Comprehensive Technology for Recycling and Regenerating Materials from Spent Lithium Iron Phosphate Battery.

The lithium iron phosphate (LFP) battery has been widely used in electric vehicles and energy storage for its good cyclicity, high level of safety, and low cost. The massive application of LFP battery generates a large number of spent batteries. Recycling and regenerating materials from spent LFP batteries has been of great concern because it can significantly recover valuable metals and protect the environment. This paper aims to critically assess the latest technical information available on the echelon utilization and recycling of spent LFP batteries. First, it focuses on the progress of disassembly, evaluation and detection, regrouping, and application in echelon utilization. Then, the recycling technologies, including pretreatment, direct repair, and material regeneration, of spent LFPs are summarized. Finally, the paper proposes some challenges in the echelon utilization and recycling of spent LFP batteries, and concludes with recommendations for an intelligent, refined, and clean LFP battery circulation system that are required to ensure the sustainable development of spent LFP battery recycling.

Environment-friendly, efficient process for mechanical recovery of waste lithium iron phosphate batteries.

Technology for recycling retired lithium batteries has become increasingly environment-friendly and efficient. In traditional recovery methods, pyrometallurgy or hydrometallurgy is often used as an auxiliary treatment method, which results in secondary pollution and increases the cost of harmless treatment. In this article, a new method for combined mechanical recycling of waste lithium iron phosphate (LFP) batteries is proposed to realize the classification and recycling of materials. Appearance inspections and performance tests were conducted on 1000 retired LFP batteries. After discharging and disassembling the defective batteries, the physical structure of the cathode binder was destroyed under ball-milling cycle stress, and the electrode material and metal foil were separated using ultrasonic cleaning technology. After treating the anode sheet with 100 W of ultrasonic power for 2 minutes, the anode material was completely stripped from the copper foil, and no cross-contamination between the copper foil and graphite was observed. After the cathode plate was ball-milled for 60 seconds with an abrasive particle size of 20 mm and then ultrasonically treated for 20 minutes with a power of 300 W, the stripping rate of the cathode material reached 99.0%, and the purities of the aluminium foil and LFP reached 100% and 98.1%, respectively.

Low-temperature thermal pretreatment process for recycling inner core of spent lithium iron phosphate batteries.

Spent lithium iron phosphate (LFP) batteries contain abundant strategic lithium resources and are thus considered attractive secondary lithium sources. However, these batteries may contaminate the environment because they contain hazardous materials. In this work, a novel process involving low-temperature heat treatment is used as an alternative pretreatment method for recycling spent LFP batteries. When the temperature reaches 300°C, the dissociation effect of the anode material gradually improves with heat treatment time. At the heat treatment time of 120 minutes, an electrode material can be dissociated. The extension of heat treatment time has a minimal effect on quality loss. The physicochemical changes in thermally treated solid cathode and anode materials are examined through scanning electron microscopy with energy-dispersive X-ray spectroscopy. The heat treatment results in the complete separation of the materials from aluminium foil without contamination. The change in heat treatment temperature has a small effect on the quality of LFP material shedding. When the heat treatment temperature reaches 300°C and the time reaches 120 minutes, heat treatment time increases, and the yield of each particle size is stable and basically unchanged. The method can be scaled up and may reduce environmental pollution due to waste LFP batteries.

Environmentally friendly automated line for recovering aluminium and lithium iron phosphate components of spent lithium-iron phosphate batteries.

Lithium iron phosphate (LFP) batteries contain metals, toxic electrolytes, organic chemicals and plastics that can lead to serious safety and environmental problems when they are improperly disposed of. The published literature on recovering spent LFP batteries mainly focuses on policy-making and conceptual design. The production line of recovering spent LFP batteries and its detailed operation are rarely reported. A set of automatic line without negative impact to the environment for recycling spent LFP batteries at industrial scale was investigated in this study. It includes crushing, pneumatic separation, sieving, and poison gas treatment processes. The optimum retaining time of materials in the crusher is 3 minutes. The release rate is the highest when the load of the impact crusher is 800 g. An air current separator (ACS) was designed to separate LFP from aluminium (Al) foil and LFP powder mixture. Movement behaviour of LFP powder and Al foil in the ACS were analysed, and the optimized operation parameter (35.46 m/s) of air current speed was obtained through theoretical analysis and experiments. The weight contents of an Al foil powder collector from vibrating screen-3 and LFP powder collector from bag-type dust collector are approximately 38.7% and 52.4%, respectively. The economic cost of full manual dismantling is higher than the recovery production line. This recycling system provides a feasible method for recycling spent LFP batteries.

Environment-friendly technology for recovering cathode materials from spent lithium iron phosphate batteries.

The consumption of lithium iron phosphate (LFP)-type lithium-ion batteries (LIBs) is rising sharply with the increasing use of electric vehicles (EVs) worldwide. Hence, a large number of retired LFP batteries from EVs are generated annually. A recovery technology for spent LFP batteries is urgently required. Compared with pyrometallurgical, hydrometallurgical and biometallurgical recycling technologies, physical separating technology has not yet formed a systematic theory and efficient sorting technology. Strengthening the research and development of physical separating technology is an important issue for the efficient use of retired LFP batteries. In this study, spent LFP batteries were discharged in 5 wt% sodium chloride solution for approximately three hours. A specially designed machine was developed to dismantle spent LFP batteries. Extending heat treatment time exerted minimal effect on quality loss. Within the temperature range of 240°C-300°C, temperature change during heat treatment slightly affected mass loss. The change in heat treatment temperature also had negligible effect on the shedding quality of LFP materials. The cathode material and the aluminium foil current collector accounted for a certain proportion in a sieve with a particle size of -1.25 + 0.40 mm. Corona electrostatic separation was performed to separate the metallic particles (with a size range of -1.5 + 0.2 mm) from the nonmetallic particles of crushed spent LFP batteries. No additional reagent was used in the process, and no toxic gases, hazardous solid waste or wastewater were produced. This study provides a complete material recovery process for spent LFP batteries.

Eddy current separation for recovering aluminium and lithium-iron phosphate components of spent lithium-iron phosphate batteries.

With the rapid development of the electric vehicle market since 2012, lithium-iron phosphate (LFP) batteries face retirement intensively. Numerous LFP batteries have been generated given their short service life. Thus, recycling spent LFP batteries is crucial. However, published information on the recovery technology of spent LFP batteries is minimal. Traditional separators and separation theories of recovering technologies were unsuitable for guiding the separation process of recovering metals from spent LFP batteries. The separation rate of the current method for recovering spent LFP batteries was rather low. Furthermore, some wastewater was produced. In this study, spent LFP batteries were dismantled into individual parts of aluminium shells, cathode slices, polymer diaphragms and anode slices. The anode pieces were scraped to separate copper foil and anode powder. The cathode pieces were thermally treated to reduce adhesion between the cathode powder and the aluminium foil. The dissociation rate of the cathode slices reached 100% after crushing when the temperature and time reached 300℃ and 120 min, respectively. Eddy current separation was performed to separate nonferrous metals (aluminium) from aluminium and LFP mixture. The optimized operation parameters for the eddy current separation were feeding speed of 1 m/s and magnetic field rotation speed of 4 m/s. The separation rate of the eddy current separation reached 100%. Mass balance of the recovered materials was conducted. Results showed that the recovery rate of spent LFP can reach 92.52%. This study established a green and full material recovery process for spent LFP batteries.

Pneumatic separation and recycling of anode and cathode materials from spent lithium iron phosphate batteries.

A novel approach to recycling of copper and aluminum fragments in the crushed products of spent lithium iron phosphate batteries was proposed to achieve their eco-friendly processing. The model of pneumatic separation that determines the optimal airflow velocity was established using aerodynamics. The influence of the airflow velocity, and the density and thickness, and their ratios, of the aluminum and copper fragments on pneumatic separation were evaluated. The results show that the optimal airflow velocities of copper and aluminum fragments with and without the electrode materials are 3.27m/s and 1.67m/s, respectively. The accuracy and reliability of the present model was verified using a pneumatic separation experiment. It is concluded that graded pneumatic separation is unnecessary for the crushed particle size more than 9 mm. The experimentally determined optimal airflow velocity of the copper and aluminum fragments with and without the electrode materials is 3.3m/s and 1.7m/s, respectively. The mass fractions of the copper and aluminum fragments upon removal of the electrode materials after pneumatic separation are 97% and 96%, respectively, and both with the electrode material achieve 97.0%. The theoretically obtained optimal airflow velocities have good agreements with the experimentally obtained ones.

Combined mechanical process recycling technology for recovering copper and aluminium components of spent lithium-iron phosphate batteries.

The recycling processes of spent lithium iron phosphate batteries comprise thermal, wet, and biological and mechanical treatments. Limited research has been conducted on the combined mechanical process recycling technology and such works are limited to the separation of metal and non-metal materials, which belongs to mechanical recovery. In this article the combined mechanical process recycling technology of spent lithium iron phosphate batteries and the separation of metals has been investigated. The spent lithium iron phosphate batteries monomer with the completely discharged electrolyte was subjected to perforation discharge. The shell was directly recycled and the inner core was directly separated into a positive electrode piece, dissepiment, and negative electrode piece. The dissociation rate of the positive and negative materials reached 100.0% after crushing when the temperature and time reached 300 °C and 120 min. The crushed products were collected and sequentially sieved after the low-temperature thermal treatment. Then, nonferrous metals (copper and aluminium) were separated from the crushed spent lithium iron phosphate batteries by eddy current separation with particle size -4 + 0.4. The optimised operation parameters of eddy current separation were fed at speeds of 40 r min-1, and the rotation speed of the magnetic field was 800 r min-1. The nonferrous metals of copper and aluminium were separated by the method of pneumatic separation. The optimal air speed was 0.34 m s-1 for the particle-size -1.6 + 0.4 mm and 12.85-14.23 m s-1 for the particle-size -4 + 1.6 mm. The present recycling process is eco-friendly and highly efficient and produces little waste.

Ferrioxalate photolysis-assisted green recovery of valuable resources from spent lithium iron phosphate batteries.

Recovering valuable resources from spent cathodes while minimizing secondary waste generation is emerging as an important objective for the future recycling of spent lithium-ion batteries, including lithium iron phosphate (LFP) batteries. This study proposes the use of oxalic acid leaching followed by ferrioxalate photolysis to separate and recover cathode active material elements from spent LFP batteries. The cathode active material can be rapidly dissolved at room temperature using appropriate quantities of oxalic acid and hydrogen peroxide, as determined through thermodynamic calculations. The dissolved ferrioxalate complex ion (Fe(C2O4)33-) is selectively precipitated through subsequent photolysis at room temperature. Depending on the initial concentration, the decomposition ratio can exceed 95 % within 1-4 h. Molecular mechanism analysis reveals that the decomposition of the Fe(C2O4)33- complex ion into water-insoluble FeC2O4·2H2O results in the precipitation of iron and the separation of metal elements. Lithium can be recovered as dihydrogen phosphates through filtration and water evaporation. No additional precipitant is needed and no other side products are generated during the process. Oxalic acid leaching followed by photolysis offers an environmentally friendly and efficient method for metal recovery from spent LFP cathodes. The photochemical process is a promising approach for reducing secondary waste generation in battery recycling.

A new model of trajectory in eddy current separation for recovering spent lithium iron phosphate batteries.

Eddy current separation (ECS) is an environment-friendly technology for separating nonferrous metallic particles whose size was from 2 mm to 10 mm. No wastes are generated in ECS. ECS quality of nonferrous metals from solid wastes is rather low in the production practice of spent lithium iron phosphate (LFP) batteries recovering. Repeating separation even manual sorting is required in the production. The traditional method of falling point prediction based on eddy current mechanics uses equivalent acceleration to replace separation motion curves. These curves have low precision and are unsuitable for predicting the motion trajectory of small particle size of sorted materials. In this work, eddy current separation of positive and negative plates in a crushed product of spent lithium iron phosphate battery is used as an example to establish the force and kinematics models of different materials in the eddy current separation. An iterative method, rather than average speed method, is used to improve the accuracy of the model. Displacement interval replaces disengagement angle as a separating index to improve the model's intuitiveness and practical guidance. In the range of 2-20 mm, test results are consistent with simulation results. The copper and aluminium foils at a magnetic roller speed of 800r/min can be separated to a maximum particle size ratio of 1.72, and the maximum particle size ratio of copper and positive electrode sheets can be large. This paper provided an environmental-friendly and effective technology for separating nonferrous metals from crushed spent LFP batteries.