicon carbon composite particles (SiC-C) as well as a cathode consisting of Lithium-Nickel-Manganese-Cobalt Oxide with molar ratio of 8:1:1 (NMC811) are studied. In a two-level homogenization approach, we compute, firstly, the effective mechanical properties of silicon composite particles and, secondly, the whole electrode microstructure. By introducing the damage strain ratio, the degradation evolution of the graphite SiC-C anode blend is studied for up to 95 charge-discharge cycles. With this work, we demonstrate an approach to how mechanical damage of battery electrodes can be treated efficiently. This is the basis for a full coupling to electrochemical simulations. Full article
(This article belongs to the Special Issue Materials Design for Electrochemical Energy Storage)
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18 pages, 5312 KiB  
Article
Processing of Aqueous Graphite–Silicon Oxide Slurries and Its Impact on Rheology, Coating Behavior, Microstructure, and Cell Performance
Batteries 2023, 9(12), 581; https://doi.org/10.3390/batteries9120581 - 05 Dec 2023
Cited by 1 | Viewed by 1656
Abstract
The mixing process is the basis of the electrode microstructure, which defines key cell performance indicators. This work investigated the effects of varying the energy input within the mixing procedure on slurry rheology, coating behavior, mechanical and electrical properties of dry electrodes and [...] Read more.
The mixing process is the basis of the electrode microstructure, which defines key cell performance indicators. This work investigated the effects of varying the energy input within the mixing procedure on slurry rheology, coating behavior, mechanical and electrical properties of dry electrodes and electrochemical performance of cells fabricated from these negative electrodes. Energy input differences were achieved by varying the solids content within the mixing procedure; however, the final total solids content of the slurries was always the same. The slurries, produced with graphite and silicon oxide as active materials and carboxymethylcellulose (CMC) and styrene-butadiene rubber as binders, showed large differences in flow behavior which were explained by changes in CMC adsorption and mechanical degradation because of increasing energy input. Low shear viscosity and the degree of shear thinning decreased with increasing energy input, resulting in a narrower stability window for slot-die coating. The resistance between the electrode and current collector decreased as more CMC was adsorbed on the active material. Electrode adhesion drastically dropped at the highest energy input, presumably due to a change in SBR distribution. Despite these variations, all fabricated pouch cells demonstrated excellent electrochemical performance and a slight trend of increased charge capability was observed in cells prepared with higher energy input. Full article
(This article belongs to the Section Battery Processing, Manufacturing and Recycling)
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26 pages, 1039 KiB  
Review
Navigating Battery Choices in IoT: An Extensive Survey of Technologies and Their Applications
Batteries 2023, 9(12), 580; https://doi.org/10.3390/batteries9120580 - 02 Dec 2023
Cited by 1 | Viewed by 1793
Abstract
In recent years, there has been significant progress in IoT solutions for a variety of fields. The real-time functionality and remote deployment of IoT solutions are two crucial aspects that are necessary for their successful implementation. To achieve this, external batteries play a [...] Read more.
In recent years, there has been significant progress in IoT solutions for a variety of fields. The real-time functionality and remote deployment of IoT solutions are two crucial aspects that are necessary for their successful implementation. To achieve this, external batteries play a major role. While lithium–ion batteries are often the go-to choice for IoT devices, it is essential to recognise that different IoT applications have unique needs. Therefore, it is important to conduct a thorough examination of existing battery solutions and their suitability for various IoT applications. This paper presents an extensive survey of different battery technologies, accompanied by an assessment of their applicability in different IoT applications. The aim is to offer a clear and practical guide for researchers and professionals seeking the best battery solutions for their IoT applications. Full article
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23 pages, 3026 KiB  
Review
The Review of Existing Strategies of End-of-Life Graphite Anode Processing Using 3Rs Approach: Recovery, Recycle, Reuse
Batteries 2023, 9(12), 579; https://doi.org/10.3390/batteries9120579 - 30 Nov 2023
Viewed by 1680
Abstract
While past recycling efforts have primarily concentrated on extracting valuable metals from discarded cathode materials, the focus is now shifting towards anode materials, particularly graphite, which makes up 10–20% of LIB mass. Escalating prices of battery-grade graphite and environmental considerations surrounding its production [...] Read more.
While past recycling efforts have primarily concentrated on extracting valuable metals from discarded cathode materials, the focus is now shifting towards anode materials, particularly graphite, which makes up 10–20% of LIB mass. Escalating prices of battery-grade graphite and environmental considerations surrounding its production highlight the significance of graphite recycling. This review categorizes methods for graphite recovery into three approaches: recovery, recycle, and reuse. Moreover, it explores their potential applications and comparative electrochemical performance analysis, shedding light on the promising prospects of utilizing spent graphite-based functional materials. The review underscores the importance of sustainable recycling practices to address the environmental and economic challenges posed by the proliferation of LIBs and the growing demand for graphite. Full article
(This article belongs to the Special Issue Recycling of Lithium-Ion Batteries: Processes and Technologies)
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26 pages, 2651 KiB  
Article
SoC Estimation in Lithium-Ion Batteries with Noisy Measurements and Absence of Excitation
Batteries 2023, 9(12), 578; https://doi.org/10.3390/batteries9120578 - 28 Nov 2023
Viewed by 1507
Abstract
Accurate State-of-Charge estimation is crucial for applications that utilise lithium-ion batteries. In real-time scenarios, battery models tend to present significant uncertainty, making it desirable to jointly estimate both the State of Charge and relevant unknown model parameters. However, parameter estimation typically necessitates that [...] Read more.
Accurate State-of-Charge estimation is crucial for applications that utilise lithium-ion batteries. In real-time scenarios, battery models tend to present significant uncertainty, making it desirable to jointly estimate both the State of Charge and relevant unknown model parameters. However, parameter estimation typically necessitates that the battery input signals induce a persistence of excitation property, a need which is often not met in practical operations. This document introduces a joint state of charge/parameter estimator that relaxes this stringent requirement. This estimator is based on the Generalized Parameter Estimation-Based Observer framework. To the best of the authors’ knowledge, this is the first time it has been applied in the context of lithium-ion batteries. Its advantages are demonstrated through simulations. Full article
(This article belongs to the Section Battery Modelling, Simulation, Management and Application)
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15 pages, 7594 KiB  
Article
Battery Impedance Spectroscopy Embedded Measurement System
Batteries 2023, 9(12), 577; https://doi.org/10.3390/batteries9120577 - 28 Nov 2023
Viewed by 1497
Abstract
The evolution of rechargeable battery characteristics have led to their use in almost every device in our everyday life. This importance has also increased the relevance of estimating the remaining battery charge (state of charge, SOC) and their health (state of health, SOH). [...] Read more.
The evolution of rechargeable battery characteristics have led to their use in almost every device in our everyday life. This importance has also increased the relevance of estimating the remaining battery charge (state of charge, SOC) and their health (state of health, SOH). One of the methods for the estimation of these parameters is based on the impedance spectroscopy obtained from the battery output impedance measured at multiple frequencies. This paper proposes an embedded measurement system capable of measuring the battery output impedance while in operation (either charging or supplying power to the intended device). The developed system generates a small amplitude stimulus that is added to the battery current. The system then measures the battery voltage and current to estimate the impedance at the stimulus frequencies. Three batteries were measured at different SOC levels, demonstrating the system principle of operation. Complementarily, a battery impedance equivalent circuit was used, together with genetic algorithms, to estimate the circuit parameters and assess their dependence on the battery SOC. Full article
(This article belongs to the Section Battery Modelling, Simulation, Management and Application)
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10 pages, 1035 KiB  
Article
Silicon Negative Electrodes—What Can Be Achieved for Commercial Cell Energy Densities
Batteries 2023, 9(12), 576; https://doi.org/10.3390/batteries9120576 - 28 Nov 2023
Viewed by 1283
Abstract
Historically, lithium cobalt oxide and graphite have been the positive and negative electrode active materials of choice for commercial lithium-ion cells. It has only been over the past ~15 years in which alternate positive electrode materials have been used. As new positive and [...] Read more.
Historically, lithium cobalt oxide and graphite have been the positive and negative electrode active materials of choice for commercial lithium-ion cells. It has only been over the past ~15 years in which alternate positive electrode materials have been used. As new positive and negative active materials, such as NMC811 and silicon-based electrodes, are being developed, it is crucial to evaluate the potential of these materials at a stack or cell level to fully understand the possible increases in energy density which can be achieved. Comparisons were made between electrode stack volumetric energy densities for designs containing either LCO or NMC811 positive electrode and silicon-graphite negative electrodes, where the weight percentages of silicon were evaluated between zero and ninety percent. Positive electrode areal loadings were evaluated between 2.00 and 5.00 mAh cm−2. NMC811 at 200 mAh g−1 has the ability to increase stack energy density between 11% and 20% over LCO depending on percentage silicon and areal loading. At a stack level, the percentage of silicon added results in large increases in energy density but delivers a diminishing return, with the greatest increase observed as the percentage of silicon is increased from zero percent to approximately 25–30%. Full article
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18 pages, 6076 KiB  
Article
Layer-Resolved Mechanical Degradation of a Ni-Rich Positive Electrode
Batteries 2023, 9(12), 575; https://doi.org/10.3390/batteries9120575 - 28 Nov 2023
Viewed by 1411
Abstract
The effects of electrochemical aging on the mechanical properties of electrodes in lithium-ion batteries are challenging to measure and are largely unknown. Mechanochemical degradation processes occur at different scales within an electrode and understanding the correlation between the degradation of mechanical properties, electrochemical [...] Read more.
The effects of electrochemical aging on the mechanical properties of electrodes in lithium-ion batteries are challenging to measure and are largely unknown. Mechanochemical degradation processes occur at different scales within an electrode and understanding the correlation between the degradation of mechanical properties, electrochemical aging, and morphological changes is crucial for mitigating battery performance degradation. This paper explores the evolution of mechanical and electrochemical properties at the layer level in a Ni-rich positive electrode during the initial stages of electrochemical cycling. The investigation involves complementary cross-section analyses aimed at unraveling the connection between observed changes on both macroscopic and microscopic scales. The macroscopic constitutive properties were assessed using a U-shaped bending test method that had been previously developed. The compressive modulus exhibited substantial dependency on both the porous structure and binder properties. It experienced a notable reduction with electrolyte wetting but demonstrated an increase with cycling and aging. During the initial stages of aging, electrochemical impedance spectra revealed increased local resistance near the particle–electrolyte interface. This is likely attributable to factors such as secondary particle grain separation and the redistribution of carbon black. The swelling of particles, compression of the binder phase, and enhanced particle contact were identified as probable factors adding to the elevation of the elastic modulus within the porous layer as a result of cycling. Full article
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24 pages, 5636 KiB  
Article
Selective Precipitation of Rare Earth Double Sulfate Salts from Industrial Ni–MH Battery Leachates: Impact of Downstream Processing on Product Quality
Batteries 2023, 9(12), 574; https://doi.org/10.3390/batteries9120574 - 28 Nov 2023
Viewed by 1329
Abstract
This work focuses on the recovery of rare earth elements (REEs = La, Ce, Nd, Pr) from spent nickel–metal hydride batteries by hydrometallurgical processing. The REEs were precipitated in the form of sodium-lanthanide double sulfate salts by adding Na2SO4 to [...] Read more.
This work focuses on the recovery of rare earth elements (REEs = La, Ce, Nd, Pr) from spent nickel–metal hydride batteries by hydrometallurgical processing. The REEs were precipitated in the form of sodium-lanthanide double sulfate salts by adding Na2SO4 to a leach liquor prepared from industrially processed spent batteries. The objectives were to better understand the parameters driving the purity of the product and to identify the phases involved, as well as their crystallographic structure. The methodology included experiments performed in a 2 L reactor, thermodynamic calculations and product characterization. We confirmed that high REE precipitation yields (>95%) can be achieved under a wide range of hydrodynamic conditions. Furthermore, we demonstrated and quantified how appropriately washing the product allows for a significant reduction in nickel losses while maintaining control over REE product purity. Finally, using X-ray Diffraction analyses, it was established that REEs form a solid solution with a chemical formula (Na0.9K0.1)(La0.65Ce0.24Pr0.04Nd0.07)(SO4)2·H2O, which has not been reported so far. Full article
(This article belongs to the Section Battery Processing, Manufacturing and Recycling)
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9 pages, 874 KiB  
Article
Disparate Redox Potentials in Mixed Isomer Electrolytes Reduce Voltage Efficiency of Energy Dense Flow Batteries
Batteries 2023, 9(12), 573; https://doi.org/10.3390/batteries9120573 - 27 Nov 2023
Viewed by 1507
Abstract
Electrolytes containing multiple redox couples are promising for improving the energy density of flow batteries. Here, two chelated chromium complexes that are structural isomers are characterized and combined to generate electrolytes containing up to 2 M of active species, corresponding to 53.6 Ah [...] Read more.
Electrolytes containing multiple redox couples are promising for improving the energy density of flow batteries. Here, two chelated chromium complexes that are structural isomers are characterized and combined to generate electrolytes containing up to 2 M of active species, corresponding to 53.6 Ah L−1. The mixed isomer approach enables a significantly higher active material content than the individual materials would allow, affording energy dense cells with Coulombic efficiencies of ≥99.6% at 100 mA cm−2 and an open circuit voltage of 1.65 V at 50% state-of-charge. This high concentration, however, comes with a caveat; at a given concentration, an equimolar mixed electrolyte leads to lower voltage efficiency compared to using the individual isomers, while Coulombic efficiency remains constant. Our work demonstrates that exploiting structural isomerism is an efficient approach to improve capacity, but active materials must be selected carefully in mixed systems as differences in operating potentials negatively affect energy efficiency. Full article
(This article belongs to the Special Issue Energy Storage of Redox-Flow Batteries)
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11 pages, 2262 KiB  
Article
Achieving Stable Copper Ion Storage in Layered Vanadium Pentoxide
Batteries 2023, 9(12), 572; https://doi.org/10.3390/batteries9120572 - 27 Nov 2023
Viewed by 1463
Abstract
Copper metal is a promising anode in aqueous batteries due to its low price, noble reaction potential (0.34 V), high theoretical specific capacity, abundance and chemical stability. However, only a few copper ion storage materials have been reported. Herein, layered vanadium pentoxide is [...] Read more.
Copper metal is a promising anode in aqueous batteries due to its low price, noble reaction potential (0.34 V), high theoretical specific capacity, abundance and chemical stability. However, only a few copper ion storage materials have been reported. Herein, layered vanadium pentoxide is chosen to store copper ions for the first time. Ex situ XRD reveals a unique two phase transition process during cycling. The V2O5 electrode shows stable copper ion storage performance. It delivers 91.9 mAh g−1 for the first cycle with a cycle life of as high as 4000 cycles at 1.0 A g−1. This work provides an intriguing copper ion storage material and expands the available options of electrode materials for copper ion storage. Full article
(This article belongs to the Special Issue High Performance Sodium Rechargeable Batteries and Beyond)
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22 pages, 4151 KiB  
Review
Second-Life Batteries: A Review on Power Grid Applications, Degradation Mechanisms, and Power Electronics Interface Architectures
Batteries 2023, 9(12), 571; https://doi.org/10.3390/batteries9120571 - 27 Nov 2023
Viewed by 2030
Abstract
The adoption of electric vehicles (EVs) is increasing due to governmental policies focused on curbing climate change. EV batteries are retired when they are no longer suitable for energy-intensive EV operations. A large number of EV batteries are expected to be retired in [...] Read more.
The adoption of electric vehicles (EVs) is increasing due to governmental policies focused on curbing climate change. EV batteries are retired when they are no longer suitable for energy-intensive EV operations. A large number of EV batteries are expected to be retired in the next 5–10 years. These retired batteries have 70–80% average capacity left. Second-life use of these battery packs has the potential to address the increasing energy storage system (ESS) demand for the grid and also to create a circular economy for EV batteries. The needs of modern grids for frequency regulation, power smoothing, and peak shaving can be met using retired batteries. Moreover, these batteries can also be employed for revenue generation for energy arbitrage (EA). While there are articles reviewing the general applications of retired batteries, this paper presents a comprehensive review of the research work on applications of the second-life batteries (SLBs) specific to the power grid and SLB degradation. The power electronics interface and battery management systems for the SLB are also thoroughly reviewed. Full article
(This article belongs to the Special Issue Second-Life Batteries)
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29 pages, 2896 KiB  
Review
Recent Research Progress on All-Solid-State Mg Batteries
Batteries 2023, 9(12), 570; https://doi.org/10.3390/batteries9120570 - 27 Nov 2023
Viewed by 1665
Abstract
Current Li battery technology employs graphite anode and flammable organic liquid electrolytes. Thus, the current Li battery is always facing the problems of low energy density and safety. Additionally, the sustainable supply of Li due to the scarce abundance of Li sources is [...] Read more.
Current Li battery technology employs graphite anode and flammable organic liquid electrolytes. Thus, the current Li battery is always facing the problems of low energy density and safety. Additionally, the sustainable supply of Li due to the scarce abundance of Li sources is another problem. An all-solid-state Mg battery is expected to solve the problems owing to non-flammable solid-state electrolytes, high capacity/safety of divalent Mg metal anode and high abundance of Mg sources; therefore, solid-state electrolytes and all-solid-state Mg batteries have been researched intensively last two decades. However, the realization of all-solid-state Mg batteries is still far off. In this article, we review the recent research progress on all-solid-state Mg batteries so that researchers can pursue recent research trends of an all-solid-state Mg battery. At first, the solid-state electrolyte research is described briefly in the categories of inorganic, organic and inorganic/organic composite electrolytes. After that, the recent research progress of all-solid-state Mg batteries is summarized and analyzed. To help readers, we tabulate electrode materials, experimental conditions and performances of an all-solid-state Mg battery so that the readers can find the necessary information at a glance. In the last, challenges to realize the all-solid-state Mg batteries are visited. Full article
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10 pages, 2834 KiB  
Article
Electrospun Si and Si/C Fiber Anodes for Li-Ion Batteries
Batteries 2023, 9(12), 569; https://doi.org/10.3390/batteries9120569 - 26 Nov 2023
Viewed by 1788
Abstract
Due to structural changes in silicon during lithiation/delithiation, most Li-ion battery anodes containing silicon show rapid gravimetric capacity fade upon charge/discharge cycling. Herein, we report on a new Si powder anode in the form of electrospun fibers with only poly(acrylic acid) (PAA) binder [...] Read more.
Due to structural changes in silicon during lithiation/delithiation, most Li-ion battery anodes containing silicon show rapid gravimetric capacity fade upon charge/discharge cycling. Herein, we report on a new Si powder anode in the form of electrospun fibers with only poly(acrylic acid) (PAA) binder and no electrically conductive carbon. The performance of this anode was contrasted to a fiber mat composed of Si powder, PAA binder, and a small amount of carbon powder. Fiber mat electrodes were evaluated in half-cells with a Li metal counter/reference electrode. Without the addition of conductive carbon, a stable capacity of about 1500 mAh/g (normalized to the total weight of the anode) was obtained at 1C for 50 charge/discharge cycles when the areal loading of silicon was 0.30 mgSi/cm2, whereas a capacity of 800 mAh/g was obtained when the Si loading was increased to ~1.0 mgSi/cm2. On a Si weight basis, these capacities correspond to >3500 mAh/gSi. The capacities were significantly higher than those found with a slurry-cast powdered Si anode with PAA binder. There was no change in fiber anode performance (gravimetric capacity and constant capacity with cycling) when a small amount of electrically conductive carbon was added to the electrospun fiber anodes when the Si loading was ≤1.0 mgSi/cm2. Full article
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