Editor’s Choice Articles

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

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

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

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

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

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

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

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

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

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

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

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 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

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

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

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

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

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

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

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

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

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

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

As the electrification sector expands rapidly, the demand for metals used in batteries is increasing significantly. New approaches for lithium-ion battery (LIB) recycling have to be investigated and new technologies developed in order to secure the future supply of battery metals (i.e., lithium, cobalt, nickel). In this work, the possibility of integrating LIB recycling with secondary copper smelting was further investigated. The time-dependent behavior of battery metals (Li, Co, Ni, Mn) in simulated secondary copper smelting conditions was investigated for the first time. In the study, copper alloy was used as a medium for collecting valuable metals and the distribution coefficients of these metals between copper alloy and slag were used for evaluating the recycling efficiencies. The determined distribution coefficients follow the order Ni >> Co >> Mn > Li throughout the time range investigated. In our study, the evolution of phases and their chemical composition were investigated in laboratory-scale experiments under reducing conditions of oxygen partial pressure p(O₂) = 10⁻¹⁰ atm, at 1300 °C. The results showed that already after 1 h holding time, the major elements were in equilibrium. However, based on the microstructural observations and trace elements distributions, the required full equilibration time for the system was determined to be 16 h. Full article

Nowadays, face masks play an essential role in limiting coronavirus diffusion. However, their disposable nature represents a relevant environmental issue. In this work, we propose the utilization of two types of disposed (waste) face masks to prepare hard carbons (biochar) by pyrolytic conversion in mild conditions. Moreover, we evaluated the application of the produced hard carbons as anode materials in Na-ion batteries. Pristine face masks were firstly analyzed through infrared spectroscopy and thermogravimetric analysis. The pyrolysis of both mask types resulted in highly disordered carbons, as revealed by field-emission scanning electron microscopy and Raman spectroscopy, with a very low specific surface area. Anodes prepared with these carbons were tested in laboratory-scale Na-metal cells through electrochemical impedance spectroscopy, cyclic voltammetry and galvanostatic cycling, displaying an acceptable specific capacity along a wide range of current regimes, with a good coulombic efficiency (>98% over at least 750 cycles). As a proof of concept, the anodes were also used to assemble a Na-ion cell in combination with a Na₃V₂(PO₄)₂F₃ (NVPF) cathode and tested towards galvanostatic cycling, with an initial capacity of almost 120 mAhg⁻¹ (decreasing at about 47 mAhg⁻¹ after 50 cycles). Even though further optimization is required for a real application, the achieved electrochemical performances represent a preliminary confirmation of the possibility of repurposing disposable face masks into higher-value materials for Na-ion batteries. Full article

A constant and homogenous temperature control of Li-ion batteries is essential for a good performance, a safe operation, and a low aging rate. Especially when operating a battery with high loads in dense battery systems, a cooling system is required to keep the cell in a controlled temperature range. Therefore, an existing battery module is set up with a water-based liquid cooling system with aluminum cooling plates. A finite-element simulation is used to optimize the design and arrangement of the cooling plates regarding power consumption, cooling efficiency, and temperature homogeneity. The heat generation of an operating Li-ion battery is described by the lumped battery model, which is integrated into COMSOL Multiphysics. As the results show, a small set of non-destructively determined parameters of the lumped battery model is sufficient to estimate heat generation. The simulated temperature distribution within the battery pack confirmed adequate cooling and good temperature homogeneity as measured by an integrated temperature sensor array. Furthermore, the simulation reveals sufficient cooling of the batteries by using only one cooling plate per two pouch cells while continuously discharging at up to 3 C. Full article

This paper presents three equivalent thermal circuit models with multiple input parameters, namely, the state of health (SOH), state of charge (SOC), current and temperature. Typical physiochemical models include parameters such as porosity and tortuosity, which are not easily experimentally available; this model allows for model parameters such as the internal impedance to be easily estimated using more practical inputs. The paper models the internal impedance resistance of a LiFePO₄ battery at five different ambient temperatures (5, 15, 25, 35, 45 °C), at three different discharge rates (1C, 2C, 3C) and at three different SOHs (90%, 83%, 65%). The internal impedance surface fit experimental measurements with a Pearson coefficient of 0.945. Three thermal models were then created that implemented the internal resistance model. The first two thermal models were 0D models that did not include the influence of the thermal conductivity of the battery. The first model assumed simple heating through internal resistance and convection energy loss, while the second also included the Bernardi Reversible heat term. The final third model was a 2D model that included all previous heat source terms as well as tab heating. The 2D model was solved using a simple Euler method and finite center difference. The R² values for the 0D thermal models were 0.9964 and 0.9962 for the simple internal resistance and reversible heating models, respectively. The R² value for the 2D thermal model was 0.996. Full article

This paper deals with the development and experimental validation of a unified power converter for application in dc microgrids, contemplating the inclusion of solar photovoltaic (PV) panels and energy storage systems (ESS), namely batteries. Considering the limitations presented by the current structure of the power grid, mostly highlighted by the accentuated integration of emerging technologies (ESS, renewables, electric vehicles, and electrical appliances that natively operate in dc), it is extremely pertinent to adopt new topologies, architectures, and paradigms. In particular, decentralized power systems, unified topologies, and correspondent control algorithms are representative of a new trend towards a reduction in the number of power converters. Thus, the developed solution is designed to operaSAVE-15te at a nominal power of 3.6 kW, with a switching frequency of 100 kHz, and in four operation modes concerning power flow: (i) solar PV panels to batteries (PV2B); (ii) solar PV panels to dc grid (PV2G); (iii) batteries to dc grid (B2G); (iv) dc grid to batteries (G2B). Moreover, a dual active bridge converter guarantees galvanic isolation, while two back-end dc–dc converters are responsible for interfacing solar PV panels and batteries. The experimental validation of the proposed unified power converter proves its application value to self-consumption production units. Full article

The novelty of this study is to suggest a novel design for electric vehicle charging stations using fuel cell technology. The proposed system benefits from the Organic Rankine Cycle (ORC) to utilize the exhaust energy of the Solid Oxide Fuel Cell (SOFC) stacks in addition to the Lithium-Ion battery to improve the efficiency by partial-load operation of the stacks at night. The study is supported by the thermodynamic analysis to obtain the characteristics of the system in each state point. To analyze the operation of the system during the partial-load operation, the dynamic performance of the system was developed during the day. Furthermore, the environmental impacts of the system were evaluated considering eighteen parameters using a life-cycle assessment (LCA). LCA results also revealed the effects of different fuels and working fluids for the SOFC stacks and ORC, respectively. Results show that the combination of SOFC and ORC units can generate 264.02 kWh with the respective overall energy and exergy efficiencies of 48.96% and 48.51%. The suggested 264.02 kWh contributes to global warming (kg CO₂ eq) by 5.17 × 10⁵, 8.36 × 10⁴, 2.5 × 10⁵, 1.98 × 10⁵, and 6.79 × 10⁴ using methane, bio-methanol, natural gas, biogas, and hydrogen as the fuel of the SOFC stacks. Full article

Li-rich layered oxides utilizing reversible oxygen redox are promising cathodes for high-energy-density lithium-ion batteries. However, they exhibit different electrochemical profiles before and after oxygen redox activation. Therefore, advanced characterization techniques have been developed to explore the fundamental understanding underlying their unusual phenomenon, such as the redox evolution of these materials. In this review, we present the general redox evolution of Li-rich layered cathodes upon activation of reversible oxygen redox. Various synchrotron X-ray spectroscopy methods which can identify charge compensation by cations and anions are summarized. The case-by-case redox evolution processes of Li-rich 3d/4d/5d transition metal O3 type layered cathodes are discussed. We highlight that not only the type of transition metals but also the composition of transition metals strongly affects redox behavior. We propose further studies on the fundamental understanding of cationic and anionic redox mixing and the effect of transition metals on redox behavior to excite the full energy potential of Li-rich layered cathodes. Full article

Electric vehicle (EV) markets have evolved. In this regard, rechargeable batteries such as lithium-ion (Li-ion) batteries become critical in EV applications. However, the nonlinear features of Li-ion batteries make their performance over their lifetime, reliability, and control more difficult. In this regard, the battery management system (BMS) is crucial for monitoring, handling, and improving the lifespan and reliability of this type of battery from cell to pack levels, particularly in EV applications. Accordingly, the BMS should control and monitor the voltage, current, and temperature of the battery system during the lifespan of the battery. In this article, the BMS definition, state of health (SoH) and state of charge (SoC) methods, and battery fault detection methods were investigated as crucial aspects of the control strategy of Li-ion batteries for assessing and improving the reliability of the system. Moreover, for a clear understanding of the voltage behavior of the battery, the open-circuit voltage (OCV) at three ambient temperatures, 10 °C, 25 °C, and 45 °C, and three different SoC levels, 80%, 50%, and 20%, were investigated. The results obtained showed that altering the ambient temperature impacts the OCV variations of the battery. For instance, by increasing the temperature, the voltage fluctuation at 45 °C at low SoC of 50% and 20% was more significant than in the other conditions. In contrast, the rate of the OCV at different SoC in low and high temperatures was more stable. Full article

Battery models are one of the most important tools for understanding the behaviour of batteries. This is particularly important for the fast-moving electrical vehicle industry, where new battery chemistries are continually being developed. The main limiting factor on how fast battery models can be developed is the experimental technique used for collection of data required for model parametrisation. Currently, this is a very time-consuming process. In this paper, a fast novel parametrisation testing technique is presented. A model is then parametrised using this testing technique and compared to a model parametrised using current common testing techniques. This comparison is conducted using a WLTP (worldwide harmonised light vehicle test procedure) drive cycle. As part of the validation, the experiments were conducted at different temperatures and repeated using two different temperature control methods: climate chamber and a Peltier element temperature control method. The new technique introduced in this paper, named AMPP (accelerated model parametrisation procedure), is as good as GITT (galvanostatic intermittent titration technique) for parametrisation of ECMs (equivalent circuit models); however, it is 90% faster. When using experimental data from a climate chamber, a model parametrised using GITT was marginally better than AMPP; however, when using experimental data using conductive control, such as the ICP (isothermal control platform), a model parametrised using AMPP performed as well as GITT at 25 °C and better than GITT at 10 °C. Full article

Safe and low-cost zinc-based flow batteries offer great promise for grid-scale energy storage, which is the key to the widespread adoption of renewable energies. However, advancement in this technology is considerably hindered by the notorious zinc dendrite formation that results in low Coulombic efficiencies, fast capacity decay, and even short circuits. In this review, we first discuss the fundamental mechanisms of zinc dendrite formation and identify the key factors affecting zinc deposition. Then, strategies to regulate zinc deposition are clarified and discussed based on electrode, electrolyte, and membrane. The underlying mechanisms, advantages, and shortcomings of each strategy are elaborated. Finally, the remaining challenges and perspectives of zinc-based flow batteries are presented. The review may provide promising directions for the development of dendrite-free zinc-based flow batteries. Full article

The explosion of electric vehicles (EVs) has triggered massive growth in power lithium-ion batteries (LIBs). The primary issue that follows is how to dispose of such large-scale retired LIBs. The echelon utilization of retired LIBs is gradually occupying a research hotspot. Solving the issue of echelon utilization of large-scale retired power LIBs brings not only huge economic but also produces rich environmental benefits. This study systematically examines the current challenges of the cascade utilization of retired power LIBs and prospectively points out broad prospects. Firstly, the treatments of retired power LIBs are introduced, and the performance evaluation methods and sorting and regrouping methods of retired power LIBs are comprehensively reviewed for echelon utilization. Then, the problems faced by the scenario planning and economic research of the echelon utilization of retired power LIBs are analyzed, and value propositions are put forward. Secondly, this study summarizes the technical challenges faced by echelon utilization in terms of security, performance evaluation methods, supply and demand chain construction, regulations, and certifications. Finally, the future research prospects of echelon utilization are discussed. In the foreseeable future, technologies such as standardization, cloud technology, and blockchain are urgently needed to maximize the industrialization of the echelon utilization of retired power LIBs. Full article

Zn-air batteries have attracted considerable attention from researchers owing to their high theoretical energy density and the abundance of zinc on Earth. The modification of battery component materials represent a common approach to improve battery performance. The effects of cell design on cell performance are seldom investigated. In this study, we designed four battery structures as follows. Cell 1: close-proximity electrode, Cell 2: equal-area electrode, Cell 3: large zinc electrode, and Cell 4: air channel flow. The effects of four factors: (1) carbon paste, (2) natural and forced air convection, (3) anode/cathode area ratio, and (4) anode–cathode distance were also investigated. Results showed that the addition of carbon paste on the air side of 25BC increased cell power density under forced air convection. Moreover, cell performance also improved by increasing the anode/cathode ratio and by decreasing the anode–cathode distance. These four types of cells were compared based on the oxygen reduction reaction electrode area. Cell 3 displayed the highest power density. In terms of volumetric power density, the proximity cell (Cell 1) exhibited the highest power density among the cells. Therefore, this cell configuration may be suitable for portable applications. Full article

The physics-based fractional-order model (FOM) for lithium-ion batteries has shown good application prospects due to its mechanisms and simplicity. To adapt the model to higher-level applications, this paper proposes an improved FOM considering electrolyte-phase diffusion (FOMe) and then proposes a complete method for parameter identification based on three characteristic SOC intervals: the positive solid phase, negative solid phase, and electrolyte phase. The method mainly determines the above three characteristic intervals and identifies four thermodynamic parameters and five dynamic parameters. Furthermore, the paper describes a framework, which first verifies the model and parameter identification method separately based on pseudo two-dimensional model simulations, and secondly verifies FOMe and its parameters as a whole based on the experiments. The results, which are based on simulations and actual $\mathrm{L}{\mathrm{i}}_{0.8}\mathrm{C}{\mathrm{o}}_{0.1}\mathrm{M}{\mathrm{n}}_{0.1}{\mathrm{O}}_2$ lithium-ion batteries under multiple typical operating profiles and comparisons with other parameter identification methods, show that the proposed model and parameter identification method is highly accurate and efficient. Full article

Differential capacity dQ/dU (capacitance) can be used for the instant diagnosis of battery performance in common constant current applications. A novel criterion allows state-of-charge (SOC) and state-of-health (SOH) monitoring of lithium-ion batteries during cycling. Peak values indicate impeding overcharge or deep discharge, while dSOC/dU = dU/dSOC = 1 is close to “full charge” or “empty” and can be used as a marker for SOC = 1 (and SOC = 0) at the instantaneous SOH of the aging battery. Instructions for simple state-of-charge control and fault diagnosis are given. Full article

Ammonium vanadium oxide (NH₄V₄O₁₀) is a promising layered cathode for aqueous zinc-ion batteries owing to its high specific capacity (>300 mA h g⁻¹). However, the structural instability causes serious cycling degradation through irreversible insertion/extraction of NH₄⁺. Herein, a new potassium ammonium vanadate K_x(NH₄)_1−xV₄O₁₀ (named KNVO) is successfully synthesized by a one-step hydrothermal method. The inserted of K⁺ can act as structural pillars, connect the adjacent layers closer and partially reduce the de-insertion of NH₄⁺. Due to the multi-functional of K⁺, the prepared KNVO presents a high specific discharge capacity of 432 mA h g⁻¹ at a current density of 0.4 A g⁻¹, long cycle stability (2000 cycles, 94.2%) as well as impressive rate performance (200 mA h g⁻¹ at 8 A g⁻¹). Full article

Nickel-rich LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) is one of the most promising Li-ion battery cathode materials and has attracted the interest of the automotive industry. Nevertheless, storage conditions can affect its properties and performance. In this work, both NMC811 powder and electrodes were storage-aged for one year under room conditions. The aged powder was used to prepare electrodes, and the performance of these two aged samples was compared with reference fresh NMC811 electrodes in full Li-ion coin cells using graphite as a negative electrode. The cells were subjected to electrochemical as well as ante- and postmortem characterization. The performance of the electrodes from aged NM811 was beyond expectations: the cycling performance was high, and the power capability was the highest among the samples analyzed. Materials characterization revealed modifications in the crystal structure and the surface layer of the NMC811 during the storage and electrode processing steps. Differences between aged and fresh electrodes were explained by the formation of a resistive layer at the surface of the former. However, the ageing of NMC811 powder was significantly mitigated during the electrode processing step. These novel results are of interest to cell manufacturers for the widespread implementation of NMC811 as a state-of-the-art cathode material in Li-ion batteries. Full article

Open circuit voltage relaxation to a steady state value occurs, and is measured, at the terminals of a lithium-ion battery when current stops flowing. It is of interest for use in determining state of charge and state of health. As voltage relaxation can take several hours, a representative model and curve fitting is necessary for practical usage. Previous studies of lithium-ion voltage relaxation investigate four characteristics: relationship between voltage relaxation magnitude and state of charge; length of relaxation required; model complexity for state of charge estimation; and model complexity for state of health evaluation. However, previous studies have inconsistent methodology or use only one type of lithium-ion cell, making comparison and generalization difficult. To address this, we conducted 3 h and 24 h voltage relaxation experiments over a range of states of charge on three different lithium ion chemistries (nickel cobalt aluminum NCA; nickel manganese cobalt NMC532; lithium iron phosphate LFP) and fitted them with a new voltage relaxation equivalent circuit model. It was found that a 3 h relaxation period was sufficient for NMC and LFP for state of charge and state of health investigations. Voltage relaxation of the NCA cell continued to evolve past 24 h. It was shown that voltage relaxation shape and magnitude changes as a function of state of charge, and the accuracy of estimating state of charge was explored. Strategically choosing a state of charge for state of health assessment can be optimized to accentuate voltage relaxation magnitude and this differs by chemistry. This suggested technique and experimental findings can be paired with battery degradation studies to determine accuracy of assessing state of health. Full article

Lithium-ion batteries have good performance and environmentally friendly characteristics, so they have great potential. However, lithium-ion batteries will age to varying degrees during use, and the process is irreversible. There are many aging mechanisms of lithium batteries. In order to better verify the internal changes of lithium batteries when they are aging, post-mortem analysis has been greatly developed. In this article, we summarized the electrical properties analysis and post-mortem analysis of lithium batteries developed in recent years and compared the advantages of varieties of both destructive and non-destructive methods, for example, open-circuit-voltage curve-based analysis, scanning electron microscopy, transmission electron microscopy, atomic force microscopy, X-ray photoelectron spectroscopy and X-ray diffraction. On this basis, new ideas could be proposed for predicting and diagnosing the aging degree of lithium batteries, at the same time, further implementation of these technologies will support battery life control strategies and battery design. Full article

The temperature of lithium-ion batteries is crucial in terms of performance, aging, and safety. The internal temperature, which is complicated to measure with conventional temperature sensors, plays an important role here. For this reason, numerous methods exist in the literature for determining the internal cell temperature without sensors, which are usually based on electrochemical impedance spectroscopy. This study presents a method in the time domain, based on the pulse resistance, for determining the internal cell temperature by examining the temperature behavior for the cylindrical formats 18650, 21700, and 26650 in isothermal and transient temperature states for different states of charge (SOCs). A previously validated component-resolved 2D thermal model was used to analyze the location of the calculated temperature $T_{\mathrm{R}}$ within the cell, which is still an unsolved question for pulse resistance-based temperature determination. The model comparison shows that $T_{\mathrm{R}}$ is close to the average jelly roll temperature. The differences between surface temperature and $T_{\mathrm{R}}$ depend on the SOC and cell format and range from $2.14$$\mathrm{K}$ to $2.70$$\mathrm{K}$ (18650), $3.07$$\mathrm{K}$ to $3.85$$\mathrm{K}$ (21700), and $4.74$$\mathrm{K}$ to $5.45$$\mathrm{K}$ (26650). The difference decreases for each cell format with increasing SOC and is linear dependent on the cell diameter. Full article