Advancing Upcycling and Regeneration of Spent LiFePO4: Failure Mechanisms and Recovery Strategies

Yi Wang , Xue Liu , Wen Luo , Rui Xu , Ze Wang , Jean-Jacques Gaumet , Liqiang Mai

Carbon Energy ›› 2026, Vol. 8 ›› Issue (6) : e70198

PDF (4692KB)
Carbon Energy ›› 2026, Vol. 8 ›› Issue (6) :e70198 DOI: 10.1002/cey2.70198
REVIEW
Advancing Upcycling and Regeneration of Spent LiFePO4: Failure Mechanisms and Recovery Strategies
Author information +
History +
PDF (4692KB)

Abstract

With the widespread application of lithium iron phosphate (LFP) batteries in electric vehicles and energy storage fields, the number of retired LFP has increased sharply. Therefore, the development of efficient and environmentally friendly regeneration methods is crucial for the sustainable utilization of resources and environmental protection. In this review, failure mechanism of LFP through advanced characterization technologies is summarized, and upcycling strategies based on the failure mechanism are highlighted. Then, the advantages and challenges of traditional hydrometallurgy, direct regeneration, and upcycling in the recovery of spent LFP (S-LFP) are explored. Among them, upcycling mainly includes strategies such as structural optimization, phase transformation, and conversion into other functional materials. Moreover, the application of materials obtained by upcycling exhibits broaden aspect, including reusing lithium-ion batteries, sodium-ion batteries, and catalytic materials, which significantly improves the economic value of S-LFP cathode materials. Finally, the upcycling method by combining advanced characterization technologies and machine learning to promote the applications and establish a unified economic and environmental analysis system to provide clear analysis standards for relevant research is emphasized.

Keywords

characterization method / direct regeneration / failure mechanism / LiFePO4 / spent battery / upcycling

Cite this article

Download citation ▾
Yi Wang, Xue Liu, Wen Luo, Rui Xu, Ze Wang, Jean-Jacques Gaumet, Liqiang Mai. Advancing Upcycling and Regeneration of Spent LiFePO4: Failure Mechanisms and Recovery Strategies. Carbon Energy, 2026, 8 (6) : e70198 DOI:10.1002/cey2.70198

登录浏览全文

4963

注册一个新账户 忘记密码

References

[1]

H. Zhao, H. D. Deng, A. E. Cohen, et al., “Learning Heterogeneous Reaction Kinetics From X-Ray Videos Pixel by Pixel,” Nature 621, no. 7978 (2023): 289–294.

[2]

P. Li, S. Luo, Y. Lin, et al., “Fundamentals of the Recycling of Spent Lithium-Ion Batteries,” Chemical Society Reviews 53, no. 24 (2024): 11967–12013.

[3]

J. Wang, J. Ma, Z. Zhuang, et al., “Toward Direct Regeneration of Spent Lithium-Ion Batteries: A Next-Generation Recycling Method,” Chemical Reviews 124, no. 5 (2024): 2839–2887.

[4]

Y. Zhao, H. Du, Y. Kang, et al., “Spent Battery Regeneration for Better Recycling,” Nature Reviews Materials 10 (2025): 722–724.

[5]

R. Fang, K. Chen, Z. Sun, G. Hu, D. W. Wang, and F. Li, “Realizing High-Energy Density for Practical Lithium-Sulfur Batteries,” Interdisciplinary Materials 2, no. 5 (2023): 761–770.

[6]

X. Sun, Y. Zhou, D. Li, et al., “A Review of Electrospun Separators for Lithium-Based Batteries: Progress and Application Prospects,” Carbon Energy 6, no. 9 (2024): e539.

[7]

J. J. Roy, D. M. Phuong, V. Verma, et al., “Direct Recycling of Li-Ion Batteries From Cell to Pack Level: Challenges and Prospects on Technology, Scalability, Sustainability, and Economics,” Carbon Energy 6, no. 6 (2024): e492.

[8]

Lithium-Ion Battery Market Size, Share, and Trends 2025 to 2034, accessed May 28, 2025, https://www.precedenceresearch.com/lithium-ion-battery-recyclingmarket.

[9]

E. Fan, L. Li, Z. Wang, et al., “Sustainable Recycling Technology for Li-Ion Batteries and Beyond: Challenges and Future Prospects,” Chemical Reviews 120, no. 14 (2020): 7020–7063.

[10]

TrendForce. Battery Recycling to Aid in Reducing Carbon Emissions, Global EV, Energy Storage Battery Recycling Market Forecast to Exceed 1TWh in 2030, accessed October 24, 2022, https://www.trendforce.com/presscenter/news/20221024-11436.html.

[11]

J. Yan, J. Qian, Y. Li, L. Li, F. Wu, and R. Chen, “Toward Sustainable Lithium Iron Phosphate in Lithium-Ion Batteries: Regeneration Strategies and Their Challenges,” Advanced Functional Materials 34, no. 44 (2024): 2405055.

[12]

C. Qi, T. Yao, W. Zhai, M. Zhang, L. Song, and J. He, “Advances in Degradation Mechanism and Sustainable Recycling of LiFePO4-Type Lithium-Ion Batteries,” Energy Storage Materials 71 (2024): 103623.

[13]

M. Zhou, B. Li, J. Li, and Z. Xu, “Pyrometallurgical Technology in the Recycling of a Spent Lithium Ion Battery: Evolution and the Challenge,” ACS ES&T Engineering 1, no. 10 (2021): 1369–1382.

[14]

J. C. Y. Jung, P. C. Sui, and J. Zhang, “A Review of Recycling Spent Lithium-Ion Battery Cathode Materials Using Hydrometallurgical Treatments,” Journal of Energy Storage 35 (2021): 102217.

[15]

Z. J. Baum, R. E. Bird, X. Yu, and J. Ma, “Lithium-Ion Battery Recycling-Overview of Techniques and Trends,” ACS Energy Letters 7, no. 2 (2022): 712–719.

[16]

T. Zhao, Y. Choi, C. Wu, et al., “A Review on Direct Regeneration of Spent Lithium Iron Phosphate: From Waste to Wealth,” Science of the Total Environment 957 (2024): 177748.

[17]

X. Liu, R. Wang, S. Liu, et al., “Organic Eutectic Salts-Assisted Direct Lithium Regeneration for Extremely Low State of Health Ni-Rich Cathodes,” Advanced Energy Materials 13, no. 44 (2023): 2302987.

[18]

X. Liu, S. Liu, J. Pu, et al., “Sustainable and Direct Upcycling of Waste Graphite Anodes via Deep Eutectic Solvents,” Advanced Science 12 (2025): e06637.

[19]

R. Fang, K. Chen, Z. Sun, G. Hu, D. W. Wang, and F. Li, “Realizing High-Energy Density for Practical Lithium-Sulfur Batteries,” Interdisciplinary Materials 2, no. 5 (2023): 761–770.

[20]

H. Ji, J. Wang, X. Qiu, et al., “A Universal Protocol for Ultrafast Direct Regeneration and Upcycling of Spent Lithium-Ion Battery Cathode Materials,” Nature Protocols 36, no. 36 (2025): 2407029.

[21]

J. Wang, H. Ji, J. Li, et al., “Direct Recycling of Spent Cathode Material at Ambient Conditions via Spontaneous Lithiation,” Nature Sustainability 7 (2024): 1283–1293.

[22]

W. Chen, J. Li, H. Ji, et al., “Efficient and Scalable Direct Regeneration of Spent Layered Cathode Materials via Advanced Oxidation,” Advanced Materials 37, no. 9 (2025): 2416818.

[23]

H. Ji, J. Wang, H. Qu, et al., “Closed-Loop Direct Upcycling of Spent Ni-Rich Layered Cathodes Into High-Voltage Cathode Materials,” Advanced Materials 36, no. 36 (2024): 2407029.

[24]

W. Wang, R. Wang, R. Zhan, et al., “Probing Hybrid LiFePO4/FePO4 Phases in a Single Olive LiFePO4 Particle and Their Recovering From Degraded Electric Vehicle Batteries,” Nano Letters 23, no. 16 (2023): 7485–7492.

[25]

M. Zheng, Y. You, and J. Lu, “Understanding Materials Failure Mechanisms for the Optimization of Lithium-Ion Battery Recycling,” Nature Reviews Materials 10 (2025): 355–368.

[26]

Z. Qin, Y. Zhang, W. Luo, et al., “A Universal Molten Salt Method for Direct Upcycling of Spent Ni-Rich Cathode Towards Single-Crystalline Li-Rich Cathode,” Angewandte Chemie International Edition 62, no. 25 (2023): e202218672.

[27]

C. R. Birkl, M. R. Roberts, E. McTurk, P. G. Bruce, and D. A. Howey, “Degradation Diagnostics for Lithium Ion Cells,” Journal of Power Sources 341 (2017): 373–386.

[28]

L. Guo, Y. Zhang, J. Wang, et al., “Unlocking the Energy Capabilities of Micron-Sized LiFePO4,” Nature Communications 6, no. 1 (2015): 7898.

[29]

A. Andersson, “Lithium Extraction/Insertion in LiFePO4: An X-Ray Diffraction and Mössbauer Spectroscopy Study,” Solid State Ionics 130, no. 1–2 (2000): 41–52.

[30]

M. S. Islam, D. J. Driscoll, C. A. J. Fisher, and P. R. Slater, “Atomic-Scale Investigation of Defects, Dopants, and Lithium Transport in the LiFePO4 Olivine-Type Battery Material,” Chemistry of Materials 17, no. 20 (2005): 5085–5092.

[31]

H. Ji, J. Wang, J. Ma, H. M. Cheng, and G. Zhou, “Fundamentals, Status and Challenges of Direct Recycling Technologies for Lithium Ion Batteries,” Chemical Society Reviews 52, no. 23 (2023): 8194–8244.

[32]

C. Ouyang, S. Shi, Z. Wang, X. Huang, and L. Chen, “First-Principles Study of Li Ion Diffusion in LiFePO4,” Physical Review B 69, no. 10 (2004): 104303.

[33]

L. Hong, L. Li, Y. K. Chen-Wiegart, et al., “Two-Dimensional Lithium Diffusion Behavior and Probable Hybrid Phase Transformation Kinetics in Olivine Lithium Iron Phosphate,” Nature Communications 8, no. 1 (2017): 1194.

[34]

Z. Zeng, H. Lei, X. Lu, et al., “Li-Fe Anti-Sites Defects in LiFePO4: Mechanism, Characterization and Cathode-Regeneration Applications,” Energy Storage Materials 74 (2024): 103947.

[35]

R. Malik, D. Burch, M. Bazant, and G. Ceder, “Particle Size Dependence of the Ionic Diffusivity,” Nano Letters 10, no. 10 (2010): 4123–4127.

[36]

X. Lv, J. Lin, X. Sun, et al., “Direct Recycling of Spent LiFePO4 Cathodes Through Photocatalytic Correction of Anti-Site Defects,” Advanced Materials 37, no. 26 (2025): 2503398.

[37]

H. Zheng, L. Tan, L. Zhang, et al., “Correlation Between Lithium Deposition on Graphite Electrode and the Capacity Loss for LiFePO4/Graphite Cells,” Electrochimica Acta 173 (2015): 323–330.

[38]

Y. L. Han, H. Wang, H. F. Di, et al., “Determination of High-Temperature Float Charge Failure Mechanisms in Lithium-Ion Batteries by Quantifying Active Lithium Loss,” Carbon Energy 7, no. 7 (2025): e70002.

[39]

Y. Kim, Y. Kim, S. Yeo, et al., “Development of a Continuous Hydrogen Generator Fueled by Ammonia Borane for Portable Fuel Cell Applications,” Journal of Power Sources 229 (2013): 170–178.

[40]

J. Wu, R. A. Davies, M. S. Islam, and S. M. HailE, “Atomistic Study of Doped BaCeO3: Dopant Site-Selectivity and Cation Nonstoichiometry,” Chemistry of Materials 17, no. 4 (2005): 846–851.

[41]

L. Wei and C. Shifu, “Preparation and Characterization of p-n Heterojunction Photocatalyst Cu2O / In2O3 and Its Photocatalytic Activity under Visible and UV Light Irradiation,” Journal of the Electrochemical Society 157, no. 11 (2010): H1029.

[42]

X. Han, L. Lu, Y. Zheng, et al., “A Review on the Key Issues of the Lithium Ion Battery Degradation Among the Whole Life Cycle,” eTransportation 1 (2019): 100005.

[43]

Z. Ren, H. Li, Y. Wang, et al., “Green Recycling Assessment on Typical Spent Lithium-Ion Batteries (LIBs): A Multi-Objective Assessment,” Resources, Conservation And Recycling 206 (2024): 107648.

[44]

D. Wang, X. Wu, Z. Wang, and L. Chen, “Cracking Causing Cyclic Instability of LiFePO4 Cathode Material,” Journal of Power Sources 140, no. 1 (2005): 125–128.

[45]

A. K. Padhi, K. S. Nanjundaswamy, and J. B. Goodenough, “Phospho-Olivines as Positive-Electrode Materials for Rechargeable Lithium Batteries,” Journal of the Electrochemical Society 144, no. 4 (1997): 1188–1194.

[46]

D. Morgan, A. Van der Ven, and G. Ceder, “Li Conductivity in Lix MPO4 (M = Mn, Fe, Co, Ni) Olivine Materials,” Electrochemical and Solid-State Letters 7, no. 2 (2004): A30.

[47]

S. Kim, H. R. Shin, K. J. Kim, M. S. Park, and J. W. Lee, “Driving Inward Growth of Lithium Metal in Hollow Microcapsule Hosts by Heteroatom-Controlled Nucleation,” Carbon Energy 6, no. 8 (2024): e525.

[48]

D. Peng, X. Wang, S. Wang, et al., “Efficient Regeneration of Retired LiFePO4 Cathode by Combining Spontaneous and Electrically Driven Processes,” Green Chemistry 24, no. 11 (2022): 4544–4556.

[49]

H. Zhang, Y. Yang, D. Ren, L. Wang, and X. He, “Graphite as Anode Materials: Fundamental Mechanism, Recent Progress and Advances,” Energy Storage Materials 36 (2021): 147–170.

[50]

P. Verma, P. Maire, and P. Novák, “A Review of the Features and Analyses of the Solid Electrolyte Interphase in Li-Ion Batteries,” Electrochimica Acta 55, no. 22 (2010): 6332–6341.

[51]

D. Aurbach, E. Zinigrad, Y. Cohen, and T. Hanan, “A Short Review of Failure Mechanisms of Lithium Metal and Lithiated Graphite Anodes in Liquid Electrolyte Solutions,” Solid State Ionics 148, no. 3–4 (2002): 405–416.

[52]

M. Li, S. Yang, and B. Li, “Advances in Electrolyte-Anode Interface Engineering of Solid-State Lithium Metal Batteries,” Interdisciplinary Materials 3, no. 6 (2024): 805–834.

[53]

N. Zhu, Y. Yang, Y. Li, Y. Bai, J. Rong, and C. Wu, “Carbon-Based Interface Engineering and Architecture Design for High-Performance Lithium Metal Anodes,” Carbon Energy 6, no. 1 (2024): e423.

[54]

P. Ding, Z. Lin, X. Guo, et al., “Polymer Electrolytes and Interfaces in Solid-State Lithium Metal Batteries,” Materials Today 51 (2021): 449–474.

[55]

D. Ouyang, M. Chen, J. Liu, R. Wei, J. Weng, and J. Wang, “Investigation of A Commercial Lithium-Ion Battery Under Overcharge/Over-Discharge Failure Conditions,” RSC Advances 8, no. 58 (2018): 33414–33424.

[56]

M. Qin, Z. Zeng, S. Cheng, and J. Xie, “Challenges and Strategies of Formulating Low-Temperature Electrolytes in Lithium-Ion Battery,” Interdisciplinary Materials 2, no. 2 (2023): 308–336.

[57]

S. Grolleau, A. Delaille, H. Gualous, et al., “Calendar Aging Of Commercial Graphite/LiFePO4 Cell-Predicting Capacity Fade Under Time Dependent Storage Conditions,” Journal of Power Sources 255 (2014): 450–458.

[58]

M. Wang, k Liu, S. Dutta, et al., “Recycling of Lithium Iron Phosphate Batteries: Status, Technologies, Challenges, and Prospects,” Renewable and Sustainable Energy Reviews 163 (2022): 112515.

[59]

M. K. Tufail, P. Zhai, W. Khokar, M. Jia, N. Zhao, and X. Guo, “Evaluation of Solid Electrolytes: Development of Conventional and Interdisciplinary Approaches,” Interdisciplinary Materials 2, no. 4 (2023): 529–568.

[60]

L. Bertoluzzi, C. C. Boyd, N. Rolston, et al., “Mobile Ion Concentration Measurement and Open-Access Band Diagram Simulation Platform for Halide Perovskite Solar Cells,” Joule 4, no. 1 (2020): 109–127.

[61]

J. Tang, H. Qu, C. Sun, et al., “A Universal Solution for Direct Regeneration of Spent Lithium Iron Phosphate,” Advanced Materials 37, no. 14 (2025): 2420238.

[62]

C. Hogrefe, T. Waldmann, M. Hölzle, and M. Wohlfahrt-Mehrens, “Direct Observation of Internal Short Circuits by Lithium Dendrites in Cross-Sectional Lithium-Ion in Situ Full Cells,” Journal of Power Sources 556 (2023): 232391.

[63]

Y. Lin, H. Liu, C. Wang, et al., “Transient Atom-Economy Utilization of Residual Binder for Upcycling the Spent LiFePO4 Cathodes,” CCS Chemistry 7 (2025): e202506030.

[64]

K. Jia, J. Ma, J. Wang, et al., “Long-Life Regenerated LiFePO4 From Spent Cathode by Elevating the d-Band Center of Fe,” Advanced Materials 35, no. 5 (2023): 2208034.

[65]

X. Huang, X. He, C. Jiang, G. Tian, and Y. Liu, “Reaction Mechanisms on Solvothermal Synthesis of Nano LiFePO4 Crystals and Defect Analysis,” Industrial & Engineering Chemistry Research 56, no. 38 (2017): 10648–10657.

[66]

U. Boesenberg, F. Meirer, Y. Liu, et al., “Mesoscale Phase Distribution in Single Particles of LiFePO4 Following Lithium Deintercalation,” Chemistry of Materials 25, no. 9 (2013): 1664–1672.

[67]

N. Meethong, H. Y. S. Huang, S. A. Speakman, W. C. Carter, and Y. M. Chiang, “Strain Accommodation During Phase Transformations in Olivine-Based Cathodes as a Materials Selection Criterion for High-Power Rechargeable Batteries,” Advanced Functional Materials 17, no. 7 (2007): 1115–1123.

[68]

L. Li, Y. Bian, X. Zhang, et al., “A Green and Effective Room-Temperature Recycling Process of LiFePO4 Cathode Materials for Lithium-Ion Batteries,” Waste Management 85 (2019): 437–444.

[69]

Z. Liang, C. Cai, G. Peng, et al., “Hydrometallurgical Recovery of Spent Lithium Ion Batteries: Environmental Strategies and Sustainability Evaluation,” ACS Sustainable Chemistry & Engineering 9, no. 17 (2021): 5750–5767.

[70]

P. Yadav, C. J. Jie, S. Tan, and M. Srinivasan, “Recycling of Cathode From Spent Lithium Iron Phosphate Batteries,” Journal of Hazardous Materials 399 (2020): 123068.

[71]

J. J. Roy, S. Rarotra, V. Krikstolaityte, et al., “Green Recycling Methods to Treat Lithium-Ion Batteries E-Waste: A Circular Approach to Sustainability,” Advanced Materials 34, no. 25 (2022): 2103346.

[72]

Y. Yang, E. G. Okonkwo, G. Huang, S. Xu, W. Sun, and Y. He, “On the Sustainability of Lithium Ion Battery Industry-A Review and Perspective,” Energy Storage Materials 36 (2021): 186–212.

[73]

T. Zhao, W. Li, M. Traversy, et al., “A Review on the Recycling of Spent Lithium Iron Phosphate Batteries,” Journal of Environmental Management 351 (2024): 119670.

[74]

Y. Xu, B. Zhang, Z. Ge, et al., “Advances and Perspectives Towards Spent LiFePO4 Battery Recycling,” Journal of Cleaner Production 434 (2024): 140077.

[75]

M. Joulié, R. Laucournet, and E. Billy, “Hydrometallurgical Process for the Recovery of High Value Metals From Spent Lithium Nickel Cobalt Aluminum Oxide Based Lithium-Ion Batteries,” Journal of Power Sources 247 (2014): 551–555.

[76]

Y. Yao, M. Zhu, Z. Zhao, B. Tong, Y. Fan, and Z. Hua, “Hydrometallurgical Processes for Recycling Spent Lithium-Ion Batteries: A Critical Review,” ACS Sustainable Chemistry & Engineering 6, no. 11 (2018): 13611–13627.

[77]

J. Cong, S. Luo, Q. Sun, et al., “Study on Deep Synergistic Leaching Mechanism of Spent Lithium Iron Phosphate Under the H2SO4─H2O2 System and Precise Chemical Precipitation Recovery Strategy of Lithium Carbonate,” Separation and Purification Technology 363 (2025): 132326.

[78]

X. Zhou, W. Yang, X. Liu, et al., “One-Step Selective Separation and Efficient Recovery of Valuable Metals From Mixed Spent Lithium Batteries in the Phosphoric Acid System,” Waste Management 155 (2023): 53–64.

[79]

J. Kumar, X. Shen, B. Li, H. Liu, and J. Zhao, “Selective Recovery of Li and FePO4 From Spent LiFePO4 Cathode Scraps by Organic Acids and The Properties of the Regenerated LiFePO4,” Waste Management 113 (2020): 32–40.

[80]

D. F. Wang, M. Chen, J. J. Zhao, et al., “Revealing Role of Oxidation in Recycling Spent Lithium Iron Phosphate Through Acid Leaching,” Rare Metals 44, no. 3 (2025): 2059–2070.

[81]

Y. Zhang, B. Wang, F. Wang, et al., “A Green Recyclable Process for Selective Recovery of Li and Fe From Spent Lithium Iron Phosphate Batteries by Synergistic Effect of Deep Eutectic Solvent and Oxygen,” Separation and Purification Technology 354 (2025): 128764.

[82]

X. Li, M. Benstead, N. Peeters, and K. Binnemans, “Recycling of Metals From LiFePO4 Battery Cathode Material by Using Ionic Liquid Based-Aqueous Biphasic Systems,” RSC Advances 14, no. 13 (2024): 9262–9272.

[83]

W. Gao, X. Zhang, X. Zheng, et al., “Lithium Carbonate Recovery From Cathode Scrap of Spent Lithium-Ion Battery: A Closed-Loop Process,” Environmental Science & Technology 51, no. 3 (2017): 1662–1669.

[84]

Y. Yang, X. Meng, H. Cao, et al., “Selective Recovery of Lithium From Spent Lithium Iron Phosphate Batteries: A Sustainable Process,” Green Chemistry 20, no. 13 (2018): 3121–3133.

[85]

Q. Zeng, K. Hu, W. Hu, et al., “Suppressing the Coordination of Ferric Ions for Efficient Recycling of Spent Lithium Iron Phosphate,” Journal of Environmental Chemical Engineering 13, no. 3 (2025): 117060.

[86]

E. Colacino, V. Isoni, D. Crawford, and F. García, “Upscaling Mechanochemistry: Challenges and Opportunities for Sustainable Industry,” Trends in Chemistry 3, no. 5 (2021): 335–339.

[87]

J. Neumann, M. Petranikova, M. Meeus, et al., “Recycling of Lithium-Ion Batteries-Current State of the Art, Circular Economy, and Next Generation Recycling,” Advanced Energy Materials 12, no. 17 (2022): 2102917.

[88]

L. Takacs, “The Historical Development of Mechanochemistry,” Chemical Society Reviews 42, no. 18 (2013): 7649–7659.

[89]

Q. Zhang, E. Fan, J. Lin, et al., “Acid-Free Mechanochemical Process to Enhance the Selective Recycling of Spent LiFePO4 Batteries,” Journal of Hazardous Materials 443 (2023): 130160.

[90]

Y. Jiang, X. Chen, S. Yan, Y. Ou, and T. Zhou, “Mechanochemistry-Induced Recycling of Spent Lithium-Ion Batteries for Synergistic Treatment of Mixed Cathode Powders,” Green Chemistry 24, no. 15 (2022): 5987–5997.

[91]

Y. Hua, Z. Xu, B. Zhao, and Z. Zhang, “Electric Potential-Determined Redox Intermediates for Effective Recycling of Spent Lithium-Ion Batteries,” Green Chemistry 24, no. 9 (2022): 3723–3735.

[92]

X. Ren, X. Hu, B. Zhang, et al., “Dual Contribution of Recyclable Oxidants and Generated Superoxide Anion (O2−) for the Selective Recycling of Spent LiFePO4 Batteries,” Separation and Purification Technology 365 (2025): 132685.

[93]

J. Du, J. Qing, K. Fang, et al., “Efficient Lithium Recovery From Spent LiFePO4 Cathodes via Alkaline Pressure Leaching,” Separation and Purification Technology 378 (2025): 134700.

[94]

K. Liu, S. Yang, F. Lai, et al., “Application of H4P2O7 as Leaching Acid in One-Step Selective Recovery for Metals From Spent LiFePO4 Batteries,” Ionics 27, no. 12 (2021): 5127–5135.

[95]

X. Qiu, B. Zhang, Y. Xu, et al., “Enabling the Sustainable Recycling of LiFePO4 From Spent Lithium-Ion Batteries,” Green Chemistry 24, no. 6 (2022): 2506–2515.

[96]

Y. Fan, Y. Kong, P. Jiang, et al., “Development and Challenges of Deep Eutectic Solvents for Cathode Recycling of End-of-Life Lithium-Ion Batteries,” Chemical Engineering Journal 463 (2023): 142278.

[97]

K. Zhou, X. Dai, P. Li, et al., “Recent Advances in Deep Eutectic Solvents for Next-Generation Lithium Batteries: Safer and Greener,” Progress in Materials Science 146 (2024): 101338.

[98]

C. Wang, R. Tao, P. Xing, et al., “State-of-the-Art Review on Liberation of Cathode Material in Pretreatment Recycling of Spent Lithium-Ion Battery,” Resources, Conservation And Recycling 218 (2025): 108257.

[99]

J. Zou, R. Zhang, Y. Huang, et al., “High Efficiency Leaching of Black Powder From Spent Lithium-Ion Battery by Ternary Deep Eutectic Solvent and Recovery of Metals by Precipitation and Electrodeposition,” Separation and Purification Technology 364 (2025): 132438.

[100]

M. Chen, X. Ma, B. Chen, et al., “Recycling End-of-Life Electric Vehicle Lithium-Ion Batteries,” Joule 3, no. 11 (2019): 2622–2646.

[101]

H. Zhou, Z. Luo, S. Wang, X. Ma, and Z. Cao, “A Mild Closed-Loop Process for Lithium–Iron Separation and Cathode Materials Regeneration From Spent LiFePO4 Batteries,” Separation and Purification Technology 315 (2023): 123742.

[102]

X. Chen, S. Li, Y. Wang, et al., “Recycling of LiFePO4 Cathode Materials From Spent Lithium-Ion Batteries Through Ultrasound-Assisted Fenton Reaction and Lithium Compensation,” Waste Management 136 (2021): 67–75.

[103]

H. Gao, D. Tran, and Z. Chen, “Seeking Direct Cathode Regeneration for More Efficient Lithium-Ion Battery Recycling,” Current Opinion In Electrochemistry 31 (2022): 100875.

[104]

Y. Wang, Y. Yang, J. Zhang, Y. Chen, and C. Wang, “Residue Carbon Removal for the High-Quality and Sustainable Direct Regeneration of Spent LiFePO4 Materials,” Applied Surface Science 689 (2025): 162512.

[105]

H. Xiao, C. Zeng, F. Fan, et al., “A One-Step Low-Temperature Closed-Loop Eutectic Salt Strategy for Direct Regeneration of Severely Degraded LiFePO4,” Energy Storage Materials 77 (2025): 104183.

[106]

G. Ji, J. Wang, Z. Liang, et al., “Direct Regeneration of Degraded Lithium-Ion Battery Cathodes With a Multifunctional Organic Lithium Salt,” Nature Communications 14, no. 1 (2023): 584.

[107]

D. Tang, G. Ji, J. Wang, et al., “A Multifunctional Amino Acid Enables Direct Recycling of Spent LiFePO4 Cathode Material,” Advanced Materials 36, no. 5 (2024): 2309722.

[108]

Y. Yang, J. Zhang, H. Zhang, Y. Wang, Y. Chen, and C. Wang, “Simultaneous Anodic De-Lithiation/Cathodic Lithium-Embedded Regeneration Method for Recycling of Spent LiFePO4 Battery,” Energy Storage Materials 65 (2024): 103081.

[109]

S. Zhou, J. Du, X. Xiong, et al., “Direct Recovery of Scrapped LiFePO4 by a Green and Low-Cost Electrochemical Re-Lithiation Method,” Green Chemistry 24, no. 16 (2022): 6278–6286.

[110]

Y. Lin, T. Wang, C. Gao, et al., “Direct and Low-Temperature Regeneration of Degraded LiFePO4 Cathodes at Ambient Conditions Using Green and Sustainable Deep Eutectic Solvent,” Advanced Science 12, no. 8 (2025): 2504683.

[111]

P. Xu, Q. Dai, H. Gao, et al., “Efficient Direct Recycling of Lithium-Ion Battery Cathodes by Targeted Healing,” Joule 4, no. 12 (2020): 2609–2626.

[112]

J. Sun, Z. Jiang, P. Jia, et al., “A Sustainable Revival Process for Defective LiFePO4 Cathodes Through the Synergy of Defect-Targeted Healing and In-Situ Construction of 3D-Interconnected Porous Carbon Networks,” Waste Management 158 (2023): 125–135.

[113]

C. Cheng, X. Cao, Z. Xing, and S. Tang, “Direct Regeneration of Severely Damaged Spent LiFePO4 Cathodes,” Journal of Materials Science & Technology 241, no. 10 (2026): 262–269.

[114]

Q. Jing, J. Zhang, Y. Liu, et al., “Direct Regeneration of Spent LiFePO4 Cathode Material by a Green and Efficient One-Step Hydrothermal Method,” ACS Sustainable Chemistry & Engineering 48, no. 48 (2020): 17622–17628.

[115]

K. Y. Park, I. Park, H. Kim, et al., “Anti-Site Reordering in LiFePO4: Defect Annihilation on Charge Carrier Injection,” Chemistry of Materials 26, no. 18 (2014): 5345–5351.

[116]

J. Yan, J. Qian, Y. Li, L. Li, F. Wu, and R. Chen, “Toward Sustainable Lithium Iron Phosphate in Lithium-Ion Batteries: Regeneration Strategies and Their Challenges,” Advanced Functional Materials 34, no. 44 (2024): 2405055.

[117]

T. Yang, D. Luo, A. Yu, and Z. Chen, “Enabling Future Closed-Loop Recycling of Spent Lithium-Ion Batteries: Direct Cathode Regeneration,” Advanced Materials 35, no. 36 (2023): 2203218.

[118]

U. Nisar, N. Muralidharan, R. Essehli, R. Amin, and I. Belharouak, “Valuation of Surface Coatings in High-Energy Density Lithium-Ion Battery Cathode Materials,” Energy Storage Materials 38 (2021): 309–328.

[119]

C. Feng, Y. Cao, L. Song, et al., “Direct Regeneration of Industrial LiFePO4 Black Mass Through a Glycerol-Enabled Granule Reconstruction Strategy,” Angewandte Chemie International Edition 64, no. 6 (2025): e202418198.

[120]

Z. Jiang, Z. Xu, L. Li, et al., “Design Principles for Efficient Hydrothermal Relithiation of Spent Lithium Iron Phosphate,” ACS Applied Materials & Interfaces 17, no. 3 (2025): 4875–4883.

[121]

Y. Yang, Z. Liu, J. Zhang, Y. Chen, and C. Wang, “Economical and Low-Carbon Regeneration of Spent LiFePO4 Materials by Hydrothermal Relithiation,” Journal of Alloys and Compounds 947 (2023): 169660.

[122]

Z. Chi, J. Li, L. Wang, et al., “Direct Regeneration Method of Spent LiNi1/3Co1/3 Mn1/3O2 Cathode Materials via Surface Lithium Residues,” Green Chemistry 23, no. 22 (2021): 9099–9108.

[123]

S. Yang, H. Luo, Y. Li, et al., “Lithium Resurrection: Synergistic Thermal-Decomposition and Electric-Drive Strategy Enabling Inactive Lithium Fully Recycling,” Journal of Energy Chemistry 102 (2025): 842–851.

[124]

P. Xu, D. H. S. Tan, B. Jiao, H. Gao, X. Yu, and Z. Chen, “A Materials Perspective on Direct Recycling of Lithium-Ion Batteries: Principles, Challenges and Opportunities,” Advanced Functional Materials 33, no. 14 (2023): 2213168.

[125]

M. Fan, Q. Meng, X. Chang, et al., “In Situ Electrochemical Regeneration of Degraded LiFePO4 Electrode With Functionalized Prelithiation Separator,” Advanced Energy Materials 12, no. 18 (2022): 2103630.

[126]

T. El Achkar, H. Greige-Gerges, and S. Fourmentin, “Basics and Properties of Deep Eutectic Solvents: A Review,” Environmental Chemistry Letters 19, no. 4 (2021): 3397–3408.

[127]

L. Chen, Y. Chao, X. Li, et al., “Engineering a Tandem Leaching System for the Highly Selective Recycling of Valuable Metals From Spent Li-Ion Batteries,” Green Chemistry 23, no. 5 (2021): 2177–2184.

[128]

M. K. Tran, M. T. F. Rodrigues, K. Kato, G. Babu, and P. M. Ajayan, “Deep Eutectic Solvents for Cathode Recycling of Li-Ion Batteries,” Nature Energy 4 (2019): 339–345.

[129]

S. Wang, Z. Zhang, Z. Lu, and Z. Xu, “A Novel Method for Screening Deep Eutectic Solvent to Recycle the Cathode of Li-Ion Batteries,” Green Chemistry 22, no. 14 (2020): 4473–4482.

[130]

H. Pu, X. Zhu, Z. Zou, and C. Jiang, “Direct Regeneration of Spent LiFePO4 Cathode via a Mild Deep Eutectic Solvent Process,” Journal of Energy Storage 111 (2025): 115421.

[131]

T. Yingnakorn, J. Hartley, J. S. Terreblanche, C. Lei, W. M. Dose, and A. P. Abbott, “Direct Re-Lithiation Strategy for Spent Lithium Iron Phosphate Battery in Li-Based Eutectic Using Organic Reducing Agents,” RSC Sustainability 1, no. 9 (2023): 2341–2349.

[132]

J. Shen, M. Zhou, W. Liu, et al., “Advanced Direct Recycling Technology Enables a Second Life of Spent Lithium-Ion Battery,” Energy Storage Materials 74 (2024): 103964.

[133]

A. Khan, H. A. Rashid, P. K. Roy, et al., “Challenges and the Way to Improve Lithium-Ion Battery Technology for Next-Generation Energy Storage,” Energy & Environmental Materials 8, no. 6 (2025): e70088.

[134]

L. Song, C. Qi, S. Wang, et al., “Direct Regeneration of Waste LiFePO4 Cathode Materials With a Solid-Phase Method Promoted by Activated CNTs,” Waste Management 157 (2023): 141–148.

[135]

X. Xu, Z. Guo, D. Zhu, J. Pan, C. Yang, and S. Li, “Green Pathways to LiFePO4 Cathodes: Exploring Sustainable Iron Sources and Recycling Strategies,” Chemical Engineering Journal 521 (2025): 166798.

[136]

Z. Zeng, P. Xu, J. Li, et al., “Large-Scale and Homogenized Strategies of Spent LiFePO4 Recycling: Reconstruction of Targeted Lattice,” Advanced Functional Materials 34, no. 6 (2024): 2308671.

[137]

S. Lei, W. Sun, and Y. Yang, “Comprehensive Technology for Recycling and Regenerating Materials From Spent Lithium Iron Phosphate Battery,” Environmental Science & Technology 58, no. 8 (2024): 3609–3628.

[138]

L. Wang, H. Chen, Y. Zhang, J. Liu, and L. Peng, “Research Progress in Strategies for Enhancing the Conductivity and Conductive Mechanism of LiFePO4 Cathode Materials,” Molecules 29, no. 22 (2024): 5250.

[139]

M. Xiao, X. Fu, M. Chen, et al., “Constructing a Homogeneous Medium Layer to Promote the Direct Regeneration of Spent Lithium Iron Phosphate,” ACS Applied Materials & Interfaces 17, no. 8 (2025): 12199–12207.

[140]

Y. Li, C. Li, F. Hu, et al., “Direct Regeneration of Spent LiFePO4 Cathode Materials Through Li+ Supplementation and Sm Doping,” Nano Research Energy 4, no. 4 (2025): e9120190.

[141]

G. Ji, D. Tang, J. Wang, et al., “Sustainable Upcycling of Mixed Spent Cathodes to a High-Voltage Polyanionic Cathode Material,” Nature Communications 15, no. 4 (2024): 4086.

[142]

S. Ji, Y. Tan, J. Wang, et al., “Defect-Engineered Gradient Reconstruction for the Upcycling of Spent LiFePO4 to Generate High-Value LiFe1−xMnxPO4/C Cathodes,” Journal of Energy Chemistry 122 (2025): 306–316.

[143]

X. T. Wang, Z. Y. Gu, J. M. Cao, et al., “Dual-Loop Upcycling of Spent LiFePO4: Defect Inheritance Enables Durable and Fast-Charging Sodium-Ion Batteries,” National Science Review 12, no. 9 (2025): nwaf321.

[144]

X. H. Yue and F. S. Zhang, “Recycling Spent LiFePO4 Battery for Fabricating Visible-Light Photocatalyst With Adsorption-Photocatalytic Synergistic Performance and Simultaneous Recovery of Lithium and Phosphorus,” Chemical Engineering Journal 450, no. 4 (2022): 138388.

[145]

M. Zhang, M. Lv, D. Zhang, et al., “Enhanced Electrochemical Properties of NCM811 Cathode Material Due to Synergistic Modification With Sm as Doping and Coating Agent,” Journal of Alloys and Compounds 909 (2022): 164712.

[146]

Z. Zeng, H. Lei, J. Li, et al., “Regenerated Spent LiFePO4 With Tailored Residual Copper-Atoms Towards Improved Energy-Storage Capacity and Reversibility,” Chemical Engineering Journal 499 (2024): 155616.

[147]

D. Wang, H. Li, S. Shi, X. Huang, and L. Chen, “Improving the Rate Performance of LiFePO4 by Fe-Site Doping,” Electrochimica Acta 50, no. 14 (2005): 2955–2958.

[148]

Y. Liu, J. Bai, R. Shi, et al., “Direct Recycling of Degraded LiFePO4 Cathode Material via Natural Electron Donors Healing and Targeted Surface Reconstruction,” Advanced Materials 38, no. 1 (2025): e11246.

[149]

Y. F. Meng, H. J. Liang, C. D. Zhao, et al., “Concurrent Recycling Chemistry for Cathode/Anode in Spent Graphite/LiFePO4 Batteries: Designing A Unique Cation/Anion-Co-Workable Dual-Ion Battery,” Journal of Energy Chemistry 64 (2022): 166–171.

[150]

V. Etacheri, R. Marom, R. Elazari, G. Salitra, and D. Aurbach, “Challenges in the Development of Advanced Li-Ion Batteries: A Review,” Energy & Environmental Science 4, no. 9 (2011): 3243–3262.

[151]

T. J. Diethrich, S. Gnewuch, K. G. Dold, K. M. Taddei, and E. E. Rodriguez, “Tuning Magnetic Symmetry and Properties in the Olivine Series LiFe1−xMnxPO4 Through Selective Delithiation,” Chemistry of Materials 34, no. 11 (2022): 5039–5053.

[152]

D. B. Ravnsbæk, K. Xiang, W. Xing, et al., “Extended Solid Solutions and Coherent Transformations in Nanoscale Olivine Cathodes,” Nano Letters 14, no. 3 (2014): 1484–1491.

[153]

S. Lei, J. Li, W. Sun, P. Ge, and Y. Yang, “Upcycling of Low-Value Cathode Materials From Spent Lithium-Ion Battery to High-Voltage Cathode With Ultrahigh Rate Capability and Reversibility,” Advanced Energy Materials 15, no. 21 (2025): 2406064.

[154]

C. Cheng, W. Mao, X. Cao, K. Xu, and S. Tang, “Sustainable Transformation of Spent Lifepo4 Cathodes into High-Voltage Olivine LiMnxFe1-xPO4 via Solvothermal Upcycling Strategy for Next-Generation Cathode Material,” Energy Storage Materials 80 (2025): 104402.

[155]

J. Ren, H. Zhu, Y. Fang, et al., “Typical Cathode Materials for Lithium-Ion and Sodium-Ion Batteries: From Structural Design to Performance Optimization,” Carbon Neutralization 2, no. 3 (2023): 339–377.

[156]

N. Wu, J. Shen, X. Zhou, et al., “Constructing Iron Vacancies in Thiospinel FeIn2S4 to Modulate Fe d-Band Center and Accelerate Sodiation Kinetics Enabling High-Rate and Durable Sodium Storage,” Advanced Energy Materials 15, no. 19 (2025): 2405729.

[157]

Y. Liu, X. Rong, R. Bai, et al., “Identifying the Intrinsic Anti-Site Defect in Manganese-Rich Nasicon-Type Cathodes,” Nature Energy 8 (2023): 1088–1096.

[158]

W. Zou, J. Li, R. Wang, et al., “Hydroxylamine Mediated Fenton-Like Interfacial Reaction Dynamics on Sea Urchin-Like Catalyst Derived From Spent LiFePO4 Battery,” Journal of Hazardous Materials 431 (2022): 128590.

[159]

J. M. F. Lucas, P. R. Prezas, S. Soreto Teixeira, et al., “Tuning the Magnetic and Electric Behavior of Lithium Ferrite Using an Eco-Friendly Pectin Sol-Gel Route,” Journal of Sol-Gel Science and Technology 98 (2021): 580–592.

[160]

C. Wang, X. Kong, L. Wang, et al., “Mechanistically Engineered Heterojunctionfrom Spent LFP for Efficient Oxygen Evolution Electrocatalysis,” Angewandte Chemie International Edition 64, no. 43 (2025): e202516122.

[161]

X. Zhang, T. Liu, F. Zhao, N. Zhang, and Y. Wang, “In-Situ-Formed Cd and Ag2S Decorated Cds Photocatalyst With Boosted Charge Carrier Spatial Separation for Enhancing Uv-Vis-Nir Photocatalytic Hydrogen Evolution,” Applied Catalysis, B: Environmental 298 (2021): 120620.

[162]

Z. Yang, X. Xu, X. Liang, et al., “MIL-53(Fe)-Graphene Nanocomposites: Efficient Visible-Light Photocatalysts for the Selective Oxidation of Alcohols,” Applied Catalysis, B: Environmental 198 (2016): 112–123.

[163]

Argonne National Laboratory (ANL). EverBatt: A Closed-Loop Battery Recycling Cost and Environmental Impacts Model, accessed, April 2019, https://publications.anl.gov/anlpubs/2019/07/153050.pdf.

[164]

J. Liu, Z. Liu, Z. Xiao, et al., “Iodine-Mediated Redox Strategy for Sustainable Lithium Extraction From Spent LiFePO4 Cathodes,” Advanced Materials 37, no. 26 (2025): 2503450.

[165]

G. Wang, T. Fearn, T. Wang, and K. L. Choy, “Machine-Learning Approach for Predicting the Discharging Capacities of Doped Lithium Nickel-Cobalt-Manganese Cathode Materials in Li-Ion Batteries,” ACS Central Science 7, no. 9 (2021): 1551–1560.

[166]

M. Alyoubi, I. Ali, and A. M. Abdelkader, “Optimising the Regeneration Process of Spent Lithium-Cobalt Oxide Cathode Through Performance Analysis Model,” Journal of Energy Storage 110 (2025): 115132.

[167]

J. Tang, H. Qu, C. Sun, et al., “A Universal Solution for Direct Regeneration of Spent Lithium Iron Phosphate,” Advanced Materials 37, no. 14 (2025): 2420238.

Rights & permissions

2026 The Author(s). Carbon Energy published by Wenzhou University and John Wiley & Sons Australia, Ltd.

PDF (4692KB)

0

Accesses

0

Citation

Detail

Sections
Recommended

/

〈 〉