Clean Technology (청정기술)

The Korean Society of Clean Technology (한국청정기술학회)
권호 표지
DOI QR코드

DOI QR Code

A Study on the Recovery of Lantanum and Neodymium from Waste Battery Through the Recycling Process

폐 전지로부터 재활용 과정을 통한 란타넘, 네오디뮴 회수에 관한 연구

  • Received : 2020.06.09
  • Accepted : 2020.06.24
  • Published : 2020.06.30
Download PDF
⟨ Previous Next ⟩

Abstract

In this paper, the recycling of waste Ni-MH battery by-products for electric vehicle is studied. Although rare earths elements still exist in waste Ni-MH battery by-products, they are not valuable as materials in the form of by-products (such as an insoluble substance). This study investigates the recovering of rare earth oxide for solvent extraction A/O ratio, substitution reaction, and reaction temperature, and scrubbing of the rare earth elements for high purity separation. The by-product (in the form of rare earth elements insoluble powder) is converted into hydroxide form using 30% sodium hydroxide solution. The remaining impurities are purified using the difference in solubility of oxalic acid. Subsequently, Yttrium is isolated by means of D2EHPA (Di-[2-ethylhexyl] phosphoric acid). After cerium is separated using potassium permanganate, lanthanum and neodymium are separated using PC88A (2-ethylhexylphosphonic acid mono-2-ethylhexyl ester) and it is calcinated at a temperature of 800 ℃. As a result of the physical and chemical measurement of the calcined lanthanum and neodymium powder, it is confirmed that the powder is a microsized porous powder in an oxide form of 99.9% or more. Rare earth oxides are recovered from Ni-MH battery by-products through two solvent extraction processes and one oxidation process. This study has regenerated lanthanum and neodymium oxide as a useful material.

본 연구에서는 유가금속 회수를 한 전기차 폐배터리 부산물의 재활용에 관하여 연구하였다. 폐배터리 부산물에는 희토류들이 남아있으나, 부산물의 형태로는 소재로서의 가치가 없기에 정제과정을 거쳐 희토류 산화물로 회수하였다. 희토류침전분말 형태의 부산물을 30% 수산화나트륨을 이용하여 가공이 편한 수산화물로 변환한 뒤, 옥살산의 용해도 차이를 이용하여 남아 있는 불순물을 정제한 뒤, D2EHPA (Di-(2-ethylhexyl) phosphoric acid)를 사용하여 이트륨을 분리하였다. 과망가니즈산 칼륨을 이용하여 세륨을 분리 후, PC88A (2-ethylhexylphosphonic acid mono-2-ethylhexyl ester)를 사용하여 란타넘과 네오디뮴을 분리하였다. 그 후 800 ℃의 온도에서 소성하여 란타넘, 네오디뮴 산화물로 재생하는 방법을 확인하였다.

Keywords

References

  1. Humphries, M., "Rare Earth Elements: The Global Supply Chain," Congressional Research Service., 16 (2013).
  2. https://www.usgs.gov/centers/nmic/rare-earths-statistics-and-information (accessed Jan. 2019).
  3. Lim, K., Han, J., and Park, S., "Mine Production and Reserves of Rare Earths," J. Korean Phys. Soc. Webzine Article., 28(9), 3-8 (2019).
  4. Gupta, C. K., and Krishnamurthy, N., "Extractive Metallurgy of Rare Earths," Int. Mater. Rev., 37(1), 197-248 (1992) https://doi.org/10.1179/imr.1992.37.1.197
  5. Abreu, R, D., and Morais, C, A., "Purification of Rare Earth Elements from Monazite Sulphuric Acid Leach Liquor and the Production of High-Purity Ceric Oxide," Miner. Eng., 23(6), 536-540 (2010). https://doi.org/10.1016/j.mineng.2010.03.010
  6. Mohammadi, M., Forsberg, K., Kloo, L., Martinez De La Cruz, J., and Rasmuson, A., "Separation of ND(III), DY(III) and Y(III) by Solvent Extraction Using D2EHPA and EHEHPA," Hydrometallurgy., 156, 215-224 (2015). https://doi.org/10.1016/j.hydromet.2015.05.004
  7. Kim, B., Ahn, N., Lee, S., and Kim, D., "A Study on the Separation of Cerium from Rare Earth Precipitates Recovered from Waste NiMH Battery," JKIRR., 28(6), 18-25 (2019).
  8. Ahn, N., Kim, D., and Yang, D., "A Study on Recovery of Rare Earth and Acid Leaching for Wet Recycling of Waste NiMH Batteries," JKIRR., 27(1), 22-30 (2018).
  9. Ahn, N., Kim, D., Shim, H., and Park, J., "A Study on Recovery of Rare Earth Oxide Powders from Waste NiMH Batteries," J. Korean Cryst. Growth Cryst. Technol., 28(2), 85-90 (2018). https://doi.org/10.6111/JKCGCT.2018.28.2.085
  10. Yoon, H., Kim, C., Eom, H., and Kim, J., "Separation of Cerium Hydroxide from Wasted Cerium Polishing Powders by the Aeration and Acidity-Controlling Method," JKIRR., 14(6), 3-9 (2005).
  11. Orhanovic, Z., Pokric, B., Furedi, H., and Branica, M., "Precipitation and Hydrolysis of Metallic Ions. III. Studies on the Solubility of Yttrium and Some Rare Earth Hydroxides," Croat. Chem. Acta., 38, 269-276 (1966).
  12. Kao, H., Yen, P., and Juang, R., "Solvent Extraction of La(III) and Nd(III) from Nitrate Solutions with 2-Ethylhexylphosphonic Acid Mono-2-Ethylhexyl Ester," Chem. Eng. J., 119(2-3), 167-174 (2006). https://doi.org/10.1016/j.cej.2006.03.024
  13. Kashi, E., Habibpour, R., Gorzin, H., and Maleki, A., "Solvent Extraction and Separation of Light Rare Earth Elements (La, Pr and Nd) in the Presence of Lactic Acid as a Complexing Agent by Cyanex 272 in Kerosene and the Effect of Citric Acid, Acetic Acid and TitriplexIII as Auxiliary Agents," J. Rare Earth, 36(3), 317-323 (2018). https://doi.org/10.1016/j.jre.2017.09.016
  14. Golden, T. D., Shang, Y., Wang, Q., and Zhou, T., "Electrochemical Synthesis of Rare Earth Ceramic Oxide Coatings," Intech, (2015).
  15. Duhan, S., "Effect of Sintering Time on Particle Size of Rare Earth Compounds (R = Nd) Prepared by Wet Chemical Method," IJPAP, 47(12), 872-875 (2009).
  16. Kepinski, L., Zawadzki, M., and Mista, W., "Hydrothermal Synthesis of Precursors of Neodymium Oxide Nanoparticles," Solid State Sci., 6(12), 1327-1336 (2004). https://doi.org/10.1016/j.solidstatesciences.2004.07.003
  17. Rosynek, M. P., and Magnuson, D. T., "Preparation and Characterization of Catalytic Lanthanum Oxide" J. Catal., 46, 402-413 (1977). https://doi.org/10.1016/0021-9517(77)90224-X
  18. Hussein, G. A. M., and Ismail, H. M., "Characterization of Lanthanum Oxide Formed as a Final Decomposition Product of Lanthanum Acetylacetonate: Thermoanalytical, Spectroscopic and Microscopic Studies" Powder Technol., 84(2), 185-190 (1995). https://doi.org/10.1016/0032-5910(95)02984-A
  19. Duhan, S., Aghamkar, P., and Singh, M., "Synthesis and Characterization of Neodymium Oxide in Silica Matrix by Solgel Protocol Method," phys. res. int., 2008, (2008)
  20. Adi, W. A., Wardiyati, S., and Dewi, S. H., "Nanoneedles of Lanthanum Oxide ($La_2O_3$): A Novel Functional Material for Microwave Absorber Material," IOP Conference Series: Materials Science and Engineering, 202, (2017).
  21. Aldebert, P., and Traverse, P. J., "Etude Par Diffraction Neutronique des Structures de Haute Temperature de $La_2O_3$ et $Nd_2O_3$" Mater. Res. Bull., 14(3), 303-323 (1979). https://doi.org/10.1016/0025-5408(79)90095-3
  22. Saravani, H., and Jehali, M., "Synthesis and Characterization of Lanthanum Oxide and Lanthanumoxid Carbonate Nanoparticles from Thermalizes of [La(acacen)($NO_3$)($H_2O$) Complex," Orient. J. Chem., 31(4), 2351-2357 (2015) https://doi.org/10.13005/ojc/310464
  23. Cheraitia, K., Lounis, A., Mohamed, M., Azzaz, M., and Osmane, K., "Neutron Activation Analysis of Nd-Fe-B Magnet and Determination of the Content of Nd After Oxalate Precipitation and Production of $Nd_2O_3$," Matter : Int. J. Sci. Technol, 1(1), 259-274 (2015). https://doi.org/10.20319/mijst.2016.s11.259274