Abstract
Numerous LiFePO4 batteries have been retired with the increasing development of electric vehicles and hybrid electric vehicles; meanwhile, the spent LiFePO4 batteries will lead to an environment contamination and the resources squander if they do not recycled reasonable. In this paper, a green process is developed for the recovery of spent LiFePO4 cathode materials with a certain amount of impurities: the Li+ and small part of PO43− have been selectively leached into solution while iron and the major PO43− as a precipitate via H2SO4 selective leaching after oxidative activation at 600 °C under air atmosphere. The process is dissimilar from the previous process of using excess H2O2 or excess mineral acid to leach the elements into solution. The leaching rates of Li, Fe, and P are 98.46%, 0.010%, and 26.59%, respectively, under the optimized conditions. Around 85.56% Li and 99.58% Fe were recovered in the form of Li3PO4 and FePO4 under the experimental conditions. This research demonstrates an effective process for the recovering of spent LiFePO4 batteries in a simple, efficient, and lucrative way, which gives it a feasible industrially application.
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References
Ansean D, Gonzalez M, Viera JC et al (2014) Evaluation of LiFePO4 batteries for electric vehicle applications. IEEE Trans Ind Appl 51(2):1855
Thackeray MM, Wolverton C, Isaacs ED (2012) Electrical energy storage for transportation-approaching the limits of, and going beyond, lithium-ion batteries. Energy Environ Sci 5(7):7854–7863
Goodenough JB, Park KS (2013) The Li-ion rechargeable battery: a perspective. J Am Chem Soc 135(4):1167–1176
Wang LH, Li J, Zhou HM et al (2018) Regeneration cathode material mixture from spent lithium iron phosphate batteries. J Mater Sci Mater Electron 29(11):1–8
Kim T, Park J, Chang SK, Choi S, Ryu JH, Song HK (2012) The current move of lithium ion batteries towards the next phase. Adv Energy Mater 2(7):860–872
Yoo HD, Markevich E, Salitra G, Sharon D, Aurbach D (2014) On the challenge of developing advanced technologies for electrochemical energy storage and conversion. Mater Today 17(3):110–121
Choi JW, Aurbach D (2016) Promise and reality of post-lithium-ion batteries with high energy densities. Nat Rev Mater 1(4):16013
Hu J, Zhang J, Li H, Chen Y, Wang C (2017) A promising approach for the recovery of high value-added metals from spent lithium-ion batteries. J Power Sources 351:192–199
Sun Z, Cao H, Xiao Y et al (2017) Toward sustainability for recovery of critical metals from electronic waste: the hydrochemistry processes. ACS Sustain Chem Eng 5(1):21–40
Kim DS, Sohn JS, Lee CK, Lee JH, Han KS, Lee YI (2004) Simultaneous separation and renovation of lithium cobalt oxide from the cathode of spent lithium ion rechargeable batteries. J Power Sources 132(1–2):145–149
Träge r T, Friedrich B, Weyhe R (2015) Recovery concept of value metals from automotive lithium-ion batteries. Chem Ing Tech 87(11):1550–1557
Xin Y, Guo X, Chen S, Wang J, Wu F, Xin B (2016) Bioleaching of valuable metals Li, Co, Ni and Mn from spent electric vehicle Li-ion batteries for the purpose of recovery. J Clean Prod 116:249–258
Bahaloo-Horeh N, Mousavi SM (2017) Enhanced recovery of valuable metals from spent lithium-ion batteries through optimization of organic acids produced by Aspergillus niger. Waste Manag 60:666–679
Chen J, Li Q, Song J, Song D, Zhang L, Shi X (2016) Environmentally friendly recycling and effective repairing of cathode powders from spent LiFePO4 batteries. Green Chem 18(8):2500–2506
Song X, Hu T, Liang C, Long H, Zhou L, Song W, You L, Wu Z, Liu J (2017) Direct regeneration of cathode materials from spent lithium iron phosphate batteries using a solid phase sintering method. RSC Adv 7(8):4783–4790
Kim HS, Shin EJ (2013) Re-synthesis and electrochemical characteristics of LiFePO4 cathode materials recycled from scrap electrodes. Bull Kor Chem Soc 34(3):851–855
Bian D, Sun Y, Li S, Tian Y, Yang Z, Fan X, Zhang W (2016) A novel process to recycle spent LiFePO4 for synthesizing LiFePO4/C hierarchical microflowers. Electrochim Acta 190:134–140
Zheng R, Zhao L, Wang W, Liu Y, Ma Q, Mu D, Li R, Dai C (2016) Optimized Li and Fe recovery from spent lithium-ion batteries via solution-precipitation method. RSC Adv 6(49):43613–43625
Shin EJ, Kim S, Noh JK, Byun D, Chung KY, Kim HS, Cho BW (2015) A green recycling process designed for LiFePO4 cathode materials for Li-ion batteries. J Mater Chem A 3(21):11493–11502
Nayaka GP, Manjanna J, Pai KV, Vadavi R, Keny SJ, Tripathi VS (2015) Recovery of valuable metal ions from the spent lithium ion battery using aqueous mixture of mild organic acids as alternative to mineral acids. Hydrometallurgy 151:73–77
Gao W, Zhang X, Zheng X, Lin X, Cao H, Zhang Y, Sun Z (2017) Lithium carbonate recovery from cathode scrap of spent lithium-ion battery: a closed-loop process. Environ Sci Technol 51(3):1662–1669
Cai G, Fung KY, Ng KM, Wibowo C (2014) Process development for the recycle of spent lithium ion batteries by chemical precipitation. Ind Eng Chem Res 53(47):18245–18259
Han XY, JQ X (2017) Recover of iron and lithium from spent lithium iron phosphate batteries by precipitation process. GD Chem Ind 44(4):12–16
Hwang SO, Chae BM, Kim DH, Park KS, Go AR, Lee SW (2017) Recovery of nickel from waste lithium ion secondary battery and fabrication of nickel nanopowder. Key Eng Mater 733:22–26
He LP, Sun SY, Mu YY, Song XF, Yu JG (2017) Recovery of lithium, nickel, cobalt, and manganese from spent lithium-ion batteries using L-tartaric acid as a leachant. ACS Sustain Chem Eng 5:714–721
Zou H, Gratz E, Apelian D, Wang Y (2013) A novel method to recycle mixed cathode materials for lithium ion batteries. Green Chem 15(5):1183–1191
Pranolo Y, Zhang W, Cheng CY (2010) Recovery of metals from spent lithium-ion battery leach solutions with a mixed solvent extractant system. Hydrometallurgy 102(1–4):37–42
Chen L, Tang X, Zhang Y, Li L, Zeng Z, Zhang Y (2011) Process for the recovery of cobalt oxalate from spent lithium-ion batteries. Hydrometallurgy 108(1):80–86
Yang Y, Zheng X, Zhao C et al (2017) A closed loop process for selective metal recovery from spent lithium iron phosphate batteries through mechanochemical activation. ACS Sustain Chem Eng 5(11):9972–9980
Yang Y, Zheng X, Cao H et al (2018) Selective recovery of lithium from spent lithium iron phosphate batteries: a sustainable process. Green Chem 20(13):1–13
Li L, Lu J, Zhai L et al (2018) A facile recovery process for cathodes from spent lithium iron phosphate batteries by using oxalic acid. CSEE JPES 4(2):219–225
Li H, Xing S, Liu Y, Li F, Guo H, Kuang G (2017) Recovery of lithium, iron, and phosphorus from spent LiFePO4 batteries using stoichiometric sulfuric acid leaching system. ACS Sustain Chem Eng 5(9):8017–8024
Zhu SM, Zhou HS, Miyoshi T et al (2005) Self-assembly of the mesoporous electrode material Li3Fe2(PO4)3 using a cationic surfactant as the template. Cheminform 36(10):2012–2017
Xiao C, Zeng L (2018) Thermodynamic study on recovery of lithium using phosphate precipitation method. Hydrometallurgy 178:283–286
Funding
This work was supported by the Natural Science Foundation of China (Grant Number 51371198) and the Natural Science Foundation of Hunan provincial (Grant Number 2017JJ2168).
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Tao, S., Li, J., Wang, L. et al. A method for recovering Li3PO4 from spent lithium iron phosphate cathode material through high-temperature activation. Ionics 25, 5643–5653 (2019). https://doi.org/10.1007/s11581-019-03070-w
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DOI: https://doi.org/10.1007/s11581-019-03070-w