Rechargeable Lithium Batteries Research Articles

Novel Ordinary Differential Equation for State-of-Charge Simulation of Rechargeable Lithium-Ion Battery

Lithium-ion battery energy storage systems are rapidly gaining widespread adoption in power systems across the globe. This trend is primarily driven by their recognition as a key enabler for reducing carbon emissions, advancing digitalization, and making electricity grids more accessible to a broader population. In the present study, we investigated the dynamic behavior of lithium-ion batteries during the charging and discharging processes, with a focus on the impact of terminal voltages and rate parameters on the state of charge (SOC). Through modeling and simulations, the results show that higher terminal charging voltages lead to a faster SOC increase, making them advantageous for applications requiring rapid charging. However, large values of voltage-sensitive coefficients and energy transfer coefficients were found to have drawbacks, including increased battery degradation, overheating, and wasted energy. Moreover, practical considerations highlighted the trade-off between fast charging and time efficiency, with charging times ranging from 8 to 16 min for different rates and SOC levels. On the discharging side, we found that varying the terminal discharging voltage allowed for controlled discharging rates and adjustments to SOC levels. Lower sensitivity coefficients resulted in more stable voltage during discharging, which is beneficial for applications requiring a steady power supply. However, high discharging rates and sensitivity coefficients led to over-discharging, reducing battery life and causing damage. These new findings could provide valuable insights for optimizing the performance of lithium-ion batteries in various applications.

High-performance lithium-ion full-cell batteries based on transition metal oxides: Towards energy density of ∼ 1300 Wh kg−1

Half-cell structure including sufficient lithium ions for theoretical studies exhibits different electrochemical performance with commercial full-cell rechargeable lithium ion batteries (LIBs) featuring moderate lithium ions. So, understanding the property correlation between half-cell and full-cell LIBs is imperative, but remains a big challenge. Herein, a series of full-cells are assembled with transition metal oxide (TMO) nanowires as cathodes and silicon/graphite (Si/G) anode via electrochemical pre-lithiation, to figure out the key determinants in comparison to their corresponding half-cells. It is found that eletrochemical performances of half-cell and full-cell batteries are basically consistent by using insertion-type cathodes of V2O5, MoO3 and MnO2, but different in the cases of conversion-type cathodes of Fe2O3 and Co3O4 due to their high polarization relieved crystal fragmentation. In addition, compared with the other five materials, V2O5 nanowire exhibits the lowest charge transfer resistance (240.2 Ω), highest lithium ion diffusion rate (10-13 ∼ 10-11 cm2 s−1) and discharge midpoint voltage (1.6 V). Thus, V2O5||PL-Si/G achieves the state-of-the-art gravimetric energy density, discharge midpoint voltage and cycle performance, giving rise to the record-high 1288 Wh kg−1 at 0.1 A g-1 in potential range of 0.3 ∼ 4.0 V. These results indicate the significance of rational material selection and effective pre-lithiation for developing high-performance full-cell LIBs.

Atomically Engineered Encapsulation of SnS2 Nanoribbons by Single-Walled Carbon Nanotubes for High-Efficiency Lithium Storage.

Rechargeable lithium-ion batteries are integral to contemporary energy storage, yet current anode material systems struggle to meet the increasing demand for extended range capabilities. This work introduces a novel composite anode material composed of one-dimensional 2H-phase tin disulfide (SnS2) nanoribbons enclosed within cavities of single-walled carbon nanotubes (SnS2@SWCNTs), achieved through precise atomic engineering. Employing aberration-corrected transmission electron microscopy, we precisely elucidated the crystal structure of SnS2 within the confines of the SWCNTs. This deliberate design effectively addresses the inherent limitations of SnS2 as a lithium-ion anode material, including its low electrical conductivity, considerable volume expansion effects, and unstable solid electrolyte interface membrane. Testing confirmed that SnS2 transforms into the Li5Sn2 alloy phase after full lithiation and back to SnS2 after delithiation, showing excellent reversibility. The composite also benefits from edge effects, improving lithium storage through stronger binding and lower migration barriers, which were supported by calculations. This pioneering work advances high-performance anode materials for applications.

Recent Progress of Deep Learning Methods for Health Monitoring of Lithium-Ion Batteries

In recent years, the rapid evolution of transportation electrification has been propelled by the widespread adoption of lithium-ion batteries (LIBs) as the primary energy storage solution. The critical need to ensure the safe and efficient operation of these LIBs has positioned battery management systems (BMS) as pivotal components in this landscape. Among the various BMS functions, state and temperature monitoring emerge as paramount for intelligent LIB management. This review focuses on two key aspects of LIB health management: the accurate prediction of the state of health (SOH) and the estimation of remaining useful life (RUL). Achieving precise SOH predictions not only extends the lifespan of LIBs but also offers invaluable insights for optimizing battery usage. Additionally, accurate RUL estimation is essential for efficient battery management and state estimation, especially as the demand for electric vehicles continues to surge. The review highlights the significance of machine learning (ML) techniques in enhancing LIB state predictions while simultaneously reducing computational complexity. By delving into the current state of research in this field, the review aims to elucidate promising future avenues for leveraging ML in the context of LIBs. Notably, it underscores the increasing necessity for advanced RUL prediction techniques and their role in addressing the challenges associated with the burgeoning demand for electric vehicles. This comprehensive review identifies existing challenges and proposes a structured framework to overcome these obstacles, emphasizing the development of machine-learning applications tailored specifically for rechargeable LIBs. The integration of artificial intelligence (AI) technologies in this endeavor is pivotal, as researchers aspire to expedite advancements in battery performance and overcome present limitations associated with LIBs. In adopting a symmetrical approach, ML harmonizes with battery management, contributing significantly to the sustainable progress of transportation electrification. This study provides a concise overview of the literature, offering insights into the current state, future prospects, and challenges in utilizing ML techniques for lithium-ion battery health monitoring.

Empowering lithium-ion batteries: The potential of 2D o-Al2N2 as an exceptional anode material through DFT analysis

Finding an appropriate new anode material with high electrochemical performance for lithium-ion batteries (LIBs) is considered one of the significant challenges for both the academic and industrial research communities. Herein, we propose to explore the efficiency of a newly designed two-dimensional (2D) material, named orthorhombic dialuminium dinitride (o-Al2N2), as an alternative anode material for LIB systems through first-principles calculations and ab initio molecular dynamics (AIMD) simulations. The obtained results show that orthorhombic-Al2N2 exhibits a high specific capacity of 1144.2913 mAhg−1, an operating voltage around 0.575 V, and a low kinetic diffusion barrier of 0.26 eV. These results prove the suitability of the o-Al2N2 monolayer as a promising anode material for LIBs with high structural stability, strong binding energy towards lithium adsorbent, fast lithium diffusion, and a high theoretical capacity. These features rank the 2D o-Al2N2 monolayer among the best choices for the anode part of the next-generation rechargeable LIBs.

A Low‐Dosage Flame‐Retardant Inorganic Polymer Binder for High‐Energy‐Density and High‐Safety Lithium‐Sulfur Batteries

AbstractThe developing electric vehicles and portable electronics urgently require rechargeable lithium batteries with high energy density and high safety. Lithium‐sulfur (Li‐S) batteries have shown significant advantages in their high energy density. However, the use of traditional polymer binders faces significant challenges, such as soluble polysulfides, large volume changes, and electrode flammability, resulting in performance degradation and safety hazards. Here, a polymeric aluminophosphate (AP) is for the first time proposed as an inorganic polymer binder to simultaneously realize high energy density, long cycling stability, and reliable safety of Li‐S batteries. Benefiting from the synergistic effect of polar P‐O and Al‐O chain segments, the AP binder provides strong mechanical adhesion, anchors polysulfides, and promotes the redox kinetics of sulfur electrodes. The AP binder also ensures high flame retardancy for sulfur electrodes at an extremely low dosage of 2 wt%. Consequently, the retardant sulfur electrode can be operated stably with high specific capacities (1190 mAh g−1), high capacity retention rates (>99.1%) during 500 cycles, and excellent rate capability (3 C). Based on the entire cell, the soft‐packaged Li‐S full battery provides high capacities (3.6 mAh cm−2), high cell energy density (415 Wh kg−1 and 297 Wh L−1), and high capacity retention rates (>99.8%).

Chemical hazard assessment toward safer electrolytes for lithium-ion batteries.

Commercialization of rechargeable lithium-ion (Li-ion) batteries has revolutionized the design of portable electronic devices and is facilitating the current transition to electric vehicles. The technological specifications of Li-ion batteries continue to evolve through the introduction of various high-risk liquid electrolyte chemicals, yet critical evaluation of the physical, environmental, and human health hazards of these substances is lacking. Using the GreenScreen for Safer Chemicals approach, we conducted a chemical hazard assessment (CHA) of 103 electrolyte chemicals categorized into seven chemical groups: salts, carbonates, esters, ethers, sulfoxides-sulfites-sulfones, overcharge protection additives, and flame-retardant additives. To minimize data gaps, we focused on six toxicity and hazard data sources, including three empirical and three nonempirical predictive data sources. Furthermore, we investigated the structural similarities among selected electrolyte chemicals using the ChemMine tool and the simplified molecular input line entry systeminputs from PubChem to evaluate whether chemicals with similar structures exhibit similar toxicity. The results demonstrate that salts, overcharge protection additives, and flame-retardant additives contain the most toxic components in the electrolyte solutions. Furthermore, carbonates, esters, and ethers account for most flammability hazards in Li-ion batteries. This study supports the complementary use of quantitative structure-activity relationship modelsto minimize data gaps and inconsistencies in CHA. Integr Environ Assess Manag 2024;20:2231-2244. © 2024 The Author(s). Integrated Environmental Assessment and Management published by Wiley Periodicals LLC on behalf of Society of Environmental Toxicology & Chemistry (SETAC).

Mapping of lithium ion concentrations in 3D structures through development of in situ correlative imaging of X-ray Compton scattering-computed tomography.

Understanding the correlation between chemical and microstructural properties is critical for unraveling the fundamental relationship between materials chemistry and physical structures that can benefit materials science and engineering. Here, we demonstrate novel in situ correlative imaging of the X-ray Compton scattering computed tomography (XCS-CT) technique for studying this fundamental relationship. XCS-CT can image light elements that do not usually exhibit strong signals using other X-ray characterization techniques. This paper describes the XCS-CT setup and data analysis method for calculating the valence electron momentum density and lithium-ion concentration, and provides two examples of spatially and temporally resolved chemical properties inside batteries in 3D. XCS-CT was applied to study two types of rechargeable lithium batteries in standard coin cell casings: (1) a lithium-ion battery containing a cathode of bespoke microstructure and liquid electrolyte, and (2) a solid-state battery containing a solid-polymer electrolyte. The XCS-CT technique is beneficial to a wide variety of materials and systems to map chemical composition changes in 3D structures.

A Naphthalenetetracarboxdiimide‐Containing Covalent Organic Polymer: Preparation, Single Crystal Structure and Battery Application

AbstractInspired by dative boron‐nitrogen (B←N) bonds proven to be the promising dynamic linkage for the construction of crystalline covalent organic polymers/frameworks (COPs/COFs), we employed 1,4‐bis(benzodioxaborole) benzene (BACT) and N,N′‐Di(4‐pyridyl)‐1,4,5,8‐naphthalenetetracarboxdiimide (DPNTCDI) as the corresponding building blocks to construct a functional COP (named as CityU‐25), which had been employed as an anode in rechargeable lithium ion batteries. CityU‐25 displayed an excellent reversible lithium storage capability of 455 mAh/g after 170 cycles at 0.1 A/g, and an impressive one of 673 mAh/g after 720 cycles at 0.5 A/g. These findings suggest that CityU‐25 is a standout candidate for advanced battery technologies, highlighting the potential application of this type of materials.

A Naphthalenetetracarboxdiimide-Containing Covalent Organic Polymer: Preparation, Single Crystal Structure and Battery Application.

Inspired by dative boron-nitrogen (B←N) bonds proven to be the promising dynamic linkage for the construction of crystalline covalent organic polymers/frameworks (COPs/COFs), we employed 1,4-bis(benzodioxaborole) benzene (BACT) and N,N'-Di(4-pyridyl)-1,4,5,8-naphthalenetetracarboxdiimide (DPNTCDI) as the corresponding building blocks to construct a functional COP (named as CityU-25), which had been employed as an anode in rechargeable lithium ion batteries. CityU-25 displayed an excellent reversible lithium storage capability of 455 mAh/g after 170 cycles at 0.1 A/g, and an impressive one of 673 mAh/g after 720 cycles at 0.5 A/g. These findings suggest that CityU-25 is a standout candidate for advanced battery technologies, highlighting the potential application of this type of materials.

Design and Validation of Advancing Autonomous Firefighting Robot

The quest for enhanced fire-fighting capabilities led to the design and validation of an autonomous firefighting robot in this study. Proteus software was leveraged for rigorous simulation, and the prototype integrated an array of components, including an IR flame sensor, servo motors, a submersible water pump, and a microcontroller-driven navigation system. Comprehensive testing was conducted with meticulous attention to component integrity and functionality, confirming the robot's ability to detect fires, navigate toward them, and effectively extinguish them using water. The robot utilized a 12V DC power supply and was powered by three 4V lithium rechargeable batteries. It seamlessly transitioned from breadboard testing to a soldered board configuration. Preliminary tests, conducted with a candle flame, validated the robot's efficacy in real-world fire detection and suppression scenarios. This innovative design highlighted the potential for robotic solutions in enhancing firefighting capabilities and ensuring safer environments.

Tartaric Acid Cross-Linking Polyvinyl Alcohol as Degradable Separators for Rechargeable Lithium Ion Batteries.

The escalating focus on environmental concerns and the swift advancement of eco-friendly biodegradable batteries raises a pressing demand for enhanced material design in the battery field. The traditional polypropylene (PP) that is monopolistically utilized in the commercial LIBs is hard to recycle. In this work, we prepare a novel water degradable separators via the cross-linking of polyvinyl alcohol (PVA) and dibasic acid (tartaric acid, TA). Through the integration of non-solvent liquid-phase separation, we successfully produced a thermally stable PVA-TA membrane with tunable thickness and a high level of porosity. These specially engineered PVA-TA separators were implemented in LiFePO4 (LFP)|separator|Li cells, resulting in superior multiplicative performance and achieving a capacity of 88 mAh g-1 under 5 C. Additionally, the straightforward small molecule cross-linking technique significantly reduced the crystalline region of the polymer, thereby enhancing ionic conductivity. Notably, after cycling, the PVA-TA separators can be easily dissolved in 95 °C hot water, enabling its reutilization for the production of new PVA-TA separators. Therefore, this work introduces a novel concept to design green and sustainable separators for recyclable lithium batteries.

Influence of iron phosphate on the performance of lithium iron phosphate as cathodic materials in rechargeable lithium batteries

Influence of iron phosphate on the performance of lithium iron phosphate as cathodic materials in rechargeable lithium batteries

3D-printed portable device for illicit drug identification based on smartphone-imaging and artificial neural networks

In this manuscript, a 3D-printed analytical device has been successfully developed to classify illicit drugs using smartphone-based colorimetry. Representative compounds of different families, including cocaine, 3,4-methylenedioxy-methamphetamine (MDMA), amphetamine and cathinone derivatives, pyrrolidine cathinones, and 3,4-methylenedioxy cathinones, have been analyzed and classified after appropriate reaction with Marquis, gallic acid, sulfuric acid, Simon and Scott reagents. A picture of the colored products was acquired using a smartphone, and the corrected RGB values were used as input data in the chemometric treatment. ANN using two active layers of nodes (6 nodes in layer 1 and 2 nodes in layer 2) with a sigmoidal transfer function and a minimum strict threshold of 0.50 identified illicit drug samples with a sensitivity higher than 83.4 % and a specificity of 100 % with limits of detection in the microgram range. The 3D printed device can operate connected to a rechargeable lithium-ion cell portable battery, is inexpensive, and requires minimal training. The analytical device has been able to discriminate the analyzed psychoactive substances from cutting and mixing agents, being a useful tool for law enforcement agents to use as a screening method.

Polyester-enhanced poly (cyclic carbonate-fluoride)-based polymer electrolyte for stable circulating solid lithium batteries

Polymer solid-state electrolytes have become one of the promising materials for constructing solid-state lithium batteries due to their excellent processability and good compatibility with electrode interfaces. However, their limited electrochemical performance and mechanical strength have hindered their widespread application. Through the adoption of an in-situ thermal curing method, we successfully prepared a poly(carbonate-fluoride) solid-state electrolyte, utilizing a polyester separator with abundant polar groups as a reinforcing framework. The introduction of ionic liquid into the solid polymer electrolyte not only enhances the mobility of polymer chain segments to improve ionic conductivity but also, in synergy with trifluoromethyl, promotes lithium salt dissociation while restricting the migration of lithium salt anions. Additionally, their reaction with the lithium metal anode generates the LiF-rich SEI, regulating the deposition of lithium dendrites. The resulting 31VPIF/OZ exhibited outstanding ionic conductivity (3.58 × 10−4 S cm−1 at 25 °C), Li-ion migration number (0.52), and electrochemical window (5.4 V). Li | 31VPIF/OZ | Li battery cycled for 1000 h at 0.1 mA cm−2 without short-circuiting. Importantly, Li | | LiFePO4 battery demonstrated a high capacity retention rate of 91.5 % after 600 cycles at 0.5C (25 °C). Thus, through the synergistic interplay of polymer structure design and fillers, we have successfully achieved stable cycling in solid-state lithium batteries, providing robust support for their application in rechargeable lithium battery technology.

Homogenous coating of Li+ conductive Li5AlO4 on single-crystalline nonstoichiometric Li1.04Ni0.92Al0.04O2 for rechargeable lithium-ion batteries

Cobalt-free, nickel-rich LiNi1-xAlxO2 (x ≤ 0.1) is an attractive cathode material because of high energy density and low cost but suffers from severe structural degradation and poor rate performance. In this study, we propose a molten salt-assisted synthesis in combination with a Li-refeeding induced aluminum segregation strategy to prepare Li5AlO4-coated single-crystalline slightly Li-rich Li1.04Ni0.92Al0.04O2. The symbiotic formation of Li5AlO4 from reaction between molten lithium hydroxide and doped aluminum in the bulk ensures a high lattice matching between the Ni-rich oxide and the homogenous conductive Li5AlO4 that permits high Li+ conductivity. Benefiting from mitigated undesirable side reactions and phase evolution, the Li5AlO4-coated single-crystalline Li1.04Ni0.92Al0.04O2 delivers a high specific capacity of 220.2 mA h g−1 at 0.1 C and considerable rate capability (182.5 mA h g−1 at 10 C). Besides, superior capacity retention of 90.8% is obtained at 1/3 C after 100 cycles in a 498.1 mA h pouch full cell. Furthermore, the particulate morphology of Li1.04Ni0.92Al0.04O2 remains intact after cycling at a cutoff voltage of 4.3 V, whereas slightly Li-deficient Li0.98Ni0.97Al0.05O2 features intragranular cracks and irreversible lattice distortion. The results highlight the value of molten salt-assisted synthesis and Li-refeeding induced elemental segregation strategy to upgrade Ni-based layered oxide cathode materials for advanced Li-ion batteries.

Recovery of lithium by pseudocapacitive electrodes in capacitive deionization

Lithium is a crucial component in rechargeable lithium-ion batteries for many applications, including the powering of electric vehicles and stationary energy storage systems. This investigation focused on two hybrid pseudocapacitive materials, the polystyrene sulfonate-MXene composite (PM) and the sodium titanate/graphene oxide composite (NG), for lithium ions recovery from aqueous Li+ resources. This was achieved by selectively removing unwanted divalent Ca2+ and Mg2+ ions, as well as monovalent K+ ions, through capacitive deionization (CDI) using a single-cell system, resulting in a final solution enriched with Li+ ions. Based on the ion selectivity order observed previously as Mg2+≈ Ca2+ >K+ > Li+, a series of CDI experiments were conducted with sequential steps to remove more selective ions first and to obtain a lithium-enriched solution with higher purity and maximum extracted fraction. Both PM and NG electrodes demonstrated promising performance when tested in binary, ternary, and quaternary ionic solutions with the recovered lithium solution purity in the range of 59.09 %-95.94 % and 59.75 %-77.17 %, respectively. Further, the highest enrichment factor values observed were SLi+,Mg2+; 268.1 for PM and SLi+,Ca2+; 44.25, for NG electrodes. The PSS-modified MXene composite electrode in obtaining the Li+ solution with the highest purity when separated Ca2+ from a binary solution. These findings offer valuable insights into the selective electrosorption of divalent ions over lithium ions through the utilization of ion intercalation pseudocapacitive nanocomposite electrodes. The obtained results hold significance in advancing novel non-precipitation techniques for the recovery of lithium ions from aqueous lithium resources.

From Inorganic to Organic Iodine: Stabilization of I+ Enabling High-Energy Lithium-Iodine Battery.

Organic materials have been considered a class of promising cathodes for metal-ion batteries because of their sustainability in preparation and source. However, organic batteries with high energy density and application potential require high discharge voltage, multielectron transfer, and long cycling performance. Here, we report an exceptional lithium-iodine (Li//I2) battery, in which the organic iodine (BPD-HI) cathode formed by the Lewis acid-base coordination between hydroiodic acid (HI) and 4,4'-bipyridine (BPD) allows 2e- transfer via the I-/I0 and I0/I+ redox couples. The I+ stabilized by BPD exhibits a high discharge voltage plateau at ∼3.4 V. Remarkably, from inorganic to organic iodine, it realizes a 2-fold increase in the achieved capacity, up to ∼400 mA h gI-1 (Theor. 422 mA h gI-1 and 245.6 mA h g-1 based on the mass of BPD-HI), and an over 2-fold energy density, reaching 1160 W h kgI-1 (Theor. 1324 W h kgI-1). More importantly, a capacity retention rate of 85% over 850 cycles is attained for the Li//BPD-HI battery at a current density of 2 A gI-1. This facile strategy enables positively charged I+ to be electrochemically active in a rechargeable lithium battery. The new redox chemistry discovered provides new insights for developing organic batteries with high energy density.

The role of graphene in SnS2@Graphene for rechargeable lithium batteries: A view from the electronic structure

Based on the first-principles study, the adsorption and electron transfer properties of Li atom at different sites of SnS2 monolayer, SnS2@Graphene 2D-nanocomposite are analyzed. The differential charge density and density of states (DOS) analysis show that the graphene substrate as an electron donor can change the 2D-nanocomposite from a semiconductor to a metal, and reduce the adsorption energy of Li atom by decreasing the charge transferring from Li atom to SnS2. This indicates that graphene substrate is beneficial for improving the performance of SnS2@Graphene. Meanwhile, the Li atoms tend not to cluster on the SnS2@Graphene 2D-nanocomposite, which is useful to prolong the lifespan of the SnS2@Graphene. The functionality of graphene in SnS2@Graphene 2D-nanocomposite is proved by other electron donor substrates, such as a two-H-atom model and a Sn (111) substrate model. All the results indicate that the graphene, as an electron donor in SnS2@Graphene 2D-nanocomposite, plays a key role in improving the performance of SnS2 in rechargeable lithium batteries.

Recent Progress in Developing High-Performance Anode Materials for Next-Generation Sodium-Ion Batteries

Rechargeable lithium-ion batteries (LIBs) have attracted great attention due to their large-scale energy storage applications such as electric vehicles (EVs) and grid-scale energy storage systems (ESSs). The ongoing transition towards EVs has accelerated ever-increasing demand for LIBs that causes the shortage of lithium metal resources and their expensive price. Therefore, great efforts have been made to exploit an alternative system that replaces the conventional LIBs. While sodium-ion batteries (SIBs) can be the most evident alternatives to LIBs based on the natural abundance and low cost of sodium resources, the major scientific challenges reside in developing the new anode materials due to the poor performance of conventional LIB anodes in Na cells, such as graphite and silicon. This article reviews the potential of SIBs as promising alternatives to LIBs and recent progress in developing high-performance anode materials for SIBs. The strengths and drawbacks of recently developed anode materials have been discussed, including graphite, hard carbon, silicon, phosphorus, and other transition metal compounds such as oxides, phosphides, and sulfides.