Abstract
An attempt has been made in the present work to investigate the role of anion for the uptake of Am(III)/Eu(III)/U(VI) by extraction chromatography (EXC) resin incorporating tetra-n-octyl-3-oxapentanediamide, commonly referred to as tetra-octyl diglycolamide (TODGA). In contrast to the nitric acid, perchloric acid medium favors extraction of trivalent metal ions even at low acidity (pH 2) and is almost insensitive to the acidity up to 5 M. Exceptionally large distribution coefficients (105–106) in the wide range of perchlorate concentration (10−2–5 M) is quite unusual and is by far the largest reported in the literature for Am(III)/Eu(III). Thermodynamic data suggests the possibility of inner sphere/cation exchange mechanism involving TODGA aggregates at higher acidity but outer sphere/cation exchange mechanism at low acidity for Eu(III). There is a possibility of employing TODGA based EXC resin for the remediation of liquid waste (contaminated with long lived transuranics like 241/243Am and 245Cm) in the wide range of acidity.
Similar content being viewed by others
References
IAEA Publication (2006) Nuclear power and sustainable development 06-30481
NEA 6962 (2010) Technology roadmap, nuclear energy
EPRI (2010) Advanced nuclear fuel cycles—main challenges and strategic choices, 1020307. EPRI, Palo Alto
The future of the nuclear fuel cycle (2011) MIT study, ISBN 978-0-9828008-4-3
Magill J, Berthou V, Haas D, Galy J, Schenkel R, Wiese H, Heusener G, Tommasi J, Youinou G (2003) Impact limits of partitioning and transmutation scenarios on radiotoxicity of actinides in radioactive waste. Nucl Energy 42:263–277
Nagyl S (2007) Nuclear waste management and nuclear fuel cycle in radiochemistry and nuclear chemistry. Encyclopedia of life support system (EOLSS Publishers), Oxford
Madic C, Testard F, Hudson MJ, Liljenzin J,Christansen B, Ferrando M, Facchini A, Geist A, Modolo G, Espartero G , Mendoza J (2004) New solvent extraction process for minor actinides-final report. CEA-report
Ansari SA, Pathak P, Mohapatra PK, Manchanda VK (2011) Aqueous partitioning of minor actinides by different processes. Sep Purif Rev 40:43–76
Andersson S, Drouet F, Ekberg C, Liljenzin J, Magnusson D, Nilsson M, Retegan T, Skarnemark G (2005) Partitioning and transmutation, annual report 2004, Chalmers University of Technology
Christiansen B, Apostolidis C, Carlos R, Malmbeck R, Pagliosa G, Romer K, Purroy DS (2004) Advanced aqueous reprocessing in P&T strategies: process demonstrations on genuine fuels and targets. Radiochim Acta 92:475–480
Horwitz EP, Kalina DG, Diamond H, Vandegrift GF, Schulz WW (1985) The TRUEX process—a process for the extraction of the transuranic elements from nitric acid in wastes utilizing modified PUREX solvent. Solvent Extr Ion Exch 3:75–109
Mahajan GR, Prabhu DR, Manchanda VK, Badheka LP (1998) Substituted malonamides as extractants for partitioning of actinides from nuclear waste solutions. Waste Manag 18:125–133
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 19:91–103
Tachimori S, Sasaki Y, Suzuki SI (2002) Modification of TODGA-n-dodecane solvent with a monoamide for high loading of lanthanides(III) and actinides(III). Solvent Extr Ion Exch 20:687–699
Jensen MP, Yaita T, Chiarizia R (2007) Reverse-micelle formation in the partitioning of trivalent F-element cations by biphasic systems containing a tetraalkyldiglycolamide. Langmuir 23(9):4765–4774
Ganguly R, Sharma JN, Choudhury N (2011) TODGA based w/o micro emulsion in dodecane: an insight into the micellar aggregation characteristics by dynamic light scattering and viscometry. J Colloid Interface Sci 355:458–463
Pathak PN, Ansari SA, Kumar S, Tomar BS, Manchanda VK (2010) Dynamic light scattering study on the aggregation behaviour of N,N,N’,N’-tetraoctyldiglycolamide (TODGA) and its correlation with the extraction behaviour of metal ions. J Colloid Interface Sci 342:114–118
Yaita T, Herlinger AW, Thiyagarajan P, Jensen MP (2004) Influence of extraction aggregation the extraction of trivalent F-element cations by a tetraalkyldiglycolamide. Solvent Extr Ion Exch 22:553–571
Nave S, Modolo G, Madic C, Testard F (2004) Aggregation properties of N,N,N’,N’-tetraoctyl-3-oxapentanediamide (TODGA) in n-dodecane. Solvent Extr Ion Exch 22:527–551
Ansari SA, Pathak PN, Hussain M, Prasad AK, Parmar VS, Manchanda VK (2005) N,N,N′,N′-tetraoctyl diglycolamide (TODGA): a promising extractant for actinide-partitioning from high-level waste (HLW). Solvent Extr Ion Exch 23:463–479
Smirnov IV (2007) Anomalous effects in extraction of lanthanides and actinides with bidentate neutral organophosphorus extractants: role of proton hydrate solvates. Radiochemistry 49:44–54
Rozen AM, Krupnov BV (1996) Usp Khim 65:1052–1079
Horwitz EP, McAlister DR, Dietz ML (2006) Extraction chromatography versus solvent extraction: how similar are they? Sep Sci Technol 41:2163–2182
Horwitz EP, Chiarizia R, Dietz ML, Diamond H, Nelson DM (1993) Separation and preconcentration of actinides from acidic media by extraction chromatography. Anal Chim Acta 281:361–372
Gopalakrishnan V, Dhami PS, Ramanujam A, Balarama Krishna MV, Murali MS, Mathur JN, Iyer RH, Bauri AK, Banerji A (1995) Extraction and extraction chromatographic separation of minor actinides from sulphate bearing high level waste solutions using CMPO. J Radioanal Nucl Chem 191(2):279–289
Ansari SA, Murali MS, Pathak PN, Manchanda VK (2004) Extraction chromatography of actinides using cyanex-923 as stationary phase. Solvent Extr Ion Exch 22(6):1013–1036
Pietrelli L, Salluzzo A, Troiani F (1990) Sorption of europium and actinides by means of octyl(phenyl)-N, N-diisobutyl carbamoylmethyl phosphine oxide (CMPO) loaded on silica. J Radioanal Nucl Chem 141(1):107–115
Ansari SA, Pathak PN, Husain M, Prasad AK, Parmar VS, Manchanda VK (2006) Extraction chromatographic studies of metal ions using N,N,N′,N′-tetraoctyl diglycolamide as the stationary phase. Talanta 68:1273–1280
Shaibu BS, Reddy MLP, Murali MS, Manchanda VK (2007) N,N,N′,N′-tetraoctyl-3-oxapentane-1,5-diamide impregnated magnetic particles for the uptake of lanthanides and actinides from nuclear waste streams. Radiochim Acta 95(3):159–164
Hecke KV, Modolo GJ (2004) Separation of actinides from low level liquid wastes (LLLW) by extraction chromatography using novel DMDOHEMA and TODGA impregnated resins. Radioanl Nucl Chem 261(2):269–275
Horwitz EP, McAlister DR, Bond AH, Barrans RE (2005) Novel extraction of chromatographic resins based on tetraalkyldiglycolamides: characterization and potential applications. Solvent Extr Ion Exch 23(3):319–344
Modolo G, Asp H, Schreinemachers und C, Vijgen H (2004) Recovery of actinides and lanthanides from high-level liquid waste by extraction chromatography using TODGA+TBP impregnated resins. Radiochim Acta 95(7):391–397
Hoshi H, Wei YZ, Kumagai M, Asakura T, Morita Y (2004) Group separation of trivalent minor actinides and lanthanides by TODGA extraction chromatography for radioactive waste management. J Alloy Compd 3741(2):451–455
Zhang A, Wei Y, Hoshi H, Kumagai M, Kamiya M, Koyama T (2005) Resistance properties of a macroporous silica-based N,N,N′,N′-tetraoctyl-3-oxapentane-1,5-diamide-impregnated polymeric adsorption material against nitric acid, temperature and γ-irradiation. Radiat Phys Chem 72:669–678
Zhang A, Kuraoka E, Kumagai M (2006) Removal of Pd(II), Zr(IV), Sr(II), Fe(III), and Mo(VI) from simulated high level liquid waste by extraction chromatography utilizing the macroporous silica-based polymeric materials. Sep Purif Technol 50(1):35–44
Zhang A, Wei Y, Hoshi H, Kumagai M (2005) Chromatographic separation of strontium(II) from a nitric acid solution containing some typically simulated elements by a novel silica-based TODGA impregnated polymeric composite in the MAREC process. Solvent Extr Ion Exch 23(2):231–247
Zhang A, Kuraoka E, Hoshi H, Kumagai M (2004) Synthesis of two novel macroporous silica-based impregnated polymeric composites and their application in highly active liquid waste partitioning by extraction chromatography. J Chromatgr A 1061(2):175–182
Pourmand A, Dauphas N (2010) Distribution coefficients of 60 elements on TODGA resin: application to Ca, Lu, Hf, U and Th isotope geochemistry. Talanta 81(3):741–753
Kim SY, Xu Y, Ito T, Wu Y, Tada T, Hitomi K, Kuraoka E, Ishii K (2013) A novel partitioning process for treatment of high level liquid waste using macroporous silica-based adsorbents. J Radioanal Nucl Chem 295(2):1043–1050
Xu Y, Kim S-Y, Usuda S, Wei Y, Ishii K (2013) Adsorption and desorption behavior of tetravalent zirconium onto a silica-based macroporous TODGA adsorbent in HNO3 solution. J Radioanal Nucl Chem 297(1):91–96
Deb AKS, Ilaiyaraja P, Ponraju D, Venkatraman B (2012) Diglycolamide functionalized multi-walled carbon nanotubes. J Radioanal Nucl Chem 291:877–883
Manchanda VK, Pathak PN (2004) Amides and diamides as promising extractants in the back end of the nuclear fuel cycle: an overview. Sep Purif Technol 35:85–103
Manchanda VK, Mohapatra PK, Veeraraghavan R (1996) 3-Phenyl-4-benzoyl-5-isoxazolone: a promising chelate extractant for actinide separation from acidic nuclear waste solutions. Anal Chim Acta 320:151–154
Ahrland S, Lizenzin JD, Rydberg J (1973) In: Bailar JC, Emeleus HJ, Nyholm R, Trotman-Dickenson AF (eds) Comprehensive inorganic chemistry. Pergamon Press, Oxford, p 577
Mohapatra PK, Manchanda VK (1991) Complexation of Am(III) with crown ethers in aqueous phase. Radiochim Acta 55:193–197
Sasaki Y, Choppin GR (1996) Solvent extraction of Eu, Th, U, Np and Am with N,N’-dimethyl-N,N’-dihexyl-3-oxapentanediamide and its analogous compounds. Anal Sci 12:225–230
Shannon RD, Prewitt CT (1969) Effective ionic radii in oxides and fluorides. Acta Crystallogr B25:925–946
Ahrland S, Lizenzin JD, Rydberg J (1973) In: Bailar JC, Emeleus HJ, Nyholm R, Trotman-Dickenson AF (eds) Comprehensive inorganic chemistry. Pergamon Press, Oxford, p 477
Andersson S, Ekberg C, Liljenzin J-O, Nilsson M, Skarnemark G (2004) Study of nitrate complex formation with trivalent Pm, Eu, Am and Cm using a solvent extraction technique. Radiochim Acta 92:863–867
Acknowledgements:
This research was supported by the National Research Foundation of Korea funded by the Ministry of Education, Science and Technology to V.K.M. (R31-2008-10029 under WCU program). Authors would like to acknowledge the cooperation and support of Mr Sangbok Lee, RI centre, CCRF, SKKU for experimental work with radionuclides.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Vyas, C.K., Joshirao, P.M., Bagla, H. et al. Distribution behavior of U(VI), Am(III) and Eu(III) on diglycolamide based extraction chromatographic resin in perchloric acid medium. J Radioanal Nucl Chem 298, 1643–1650 (2013). https://doi.org/10.1007/s10967-013-2642-4
Received:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10967-013-2642-4