Battery Technology Research Articles

Exploring Chemical and Electrochemical Limitations in Sulfide Solid State Electrolytes: A Critical Review on Current Status and Manufacturing Scope.

Lithium-ion batteries (LIBs) have gained recognition for their high energy density and cost-effectiveness. However, issues such as safety concerns, dendrite formation, and limited operational temperatures necessitate alternative solutions. A promising approach involves replacing flammable liquid electrolytes with non-flammable solid electrolytes (SEs). SEs represent a transformative shift in battery technology, offering stability, safety, and expanded temperature ranges. They effectively mitigate dendrite growth, enhancing battery reliability and lifespan. SEs also improve energy density, making them crucial for applications like portable gadgets, electric vehicles, and renewable energy storage. However, challenges such as ionic conductivity, chemical and thermal stability, mechanical strength, and manufacturability must be addressed. This review paper briefly identifies SE types, discusses their advantages and disadvantages, and explores ion transport fundamentals and all-solid-state batteries (ASSBs) production challenges. It comprehensively analyzes sulfide SEs (SSEs), focusing on recent advancements, chemical and electrochemical challenges, and potential future improvements. Electrochemical reactions, electrolyte materials, compositions, and cell designs are critically assessed for their impact on battery performance. The review also addresses challenges in ASSB production. The objective is to provide a comprehensive understanding of SSEs, laying the groundwork for advancing sustainable and efficient energy storage systems.

From in-situ experimentation to in-line metrology: Advanced imaging characterization for battery research and manufacturing

The continuous advancement of battery technology necessitates innovative approaches in both research and manufacturing to ensure improved performance, reliability, and safety. This article explores the critical role of advanced imaging characterization techniques, spanning from in-situ experimentation to in-line metrology, in the development and production of lithium-ion batteries. By integrating real-time imaging and diagnostic tools, researchers and manufacturers can gain unprecedented insights into the electrochemical processes, material behaviors, structural defects and their evolutions in commercial-grade batteries. This comprehensive characterization enables the optimization of material compositions, electrode designs, and manufacturing processes, ultimately enhancing the efficiency and longevity of batteries. The synergy between in-situ experimentation and in-line metrology provides a robust framework for addressing the complex challenges in battery research and manufacturing, paving the way for innovations that will meet the growing demands of energy storage systems.

Optimizing and investigating the charging time of phase change materials in a compact-latent heat storage using pareto front analysis, artificial neural networks, and numerical simulations

There's a growing emphasis on adopting eco-friendly energy sources to mitigate greenhouse gas emissions and foster sustainability. While renewable energy sources like solar power offer numerous benefits, they have some limitations. Additionally, storing electricity generated from solar panels can be costly and challenging due to limitations in battery technology and storage capacity. Therefore, phase change material-based thermal energy storage systems offer a promising solution to these challenges. These systems also play a crucial role in enhancing buildings' energy efficiency and sustainability. The dimensionality of these systems affects their performance. Traditional systems often rely on fixed dimensions, leading to non-uniform thermal conditions within the storage medium. To address these challenges, adopting a compact-latent heat storage (C-LHS) mechanism was recommended herein. Besides, some fins were inserted into the C-LHS system to alter the heat transfer dynamics within the device. Three of the critical parameters of the fins were changed to examine their impact on the charging time. Artificial neural networks and genetic algorithms were employed to determine the optimal positioning of fins to minimize the duration of material to get both part (melt fraction of 0.8) and full (melt fraction of 1) melting capacities. Here, the primary aim was to present a predictive model capable of accurately forecasting the charging time of the material. In all the presented finned samples, the entire PCM melted in less than 15,110 s (4 h and 12 min) and was able to fully utilize the energy absorption capacity in latent form, whereas in the non-finned system, only 68.6 % of the material managed to melt within the entire duration of the investigation (5 h). After analyzing the data, two optimal configurations of OS1 and OS2 with the minimum time for melt fractions of 0.8 and 1 were introduced. In the OS2 configuration, it took 16,200 s (4 h and 30 min) to absorb 4929 kJ of energy. The non-finned sample absorbed only 3250 kJ of energy during the same period. In General, OS2 achieved total energy absorption 51.6 % faster than the non-finned sample. Therefore, the introduced system has the potential to increase absorbed energy in the rest of the daylight hours to further amounts by increasing the number of units and employing a larger volume of material.

High-Energy-Density All-V2O5 Battery.

Symmetrical batteries hold great promise as cost-effective and safe candidates for future battery technology. However, they realistically suffer low energy density due to the challenge in integrating high specific capacity with high voltage plateau from the limited choice of bipolar electrodes. Herein, a high-voltage all-V2O5 symmetrical battery with clear voltage plateau is conceptualized by decoupling the cathodic/anodic redox reactions based upon the episteme of V2O5intercalation chemistry. As the proof-of-concept, a hierarchical V2O5-carboncomposite (VO-C) bipolar electrode with boosted electron/ion transport kinetics is fabricated, which shows high performance as both cathode and anode in their precisely clamped working potential windows. Accordingly, the symmetrical full-battery exhibits a high capacity of 174 mAh g-1 along with peak voltage output of above 2.9V at 0.5C, remarkable capacity retention of 81% from 0.5C to 10C, and good cycling stability of 70% capacity retention after 300 cycles at 5C. Notably, its energy density reaches 429Wh kg-1 at 0.5C estimated by the cathode mass, which outperforms most of the existing Li/Na/K-based symmetrical batteries. This study leaps forward the performance of symmetrical battery and provides guidance to extend the scope of future battery designs.

Eutectogels: The Multifaceted Soft Ionic Materials of Tomorrow.

Eutectogels, a rising category of soft materials, have recently garnered significant attention owing to their remarkable potential in various domains. This innovative class of materials consists of a eutectic solvent immobilized in a three-dimensional network structure. The use of eco-friendly and cost-effective eutectic solvents further emphasizes the appeal of these materials in multiple applications. Eutectogels exhibit key characteristics of most eutectic solvents, including environmental friendliness, facile preparation, low vapor pressure, and good ionic conductivity. Moreover, they can be tailored to display functionalities such as self-healing capability, adhesiveness, and antibacterial properties, which are facilitated by incorporating specific combinations of the eutectic mixture constituents. This perspective article delves into the current landscape and challenges associated with eutectogels, particularly focusing on their potential applications in CO2 separation, drug delivery systems, battery technologies, biocatalysis, and food packaging. By exploring these diverse realms, we aim to shed light on the transformative capabilities of eutectogels and the opportunities they present to address pressing industrial, academic, and environmental challenges.

Evaluating an autonomous electric robot for real farming applications

Mobile robotic technologies are emerging in agriculture in recent years, driven by labor shortages, the need of precision farm management, and the improvement of farmers' quality of life. Mobile robotic technologies, both aerial and ground, have been considered as one of the most important and promising solutions to address agricultural challenges. Nevertheless, the implementation rate in farms is still low. The aim of this study was to evaluate the performance of a mobile agricultural ground robot to assess its possible implementation in the farm environment. The mobility performances as well as the energy consumption of the mobile robot were evaluated considering different interaction systems (teleoperated, autonomous driving) and application areas (weeding, tilling). The results show that the forward speed of the tested mobile robot is affected by the towed load, up to 230 kg, and that the robot could be driven continuously for 2 h in the field without decreasing its performances at a maximum speed between 0.71–0.77 m s-1. The autonomy of the tested robot is limited, but this is mainly due to the battery technology used. The mobile robot effectively tow implements for weeding and tilling operations managing grass with a single pass (40 % weed removal) and improving soil bulk density. The average energy consumption across the different settings was about 1.43 kWh for each hour of use. Moreover, although the RTK-GNSS autonomous navigation used was a low-cost system, the results showed a good accuracy, which allowed the mobile robot to navigate autonomously in the 2 m inter-row of the vineyard. Finally, the working capacity of the mobile robots, considering the implements used, is on average 0.29 ha h-1. This study provides further evidence for the possible use of ground mobile robot in agriculture to carry out autonomous or semi-autonomous operations.

Optimal estimation of SoC, SoH using machine learning models and design of control algorithm for active cell balancing in lithium ion batteries

Abstract Electric vehicles transform the automotive industry by replacing traditional vehicles powered by fossil fuels with less polluting and efficient vehicles. They are powered by rechargeable Li-ion batteries. While there are drawbacks associated with Li-ion battery technology, it's important to note that these challenges can be addressed or mitigated effectively. A battery management system ensures the tracking of all functions performed by the battery. An advanced battery management system should accurately estimate the battery's state of health and state of charge. This paper aims to develop machine learning models for the estimation of the state of health and state of charge and to implement cell balancing in a battery management system. A dataset of battery charging and discharging profiles was used to train various machine learning models for estimation. These methods are computationally less complex than conventional methods. In addition, a cell balancing algorithm is implemented to control the charging and discharging of individual cells in a battery pack and balance the state of charge of each cell. The machine learning solution is created using several machine learning models, including Gradient Boosting, Random Forest, Linear Regression, AdaBoost, and Multi-layer Perceptron. Among the models Gradient Boosting and Random Forest provide good MSE and R2 score. The use of machine learning algorithms for the assessment of state of health and charge estimation combined with the design of an efficient control algorithm for active cell balancing offers significant advancements in the battery management system to optimise the performance, reliability, and useful life of Li-ion batteries. The paper also presents a case study utilising a combination of deep learning-based SoC, SoH estimation algorithms in a simulated data set. A well-designed control algorithm for active cell balancing presents a holistic and effective approach to optimise the performance, reliability, and lifespan of Li-ion batteries.

A Versatile Metal‐Organic‐Framework Pillared Interlayer Design for High‐Capacity and Long‐Life Lithium‐Sulfur Batteries

Developing high‐performance lithium‐sulfur batteries is a promising way to attain higher energy density at lower cost beyond the state‐of‐the‐art lithium‐ion battery technology. However, the major issues blocking their practical application are the sluggish kinetics and parasitic shuttling reactions for sulfur and polysulfides. Here, pillaring multilayer graphene with the metal‐organic framework (MOF) demonstrates the substantial impact of a versatile interlayer design in tackling those issues. Unlike regular composite separators reported so far, the participation of tri‐metallic Ni‐Co‐Mn MOF (NCM‐MOF) as pillars supports the construction of an ion‐channel interconnected interlayer structure, unexpectedly balancing the interfacial concentration polarization, spatially confining the soluble polysulfides and vastly affording lithiophilic sites for highly efficient polysulfide sieving/conversion. As a demonstration, we show that the MOF‐pillared interlayer structure enables outstanding capacity (1634 mAh g‐1 at 0.1C) and longevity (average capacity decay of 0.034% per cycle in 2000 cycles) of lithium‐sulfur batteries. Besides, the multilayer separator can be readily integrated into the high‐nickel cathode (LiNi0.91Mn0.03Co0.06O2)‐based lithium‐ion batteries, which efficiently suppresses the undesired phase evolution upon cycling. These findings suggest the potential of “gap‐filling” materials in fabricating multi‐functional separators, bring forward the pillared interlayer structure for energy‐storage applications.

Recent Advances in Cost‐Effective ZnO‐Based Electrode Material for Lithium‐Ion Batteries

AbstractFuel cell and lithium ion battery (LIB) technologies are increasingly recognized as cutting‐edge power sources that are gradually displacing various versions of older systems. High‐performance electrode materials must be developed for enhanced next‐generation LIBs. Because of their low cost, high theoretical specific capacity, and environmental friendliness, nanoparticles based on zinc oxide (ZnO) have been regarded as promising alternatives. However, significant problems including intrinsic poor conductivity and significant volume expansion have made ZnO‐based nanomaterials for less viable. In this review we discussed about the mechanism of lithium ion battery and how strategies to overcome intrinsic poor conductivity and significant volume expansion of ZnO‐based nanomaterials. Followed by the best methods for improving the lithium ion storage capacity of ZnO‐based materials as cathode and anode separately reviewed. And summarized the challenges and potential lines of inquiry for Zn‐based nanomaterials in the future.

A Versatile Metal-Organic-Framework Pillared Interlayer Design for High-Capacity and Long-Life Lithium-Sulfur Batteries.

Developing high-performance lithium-sulfur batteries is a promising way to attain higher energy density at lower cost beyond the state-of-the-art lithium-ion battery technology. However, the major issues blocking their practical application are the sluggish kinetics and parasitic shuttling reactions for sulfur and polysulfides. Here, pillaring multilayer graphene with the metal-organic framework (MOF) demonstrates the substantial impact of a versatile interlayer design in tackling those issues. Unlike regular composite separators reported so far, the participation of tri-metallic Ni-Co-Mn MOF (NCM-MOF) as pillars supports the construction of an ion-channel interconnected interlayer structure, unexpectedly balancing the interfacial concentration polarization, spatially confining the soluble polysulfides and vastly affording lithiophilic sites for highly efficient polysulfide sieving/conversion. As a demonstration, we show that the MOF-pillared interlayer structure enables outstanding capacity (1634 mAh g-1 at 0.1C) and longevity (average capacity decay of 0.034% per cycle in 2000 cycles) of lithium-sulfur batteries. Besides, the multilayer separator can be readily integrated into the high-nickel cathode (LiNi0.91Mn0.03Co0.06O2)-based lithium-ion batteries, which efficiently suppresses the undesired phase evolution upon cycling. These findings suggest the potential of "gap-filling" materials in fabricating multi-functional separators, bring forward the pillared interlayer structure for energy-storage applications.

Environmental impacts of a stand-alone photovoltaic system in sub-saharan Africa: A case study in Burkina Faso

This study aims to evaluate and compare the environmental impacts of stand-alone photovoltaic (PV) systems with storage installed in Burkina Faso using the life cycle assessment (LCA). SimaPro 9.4 software, Ecoinvent 3.7 database, and the ReCiPe 2018 (H) median method were used to assess the environmental impacts. The functional unit considered is “1 kWh of electricity produced in Burkina Faso by a stand-alone PV system”. Four scenarios combining two variables, battery technology (lead-acid and lithium-ion) and end-of-life management (landfill and recycling), were studied to assess 08 environmental indicators. The results show that production and end-of-life management of batteries and PV modules are the main contributors to the environmental impact, with batteries' impact ranging from 73 to 98 % for lead-acid and 50–68 % for lithium-ion batteries. Compared to landfilling, recycling significantly reduces environmental impacts, achieving reductions of 17–77 % for lead-acid batteries (LABs) and 3–99 % for lithium-ion batteries (LIBs). The comparison between scenarios indicates that the LABs PV system with landfilling generates significantly higher scores across all impact categories than LIBs PV scenarios. Specifically, it shows scores over 10 times higher for human carcinogenic toxicity, 5 times higher for human non-carcinogenic toxicity, and 2 times higher for freshwater ecotoxicity. Despite extending battery lifespan, the sensitivity analysis revealed that landfill PV systems remain the most polluting, while in recycled scenarios, this extension brings them closer to the environmental performance of LIBs PV systems. The use of LIBs in photovoltaic systems is more environmentally friendly than that of LABs, regardless of the end-of-life scenario.

Study on the parameter identification of lithium-ion battery model under high-rate pulse discharge conditions

With the rapid development of the new energy sector and lithium-ion (Li-ion) battery technologies, using Li-ion batteries with high energy density and high discharge rate to form the primary energy subsystem can further improve the compactness and miniaturization level of pulsed power systems. In traditional electric power systems, Li-ion batteries normally operate under the discharge condition of low current and long time. However, as the main power source of pulsed power systems, it is required that Li-ion batteries should have the capability for high-rate pulse discharge. To ensure the safe and reliable operation of the battery energy storage system, it is necessary to conduct the parameter identification of the Li-ion battery model to establish an accurate pulse discharge model under such working conditions. This paper focuses on the discharge characteristics of a cylindrical high-rate single Li-ion battery with a capacity of 3 Ah. At a 20 C rate, the discharge data were obtained when the pulse repetition frequency was 10 Hz and the duty cycle was 90%. By using the mathematical expressions of the Thevenin equivalent circuit model, the recursive relationship of the circuit parameters was obtained, and the parameter identification of the battery model was conducted based on the experimental data by using the genetic algorithm. The results show that the fitting accuracy of the parameter identification reaches 0.9995, indicating the high precision of the model for the Li-ion battery. This work provides a significant reference for the modeling and parameter identification of Li-ion batteries under high-rate pulse discharge conditions.

Rice husk-based activated carbon/carbon nanotubes composites for synergistically enhancing the performance of lead-carbon batteries

Lead-carbon batteries (LCBs), an advanced form of lead-acid battery (LAB) technology, incorporate super-capacitive carbon materials into the negative electrode. Rice husk-based activated carbon (RHAC) is a promising additive for LCBs due to its favorable properties. However, RHAC's amorphous structure impedes electronic conduction, and its zigzag microporous channels hinder ion transport, leading to degraded high-rate performance. This study addresses these issues by growing carbon nanotubes (CNTs) in situ on RHAC through a one-step heat treatment, resulting in carbon nanotubes-loaded RHAC (CNTs/RHAC), and the electronic conductivity and ionic conductivity are simultaneously enhanced. When CNTs constitute 30 wt.% of CNTs/RHAC, the negative electrode achieves a cycle life of 4721 cycles at a 2C rate under 50% state of charge, which is 10.04 times that of the blank anode. The enhanced performance is attributed to the synergistic effects of CNTs and RHAC, where CNTs form long-range conductive networks among the negative electrode active material (NAM) and facilitate the diffusion and electro-deposition of Pb2+, while the high specific surface area (SSA) and hierarchical porous structure of RHAC enhance its capacitive function, leading to a stable lead-carbon composite structure.

Porous activated carbon integrated carbon nitride nanosheets as functionalized separators for the efficient polysulfide entrapment in Li[sbnd]S batteries

Electrification of vehicles, hybrid aircraft and the advancement of portable electronics are exacting the deployment of high energy-dense batteries. The high theoretical capacity of sulfur (1675 mAh g−1), cost-effectiveness and environmental benignity of the lithium‑sulfur batteries (LSBs) are propitious for electrochemical energy storage beyond Li-ion battery technology. In this work, we described a simple, scalable preparation and electrochemical performance of porous activated carbon (PC)-infused graphitic carbon nitride (GCN) nanosheets with various ratios (PC@GCN 11, PC@GCN 12 and PC@GCN 21) as a polysulfide anchoring functionalized separator for LSBs. The high specific area (822 m2/g), hetero porosity, conductive carbon framework, surface functionalities and enriched N-doping of the PC@GCN synergistically induce mitigation of polysulfides via chemical and physical adsorption pathways in LSBs. The PC@GCN 21 modified separator demonstrates a high initial discharge capacity of 1389 mAh g−1 at a 0.1C rate and exhibits better capacity retention over 500 cycles at a 1C rate (655 mAh g−1) with sulfur loading of 3.8 mg/cm2 accompanied by high coulombic efficiency (94 %). The assembled cell with high S-loading (5.12 mg/cm2) shows a high initial discharge capacity of 712 mAh g−1 at 0.1C rate conditions. High Li-ion transference number (0.714), stable shuttle current, minimal coulombic efficiency loss (0.84 %), low shuttle factor and negligible self-discharge behaviour support the superior performance of the PC@GCN 21 coated cells. This report demonstrates that combining the high surface area, non-polar porous carbon with polar graphitic carbon nitride is a practical approach for designing metal-free functionalized separators for energy-dense LSBs.

Nitrogen-doped carbon embedded with heterostructured Co3Fe7-Co5.47N nanoalloys for electrocatalytic oxygen reduction reaction in zinc-air battery

The oxygen reduction reaction (ORR) is the cathodic process in zinc-air batteries, but its sluggish kinetics significantly limit the energy conversion efficiency of these batteries. Therefore, developing high-performance ORR electrocatalysts is essential to support the advancement of zinc-air battery technology. Herein, a nitrogen-doped carbon embedded with heterostructured Co3Fe7-Co5.47N nanoalloys (FeCo@NC-900) was fabricated, and its electrocatalytic ORR activity and stability of FeCo@NC-900 were investigated in alkaline media. The FeCo@NC-900 catalyst exhibited a half-wave potential of 0.84 V, a Tafel slope of 76.06 mV·dec−1, and an electron transfer number (n) of approximately 3.83 for ORR. A rechargeable zinc-air battery was assembled using FeCo@NC-900 as the air cathode, achieving an open-circuit voltage of 1.435 V and a maximum power density of 81 mW cm−2, along with good cycling stability.

Scheme design and assessment of hybrid pump feed system with energy management for throttleable liquid rocket engine

Currently, there is considerable emphasis on the electric pump-fed cycle for liquid engine, primarily due to its design simplicity. However, its development is hindered by the underdeveloped state of power battery technology. Drawing inspiration from hybrid power technology used in electric vehicles and turbochargers, a hybrid pump feed system for throttleable engines is originally proposed as a promising solution. This system integrates the electric motor into the gas generator cycle, with several topologies evaluated. The parallel configuration featuring a mid-motor is selected for its compact structure, efficient power-splitting and energy recovery. Additionally, customized energy management strategies and optimization models are developed to effectively allocate power throughout the operational processes of liquid engines. A comparative analysis of four engine cycles is conducted under the typically variable-thrust mission. The results indicate that attributed to the conservation of turbo-gas and battery energy, the optimized hybrid pump achieves a reduction of 2.39 % compared to the turbopump and 7.15% to the electric pump in total mass. Adaptability assessment further indicates that the mass advantage of the hybrid pump system is more significant during prolonged engine burning and deep throttling. Specific working conditions are found in which the system prefers electric-motor driving or regenerating turbine energy. Although energy-recovery results in the system efficiency decrease, it serves to lower energy demand of battery pack, thus easing the burden on cell thermal management and structural design. This study provides a practical design framework for hybrid pump-fed rocket engines in future variable-thrust missions.

Enhanced strain mapping Unveils internal deformation dynamics in Silicon-based lithium-ion batteries during electrochemical cycling

Silicon-based anodes have emerged as a promising advancement in lithium-ion battery technology, offering significantly higher lithium storage capacities than traditional graphite. However, the volumetric expansion of silicon—anodes can swell by up to 300 % during lithiation—presents serious challenges to their structural integrity and electrochemical stability. This study investigates the internal structural dynamics of silicon anodes during lithiation and delithiation cycles. A novel cell design for a 18,650 cylindrical cell featuring micro-sized internal speckles within the silicon anode is presented. This design improves the simulation of electrochemical conditions and allows for precise displacement tracking, mitigating impacts on capacity and cycle performance while enhancing Digital Volume Correlation (DVC) analysis. The research prioritizes reducing scan time and radiation exposure in micro-CT assessments of Li-ion cells, and improves the accuracy of internal strain mapping via DVC. Displacement fields over three charging and discharging cycles are documented. Notably, uneven volumetric changes are observed, with local displacements reaching up to 35 µm in areas smaller than 2.5 mm in radius, which contracted during charging and expanded during discharging. This protocol offers insights into the relationship between electrode mechanics and cell performance, promoting non-destructive evaluations of internal structures in commercial cells.

Establishing laser cutting of components for sulfide-based solid-state batteries

The demand for safe, power- and energy-dense, low-cost batteries is constantly increasing due to the global shift toward renewable energy sources and the associated need for battery electric vehicles and grid-level energy storage. However, current-generation lithium-ion batteries are struggling to meet the requirements and are reaching their physicochemical limits regarding energy density. Solid-state battery technology promises to improve the current state of the art in electrochemical energy storage and has proven itself in research, although not yet in commercial applications. One of the main challenges in bringing the technology to the market is the limited knowledge and research on the production of solid-state batteries with commercially viable technologies. This study investigates the application of laser cutting technology to improve the cutting process in the production of sulfide-based solid-state batteries. Challenges such as the production atmosphere, handling of the components, and differences compared to conventional battery components are discussed. Using a picosecond laser source, the influence of the pulse frequency, peak fluence, scanning speed, and laser passes was investigated to identify appropriate parameters for cutting sulfide-based composite cathodes. The findings were then successfully applied to the cutting of sulfide-based solid electrolyte separators. An improvement in edge quality compared to mechanical punching is demonstrated, marking a crucial step toward the commercialization of solid-state batteries.

A three-in-one strategy of high-entropy, single-crystal, and biphasic approaches to design O3-type layered cathodes for sodium-ion batteries

O3-type layered oxides are promising cathodes for sodium-ion batteries (SIBs). However, severe volume changes, irreversible phase transitions, and sluggish Na+ ion transport kinetics lead to structural collapse and severe capacity loss. Herein, a three-in-one strategy “high entropy, single crystal, and biphase” is proposed to design O3-type layered cathodes for SIBs, which achieves enhanced structural stability and Na+ transport kinetics by the combination effect of multimetal high-entropy, the single crystal, and Li substitution. The as-prepared high-entropy oxide (HEO) cathode, Na(Fe1/6Co1/6Ni1/6Mn1/6Ti1/6)Li1/6O2, exhibits a high reversible capacity of 140.3 mAh g−1, robust cycling stability, exceptional rate capability (86 mAh g−1 at rates of 15C), excellent air-stability, and water-resistance ability. In situ X-ray diffraction reveals that the HEO cathode has highly reversible phase transitions and small volume change (ΔV=3.28 %). Ex situ X-ray absorption spectroscopy reveals that reversible Ni2+/Ni4+, Fe3+/Fe3.6+, and Co3+/Co3.6+ redox couples provide charge compensation for the high-entropy cathode at 2.0∼4.2 V. Notably, the full-cell battery based on the high-entropy cathode and hard carbon anode delivers a specific capacity of 134.3 mAh g−1 and an energy density of 390.8 Wh kg−1. This work provides valuable insights into the design of novel high-performance high-entropy cathodes for SIBs, highlighting a promising avenue for advancing rechargeable battery technology.

Quantitative pre-lithiation modulation of aluminum foil anode kinetics enables high rate and stable cycling of high-loading all-solid-state batteries

Aluminum (Al) foil holds great promise as a pure alloy anode for all-solid-state batteries (ASSBs) due to its suitable potential, high theoretical capacity, and excellent electronic conductivity. However, it remains challenging to achieve high reversibility and stability of the Al foil anode for ASSBs. Herein, we investigate the morphological and lithium (Li) kinetics evolutions of the Al foil anode paired with sulfide solid-state electrolyte (SSE). We identify that the significant reversible capacity loss stems from diminished Li kinetics at low Li contents (LixAl, 0 < x < 0.5), where the accumulation of pores and pure delithiated Al phase obstructs Li diffusion, increasing interfacial resistance and overpotential. Conversely, the Al foil anode with high Li contents (LixAl, 0.5 < x < 1) demonstrates reversible structures and rapid Li kinetics. Through precise pre-lithiation control, ASSBs with LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes exhibit outstanding rate capabilities and cycling stability, achieving over 4,000 cycles with 82.1 % capacity retention at 5C and demonstrating long-term cycling over 1,000 cycles with nearly 100 % capacity retention at ultra-high loadings. This work offers a viable strategy for advancing practical-level ASSBs with enhanced performance and longevity, contributing valuable insights to future battery technology.