Recovery of Rare-Earth Elements from Neodymium Magnet Waste Using Glycolic, Maleic, and Ascorbic Acids Followed by Solvent Extraction

Journal of Sustainable Metallurgy - Tập 5 - Trang 85-96 - 2018
Marino Gergoric1, Antonin Barrier2, Teodora Retegan1
1Nuclear Chemistry and Industrial Materials Recycling, Chemistry and Chemical Engineering, Chalmers University of Technology, Göteborg, Sweden
2National School of Chemistry Montpellier, Montpellier, France

Tóm tắt

Rare-earth elements (REEs) play a key role in modern societies as their usage keeps increasing in new technologies and green energy sources. However, they are also considered the most critical raw materials in the EU and the USA in terms of supply. There is an increased global interest in the recycling of REEs from end-of-life products and industrial waste. Some REEs, such as Nd, Pr, and Dy, can be recovered from neodymium magnets. These magnets are of special interest since they are present in various technological wastes, such as hard disk drives, electric generators for wind turbines, electric motors, etc. Separation of REEs from other magnet components, such as Fe, which is the main part of the alloy, and further reprocessing of REEs, is the main goal of this work. In this work, neodymium magnet powder was successfully leached using the fully combustible organic lixiviants maleic, glycolic, and ascorbic acids, in order to potentially decrease the usage of strong mineral acids in the hydrometallurgical recovery of REEs. Subsequently, the REEs were selectively extracted from these leachates. For this separation step, several phosphate extractants (TBP, D2EHPA, Cyanex 272, and 923) were investigated, alongside TODGA, which follows the CHON principle and is fully combustible, with no ash or acidic gases being produced. The influences of various diluents (1-octanol, cyclohexanone, hexane, pentane, and dodecane) on the extraction were also studied since the diluents can play an important role in the extraction process and increase selectivity between the extraction of REEs and other impurities. Leaching was shown to be more efficient with maleic and glycolic acids than with ascorbic acid, even at room temperature. Values above 95% were reached for REEs with 1 M concentration and 1/80 solid/liquid ratio. For ascorbic acid, heating the leaching system to 70 °C allowed similar values to be reached. D2EHPA has shown good extraction properties for the recovery of REEs from both glycolic and maleic leachate, mostly with nonpolar diluents such as pentane and hexane, without extracting transition metals (distribution ratios under 0.1). TODGA also showed good extraction of REEs and selectivity between elements, but only in the maleic leachate. As expected, the increasing concentration of the D2EHPA led to the increased distribution ratios. Thus, glycolic, maleic, and ascorbic organic acids, which have not been used before for leaching of neodymium magnet waste, showed good potential for the recovery of REEs from neodymium magnets and for the further development of large-scale recovery processes for REEs.

Tài liệu tham khảo

Cotton S (2006) Lanthanide and actinide chemistry. Wiley, Chichester Binnemans K, Jones PT, Müller T, Yurramendi L (2018) Rare earths and the balance problem: how to deal with changing markets? J Sustain Metall 4(1):126–146 Yang Y, Walton A, Sheridan R, Güth K, Gauß R, Gutfleisch O, Buchert M, Steenari B-M, Van Gerven T, Jones PT, Binnemans K (2017) REE recovery from end-of-life NdFeB permanent magnet scrap: a critical review. J Sustain Metall 3(1):122–149 Tunsu C, Petranikova M, Gergorić M, Ekberg C, Retegan T (2015) Reclaiming rare earth elements from end-of-life products: a review of the perspectives for urban mining using hydrometallurgical unit operations. Hydrometallurgy 156:239–258 Binnemans K, Jones PT, Blanpain B, Van Gerven T, Yang Y, Walton A, Buchert M (2013) Recycling of rare earths: a critical review. J Clean Prod 51:1–22 European Commission (2018) Critical raw materials for the EU. In: European Commission (ed) Report of the ad-hoc working group on defining critical raw materials. European Commission, Brussels Xie F, Zhang TA, Dreisinger D, Doyle F (2014) A critical review on solvent extraction of rare earths from aqueous solutions. Miner Eng 56:10–28 Lyman JW, Palmer GR (1993) Recycling of neodymium iron boron magnet scrap. United States Department of the Interior, Washington DC Yoon H-S, Kim C-J, Chung KW, Lee S-J, Joe A-R, Shin Y-H, Lee S-I, Yoo S-J, Kim J-G (2014) Leaching kinetics of neodymium in sulfuric acid from E-scrap of NdFeB permanent magnet. Korean J Chem Eng 31(4):706–711 Gergoric M, Ekberg C, Foreman MRSJ, Steenari B-M, Retegan T (2017) Characterization and leaching of neodymium magnet waste and solvent extraction of the rare-earth elements using TODGA. J Sustain Metall 3(3):638–645 Önal MAR, Aktan E, Borra CR, Blanpain B, Van Gerven T, Guo M (2017) Recycling of NdFeB magnets using nitration, calcination and water leaching for REE recovery. Hydrometallurgy 167:115–123 Lee C, Chen Y, Liao C, Popuri SR, Tsai S, Hung C (2013) Selective leaching process for neodymium recovery from scrap Nd–Fe–B magnet. Metall Mater Trans 44(13):5825–5833 Tanaka Y, Zhang Q, Saito F (2002) Sonochemical recovery of metals from recording media. J Chem Eng Jpn 35(2):173–177 Itakura T, Sasai R, Itoh H (2006) Resource recovery from Nd–Fe–B sintered magnet by hydrothermal treatment. J Alloy Compd 408:1382–1385 Behera SS, Parhi PK (2016) Leaching kinetics study of neodymium from the scrap magnet using acetic acid. Sep Purif Technol 160:59–66 Koivistoinen OM, Kuivanen J, Barth D, Turkia H, Pitkänen JP, Penttilä M, Richard P (2013) Glycolic acid production in the engineered yeasts Saccharomyces cerevisiae and Kluyveromyces lactis. Microb Cell Fact 12:82 Sigel A, Operschall BP, Sigel H, Roland KO (2017) Lead: its effects on environment and health. University of Zurich, Zurich, pp 319–402 Yang X, Zhang Y, Fang X (2014) Rare earth element recycling from waste nickel-metal hydride batteries. J Hazard Mater 279:384–388 Mohammadi M, Forsberg K, Kloo L, Martinez De La Cruz J, Rasmuson Å (2015) Separation of ND(III), DY(III) and Y(III) by solvent extraction using D2EHPA and EHEHPA. Hydrometallurgy 156:215–224 Yang J, Retegan T, Steenari B-M, Ekberg C (2016) Recovery of indium and yttrium from Flat Panel Display waste using solvent extraction. Sep Purif Technol 166:117–124 Kuipa PK, Hughes MA (2002) Diluent effect on the solvent extraction rate of copper. Sep Sci Technol 37:1135–1152 Gergoric M, Ekberg C, Steenari B-M, Retegan T (2017) Separation of heavy rare-earth elements from light rare-earth elements via solvent extraction from a neodymium magnet leachate and the effects of diluents. J Sustain Metall 3(3):601–610 Rydberg J, Cox M, Musicas C, Choppin GR (2004) Solvent extraction principles and practice. Taylor & Francis, Boca Raton Önal MAR, Jönsson C, Zhou W, Van Gerven T, Guoa M, Walton A, Blanpain B (2017) Comparative oxidation behavior of Nd–Fe–B magnets for potential recycling methods: effect of hydrogenation pre-treatment and magnet composition. J Alloys Compd 728C:727–738 Haynes W (ed) CRC handbook of chemistry and physics, 94th edn. CRC Press, Boca Raton do Nascimento ALCS, Teixeira JA, Nunes WDG, Gomes DJC, Gaglieri C, Treu-Filho O, Pivatto M, Caires FJ, Ionashiro M (2017) Thermal behavior of glycolic acid, sodium glycolate and its compounds with some bivalent transition metal ions in the solid state. J Therm Anal Calorim 130:1463 Pelendritis M (2017) Nuclear fuel waste extraction: third phase revisited. The University of Manchester, Manchester Wypych G (2008) Knovel solvents—a properties database. ChemTec Publishing, Toronto