Life Research Articles

Redox‐Mediated Lithium Recovery From Spent LiFePO4 Stabilizes Ferricyanide Catholyte for Durable Zinc‐Ferricyanide Flow Batteries

AbstractThe scarcity of lithium resources and the increasing volume of spent lithium‐ion batteries (LIBs) exacerbate the imbalance between lithium supply and demand. The development of efficient recovery strategies of valuable lithium ion (Li+) from spent LIBs and their subsequent utilization presents both significant opportunities and challenges. Here, we propose an innovative approach for Li+ recovery from spent lithium iron phosphate (LiFePO4) batteries (LFPs) and its subsequent utilization in alkaline zinc‐ferricyanide flow batteries (AZFFBs). Utilizing a redox‐mediated reaction, we achieve exceptional Li+ recovery efficiency from spent LFPs. Furthermore, the recovered Li+ in solution leads to the elevated ionic strength in the electrolyte, enhancing the concentration of [Fe(CN)6]4− to a remarkable level of 1.74 M. Utilizing the above catholyte, an AZFFB cell demonstrates the cycling life extending to 11 000 cycles with a degradation rate as low as 0.00019% per cycle and 0.09% per day at a current density of 120 mA cm−2. This study introduces a straightforward and efficient protocol that eliminates additional intermediate processes, achieving effective Li+ recovery from spent LFPs and subsequent utilization in flow batteries. The resulting AZFFB exhibits high energy density and long lifespan, positioning it as a promising candidate for large‐scale energy storage solutions.

Redox-Mediated Lithium Recovery From Spent LiFePO4 Stabilizes Ferricyanide Catholyte for Durable Zinc-Ferricyanide Flow Batteries.

The scarcity of lithium resources and the increasing volume of spent lithium-ion batteries (LIBs) exacerbate the imbalance between lithium supply and demand. The development of efficient recovery strategies of valuable lithium ion (Li+) from spent LIBs and their subsequent utilization presents both significant opportunities and challenges. Here, we propose an innovative approach for Li+ recovery from spent lithium iron phosphate (LiFePO4) batteries (LFPs) and its subsequent utilization in alkaline zinc-ferricyanide flow batteries (AZFFBs). Utilizing a redox-mediated reaction, we achieve exceptional Li+ recovery efficiency from spent LFPs. Furthermore, the recovered Li+ in solution leads to the elevated ionic strength in the electrolyte, enhancing the concentration of [Fe(CN)6]4- to a remarkable level of 1.74M. Utilizing the above catholyte, an AZFFB cell demonstrates the cycling life extending to 11000 cycles with a degradation rate as low as 0.00019% per cycle and 0.09% per day at a current density of 120mA cm-2. This study introduces a straightforward and efficient protocol that eliminates additional intermediate processes, achieving effective Li+ recovery from spent LFPs and subsequent utilization in flow batteries. The resulting AZFFB exhibits high energy density and long lifespan, positioning it as a promising candidate for large-scale energy storage solutions.

Direct Upcycling Spent LiFePO4 Cathode Material by Pre-Oxidation and Al-V Co-Doping Strategy

Abstract The growing volume of spent lithium iron phosphate (LFP) batteries underscores the need for efficient recycling to mitigate environmental concerns and recover valuable materials. This study presents an upcycling strategy integrating pre-oxidation treatment and Al-V co-doping to produce regenerated LFP (RLFP) from spent LFP (SLFP). The pre-oxidation process effectively removes residual binders, carbon, and electrolytes, while Al-V co-doping shortens the Li⁺ migration path, reduces charge-transfer resistance, and enhances the electrochemical performance of RLFP. Notably, one of the RLFPs prepared by co-doping achieves an outstanding discharge capacity of 146.7 mAh/g at 1C, and exceptional cycling stability, retaining 95.4% capacity after 200 cycles at 1C, which amounts to a 21.5% improvement in capacity retention compared to undoped RLFP. This work thus provides a scalable recycling pathway by offering new insights into impurity control in processing SLFP and highlighting the potential of co-doping to enhance SLFP upcycling.

Evaluating economic and environmental viability of recycling lithium-ion battery for electric vehicles in the middle east: a case study in the UAE

The environmental impacts caused by the manufacturing of spent lithium-ion batteries (LIBs) and the supply risks of the valuable metals in electric vehicle (EV) batteries can be mitigated by recycling used LIBs. This study employed a Cradle-to-Gate life cycle assessment (LCA) and cost-benefit analysis, to evaluate the environmental and economic advantages of recycling and remanufacturing Nickel Manganese Cobalt (NMC) cells using hydrometallurgical and pyrometallurgical processes, compared to manufacturing with virgin materials. In the regional context, hydrometallurgy-based LIB remanufacturing has the potential to reduce energy consumption and greenhouse gas (GHG) emissions by 10.7%, accompanied by 11.3% cost savings, compared to virgin material manufacturing. However, despite its potential for GHG emission reduction, pyrometallurgy-based remanufacturing is economically unviable across all scenarios considered. The economics of LIB recycling are significantly influenced by spent LIB costs, requiring careful management of market trends and purchase expenses for feasibility. Challenges have arisen from the increasing volume of spent LIBs and production cost fluctuations. Various LIB chemical compositions yield nuanced outcomes, with NMC111 and NMC811 showing promise for economic and environmental aspects, respectively, while NMC532 and NMC111 demonstrate relative suitability for a cell remanufacturing. Preliminary analysis of Lithium Iron Phosphate (LFP) batteries, an emerging chemistry with growing adoption, highlights unique challenges underscoring the need for further research. This study marks the first economic and environmental evaluation of LIB recycling in the oil-rich Middle East, emphasizing the need for an assessment tailored to the UAE to inform regional policy development. This framework could be adapted for use in other Middle Eastern countries, aiding the formulation of effective regional policies and regulations.

Salt‐Free Solid Polymer Electrolytes Enabling Inorganic‐Rich Solid‐Electrolyte Interphase for Stable and Cost‐Effective Li‐Metal Batteries

AbstractConstructing robust solid‐electrolyte interphase (SEI) on electrodes is crucial for achieving stable lithium metal batteries in liquid electrolytes. However, intrinsic issues associated with liquid electrolytes remain unavoidable, such as the continuous corrosion of SEI and the high costs involved. Herein, a novel lithium salt‐free solid‐state polymer electrolyte (SPE) is introduced enabled by in situ polymerization of 1,3‐dioxolane and 1,3,5‐trioxane with the addition of ionic liquid to eliminate the drawbacks of liquid electrolyte. The homogeneous interaction between the polymer and ionic liquid constructs a synergistic Li+ conduction pathway, promoting the extraction of Li+ out of the cathode/anode and the smooth transport throughout the polymer network to endow a higher Li+ transference number (0.63) and a comparable ionic conductivity (1.21 mS cm−1) to the conventional liquid electrolyte (0.45 and 5.51 mS cm−1). The absence of lithium salt prevents the oxidative decomposition of lithium salts in electrolytes to generate hazardous and corrosive acidic species. More intriguingly, an anion‐dominated solvation configuration can be realized by the incorporation of ionic liquid with the polymer matrix, inducing the formation of an inorganic‐rich and anti‐corrosive SEI on the electrodes. The resulting salt‐free SPE enables superior cycling stability in lithium||LiFePO4 battery with a high capacity retention of over 92% after 780 cycles.

Research of Ternary Lithium/Iron Phosphate Lithium Battery SOC Estimation Based on Data-Driven Model Integrating Self-Attention Mechanism

To enhance the accuracy of lithium-ion battery state-of-charge (SOC) prediction, this study develops an improved deep learning model optimized by the novel improved dung beetle optimizer (NIDBO). The NIDBO algorithm is derived from traditional dung beetle optimizer by introducing an optimal value guidance strategy and a reverse learning strategy. The deep learning model integrates convolutional neural networks (CNN), bidirectional gated recurrent units (BIGRU), and a self-attention mechanism to form the CNN-BIGRU-SA model. Subsequently, the NIDBO algorithm is employed to optimize the hyperparameters of the model, aiming to improve prediction performance. Discharge data from ternary lithium batteries and lithium iron phosphate batteries were collected. Each type of battery was subjected to 12 operating conditions, totaling 24 sets of battery operating condition data, which were used to test and validate the effectiveness of the model. The results demonstrate that the proposed model exhibits exceptional accuracy in SOC prediction, offering significant advantages over traditional methods and unoptimized models. At the same time, the model was tested under dynamic stress test and federal urban driving schedule conditions. Additionally, the generalization capability of the model is verified by cross-validating the discharge data of the two types of batteries.

Reaction mechanism of extracting Li and Fe from retired lithium iron phosphate battery powder through roasting and water leaching with sulfamic acid

Reaction mechanism of extracting Li and Fe from retired lithium iron phosphate battery powder through roasting and water leaching with sulfamic acid

Early warning of thermal runaway for larger-format lithium iron-phosphate battery by coupling internal pressure and temperature

Early warning of thermal runaway for larger-format lithium iron-phosphate battery by coupling internal pressure and temperature

Selective recovery of lithium from spent LiFePO4 batteries based on PMS advanced oxidation process

Selective recovery of lithium from spent LiFePO4 batteries based on PMS advanced oxidation process

A novel state of charge estimation method for LiFePO4 battery based on combined modeling of physical model and machine learning model

A novel state of charge estimation method for LiFePO4 battery based on combined modeling of physical model and machine learning model

Research on aging-thermal characteristics coupling and aging thermal management analysis of large-capacity LiFePO4 battery

Research on aging-thermal characteristics coupling and aging thermal management analysis of large-capacity LiFePO4 battery

Lithium Iron Phosphate Battery Regeneration and Recycling: Techniques and Efficiency

This study investigates advanced strategies for r regenerating and recycling lithium iron phosphate (LiFePO4, LFP) materials from spent lithium-ion batteries. Recovery techniques are categorized into direct regeneration, which restores positive electrode materials with high electrochemical performance, and recycling, which produces intermediate compounds such as lithium carbonate and iron phosphate. Additionally, resynthesis methods are explored to convert recovered precursors into high-quality LFP materials, ensuring their reuse in battery production. Innovative approaches, including carbothermic reduction, doping, and hydrothermal resynthesis, are highlighted for their ability to enhance material properties, improve energy efficiency, and maintain the olivine structure of LFP. Key advancements include the use of eco-friendly reagents, automation, and optimization strategies to reduce environmental impacts and costs. Regenerated and resynthesized positive electrodes demonstrated performance metrics comparable to or exceeding commercial LFP, showcasing their potential for widespread application. This work underscores the importance of closed-loop recycling systems and identifies pathways for scaling, improving economic feasibility, and minimizing the ecological footprint of the lithium-ion battery lifecycle.

Geometry‐Dependent Dynamic Impact Behavior of Lithium–Iron Phosphate Batteries at Different Velocities: An Experimental and Numerical Approach

The present work reports the drop weight impact tests with 18650 lithium–iron phosphate batteries (LFPB) at different impact velocities (1.04, 1.26, 1.36, and 1.69 m s−1) at 0% and 50% state of charge (SOC). The investigation is extended for other battery geometry namely, 22650, 26650, and 32650. The thermal runaway triggering point is characterized by the event of internal short‐circuit (ISC) resulting in voltage drop. The voltage drop phenomenon is ruled out to be present in the case of the tests at SOC 0%, while it is noticed for velocities 1.26 m s−1 and above at SOC 50%. For SOC 50%, the voltage‐time curve exhibits 87.5% and 21.2% drop corresponding to the highest and lowest impact velocity respectively. Further, the dynamic impact behavior is numerically simulated. The findings shows that the ultimate stress observed is maximum (0.53 MPa) for 32650 while it is minimum (0.47 MPa) for 22650 corresponding to SOC 0%. On the other hand, the ultimate stress is found to be maximum (0.68 MPa) for 22650 and minimum (0.47 MPa) for 26650. The outperformance of LFPB 26650 is observed in terms of its dynamic impact behavior.

A novel method for selective lithium recovery from end-of-life LiFePO4 automotive batteries via thermal treatment combined with a leaching process.

As the demand for electric vehicles increases, effective solutions for recycling end-of-life lithium-ion batteries become crucial. Since lithium iron phosphate (LFP) batteries represent a significant portion of the automotive battery market, this research introduces an innovative method to produce concentrated lithium solutions by combining a calcination process with a microwave-assisted hydrometallurgical process. The initial steps involve safe collection and disassembly of discarded batteries to preserve components and minimize contamination. The cathode coils are separated and ground to a particle size smaller than 0.25mm, concentrating 96% of the lithium compounds. Afterward, the cathode material undergoes calcination for 1h at temperatures ranging from 300 to 900 °C in air and N₂ atmospheres. For samples treated in an oxidative atmosphere, the complete phase conversion of LiFePO₄ to Li₂Fe₃(PO₄)₃ occurs at 500 °C, whereas in an inert atmosphere, this phase change fully manifests at 700 °C. Different sulfuric acid concentrations (0.5, 1.0, and 1.5mol/L) are subsequently used in the microwave-assisted leaching process for all the calcined and non-calcined cathodic powders. Using leaching with aqua regia as a reference for the complete leaching of metals, the best results in terms of lithium selectivity are achieved with samples calcined at 500 °C and leached with 0.5mol/L sulfuric acid. Under these conditions, 75% of all the lithium and only 2.5% of all the iron are extracted in solution. This result demonstrates that calcination in an air atmosphere prior to a hydrometallurgical process plays a fundamental role in achieving high lithium selectivity without the need for any other additives.

Nanoengineering of Ultrathin Carbon-Coated T-Nb2O5 Nanosheets for High-Performance Lithium Storage

Niobium pentoxide (Nb2O5) is a promising anode candidate for lithium-ion batteries due to its high theoretical capacity, excellent rate capability, and safe working potential. However, its inherent low conductivity limits its practical application in fast-charging scenarios. In this work, we develop an ultrathin carbon-coated two-dimensional T-Nb2O5 nanosheet composite (T-Nb2O5@UTC) through a facile solvothermal reaction and subsequent CVD acetylene decomposition. This unique design integrates a two-dimensional nanosheet structure with an ultrathin carbon layer, significantly enhancing electronic conductivity, reducing ion diffusion pathways, and preserving structural integrity during cycling. The T-Nb2O5@UTC electrode demonstrates an impressive specific capacity of 214.7 mAh g−1 at a current density of 0.1 A g−1, maintaining 117.9 mAh g−1 at 5 A g−1, much outperforming the bare T-Nb2O5 (179.6 mAh g−1 at 0.1 A g−1 and 62.9 mAh g−1 at 5 A g−1). It exhibits outstanding cyclic stability, retaining a capacity of 87.9% after 200 cycles at 0.1 A g−1 and 83.7% after 1000 cycles at 1 A g−1. In a full-cell configuration, the assembled T-Nb2O5@UTC||LiFePO4 battery exhibits a desirable specific capacity of 186.2 mAh g−1 at 0.1 A g−1 and only a 1.5% capacity decay after 120 cycles. This work underscores a nanostructure engineering strategy for enhancing the electrochemical performance of Nb2O5-based anodes toward high-energy-density and fast-charging applications.

A Multifunctional Molecular Modulated Strategy Featuring Novel Li+ Transport Centers and Li2O‐Rich SEI Layer for High‐Performance All‐Solid‐State Lithium Metal Batteries

AbstractThe poor ionic conductivity and interfacial instability severely limit the application of polyethylene oxide (PEO)‐based polymer electrolytes. In this work, we introduce a multifunctional molecular modulated strategy using coumarin, which simultaneously boosts the ionic conductivity and interfacial stability of PEO‐coumarin (PLC) membrane. Unlike conventional additives that diminish PEO's crystallinity, coumarin, with its higher Li+ adsorption energy and stronger dipole moments, acts as a novel ‘carrier’ for Li+ without compromising the mechanical properties of the PEO matrix. Its synergistic effect with PEO creates a more efficient Li+ transport pathway to achieve a high ionic conductivity of 1.1 mS cm−1 at 60 °C. Simultaneously, coumarin as a sacrificial agent by utilizing its carbonyl group, preferentially reacts with lithium metal to prevent the decomposition of PEO and lithium salts. Furthermore, coumarin acts as an in situ Li2O‐inducer, facilitating the formation of a dense Li2O‐rich solid electrolyte interphase (SEI) layer with faster ion diffusion kinetics at the interface. The beneficial effect of the multifunctional molecular engineering design enables the Li|PLC|Li symmetric cell to cycle over 5000 h and allows the Li|PLC|LiFePO4 battery to deliver a high initial discharge capacity of 161.9 mAh g−1 with a capacity retention ratio of 93 % after 550 cycles at 0.5 C.

Failure analysis of lithium iron phosphate batteries under squeezing conditions

This study investigated the influence of various factors on the safety performance of lithium iron phosphate (LFP) batteries by examining the internal structural changes under squeezing conditions. Squeezing tests were conducted on square LFP batteries, and deformation and failure mechanisms were analyzed using industrial computed tomography (CT) scan technology. The results reveal that the deformation of the battery decreases as the state of charge (SOC) value increases. Furthermore, increasing squeezing pressure leads to increased deformation and raises the risk of an internal short circuit. Additionally, compared to the front squeezing direction, the battery exhibits more significant deformation in the lateral direction. The SOC value has a minor effect on voltage, whereas high squeezing pressure or significant deformation can lead to a substantial voltage drop, potentially followed by a partial or complete recovery to a stable state. Moreover, within a specific range, squeezing exerts minimal influence on the surface temperature of the battery. These research findings provide valuable insights for optimizing the design and safety assessment of LFP batteries.

Multi-factor aging in Lithium Iron phosphate batteries: Mechanisms and insights

Multi-factor aging in Lithium Iron phosphate batteries: Mechanisms and insights

An Online Monitoring Method for Lithium Iron Phosphate Batteries Based on Matlab Model

An Online Monitoring Method for Lithium Iron Phosphate Batteries Based on Matlab Model

Enhancing early warning systems: Experimental investigation of physical signals in thermal runaway evolution of large-capacity lithium iron phosphate batteries

Enhancing early warning systems: Experimental investigation of physical signals in thermal runaway evolution of large-capacity lithium iron phosphate batteries