Transport of low 240 Pu/ 239 Pu atom ratio plutonium-species in the Ob and Yenisey Rivers to the Kara Sea

Abstract Plutonium (Pu) isotope ratios can be used to differentiate between sources of Pu contamination such as nuclear weapon production, weapon fallout as well as accidental and routine releases from nuclear installations. To obtain information on the contamination level, speciation and sources of Pu in the Ob and Yenisey river systems (Siberia, Russia) and the adjacent Kara Sea, water was size fractionated onboard ship and the concentrations and atom ratios of 240 Pu and 239 Pu in obtained water fractions (i.e. particles, colloids and low molecular mass species) were determined by accelerator mass spectrometry (AMS). Results show a clear difference in speciation between high 240 Pu/ 239 Pu atom ratio Pu derived from global weapon fallout and low 240 Pu/ 239 Pu atom ratio Pu, presumably originating from weapons grade Pu. In particular, the 240 Pu/ 239 Pu atom ratios (mean 0.18 ± 0.06) for particles (> 0.45 μm) could not be distinguished from global fallout Pu (0.17–0.19), whereas for low molecular mass (LMM; 240 Pu/ 239 Pu atom ratio 0.052 ± 0.023), where the difference was statistically significant (paired t -test, P  = 0.02, n  = 4). The low 240 Pu/ 239 Pu atom ratios in filtered ( 239,240 Pu in filtered ( − 3 in the rivers, somewhat higher than in the open Kara Sea (2.4–7.7 mBq m − 3 ) in agreement with previously reported values.

[1]  V. Rachold,et al.  Geochemical Processes in the Yenisei River and Estuary , 2003 .

[2]  V. Gordeev.  River Input of Water, Sediment, Major Ions, Nutrients and Trace Metals from Russian Territory to the Arctic Ocean , 2000 .

[3]  A. Bolsunovsky.  Artificial radionuclides in aquatic plants of the Yenisei River in the area affected by effluents of a Russian plutonium complex , 2004, Aquatic Ecology.

[4]  Bolsunovsky AYa,et al.  Hot particles of the Yenisei River flood plain, Russia. , 2001, Journal of environmental radioactivity.

[5]  G. Millward.  Processes affecting trace element speciation in estuaries. A review , 1995 .

[6]  R. Stein,et al.  Siberian River run-off in the Kara Sea : characterisation, quantification, variability, and environmental significance , 2003 .

[7]  R. Stein,et al.  Scientific Cruise Report of the Kara-Sea Expedition 2001 of RV "Akademik Boris Petrov": The German-Russian Project on Siberian River Run-off (SIRRO) and the EU Project "ESTABLISH" , 2002 .

[8]  P. Mitchell,et al.  Transport of plutonium in surface and sub-surface waters from the Arctic shelf to the North Pole via the Lomonosov Ridge. , 2002, Journal of environmental radioactivity.

[9]  L. K. Fifield,et al.  Accelerator mass spectrometry of plutonium isotopes , 1996 .

[10]  M. I. Vorobiova,et al.  Review of historical monitoring data on Techa River contamination. , 1999, Health physics.

[11]  J. Grebmeier,et al.  Distributions of nuclear fuel-reprocessing tracers in the Arctic Ocean: Indications of Russian river influence , 1999 .

[12]  H. Palmer.  Environmental radioactivity in the Arctic, Antarctic , 1993 .

[13]  V. Tcherkezian,et al.  Forms of contamination of the environment by radionuclides after the Tomsk accident (Russia, 1993) , 1995 .

[14]  A. W. Morris,et al.  Distributions and behaviour of dissolved Cu, Zn and Mn in the Tamar estuary , 1986 .

[15]  R. H. Meade,et al.  World-Wide Delivery of River Sediment to the Oceans , 1983, The Journal of Geology.

[16]  Peter Wadhams,et al.  The freshwater budget of the Arctic Ocean , 2000 .

[17]  H. Eicken,et al.  The potential transport of pollutants by Arctic sea ice , 1995 .

[18]  I. Harms,et al.  Salt intrusions in Siberian River Estuaries - Observations and model experiments in Ob and Yenisei , 2002 .

[19]  F. Sayles,et al.  The history and source of particulate 137Cs and 239,240Pu deposition in sediments of the Ob River Delta, Siberia. , 1997, The Science of the total environment.

[20]  V. N. Potapov,et al.  Radioactive contamination of the Balchug (Upper Yenisey) floodplain, Russia in relation to sedimentation processes and geomorphology. , 2005, The Science of the total environment.

[21]  Sabine Charmasson,et al.  Importance of colloids in the transport within the dissolved phase (<450 nm) of artificial radionuclides from the Rhône river towards the Gulf of Lions (Mediterranean Sea). , 2004, Journal of environmental radioactivity.

[22]  R. Wollast,et al.  Ocean margin processes in global change. , 1991 .

[23]  S. B. Moran,et al.  Sources and transport of anthropogenic radionuclides in the Ob River system, Siberia , 2000 .

[24]  J. Grebmeier,et al.  Sources of the transuranic elements plutonium and neptunium in arctic marine sediments , 2000 .

[25]  A. Spitzy,et al.  Role of Suspended Matter and Dissolved Organic Substances in Behavior and Migration of Anthropogenic Radionuclides in River-Sea Aquatic Systems , 2003 .

[26]  L. León Vintró,et al.  Trends in plutonium, americium and radiocaesium accumulation and long-term bioavailability in the western Irish Sea mud basin , 1999 .

[27]  Brit Salbu,et al.  AMAP Assessment 2002: Radioactivity in the Arctic , 2004 .

[28]  B. Salbu,et al.  Speciation of 137Cs and 90Sr in discharges from the pulp industry and the marine recipient , 1996 .

[29]  L. K. Fifield,et al.  Plutonium from Mayak : Measurement of isotope ratios and activities using accelerator mass spectrometry , 2000 .

[30]  F. Sayles,et al.  The distribution and history of nuclear weapons related contamination in sediments from the Ob River, Siberia as determined by isotopic ratios of plutonium and neptunium. , 2002, Journal of environmental radioactivity.

[31]  E. Carmack,et al.  The role of sea ice and other fresh water in the Arctic circulation , 1989 .

[32]  D. Oughton,et al.  Plutonium isotope ratios in the Yenisey and Ob estuaries. , 2004, Applied radiation and isotopes : including data, instrumentation and methods for use in agriculture, industry and medicine.

[33]  K. Compton,et al.  Releases of Radionuclides to Surface Waters at Krasnoyarsk-26 and Tomsk-7 , 1999 .

[34]  Y. Savitsky,et al.  Radioactive contamination of the Yenisei River , 1995 .

[35]  A. Aarkrog,et al.  Determination of plutonium in environmental samples by controlled valence in aniion exchange , 1993 .

[36]  D. Unger,et al.  Recent particulate organic carbon and total suspended matter fluxes from the Ob and Yenisei Rivers into the Kara Sea (Siberia) , 2004 .

[37]  Brit Salbu,et al.  Trace Elements in Natural Waters , 1994 .

[38]  A. Aarkrog,et al.  Isotopic Pu, U, and Np signatures in soils from semipalatinsk-21, Kazakh Republic and the Southern Urals, Russia , 1998 .

[39]  P. Day,et al.  Accelerator mass spectrometry measurement of 240Pu/239Pu isotope ratios in Novaya Zemlya and Kara Sea sediments. , 2004, Applied radiation and isotopes : including data, instrumentation and methods for use in agriculture, industry and medicine.

[40]  Arctic Monitoring and Assessment Programme.  AMAP Assessment Report: Arctic Pollution Issues , 1998 .

[41]  K. Buesseler,et al.  Size-fractionated plutonium isotopes in a coastal environment. , 2001, Journal of environmental radioactivity.

[42]  J. Martin,et al.  First data on trace metal level and behaviour in two major Arctic river-estuarine systems (Ob and Yenisey) and in the adjacent Kara Sea, Russia , 1995 .

[43]  Michael Karcher,et al.  Modelling Siberian river runoff — implications for contaminant transport in the Arctic Ocean , 2000 .

[44]  T. Beasley,et al.  Global distribution of Pu isotopes and 237Np. , 1999, The Science of the total environment.

[45]  Tritium in surface waters of the Yenisei River basin. , 2003, Journal of environmental radioactivity.

[46]  J. M. Martin,et al.  A reassessment of the Eurasian river input of water, sediment, major elements, and nutrients to the Arctic Ocean , 1996 .

[47]  D. K. Smith,et al.  Migration of plutonium in ground water at the Nevada Test Site , 1999, Nature.

[48]  J. Milliman,et al.  Flux and fate of fluvial sediment and water in coastal seas , 1991 .

[49]  A. I. Sobolev,et al.  New data on the content of transuranic elements in bottom sediments of the Yenisei River , 2002 .