Abstract
We studied the stepwise formation constants (β) of water-soluble diglycolamide (DGA) and dioxaoctanediamide (DOODA) for the mutual separation of Ln in a solvent extraction system. TODGA (N,N,Nʹ,Nʹ-tetraoctyl-diglycolamide) and DOODA(C8) (N,N,Nʹ,Nʹ-tetraoctyl-dioxaoctanediamide) exhibit opposite behaviors in extracting both light and heavy Ln through Ln-patterns. Metal complexes of two- and three-folding with water-soluble DOODA and DGA, respectively, were found, and each β value was calculated using distribution ratios. Taking β, their distribution ratio, D, and separation factor, SF, values into consideration, the suitable separation conditions (aqueous phase: 30 mM DOODA(C2) in 1 M HNO3; organic phase: 0.1 M TODGA in n-dodecane) of multistage extraction (10 × 10 extraction using aqueous and organic phases, including one sample solution) were determined. In this study, La, Pr, and Nd were mainly present in the aqueous phase, whereas Sm–Dy existed in the organic phase. Although these two groups can be easily separated into two phases, the resolution, Rs, values provide for little mutual separation between La–Nd and Sm–Dy under the present conditions.
Similar content being viewed by others
References
Nishihira K, Nakayama S, Morita Y, Oigawa H, Iwasaki T (2008) Impact of partitioning and transmutation on LWR high-level waste disposal. J Nucl Sci Technol 45(1):84–97
Naito K, Matsui T, Tanaka Y (1986) Recovery of noble metals from insoluble residue of spent fuel. J Nucl Sci Technol 23(6):540–549
Manohar S, Sharna J, Shah B, Wattal P (2007) Process development for bulk separation of trivalent actinides and lanthanides from radioactive high-level liquid waste. Nucl Sci Eng 156:96–102
Jose J, Prathibha T, Karthikeyan N, Venkatesan K, Sriram S, Seshadri H, Venkatachalapathy B, Ravichandram C (2020) Studies on the separation of Am(III) from trivalent lanthanides in high-level waste solution using modifier-free solvents and aqueous soluble bis-1,2,4-triazines. J Radioanal Nucl Chem 326:1819–1829
Prathibha T, Kumaresan R, Nayak P, Venkatesan K, Subramanian G, Rajeswari S, Kalaiyarasu T, Karunakaran R, Antony M (2017) Modifier-free separation of trivalent actinides and lanthanides from fast reactor simulated high-level waste using N,N-di-octyl-2-hybroxyacetamide. J Radioanal Nucl Chem 314:2365–2375
Peng L, Yang Q, Zhang H, Xu G, Zhang M, Wang J (2008) Rare earth permanent magnets Sm2(Co, Fe, Cu, Zr)17 for high temperature applications. J Rare Earth 26(3):378–382
Rao R, Devine D (2000) RE-activated lanthanide phosphate phosphors for PDP applications. J Lumin 87–89:1260–1263
Binnemans K (2009) Lanthanide-based luminescent hybrid materials. Chem Rev 109:4283–4374
Du X, Graedel T (2011) Global In-use stocks of the rare earth elements: a first estimate. Environ Sci Technol 45:4096–4101
Topp N (1965) Chemistry of the rare-earth elements. Elsevior, New York
Siekierski S, Fidelis I (1960) Separation of some rare earths by reversed-phase partition chromatography. J Chromatogr A 4:60–64
Winchester J (1963) Rare earth choromatography using Bis-(2-ethylhexyl) orthophosphoric acid. J Chromatogr A 10:502–506
Starý J (1966) Separation of transplutonium elements. Talanta 13:421–437
Tkac P, Vandegrift G, Lumetta G, Gelis A (2012) Study of the interaction between HDEHP and CMPO and its effect on the extraction of selected lanthanides. Ind Eng Chem Res 51:10433–10444
Tachimori S, Sato A, Nakamura H (1979) Separation of transplutonium and rare-earth elements by extraction with di-isodecyl phosphoric acid from DTPA solution. J Nucl Sci Technol 16:434–440
Matsubayashi I, Ishiwata E, Shionoya T, Hasegawa Y (2004) Synergistic extraction of lanthanoids(III) with 2-thenoyltrifluoroacetone and benzoic acid: thermodynamic parameters in the complexation in organic phases and the hydration. Talanta 63:625–633
Sasaki Y, Sugo Y, Suzuki S, Tachimori S (2001) The novel extractants, diglycolamides, for the extraction of lanthanides and actinides in HNO3–n-dodecane system. Solvent Extr Ion Exch 19(1):91–103
Sasaki Y, Tachimori S (2002) Extraction of actinides(III), (IV), (V), (VI), and lanthanides(III) by structurally tailored diamides. Solvent Extr Ion Exch 20(1):21–34
Sasaki Y, Sugo Y, Suzuki S, Kimura T (2005) A method for the determination of extraction capacity and its application to N,N,Nʹ,Nʹ-tetraalkylderivatives of diglycolamide-monoamide/n-dodecane media. Anal Chim Acta 543:31–37
Sasaki Y, Morita Y, Kitatsuji Y, Kimura T (2010) Extraction behavior of actinides and metal ions by the promising extractant, N,N,N′,N′-tetraoctyl-3,6-dioxaoctanediamide (DOODA). Solvent Extr Ion Exch 28:335–349
Narita H, Yaita T, Tachimori S (2004) Extraction of lanthanides with N,N′-dimethyl-N,N′-diphenyl-malonamide and 3,6-dioxaoctanediamide. Solvent Extr Ion Exch 22(2):135–145
Nakamura S, Suzuki N (1988) Synergic extraction of lanthanide(III) ions with 2-thenoyltrifluoroacetone in the presence of 2,2ʹ-bipyridine or pyridine. Polyhedron 7(2):155–159
Imura H, Ebisawa M, Kato M, Ohashi K (2006) Novel synergism by complex ligands in solvent extraction of rare earth metals(III) with β-diketones. J Alloys Compd 408–412:952–957
Craig L, Post O (1949) Apparatus for counter current distribution. Anal Chem 21(4):500–504
Craig L, Hausmann W, Ahrens E, Harfenist E (1951) Automatic countercurrent distribution equipment. Anal Chem 23(9):1236–1244
Sasaki Y, Matsumiya M, Tsuchida Y (2020) Basic research on batchwise multi-stage extractions using TODGA for Dy/Nd separation. Anal Sci 36:1303–1309
Sasaki Y, Morita K, Matsumiya M, Ono R, Shiroishi H (2021) Fundamental study on multistage extraction using TDdDGA for separation of lanthanides present in Nd magnets. JOM 73:1037–1043
Matsutani T, Sasaki Y, Katsuta S (2021) separation of light and middle lanthanides using multistage extraction with diglycolamide extractant. Anal Sci 37:1603–1609
Jastrebova J, Witthoft C, Grahn A, Svensson U, Jagerstad M (2003) HPLC determination of folates in raw and processed beetroots. Food Chem 80:579–588
Li M, Huang J, Li T (2008) Enantiomeric separation of alcohols and amines on a proline chiral stationary phase by gas chromatography. J Chromatogr A 1191:199–204
Sasaki Y, Kitatsuji Y, Tsubata Y, Sugo Y, Morita Y (2011) Separation of Am, Cm and Ln by the solvent extraction with hydrophilic and lipophilic organic ligands. Solvent Extr Res Dev Jpn 18:93–101
Sasaki Y, Sugo Y, Kitatsuji Y, Kirishima A, Kimura T, Choppin G (2007) Complexation of various metals by water-soluble diglycolamide (DGA). Anal Sci 23:727–731
Murakami S, Matsumiya M, Sasaki Y, Suzuki S, Hisamatsu S, Takao K (2017) Investigation into coordination states of diglycolamide and dioxaoctanediamide complexes with lanthanide elements using spectroscopic methods. Solvent Extr Ion Exch 34:233–250
Wei M, He Q, Feng X, Chen J (2012) Physical properties of N, N, Nʹ, Nʹ-tetramethyl diglycolamide and thermodynamic studies of its complexation with zirconium, lanthanides and actinides. J Radioanal Nucl Chem 293:689–697
Klaβ L, Wilden A, Kreft F, Wagner C, Geist A, Panak P, Koniecko I, Narbutt J, Modolo G (2019) Evaluation of the hydrophilic complxant N,N,Nʹ,Nʹ-tetraethyldiglycolamide (TEDGA) and its methyl-substituted analogues in the selective Am(III) separation. Solvent Extr Ion Exch 37:297–312
Acknowledgements
We gratefully acknowledge Dr. M. Watanabe of the Research Group for Radiochemistry at JAEA for managing the laboratory and ensuring safety. We also thank Mr. R. Ono of Tokyo Institute of Technology, Y. Tsuchida at Yokohama National University, and T. Matsutani at Chiba University for useful information on this work.
Author information
Authors and Affiliations
Corresponding author
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Nomizu, D., Sasaki, Y., Kaneko, M. et al. Complex formation of light and heavy lanthanides with DGA and DOODA, and its application to mutual separation in DGA–DOODA extraction system. J Radioanal Nucl Chem 331, 1483–1493 (2022). https://doi.org/10.1007/s10967-022-08204-5
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10967-022-08204-5