publication . Article . 2015

Rapid selective separation of americium/curium from simulated nuclear forensic matrices using triazine ligands

Matthew A. Higginson; Paul Thompson; Olivia J. Marsden; Francis R. Livens; Laurence M. Harwood; Frank W. Lewis; Michael J. Hudson; Sarah L. Heath;
Open Access English
  • Published: 28 Jan 2015
  • Publisher: De Gruyter
  • Country: United Kingdom
Abstract
In analysis of complex nuclear forensic samples\ud containing lanthanides, actinides and matrix elements,\ud rapid selective extraction of Am/Cm for quantification\ud is challenging, in particular due the difficult separation\ud of Am/Cm from lanthanides. Here we present\ud a separation process for Am/Cm(III) which is achieved\ud using a combination of AG1-X8 chromatography followed\ud by Am/Cm extraction with a triazine ligand. The ligands\ud tested in our process were CyMe4-BTPhen, CyMe4-\ud BTBP, CA-BTP and CA-BTPhen. Our process allows for\ud purification and quantification of Am and Cm (recoveries\ud 80%–100%) and other major actinides in < 2d without\ud th...
Subjects
free text keywords: F100, F200, Americium, chemistry.chemical_element, chemistry, Separation process, Actinide, Thiocyanate, chemistry.chemical_compound, Curium, Ligand, Nuclear chemistry, Lanthanide, Triazine
Related Organizations
17 references, page 1 of 2

1. Mayer, K., Wallenius, M., Ray, I.: Nuclear forensics - a methodology providing clues on the origin of illicitly trafcifked nuclear materials. Analyst 130, 433 (2005). [OpenAIRE]

2. Goldstein, S. L., Hensley, C. A., Armenta, C. E., Peters, R. J.: Environmental and human monitoring of americium-241 utilizing extraction chromatography and -spectrometry. Anal. Chem. 69, 809 (1997).

3. Wallenius, M., Mayer, K.: Age determination of plutonium material in nuclear forensics by thermal ionisation mass spectrometry. Fresenius, J. Anal. Chem. 366, 234 (2000). [OpenAIRE]

4. Maxwell, S. L.: Rapid method for determination of plutonium, americium and curium in large soil samples. J. Radioanal. Nucl. Chem. 275, 395 (2008).

5. Maxwell, S. L., Culligan, B. K., Kelsey-Wall, A., Shaw, P. J.: Rapid radiochemical method for determination of actinides in emergency concrete and brick samples. Anal. Chim. Acta 701, 112 (2011). [OpenAIRE]

6. Luisier, F., Alvarado, J. A. C., Steinmann, P., Krachler, M., Froidevaux, P. J.: A new method for the determination of plutonium and americium using high pressure microwave digestion and alpha-spectrometry or ICP-SMS. Radioanal. Nucl. Chem. 281, 425 (2009). [OpenAIRE]

7. Lewis, F. W., Hudson, M. J., Harwood, L. M.: Development of highly selective ligands for separations of actinides from lanthanides in the nuclear fuel cycle. Synlett 2609 (2011).

8. Adam, C., Kaden, P., Beele, B. B., Müllich, U., Trumm, S., Geist, A., Panak, P. J., Denecke, M. A.: Evidence for covalence in a N-donor complex of americium(III). Dalton Trans. 42, 14068 (2013).

9. Lewis, F. W., Harwood, L. M., Hudson, M. J., Drew, M. G. B., Desreux, J. F., Vidick, G., Bouslimani, N., Modolo, G., Wilden, A., Sypula, M., Vu, T.-H., Simonin, J.-P.: Highly eficient separation of actinides from lanthanides by a phenanthroline-derived bis-triazine ligand. J. Am. Chem. Soc. 133, 13093 (2011).

10. Modolo, G., A. Wilden, A. Geist, D., Magnusson, R., Malmbeck, A.: Review of the demonstration of innovative solvent extraction processes for the recovery of trivalent minor actinides from PUREX rafinate. Radiochim. Acta 100 (8-9), 715 (2012).

11. Higginson, M. A., Marsden, O. J,. Thompson, P., Livens F, R., Heath, S, L., Separation of americium from complex radioactive mixtures using a BTPhen extraction chromatography resin. React. Funct. Polym. DOI: 10.1016/j.reactfunctpolym.2015.05.002 (2015).

12. Trumm, S., Geist, A., Panak, P. J., Fanghänel, T.: An improved hydrolytically-stable bis-triazinyl-pyridine (BTP) for selective actinide extraction. Solvent Extr. Ion Exch. 29, 213 (2011). [OpenAIRE]

13. Hudson, M. J., Harwood, L. M., Laventine, D. M., Lewis, F. W.: Use of soft heterocyclic N-donor ligands to separate actinides and lanthanides. Inorg. Chem. 52, 3414 (2013).

14. Whittaker, D. M., Gritfihs, T. L., Helliwell, M., Swinburne, A. N., Natrajan, L. S., Lewis, F. W., Harwood, L. M., Parry, S. A., Sharrad, C. A.: Lanthanide speciation in potential SANEX and GANEX actinide/lanthanide separations using tetra-N-donor extractants. Inorg. Chem. 52, 3429 (2013).

15. Laventine, D. M., Afsar, A., Hudson, M. J., Harwood, L. M.: Tuning the solubilities of bis-triazinylphenanthroline ligands (BTPhens) and their complexes. Heterocycles 86, 1419 (2012). [OpenAIRE]

17 references, page 1 of 2
Related research
Abstract
In analysis of complex nuclear forensic samples\ud containing lanthanides, actinides and matrix elements,\ud rapid selective extraction of Am/Cm for quantification\ud is challenging, in particular due the difficult separation\ud of Am/Cm from lanthanides. Here we present\ud a separation process for Am/Cm(III) which is achieved\ud using a combination of AG1-X8 chromatography followed\ud by Am/Cm extraction with a triazine ligand. The ligands\ud tested in our process were CyMe4-BTPhen, CyMe4-\ud BTBP, CA-BTP and CA-BTPhen. Our process allows for\ud purification and quantification of Am and Cm (recoveries\ud 80%–100%) and other major actinides in < 2d without\ud th...
Subjects
free text keywords: F100, F200, Americium, chemistry.chemical_element, chemistry, Separation process, Actinide, Thiocyanate, chemistry.chemical_compound, Curium, Ligand, Nuclear chemistry, Lanthanide, Triazine
Related Organizations
17 references, page 1 of 2

1. Mayer, K., Wallenius, M., Ray, I.: Nuclear forensics - a methodology providing clues on the origin of illicitly trafcifked nuclear materials. Analyst 130, 433 (2005). [OpenAIRE]

2. Goldstein, S. L., Hensley, C. A., Armenta, C. E., Peters, R. J.: Environmental and human monitoring of americium-241 utilizing extraction chromatography and -spectrometry. Anal. Chem. 69, 809 (1997).

3. Wallenius, M., Mayer, K.: Age determination of plutonium material in nuclear forensics by thermal ionisation mass spectrometry. Fresenius, J. Anal. Chem. 366, 234 (2000). [OpenAIRE]

4. Maxwell, S. L.: Rapid method for determination of plutonium, americium and curium in large soil samples. J. Radioanal. Nucl. Chem. 275, 395 (2008).

5. Maxwell, S. L., Culligan, B. K., Kelsey-Wall, A., Shaw, P. J.: Rapid radiochemical method for determination of actinides in emergency concrete and brick samples. Anal. Chim. Acta 701, 112 (2011). [OpenAIRE]

6. Luisier, F., Alvarado, J. A. C., Steinmann, P., Krachler, M., Froidevaux, P. J.: A new method for the determination of plutonium and americium using high pressure microwave digestion and alpha-spectrometry or ICP-SMS. Radioanal. Nucl. Chem. 281, 425 (2009). [OpenAIRE]

7. Lewis, F. W., Hudson, M. J., Harwood, L. M.: Development of highly selective ligands for separations of actinides from lanthanides in the nuclear fuel cycle. Synlett 2609 (2011).

8. Adam, C., Kaden, P., Beele, B. B., Müllich, U., Trumm, S., Geist, A., Panak, P. J., Denecke, M. A.: Evidence for covalence in a N-donor complex of americium(III). Dalton Trans. 42, 14068 (2013).

9. Lewis, F. W., Harwood, L. M., Hudson, M. J., Drew, M. G. B., Desreux, J. F., Vidick, G., Bouslimani, N., Modolo, G., Wilden, A., Sypula, M., Vu, T.-H., Simonin, J.-P.: Highly eficient separation of actinides from lanthanides by a phenanthroline-derived bis-triazine ligand. J. Am. Chem. Soc. 133, 13093 (2011).

10. Modolo, G., A. Wilden, A. Geist, D., Magnusson, R., Malmbeck, A.: Review of the demonstration of innovative solvent extraction processes for the recovery of trivalent minor actinides from PUREX rafinate. Radiochim. Acta 100 (8-9), 715 (2012).

11. Higginson, M. A., Marsden, O. J,. Thompson, P., Livens F, R., Heath, S, L., Separation of americium from complex radioactive mixtures using a BTPhen extraction chromatography resin. React. Funct. Polym. DOI: 10.1016/j.reactfunctpolym.2015.05.002 (2015).

12. Trumm, S., Geist, A., Panak, P. J., Fanghänel, T.: An improved hydrolytically-stable bis-triazinyl-pyridine (BTP) for selective actinide extraction. Solvent Extr. Ion Exch. 29, 213 (2011). [OpenAIRE]

13. Hudson, M. J., Harwood, L. M., Laventine, D. M., Lewis, F. W.: Use of soft heterocyclic N-donor ligands to separate actinides and lanthanides. Inorg. Chem. 52, 3414 (2013).

14. Whittaker, D. M., Gritfihs, T. L., Helliwell, M., Swinburne, A. N., Natrajan, L. S., Lewis, F. W., Harwood, L. M., Parry, S. A., Sharrad, C. A.: Lanthanide speciation in potential SANEX and GANEX actinide/lanthanide separations using tetra-N-donor extractants. Inorg. Chem. 52, 3429 (2013).

15. Laventine, D. M., Afsar, A., Hudson, M. J., Harwood, L. M.: Tuning the solubilities of bis-triazinylphenanthroline ligands (BTPhens) and their complexes. Heterocycles 86, 1419 (2012). [OpenAIRE]

17 references, page 1 of 2
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