锂电池

Lithium-ion batteries have aided the portable electronics revolution for nearly three decades. They are now enabling vehicle electrification and beginning to enter the utility industry. The emergence and dominance of lithium-ion batteries are due to their higher energy density compared to other rechargeable battery systems, enabled by the design and development of high-energy density electrode materials. Basic science research, involving solid-state chemistry and physics, has been at the center of this endeavor, particularly during the 1970s and 1980s. With the award of the 2019 Nobel Prize in Chemistry to the development of lithium-ion batteries, it is enlightening to look back at the evolution of the cathode chemistry that made the modern lithium-ion technology feasible. This review article provides a reflection on how fundamental studies have facilitated the discovery, optimization, and rational design of three major categories of oxide cathodes for lithium-ion batteries, and a personal perspective on the future of this important area. The 2019 Nobel Prize in Chemistry has been awarded to a trio of pioneers of the modern lithium-ion battery. Here, Professor Arumugam Manthiram looks back at the evolution of cathode chemistry, discussing the three major categories of oxide cathode materials with an emphasis on the fundamental solid-state chemistry that has enabled these advances.

… cathode electrochemical performance. As the charge capacity, rate capability and cyclability of lithium ion batteries … of graphene implementation into lithium ion battery cathodes to meet …

… in battery development 11,12,13 . Here, we demonstrate that the strong coupling between lithium ion concentration and cathode … electric field into the cathode, triggering lithium ions to …

… (cathode, anode and electrolyte) of LIB, cathode material is usually the most expensive one with highest weight in the battery, … high power cathode materials for lithium ion batteries. …

… cathodes, the amount of metal ion dissolution from various lithium ion battery cathodes (… total transition metal ion dissolution found from cathodes containing , such as layered and spinel …

This paper develops a computational model that resolves the complex three-dimensional microstructure of Li-ion battery cathodes. The microstructural geometry is reconstructed from …

… and ionic conductivities of phosphate polyanion cathodes, namely, surface coating, particle … cathode materials are envisioned, which are expected to deliver lithium-ion battery cathodes …

Rapid adoption of lithium‐ion batteries for electronics and electric vehicles requires cost‐effective and efficient recycling of battery components especially the valuable cathode active materials. The direct recycling method transforms end‐of‐life (EOL) cathode materials into battery grade materials with minimal energy consumption and least environmental disruption. In direct recycling, the relithiation step to restore the lithium stoichiometry of the cathode materials is critical. In this work, a novel electrochemical relithiation approach in an aqueous electrolyte followed by a heat treatment for recycling cathode materials in EOL lithium‐ion batteries is demonstrated and analyzed. Using LiCoO2 as an example, it is shown that the recycled LiCoO2 materials show equivalent crystal structure, morphology, and electrochemical performance to the commercial LiCoO2.

The surface coating of cathodes using insulator films has proven to be a promising method for high-voltage cathode stabilization in Li-ion batteries, but there is still substantial uncertainty about how these films function. More specifically, there is limited knowledge of lithium solubility and transport through the films, which is important for coating design and development. This study uses first-principles calculations based on density functional theory to examine the diffusivity of interstitial lithium in the crystals of α-AlF3, α-Al2O3, m-ZrO2, c-MgO, and α-quartz SiO2, which provide benchmark cases for further understanding of insulator coatings in general. In addition, we propose an ohmic electrolyte model to predict resistivities and overpotential contributions under battery operating conditions. For the crystalline materials considered we predict that Li+ diffuses quite slowly, with a migration barrier larger than 0.9 eV in all crystalline materials except α-quartz SiO2, which is predicted to have a migration barrier of 0.276 eV along 〈001〉. These results suggest that the stable crystalline forms of these insulator materials, except for oriented α-quartz SiO2, are not practical for conformal cathode coatings. Amorphous Al2O3 and AlF3 have higher Li+ diffusivities than their crystalline counterparts. Our predicted amorphous Al2O3 resistivity (1789 MΩ m) is close to the top of the range of the fitted resistivities extracted from previous experiments on nominal Al2O3 coatings (7.8 to 913 MΩ m) while our predicted amorphous AlF3 resistivity (114 MΩ m) is very close to the middle of the range. These comparisons support our framework for modeling and understanding the impact on overpotential of conformal coatings in terms of their fundamental thermodynamic and kinetic properties, and support that these materials can provide practical conformal coatings in their amorphous form.

This article briefly reviews the status and new progress on the characterization of popular cathode materials for lithium-ion batteries by scanning transmission electron microscopy (…

The past decades have witnessed the rapid development of lithium-ion batteries (LIBs), whose applications nearly cover every aspect of our life. The increasing number of the spent LIBs (S-LIBs) endows...

… Olivine-based cathode materials, such as lithium iron phosphate (LiFePO4), prioritize safety … Thus, this review scrutinizes recent advancements in Li-ion battery cathode materials, …

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… As the production and consumption of lithium ion batteries (LIBs) … , Co, Al and Cu from treated cathode active materials, which are … It is confirmed that the cathode active materials are a …

Abstract With the increasing market share of lithium-ion battery in the secondary battery market and their applications in electric vehicles, the recycling of the spent batteries has become necessary. The number of spent lithium-ion batteries grows daily, which presents a unique business opportunity of recovering and recycling valuable metals from the spent lithium-ion cathode materials. Various metals including cobalt, manganese, nickel, aluminum, and lithium can be extracted from these materials through leaching with chemicals such as hydrochloric acid ( HCl ), nitric acid ( HN O 3 ), sulfuric acid ( H 2 S O 4 ), oxalate ( H 2 C 2 O 2 ), DL-malic acid ( C 4 H 5 O 6 ), citric acid ( C 6 H 8 O 7 ), ascorbic acid ( C 6 H 8 O 6 ), phosphoric acid ( H 3 P O 4 ) or acidithiobacillus ferrooxidans. This paper provides a comprehensive review on the available hydrometallurgical technologies for recycling spent lithium-ion cathode materials. The recycling processes, challenges and perspectives reported to date and recycling companies in the market are summarized. To accelerate the development of battery recycling technology toward commercialization, some potential research directions are also proposed in this paper.

… of cathode materials for high-energy lithium-ion battery and beyond-lithium-ion rechargeable battery … density and stable voltage profiles of lithium-ion batteries based on surface-coated …

… By computing stability and battery properties for those different chemical … battery properties should be expected. From this analysis, we present several novel and promising cathode …

… use of these batteries has led to significant … batteries requires necessary and appropriate solutions. Therefore, this work reviews national and international treatment methods of cathode …

Degradation mechanisms such as lithium plating, growth of the passivated surface film layer on the electrodes and loss of both recyclable lithium ions and electrode material adversely affect the longevity of the lithium ion battery. The anode electrode is very vulnerable to these degradation mechanisms. In this paper, the most common aging mechanisms occurring at the anode during the operation of the lithium battery, as well as some approaches for minimizing the degradation are reviewed.

… anode materials. This paper reviews the recent progress of using carbon nanotubes as components of anode material to improve the performance of lithium ion batteries. …

Lithium-ion battery (LIB) research and development has witnessed an immense spike in activity in recent years due to the astonishing surge in demand for portable, environmentally …

Since the birth of lithium ion battery in the end of 1980s and early 1990s many kinds of anode … As a result, modification of carbonaceous anode materials has been a research focus. In …

… anodes in the lithium ion battery and will survey use of different materials, nanoscale design of anodes … The review paper not only discusses the success of using a nanoscale anode …

The rapid expansion of electric vehicles and mobile electronic devices is the main driver for the improvement of advanced high-performance lithium-ion batteries (LIBs). The electrochemical performance of LIBs depends on the specific capacity, rate performance and cycle stability of the electrode materials. In terms of the enhancement of LIB performance, the improvement of the anode material is significant compared with the cathode material. There are still some challenges in producing an industrial anode material that is superior to commercial graphite. Based on the different electrochemical reaction mechanisms of anode materials for LIBs during charge and discharge, the advantages/disadvantages and electrochemical reaction mechanisms of intercalation-, conversionand alloyingtype anode materials are summarized in detail here. The methods and strategies for improving the electrochemical performance of different types of anode materials are described in detail. Finally, challenges for the future development of LIBs are also considered. This review offers a meaningful reference for the construction and performance optimization of anode materials for LIBs.

… Lithium ion batteries (LIBs) possess energy densities higher than those of the conventional batteries, but … Here, the lithium storage mechanism of anode materials and the Goodenough …

… lithium-ion battery technology. Owing to the research and discoveries in recent years, lithium-ion batteries (… In this review article, recent advances in the development of anode materials …

Since the invention of lithium‐ion batteries as a rechargeable energy storage system, it has uncommonly promoted the development of society. It has a wide variety of applications in electronic equipment, electric automobiles, hybrid vehicles, and aerospace. As an indispensable component of lithium‐ion batteries, anode materials play an essential role in the electrochemical characteristics of lithium‐ion batteries. In this review, we described the development from lithium‐metal batteries to lithium‐ion batteries in detail on the time axis as the first step; This was followed by an introduction to several commonly used anode materials, including graphite, silicon, and transition metal oxide with discussions the charge‐discharge mechanism, challenges and corresponding strategies, and a collation of recent interesting work; Finally, three anode materials are summarized and prospected. Hopefully, this review can serve both the newcomers and the predecessors in the field.

… Like the suppression of Li dendrite growth in Li metal anodes, for lithium ion batteries, … be applied in lithium ion batteries as well. In addition, as Li deposition on graphite anode is an …

… of graphynes as lithium ion battery anodes through the first-… the range suitable to be used as anodes. Furthermore, the maximum … can serve as high-capacity lithium ion battery anodes. …

… In order to evaluate the thermal safety issue of carbon-coated Si as an anode material for lithium-ion batteries, we performed differential scanning calorimetry (DSC) studies on lithiated …

… Since lithium-ion batteries were introduced by Sony in the … , remained unchanged (graphitic anode, cathode). Nevertheless, … anode materials to increase the energy stored in lithium-ion …

… generation lithium-ion battery (LIB) anodes due … anode. Extensive research has been carried out to resolve the problem since early 1990s. For the first time, the studies on the Si anode …

… Silicon has long been regarded as a prospective anode material for lithium-ion batteries. … This work provides a historical context for the development of silicon anodes and focuses on …

… and graphitic anodes seem to be the preferred electrode materials for lithium ion batteries in … The performance of lithium ion batteries strongly depends on the type of electrode material […

… of lithium-ion batteries for … lithium-ion batteries. Although “common” TVD carbon-coated natural graphite can meet most of the practical needs for anode materials in lithium-ion batteries …

As the most commonly used potential energy conversion and storage devices, lithium-ion batteries (LIBs) have been extensively investigated for a wide range of fields including information technology, electric and hybrid vehicles, aerospace, etc. Endowed with attractive properties such as high energy density, long cycle life, small size, low weight, few memory effects and low pollution, LIBs have been recognized as the most likely approach to be used to store electrical power in the future. This review will start with a brief introduction to charge–discharge principles and performance assessment indices. The advantages and disadvantages of several commonly studied anode materials including carbon, alloys, transition metal oxides and silicon along with lithium intercalation will be reviewed. The mechanism and synthesis methods, followed by strategies to enhance battery performance by virtue of interesting structural designs will be examined. Finally, a few issues needing further exploration will be discussed followed by a brief outline of the prospects and outlook for the LIB field.

… Lithium-ion batteries are used in different technologies such as the Hybrid Electric Vehicles (… both battery as well as electric motor engines to increase the fuel efficiency [1]. A battery is …

… lithium-ion (Li-ion) battery anodes. Various elements have been utilized in innovative structures to enable these anodes… decrease the cost of Li-ion batteries. In this review, electrode and …

In recent years, the rapid development of modern society is calling for advanced energy storage to meet the growing demands of energy supply and generation. As one of the most promising energy storage systems, secondary batteries are attracting much attention. The electrolyte is an important part of the secondary battery, and its composition is closely related to the electrochemical performance of the secondary batteries. Lithium-ion battery electrolyte is mainly composed of solvents, additives, and lithium salts, which are prepared according to specific proportions under certain conditions and according to the needs of characteristics. This review analyzes the advantages and current problems of the liquid electrolytes in lithium-ion batteries (LIBs) from the mechanism of action and failure mechanism, summarizes the research progress of solvents, lithium salts, and additives, analyzes the future trends and requirements of lithium-ion battery electrolytes, and points out the emerging opportunities in advanced lithium-ion battery electrolytes development.

This paper reviews electrolyte additives used in Li-ion batteries. According to their functions, the additives can be divided into these categories: (1) solid electrolyte interface (SEI) …

… of present liquid electrolytes), we then discuss innovative electrolyte systems based on … as lithium-ion conducting media, finally closing with a brief paragraph on solid-state electrolytes (…

… electrolytes such as LiPF 6 salt in mixed-carbonate solvents with additives for the state-of-the-art Li-ion batteries as well as new electrolyte … the characterization of electrolyte materials for …

… the electrolyte, were found to be operable at temperatures down to −40C. Further, the new electrolyte … electrodes in lithium-ion cells, was also investigated in the new electrolyte and the …

A solid electrolyte interphase (SEI) is generated on the anode of lithium-ion batteries during the first few charging cycles. The SEI provides a passivation layer on the anode surface, which inhibits further electrolyte decomposition and affords the long calendar life required for many applications. However, the SEI remains poorly understood. Recent investigations of the structure of the initial SEI, along with changes which occur to the SEI upon aging, have been conducted. The investigations provide significant new insight into the structure and evolution of the anode SEI. The initial reduction products of ethylene carbonate (EC) are lithium ethylene dicarbonate (LEDC) and ethylene. However, the instability of LEDC generates an intricate mixture of compounds, which greatly complicates the composition of the SEI. Mechanisms for the generation of the complicated mixture of products are presented along with the differences in the SEI structure in the presence of electrolyte additives.

Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) is a widely used lithium (Li) salt that is extensively studied in the field of electrolytes for Li‐ion batteries (LIBs) to improve their performance. A thorough understanding of its underlying mechanisms in LIBs is crucial for gaining deeper insights into its future development. This paper provides an extensive review of the role of LiTFSI in enhancing battery performance, including its benefits for negative electrode protection, the facilitation of fast charging capabilities, and the promotion of battery operation across a wide temperature range. It also highlights the specific drawbacks of LiTFSI in the electrolyte domain and examines potential solutions. By leveraging the unique properties of LiTFSI, the strategies for its effective utilization in current research are outlined. Finally, the paper discusses the lack of research into the mechanism of LiTFSI in interface protection, particularly the evolution mechanisms of multi‐component Li salts at the positive and negative electrode interfaces, and it reasonably anticipates the potential applications of LiTFSI in the realm of non‐liquid batteries. This study not only provides a more comprehensive and profound understanding of LiTFSI but also aids in the exploration of novel electrolyte systems.

… formation mechanism depend mainly on the electrolyte's composition. The most … lithium ion batteries is the use of electrolyte additives. During the past several years, various electrolyte …

… are widely used as electrolytes in lithium-ion batteries. They are … of the requirements for the lithium-ion battery electrolytes (high … of the electrolyte decomposition is of great importance. …

Abstract Electrolyte as the most flammable component of lithium ion battery is always considered to be closely related to its safety. Great efforts are made to optimize electrolyte since it is the ultimate means to improve the lithium ion battery safety. This article reviews the thermal risk of commercial electrolytes and the development of safer electrolytes. The main reason for the thermal instability of the traditional nonaqueous electrolyte is the thermal decomposition of lithium hexafluorophosphate (LiPF6) and highly flammable solvents. Substitution technique of the lithium salt is under developing and the electrolyte flame retardant additives are widely studied. Novel addition technologies like electrospinning and microcapsules are introduced to reduce the restrictions on physical properties of flame retardants and improve electrochemical performances. Overcharge protection additives are simply summarized according to their reaction mechanism. For the breakthrough of new generations of safer electrolytes, nonflammable solvents with new salts and solid state electrolytes are reviewed as well as their existing problems at present. This shall serve as a summary for the development of electrolytes and a reference for the design of next generation of safer electrolytes.

A review on liquid electrolyte design for LIBs operating under low-temperature (<0 °C) conditions. Covers various processes that determine performance below 0 °C and recent literature on electrolyte-based strategies to improve said performance.

… the flammability of the electrolyte when exposed to air and also … new electrolytes are often called “functional electrolytes”. … salt electrolytes applied to alkali metal and lithium-ion batteries. …

With increasing energy storage demands across various applications, reliable batteries capable of performing in harsh environments, such as extreme temperatures, are crucial. However, current lithium‐ion batteries (LIBs) exhibit limitations in both low and high‐temperature performance, restricting their use in critical fields like defense, military, and aerospace. These challenges stem from the narrow operational temperature range and safety concerns of existing electrolyte systems. To enable LIBs to function effectively under extreme temperatures, the optimization and design of novel electrolytes are essential. Given the urgency for LIBs operating in extreme temperatures and the notable progress in this research field, a comprehensive and timely review is imperative. This article presents an overview of challenges associated with extreme temperature applications and strategies used to design electrolytes with enhanced performance. Additionally, the significance of understanding underlying electrolyte behavior mechanisms and the role of different electrolyte components in determining battery performance are emphasized. Last, future research directions and perspectives on electrolyte design for LIBs under extreme temperatures are discussed. Overall, this article offers valuable insights into the development of electrolytes for LIBs capable of reliable operation in extreme conditions.

… electrolytes effectively improve the reaction kinetics via accelerating Li-ion diffusion in the bulk electrolyte … offers perspectives on electrolyte designs for low-temperature Li-ion batteries. …

… battery’s charge capacity, cycling performance, safety performance, and so on. In general, the electrolyte of a lithium-ion battery is … ideal electrolyte solvent for lithium-ion batteries should …

Lithium-ion batteries have dominated the energy market from portable electronic devices to electric vehicles. However, the LIBs applications are limited seriously when they were operated in the cold regions and seasons if there is no thermal protection. This is because the Li+ transportation capability within the electrode and particularly in the electrolyte dropped significantly due to the decreased electrolyte liquidity, leading to a sudden decline in performance and short cycle-life. Thus, design a low-temperature electrolyte becomes ever more important to enable the further applications of LIBs. Herein, we summarize the low-temperature electrolyte development from the aspects of solvent, salt, additives, electrolyte analysis, and performance in the different battery systems. Then, we also introduce the recent new insight about the cation solvation structure, which is significant to understand the interfacial behaviors at the low temperature, aiming to guide the design of a low-temperature electrolyte more effectively.

… electrolyte. Turning to Newman’s original lithium ion battery models, we demonstrate that electrolytes … traditional carbonate-based liquid electrolytes would allow higher power densities …

The mitigation of decomposition reactions of lithium-ion battery electrolyte solutions is of critical importance in controlling device lifetime and performance. However, due to the complexity of the system, exacerbated by the diverse set of electrolyte compositions, electrode materials, and operating parameters, a clear understanding of the key chemical mechanisms remains elusive. In this work, operando pressure measurements, solution NMR, and electrochemical methods were combined to study electrolyte oxidation and reduction at multiple cell voltages. Two-compartment LiCoO2/Li cells were cycled with a lithium-ion conducting glass–ceramic separator so that the species formed at each electrode could be identified separately and further reactions of these species at the opposite electrode prevented. One principal finding is that chemical oxidation (with an onset voltage of ∼4.7 V vs Li/Li+ for LiCoO2), rather than electrochemical reaction, is the dominant decomposition process at the positive electrode surface in this system. This is ascribed to the well-known release of reactive oxygen at higher states-of-charge, indicating that reactions of the electrolyte at the positive electrode are intrinsically linked to surface reactivity of the active material. Soluble electrolyte decomposition products formed at both electrodes are characterized, and a detailed reaction scheme is constructed to rationalize the formation of the observed species. The insights on electrolyte decomposition through reactions with reactive oxygen species identified through this work have a direct impact on understanding and mitigating degradation in high-voltage/higher-energy-density LiCoO2-based cells, and more generally for cells containing nickel-containing cathode materials (e.g., LiNixMnyCozO2; NMCs), as they lose oxygen at lower operating voltages.

Lithium metal (Li0 ) rechargeable batteries (LMBs), such as systems with a Li0 anode and intercalation and/or conversion type cathode, lithium-sulfur (Li-S), and lithium-oxygen (O2 )/air (Li-O2 /air) batteries, are becoming increasingly important for electrifying the modern transportation system, with the aim of sustainable mobility. Although some rechargeable LMBs (e.g. Li0 /LiFePO4 batteries from Bolloré Bluecar, Li-S batteries from OXIS Energy and Sion Power) are already commercially viable in niche applications, their large-scale deployment is hampered by a number of formidable challenges, including growth of lithium dendrites, electrolyte instability towards high voltage intercalation-type cathodes, the poor electronic and ionic conductivities of sulfur (S8 ) and O2 , as well as their corresponding reduction products (e.g. Li2 S and Li2 O), dissolution, and shuttling of polysulfide (PS) intermediates. This leads to a short lifecycle, low coulombic/energy efficiency, poor safety, and a high self-discharge rate. The use of electrolyte additives is considered one of the most economical and effective approaches for circumventing these problems. This Review gives an overview of the various functional additives that are being applied and aims to stimulate new avenues for the practical realization of these appealing devices.

Abstract Due to the rapid growth in the demand for high-energy density lithium battery in energy storage systems and inadequate global lithium reserves, the configuration of limited lithium (e.g., with a thickness of 20 ​μm or less) as anode offers a path for the widespread deployment of lithium metal batteries (LMBs) with high safety as well as high energy density. The contradiction between the high cost of thin Li foil and severe safety hazard of huge excess Li has inspired the development of LMBs with zero-excess Li anode, also called anode-free lithium metal batteries (AFLMBs). In this review, we aim to spotlight the researches of AFLMBs over the past two decades, the main progress and remaining obstacles for the development of AFLMBs are comprehensively evaluated and the feasibility and limitations of the state-of-the-art anode-free designs are also discussed. Moreover, the prospects of AFLMBs with respect to both scientific research and practical application are also given.

… if the Li + ions extracted from a cathode can be reversibly plated onto and stripped from a Cu current collector (as Li metal), then it is possible to assemble a rechargeable Li battery with …

… Based on these outstanding properties, lithium metal batteries were proposed … rechargeable Li metal batteries were developed. A notable example was a battery composed of a Li metal …

… We can conclude from these studies that rechargeable batteries with lithium metal anodes containing electrolyte solutions based on alkyl carbonates, ethers, or ester solvents may have, …

… Li metal in a rechargeable Li metal battery needs to be plated on or stripped from substrates repeatedly during charge/discharge processes. Therefore, Li … rechargeable Li metal batteries…

… protocol for handling rechargeable Li metal batteries, but rather a summary of the knowledge gathered during the early stage of research on rechargeable Li metal batteries and subject …

For Abstract see ChemInform Abstract in Full Text.

… Rechargeable lithium metal batteries have been regarded as one of the most attractive high-energy-density batteries … reduction potential of metallic lithium. However, the uncontrollable …

In this review, we focus on the conversion reaction in newly raised rechargeable lithium batteries instanced by lithium-sulfur and lithium-oxygen batteries. A comprehensive discussion is made on the fundamental electrochemistry and recent advancements in key components of both types of the batteries. The critical problems in the Li-S and Li-O2 conversion electrochemistry are addressed along with the corresponding improvement strategies, for the purpose of shedding light on the rational design of batteries to reach optimal performance.

Rechargeable lithium metal batteries (LMBs) have attracted wide attention for future electric vehicles and next‐generation energy storage because of their exceptionally high specific energy density. Recently, the development of electrode materials for LMBs has been extensively discussed and reviewed in the literature, but there have been very few reports that systematically review the status and progress of electrolytes for such applications. Actually, the viability of practical LMBs critically depends on the development of suitable liquid electrolytes due to the high reactivity of Li metals toward most solvents. This paper provides a systematic summary of the background and recent advances of the electrolytes for LMBs with an emphasis on the thermodynamic and kinetic stabilities at the interfaces. In addition, the emerging advanced characterization techniques for understanding the electrolyte–electrode interfaces are surveyed. Finally, a perspective for future directions is provided.

Abstract Enabling the rechargeable lithium metal batteries (LMBs) is essential for exceeding the energy density of today's Lithium-ion batteries. However, practical challenges in almost all components of LMBs, of which the most serious issues are formation of Li dendrites and uncontrollable volume expansion of lithium metal anodes, hinder their practical applications. Traditional LMBs’ fabrication techniques have some limitations in controlling the geometry and structure of components, which compromises their performance. 3D printing is an ideal manufacturing technique that can increase the specific energy and power density of devices by precisely controlling their geometry and structure from nanoscale to macroscale without relying on any templates. In this work, we review recent advances of 3D printing in rechargeable LMBs in combination with their fundamental principles and representative printing techniques. Then we discuss the applications at component levels. Finally, we summarize the design rationales and practical challenges of 3D printed rechargeable LMBs and give our insights about future outlook of this emerging field.

Rechargeable lithium-metal batteries with a cell-level specific energy of >400 Wh kg -1 are highly desired for the next-generation storage applications, yet the research has been retarded by poor electrolyte-electrode compatibility and rigorous safety concerns. In this work, we show that by simply formulating the composition of conventional electrolytes, a hybrid electrolyte was constructed to ensure high (electro)chemical and thermal stability with both the Li-metal anode and the high-nickel layered oxide cathodes. By employing the new electrolyte, Li||LiNi 0.6 Co 0.2 Mn 0.2 O 2 cells show favorable cycling and rate performance, and a 10-Ah Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch cell demonstrates a practical specific energy of >450 Wh kg -1 . Our findings shed light on reasonable design of electrolyte and electrode/electrolyte interface towards practical realization of high-energy rechargeable batteries.

… Lithium metal is recognized as promising anode materials for achieving high energy density lithium metal batteries (LMBs) due to it has high theoretical capacity (3860 mAh g -1 ) and …

The formation of electrochemically inactive, or “dead”, lithium limits the reversibility of lithium metal batteries. Here the authors elucidate the (electro)chemical roles of ethylene gas produced from electrolyte decomposition on the formation of inactive lithium. The formation of inactive lithium by side reactions with liquid electrolyte contributes to cell failure of lithium metal batteries. To inhibit the formation and growth of inactive lithium, further understanding of the formation mechanisms and composition of inactive lithium are needed. Here we study the impact of gas producing reactions on the formation of inactive lithium using ethylene carbonate as a case study. Ethylene carbonate is a common electrolyte component used with graphite-based anodes but is incompatible with Li metal anodes. Using mass spectrometry titrations combined with ^13C and ^2H isotopic labeling, we reveal that ethylene carbonate decomposition continuously releases ethylene gas, which further reacts with lithium metal to form the electrochemically inactive species LiH and Li_2C_2. In addition, phase-field simulations suggest the non-ionically conducting gaseous species could result in an uneven distribution of lithium ions, detrimentally enhancing the formation of dendrites and dead Li. By optimizing the electrolyte composition, we selectively suppress the formation of ethylene gas to limit the formation of LiH and Li_2C_2 for both Li metal and graphite-based anodes.

Rechargeable Li‐metal batteries (RLBs) can boost energy yet possess poor cycle stability and safety concerns when utilizing carbonate electrolytes. Countless effort has been invested in researching and developing electrolytes for RLBs to obtain stable and safe batteries. However, only few existing electrolytes meet the requirements for practical RLBs. In this perspective, the challenges of organic liquid electrolytes in the application in RLBs are summarized, and requirements for electrolytes for practical RLBs are proposed. This perspective briefly reviews the recent achievements of electrolytes (liquid‐ and solid‐state) for RLBs and analyzes the corresponding drawbacks of each electrolyte. Further, possible solutions to the existing shortcomings of various electrolytes are proposed. In particular, this perspective outlines the development strategy of in situ gelation electrolytes, accompanied by a call for people using pouch cells to evaluate performance and paying more attention to battery safety research. This perspective aims to expound on the challenges and the possible research directions of RLBs electrolytes to promote practical RLBs better.

Summary Lithium (Li)-metal batteries have regained broad interest in the battery research community. Although many studies on Li anode have been published in recent years, it is difficult to evaluate and compare these advances for practical applications. A key challenge is a gap between materials and component properties and the achievable large-format cell-level performance. In this paper, we investigate the critical experimental parameters that determine the cycle number of coin cells to understand the performance variations reported in the literature. To define the range of cell parameters, we exemplify a representative Li-metal pouch cell with specific energy of 300 Wh/kg to provide an effective validation of electrode materials and accurate cell performance evaluations. Based on the pouch-cell-level requirements, we propose a set of coin-cell parameters and testing conditions to expedite the discovery of new materials and their full integration into realistic battery systems.

… However, uncontrollable lithium … lithium metal batteries out of practical applications. This review presents a comprehensive overview of the lithium metal anode and its dendritic lithium …

… To summarize, we have shown that a solid block copolymer electrolyte addresses some of the problems with rechargeable lithium metal batteries. By replacing a homopolymer …

Lithium-ion (Li-ion) batteries have been utilized increasingly in recent years in various applications, such as electric vehicles (EVs), electronics, and large energy storage systems due to their long lifespan, high energy density, and high-power density, among other qualities. However, there can be faults that occur internally or externally that affect battery performance which can potentially lead to serious safety concerns, such as thermal runaway. Thermal runaway is a major challenge in the Li-ion battery field due to its uncontrollable and irreversible nature, which can lead to fires and explosions, threatening the safety of the public. Therefore, thermal runaway prognosis and diagnosis are significant topics of research. To efficiently study and develop thermal runaway prognosis and diagnosis algorithms, thermal runaway modeling is also important. Li-ion battery thermal runaway modeling, prediction, and detection can help in the development of prevention and mitigation approaches to ensure the safety of the battery system. This paper provides a comprehensive review of Li-ion battery thermal runaway modeling. Various prognostic and diagnostic approaches for thermal runaway are also discussed.

The broader application of lithium-ion batteries (LIBs) is constrained by safety concerns arising from thermal runaway (TR). Accurate prediction of TR is essential to comprehend its underlying mechanisms, expedite battery design, and enhance safety protocols, thereby significantly promoting the safer use of LIBs. The complex, nonlinear nature of LIB systems presents substantial challenges in TR modeling, stemming from the need to address multiscale simulations, multiphysics coupling, and computing efficiency issues. This paper provides an extensive review and outlook on TR modeling technologies, focusing on recent advances, current challenges, and potential future directions. We begin with an overview of the evolutionary processes and underlying mechanisms of TR from multiscale perspectives, laying the foundation for TR modeling. Following a comprehensive understanding of TR phenomena and mechanisms, we introduce a multiphysics coupling model framework to encapsulate these aspects. Within this framework, we detail four fundamental physics modeling approaches: thermal, electrical, mechanical, and fluid dynamic models, highlighting the primary challenges in developing and integrating these models. To address the intrinsic trade-off between computational accuracy and efficiency, we discuss several promising modeling strategies to accelerate TR simulations and explore the role of AI in advancing next-generation TR models. Last, we discuss challenges related to data availability, model scalability, and safety standards and regulations.

… to destabilize and degrade, which eventually leads to the failure of the battery. … thermal runaway processes, which consists of thermal runaway initiation mechanisms, thermal runaway …

Summary This paper summarizes the mitigation strategies for the thermal runaway of lithium-ion batteries. The mitigation strategies function at the material level, cell level, and system level. A time-sequence map with states and flows that describe the evolution of the physical and/or chemical processes has been proposed to interpret the mechanisms, both at the cell level and at the system level. At the cell level, the time-sequence map helps clarify the relationship between thermal runaway and fire. At the system level, the time-sequence map depicts the relationship between the expected thermal runaway propagation and the undesired fire pathway. Mitigation strategies are fulfilled by cutting off a specific transformation flow between the states in the time sequence map. The abuse conditions that may trigger thermal runaway are also summarized for the complete protection of lithium-ion batteries. This perspective provides directions for guaranteeing the safety of lithium-ion batteries for electrical energy storage applications in the future.

The cause of the thermal runaway problem in lithium-ion batteries problem is still unclear. This bottle neck has prevented increases in the energy density of lithium-ion batteries, of which the technology may stagnate for many years. The diversity of cell chemistries makes this problem more difficult to analyze. This paper reports work conducted by Tsinghua University and its collaborators into the establishment of a thermal analysis database. The database contains comparable data for different kinds of cells using accelerating rate calorimetry and differential scanning calorimetry. Three characteristic temperatures are summarized based on the common features of the cells in the database. In attempting to explain the mechanisms that are responsible for the characteristic temperature phenomena, we have gained new insight into the thermal runaway mechanisms of lithium-ion batteries. The results of specially designed tests show that the major heat source during thermal runaway for cells with Li(NixCoyMnz)O2 cathode and carbon-based anode is the redox reaction between the cathode and anode at high temperature. In contrast to what is commonly thought, internal short circuits are responsible for very little of the total heat generated during thermal runaway, although they contribute to triggering the redox reactions after the separator collapses. The characteristic temperatures provide comparable parameters that are useful in judging the safety of a newly designed battery cell. Moreover, the novel interpretation of the thermal runaway mechanism provide guidance for the safety modelling and design of lithium-ion batteries.

… Finally, the methods of thermal runaway monitoring and thermal management are … This article introduces the thermal runaway of lithium-ion batteries comprehensively, involving the cell …

Summary We demonstrate herein that not only internal short circuiting, but also chemical crossover, is the mechanism behind thermal runaway that can occur in lithium-ion batteries due to abuse conditions. In situ experiments showed that during thermal runaway, the cathode releases oxygen by a phase transition, and this oxygen is consumed by the lithiated anode. The released highly oxidative gas reacts with reductive LiCx with tremendous heat generation centered at 274.2°C with heat flow of 87.8 W g−1. To confirm the proposed mechanism, we froze a battery undergoing the thermal runaway process by liquid nitrogen and subjected it to detailed post-test analysis. Our results revealed the hidden thermal runaway mechanism of chemical crossover between the battery components without a severe internal short circuit. These findings provide an important insight into the rational design of automotive lithium-ion batteries as well as solid-state batteries.

Abstract Thermal runaway is a major concern for the large-scale application of lithium-ion batteries. The thermal runaway performance of lithium-ion batteries not only depends on materials and cell design, but also changes with degradation. This paper presents a comparative investigation of the aging effects on the thermal runaway behavior of a large format lithium-ion battery. The batteries are first degraded under four different aging paths. The aging mechanisms are then investigated through post-mortem analysis on the battery at the end of life, by comparing the electrochemical properties, morphology and composition of the fresh and degraded electrodes. The thermal stabilities of the fresh and degraded electrodes are also evaluated using differential scanning calorimetry. Adiabatic thermal runaway tests are performed on the batteries at different states of health using accelerating rate calorimetry to reveal the evolution of battery thermal runaway performance under the four degradation paths. Finally, the correlations between the aging mechanism and the changes in battery thermal runaway behavior are summarized. The results show that the thermal stability of the anode+electrolyte thermodynamic system exhibits obvious changes, which contribute to the evolution of battery thermal runaway performance, while the thermal stability of the cathode remained unchanged. Lithium plating turns out to be the key reason for the deterioration of battery thermal runaway performance during aging process.

Lithium-ion batteries are widely used in electric vehicles because of their high energy density and long cycle life. However, the spontaneous combustion accident of electric vehicles caused by thermal runaway of lithium-ion batteries seriously threatens passengers' personal and property safety. This paper expounds on the internal mechanism of lithium-ion battery thermal runaway through many previous studies and summarizes the proposed lithium-ion battery thermal runaway prediction and early warning methods. These methods can be classified into battery electrochemistry-based, battery big data analysis, and artificial intelligence methods. In this paper, various lithium-ion thermal runaway prediction and early warning methods are analyzed in detail, including the advantages and disadvantages of each method, and the challenges and future development directions of the intelligent lithium-ion battery thermal runaway prediction and early warning methods are discussed.

… of thermal runaway in commercial lithium-ion cells of the type … temperature of exothermic reactions of thermal runaway and … of the thermal runaway and decreases the temperature of its …

… However, thermal runaway behavior has become the biggest safety hazard. To … of thermal runaway warning techniques. The mechanism and characteristic behavior of thermal runaway …

… Thermal runaway is the key scientific problem in battery safety research. Therefore, this … review on the thermal runaway mechanism of the commercial lithium ion battery for electric …

… the overcharge problem of lithium ion battery. The result shows … temperature of thermal runaway are the two effective ways to improve the overcharge performance of lithium ion battery…

… The cell-to-cell thermal runaway propagation behavior has been characterized. Results … The present work details the thermal runaway propagation behavior of the lithium-ion battery …

Thermal runaway incidents involving lithium-ion batteries (LIBs) occur frequently and pose a considerable safety risk. This comprehensive review explores the characteristics and …

Abstract Lithium-ion batteries have many advantages such as the high specific energy, the high specific power, the long calendar life, being environmentally friendly, and can be used without the memory effect. Thus this type of battery is widely used as the core component in many applications such as electric vehicles, portable electronic devices, and distributed energy storage systems. However, lithium-ion batteries can easily develop into thermal runaways due to the stress and abuse from mechanical, electrical, and thermal perspectives, posing a major threat to the overall safety of many battery systems. On the premise of passing the manufacturer's safety inspections, a variety of methods for monitoring and detecting thermal runaway events are developed to enhance the safety and robustness of lithium-ion batteries in different application scenarios. This paper thus summarizes the existing literature on this topic and presents a comparative study on the sensitivity of various monitoring and detection methods. Potential future research directions are also discussed in detail to further enhance the safety and robustness of lithium-ion battery systems.

… This thermal runaway poses a significant threat to the safe operation of lithium-ion batteries. In this paper, we delve into the working principles of lithium-ion batteries and provide a …

Abstract The issue of thermal runaway (TR) of Li-ion batteries is a topic of serious concern in electric vehicles and energy storage systems. In this paper, the feature of battery TR, including self-accelerating decomposition temperature, voltage variation, temperature rise, and composition transformation, were comprehensively investigated under various states of charge (SOC). Li-ion batteries with five degrees of SOC from 0% to 100% were tested under four levels of oven temperature from 145 to 205 °C. The response to thermal behavior indicates that the ambient condition can be divided into safe, critical, and hazardous regions. The lower limit of the critical region decreases by about 40 °C when the SOC increases from 0% to 100%. During the transition process of TR, cathode material gradually degrades to small particles and finally turns to powdered metallic oxide, and the inorganic compounds on anode surface become uneven. Through heat flow tests and the modified Thomas model, the critical temperatures of TR were predicted at 212 °C, 220 °C, 179 °C, 164 °C and 183 °C for 0%, 25%, 50%, 75% and 100% SOC cells, respectively. The predictions are close to the critical regions divided by oven tests.

Thermal runaway (TR) is a major safety concern in lithium-ion batteries. Model-based TR prediction is critically needed to optimize safety designs of cells. This paper presents a novel scheme for developing reliable battery TR model from kinetics analysis of cell components. First, differential scanning calorimetry (DSC) tests on the individual cell components and their mixtures are conducted to reveal the TR mechanism and characterize the exothermic reactions, of which the major six (such as the decomposition of solid electrolyte interface (SEI) film) are determined as the dominant heat sources. The kinetics parameters of each exothermic reactions are identified from the DSC tests results at variant heating rates using Kissinger’s method and nonlinear fitting method. A predictive battery TR model is established by superimposing the chemical kinetics equations of the six exothermic reactions. The model fits well with the adiabatic TR test results and the oven tests results of a 24 Ah lithium-ion battery, indicating that the model can well reflect the battery TR mechanism and be trusted to predict battery safety performance without assembling a real battery.

The last couple of decades have seen unprecedented demand for high-performance batteries for electric vehicles, aerial surveillance technology, and grid-scale energy storage. The European Council for Automotive R&D has set targets for automotive battery energy density of 800Wh L , with 350Wh kg 1 specific energy and 3500W kg 1 peak specific power. However, the push toward ever higher energy and power densities increases the risk of dangerous accidental release of energy from the batteries. Although lithium-ion batteries have become safer in many ways since their invention, there remains the risk of fire and explosion caused by thermal runaway (TR). This is an exponential increase in temperature at a rate that cannot be dissipated quickly enough to the surroundings, caused by exothermic chemical decomposition of the materials inside the cells. The heat generated can propagate to other cells, causing a dangerous chain reaction where neighboring cells also begin to undergo TR. This can result in the entire battery pack being consumed in a fire or even exploding. Most reported incidents of TR were caused by internal or external short circuits resulting from abuse of the cell or by suboptimal cell design. For example, short circuits resulting from the crash of a Tesla model X in China in 2017 caused the battery pack to catch fire. A famous example of a design issue is the recall of the Samsung Note 7 in 2016 due to an excessively thin separator which led to short circuits, causing several devices to explode. The risks associated with TR have practical implications for how lithium-ion batteries can be transported, stored, and used. For example, lithium-ion batteries have caught fire in the hold of commercial aircraft, and there are now UN regulations regarding their safe transportation. Fires caused by lithium-ion battery failure onboard a ferry in 2019, in a parked Jaguar i-Pace in 2018, and other similar incidents have prompted requests for further improvement in lithium-ion battery testing standards to reflect real conditions of use. All lithium-ion batteries must go through safety and abuse tests, based on those recommended by the Society of Automotive Engineers (SAE). These include mechanical, thermal, and electrical abuses, designed to create conditions that could lead to TR (Figure 1). It is essential to develop lithiumion batteries that do not undergo TR, even when subjected to conditions of extreme abuse. The ideal design would prevent flow of electric current as soon as the internal cell temperature starts to increase close to the level that can cause TR, to prevent any risks of fire or damage to the cells. This Review provides an overview of the recent progress in various aspects of TR prevention. Different strategies for Dr. R. D. McKerracher, Dr. J. Guzman-Guemez, Prof. R. G. A. Wills, Prof. S. M. Sharkh Faculty of Engineering & the Environment University of Southampton Southampton SO17 1BJ, UK E-mail: R.D.McKerracher@soton.ac.uk Prof. D. Kramer Faculty of Mechanical Engineering Helmut-Schmidt University Holstenhofweg 85, 22043 Hamburg, Germany

… of separators on lithium-ion transport, and how separators can be … in membrane separators for rechargeable lithium-ion batteries. … A review describing lithium-ion battery separator types, …

For the proper design and evaluation of next‐generation lithium‐ion batteries, different physical‐chemical scales have to be considered. Taking into account the electrochemical principles and methods that govern the different processes occurring in the battery, the present review describes the main theoretical electrochemical and thermal models that allow simulation of the performance of lithium‐ion batteries, including different materials and components (electrodes and separators) and battery geometries. As the separator plays an essential role in the performance and safety of lithium‐ion batteries, the recent theoretical simulation work for this battery component are shown, with particular emphasis on morphology, dendrite growth, ionic transport, and mechanical properties. Further theoretical simulations and modeling of this battery component are still required for improving performance, taking into consideration varying geometric parameters such as pore size, porosity, and tortuosity as well as the optimization of the lithium diffusion process and ionic conductivity value. Theoretical simulations of battery separators will play an essential role in the new generation of lithium‐ion batteries, allowing the improvement of their performance while reducing experimental probes and time.

Abstract Lithium-ion battery separators are receiving increased consideration from the scientific community. Single-layer and multilayer separators are well-established technologies, and the materials used span from polyolefins to blends and composites of fluorinated polymers. The addition of ceramic nanoparticles and separator coatings improves thermal and mechanical properties, as well as electrolyte uptake and ionic conductivity. The state-of-art separators are actively involved in the cell chemistry through specific functional groups on their surface. Among the numerous properties, safety features and long cycle life are high-priority requirements for next-generation lithium-ion batteries.

… The overall stability of the lithium ion battery separators, under potentially extreme battery … It is worthwhile to note that the commercial separator tested in this work is a separator with a …

Ionic liquids (ILs) are widely studied as a safer alternative electrolyte for lithium‐ion batteries. The properties of IL electrolytes compared to conventional electrolytes make them more thermally stable, but they also have poor wetting with commercial separators. In a lithium‐ion battery, the electrolyte should completely wet out the separator and electrodes to reduce the cell internal resistance. Investigations of cell materials with IL electrolytes have shown that the wetting issues in IL–electrolyte cells are most likely due to poor separator compatibility, not electrode compatibility. A compatible separator must be developed before IL electrolytes can be used in commercial lithium‐ion batteries. Herein, separators for IL electrolytes, including commercial and novel separators, are reviewed. Separators with different processing methods, polymers, additives, and different IL electrolytes are considered. Collated, the separator studies show a strong correlation between ionic conductivity and membrane porosity, even more than the electrolyte type. The challenge of a suitable separator for IL electrolytes is not solved yet. Herein, it is revealed that a separator for IL electrolytes will most likely require a combination of high thermal and mechanical stability polymer, ceramic additives, and an optimized manufacturing process.

In recent years, the applications of lithium-ion batteries have emerged promptly owing to its widespread use in portable electronics and electric vehicles. Nevertheless, the safety of the battery systems has always been a global concern for the end-users. The separator is an indispensable part of lithium-ion batteries since it functions as a physical barrier for the electrode as well as an electrolyte reservoir for ionic transport. The properties of separators have direct influences on the performance of lithium-ion batteries, therefore the separators play an important role in the battery safety issue. With the rapid developments of applied materials, there have been extensive efforts to utilize these new materials as battery separators with enhanced electrical, fire, and explosion prevention performances. In this review, we aim to deliver an overview of recent advancements in numerical models on battery separators. Moreover, we summarize the physical properties of separators and benchmark selective key performance indicators. A broad picture of recent simulation studies on separators is given and a brief outlook for the future directions is also proposed.

… for a liquid electrolyte battery separator provided by the US Advanced Battery Consortium (… [36] patented a battery separator made of a blend of PE and PP. The separator was produced …

Optimizing the desired properties for stretch monolayer separators used in Lithium-ion batteries has been a challenge. In the present study a cellulose nanofiber/PET nonwoven composite separator is successfully fabricated, using a wet-laid nonwoven (papermaking) process, which can attain optimal properties in wettability, mechanical strength, thermal resistance, and electrochemical performance simultaneously. The PET nonwoven material, which is fabricated from ultrafine PET fibers by a wet-laid process, is a mechanical support layer. The porous structure of the composite separator was created by cellulose nanofibers coating the PET in a papermaking process. Cellulose nanofibers (CNFs), which are an eco-friendly sustainable resource, have been drawing considerable attention due to their astounding properties, such as: incredible specific surface area, thermal and chemical stability, high mechanical strength and hydrophilicity. The results show that the CNF separator exhibits higher porosity (70%) than a PP (polypropylene) separator (40%). The CNF separator can also be wetted by electrolyte in a few seconds while a PP separator cannot be entirely wetted after 1 min. The CNF separator has an electrolyte uptake of 250%, while a PP separator has only 65%. Another notable finding is that the CNF separator has almost no shrinkage when exposed to 180 °C for 1 h, whereas a PP separator shrinks by more than 50%. Differential Scanning Calorimetry (DSC) shows that the CNF separator has a higher melting point than a PP separator. These findings all indicate that the CNF 29 separator will be more favorable than stretch film for use in Lithium-ion batteries.

… demands and challenges on separators for lithium-ion batteries. A separator plays two main … the cathode and anode to maintain the safety of batteries and (2) providing a path for ionic …

… of lithium-ion battery separators plays an important role in separator performance; however, here we show that a geometrical analysis falls short in predicting the lithium-ion transport in …

… of battery separators play a crucial role in integrity of Lithium-ion batteries during an electric … In this study, four types of commonly used battery separators are characterized and their …

The recent advance of high-safety separators with high mechanical strength, high thermal stability and good lithium dendritic resistance is the main focus in this review. The future challenges and perspectives of separators are provided for building high safety rechargeable lithium batteries.

… Recently, much effort has been devoted to the development of battery separators for lithium-ion batteries for high-power, high-energy applications ranging from portable electronics to …

… of membrane separators for lithium-ion batteries are reviewed… battery separators for rechargeable lithium-ion batteries for … This paper introduces the requirements of battery separators …

… as lithium-ion battery separator via an … separator displayed better rate capability and enhanced capacity retention, when compared to those of commercialized polypropylene separator …

… -ion batteries. This review summarizes and discusses lithium-ion battery separators from a … development status of sodium-ion battery separators and the difference between lithium-ion …

… for battery separators from these materials. This review focused on battery separators and … -TrFE and PVDF-CTFE, for lithium-ion battery application due to the recent advances and …

… We provide the 3D microstructural data of a PE separator open source 14 to encourage future efforts in modeling lithium ion diffusion, heat conduction, or dendrite growth. We hope that …

… Besides the large quantity of LIBs separators provided by China, the quality of separators … Taking the wet process separator with 5 μm thickness as an example, the thinner separator …

The maximum energy that lithium-ion batteries can store decreases as they are used because of various irreversible degradation mechanisms. Many models of degradation have been …

Lithium-ion (Li-ion) batteries undergo complex electrochemical and mechanical degradation. This complexity is pronounced in applications such as electric vehicles, where highly demanding cycles of operation and varying environmental conditions lead to non-trivial interactions of ageing stress factors. This work presents the framework for an ageing diagnostic tool based on identifying and then tracking the evolution of model parameters of a fundamental electrochemistry-based battery model from non-invasive voltage/current cycling tests. In addition to understanding the underlying mechanisms for degradation, the optimisation algorithm developed in this work allows for rapid parametrisation of the pseudo-two dimensional (P2D), Doyle-Fuller-Newman, battery model. This is achieved through exploiting the embedded symbolic manipulation capabilities and global optimisation methods within MapleSim. Results are presented that highlight the significant reductions in the computational resources required for solving systems of coupled non-linear partial differential equations.

… to battery design and management. This study analyzes the electrochemical degradation … , linking these mechanisms to the evolution of battery safety. The findings reveal that during …

… aging and degradation are inevitable during the operational life cycle of lithium-ion batteries, … a significant challenge to battery performance and longevity. Despite the widespread use of …

The expansion of lithium-ion batteries from consumer electronics to larger-scale transport and energy storage applications has made understanding the many mechanisms responsible for battery degradation increasingly important. The literature in this complex topic has grown considerably; this perspective aims to distil current knowledge into a succinct form, as a reference and a guide to understanding battery degradation. Unlike other reviews, this work emphasises the coupling between the different mechanisms and the different physical and chemical approaches used to trigger, identify and monitor various mechanisms, as well as the various computational models that attempt to simulate these interactions. Degradation is separated into three levels: the actual mechanisms themselves, the observable consequences at cell level called modes and the operational effects such as capacity or power fade. Five principal and thirteen secondary mechanisms were found that are generally considered to be the cause of degradation during normal operation, which all give rise to five observable modes. A flowchart illustrates the different feedback loops that couple the various forms of degradation, whilst a table is presented to highlight the experimental conditions that are most likely to trigger specific degradation mechanisms. Together, they provide a powerful guide to designing experiments or models for investigating battery degradation.

… Lithium-ion batteries (LIBs) are increasingly popular for electric vehicle and grid storage applications, but degradation … of internal degradation in LIBs using an electrochemical model (…

Although Li-ion batteries have emerged as the battery of choice for electric-drive vehicles and large-scale smart grids, significant research efforts are devoted to identifying materials that offer higher energy density, longer cycle life, lower cost, and/or improved safety compared with conventional Li ion batteries based on intercalation electrodes. By moving beyond intercalation chemistry, gravimetric capacities that are two-to-five times higher than conventional intercalation materials (e.g., LiCoO2 and graphite) can be achieved. The transition to higher-capacity electrode materials in commercial applications is complicated by several factors. This Review highlights the developments of electrode materials and characterization tools for rechargeable lithium-ion batteries, with a focus on the structural and electrochemical degradation mechanisms that plague these systems.

Abstract The investigation of the aging and degradation mechanism of lithium ion batteries in automotive and energy storage applications is of particular importance for the acceptance of the battery technology. However, several factors interact to generate complicated battery aging phenomena, thus leading to limited accuracy of the established models when applied to degradation prediction under complex real running conditions. Here, a coupled electrochemical-thermal-mechanical model is presented for the degradation investigation of lithium-ion batteries. The model includes both side reactions on anode and the loss of active material of cathode and is employed to study the aging behavior of the battery applying different C-rates and ambient temperatures. Simulation results indicate that the aging of the battery is dominated by various aging factors under different operating conditions. Higher ambient temperature can accelerate SEI formation reaction, while low temperature can cause severe lithium-plating. Active material loss is affected by cycling current significantly and becomes the dominant aging factor under extremely high C-rate. The model is fitted under two accelerated aging cycles and agrees well with the experimental results.

… and electrochemical degradation mechanism … electrochemical degradation, respectively. For the first and the following cycles, the effect of the adsorbed species on the electrochemical …

… in the lithium-ion battery electrodes are predominant degradation mechanisms, which cause capacity fade and cell impedance rise. Physics-based degradation models reveal new …

… application to battery degradation and aging research. The capabilities and custom procedures to employ different electrochemical impedance techniques for battery degradation and …

Polytetrafluoroethylene (PTFE)-based dry process for lithium-ion batteries is gaining attention as a battery manufacturing scheme can be simplified with drastically reducing environmental damage. However, the electrochemical instability of PTFE in a reducing environment has hampered the realization of the high-performance dry-processed anode. In this study, we present a non-electroconductive and highly ionic-conductive polymer coating on graphite to mitigate the electrochemical degradation of the PTFE binder and minimize the coating resistance. Poly(ethylene oxide) (PEO) and poly(vinylidene fluoride-trifluoroethylene-chlorofluoroethylene) (P(VDF-TrFE-CFE)) coatings on the anode material effectively inhibit the electron transfer from graphite to PTFE, thereby alleviating the PTFE breakdown. The graphite polymer coatings improved initial Coulombic efficiencies of full cells from 67.2% (bare) to 79.1% (PEO) and 77.8% (P(VDF-TrFE-CFE)) and increased initial discharge capacity from 157.7 mAh g(NCM)-1 (bare) to 185.1 mAh g(NCM)-1 (PEO) and 182.5 mAh g(NCM)-1 (P(VDF-TrFE-CFE)) in the full cells. These outcomes demonstrate that PTFE degradation in the anode can be surmounted by adjusting the electron transfer to the PTFE.

Abstract The Lithium-ion batteries (LiBs) are the core component of the all-climate electric vehicles. The aging state recognition is carried out based on the proposed electrochemical model (EM) instead of the traditional equivalent circuit model (ECM) and black boxes model in this paper. Firstly, a group of mathematical equations are built to describe the physical and chemical behaviors of batteries based on the electrochemical theory. Then, the finite analysis method and the numerical computation method are used to solve the mathematical equations and the model has been built. Next, the optimization algorithm is used for identifying the parameters of the model. The aging state recognition of the battery on whole lifetime is carrying out based on the ageing data. Five aging characteristic parameters are determined to describe the health state of the battery, and their degradation trajectories are obtained. Finally, a battery-in-loop approach is employed to verify the model based degradation recognition. Results show that the maximum voltage error is within 50 mV and the state of health estimation error is bounded to 3%.

… The electrochemical stability of defective batteries induced by mechanical abuse raises … In this work, we systematically investigate the vibration-induced electrochemical degradation …

… It is therefore necessary first to study the electrochemical … , who studied the oxidative decomposition of PC at graphite,11 we … We can therefore conclude that electrolytic decomposition …

… , loss of usable capacity of the cell, and increase of cell impedance. Cell performance degradation due to side reactions is termed as chemical degradation, which is known to be the …

… Lithium-ion batteries are commonly maintained at low state-of-… Methodological analysis of capacity degradation mechanisms and … Beyond this threshold, pronounced loss of lithium-ion …

Abstract The demand for lithium-ion batteries (LIBs) with high mass-specific capacities, high rate capabilities and long-term cyclabilities is driving the research and development of LIBs with nickel-rich NMC (LiNi x Mn y Co 1− x − y O 2 , $$x \geqslant 0.5$$ x ⩾ 0.5 ) cathodes and graphite (Li x C 6 ) anodes. Based on this, this review will summarize recently reported and widely recognized studies of the degradation mechanisms of Ni-rich NMC cathodes and graphite anodes. And with a broad collection of proposed mechanisms on both atomic and micrometer scales, this review can supplement previous degradation studies of Ni-rich NMC batteries. In addition, this review will categorize advanced mitigation strategies for both electrodes based on different modifications in which Ni-rich NMC cathode improvement strategies involve dopants, gradient layers, surface coatings, carbon matrixes and advanced synthesis methods, whereas graphite anode improvement strategies involve surface coatings, charge/discharge protocols and electrolyte volume estimations. Electrolyte components that can facilitate the stabilization of anodic solid electrolyte interfaces are also reviewed, and trade-offs between modification techniques as well as controversies are discussed for a deeper understanding of the mitigation strategies of Ni-rich NMC/graphite LIBs. Furthermore, this review will present various physical and electrochemical diagnostic tools that are vital in the elucidation of degradation mechanisms during operation to supplement future degradation studies. Finally, this review will summarize current research focuses and propose future research directions. Graphic Abstract The demand for lithium-ion batteries (LIBs) with high mass specific capacities, high rate capabilities and longterm cyclabilities is driving the research and development of LIBs with nickel-rich NMC (LiNi x Mn y Co 1− x − y O 2 , x  ≥ 0.5) cathodes and graphite (Li x C 6 ) anodes. Based on this, this review will summarize recently reported and widely recognized studies of the degradation mechanisms of Ni-rich NMC cathodes and graphite anodes. And with a broad collection of proposed mechanisms on both atomic and micrometer scales, this review can supplement previous degradation studies of Ni-rich NMC batteries. In addition, this review will categorize advanced mitigation strategies for both electrodes based on different modifications in which Ni-rich NMC cathode improvement strategies involve dopants, gradient layers, surface coatings, carbon matrixes and advanced synthesis methods, whereas graphite anode improvement strategies involve surface coatings, charge/discharge protocols and electrolyte volume estimations. Electrolyte components that can facilitate the stabilization of anodic solid-electrolyte interfaces (SEIs) are also reviewed and tradeoffs between modification techniques as well as controversies are discussed for a deeper understanding of the mitigation strategies of Ni-rich NMC/graphite LIBs. Furthermore, this review will present various physical and electrochemical diagnostic tools that are vital in the elucidation of degradation mechanisms during operation to supplement future degradation studies. Finally, this review will summarize current research focuses and propose future research directions.

… lithium-ion button cells that show linear behavior from 20 to 100% DOD [8]. In summary, the data from lithium-ion battery manufacturers indicates that lithium-ion cells with a cycle life of …

… Objectives of this study were to clear the abovementioned ambiguity and to determine the mechanism of the capacity fade of Sony lithium-ion batteries during continuous cycling. Using …

… processes explicitly in their mathematical description of battery behavior. The objective of … the mechanisms of capacity fade in lithiumion batteries. Advances in modeling lithium-ion cells …

… Our study shows that there could be multiple stages in the capacity fade of the cell. In this section, the scenarios behind those stages for cell capacity fade are presented. …

Abstract Lithium-ion batteries are extensively used in electric vehicles, however, their significant degradation over discharge and charge cycles results in severe capacity fade, limiting driving ranges of electric vehicles over time and useful lifetime of batteries. In this study, capacity fade for lithium-ion battery has been investigated through modeling and experiment. A predictive model is developed based on first principles incorporating degradation mechanisms. The mechanisms of degradation considered include solid-electrolyte interface (SEI) growth and active material loss at both negative and positive electrodes. Battery performance including capacity is measured experimentally under discharge and charge cycling with battery operation temperature controlled. It is shown that battery capacity is reduced over battery discharge/charge cycling at a given battery operation temperature, and the model predicted battery performance, including capacity fade, agrees well with the experimental results. As the number of discharge/charge cycles are increased, battery capacity is reduced significantly; battery capacity fade is increased substantially when battery operation temperature is increased, indicating significantly accelerated aging of the battery at elevated operation temperatures and hence the importance of battery thermal management in the control of battery operation temperature for practical applications such as electric vehicles. Battery capacity fade is mainly caused by SEI film growth at the negative electrode, which is the largest contributing factor to the capacity fade, and the active material isolation at the negative electrode, which is the second largest influencing aging factor.

… technology to predict capacity fading of lithium-ion cells using the analysis of their discharge curves. A cell capacity is deduced from the cell voltage window and the cell discharge curve…

… using a simple charge/discharge model of a Sony 18650 lithium ion battery. Loss of capacity and … using cycling data from an experimental cell with over 1600 charge–discharge cycles. …

… In this paper, a dynamic model of lithium-ion battery considering the significant temperature and capacity fading effects is proposed. The simulation results shows that the developed …

… The obtained values suggest that the capacity fade of the Li-ion battery due to … capacity. These results suggest the validity of the equivalent circuit to interpret the causes of capacity fade. …

… improve the predictive capability of battery models but also help to elucidate the mechanism of capacity fade. In this paper, capacity fade of Sony US 18650 lithium-ion batteries cycled …

… capacity fading behavior of large format lithium-ion batteries with Li y Ni 1/3 Co 1/3 Mn 1/3 O 2 + Li y Mn 2 O 4 composite cathode. The capacity … and incremental capacity analysis (ICA). …

Abstract Forecasting the lifetime of Li-ion batteries is a critical challenge that limits the integration of battery electric vehicles (BEVs) into the automotive market. Cycle-life performance of Li-ion batteries is intrinsically linked to the fundamental understanding of ageing mechanisms. In contrast to most previous studies which utilise empirical trends (low real-time information) or rough simplifications on mathematical models to predict the lifetime of a Li-ion battery, we deployed a novel ageing formulation that includes heterogeneous dual-layer solid electrolyte interphase (SEI) and lithium-plating ageing mechanisms with porosity evaluation. The proposed model is parameterized and optimized for mass transport and ageing parameters based on fresh and an aged cell and validated against our experimental results. We show that our advanced ageing mechanisms can accurately calculate experimentally observed cell voltage and capacity fade with respect to cycling number and can predict future fade for new operating scenarios based on constant-current and a dynamic power profile cycling experimental data consisting of high discharge C-rates and fast-charging periods. Our model is able to capture the linear and nonlinear (knee-point) capacity fade characteristics with a high accuracy of 98% goodness-of-fit-error and we compared our model performance with well-accepted existing model in literature.

Lithium ion cells, when cycled, exhibit a two‐stage degradation behavior characterized by a first linear stage and a second nonlinear stage where degradation is rapid. The multitude of degradation phenomena occurring in lithium ion batteries complicates the understanding of this two‐stage degradation behavior. In this work, a simple and intuitive model is presented to analyze the coupled effect of resistance growth and the shape of the state of charge (SOC)‐open circuit voltage (OCV) relationship in representing the complete degradation behavior. The model simulations demonstrate that a single resistance that increases linearly on cycling can capture the transition from slow to fast degradation, primarily due to the shape of the SOC‐OCV curve. Further, the model simulations indicate that the shape of the degradation curve depends strongly on the magnitude of current at the end of discharge of the cycling protocol. To verify these observations, specific experiments are designed with minimal capacity loss but with shrinking operating voltage ranges that result in shrinking operating OCV range. The results of the experiments validate the observations of model simulations. Further, long‐term cycling experiment with a commercial lithium ion cell shows that the operating OCV range shrinks substantially with aging and is a major reason for the observed accelerated degradation. The analysis of the present work provides significant insights towards developing simple semiempirical models suitable for battery life management in microcontrollers.

In this study, aging mechanisms and state of health prediction of lithium-ion battery in total lifespan are investigated. Battery capacity fading can be divided into three stages: stable …

… lithium-ion battery model is presented in this paper to study the capacity fade under cyclic charge-… responsible for the capacity fade and power fade. The temperature variation inside the …

… This indicates that the capacity fade during … lithium-ion loss by SEI formation on the anode 25 seem to be overlaid on the degradation of the positive electrode in the total capacity fade. …

… The next sections describe the lithium-ion battery model used in this study, the numerical algorithms used to implement the discrete approach to capacity fade prediction, the results and …

… the cycling performance and power fade mechanism of various battery chemistries during … the cell capacity [8]. Part of our goal is to elucidate differences in the capacity and power fade …

… of the power and capacity fade resulting from the cycle-life testing using PNGV (now referred to as FreedomCAR) test protocols at 25 and 45 C of 18650-size Li-ion batteries developed …

… A one dimensional model incorporating solvent diffusion and kinetics of solid electrolyte interphase (SEI) formation is developed to study capacity fade in lithium ion batteries. The …