LFP Cathode Research Articles

Enhanced graphitization of CO2-derived carbon anodes via Joule heating reformation for high-performance lithium-ion batteries

Molten salt electrolysis of CO2 represents a promising technology for highly efficient CO2 capture and the production of economically valuable CO2-derived carbon materials. In this study, we established a 100-A-scale molten salt CO2 electrolysis cell to synthesize hundreds of grams of CO2-derived carbon. Subsequent Joule heating at 2800 °C transformed these materials into high-quality graphite. Further composite modification with asphalt and petroleum coke effectively reduced surface area, resulting in high-performance graphite for lithium-ion battery. The CO2-derived graphite anodes demonstrated high reversible capacities ranging from 297.7 to 378.1 mAh g−1, exhibiting outstanding rate capability and stability over 300 charge-discharge cycles at a current density of 1 A g−1. Finally, we assembled a coin full-cell using AG-2/2/6 anode and LFP cathode, which demonstrated good cycling performance. XPS analysis revealed a significant reduction in oxygen content by the post-reformation, facilitating the formation of highly graphitized structures. This study not only pioneers the up-class synthesis of CO2-derived carbon but also underscores its potential for sustainable energy applications, particularly in lithium-ion battery technology.

Improvement of LiFePO4 electrochemical performance by organic zinc source doping in combination with crystalline carbon layer capping

In this paper, LiFePO4 cathode materials are prepared by hydrothermal method and co-modified using the synergistic effect of doping and capping. We investigate the effects of Zn[Formula: see text] doping and DPHP capping layer on the crystalline, microstructure, and electrochemical properties of LFP cathode materials, and the results indicate that the discharge capacity of the co-modified cathode material with 5% Zn[Formula: see text] doped and 7% DPHP capping layer is 162.1 mAh ⋅ g[Formula: see text], and the rate of capacity retention is still as high as 98.5% after 200 times of discharging and charging.

Catalytic Strategies Enabled Rapid Formation of Homogeneous and Mechanically Robust Inorganic‐Rich Cathode Electrolyte Interface for High‐Rate and High‐Stability Lithium‐Ion Batteries

AbstractLithium iron phosphate (LFP) cathode is renowned for high thermal stability and safety, making them a popular choice for lithium‐ion batteries. Nevertheless, on one hand, the fast charge/discharge capability is fundamentally constrained by low electrical conductivity and anisotropic nature of sluggish lithium ion (Li+) diffusion. On the other hand, the interface and internal structural degradation occurs when subjected to high‐rate condition. Herein, a multifunctional boron‐doping graphene/lithium carbonate (BG/LCO) nanointerfacial layer on surface of commercial LiFePO4 particles is designed, in which the BG layer catalyzes the rapid reaction of Li2CO3‐LiPF6 for homogeneous and mechanically robust inorganic LiF‐rich structure across the cathode‐electrolyte interphase (CEI), forms a conductive network to significantly enhance both electron and Li+ transport, and strengthens the FeO bonding to minimize both Fe loss and the formation of Fe‐Li antisite defects. Correspondingly, the modified LFP cathode achieves a high capability of 113.2 mAh g−1 at 10 C and extraordinary cyclic stability with 88.0% capacity retention over 1000 cycles as compared to the pristine LFP cathode with a capacity of only 94.0 mAh g−1 and 64.6% capacity retention. It also exhibits great enhancements of 20.1% and 3.7% at higher‐rate condition (room temperature/15 C) and the low temperature condition (−10 °C/1 C), respectively.

Synergistic enhancement of lithium iron phosphate electrochemical performance by organic zinc source doping and crystalline carbon layer capping

In this study, lithium iron phosphate (LFP) is prepared as cathode material by hydrothermal synthesis method and the combined effect of doping and capping is applied to co-modify it. We thoroughly investigate how Zn2+ doping and PA capping layer affect the crystal structure, microscopic morphology, and electrochemical properties of LFP cathode materials. The experimental results show that when co-modified with 5 % Zn2+ doping combined with 7 % PA capping layer, the resulting cathode material exhibits a discharge specific capacity of 165.5 mAh g−1, and the capacity retention rate can still be maintained at a high level of 98.6 % after 200 charge–discharge cycles.

Electrochemical Kinetics of LiFePO4 Cathode Material in Non-flammable Inorganic Liquid Electrolyte.

We unveil the fundamental insights of electrochemical kinetics of LFP cathode material and the passivation layer formation in the SO2-based non-flammable inorganic liquid electrolyte (IE). The influence of temperature and electrochemical potential cutoff in the electrochemical activity of LFP cathode and IE is disclosed. Furthermore, the materials compatibility, structural and chemical stability of LFP in IE is demonstrated using very slow galvanostatic cycling in combination with LiFePO4||Li0.1FePO4 symmetric cells. The lithium storage performance of LFP half-cell using inorganic electrolyte is presented with the optimum voltage window. LFP half-cells exhibit discharge capacities of 147, 111, and 75 mAh/g at 1, 4, 8 C rates, respectively, with coulombic efficiencies of ~99.98 %. The electrochemical behavior and mechanism of LFP||Graphite cell in IE is investigated while concurrently tracking the electrochemical potentials of LFP and Graphite half-cell.

Recycling of Spent Lithium Iron Phosphate Cathodes: Challenges and Progress.

The number of spent lithium iron phosphate (LiFePO4, LFP) batteries will increase sharply in the next few years, owing to their large market share and development potential. Therefore, recycling of spent LFP batteries is necessary and urgent from both resource utilization and environmental protection standpoints. In this review, the significance of pretreatment for LFP recycling is first underscored, and its technical challenges and recent advancements are presented. Following that, the current recycling methods for spent LFP cathodes are outlined in terms of the respective treating processes, advantages, and disadvantages. Additionally, the preparation methods of LFP cathode material are reviewed to guide the resynthesis of LFP that uses salts obtained from spent LFP, which are beneficial for closed-loop recycling of LFP batteries. Lastly, we explore the future development direction of spent LFP battery recycling, highlighting the importance of technological innovation to advance the sustainable growth of the LFP battery industry.

2D Metal-Oxide Nanosheets as a Homogeneous Li-Ion Flux Regulator for High-Performance Anodeless Lithium Metal Batteries.

The anodeless battery design has recently gained significant interest by eliminating the direct use of a thick lithium (Li) foil. However, it suffers from inhomogeneous Li+ flux, resulting in dendrite growth and a short cycling life. To address this, the exfoliation of layered-structure titanium oxide to 2D nanosheets (2DTiOx) is proposed to precisely control Li+ flux at the atomic scale by maximizing Li+ affinitive Ti sites. Compared to cells without these nanosheets, the Li|2DTiOx|Cu half-cell demonstrates stable cyclability over 900 cycles, with a Coulombic efficiency (CE) over 99% at 0.5 mA cm-2 and 0.5 mAh cm-2. Similarly, a long stable cycling life over 1500 h at 1.0-3.0 mA cm-2 is observed for a 2DTiOx-based symmetric cell containing a limited Li amount from electrodeposited Li metal (e-Li|2DTiOx|e-Li). The full cells (e-Li|2DTiOx||NCM811 and e-Li|2DTiOx||LFP) coupled with NCM811 and LFP cathodes showed a long cycle life of 400 cycles at 1.0 C and 0.5 C, respectively. The exceptional battery performance is attributed to the uniform Li disposition on the 2DTiOx electrode, emphasizing the crucial role of the exposed basal plane in 2DTiOx as an efficient atomic scale Li+ flux regulator. This strategy is expected to advance next-generation lithium metal batteries (LMBs) by highlighting the significance of Li+ affinity at the Ti sites of 2DTiOx nanosheets.

High-Viscosity Phase Inversion Separators for Freestanding and Direct-on-Electrode Manufacturing in Lithium-Ion Batteries.

Separators play a critical role in lithium-ion batteries (LIBs) by facilitating lithium-ion (Li-ion) transport while enabling safe battery operation. However, commercial separators made from polypropylene (PP) or polyethylene (PE) impose a discrete processing step in current LIB manufacturing as they cannot be manufactured with the same slot-die coating process used to fabricate the electrodes. Moreover, commercial separators cannot accommodate newer manufacturing processes used to produce leading-edge microbatteries and flexible batteries with customized form factors. As a path toward rethinking LIB fabrication, we have developed a high-viscosity polymer composite separator slurry that enables the fabrication of both freestanding and direct-on-electrode films. A streamlined phase inversion process is used to impart porosity in cast separator films upon drying. To understand the impacts of material composition and rheology on phase inversion processing and separator performance, we investigated four different separator formulations. We used either diethylene glycol (DEG) or triethyl phosphate (TEP) as a nonsolvent, and either silica (SiO2) or alumina (Al2O3) as an inorganic additive in a polyvinylidene fluoride-co-hexafluoropropylene (PVDF-HFP) matrix. Through a down-selection process, we developed a TEP-SiO2 separator formulation that matched or outperformed a commercial Celgard 2325 (PP/PE/PP) separator and a Beyond Battery ceramic-coated PE (CC/PE/CC) separator under rate and cycle life tests in LiFePO4|Li4Ti5O12 (LFP|LTO) and LiNi0.5Mn0.3Co0.2O2|graphite (NMC-532|graphite) coin cells at C/10-1C rates. Our TEP-SiO2 slurry had a viscosity of 298 Pa s at a 1 s-1 shear rate and shear-thinning behavior. When deposited directly onto an LTO anode and cycled against an LFP cathode, the direct-on-electrode TEP-SiO2 separator increased the specific capacity by 58% and 304% at 2C rates relative to the PP/PE/PP and CC/PE/CC separators, respectively. Additionally, the freestanding TEP-SiO2 separator maintained dimensional stability when heated to 200 °C for 1 h and demonstrated a higher elastic modulus and hardness than the PP/PE/PP and CC/PE/CC separators when measured with nanoindentation.

Functional Protective Coatings Based on Polysaccharides and Single-Ion Conducting Polymers for Li Metal Batteries

This work aims to study a protective coating based on cellulose and P(LiMTFSI) single-ion conductor polymer and its effects on Li metal anode stability and reversibility. The strategy used involves the physical mixture of the aforementioned polymers to enhance the electrochemical performance through Li-ion flux homogenization at the Li metal surface, promoting the formation of a dense plating. Single-ion conducting polymers (SICPs) are incorporated due to their beneficial effects such as enhancing lithium ion transport, boosting lithium transference number (𝑡𝐿𝑖 +), and diminishing the effects of concentration polarization, avoiding the initiation and propagation of high surface area lithium (HSAL). Furthermore, a quasi-solid-state Li metal battery system is explored which brings additional advantages over the typically used organic electrolytes. In this sense, during this study we propose using the protective coating based on cellulose and P(LiMTFSI) to tailor an adequate interphase that creates a good adhesion, by taking advantage of the polymers film formation ability, and therefore improving the lifespan and safety of the battery. The coating effectiveness is tested by casting the solution on an activated lithium surface and performing lithium platting/stripping protocols in Li/Li and Li/Cu pouch cells under selected current densities (0.5, 1 and 2 mA/cm2). Complementary electrochemical tests are carried out to study transport, conductivity parameters, and its performance in full cell coupled with LFP cathode. Finally, we analyze the correlation with the physicochemical properties and electrochemical performed based on spectroscopic techniques and microscopy to study the most relevant parameters influencing a high Coulombic Efficiency. Acknowledgments This work has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska – Curie Grant Agreement N° 945357, and co-financing from the Slovenian Research and Innovation Agency (ARIS) is fully acknowledged.

Room Temperature Efficient Regeneration of Spent LiFePO4 by Direct Chemical Lithiation

The exponential production of lithium-ion batteries for electric vehicles (EVs) and electronic applications leads to the creation of a huge stock of batteries at the end of life. Considering the current economic, geopolitical and environmental context, the recycling of these spent batteries is becoming an urgent need in order to mitigate environmental pollution and limit the waste of valuable and critical resources1.In this work, we report a rewarding direct recycling process of spent LiFePO4 cathode material by direct chemical lithiation in solution2. After safe opening of the spent commercial battery, a structural, morphological, spectroscopic and electrochemical characterization of the spent LFP cathode was carried out to identify the reason(s) of battery failure. The results obtained by XRD (Fig 1a) and Mössbauer spectroscopy (Fig 1b) show that the loss of lithium in the cathode (up to 50%) consumed during formation and growth of the SEI during cycling, is the major reason of the end of life of these batteries, in total agreement with the literature3.To address the lithium shortage problem, a recycling process via direct chemical lithiation in organic solution at room temperature of the LFP cathode has been implemented. Lithium iodide (LiI) dissolved in several solvents such as acetonitrile, cyclohexane, ethanol, DMSO, methanol and propan-1,2-diol was used as both the reductant and the lithiation agent. The best results were obtained with the cathode regenerated in ethanol, which is also the most captivating and environmentally friendly solvent. The different characterizations of this regenerated cathode allow evaluating the efficiency of the regeneration process. Mössbauer spectroscopy (Fig. 2a) confirms the total reduction of FeIIIPO4 to LiFeIIPO4, while electrochemical characterization (Fig. 2b) shows encouraging properties with a reversible capacity of ~168 mAh/g for the regenerated LFP.

(General Student Poster Award Winner, 3rd Place) Lithium Niobate Coatings on Lithium Iron Phosphate Cathode Materials for Applications in Lithium-Ion Batteries

Lithium-ion batteries have become a crucial tool in countering global fossil fuel reliance; when paired with electric motors, they provide an alternative to petroleum-based energy storage for internal combustion engines. Typical cathode materials used in lithium-ion batteries present a unique set of challenges. Some of the electrochemical materials that have a relatively high performance also have serious impacts on the environment and human health.1 Other materials that lack these specific drawbacks, such as lithium iron phosphate (LFP), face other issues. For example, LFP suffers from a relatively low electrical conductivity and a relatively slow lithium-ion diffusion, both of which affect the general electrochemical performance of this material. These weaknesses can be addressed using coatings applied to LFP nanoparticles. Carbon coatings have already been shown to improve the performance of LFP nanoparticles, but materials with higher ionic conductivities have remained relatively undeveloped.2 By synthesizing a composite coating of both carbon and lithium niobate, further improvements to LFP nanoparticles were sought to enable a wider range of applications for this cathode material.In this work, lithium niobate coatings on carbon coated LFP nanoparticles were synthesized using a low temperature solvothermal method. Lithium niobate coatings have been shown to improve the specific capacity, rate capability, and durability of other cathode materials for lithium-ion batteries.3 Half-cells were fabricated to examine the effect of adding a lithium niobate coating to the carbon coated LFP cathode materials. Electrochemical testing techniques such as galvanostatic cycling and cyclic voltammetry were used to compare the properties and performance of the composite coated LFP relative to the carbon coated LFP. The composite coatings were also characterized using transmission electron microscopy, energy dispersive spectroscopy, and X-ray photoelectron spectroscopy. This coating method has resulted in the successful synthesis of lithium niobate coatings on carbon coated LFP nanoparticles with an observed improvement in durability. Goodenough, J. B.; Kim, Y. Challenges for Rechargeable Li Batteries. Mater. 2010, 22 (3), 587–603.Wang, J.; Sun, X. Understanding and Recent Development of Carbon Coating on LiFePO4 Cathode Materials for Lithium-Ion Batteries. Energy Environ. Sci. 2012, 5 (1), 5163–5185.Kim, J. H.; Kim, H.; Choi, W.; Park, M.-S. Bifunctional Surface Coating of LiNbO3 on High-Ni Layered Cathode Materials for Lithium-Ion Batteries. ACS Appl. Mater. Interfaces 2020, 12 (31), 35098–35104.

Full-Dimensional Analysis of Gaseous Products to Unlocking In Depth Thermal Runaway Mechanism of Li-Ion Batteries.

In this study, state-of-the-art on-line pyrolysis MS (OP-MS) equipped with temperature-controlled cold trap and on-line pyrolysis GC/MS (OP-GC/MS) injected through high-vacuum negative-pressure gas sampling (HVNPGS) programming are originally designed/constructed to identify/quantify the dynamic change of common permanent gases and micromolecule organics from the anode/cathode-electrolyte reactions during thermal runaway (TR) process, and corresponding TR mechanisms are further perfected/complemented. On LiCx anode side, solid electrolyte interphase (SEI) would undergo continuous decomposition and regeneration, and the R-H+ (e.g., HF, ROH, etc.) species derived from electrolyte decomposition would continue to react with Li/LiCx to generate H2. Up to above 200°C, the O2 would release from the charged NCM cathode and organic radicals would be consumed/oxidized by evolved O2 to form COx, H2O, and more corrosive HF. On the contrary, charged LFP cathode does not present obvious O2 evolution during heating process and the unreacted flammable/toxic organic species would exit in the form of high temperature/high-pressure (HT/HP) vapors within batteries, indicating higher potential safety risks. Additionally, the in depth understanding of the TR mechanism outlined above provides a clear direction for the design/modification of thermostable electrodes and non-flammable electrolytes for safer batteries.

Constructing Sn-Cu2O Lithiophilicity Nanowires as Stable and High-Performance Lithium Metal Anodes.

Lithium (Li) metal batteries (LMBs) have garnered significant research attention due to their high energy density. However, uncontrolled Li dendrite growth and the continuous accumulation of "dead Li" directly lead to poor electrochemical performance in LMBs, along with serious safety hazards. These issues have severely hindered their commercialization. In this study, a lithiophilic layer of Sn-Cu2O is constructed on the surface of copper foam (CF) grown with Cu nanowire arrays (SCCF) through a combination of electrodeposition and plasma reduction. Sn-Cu2O, with excellent lithiophilicity, reduces the Li nucleation barrier and promotes uniform Li deposition. Simultaneously, the high surface area of the nanowires reduces the local current density, further suppressing the Li dendrite growth. Therefore, at 1 mA cm-2, the half cells and symmetric cells achieve high Coulombic efficiency (CE) and stable operation for over 410 cycles and run smoothly for more than 1350 h. The full cells using an LFP cathode demonstrate a capacity retention rate of 90.6% after 1000 cycles at 5 C, with a CE as high as 99.79%, suggesting excellent prospects for rapid charging and discharging and long-term cyclability. This study provides a strategy for modifying three-dimensional current collectors for Li metal anodes, offering insights into the construction of stable, safe, and fast-charging LMBs.

Enhanced rate capability and capacity of LIB full cells achieved through aerosol jet printing

Thick lithium-iron phosphate (LFP) cathodes (31 mg cm−2) with rationally engineered pore structure and tortuosity were manufactured with an aerosol jet (AJ) printer. Cathode pore structuring was tuned by controlling the rate at which the printed ink dried. Slow-drying prints yielded smoother cathodes while fast-drying prints resulted in mesoscale structuring with substantial surface roughness. X-ray tomography further revealed that the rapid drying of AJ printed LFP cathodes produced low-tortuosity pore channels which were preserved after calendering. Full cells comprised of AJ print optimized LFP cathodes, with 30 mg cm−2 active material loadings, and capacity-matched, AJ printed lithium titanate anodes were assembled and electrochemically tested. Performance of the AJ printed full cells was compared to tape-cast (TC) full cells. At equivalent electrode loadings, compositions, and thicknesses, the AJ full cells outperformed the TC cells, averaging approximately 14% greater capacity per cycle after 100 cycles at a C/2 rate. Furthermore, at 1C, the AJ printed full cells realized a near two-fold increase in discharge capacity over the TC cells.

Enhanced electrochemical performance of a LiFePO4 cathode with an environmentally friendly pectin/polyethylene glycol binder

The advancement of lithium-ion battery technology relies on the development of materials that not only improve performance but also align with environmental sustainability. This work presents a novel water-based pectin-PEG binder for LiFePO4 cathodes that combines eco-friendliness with electrochemical innovation. The binder material is made by mixing pectin, a flexible natural substance, with polyethylene glycol through a radical copolymerization process. This combination gives the binder both flexibility and a boost in electrical performance. Our experimental results demonstrate that LFP cathodes with this binder have an intriguing self-healing ability in comparison with the conventional PVDF binder, enhanced charge-discharge capacities, improved cycling stability, and higher ionic conductivity. Specifically, electrodes utilizing the pectin-PEG binder exhibit an impressive retention of discharge capacity. They maintain roughly 150 mAh g−1 after 500 cycles at 1C with 99% retention, and about 141 mAh g−1 with 97% retention at 3C. Cyclic voltammetry (CV) confirms that the PP binder maintains its ionic diffusion properties at high sweep rates, whereas galvanostatic intermittent titration technique reveals a much higher lithium ion diffusion coefficient (DLi+) within the operational voltage range of the LFP-PP250 electrodes. These findings establish an attractive direction for the development of electrodes for high-energy density, sustainable lithium-ion batteries.

Comparison of laser processability for [formula omitted] cathode material with nanosecond and femtosecond laser

Exploration of increased electrode surface area through laser structuring is undertaken to improve performance. While nanosecond lasers offer cost-effective processing, femtosecond lasers achieve a minimal heat effect, excelling in precision. Prior research has mainly focused on changes in electrode performance due to the duration of laser pulses, with insufficient attention to optimizing processability. This study, therefore, aims to compare the processability of active material coating layer in LFP cathodes using both nanosecond and femtosecond lasers. The specimens were subsequently analyzed morphologically for processability using scanning electron microscopy (SEM). Differences in the cross-sectional morphology of LFP cathodes processed by the two types of lasers revealed that nanosecond lasers require a higher pulse energy density for material removal.

Enhancing Lithium-Ion Diffusion Kinetics in a 3D Lithium Metal Host through Surface Modification with Hierarchical Multimetal Oxides.

Lithium metal is a promising anode candidate to achieve high-energy-density lithium metal batteries (LMBs) due to its ultrahigh theoretical capacity (3860 mA h g-1) and low electrochemical potential (-3.04 V vs S.H.E). Unfortunately, the commercialization of lithium metal anodes is hindered by the growth of Li dendrites and the infinite Li volume changes during the cycling process. Herein, we introduce a 3D hierarchical multimetal oxide nanowire framework as a current collector for Li metal anodes. The hierarchical metal oxide layers of CoO and CuxO provide abundant Li nucleation sites and thus offer uniform Li plating and regulate Li nucleation during the charge/discharge process. As a result, half cells present a prolonging Coulombic efficiency of 97% at 1 mA cm-2 with a capacity of 1 mA h cm-2 for over 300 cycles. A stable cyclability of symmetric cells is demonstrated under 1 mA cm-2 with a capacity of 1 mA h cm-2 for 1500 h. Full cells paired with an LFP cathode show a stable capacity of 131.5 mA h g-1 with a capacity retention of 92% for 200 cycles. These results will shed insights into the design of 3D Cu current collectors for high-performance composite Li metal anodes.

Heavily vanadium-doped LiFePO4 olivine as electrode material for Li-ion aqueous rechargeable batteries

Since LiFePO4 batteries play a major role in the transition to safe, more affordable and sustainable energy production, numerous strategies have been applied to modify LFP cathode, with the aim of improving its electrochemistry. In this contribution, a highly vanadium-doped LiFe0.9V0.1PO4/C composite (LFP/C-10V) is synthesized using the glycine combustion method and characterized by x-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Thermogravimetry Differential Thermal Analysis (TGDTA) and Cyclic Voltammetry (CV). It is shown that 10wt.% of vanadium can substitute Fe positions, thus decreasing unit cell volume, which is followed by generation of Li3V2PO4 traces, as detected by CV. High vanadium doping does not change the carbon content in the composite (≈13 wt%) but improves its electronic conductivity and electrochemical performance in both aqueous and organic electrolytes. The reversibility and current response are increasing following the trend: LFP/C, LFP/C -3mol%V, LFP/C - 5 mol % and LFP/C-10 mol %. The best specific capacity is obtained for the most highly doped olivine, which exhibits a reversible process at 1 mV s−1 in an aqueous electrolyte, thus showing a peak-to-peak distance of 56 mV. The high capacity of LFPC-10V is measured in both LiNO3 and NaNO3 electrolytes amounting to around 100 mAh g−1 at 20 mV s−1. Still, the material is only stable in LiNO3 electrolyte, making it more suitable for Li than Na-ion aqueous rechargeable batteries.

Pyrolysis-based modelling of 18650-type lithium-ion battery fires in thermal runaway with LCO, LFP and NMC cathodes

This study presents a modelling approach for simulating fires in thermal runaway and here, it is applied to 18650-type batteries with LCO, NMC, and LFP cathodes at 100% SOC. The model assumes a single-step pyrolysis, where a solid lumped substance, representing the battery components, degrades into volatiles which are vent gases here. Coupling an in-house MATLAB code and FDS solver, a parameter estimation using Bayesian optimization was performed to fit the simulated mass loss and heat release rate to the experimental measurements. One-step kinetics are used for vent gas combustion, with CO yield obtained from literature and soot yield determined via 1-D diffusion flame simulations with CRECK kinetic mechanism in Cantera solver. 3-D simulations using the obtained models yielded maximum values of flame temperature, CO2 and H2O mole fractions, velocity, radiative heat flux, and flame height as 2520 K, 0.47, 0.15, 10.08 m/s, 13.29 kW/m2, and 0.62 m, respectively. The novelties associated with this approach are that, unlike the past studies, there is no need to model the thermal runaway process prior to flaming and, the resulting heat release rate is experimentally verified which makes further analyses, such as flame temperature, height and heat emissions possible.

The trade-off characteristic between battery thermal runaway and combustion

Lithium iron phosphate (LFP) lithium-ion batteries are widely believed to be more thermally safe than nickel-rich layered LiNixCoyMnzO2 (NCM) batteries because LFP cathodes are more stable. However, LFP batteries have been reported to cause serious combustion accidents. The relationship between internal thermal runaway and external combustion in LFP and NCM batteries remain unclear. Herein, we found that there is a trade-off between thermal runaway within the battery and external combustion. Cathode oxidizability is linearly correlated with the intensity of thermochemical reactions within battery components. The nickel-rich LiNi0.9Co0.05Mn0.05O2|Graphite (NCM955|Gr) battery exhibits the most intense exothermic reactions and energy release due to the strong oxidation of its cathode, leading to the highest thermal runaway temperature of 862.4 °C within the battery. The LiFePO4|Graphite (LFP|Gr) battery with the weak cathode oxidizability shows the lowest temperature of 297.4 °C within the battery, but with the highest laminar flame speed of 55 cm s−1 outside the battery. The reason for this is that the LFP cathode rarely oxidizes the electrolyte, instead, the electrolyte reacts with the anode primarily, thereby generating substantial reductive gases and accumulating the explosion risks. This work provides the theoretical basis and data support for future battery selection and design.