Investigating Leaching Parameters for Enhanced Rare Earth Elements Sustainability and Recovery from Phosphogypsum

Raouf Jebali1, Khaled Brahmi1, Sana Ncib1, Elimame Elaloui1, Wided Bouguerra1
1Laboratory of Materials Application to Water, Environment and Energy (LAM3E), Faculty of Sciences of Gafsa, University of Gafsa, Sidi Ahmed Zarroug University Campus, Gafsa, Tunisia

Tóm tắt

Substantial volumes of phosphogypsum (PG) are generated globally as a by-product in phosphoric acid production, categorizing it as a widespread waste. Managing such substantial amounts of PG poses challenges due to its composition containing various pollutants, including persistent rare earth elements (REEs) with non-biodegradable characteristics. Conversely, an encouraging approach for valorizing PG involves extracting REEs, as these elements play a critical role in diverse modern technologies. However, any recovery process must be cost-effective and environmentally compliant. This research aims to enhance leaching efficiency and explore the correlation between the extraction efficiency of REEs from PG and gypsum solubility. The results reveal that the leaching efficiency of REEs increases with higher acid concentration, extended leach duration, and an optimized solid/liquid ratio, primarily due to the improved solubility of phosphogypsum. Notably, hydrochloric acid ( $${\text{HCl}}$$ ) leaching exhibits superior efficiency at ambient temperatures, presenting advantages in terms of lower industrial energy demand and reduced cost.Furthermore, the addition of ammonium chloride or sodium chloride to HCl as a leaching agent significantly enhances the leaching efficiency of REEs from PG. The optimal content of sodium and ammonium (ion-exchangeable) for achieving the highest REEs leaching efficiency was found to be 2% and 4%, respectively. The highest leaching efficiency for the combined elements Nd, Y, and La in hydrochloric acid was achieved with an acid concentration of 3 mol L−1, and a solid/liquid ratio of 1/40, and a temperature of 25 °C. These promising results are noteworthy, especially considering that no heating system is required for REEs extraction from PG, aligning with the circular economy goals and environmental protection. High recovery efficiency achieved (about 87%) while minimizing costs is essential for the economic viability of REEs extraction.

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Filho WL, Kotter R, Özuyar PG, Abubakar IR, Eustachio JHPP, Matandirotya NR (2023) Understanding rare earth elements as critical raw materials. Sustainability 15:1919. https://doi.org/10.3390/su15031919 Borges De Lima I, Leal FW (eds) (2016) Rare earth industry: technological, economic, and environmental implications. Elsevier, Amsterdam (9780128023280) Weiss D (2019) Developments in aluminum-scandium-ceramic and aluminum-scandium-cerium alloys. In: Chesonis C (ed) Light metals 2019. Springer Nature, Cham, pp 1439–1443 (978-3-030-05864-7) Massari S, Ruberti M (2013) Rare earth elements as critical raw materials: focus on international markets and future strategies. Resour Policy 38:36–43 Calvo G, Valero A (2021) Strategic mineral resources: availability and future estimations for the renewable energy sector. Environ Dev 41:100640 Balaram V (2019) Rare earth elements—a review of applications, occurrence, exploration, analysis, recycling, and environmental impact. Geosci Front 10:1285–1303 Jorjani E, Bagherieh AH, Chelgani SC (2011) Rare earth elements leaching from Chadormalu apatite concentrate: laboratory studies and regression predictions. Korean J Chem Eng 28(2):557–562 Jebali R, Triki M, Abdullah AN, Kochkarc H (2019) From adsorption of rare earth elements on TiO2 nanotubes to preconcentration column application. Microchem J 149(10):104021. https://doi.org/10.1016/j.microc.2019.104021 Cánovas CR, Chapron S, Arrachart G, Pellet-Rostaing S (2019) Leaching of rare earth elements (REEs) and impurities from phosphogypsum: a preliminary insight for further recovery of critical raw materials. J Clean Prod 219:225–235 Koopman C, Witkamp GJ (2000) Extraction of lanthanides from the phosphoric acid production process to gain a purified gypsum and a valuable lanthanide by-product. Hydrometallurgy 58(1):51–60 Silva Luis FO (2022) A review on the environmental impact of phosphogypsum and potential health impacts through the release of nanoparticles. Chemosphere 286:131513 (Part 1) Soudi A, Hezarkhani A (2016) Geochemical investigation and statistical analysis on rare earth elements in Lakehsiyah deposit, Bafq district. J Afr Earth Sci 124:139–150 Degirmenci N (2008) Utilization of phosphogypsum as raw and calcined material in manufacturing of building products. Constr Build Mater 22:1857–1862 Oliveira K, Menezes M, Von Sperling E, Jacomino V (2012) Transfer factor of rare earth elements from phosphogypsum amended Brazilian tropical soils to lettuce, corn and soybean. J Solid Waste Technol Manag 38:202–210 Alcordo IS, Rechcigl JE (1993) Phosphogypsum in agriculture: a review. Adv Agron 49:55–118 Smadi MM, Haddad RH, Akour AM (1999) Potential use of phosphogypsum in concrete. Cem Concr Res 29:1419–1425 Garbaya H, Jraba A, Khadimallah MA, Elaloui E (2021) The development of a new phosphogypsum-based construction material: a study of the physicochemical, mechanical and thermal characteristics. Materials 14:7369. https://doi.org/10.3390/ma14237369 Calderon-Morales BRS, García-Martínez A, Pineda P, García-Tenorio R (2021) Valorization of phosphogypsum in cement-based materials: limits and potential in eco-efficient construction. J Build Eng 44:102506. https://doi.org/10.1016/j.jobe.2021.102506 Liang H, Zhang P, Jin Z, DePaoli D (2017) Rare-earth leaching from Florida phosphate rock in wet-process phosphoric acid production. Miner Metall Process 34:146–153 Xie G, Guan Q, Zhou F, Yu W, Yin Z, Tang H, Zhang Z, Chi R (2023) A critical review of the enhanced recovery of rare earth elements from phosphogypsum. Molecules 28:6284. https://doi.org/10.3390/molecules28176284 Li S, Malik M, Azimi G (2022) Extraction of rare earth elements from phosphogypsum using mineral acids: process development and mechanistic investigation. Ind Eng Chem Res 61:102–114 Masmoudi-Soussi A, Hammas-Nasri I, Horchani-Naifer K, Férid M (2019) Study of rare earths leaching after hydrothermal conversion of phosphogypsum. Chem Afr 2:415–422. https://doi.org/10.1007/s42250-019-00048-z Binnemans K, Pontikes Y, Jones PT, Van GervenT, Blanpain B (2013) Recovery of rare earths from industrial waste residues: a concise review. In: 3rd International Slag Valorisation Symposium, Leuven, 193–205 Grabas C, Nützenade A (2014) Industrial policy in Europe after 1945: wealth, power and economic development in the cold war, Springer Jarosiniski A, Kowalczyk J, Mazanek CZ (1993) Development of the Polish wasteless technology of apatite phosphogypsum utilization with recovery of rare earths. J Alloys Compd 200:147–150 Jyothi RK, Thenepalli T, Ahn JW, Parhi PK, Chung KW, Lee JY (2020) Review of rare earth elements recovery from secondary resources for clean energy technologies: grand opportunities to create wealth from waste. J Clean Prod 267:122048 Antonick PJ, Hu Z, Fujita Y, Reed DW, Das G, Wu L, Shivaramaiah R, Kim P, Eslamimanesh A, Lencka MM, Jiao Y, Anderko A, Navrotsk A, Riman RE (2019) Bio-and mineral acid leaching of rare earth elements from synthetic phosphogypsum. J Chem Thermodyn 132:491–496 Lütke SF, Oliveira MLS, Waechter SR, Silva LFO, Cadaval TRS Jr, Duarte FA, Dotto GL (2022) Leaching of rare earth elements from phosphogypsum. Chemosphere 301:134661 Hammas-Nasri I, Horchani-Naifer K, Mokhtar F, Barca D (2016) Rare earths concentration from phosphogypsum waste by two-step leaching method. Int J Min Proc 149C:78–83 Jowitt SM (2018) Criticality of the rare earth elements: current and future sources and recycling. Reprinted from: Resources 7:35. https://doi.org/10.3390/resources7020035 Beer G, Mackowski S, Raiter R, (2008) Development of a processing flowsheet for the Nolans project. In: Proceedings of ALTA Uranium 2008, ALTA Metallurgical Services, Perth (WA) 1–30 Kijkowska R, Kowalczyk J, Mazanek C, Pawłowska-Kozińska D (1988)Apatite phosphogypsum—raw material for the production of rare earths and gypsum. Wyd. Geologiczne, Warszawa Walawalkar M, Nichol CK, Gisele AG (2016) Process investigation of the acid leaching of rare earth elements from phosphogypsum using HCl, HNO3 and H2SO4. Hydrometallurgy 166:195–204 Wu S, Zhao L, Wang L, Huang X, Zhang Y, Feng Z, Cui D (2019) Simultaneous recovery of rare earth elements and phosphorus from phosphate rock by phosphoric acid leaching and selective precipitation: towards green process. J Rare Earths 37(652–658):28 Mukaba J-L, Eze CP, Pereao O, Petrik LF (2012) Rare Earths’ recovery from phosphogypsum: an overview on direct and indirect leaching techniques. Minerals 11:1051. https://doi.org/10.3390/min11101051 Linke WF (1965) Solubilities of inorganic and metal organic compounds. Am Chern Soc (4th Edition) Vol. I and 2 Stone K, Bandara AMTS, Senanayake G, Jayasekera S (2016) Processing of rare earth phosphate concentrates: a comparative study of pre-leaching with perchloric, hydrochloric, nitric and phosphoric acids and deportment of minor/major elements. Hydrometallurgy 163:137–147 Kaasa B (1998) Prediction of pH, mineral precipitation and multiphase equilibria during oil recovery. Norges Teknisk-Naturvitenskapelige Universitet (NTNU), Institutt for unorganisk kjemi Kharaka YK, Gunter WD, Aggarwal PK, Perkins EH, DeBraal JD (1989) A computer program for geochemical modeling of water-rock interactions. Department of the Interior, US Geological Survey Helgeson HC, Kirkham DH, Flowers GC (1981) Theoretical prediction of the thermodynamic behaviour of aqueous electrolytes by high pressures and temperatures: IV. Calculation of activity coefficients, osmotic coefficients, and apparent molal and standard and relative partial molal properties to 600 C and 5 kb. Am J Sci 281:1249–1516 Zhang YX, Yang ZH, Guo D, Geng H, Dong C (2013) Effect of chloride salts and bicarbonate on solubility of CaSO4 in aqueous solutions at 37 °C. Procedia Environ Sci 18:84–91 Tian J, Yin J, Chi R, Rao G, Jiang M, Ouyang K (2010) Kinetics on leaching rare earth from the weathered crust elution-deposited rare earth ores with ammonium sulfate solution. Hydrometallurgy 101:166–170 Moldoveanu GA, Papangelakis VG (2012) Recovery of rare earth elements adsorbed on clay minerals: I. Desorption mechanism. Hydrometallurgy 117–118:71–78. https://doi.org/10.1016/j.hydromet.2012.02.007 Kumar A, Sanghavi R, Mohandas VP (2007) Solubility pattern of CaSO42H2O in the system NaCl + CaCl2 + H2O and solution densities at 35 C: non-ideality and ion pairing. J Chem Eng Data 52:902–905 Yang Y, Li Y (1978) Physical and chemical constants of rare earth. Metallurgical Industry Press, Beijing ((in Chinese)) Dai Z, Kan AT, Shi W, Zhang N, Zhang F, Yan F, Bhandari N, Zhang Z, Liu Y, Ruan G, Tomson MB (2017) Solubility measurements and predictions of gypsum, anhydrite, and calcite over wide ranges of temperature, pressure, and ionic strength with mixed electrolytes. Rock Mech Rock Eng 50:327–339. https://doi.org/10.1007/s00603-016-1123-9