Lithium-ion Batteries Research Articles

Study on the thermal runaway behavior and mechanism of 18650 lithium-ion battery induced by external short circuit

This study investigated the external short circuit (ESC) characteristics of 18650-type NCM lithium-ion batteries under different states of charge (SOC) and short-circuit currents. The research includes the macroscopic electro-thermal characteristics, microscopic morphology, structural damage, and internal damage evolution mechanism of short-circuited batteries. The tests provided an in-depth study of external short circuit (ESC) failure and thermal runaway (TR) behavioral characteristics. The results indicate that all the temperature changes of the short-circuit batteries were found to be in an upward and then downward trend. The surface temperature rise rate of batteries with low SOC were faster, and the maximum surface temperature rise of batteries with high SOC were higher. And with the increase of short-circuit current rate, the temperature rise gradually increased. In particular, thermal runaway occurred at 25C and the maximum temperature exceeds 500 °C. Different SOC batteries showed different degree of voltage fluctuation. The voltage curve of low SOC batteries showed “falling-rising-falling” trend with a brief platform. High SOC batteries formed a distinct voltage platform near 2.75 V. As the short-circuit current increased, the voltage platform shortened, followed by the rapid drop to zero. X-ray CT and SEM test results showed that the deformation of the battery jelly roll was mainly due to the separator shrinkage and tearing. Major changes occurred in the cathode and separator, including secondary particle rupture and irreversible pore blockage in the separator. The damage mechanism of ESC and its evolution are revealed. The results of this study can provide support for the research work on the thermal safety design of lithium batteries.

A 500 kW hydrogen fuel cell-powered vessel: From concept to sailing

This paper presents the “Three Gorges Hydrogen Boat No. 1”, a novel green hydrogen-powered vessel that has been successfully delivered and is currently sailing. This vessel, integrated with a hydrogen production and bunkering station at its dedicated dock, achieves zero-carbon emissions. It stores 240 kg of 35 MPa gaseous hydrogen and has a fuel cell system rated at 500 kW. We analysed the engineering details of the marine hydrogen system, including hydrogen bunkering, storage, supply, fuel cell, and the hybrid power system with lithium-ion batteries. In the first bunkering trial, the vessel was safely refuelled with 200 kg of gaseous hydrogen in 156 min via a bunkering station 13 m above the water surface. The maximum hydrogen pressure and temperature recorded during bunkering were 35.05 MPa and 39.04 °C, respectively, demonstrating safe and reliable shore-to-ship bunkering. For the sea trial, the marine hydrogen system operated successfully during a 3-h voyage, achieving a maximum speed of 28.15 km/h (15.2 knots) at rated propulsion power. The vessel exhibited minimal noise and vibration, and its dynamic response met load change requirements. To prevent rapid load changes to the fuel cells, 68 s were used to reach 483 kW from startup, and 62 s from 480 kW to zero. The successful bunkering and operation of this hydrogen-powered vessel demonstrates the feasibility of zero-carbon emission maritime transport. However, four lessons were identified concerning bunkering speed, hydrogen cylinder leakage, hydrogen pressure regulator malfunctions, and fuel cell room space. The novelty of this work lies in the practical demonstration of a fully operational, hydrogen-powered maritime vessel achieving zero emissions, encompassing its design, building, operation, and lessons learned. These parameters and findings can be used as a baseline for further engineering research.

On the moisture tolerance of LiFSI based lithium-ion batteries: A systematic study on NMC622/graphite full cells

Lithium-ion battery (LIB) technology is state-of-the-art energy storage technology for portable electronics and electric vehicles (EVs). In this incumbent LIB technology, lithium hexafluorophosphate (LiPF6) is the most widely used electrolyte salt to date. However, the challenges related to its chemical/thermal stability, sensitivity to moisture and the consequent formation of strong acids such as hydrogen fluoride (HF) need to be resolved with alternative salts. Due to its better chemical/thermal stability, resistance to moisture and HF formation, and better ionic conductivity, lithium bis(fluorosulfonyl)imide (LiFSI) has been considered as a promising alternative electrolyte salt to LiPF6. In this study, the effect of addition of 1000 ppm water on LiFSI based electrolytes was systematically investigated by testing NMC622/lithium and artificial graphite/lithium half and NMC622/graphite full cells in four LiFSI based electrolytes; plain LiFSI, LiFSI + 1000 ppm H2O, LiFSI + 10 wt% FEC, and LiFSI + 1000 ppm H2O + 10 wt% FEC. Post mortem characterization of selected electrodes was also conducted with SEM imaging and XPS to study the surface chemistry and morphology of cycled electrodes. Overall, this study shows that 1000 ppm water can slightly improve the electrochemical performance of NMC622/lithium half cells; however, the same amount of moisture severly degrades the graphite half and NMC622/graphite full cells.

GenAI for Scientific Discovery in Electrochemical Energy Storage: State-of-the-Art and Perspectives from Nano- and Micro-Scale.

The transition to electric vehicles (EVs) and the increased reliance on renewable energy sources necessitate significant advancements in electrochemical energy storage systems. Fuel cells, lithium-ion batteries, and flow batteries play a key role in enhancing the efficiency and sustainability of energy usage in transportation and storage. Despite their potential, these technologies face limitations such as high costs, material scarcity, and efficiency challenges. This research introduces a novel integration of Generative AI (GenAI) within electrochemical energy storage systems to address these issues. By leveraging advanced GenAI techniques like Generative Adversarial Networks, autoencoders, diffusion and flow-based models, and multimodal large language models, this paper demonstrates significant improvements in material discovery, battery design, performance prediction, and lifecycle management across different types of electrochemical storage systems. The research further emphasizes the importance of nano- and micro-scale interactions, providing detailed insights into optimizing these interactions for improved efficiency and longevity. Additionally, the paper discusses the challenges and future directions for integrating GenAI in energy storage research, highlighting the importance of data quality, model transparency, workflow integration, scalability, and ethical considerations. By addressing these aspects, this research sets a new benchmark for the use of GenAI in battery development, promoting sustainable, efficient, and safer energy solutions.

Coaxial Nanofiber Binders Integrating Thin and Robust Sulfide Solid Electrolytes for High‐Performance All‐Solid‐State Lithium Battery

AbstractTo access the theoretically high energy density of sulfide‐based all‐solid‐state lithium batteries (ASSLBs), a thin and robust sulfide electrolyte membrane is essential. Given the pivotal role of binder in preserving the structural integrity and interfacial stability of sulfide electrolytes upon cycling, it is desired to integrate binding capability, toughness, and stiffness into one binder, yet remains difficult. Herein, this challenge is addressed using a nanofiber‐reinforced strategy in the solvent‐free dry‐film process. A coaxial polyvinylidene poly(vinylidene fluoride‐co‐hexafluoropropylene) @ thermoplastic polyurethane (PVDF‐HFP@TPU) nanofiber binder is embedding into a Li6PS5Cl (LPSCl) matrix to obtain a sulfide thin‐layer (LPSCl‐P@T). During hot calendering of the sulfide‐binder mixture, the PVDF‐HFP shell layer melts and tightly binds LPSCl particles. The underlying TPU core layer, which maintains the fibrous structure, reinforces the structural stability of the membrane. Particularly, the fiber‐matrix connection is improved with the assistance of the molten PVDF‐HFP, collectively contributing to the effective dissipation of the mechanical stress. Controlled fusion of the core‐shell nanofiber also leads to enhanced interfacial anchoring of the cathode and electrolyte. The assembled cells with LPSCl‐P@T deliver stable cycling performances. The PVDF‐HFP@TPU nanofiber binder overcomes the long‐existing incompatible problems between binder toughness and stiffness, and shows promises in developing high‐performance sulfide‐based ASSLBs.

Application of DBN-based KRLS method for RUL prediction of lithium-ion batteries

The Remaining Useful Life (RUL) of lithium batteries is vital for maintaining and safely operating the batteries, making precise RUL predictions highly significant. This paper introduces a method for predicting the RUL of lithium-ion batteries, utilizing a kernel adaptive filtering algorithm integrated with Deep Belief Networks (DBN). The method constructs a novel prediction model based on the Fixed-Budget Kernel Recursive Least Squares (FB-KRLS) algorithm. In this approach, the DBN extracts features from the original lithium battery data to reduce data complexity. The Square-root Cubature Kalman Filter (SCKF) is integrated with the FB-KRLS algorithm, employing a dual al-ternating learning strategy to improve the model's nonlinear fitting performance. The model was validated using NASA's lithium battery data, showing that the minimum val-ues for the MAPE, RMSE and MAE were 0.102%, 0.0016 and 0.0014, respectively. Therefore, the proposed method demonstrates potential for application in predicting the RUL of lithium-ion batteries.

Lithium ion transportation in lignin infused polyvinyl alcohol based eutectogel: A molecular dynamics framework

Eutectogels are an arising material in the field of energy storage applications like high-energy Lithium-Ion batteries (LIBs) due to their properties like higher ionic conductivity, environment friendly and enhanced safety. However, it is important to understand the working mechanism of eutectogels at an atomistic level with the help of Molecular Dynamics (MD) simulations, in order to enhance their performance as electrolytes for LIBs. Eutectogels are formed by integrating deep eutectic solvent (DES) involving Lithium Chloride (LiCl) and ethylene glycol (EG) in the molar ratio of 1:5 with the polymeric matrix of Polyvinyl alcohol (PVA) chains considered for this study. Thereafter, lignin molecules are induced in the eutectogel system to improve the characteristics of an eutectogel. The elaborate study of the effect of lignin on the lithium ions movement through the lignin-added-eutectogel is involved in this work. The increase in hydrogen bonds among PVA polymeric chains and lignin molecules show the strength enhancement. From the Radial Distribution Function results it is derived that the lithium ions are showing enhanced interactions with chlorine ions than any other component of the system. Mean Square Displacement gives an idea about diffusivity of lithium ions through the systems and it suggests that the Li+ ion diffusivity is improved after Lignin imposition. On the basis of findings from this work, the modified Lignin infused PVA based eutectogel can be the potential candidate for the battery and energy storage applications.

A liquid-cooled plate based on bionic flow channels evolved from the shape of leaf veins and tree roots

With the rapid development of lithium-ion (Li-ion) batteries, battery thermal management (BTMS) is increasingly essential for the temperature control of Li-ion batteries. The energy required to control temperature is coming into focus. In order to consume less energy to control temperature and improve temperature uniformity, the liquid-cooled plate (LCP) based on bionic flow channels evolved from the shape of leaf veins and tree roots is proposed. In this BLCP, different from the others BLCPs, it is divided into a reinforced heat exchange area located in the middle and back part of the plate and a normal area located in the front part of the plate. Firstly, 16 sets of orthogonal tests are conducted based on four parameters: the distance of the hexagon from the outlet (a), the distance from the inlet (b), the distance between two adjacent hexagons (c) and the size of the hexagon (d). Secondly, Optimization was investigated based on NSGA-II for two objectives: temperature and pressure drop. The simulation results are analyzed based on the optimized structural parameters (a = 30 mm, b = 8 mm, c = 50 mm and d = 90 mm). After Comparing the optimization results with the simulation results, the temperature and pressure drop errors were 0.56 percent and 3.8 percent, respectively. The effects of flow rate and thickness of the fluid domain on temperature and pressure drop are next discussed separately. Finally, after comparing the optimized bionic liquid cooling plate (BLCP) with the conventional liquid cooling plate (CLCP) based on temperature pressure drop, velocity, and synergy angle, conclusions are made at the same inlet width, height, flow rate, and velocity (V = 0.2 m/s). This leads to the criterion of energy loss becoming only the pressure drop. The BLCP for pressure drop is 14.2 percent lower than the CLCP, which means less energy loss. The maximum temperature of the BLCP is 0.7 °C lower than that of the CLCP. Furthermore, the former has a better ability to suppress the rate of temperature rise and better temperature uniformity. In addition, this proposed new structure and research methods can be applied to the subsequent study of LCP.

Evaluating Fire and Smoke Risks with Lithium-Ion Cells, Modules, and Batteries

Evaluating Fire and Smoke Risks with Lithium-Ion Cells, Modules, and Batteries

Modelling of a Cylindrical Battery Mechanical Behavior under Compression Load

The extensive utilization of lithium-ion (Li-ion) batteries within the automotive industry necessitates rigorous measures to ensure their mechanical robustness, crucial for averting thermal runaway incidents and ensuring vehicle safety. This paper introduces an innovative methodology aimed at homogenizing the mechanical response of Li-ion batteries under compression load, using Finite Element Method (FEM) techniques to improve computational efficiency. A novel approach is proposed, involving the selective application of compression loads solely to the Jelly Roll and its casing, achieved by cutting the battery heads. Through this method, distinct mechanical behaviors are identified within the battery force displacement curve: an elastic region, a zone characterized by plastic deformation, and a segment exhibiting densification. By delineating these regions, our study facilitates a comprehensive understanding of the battery’s mechanical response under compression. Two battery models were employed in this study: one representing the battery as a solid volume, and another featuring the jelly roll as a solid volume enclosed by a shell representing the casing. The material utilized was LS Dyna MAT24, chosen for its piecewise characteristics’ definition, and its validation was primarily conducted through the curve fitting method applied to the force–displacement curve, taking in account the three regions of the compression force behavior. This approach not only optimizes computational resources but also offers insights crucial for enhancing the mechanical stability of Li-ion batteries in automotive applications.

Microsphere LiMn0.6Fe0.4PO4/C cathode with unique rod-like secondary architecture for high energy lithium ion batteries

LiMnxFe1-xPO4/C is considered a promising next-generation cathode material with significant commercial potential, inheriting the safety of LiFePO4 while offering higher energy densities. However, the extremely low conductivity and the Jahn-Teller effect induced by Mn3+ limit its practical capacity and rate performance. Effective modifications can be achieved through particle nanonization and uniform carbon coating. Here, we synthesized microspherical LiMn0.6Fe0.4PO4/C cathode materials using a hydrothermal method combined with spray drying carbon coating. The cathode material exhibits a microsphere structure composed of aggregated nanorods with a uniform 3 nm carbon coating, showing good dispersibility, small specific surface area and high tap density. In-situ diffraction analysis showed that expanding the single-phase solid solution region during (de)lithiation can reduce the energy barrier for electron transport, improve the kinetics of the (dis)charge process, and enhance both cycling and rate performance. The initial capacity at 0.1C can reach 155 mAh/g, and the capacity remains at 133.5 mAh/g with a retention rate of 97.1 % after 300 cycles. The synergistic effect of particle nanonization and uniform carbon coating endows the LiMnxFe1-xPO4/C material with excellent electrochemical performance.

MXene Electrodes for All Strain-Free Solid-State Batteries.

All-solid-state batteries with nonflammable inorganic solid electrolytes are the key to addressing the safety issues of lithium-ion batteries with flammable organic liquid electrolytes. However, conventional electrode materials suffer from substantial volume changes during Li+ (de)intercalation, leading to mechanical failure of interfaces between electrode materials and solid electrolytes and then severe performance degradation. In this study, we report strain-free charge storage via the interfaces between transition metal carbides (MXenes) and solid electrolytes, where MXene shows negligible structural changes during Li+ (de)intercalation. Operando scanning electron transmission microscopy with electron energy-loss spectroscopy reveals the pillar effect of trapped Li+ in the interlayer spaces of MXene to achieve the strain-free features. An all strain-free solid-state battery, which consists of a strain-free Ti3C2Tx negative electrode and a strain-free disordered rocksalt Li8/7Ti2/7V4/7O2 positive electrode, demonstrates long-term stable operation while preserving the interfacial contact between electrode materials and solid electrolytes.

Direct regeneration of LiFePO4 cathode by inherent impurities in spent lithium-ion batteries

The direct regeneration method, recognized for its cost-effectiveness, has garnered considerable attentions in the field of battery recycling. In this study, a novel direct regeneration strategy is proposed to repair spent LiFePO4 (S-LFP) cathodes without the need for impurity removal. Instead, the residual conductive carbon and polyvinylidene fluoride (PVDF) in S-LFP are employed as inherent reductive agents. Systematic characterization and analysis reveal that the failure of S-LFP primarily originates from a substantial loss of Li+ and the conversion of LiFePO4 to FePO4. Meanwhile, it is demonstrated that both residual conductive carbon and PVDF play positive roles in promoting the regeneration of S-LFP through distinct mechanisms. As a result, the regenerated LFP exhibits significant recovery in crystal structure and chemical composition as compared to S-LFP, which leads to notably improved lithium storage performance. Furthermore, to further enhance the lithium storage property, a specific amount of glucose (10 %) is introduced during the regeneration of S-LFP, yielding a regenerated product that performs comparably to commercial LFP. Clearly, our approach, in contrast to traditional regeneration methods, maximizes the utilization of residual impurities within S-LFP, resulting in effective regeneration of S-LFP, thereby proving both informative and cost-effective.

Application of precursor with ultra-small particle size and uniform particle distribution for ultra-high nickel single-crystal cathode materials by coprecipitation method

Ultra-high nickel single-crystal cathode materials have become the most promising for lithium-ion batteries. However, the preparation of ultra-high nickel single-crystal precursors by a continuous coprecipitation method has the disadvantages of large particle size, wide distribution, poor morphology. The extent of the inhomogeneous reactions can be more severe in single-crystal cathodes with larger particle size. Herein, the coprecipitation method with a solid concentrator was adopted, and citrate sodium was used as a complexing agent to improve the physical properties of precursors and electrochemical performance of single-crystal cathode materials. By analyzing the morphology and agglomeration mechanism of the precursor nucleuses under different pH values, it was found that hexagonal nanosheets grew along the 101 direction, and the primary particles showed thicker at pH of 11.4. The hexagonal nanosheets grew along the 001 direction, and the primary particles showed finer at pH of 12.2. The morphology and particle size uniformity of the secondary particles formed by agglomeration at these two pH values showed poor. However, hexagonal nanosheets grew synergistically along the 001 and 101 directions at pH of 11.8, so the primary particles with uniform particle size gradually agglomerated, and then the secondary particles with ultra-small particle size and uniform distribution obtained. Compared to materials prepared by the traditional continuous coprecipitation method, the precursor displays a smaller particle size(D50 = 1.8 µm), higher sphericity, uniformity and denser internal structure. In order to evaluate the performance of Ni0.94Co0.04Mn0.02(OH)2 with ultra-small particle size, the sintering conditions of LiNi0.94Co0.04Mn0.02O2 need to be explored. It was found that the LiNi0.94Co0.04Mn0.02O2 cathode material prepared at 790 °C exhibited higher discharge capacity, cycle and rate performance, compared to materials prepared at 760 °C and 820 °C. We further utilized TEM, EPMA, and XPS to test the internal structure and valence state of LiNi0.94Co0.04Mn0.02O2 cathode material. The results show that the LiNi0.94Co0.04Mn0.02O2 calcined at 790 °C has a good single crystal structure. The LiNi0.94Co0.04Mn0.02O2 cathode materials inherited the structure and particle size of Ni0.94Co0.04Mn0.02(OH)2 precursors, and displayed discharge capacity of 194.7 mAh/g and capacity retention rate of 89.8 % after 100 cycles at 1 C. The microstructure and phase transition of the as-prepared cathode material are well-maintained after long-term cycling, without obvious inter-crystalline micro-crack. The results indicate that its electrochemical performance is better than that of cathode materials with precursors prepared by a continuous coprecipitation method. This work provides new insights for the preparation of small-particle-size precursor and single-crystal cathode materials.

Thermal Runaway Diagnosis of Lithium-Ion Cells Using Data-Driven Method

Fault diagnosis is crucial to guarantee safe operation and extend the operating time while preventing the thermal runaway of the lithium-ion battery. This study presents a data-driven thermal runaway diagnosis framework where Bayesian optimization techniques are applied to optimize the hyperparameter of various machine learning techniques. We use different machine learning models such as support vector machine, naive Bayes, decision tree ensemble, and multi-layer perceptron to estimate a high likelihood of causes of thermal runaway by using the experimental measurements of open-source battery failure data. We analyze different evaluation metrics, including the prediction accuracy, confusion metrics, and receiver operating characteristic curves of different models. An experimental evaluation shows that the classification accuracy of the decision tree ensemble outperforms that of other models. Furthermore, the decision tree ensemble provides robust prediction accuracy even with the strictly limited dataset.

Cocross-Linked Nanofibrous Separator with High Ion Transport Capacity for Lithium-Ion Batteries

Cocross-Linked Nanofibrous Separator with High Ion Transport Capacity for Lithium-Ion Batteries

Direct recycling of anode active material from Li-ion batteries using TiNb2O7 anode

As the demand for large lithium-ion batteries (LIBs) for automotive and other applications rapidly grows, recycling of electrode materials has become essential owing to the large amount of waste material generated by battery manufacturing (e.g., battery scrap) and end-of-life (EOL) batteries. While there have been many studies on recycling of cathode materials, we propose a direct recycling process for anode material using TiNb2O7 (TNO) as the active material, as it offers high capacity and long life. Calcination was introduced to separate the anode active material from the current-collecting foil, and a regeneration method was investigated for TNO anodes from scrap and EOL battery waste. After calcination, the active material can be easily separated from the aluminum current-collecting foil owing to the binder disappearing. The structure of the active material was investigated using X-ray diffraction and scanning electron microscopy. TNO active material recycled from scrap and EOL was found to maintain the structure of virgin material. A cell was fabricated using recycled TNO and cell performance was evaluated. The cell capacity and rate capacity were found to be almost equivalent to those of virgin material. In terms of the carbon footprints of products (CFP), CO2 emissions during the recycling process were compared between recycled material and virgin material, and it was found that CO2 emissions were reduced to 0.7-CO2eq/kg for scrap material and 3.8-CO2eq/kg for EOL waste material, compared with 4.8-CO2eq/kg for virgin material. Thus, the feasibility of low CO2 emissions during TNO anode direct recycling was confirmed in principle. A simple and low CO2 emission recycling loop can thus be constructed by employing a stable TNO active material structure and direct-recycling process with calcination.

Enhancing the Reaction Kinetics and Stability of Co-Free Li-Rich Cathode Materials via a Multifunctional Strategy.

Co-free Li-rich layered oxides (CFLLOs) with anionic redox activity are among the most promising cathode materials for high-energy-density and low-cost lithium-ion batteries (LIBs). However, irreversible oxygen release often causes severe structural deterioration, electrolyte decomposition, and the formation of unstable cathode-electrolyte interface (CEI) film with high impedance. Additionally, the elimination of cobalt elements further deteriorates the reaction kinetics, leading to reduced capacity and poor rate performance. Here, a multifunctional strategy is proposed, incorporating Li2MnO3 phase content regulation, micro-nano structure design, and heteroatom substitution. The increased content of Li2MnO3 phase enhances the capacity through oxygen redox. The smaller nanoscale primary particles induce greater tensile strain and introduce more grain boundaries, thereby improving the reaction kinetics and reactivity, while the larger micron-sized secondary particles help to reduce interfacial side reactions. Furthermore, Na⁺ doping modulates the local coordination environment of oxygen, stabilizing both the anion framework and the crystal structure. As a result, the designed cathode exhibits enhanced rate performance, delivering a capacity of 158 mAh g⁻¹ at 5.0 C and improved cyclic stability, with a high capacity retention of 99% after 400 cycles at 1.0 C. This multifunctional strategy holds great promise for advancing the practical application of CFLLOs in next-generation LIBs.

Remaining useful life prediction of high-capacity lithium-ion batteries based on incremental capacity analysis and Gaussian kernel function optimization

Remaining useful life (RUL) is a key indicator for assessing the health status of lithium (Li)-ion batteries, and realizing accurate and reliable RUL prediction is crucial for the proper operation of battery systems. As high-capacity Li batteries have more complex chemical properties, most of the current RUL prediction methods rely mainly on a priori knowledge to make judgments. As a result, prediction accuracy is not high. In this study, we developed a health indicator-capacity (HI-C) dual Gaussian process regression (GPR) model based on incremental capacity analysis (ICA) and optimized its kernel function to achieve accurate RUL prediction for 280 Ah high-capacity Li batteries. Validation against the United States National Aeronautics and Space Administration’s four battery test datasets showed that the use of the HI-C dual GPR model resulted in a mean absolute percentage error and root mean square error of less than 0.02 and 0.04, respectively, for the four battery-rated capacity predictions. Additionally, this model achieved an absolute error of less than five battery failure turns. Compared with a single model, the HI-C dual GPR model not only had high accuracy but also solved the problem that the HI was not measurable in the actual battery operation, which made it more suitable for RUL prediction of Li batteries.

Multidimensional, Superflexible, and Binder-free CNT-rGO/Si Buckypaper as Anodes for Lithium-Ion Batteries and Electrochemical Performance

Multidimensional, Superflexible, and Binder-free CNT-rGO/Si Buckypaper as Anodes for Lithium-Ion Batteries and Electrochemical Performance