Browse > Article
http://dx.doi.org/10.4491/eer.2018.392

Recycling of end-of-life LiNixCoyMnzO2 batteries for rare metals recovery  

Sattar, Rabia (Mineral and Material Chemistry Lab, Department of Chemistry, University of Agriculture Faisalabad)
Ilyas, Sadia (Mineral and Material Chemistry Lab, Department of Chemistry, University of Agriculture Faisalabad)
Kousar, Sidra (Mineral and Material Chemistry Lab, Department of Chemistry, University of Agriculture Faisalabad)
Khalid, Amaila (Mineral and Material Chemistry Lab, Department of Chemistry, University of Agriculture Faisalabad)
Sajid, Munazzah (Mineral and Material Chemistry Lab, Department of Chemistry, University of Agriculture Faisalabad)
Bukhari, Sania Iqbal (Mineral and Material Chemistry Lab, Department of Chemistry, University of Agriculture Faisalabad)
Publication Information
Abstract
An investigation of rare metals recovery from LiNixCoyMnzO2 cathode material of the end-of-life lithium-ion batteries is presented. To determine the influence of reductant on the leach process, the cathode material (containing Li 7.6%, Co 20.4%, Mn 19.4%, and Ni 19.3%) was leached in H2SO4 solutions either with or without H2O2. The optimal process parameters with respect to acid concentration, addition dosage of H2O2, temperature, and the leaching time were found to be 2.0 M H2SO4, 4 vol.% H2O2, 70℃, and 150 min, respectively. The yield of metal values in the leach liquor was > 99%. The leach liquor was subsequently treated by precipitation techniques to recover nickel as Ni(C4H7N2O2)2 and lithium as Li2CO3 with stoichiometric ratios of 2:1 and 1.2:1 of dimethylglyoxime:Ni and Na2CO3:Li, respectively. Cobalt was recovered by solvent extraction following a 3-stage process using Na-Cyanex 272 at pHeq ~5.0 with an organic-to-aqueous phase ratio (O/A) of 2/3. The loaded organic phase was stripped with 2.0 M H2SO4 at an O/A ratio of 8/1 to yield a solution of 114 g/L CoSO4; finally recovered CoSO4.xH2O by crystallization. The process economics were analyzed and found to be viable with a margin of $476 per ton of the cathode material.
Keywords
Lithium-ion battery; Precipitation; Rare metals; Recycling; Solvent extraction;
Citations & Related Records
연도 인용수 순위
  • Reference
1 Srivastava RR, Kim MS, Lee JC, Jha MK, Kim BS. Resource recycling of superalloys and hydrometallurgical challenges. J. Mater. Sci. 2014;49:4671-4686.   DOI
2 Choubey PK, Chung KS, Kim MS, Lee JC, Srivastava RR. Advance review on the exploitation of the prominent energy-storage element: Lithium. Part II: From sea water and spent lithium ion batteries (LIBs). Miner. Eng. 2017;110:104-121.   DOI
3 Li T, Liu H, Shi P, Zhang Q. Recent progress in carbon/lithium metal composite anode for safe lithium metal batteries. Rare Met. 2018;37:449-458.   DOI
4 Ilyas S, Kim MS, Lee JC. Integration of microbial and chemical processing for a sustainable metallurgy. J. Chem. Technol. Biotechnol. 2018;93:320-332.   DOI
5 Zhang W, Xu C, He W, Li G, Huang J. A review on management of spent lithium ion batteries and strategy for resource recycling of all components from them. Waste Manage. Res. 2018;36:99-112.   DOI
6 Chen L, Tang X, Zhang Y, Li L, Zeng Z, Zhang Y. Process for the recovery of cobalt oxalate from spent lithium-ion batteries. Hydrometallurgy 2011;108:80-86.   DOI
7 Dorella G, Mansur MB. A study of the separation of cobalt from spent Li-ion battery residues. J. Power Sour. 2007;170:210-215.   DOI
8 Ferreira DA, Prados LM, Majuste D, Mansur MB. Hydrometallurgical separation of aluminium, cobalt, copper and lithium from spent Li-ion batteries. J. Power Sour. 2009;187:238-246.   DOI
9 Pathak P, Srivastava RR, Ojasvi. Assessment of legislation and practices for the sustainable management of waste electrical and electronic equipment in India. Renew. Sust. Energ. Rev. 2017;78:220-232.   DOI
10 Jang YC, Townsend TG. Leaching of lead from discarded notebook computers using the scale-up TCLP and other standard leaching tests. Environ. Eng. Res. 2006;11:14-27.   DOI
11 Chen X, Zhou T. Hydrometallurgical process for the recovery of metal values from spent lithium-ion batteries in citric acid media. Waste Manage. Res. 2014;32:1083-1093.   DOI
12 Li L, Chen R, Sun F, Wu F, Liu J. Preparation of $LiCoO_2$ films from spent lithium-ion batteries by a combined recycling process. Hydrometallurgy 2011;108:220-225.   DOI
13 Mantuano DP, Dorella G, Elias RC, Mansur MB. Analysis of a hydrometallurgical route to recover base metals from spent rechargeable batteries by liquid-liquid extraction with Cyanex 272. J. Power Sour. 2006;159:1510-1518.   DOI
14 Lee CK, Rhee KI. Reductive leaching of cathodic active materials from lithium ion battery wastes. Hydrometallurgy 2003;68:510-518.
15 Fan B, Chen X, Zhou T, Zhang J, Xu B. A sustainable process for the recovery of valuable metals from spent lithium-ion batteries. Waste Manage. Res. 2016;34:474-481.   DOI
16 Ilyas N, Ilyas S, Rahman SU, Yousaf S, Zia A, Sattar S. Removal of copper from an electroplating industrial effluent using the native and modified spirogyra. Water Sci. Technol. 2018;78:147-155.   DOI
17 Pathak P. An assessment of strontium sorption onto bentonite buffer material in waste repository. Environ. Sci. Pollut. Res. 2017;24:8825-8836.   DOI
18 Li L, Ge J, Chen R, Wu F, Chen S, Zhang X. Environmental friendly leaching reagent for cobalt and lithium recovery from spent lithium-ion batteries. Waste Manage. 2010;30:2615-2621.   DOI
19 Li L, Ge J, Wu F, Chen R, Chen S, Wu B. Recovery of cobalt and lithium from spent lithium ion batteries using organic citric acid as leachant. J. Hazard. Mater. 2010;176:288-293.   DOI
20 Li L, Qu W, Zhang X, et al. Succinic acid-based leaching system: A sustainable process for recovery of valuable metals from spent Li-ion batteries. J. Power Sour. 2015;282:544-551.   DOI
21 Chen X, Fan B, Xu L, Zhou T, Kong J. An atom-economic process for the recovery of high value-added metals from spent lithium-ion batteries. J. Clean. Prod. 2016;112:3562-3570.   DOI
22 Agrawal A, Pathak P, Mishra D, Sahu KK. Solvent mediated interactions for the selective recovery of Cadmium from Ni-Cd battery waste. J. Mol. Liq. 2012;173:77-84.   DOI
23 Zhang X, Bian Y, Xu S, et al. Innovative application of acid leaching to regenerate $Li(Ni_{1/3}Co_{1/3}Mn_{1/3})O_2$ cathodes from spent lithium-ion batteries. ACS Sustain. Chem. Eng. 2018;6:5959-5968.   DOI
24 He LP, Sun SY, Song XF, Yu JG. Leaching process for recovering valuable metals from the $LiNi_{1/3}Co_{1/3}Mn_{1/3}O_2$ cathode of lithium-ion batteries. Waste Manage. 2017;64:171-181.   DOI
25 Sattar R, Ilyas S, Bhatti HN, Ghaffar A. Resource recovery of critically-rare metals by hydrometallurgical recycling of spent lithium ion batteries. Sep. Purif. Technol. 2019;209:725-733.   DOI
26 Saleh TA. Advanced nanomaterials for water engineering, treatment, and hydraulics (Advances in environmental engineering and green technologies). 1st ed. Hershey: IGI Global; 2017.
27 Pathak P, Sharma S. Sorption isotherm, kinetics, and thermodynamics of contaminants in Indian soils. J. Environ. Eng. 2018;144:1-9.
28 Rahimi E, Mohaghegh N. Removal of toxic metal ions from sungun acid rock drainage using mordenite zeolite, graphene nanosheets, and a novel metal-organic framework. Mine Water Environ. 2016;35:18-28.   DOI
29 Saleh TA, Gupta VK. Nanomaterial and polymer membranes. 1st ed. Synthesis, characterization, and applications. Amsterdam: Elsevier Inc.; 2016.
30 Siddiqui MN, Redhwi HH, Al-Saadi AA, Rajeh M, Saleh TA. Kinetic and computational evaluation of activated carbon produced from rubber tires toward the adsorption of nickel in aqueous solutions. Desalin. Water Treat. 2016;57:17570-17578.   DOI
31 Rath M, Behera LP, Dash B, Sheik AR, Sanjay K. Recovery of dimethylglyoxime (DMG) from Ni-DMG complexes. Hydrometallurgy 2018;176:229-234.   DOI
32 Srivastava RR, Kim MS, Lee JC. Novel aqueous processing of the reverted turbine-blade superalloy for rhenium recovery. Ind. Eng. Chem. Res. 2016;55:8191-8199.   DOI
33 Lv W, Wang Z, Cao H, et al. A sustainable process for metal recycling from spent lithium-ion batteries using ammonium chloride. Waste Manage. 2018;79:545-553.   DOI
34 Ritcey GM, Ashbrook AW. Solvent Extraction Part I. Amsterdam: Elsevier; 1984.
35 Devi SS, Sethu M, Lalithambigai P, Priya PG. Study on the toxicokinetics of Ni(II) on Artemia franciscana. Desalin. Water Treat. 2016;57:10723-10729.   DOI
36 Saleh TA. Mercury sorption by silica/carbon nanotubes and silica/activated carbon: A comparison study. J. Water Supply Res. T 2015;64:892-903.   DOI
37 Paustenbach DJ, Tvermoes BE, Unice KM, Finley BL, Kerger BD. A review of the health hazards posed by cobalt. Crit. Rev. Toxicol. 2013;43:316-362.   DOI
38 Waring WS. Management of lithium toxicity. Toxicol. Rev. 2006;25:221-230.   DOI
39 Choubey PK, Kim MS, Srivastava RR, Lee JC, Lee JY. Advance review on the exploitation of the prominent energy-storage element: Lithium. Part I: From mineral and brine resources. Miner. Eng. 2016;89:119-137.   DOI
40 Cheema HA, Ilyas S, Masud S, Muhsan MA, Mahmood I, Lee JC. Selective recovery of rhenium from molybdenite flue-dust leach liquor using solvent extraction with TBP. Sep. Purif. Technol. 2018;191:116-121.   DOI
41 Jun M, Srivastava RR, Jeong J, Lee JC, Kim MS. Simple recycling of copper by the synergistic exploitation of industrial wastes: A step towards sustainability. Green Chem. 2016;18:3823-3834.   DOI
42 Muhsan MA, Ilyas S, Cheema HA, Masud S, Shabbir N. Recovery of nitric acid from effluent streams using solvent extraction with TBP: A comparative study in absence and presence of metal nitrates. Sep. Purif. Technol. 2017;186:90-95.   DOI
43 Ishfaq A, Ilyas S, Yasen A, Farhan M. Hydrometallurgical valorization of chromium, iron, and zinc from an electroplating effluent. Sep. Purif. Technol. 2019;209:964-971.   DOI
44 Foster M, Isely P, Standridge CR, Hasan MM. Feasibility assessment of remanufacturing, repurposing, and recycling of end of vehicle application lithium-ion batteries. J. Ind. Eng. Manage. 2014;7:698-715.