Abstract
A new rapid method for the determination of actinides in seawater samples has been developed at the Savannah River National Laboratory. The actinides can be measured by alpha spectrometry or inductively-coupled plasma mass spectrometry. The new method employs novel pre-concentration steps to collect the actinide isotopes quickly from 80 L or more of seawater. Actinides are co-precipitated using an iron hydroxide co-precipitation step enhanced with Ti+3 reductant, followed by lanthanum fluoride co-precipitation. Stacked TEVA Resin and TRU Resin cartridges are used to rapidly separate Pu, U, and Np isotopes from seawater samples. TEVA Resin and DGA Resin were used to separate and measure Pu, Am and Cm isotopes in seawater volumes up to 80 L. This robust method is ideal for emergency seawater samples following a radiological incident. It can also be used, however, for the routine analysis of seawater samples for oceanographic studies to enhance efficiency and productivity. In contrast, many current methods to determine actinides in seawater can take 1–2 weeks and provide chemical yields of ~30–60 %. This new sample preparation method can be performed in 4–8 h with tracer yields of ~85–95 %. By employing a rapid, robust sample preparation method with high chemical yields, less seawater is needed to achieve lower or comparable detection limits for actinide isotopes with less time and effort.
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References
Mexico Finds Stolen Radioactive Material Amid Dirty Bomb Fears. http://www.voanews.com/content/nuclear-material-stolen-in-mexico/1803195.html. Accessed 12 April 13
Japan to Spend Over $300 M On ‘Ice Wall’ To Isolate Fukushima Water Leaks. http://abcnews.go.com/Technology/japan-spend-300m-ice-wall-isolate-fukushima-water/story?id=20144627. Accessed 9 March 2013
Stricklin D, Tjarnhage A, Nygren U (2002) Application of low energy gamma-spectrometry in rapid actinide analysis for emergency preparedness. J Radioanal Nucl Chem 251(1):69–74
Maxwell S, Culligan B, Hutchison J (2013) Rapid fusion method for determination of plutonium isotopes in large rice samples. J Radioanal Nucl Chem 298:1367–1374
Hirose K (2009) Plutonium in the ocean environment: its distributions and behavior. J Nucl Radiochem Sci 10(1):R7–R16
Povinec P, Livingston H, Shima S, Aoyama M, Gastaud J, Goroncy I, Hirose K, Hynh-Ngoc L, Ikeuchi Y, Ito T, LaRosa J, Kwong LLW, Lee S-H, Moriya H, Mulsow S, Oregioni B, Pettersson H, Togawa T (2003) IAEA’97 expedition to the NW Pacific Ocean-results of oceanographic and radionuclide investigations of the water column. Deep-Sea Res II 50:2607–2637
Lee S, Gastaud J, La Rosa J, Ling Wee Kwong L, Povinec P, Wyse E, Fifield L, Hausladen P, Di Tada L, Santos G (2001) Analysis of plutonium isotopes in marine samples by radiometric, ICP-MS and AMS techniques. J Radioanal Nucl Chem 248:757–764
Maxwell S, Jones V (2009) Rapid determination of actinides in urine by inductively coupled plasma mass spectrometry and alpha spectrometry: a hybrid approach. Talanta 80(1):143–150
Ayranov M, Krahenbuhl U, Sahli H, Rollin S, Burger M (2005) Radiochemical separation of actinides from environmental samples for determination with DF-ICP-MS and alpha spectrometry. Radiochim Acta 93(5):249–258
Quinto F, Steier P, Wallner G, Wallner A, Srncik M, Bichler M, Kutschera W, Terrasi F, Petraglia A, Sabbarese C (2009) The first use of 236U in the general environment and near a shutdown nuclear power plant. Appl Radiat Isot 67:1775–1780
Hirose K, Sugimura Y (1985) A new method of plutonium speciation in seawater. J Radioanal Nucl Chem 92:363
Sidhu R (2002) A robust procedure for the determination of plutonium and americium in seawater. J Radioanal Nucl Chem 256:501–504
La Rosa J, Gastaud J, Lagan L, Lee H, Levy-Palomo I, Povinec P, Wyse E (2005) Recent developments in the analysis of transuranics (Np, Pu, Am) in seawater. J Radioanal Nucl Chem 263(2):427–436
Kim CS, Kim CK (2002) Determination of Pu isotopes in seawater by an on-line sequential injection technique with sector field inductively coupled plasma mass spectrometry. Anal Chem 74:3824–3832
Zheng J, Yamada M (2012) Determination of plutonium isotopes in seawater reference materials using isotope. Appl Radiat Isot 70(9):1944–1948
Qiao J, Hou X, Steier P, Golser R (2013) Sequential injection method for rapid and simultaneous determination of 236U, 237Np, and Pu isotopes in seawater. Anal Chem 85:11026–11033
Maxwell S, Culligan B, Utsey R (2013) Rapid determination of radiostrontium in seawater samples. J Radioanal Nucl Chem 298:867–875. doi:10.1007/s10967-013-2430-1
Maxwell S, Culligan B, Noyes G, Jones V, Nichols ST, Bernard M (2010) Rapid determination of 237Np and Pu isotopes in urine by inductively-coupled plasma mass spectrometry and alpha spectrometry. Health Phys 101(2):180–186
Zheng J, Yamada M (2006) Inductively coupled plasma-sector field mass spectrometry with a high-efficiency sample introduction system for the determination of Pu isotopes in settling particles at femtogram levels. Talanta 69:1246–1253
Epov V, Benkhedda K, Cornett RJ, Evans RD (2005) Rapid determination of plutonium in urine using flow injection on-line preconcentration and inductively-coupled plasma mass spectrometry. J Anal At Spectrom 20:424–430
Kim CS, Vajda N (2007) Determination of Pu isotope concentrations and isotope ratio by inductively coupled plasma mass spectrometry: a review of analytical methodology. J Anal At Spectrom 22:827–841
Maxwell S, Culligan B, Hutchison J, Utsey R, McAlister D (2013) Rapid determination of 210Po in water samples. J Radioanal Nucl Chem 298(3):1977–1989
Horwitz P, McAlister D, Bond A, Barrans AB Jr (2005) Novel extraction chromatographic resins based on tetraalkyldiglycolamides: characterization and potential applications. Solvent Extr Ion Exch 23(3):319
Levy I, Povinec P, Aoyama M, Hirose K, Sanchez-Cabeza J, Comanducci J, Gastaud J, Eriksson M, Hamajima Y, Kim CS, Komura K, Osvath I, Roos P, Yim S (2011) Marine anthropogenic radiotracers in the Southern Hemisphere: new sampling and analytical strategies. Prog Oceanogr 89:120–133
Currie L (1968) Limits for qualitative and quantitative determination. Anal Chem 40:586–593
Acknowledgments
This work was performed under the auspices of the Department of Energy, DOE Contract No. DE-AC09-96SR18500. The authors wish to acknowledge Staci Britt, Phil Demaere, Jack Herrington and Becky Chavous for their assistance with this work.
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Maxwell, S.L., Culligan, B.K., Hutchison, J.B. et al. Rapid determination of actinides in seawater samples. J Radioanal Nucl Chem 300, 1175–1189 (2014). https://doi.org/10.1007/s10967-014-3079-0
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DOI: https://doi.org/10.1007/s10967-014-3079-0