Solvent extraction of Ce(IV) from sulfuric acid solutions using Cyanex 921 and its mixtures with D2EHPA

Document Type : Original Research

Authors

1 Associate Professor, Nuclear Fuel Cycle Research School, Nuclear Science and Technology Research Institute, Tehran-Iran

2 Student in Faculty of mining engineering, School of engineering, Yazd university, Yazd-Iran

3 Assistant Professor, Nuclear Fuel Cycle Research School, Nuclear Science and Technology Research Institute, AEOI, Tehran-Iran

Abstract
Research subject: With the rapid development of science and technology, cerium and cerium oxide are widely used in various fields, including in the manufacture of aluminum, aluminum alloys, some steels and in permanent magnets, catalysts, Polishing powder, Glass, Cinema, and Ceramic Technology. Solvent extraction is one of the effective techniques for extraction, separation, and purification of cerium.

Research approach: The extraction of cerium­(IV) from sulfuric acid solutions using Cyanex 921 in kerosene was investigated. The different parameters affecting the extraction process of cerium(IV) such as pH of aqueous solutions­, reagent, metal ion concentration, contact time as well as temperature, are separately investigated. Experiments in the pH range of 0.5 to 5.5, at 25±1 oC­, using Cyanx 921 in the concentration range of 0.06 to 0.4 mol L-1, and a mixture of Cyanx 921 and D2EHPA was performed in different ratios.

Main results: From the temperature study, the extraction reaction for Ce­(IV) was found to be exothermic in nature. The results indicated that the effective extraction of cerium(IV) from sulfuric acid solutions cannot be achieved in a single equilibration because the solubility of Cyanex 921 in aliphatic diluents is limited at ambient temperature. To rectify this issue, the possibility of using a synergistic mixture of Cyanex 921 and D2EHPA as extractant system to recover cerium(IV) from sulfuric acid solutions was investigated. Mixtures of Cyanex 921 and D2EHPA resulted in synergistic extraction of cerium­(IV) from sulfuric acid solutions. The results indicated that, under experimental conditions, the maximum synergistic coefficient was obtained at the molar ratio of (0.6M D2EHPA­/­0.2­M Cyanex 921) 3.0, and cerium(IV) was extracted into organic phase in the form of Ce(SO4)(HSO4)2.­Cyanex 921.

Keywords

Subjects


[1] L. ZHANG, C. Ji, J. Weiqun, D. Yuefeng, T. Jun, and Y. ZHANG, "Extraction mechanism of cerium (IV) in H2SO4/H3PO4 system using bifunctional ionic liquid extractants," Journal of Rare Earths, vol. 31, pp. 1195-1201, 2013.
[2] F. Spedding, A. Voigt, E. M. Gladrow, and N. Sleight, "The separation of rare earths by ion exchange. 1, 2 I. cerium and yttrium," Journal of the American Chemical Society, vol. 69, pp. 2777-2781, 1947.
[3] M. A. Keane, "The role of the alkali metal co-cation in the ion exchange of Y zeolites IV. Cerium ion exchange equilibria," Microporous materials, vol. 7, pp. 51-59, 1996.
[4] F. Laufer, S. Yariv, and M. Steinberg, "The adsorption of quadrivalent cerium by kaolinite," Clay Minerals, vol. 19, pp. 137-149, 1984.
[5] Z. Murthy and A. Choudhary, "Separation of cerium from feed solution by nanofiltration," Desalination, vol. 279, pp. 428-432, 2011.
[6] P. Ramakul, U. Mooncluen, Y. Yanachawakul, and N. Leepipatpiboon, "Mass transport modeling and analysis on the mutual separation of lanthanum (III) and cerium (IV) through a hollow fiber supported liquid membrane," Journal of Industrial and Engineering Chemistry, vol. 18, pp. 1606-1611, 2012.
[7] P. Ura, R. Prakorn, and P. Weerawat, "Purely extraction and separation of mixture of cerium (IV) and lanthanum (III) via hollow fiber supported liquid membrane," Journal of Industrial and Engineering Chemistry, vol. 11, pp. 926-931, 2005.
[8] Z. Dan, C. Ji, and L. Deqian, "Separation chemistry and clean technique of cerium (IV): A review," Journal of Rare Earths, vol. 32, pp. 681-685, 2014.
[9] J. Zhao, Y. Zuo, D. Li, and S. Liu, "Extraction and separation of cerium (IV) from nitric acid solutions containing thorium (IV) and rare earths (III) by DEHEHP," Journal of alloys and compounds, vol. 374, pp. 438-441, 2004.
[10] K. Li, J. Chen, D. Zou, Y. Deng, and D. Li, "Recovery of cerium (IV) in acidic nitrate solutions by solvent extraction with a novel extractant tris (2-ethylhexyl) phosphine oxide," Hydrometallurgy, vol. 190, p. 105155, 2019.
[11] P. Tedesco, V. De Rumi, and J. Gonza, "Extraction of tetravalent metals with di-(2-ethylhexyl) phosphoric acid—III: Cerium," Journal of Inorganic and Nuclear Chemistry, vol. 29, pp. 2813-2817, 1967.
[12] D. Li, Z. Wang, and G. Zeng, "The mechanism of extraction of Ce (IV) from sulphuric acid solution by primary amine N1923," Nucl. Chem. Radio. Chem, vol. 6, pp. 153-160, 1984.
[13] D. Li, Z. Wang, G. Zeng, and Z. Xue, "Solvent extraction of Ce (IV) with HEH (EHP) from sulfuric acid solution," J. Chin. Rare Earth Soc., vol. 2, pp. 9-18, 1984.
[14] Z. Long, X. Huang, W. Huang, and G. Zhang, "Ce4+ extraction mechanism from rare earth sulfate solution containing fluorine with DEHPA," J. Chin. Rare Earths Soc, vol. 18, pp. 18-20, 2000.
[15] Z. N. Zhu ZW, Long ZQ, Li DD, Cui DL, Zhang GC, "New Environment-Friendly Approach for Bastnasite Metallurgic Treatment (Ⅰ): Extraction of Tetravalent Cerium from Sulphuric Acid Medium with Di (2-ethylhexyl) Phosphoric Acid," Journal of Rare Earths, vol. 23, pp. 178-182, 2005.
[16] J. Qiao, Z. Long, C. Zhang, and X. Hao, "Process for separating cerium (IV) from the sulfate system containing several components through extracting with 2-ethyl hexyl 2-ethyl hexyl phosphonic acid on industrial-scale," Chin. Rare Earths, vol. 20, pp. 119-123, 1999.
[17] L. Xinghua, X. HUANG, Z. Zhaowu, L. Zhiqi, and L. Ying, "Synergistic extraction of cerium from sulfuric acid medium using mixture of 2-ethylhexyl phosphonic acid mono 2-ethylhexyl ester and Di-(2-ethyl hexyl) phosphoric acid as extractant," Journal of Rare Earths, vol. 27, pp. 119-122, 2009.
[18] J. Zhao, S. Meng, and D. Li, "Coordination reactions in the extraction of cerium (IV) and fluorine (I) by DEHEHP from mixed nitric acid and hydrofluoric acid solutions," Solvent extraction and ion exchange, vol. 22, pp. 813-831, 2004.
[19] L. Jun, W. Zhenggui, L. Deqian, M. Gengxiang, and J. Zucheng, "Recovery of Ce (IV) and Th (IV) from rare earths (III) with Cyanex 923," Hydrometallurgy, vol. 50, pp. 77-87, 1998.
[20] J. Lu, D. Li, Z. Wei, and Z. Jiang, "SEPARATION OF Ce (Ⅳ) AND Th (Ⅳ) FROM RE (Ⅲ) IN HNO_3 SOLUTION BY CYANEX 923 EXTRACTANT," Acta Metallurgica Sinica (English Letters), vol. 12, pp. 191-197, 2009.
[21] Y. S. Yu GH, Li DQ, Feng YY, "Kinetic Study of Ce 4+ Extraction with Cyanex 923," Journal of Rare Earths, pp. 250-254, 2001.
[22] W. Liao, G. Yu, and D. Li, "Solvent extraction of cerium (IV) and fluorine (I) from sulphuric acid leaching of bastnasite by Cyanex 923," Solvent Extraction and Ion Exchange, vol. 19, pp. 243-259, 2001.
[23] W. Liao, G. Yu, S. Yue, and D. Li, "Kinetics of cerium (IV) extraction from H2SO4–HF medium with Cyanex 923," Talanta, vol. 56, pp. 613-618, 2002.
[24] Z. Zhang, H. Li, F. Guo, S. Meng, and D. Li, "Synergistic extraction and recovery of Cerium (IV) and Fluorin from sulfuric solutions with Cyanex 923 and di-2-ethylhexyl phosphoric acid," Separation and purification technology, vol. 63, pp. 348-352, 2008.
[25] Z. Zhang, F. Guo, S. Meng, Q. Jia, H. Li, and D. Li, "Simultaneous recovery of cerium and fluorine from bastnaesite leach liquor by mixtures of Cyanex 923 and HEH (EHP)," Industrial & engineering chemistry research, vol. 49, pp. 6184-6188, 2010.
[26] A. Chatterjee and S. Basu, "Solvent extraction of cerium (III) with high molecular weight amines," Journal of the Indian Chemical Society, vol. 69, pp. 29-31, 1992.
[27] D. Peppard, G. Mason, W. Driscoll, and R. Sironen, "Acidic esters of orthophosphoric acid as selective extractants for metallic cations—tracer studies," Journal of Inorganic and Nuclear Chemistry, vol. 7, pp. 276-285, 1958.
[28] D. Peppard, W. Driscoll, R. Sironen, and S. McCarty, "Nonmonotonic ordering of lanthanides in tributyl phosphate-nitric acid extraction systems," Journal of Inorganic and Nuclear Chemistry, vol. 4, pp. 326-333, 1957.
[29] D. Peppard, G. Mason, J. Maier, and W. Driscoll, "Fractional extraction of the lanthanides as their di-alkyl orthophosphates," Journal of Inorganic and Nuclear Chemistry, vol. 4, pp. 334-343, 1957.
[30] J. C. Warf, "Extraction of cerium (IV) nitrate by butyl phosphate," Journal of the American Chemical Society, vol. 71, pp. 3257-3258, 1949.
[31] G. Korpusov, V. Levin, N. Brezhneva, N. Prokhorova, I. Eskevich, and P. Seredenko, "The separation of cerium by extraction," Russ. J. Inorg. Chem., vol. 7, pp. 1167-1171, 1962.
[32] T. Healy and H. McKay, "Complexes between tributyl phosphate and inorganic nitrates," Recueil des Travaux Chimiques des Pays‐Bas, vol. 75, pp. 730-736, 1956.
[33] L. Hafner, "German patent 2, 633, 115," in Chemical Abstracts, 1977, p. 124825t.
[34] B. Gupta, P. Malik, and A. Deep, "Extraction of uranium, thorium and lanthanides using Cyanex-923: their separations and recovery from monazite," Journal of radioanalytical and nuclear chemistry, vol. 251, pp. 451-456, 2002.
[35] K. Li, J. Chen, and D. Zou, "Extraction and recovery of cerium from rare earth ore by solvent extraction," in Cerium Oxide-Applications and Attributes, ed: IntechOpen, 2018.
[36] D. C. Shallcross, R. Paimin, and L. Prvcic, "Value adding through solvent extraction. Volume 2. Proceedings of ISEC'96," 1996.
[37] T. Sato, T. Nishida, and M. Yamatake, "The extraction of uranium (VI) and thorium (IV) from nitric acid solutions by tri‐n‐octyl phosphine oxide," Journal of Applied Chemistry and Biotechnology, vol. 23, pp. 909-917, 1973.
[38] R. Heddur and S. Khopkar, "Reversed phase extraction chro-matographic separation of antimony (III) with trioctyl phosphine oxide," Journal of liquid chromatography, vol. 8, pp. 95-106, 1985.
[39] A. Tayeb, G. Goetz-Grandmont, J. Brunette, and M. Leroy, "ANALYTICAL AND SPECTROSCOPIC STUDY OF ZINC EXTRACTION WITH 1, 10-BIS [1-PHENYL-3-METHYL-5-HYDHOXY-1-PYFAZOLYL]-1, 10-DECANEDIONE AND THI-n-OCTYLPHOSPHINE OXIDE," Solvent Extraction and Ion Exchange, vol. 8, pp. 1-34, 1990.
[40] Y. Hasegawa, I. Kobayashi, and S. Yoshimoto, "Extraction of palladium (II) and platinum (IV) as chlorocomplex acids into basic organic solvents," Solvent Extraction and Ion Exchange, vol. 9, pp. 759-768, 1991.
[41] M. Zapatero, M. Olazabal, M. Elizalde, and J. Castresana, "SOLVENT EXTRACTION OF COPPER (II) WITH THE ACTIVE COMPONENT OF LIX 54. SYNERGIC EFFECT IN THE PRESENCE OF TRI-n-OCTYLPHOSPHINE OXIDE," SOLVENT EXTRACTION AND ION EXCHANGE, vol. 9, pp. 177-194, 1991.
[42] F. Bunuş and R. Dumitrescu, "Simultaneous extraction of rare earth elements and uranium from phosphoric acid," Hydrometallurgy, vol. 28, pp. 331-338, 1992.
[43] I. Lav and G. Hayward, "Recovery of fatty acids by immobilized solvent extraction," The Canadian Journal of Chemical Engineering, vol. 68, pp. 376-381, 1990.
[44] T. SERINE, Y. KATAYAMA, Y. WAKABAYASHI, and H. NAGANAWA, "Solvent extraction of picric acid from acid aqueous solutions into cyclohexane with trioctylphosphine oxide and trioctylamine," Solvent Extraction and Ion Exchange, vol. 7, pp. 73-86, 1989.
[45] A. Ohki, Y. Fujino, K. Ohmori, and M. Takagi, "A POSSIBLE USE OF PHOTO-REACTION IN LIQUID-LIQUID EXTRACTION OF SUBSTITUTION-INERT METAL COMPLEXES. EXTRACTION OF CHROMIUM (III) AND COBALT (III) COMPLEXES," Solvent Extraction and Ion Exchange, vol. 4, pp. 639-662, 1986.
[46] J. White and W. Ross, "Extraction of chromium with trioctylphosphine oxide," Oak Ridge National Lab., Tenn.1957.
[47] P. Santhi, M. Reddy, T. Ramamohan, and A. Damodaran, "Liquid-liquid extraction of yttrium (III) with mixtures of organophosphorus extractants: theoretical analysis of extraction behaviour," Hydrometallurgy, vol. 27, pp. 169-177, 1991.
[48] X. Wang, W. Li, S. Meng, and D. Li, "The extraction of rare earths using mixtures of acidic phosphorus‐based reagents or their thio‐analogues," Journal of Chemical Technology & Biotechnology: International Research in Process, Environmental & Clean Technology, vol. 81, pp. 761-766, 2006.
[49] M. Tian, N. Song, D. Wang, X. Quan, Q. Jia, W. Liao, et al., "Applications of the binary mixture of sec-octylphenoxyacetic acid and 8-hydroxyquinoline to the extraction of rare earth elements," Hydrometallurgy, vol. 111, pp. 109-113, 2012.
[50] T. Miaomiao, J. Qiong, and L. Wuping, "Studies on synergistic solvent extraction of rare earth elements from nitrate medium by mixtures of 8-hydroxyquinoline with Cyanex 301 or Cyanex 302," Journal of Rare Earths, vol. 31, pp. 604-608, 2013.
[51] H. Tong, Y. Wang, W. Liao, and D. Li, "Synergistic extraction of Ce (IV) and Th (IV) with mixtures of Cyanex 923 and organophosphorus acids in sulfuric acid media," Separation and Purification Technology, vol. 118, pp. 487-491, 2013.
[52] A. Yadollahi, K. Saberyan, M. Torab-Mostaedi, A. Charkhi, and M. R. Pourjavid, "Solvent extraction separation of zirconium and hafnium from nitric acid solutions using mixture of Cyanex-272 and TBP," Radiochimica Acta, 2018.
[53] A. Babakhani, F. Rashchi, A. Zakeri, and E. Vahidi, "Selective separation of nickel and cadmium from sulfate solutions of spent nickel–cadmium batteries using mixtures of D2EHPA and Cyanex 302," Journal of Power Sources, vol. 247, pp. 127-133, 2014.
[54] M. Noori, F. Rashchi, A. Babakhani, and E. Vahidi, "Selective recovery and separation of nickel and vanadium in sulfate media using mixtures of D2EHPA and Cyanex 272," Separation and Purification Technology, vol. 136, pp. 265-273, 2014.
[55] D. Bi and Y. Xu, "Synergism between Fe2O3 and WO3 particles: Photocatalytic activity enhancement and reaction mechanism," Journal of Molecular Catalysis A: Chemical, vol. 367, pp. 103-107, 2013.
[56] F. Hadri, A. Besq, S. Guillou, and R. Makhloufi, "Drag reduction with an aqueous solution of CTAC-NaSal: Study of the wall slip with a Couette geometry," Academie des Sciences. Comptes Rendus. Mecanique, vol. 338, pp. 152-157, 2010.
[57] Z. Lin, L. Chou, B. Lu, Y. Zheng, H. T. Davis, L. Scriven, et al., "Experimental studies on drag reduction and rheology of mixed cationic surfactants with different alkyl chain lengths," Rheologica acta, vol. 39, pp. 354-359, 2000.
[58] I. Dibrov, D. Chirkst, and T. Litvinova, "Thermodynamic analysis of cerium (III) extraction from sulfate solutions with salts of quaternary ammonium bases," Russian journal of applied chemistry, vol. 75, pp. 191-194, 2002.
[59] F. Zahakifar, R. Davarkhah, A. Charkhi, and M. Torab-Mostaedi, "Solvent extraction of uranium (VI) from leach liquor solution of Bandar Abbas Gachin ore using Alamine 336," Nuclear Science and Technology, 2017.
[60] F. A. Settle, Handbook of instrumental techniques for analytical chemistry: Prentice Hall PTR, 1997.
[61] S. G. Galbraith, P. G. Plieger, and P. A. Tasker, "Cooperative sulfate binding by metal salt extractants containing 3-dialkylaminomethylsalicylaldimine units," Chemical communications, pp. 2662-2663, 2002.
[62] B. R. Reddy, J. R. Kumar, and A. V. Reddy, "Liquid-liquid extraction of tetravalent zirconium from acidic chloride solutions using Cyanex 272," Analytical sciences, vol. 20, pp. 501-505, 2004.
[63] A. A. Maryott and E. R. Smith, Table of dielectric constants of pure liquids vol. 514: US Government Printing Office, 1951.
[64] A. M. Margarella, K. A. Perrine, T. Lewis, M. Faubel, B. Winter, and J. C. Hemminger, "Dissociation of Sulfuric Acid in Aqueous Solution: Determination of the Photoelectron Spectral Fingerprints of H2SO4, HSO4–, and SO42–in Water," The Journal of Physical Chemistry C, vol. 117, pp. 8131-8137, 2013.
[65] G. Xu, W. Wang, and J. Wu, "Extraction chemistry of the nuclear fuel (I): synergistic extraction with chelating and complexing extractants," Atomic Energy Science and Technology, vol. 7, pp. 487-508, 1963.