Colloid Transport of Plutonium in the Far-Field of the Mayak Production Association, Russia

American Association for the Advancement of Science (AAAS) - Tập 314 Số 5799 - Trang 638-641 - 2006
А. П. Новиков1,2,3,4,5, Stepan N. Kalmykov1,2,3,4,5, Satoshi Utsunomiya1,2,3,4,5, Rodney C. Ewing1,2,3,4,5, F. Horréard1,2,3,4,5, A. Merkulov1,2,3,4,5, Sue B. Clark1,2,3,4,5, В. В. Ткачев1,2,3,4,5, B. F. Myasoedov1,2,3,4,5
1Cameca, 92622 Gennevilliers Cedex, 92403, France.
2Department of Chemistry and Nuclear Radiation Center, Washington State University, Pullman, WA 99164–4630, USA.
3Department of Geological Sciences, University of Michigan, Ann Arbor, MI 48109‐1005, USA.
4Radiochemistry Division, Chemistry Department, Lomonosov Moscow State University, Moscow 119992, Russia.
5Vernadsky Institute of Geochemistry and Analytical Chemistry, Russian Academy of Sciences, Moscow, 119991, Russia

Tóm tắt

Sorption of actinides, particularly plutonium, onto submicrometer-sized colloids increases their mobility, but these plutonium colloids are difficult to detect in the far-field. We identified actinides on colloids in the groundwater from the Mayak Production Association, Urals, Russia; at the source, the plutonium activity is ∼1000 becquerels per liter. Plutonium activities are still 0.16 becquerels per liter at a distance of 3 kilometers, where 70 to 90 mole percent of the plutonium is sorbed onto colloids, confirming that colloids are responsible for the long-distance transport of plutonium. Nano–secondary ion mass spectrometry elemental maps reveal that amorphous iron oxide colloids adsorb Pu(IV) hydroxides or carbonates along with uranium carbonates.

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Tài liệu tham khảo

J. F. McCarthy, J. M. Zachara, Environ. Sci. Technol.23, 496 (1989).

J. I. Kim, Mater. Res. Soc. Bull.19, 47 (1994).

J. I. Kim, Radiochim. Acta52/53, 71 (1991).

C. Degueldre et al., Appl. Geochem.15, 1043 (2000).

J. I. Kim, Mater. Res. Soc. Symp. Proc.294, 3 (1993).

10.1021/es00072a012

R. C. Marty, D. Bennett, P. Thullen, Environ. Sci. Technol.31, 2020 (1997).

D. I. Kaplan, P. M. Bertsch, D. C. Adriano, K. A. Orlandini, Radiochim. Acta66/67, 181 (1994).

A. B. Kersting et al., Nature396, 56 (1999).

J. S. Contardi, D. R. Turner, T. M. Ahn, J. Contaminant Hydrol.47, 323 (2001).

W. L. Keeney-Kennicutt, J. W. Morse, Geochim. Cosmochim. Acta49, 2577 (1985).

A. L. Sanchez, J. W. Murray, T. H. Sibley, Geochim. Cosmochim. Acta49, 2297 (1985).

M. C. Duff et al., Environ. Sci. Technol.33, 2163 (1999).

Mayak produced Pu for nuclear weapons by reprocessing spent nuclear fuel. After more than 50 years there have been major episodes of contamination of the surrounding area—Chelyabinsk Kurgan and Sverdlovsk ( 15 16 ).

B. F. Myasoedov, E. G. Drozko, J. Alloy. Comp.271-273, 216 (1998).

G. C. Christensen et al., Sci. Total Environ.202, 237 (1997).

N. Solodov, A. V. Zotov, A. D. Khoteev, A. P. Mukhamet-Galeev, B. R. Tagirov, Appl. Geochem.13, 921 (1998).

Materials and methods are available as supporting material on Science Online.

A. P. Novikovet al. “Radiomonitoring of groundwater in the zone of Lake Karachay” (LBNL Report under Contract no. 4698-01-1 p42 Lawrence Berkeley National Laboratory Berkeley CA 1996).

The Geochemist's Workbench Release 3.1; RockWare.

V. Neck, J. I. Kim, Radiochim. Acta89, 1 (2001).

G. R. Choppin, Radiochim. Acta91, 645 (2003).

M. L. Pierce, C. B. Moore, Environ. Sci. Technol.14, 214 (1980).

N. Lu, P. W. Reimus, G. R. Parker, J. L. Conca, I. R. Triay, Radiochim. Acta91, 713 (2003).

W. Stumm, J. J. Morgan, Aquatic Chemistry: An Introduction Emphasizing Chemical Equilibria in Natural Waters (Wiley-Interscience, New York, ed. 2, 1981), pp. 627–635.

C. Kantar, B. D. Honeyman, Radiochim. Acta93, 757 (2005).

D. L. Clark, D. R. Hobart, M. P. Neu, Chem. Rev.95, 25 (1995).

P. Vitorge, H. Capdevila, Radiochim. Acta91, 623 (2003).

The work was supported by The Office of Basic Energy Sciences of the U.S. Department of Energy (DE-FG02-04ER15582 and DE-FG03-01ER15168) Russian Academy of Sciences (RC0-20003-SC14 and RG0-20102-RW40) and by Russian Basic Research Foundation (05-03-33028). We thank W. Halsey (Lawrence Livermore National Laboratory) for useful discussion.