Rechargeable Lithium Batteries Research Articles

Development of an azo-based organic electrode material for aqueous rechargeable lithium batteries

Development of an azo-based organic electrode material for aqueous rechargeable lithium batteries

Polyoxometalate–Polymer Composites with Distinct Compositions and Structures as High-Performance Solid Electrolytes

Solid electrolytes, including polymer electrolytes, are a promising option for improving the performance of environmentally friendly batteries such as rechargeable lithium-ion batteries or fuel cells. Hydrogen–oxygen fuel cells producing only water under power generation are attracting widespread attention, and they need proton conductors as electrolytes. Fluoropolymer electrolytes such as Nafion® have been utilized for hydrogen–oxygen fuel cells below 100 °C; however, they are not applicable over the working temperature. Therefore, other types of polymer electrolytes are demanded for hydrogen–oxygen fuel cells. Polyoxometalate (POM) inorganic clusters are known as proton conductors and are utilized to prepare POM–polymer composites for solid electrolyte application. In such POM–polymer composites, distinct compositions and structures are significant for improving the performance of proton conductivity. Recently, POM–polymer composites with distinct compositions and structures have been synthesized to obtain high proton conductivity. The key factor is to use single-crystalline compounds. Here, several examples are overviewed by classifying them into three categories: (i) single-crystalline POM–polymer composites, (ii) organically modified POM (org-POM) polymers, and (iii) POM hybrid polymers using polymerizable cations. The application of proton-conductive solid electrolytes is focused on.

Rational Fabrication of One‐Dimensional TiO2 Nanowires for Enhanced Supercapacitor and Rechargeable Lithium Ion Battery

AbstractHydrothermal synthesis of titanium dioxide nanowires yields high‐purity and well‐developed grains while exhibiting a low degree of aggregation. TiO2‐0.5 and TiO2‐0.7 (0.5 ml and 0.7 ml tetrabyl titanate were added to the mixture for TiO2‐0.5 and TiO2‐0.7) are obtained by varying the content of tetrabutyl titanate through a simple to obtain nanowire particles, followed by annealing at 500 °C in air. The electrochemical properties of the nanoparticles can be improved solely by adjusting the amount of tetrabutyl titanate. Herein, TiO2‐0.5 and TiO2‐0.7 were synthesized, and their electrochemical performance as negative electrodes for Lithium‐ion batteries (LIBs) and supercapacitors was investigated. As a negative electrode for LIBs, the reversible capacity of TiO2‐0.7 nanomaterial after 65 cycles at a current density of 100 mA/g is 221.9 mAh/g. In contrast, at current densities of 200 mA/g, 300 mA/g, and 500 mA/g, it is measured as 173.8 mAh/g, 148.4 mAh/g, and 120 mAh/g, respectively. As a supercapacitor electrode material, TiO2‐0.7 exhibited a specific capacitance of 121.8 F/g at a current density of 0.2 A/g. These results suggest that this electrode material material has great potential for portable electronic devices in the future due to its ability to modulate the concentration of TiO2 nanowires (TiO2 NWs) by adjusting the content of tetrabutyl titanate.

Advanced Algorithms in Battery Management Systems for Electric Vehicles: A Comprehensive Review

Electric vehicles and hybrid electric vehicles (EV) are increasingly common on roads today compared to a decade ago, driven by advancements in technology and a growing focus on sustainable transportation. These vehicles are powered by rechargeable lithium-ion batteries. A battery management system (BMS) is indispensable for ensuring the optimal performance, safety, and longevity of the EV’s batteries. In this review, the latest algorithm trends for BMS software are discussed. This work also focuses on several key functionalities of BMS like the state of charge (SOC) estimation, state of health (SOH) monitoring, state of energy (SOE), and state of power (SOP). Advanced algorithms for BMS are comprehensively reviewed, including those designed for specific functionalities, as well as those developed based on existing optimization, artificial intelligence, and estimation algorithms. These algorithms address critical challenges such as maintaining symmetry during charging and discharging, preventing thermal runaway, and managing battery faults in EV systems. This work provides valuable insights for researchers and practitioners in the field of EV design and development, particularly those focusing on the advancement of BMS technologies.

A novel SnC/graphene heterostructure as an efficient host material for Li- and Na-ion batteries: computational insight

The rapid growth of technologies has influenced our daily lives in building efficient energy storage systems such as lithium-ion batteries (LIBs) for various electric automobiles and portable electronic devices. Graphite, the commercial anode material for LIBs, has several limitations including low lithium storage capacity (372 mAh g-1), low power rate capability, and sluggish charging for applications in grids and heavy electric vehicles. Herein, we propose a novel SnC/graphene heterostructure (SnC/G-H) as a potential anode material for LIBs and sodium-ion batteries, supported by first-principles calculations. The graphene layer in the SnC/G-H model provides high mechanical stability and electrical conductivity, enhancing device application and potentially solving the structural issues of the SnC monolayer. SnC/G-H serves as an excellent Li/Na host material, offering low average voltages (0.34-0.39 V), impressive Li/Na storage capacities of 870 mAh g-1 (exceeding those of pristine SnC and graphite), and minimal activation energy barriers of 0.043/0.079 eV, which promote efficient lithiation/delithiation and sodiation/desodiation processes. These enthralling findings indicate that the SnC/G-H could serve as an efficient host material for rechargeable LIBs and sodium-ion batteries.

Research of Different Materials Used in Lithium Batteries and Combination with Nanomaterials

Ever since the 2nd industrial revolution, people’s demand of energy has increased a lot not just high power but also convenience and security. Batteries have been popular among people of all ages since it was invented for it satisfied most of them. However, most of them can only be used once so that is the reason why lithium-ion rechargeable batteries are invented. Lithium-ion batteries hold well on their mass and volume, which solves the bulks’ obstacles over centuries. More importantly, they own wonderful voltage as well as capacity. With the development of lithium-ion batteries, people’s demand of better materials became more and more stronger. Graphite material has had a dominant position in both commercial and industrial area. However, there are more extraordinary compounds whose properties like capacity and potential are better than those of carbon. Therefore, several new materials that scientists researched about are introduced below to compare them with carbon. Meanwhile, nanomaterials have caught people’s eyes because they are newborn subject for science. By modification, they can improve properties of different materials. This article is a literature review of lithium-ion batteries. Moreover, it will combine batteries with nanomaterials together to explore better methods to use in lithium-ion batteries.

Intrinsic Structural and Coordination Chemistry Insights of Li Salts in Rechargeable Lithium Batteries.

Lithium batteries, favored for their high energy density and long lifespan, are staples in electric vehicles, portable electronics, and aerospace. A key component, Li salts, aids lithium ion migration and electrode protection, significantly impacting battery performance. Developing an ideal Li salt, balancing stability, solubility, dissociation, solvation, and eco-friendliness, remains challenging. Given the scarcity of relevant reviews, it is endeavored here to present a novel perspective on Li salt chemistry, offering a concise roadmap for future designs and innovations. It is delved into the trends, opportunities, design principles, and evaluation methodologies related to Li salt chemistry, with a particular emphasis on organic anionic compositions. Furthermore, the latest and most representative organic Li salts from their intrinsic structure and coordination chemistry, highlighting their unique features and contributions are organized and presented. Finally, a visionary outlook is articulated for this field, exploring avenues, such as customizing Li salts for specific applications, synthesizing Li salts on demand, and discussing the potential of F-free Li salts alongside with their electrochemical window challenges. Here it is served as a strategic compass, addressing the shortcomings of existing reviews and guiding the design of functionalized Li salts.

Mechanisms of Enhanced Electrochemical Performance by Chemical Short-Range Disorder in Lithium Oxide Cathodes.

LiCoO2 has been one of the dominant cathode materials commercially used in rechargeable lithium-ion batteries, while the performance is severely limited by its low reversible capacity (∼140 mAh/g), primarily due to the destructive phase transitions at high voltages (>4.2 V vs Li/Li+), leading to structural degradation and rapid decay of capacity. A recent experimental study [Wang et al. Nature 2024, 629, 341] showed that chemical short-range disorder (CSRD) in LiCoO2 can effectively prevent phase transitions and structural deterioration. To better understand the underlying mechanisms, we carry out a theoretical study on CSRD-based LiCoO2 by performing ab initio molecular dynamics simulations accelerated by machine learning and find that CSRD effectively suppresses phase transitions from hexagonal to monoclinic at Li0.5CoO2 and from O3 to H1-3 at Li0.25CoO2. The enhanced phase stability is attributed to the reduced lattice variation in the c-axis, the increased oxygen vacancy formation energies, the higher oxygen dimer formation energies, and the stabilization of Co atoms in the Li layers during delithiation. The high Li+ diffusion coefficients are found to arise from the low-barrier 0-TM diffusion channels and an expanded diffusion network from 2D to quasi-3D induced by CSRD. Furthermore, CSRD narrows the band gap of LiCoO2 with enhanced electronic conductivity, driven by the changes in the Co valence state and the introduction of linear Li-O-Li configurations. Equally important, CSRD can also enhance the stability of Li-rich cathode Li1.2Co0.8O2 for high capacity and excellent cycling performance. This work provides theoretical insights into the effects of CSRD on LiCoO2 and Li-rich cathodes for rational design and synthesis.

Self-Regulatory Lean-Electrolyte Flow for Building 600Wh Kg-1-Level Rechargeable Lithium Batteries.

Reducing excess electrolytes offers a promising approach to improve the specific energy of electrochemical energy storage devices. However, using lean electrolytes presents a significant challenge for porous electrode materials due to heterogeneous wetting. The spontaneous wetting of nano- or meso-pores within particles, though seldom discussed, adversely affects wetting under lean electrolyte conditions. Herein, this undesired wetting behavior is mitigated by enlarging the pore-throat ratio, enabling Li-rich layered oxide to function effectively at very low electrolyte/capacity (E/C) ratio of 1.4g Ah-1. The resulting pouch cell achieves 606Wh kg-1 and retains 80% capacity (75% energy) after 70 cycles. Through imaging techniques and molecular dynamics simulations, it is demonstrated that the pore-throat ratio effectively determines the permeability of electrolyte within particles. By elucidating pore-relating mechanisms, this work unveils promising potential of manipulating pore structures in porous electrode materials, an approach that can be applied to improve the specific energy of other devices including semi-solid-state lithium batteries.

Insights into Homogeneous Bulk Boron Doping at the Tetrahedral Site of NCM811 Cathode Materials: Structure Stabilization by Inductive Effect on TM-O-B Bonds.

Rechargeable lithium-ion batteries (LIBs) are critical for enabling sustainable energy storage. The capacity of cathode materials is a major limiting factor in the LIB performance, and doping has emerged as an effective strategy for enhancing the electrochemical properties of nickel-rich layered oxides such as NCM811. In this study, boron is homogeneously incorporated into the tetrahedral site of NCM811 through co-precipitation, leading to an inductive effect on transition metal (TM)-O-B bonds that delayed structural collapse and reduced oxygen release. Consequently, these changes culminate in an enhancement of cycling performance, translating to an initial specific capacity of 210mAh g-1 and a 95.3% capacity retention after 100 cycles. These interesting findings deepen the understanding of boron doping and shed light on the design of better lithium cathode materials on an applicable scale.

Advanced carbon as emerging energy materials in lithium batteries: A theoretical perspective

AbstractLithium batteries are becoming increasingly vital thanks to electric vehicles and large‐scale energy storage. Carbon materials have been applied in battery cathode, anode, electrolyte, and separator to enhance the electrochemical performance of rechargeable lithium batteries. Their functions cover lithium storage, electrochemical catalysis, electrode protection, charge conduction, and so on. To rationally implement carbon materials, their properties and interactions with other battery materials have been probed by theoretical models, namely density functional theory and molecular dynamics. This review summarizes the use of theoretical models to guide the employment of carbon materials in advanced lithium batteries, providing critical information difficult or impossible to obtain from experiments, including lithiophilicity, energy barriers, coordination structures, and species distribution at interfaces. Carbon materials under discussion include zero‐dimensional fullerenes and capsules, one‐dimensional nanotubes and nanoribbons, two‐dimensional graphene, and three‐dimensional graphite and amorphous carbon, as well as their derivatives. Their electronic conductivities are explored, followed by applications in cathode and anode performance. While the role of theoretical models is emphasized, experimental data are also touched upon to clarify background information and show the effectiveness of strategies. Evidently, carbon materials prove promising in achieving superior energy density, rate performance, and cycle life, especially when informed by theoretical endeavors.image

Enhancing the durability of aluminium-foil anodes in rechargeable lithium batteries via uniformly distributed alloy addition in the matrix phase

Uniformly distributed Si in the Al matrix as a solid solution induces a pinning effect, prevents cracking of the Al grains, suppresses pulverization and improves the cycling stability of Al-foil anodes in rechargeable lithium batteries.

Correction: Enhancing the durability of aluminium-foil anodes in rechargeable lithium batteries via uniformly distributed alloy addition in the matrix phase

Correction for ‘Enhancing the durability of aluminium-foil anodes in rechargeable lithium batteries via uniformly distributed alloy addition in the matrix phase’ by Hongyi Li et al., J. Mater. Chem. A, 2025, https://doi.org/10.1039/D4TA07956F.

Interfacially-localized high-concentration electrolytes for high-performance rechargeable aqueous lithium-ion batteries

Interfacially-localized high-concentration electrolytes were developed using an anionic surfactant and a magnesium(ii) salt to achieve selective Li ion transport, high electrochemical stability and superior SEI formation in aqueous electrolytes.

Optimizing Si─O Conjugation to Enhance Interfacial Kinetics for Low-Temperature Rechargeable Lithium-Ion Batteries.

With the growing demand for high-voltage and wide-temperature range applications of lithium-ion batteries (LIBs), the requirements for electrolytes have become increasingly stringent. While fluorination engineering has enhanced the performance of traditional solvent systems, it has also raised concerns regarding cost, environmental hazards, and low reduction stability. Through strategic molecular bond design, a novel class of low-temperature (LT) solvents-siloxanes-is identified, meeting the demands of LT and high-voltage applications in LIBs. The d-p conjugation of the Si─O bond enhances voltage resistance and weakens the Li+-solvent interactions. By modulating the number of Si─O conjugated bonds, the type of anion clusters in the solvation structure can be controlled, ultimately leading to the formation of a LiF and Si─O-rich interfacial layer and facilitating rapid Li+ conduction. Consequently, the graphite||NCM811 pouch cell (2.3 Ah, 4.45 V) with a siloxane-based electrolyte retains 75.1% of room temperature capacity (RTC) at -50°C. The rapid interface kinetics allow a superior reversible charging capacity retention of 67.6% at -40°C, with good cycle stability at -20°C. This study provides new insights into solvent design to fortify LIB performance in harsh conditions.

Smart Shoe Using Peizo Electric Sensors

Abstract: In this article, a piezoelectric shoe system that stores and harnesses walking kinetic energy to generate electric current for cell measurement and charging a smartphone is designed and constructed. It captures the forces exerted by walking, utilising mechanical stress through piezoelectric sensors, into electrical energy by means of a 27mm piezoelectric disk. Main components include: piezoelectric sheets, silicone adhesives, 1N4007 diodes, and a 3.7V rechargeable lithium-ion battery. This intelligent shoe therefore has the potential of being used independently without much effort towards its maintenance. Preliminary tests promise that the smart shoes would really be able to provide their users with a source of sustainable power, particularly in remote or outdoor settings.

Roles of the Polymer Backbone for Sulfurized Polyacrylonitrile Cathodes in Rechargeable Lithium Batteries.

Sulfurized polyacrylonitrile (SPAN) has emerged as a highly promising cathode material for next-generation lithium-sulfur (Li-S) batteries primarily due to its non-polysulfide dissolution and excellent cycle stability. Nevertheless, the specific roles and impacts of the pyrolyzed polyacrylonitrile, which constitutes the polymer backbone of SPAN, remain inadequately understood. In this study, comprehensive investigations from multiple aspects, including electrochemistry, spectroscopy, electron microscopy, and theoretical calculations, were conducted on a series of SPAN materials with various sulfur contents. The results reveal that the polymer backbone serves at least four critical functions. First, during the synthesis of SPAN, the polymer backbone provides reactive sites for the incorporation of sulfur through chemical bonding. Second, it establishes an extensive π-conjugated network via a dehydrogenation reaction by sulfur and serves as a conductive framework for SPAN. The chemically bonded sulfur atoms dope the polymer backbone, which narrows the highest occupied molecular orbitals-lowest unoccupied molecular orbitals (HOMO-LUMO) energy gap. Third, the polymer backbone plays an essential role in determining the first Coulombic efficiency, and the irreversibly inserted Li atoms further dope the polymer backbone and reduce the HOMO-LUMO energy gap. Lastly, the pyridine nitrogen within the polymer backbone exhibits an adsorption effect on lithium sulfide (Li2S) species, which stabilizes the cycling performances of the SPAN cathode. It is worth noting that the polymer backbone hardly contributes reversible capacity for the SPAN cathode in carbonate electrolytes within the 1 to 3 V operating voltage range. This study enhances our understanding of SPAN and may provide valuable guidance for the development of better SPAN materials and rechargeable batteries.

Hierarchically Porous Carbon Microspheres Coated with MnO2 Nanosheets as the Sulfur Host for High-Loading Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries have emerged as a promising candidate for next-generation high-energy rechargeable lithium batteries, but their practical application is impeded by the sluggish redox kinetics and low sulfur loading. Here, we report the in situ growth of δ-MnO2 nanosheets onto hierarchical porous carbon microspheres (HPCs) to form an HPCs/S@MnO2 composite for advanced lithium-sulfur batteries. The delicately designed hybrid architecture can effectively confine LiPSs and obtain high sulfur loading up to 10 mg cm-2, in which the inner carbon microspheres with a large pore volume and large specific surface area can encapsulate high sulfur content, and the outer MnO2 nanosheets, as a catalytic layer, can improve the conversion reaction of LiPSs and suppress the shuttle effect. The thick HPCs/S@MnO2 electrode with 7 mg cm-2 sulfur loading delivers an areal capacity of 4.0 mAh cm-2 at 0.1 C and provides stable cycling stability with a low-capacity decay rate of 0.063 % per cycle after 200 cycles at 0.1 C. Furthermore, a Li-S pouch cell with a capacity of 2.5 A h is fabricated and demonstrates high cycling stability. This work offers a feasible method to build advanced sulfur electrodes with high areal loading and sheds light on their commercial application in high-performance Li-S batteries.

Beyond Organic Electrolytes: An Analysis of Ionic Liquids for Advanced Lithium Rechargeable Batteries

The fast-growing area of battery technology requires the availability of highly stable, energy-efficient batteries for everyday applications. This, in turn, calls for research into new battery materials, especially with regard to a battery’s main component: the electrolytes. Besides the demands associated with solid ionic conduction and appropriate electrochemical behaviour, considerable effort will be necessary to thoroughly reduce safety risks in terms of flammability, leakage, and thermal runaway. Consequently, completely new classes of electrolytes need to be developed that are compatible with energy storage systems. Despite the progress made in solid polymer electrolytes, such materials have suffered from limitations to their real-world application. Now, ionic liquids are considered a class of electrolytes with the most potential for the creation of more advanced and safer lithium–ion batteries. In recent decades, ILs have been widely explored as potential electrolytes in the search for new breakthroughs in the ESS field, such those associated with fuel cells, lithium–ion batteries, and supercapacitors. The present review will discuss ILs that present high ionic conductivity, a lower melting point below 100 °C, and which feature up to 5–6 V wide electrochemical potential windows vs. Li+/Li. Furthermore, ILs exhibit good thermal stability, non-flammability, and low volatility—all of which are attributes realized by appropriate cation–anion combinations. This paper seeks to review the status of research concerning ILs, along with the advantages and challenges yet to be overcome in their development.

Electrostatic Aspect of the Proton Reactivity in Concentrated Electrolyte Solutions.

Water-in-salt electrolytes with a surprisingly large electrochemical stability window of ≤3 V have revived interest in aqueous electrolytes for rechargeable lithium-ion batteries. However, recent reports of acidic pH measured in concentrated electrolyte solutions appear to be in contradiction with the suppressed activity of the hydrogen evolution reaction (HER). Therefore, the fundamental thermodynamics of proton reactivity in concentrated electrolyte solutions remains elusive. In this work, we have used density functional theory-based molecular dynamics (MD) simulations and the proton insertion method to investigate how the HER potential shifts in concentrated LiCl solutions under both acidic and alkaline conditions. Our results show that the intrinsic HER activity increases significantly with the salt concentration under acidic conditions but remains relatively constant under alkaline conditions. Moreover, by leverage over finite-field MD simulations, it is found that a determining factor for the HER activity is the Poisson potential of the liquid phase, which increases in concentrated electrolyte solutions with comparable values from both density functional theory and point-charge models.