Abstract
In order to directly separate trivalent minor actinides (MA: Am, Cm) from fission products (FP) containing rare earths (RE) in high level radioactive liquid waste (HLLW), the authors have challenged to develop a simplified MA separation process by extraction chromatography using a single column. Attention has been paid to a new type of nitrogen-donor ligands, R-BTP (2,6-bis(5,6-dialkyl-1,2,4-triazin-3-yl) pyridine, R: alkyl group) as an extractant because it shows high extraction selectivity for Am(III) over RE(III). It is known that the R-BTP ligands show different properties such as adsorbability and stability by having different alkyl groups. Therefore, some novel adsorbents were prepared by impregnating different types of R-BTP ligands (isohexyl-, isoheptyl- and cyheptyl-BTP) and a similar ligand to the R-BTP, ATP (2,6-bis(1-aryl-1H-tetrazol-5-yl)pyridines), into the porous silica/polymer support (SiO2-P particles). This work deals with comparison in adsorption and desorption properties of Am and some FP in HNO3 solution onto such R-BTP type adsorbents, as well as chemical and radiolytic stability of the adsorbents. Then the possibility of a single-column separation of MA from main FP was pursued by evaluating the results of column experiments using the most promising adsorbent (isohexyl-BTP/SiO2-P) under temperature control. In addition, elution behaviors of U and Pd were also estimated.
Similar content being viewed by others
References
Kolarik Z, Mullich U, Gassner F. Selective extraction of Am(III) over Eu(III) by 2,6-ditriazoyl- and 2,6-ditriazinylpyridines. Solv Extr Ion Exch, 1999, 17: 23–32
Kolarik Z, Mullich U, Gassner F. Extraction of Am(III) and Eu(III) nitrates by 2,6-di-(5,6-dipropyl-1,2,4-triazine-3-yl-) pyridines. Solv Extr Ion Exch, 1999, 17: 1155–1170
Ekberg K, Fermvik A, Retegan T, Skarnemark G, Foreman MRS, Hudson MJ, Englund S, Nilsson M. An overview and historical look back at the solvent extraction using nitrogen donor ligands to extract and separate An(III) from Ln(III). Radiochim Acta, 2008, 96: 225–233
Wei YZ, Hoshi H, Kumagai M. A hot test on minor actinides/ lanthanides separation from HLLW using an R-BTP extraction resin. Proceedings of 16 th Pacific Basin Nuclear Conference (16PBNC), Aomori, Japan, Oct. 13–18, 2008, Paper ID P16 P1033
Zhang A, Kuraoka E, Kumagai M. Preparation of a novel macroporous silica-based 2,6-bis(5,6-diisobutyl-1,2,4-triazine-3-yl)pyridine impregnated polymeric composite and its application in the adsorption for trivalent rare earths. J Radioanal Nucl Chem, 2007, 274: 455–464
Hoshi H, Wei YZ, Kumagai M, Asakura T, Morita Y. Separation of trivalent actinides from lanthanides by using R-BTP resins and stability of R-BTP resin. J Alloys Comp, 2006, 408–412: 1274–1277
Wei YZ, Hoshi H, Kumagai M, Asakura T, Morita Y. Separation of Am(III) and Cm(III) from trivalent lanthanides by 2,6-bistriazinyl pyridine extraction chromatography for radioactive waste management. J Alloys Comp, 2004, 374: 447–450
Wei YZ, Hoshi H, Kumagai M, Asakura T, Uchiyama G. Preparation of novel silica-based R-BTP extraction-resins and their application to trivalent actinides and lanthanides separation. J Nucl Sci Technol, 2002, Suppl. 3: 761–764
Wei YZ, Sabharwal KN, Kumagai M, Asakura T, Uchiyama G, Fujine S. Preparation of novel silica-based nitrogen donor extraction resins and their adsorption performance for trivalent americium and lanthanides. J Nucl Sci Technol, 2000, 37: 1108–1109
Wei YZ, Kumagai M, Takashima Y, Modolo G, Odoj R. Studies on the separation of minor actinides from high-level wastes by extraction chromatography using novel silica-based extraction resins. Nucl Technol, 2000, 132: 413–423
Usuda S, Liu R, Wei YZ, Xu Y, Yamazaki H, Wakui Y. Evaluation study on properties of a novel R-BTP extraction resin-From a viewpoint of simple separation of minor actinides. J Ion Exch, 2010, 21: 35–40
Liu R, Wei YZ, Xu Y, Usuda S, Yamazaki H, Ishii K. Evaluation study on properties of isohexyl-BTP/SiO2-P resin for direct separation of trivalent minor actinides from HLLW. J Radioanal Nucl Chem, 2012, 292: 537–544
Usuda S, Wei YZ, Xu Y, Liu Z, Li R, Kim SY, Wakui Y, Hayashi H, Yamazaki H. Development of a simplified separation process of trivalent minor actinides from fission products using novel R-BTP/SiO2-P adsorbents. J Nucl Sci Technol, 2012, 49: 334–342
Smirnov IV, Chirkov AV, Babain VA, Pokrovskaya EYu, Artamonova TA. Am and Eu extraction from acidic media by synergistic mixtures of substituted bis-tertrazolyl pyridines with chlorinated cobalt dicarbollide. Radiochim Acta, 2009, 97: 593–601
Wei YZ, Horiguchi K, Kumagai M, Bruggeman A, Goethals P. Palladium removal from spent nuclear fuel solution using SiPyR-N3 anion exchanger. Ion exchange technology for today and tomorrow, Cox M (ed.), SCI, London, 2004, 103–110
Sano Y, Surugaya N, Yamamoto M. Selective recovery of minor trivalent actinides from high level liquid waste by R-BTP/SiO2-P adsorbents. Actinides 2009 (IOP Conf. Series: Materials Science and Engineering 9, 012064), 2010, 1–8
Surugaya N, Sano Y, Yamamoto M, Kurosawa A, Hiyama T. Extraction chromatographic separation of trivalent minor actinides using Hex-BTP/SiO2-P resin. American Chemical Society, ACS Symposium Series 1046 (Nuclear Energy and the Environment) (ISBN: 978-0-8414-2585-5), 2010, 131–139
Matsumura T, Matsumura K, Morita Y, Koma Y, Sano Y, Nomura K. Separation of trivalent minor actinides from fission products using single R-BTP column extraction chromatography. J Nucl Sci Technol, 2011, 48: 855–858
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Usuda, S., Wei, Y., Liu, R. et al. Challenges to develop single-column MA(III) separation from HLLW using R-BTP type adsorbents. Sci. China Chem. 55, 1732–1738 (2012). https://doi.org/10.1007/s11426-012-4691-x
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11426-012-4691-x