The current content of artificial radionuclides in the water of the Tobol-Irtysh river system (from the mouth of the Iset River to the confluence with the Ob River)

Data on content of (90)Sr, (137)Cs, (239,240)Pu and (3)H in water of the Tobol-Irtysh part of the Techa-Iset-Tobol-Irtysh-Ob river system (through which the "Mayak" PA radioactive wastes are transported) are presented and discussed. The data were received in 2004-2005 under the ISTC project on radioecological monitoring of the Tobol and Irtysh rivers. Monthly observations of (137)Cs, (90)Sr and (3)H content in water in the area of the Tobol and Irtysh confluence have been conducted starting from May 2004. To obtain information on the investigated river system as a whole, the radioecological survey of the Tobol and Irtysh rivers at the section from the mouth of the Iset River to the confluence with the Ob River was carried out in 2004. It is shown that the impact of "Mayak" PA waste transport by (90)Sr is distinctly traced as far as the area of the Irtysh and Ob confluence.     

Association of plutonium with sediments from the Ob and Yenisey Rivers and Estuaries

The present study applied sequential extraction techniques to investigate the binding and mobility of plutonium (Pu) in sediments from the rivers and estuaries of the Ob and Yenisey. As a study site, the Ob and Yenisey are particularly interesting as both rivers have weapons-grade Pu sources in their catchment areas, including the Russian Pu production and reprocessing plants at Mayak, Tomsk-7 and Krashnoyarsk, and the Semipalantinsk nuclear weapons testing site in Kazakhstan. Plutonium activity and ²⁴⁰Pu/²³⁹Pu ratios were determined using accelerator mass spectrometry (AMS). Sequential extractions showed that between 47 and 80% of the Pu in Yenisey River sediments and 35–53% of the Pu in soils around the Techa River are mobilized with weak oxidising agents, which can indicate that Pu is bound to organic material. In contrast, Pu in Ob and Yenisey Estuarine sediments was more strongly bound, with 60–100% being found in the HNO₃-extractable fraction. This change in speciation could reflect either that Pu bound to organic material in the Techa and Yenisey River sediments becomes more fixed to the sediments with time, or that organic-bound Pu is mobilized and released to the water when the sediments encounter the more saline water of the Ob and Yenisey estuaries. In general, ²⁴⁰Pu/²³⁹Pu ratios were relatively consistent between different extraction fractions, although, in whole sediments, an increase in ratio was observed with distance from the source. This reflects the increased influence of weapon fallout from catchment runoff within the river systems, as compared to the weapons-grade sources close to the production and reprocessing plants. Knowledge of Pu speciation in the Ob and Yenisey Rivers, and the processes controlling its behaviour in estuarine systems, can improve predictions of its transfer and subsequent environmental impact to Arctic Seas.     

Using sequential extraction techniques to assess the partitioning of plutonium and neptunium-237 from multiple sources in sediments from the Ob River (Siberia)

Sequential extraction techniques have been developed to assess partitioning of anthropogenic radionuclides (²⁴⁰Pu, ²³⁹Pu, and ²³⁷Np), originating from a variety of sources, as identified by using bulk sediment isotopic composition. Sediments were leached sequentially with a series of six chemical treatments designed to approximate different environmental processes that may occur or to selectively extract trace metals contained in different solid phases of the sediments (i.e., exchangeable, reducible, carbonate, organic, acid leachable, and refractory). Results indicate the majority of Pu and Np is similarly distributed within many of the extracted fractions, with the largest percentage (66–97%) of both elements being observed in sediments treated with buffered citrate dithionite (CDB), which targets easily reduced constituents such as Mn and Fe hydrous oxides. While these results do indicate an association of Pu and Np with redox sensitive elements, the environmental implications are unclear given that the CDB treatment is more extreme than naturally occurring conditions. Minor amounts of Np partition differently from Pu in sediments. The NH₄-acetate treatment, which is designed to liberate trace metals that are loosely adsorbed onto the surfaces of sedimentary materials such as hydrated iron oxides and humic substances, or present at exchangeable sites in clay minerals, mobilized ∼12% of the total Np while Pu levels were below detection. The H₂O₂ treatment, which is designed to liberate trace metals bound to organic matter, mobilized ∼8 and ∼1% of Np and Pu, respectively. These results indicate that a minor portion of the total Np may be affected by environmental conditions that have little or no effect on Pu. Between 7 and 24% of the Pu was observed in treatments designed to liberate Pu and Np that are tightly bound to lithogenic phases or refractory silicates. The ²⁴⁰Pu/²³⁹Pu observed in accessible and refractory fractions ranged between 0.11 and 0.18. With the exception of one sample, the ²⁴⁰Pu/²³⁹Pu isotope ratios measured in the refractory fractions are essentially identical having a mean ratio value of 0.123 ± 0.001 (1σ). The ²⁴⁰Pu/²³⁹Pu ratios provide isotopic evidence that suggests a portion of non-fallout contamination has a refractory nature. The presence of similarly low ²⁴⁰Pu/²³⁹Pu ratios in refractory fractions of sediments from the Ob and Irtysh Rivers suggests the existence of a source of refractory Pu which is consistent with refractory “hot particles” derived from surface tests at the Semipalitinsk test site.     

Radioisotope contaminations from releases of the Tomsk-Seversk nuclear facility (Siberia, Russia)

Soils have been sampled in the vicinity of the Tomsk-Seversk facility (Siberia, Russia) that allows us to measure radioactive contaminations due to atmospheric and aquatic releases. Indeed soils exhibit large inventories of man-made fission products including 137Cs (ranging from 33,000 to 68,500 Bq m(-2)) and actinides such as plutonium (i.e. 239+240Pu from 420 to 5900 Bq m(-2)) or 241Am (160-1220 Bq m(-2)). Among all sampling sites, the bank of the Romashka channel exhibits the highest radioisotope concentrations. At this site, some short half-life gamma emitters were detected as well indicating recent aquatic discharge in the channel. In comparison, soils that underwent atmospheric depositions like peat and forest soils exhibit lower activities of actinides and 137Cs. Soil activities are too high to be related solely to global fallout and thus the source of plutonium must be discharges from the Siberian Chemical Combine (SCC) plant. This is confirmed by plutonium isotopic ratios measured by ICP-MS; the low 241Pu/239Pu and 240Pu/239Pu atomic ratios with respect to global fallout ratio or civil nuclear fuel are consistent with weapons grade signatures. Up to now, the influence of Tomsk-Seversk plutonium discharges was speculated in the Ob River and its estuary. Isotopic data from the present study show that plutonium measured in SCC probably constitutes a significant source of plutonium in the aquatic environment, together with plutonium from global fallout and other contaminated sites including Tomsk, Mayak (Russia) and Semipalatinsk (Republic of Kazakhstan). It is estimated that the proportion of plutonium from SCC source can reach 45% for 239Pu and 60% for 241Pu in the sediments.     

Distribution of Np and Pu in Swedish lichen samples (Cladonia stellaris) contaminated by atmospheric fallout

The activity concentrations of (237)Np and the two Pu isotopes, (239)Pu and (240)Pu, were determined in lichen samples (Cladonia stellaris) contaminated by fallout from atmospheric nuclear test explosions and the Chernobyl accident. The samples were collected at 18 locations in Sweden, from north to south, between 1986 and 1988 and analysed with high-resolution inductively coupled plasma mass spectrometry (HR-ICP-MS) and alpha spectrometry. Data on the activity ratios (238)Pu/(239+240)Pu and (134)Cs/(137)Cs measured previously were also included in this study for comparison. The (237)Np activity concentration ranged from 0.08 +/- 0.01 to 2.08 +/- 0.17 MBq kg(-1), depending on the location of the sampling site and time of collection. The (239+240)Pu activity concentration ranged from 0.09 +/- 0.01 to 4.09 +/- 0.15 Bq kg(-1), with the (240)Pu/(239)Pu atomic ratio ranging between 0.16 +/- 0.01 and 0.44 +/- 0.03, the higher ratios indicating a combination of weapons test fallout and Chernobyl fallout. The (237)Np/(239)Pu atomic ratios ranged between 0.06 +/- 0.01 and 0.42 +/- 0.04, the lower ratios indicating combination of weapons test fallout and Chernobyl fallout. At a well-defined sampling site at Lake Rogen (62.32 degrees N, 12.38 degrees E), additional lichen samples were collected between 1987 and 1998 to study the distribution of Np and Pu in different layers. The concentrations of the two elements follow each other quite well in the profile.     

Spatial and temporal distribution of Pu in the Northwest Pacific Ocean using modern coral archives

Historical ²³⁹Pu activity concentrations and ²⁴⁰Pu/²³⁹Pu atom ratios were determined in skeletons of dated modern corals collected from three locations (Chuuk Lagoon, Ishigaki Island and Iki Island) to identify spatial and temporal variations in Pu inputs to the Northwest Pacific Ocean. The main Pu source in the Northwest Pacific is fallout from atmospheric nuclear weapons testing which consists of global fallout and close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands. PPG close-in fallout dominated the Pu input in the 1950s, as was observed with higher ²⁴⁰Pu/²³⁹Pu atom ratios (> 0.30) at the Ishigaki site. Specific fallout Pu contamination from the Nagasaki atomic bomb and the Ivy Mike thermonuclear detonation at the PPG were identified at Ishigaki Island from the ²⁴⁰Pu/²³⁹Pu atom ratios of 0.07 and 0.46, respectively. During the 1960s and 1970s, global fallout was the major Pu source to the Northwest Pacific with over 60% contribution to the total Pu. After the cessation of the atmospheric nuclear tests, the PPG again dominated the Pu input due to the continuous transport of remobilised Pu from the Marshall Islands along the North Equatorial Current and the subsequent Kuroshio Current. The Pu contributions from the PPG in recent coral bands (1984 onwards) varied over time with average estimated PPG contributions between 54% and 72% depending on location.     

Plutonium as a chronomarker in Australian and New Zealand sediments: a comparison with Cs

The construction of high resolution chronologies of sediment profiles corresponding to the last 50-100 years usually entails the measurement of fallout radionuclides ²¹⁰Pb and ¹³⁷Cs. The anthropogenic radionuclide, ¹³⁷Cs, originating from atmospheric nuclear weapons testing can provide an important “first appearance” horizon of known age (1954-1955), providing much-needed validation for the sometimes uncertain interpretations associated with ²¹⁰Pb geochronology. However, while ¹³⁷Cs usually provides a strong signal in sediment in the northern hemisphere, total fallout of ¹³⁷Cs in the southern hemisphere was only 25% that of the north and the low activities of ¹³⁷Cs seen in Australian and New Zealand sediments can make its horizon of first appearance somewhat arguable. Low ¹³⁷Cs fallout also limited the size of the 1963-1964 fallout peak, a peak that is usually seen in northern hemisphere sediment profiles but is often difficult to discern south of the equator.This paper shows examples of the use of nuclear weapons fallout Pu as a chronomarker in sediment cores from Australia (3 sites) and New Zealand (1 site). The Pu profiles of five cores are examined and compared with the corresponding ¹³⁷Cs profiles and ²¹⁰Pb geochronologies. We find that Pu has significant advantages over ¹³⁷Cs, including greater measurement sensitivity using alpha spectrometry and mass spectrometric techniques compared to ¹³⁷Cs measurements by gamma spectrometry. Moreover, Pu provides additional chronomarkers associated with changes in the Pu isotopic composition of fallout during the 1950s and 1960s. In particular, the ²³⁸Pu/^239+240Pu activity ratio shows distinct shifts in the early 1950s and the mid to late 1960s, providing important known-age horizons in southern hemisphere sediments. For estuarine and near-shore sediments Pu sometimes has another significant advantage over ¹³⁷Cs due to its enrichment in bottom sediment relative to ¹³⁷Cs resulting from the more efficient scavenging of dissolved Pu in seawater by sediment particles.     

Depth profile of ²³⁶U/²³⁸U in soil samples in La Palma, Canary Islands

The vertical distribution of the ²³⁶U/²³⁸U isotopic ratio was investigated in soil samples from three different locations on La Palma (one of the seven Canary Islands, Spain). Additionally the ²⁴⁰Pu/²³⁹Pu atomic ratio, as it is a well establish tool for the source identification, was determined. The radiochemical procedure consisted of a U separation step by extraction chromatography using UTEVA^® Resin (Eichrom Technologies, Inc.). Afterwards Pu was separated from Th and Np by anion exchange using Dowex 1x2 (Dow Chemical Co.). Furthermore a new chemical procedure with tandem columns to separate Pu and U from the matrix was tested. For the determination of the uranium and plutonium isotopes by alpha spectrometry thin sources were prepared by microprecipitation techniques. Additionally these fractions separated from the soil samples were measured by Accelerator Mass Spectrometry (AMS) to get information on the isotopic ratios ²³⁶U/²³⁸U, ²⁴⁰Pu/²³⁹Pu and ²³⁶U/²³⁹Pu, respectively. The ²³⁶U concentrations [atoms/g] in each surface layer (∼2 cm) were surprisingly high compared to deeper layers where values around two orders of magnitude smaller were found. Since the isotopic ratio ²⁴⁰Pu/²³⁹Pu indicated a global fallout signature we assume the same origin as the probable source for ²³⁶U. Our measured ²³⁶U/²³⁹Pu value of around 0.2 is within the expected range for this contamination source.     

Activity ratios of 137Cs, 90Sr and 239+240Pu in environmental samples

Both global and Chernobyl fallout have resulted in environmental contamination with radionuclides such as 137Cs, 90Sr and 239+240Pu. In environmental samples, 137Cs and 239+240Pu can be divided into the contributions of either source, if also the isotopes 134Cs and 238Pu are measurable, based on the known isotopic ratios in global and Chernobyl fallout. No analogous method is available for 90Sr. The activity ratios of Sr to Cs and Pu, respectively, are known for the actual fallout mainly from air filter measurements; but due to the high mobility of Sr in the environment, compared to Cs and Pu, these ratios generally do not hold for the inventory many years after deposition. In this paper we suggest a method to identify the mean contributions of global and Chernobyl fallout to total Sr in soil, sediment and cryoconite samples from Alpine and pre-Alpine regions of Austria, based on a statistical evaluation of Sr/Cs/Pu radionuclide activity ratios. Results are given for Sr:Cs, Sr:Pu and Cs:Pu ratios. Comparison with fallout data shows a strong depletion of Sr against Cs and Pu.     

Time pattern of off-site plutonium deposition from rocky flats plant by lake sediment analyses

A sediment core from a lake downwind of the Rocky Flats Plant, where nuclear weapons components are produced, was used to reconstruct a time pattern of off-site plutonium deposition. Core sections were dated by analyses of ¹³⁷Cs, ^239,240Pu, ²³⁸Pu, and ²⁴¹Am fallout from nuclear testing and ²³⁸Pu fallout from a satellite failure. A peak in transuranic concentrations occurred in late 1969 which was attributable to the Plant. This was confirmed by mass isotopic analysis of plutonium isotopes in selected core segments where the global fallout and Plant contributions could be differentiated. The 18 nCi ^239,240Pu per m² from the Plant that had accumulated in the sediment is reasonable when compared to soil analyses.     

Characterization of plutonium in deep-sea sediments of the Sulu and South China Seas

Anthropogenic Pu isotopes are important geochemical tracers for sediment studies. Their distributions and sources in the water columns as well as the sediments of the North Pacific have been intensively studied; however, information about Pu in the Southeast Asian seas is limited. To study the isotopic composition of Pu, and thus to identify its sources, we collected sediment core samples in the South China Sea and the Sulu Sea during the KH-96-5 Cruise of the R/V Hakuho Maru. We analysed the activities of ^239+240Pu and the atom ratios of ²⁴⁰Pu/²³⁹Pu using isotope dilution sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS). The ²⁴⁰Pu/²³⁹Pu atom ratios in the sediments of both areas (inventory weighted mean: 0.251 for the South China Sea and 0.280 for the Sulu Sea) were higher than the global fallout value (0.178 ± 0.019), suggesting the existence of Pu from the Pacific Proving Grounds in the North Pacific. Low inventories of ^239+240Pu in sediments were observed in the South China Sea (3.75 Bq/m²) and the Sulu Sea (1.38 Bq/m²). Most of the Pu input is still present in the water column. Scavenging and benthic mixing processes were considered to be the main processes controlling the distribution of Pu in the deep-sea sediments of both study areas.     

240Pu/239Pu atom ratios in seawater from Sagami Bay, western Northwest Pacific Ocean: sources and scavenging

Seawater samples were collected in Sagami Bay, western Northwest Pacific Ocean, and their (239+240)Pu activities and (240)Pu/(239)Pu atom ratios were determined by alpha-spectrometry and sector field high-resolution ICP-MS. A few samples also were analyzed for (137)Cs activities. The (239+240)Pu inventory of 41.1 Bq m(-2) was equivalent to the expected cumulative deposition density of atmospheric global fallout at the same latitude and this inventory was considerably lower than inventories in the underlying sediment columns. This result indicated that a significant amount of (239+240)Pu has been removed into the underlying sediments through enhanced scavenging from the water column by the high fluxes of particles in this region. The atom ratio of (240)Pu/(239)Pu showed no notable variation from the surface to the bottom; the average value was 0.234+/-0.004. This atom ratio was significantly higher than the mean global fallout ratio of 0.18, proving the existence of close-in fallout plutonium originating from the Pacific Proving Grounds (PPG). The relative contributions of the global stratospheric fallout and the PPG close-in fallout were evaluated by using the two end-member mixing model. The contribution of the PPG close-in fallout was estimated to be 15.2 Bq m(-2), which corresponded to 37% of the (239+240)Pu inventory in the water column. Thus (239)Pu and (240)Pu from the two sources of global fallout and close-in fallout have been homogenized in the water masses in the western Northwest Pacific margin during the past three decades.     

Depositional records of plutonium and (137)Cs released from Nagasaki atomic bomb in sediment of Nishiyama reservoir at Nagasaki

In a sediment core of Nishiyama reservoir at Nagasaki city, depth profiles of (240)Pu/(239)Pu isotopic ratio, (239+240)Pu and (137)Cs activities were determined. Sediments containing plutonium and (137)Cs, which were deposited immediately after a detonation of Nagasaki atomic bomb, were identified in the core. Observed below the sediments were macroscopic charcoals, providing evidence for initial deposit of the fallout of the Nagasaki atomic bomb. This is the first entire depositional records of plutonium and (137)Cs released from the Nagasaki atomic bomb together with those from atmospheric nuclear tests.     

An assessment of the reported leakage of anthropogenic radionuclides from the underground nuclear test sites at Amchitka Island, Alaska, USA to the surface environment

Three underground nuclear tests representing approximately 15-16% of the total effective energy released during the United States underground nuclear testing program from 1951 to 1992 were conducted at Amchitka Island, Alaska. In 1996, Greenpeace reported that leakage of radionuclides, 241Am and 239+240Pu, from these underground tests to the terrestrial and freshwater environments had been detected. In response to this report, a federal, state, tribal and non-governmental team conducted a terrestrial and freshwater radiological sampling program in 1997. Additional radiological sampling was conducted in 1998. An assessment of the reported leakage to the freshwater environment was evaluated by assessing 3H values in surface waters and 240Pu/239Pu ratios in various sample media. Tritium values ranged from 0.41 Bq/l +/- 0.11 two sigma to 0.74 Bq/1 +/- 0.126 two sigma at the surface water sites sampled, including the reported leakage sites. Only at the Long Shot test site, where leakage of radioactive gases to the near-surface occurred in 1965. were higher 3H levels of 5.8 Bq/1 +/- 0.19 two sigma still observed in 1997, in mud pit #3. The mean 240Pu/239Pu for all of the Amchitka samples was 0.1991 +/- 0.0149 one standard deviation, with values ranging from 0.1824 +/- 1.43% one sigma to 0.2431 +/- 6.56% one sigma. The measured 3H levels and 240Pu/239Pu ratios in freshwater moss and sediments at Amchitka provide no evidence of leakage occurring at the sites reported by Buske and Miller (1998 Nuclear-Weapons-Free America and Alaska Community Action on Toxics, Anchorage, Ak, p.38) and Miller and Buske (1996 Nuclear Flashback: The Return to Anchitka, p.35). It was noted that the marine sample; 240Pu/239Pu ratios are statistically different than the global fallout ratios presented by Krey et al. (1976) and Kelley, Bond, and Beasley (1999). The additional non-fallout component 240Pu/239Pu ratio, assuming a single unique source, necessary to modify the global fallout 240Pu/239Pu ratio to that measured in the marine samples is on the order of 0.65 (Hameedi, Efurd, Harmon, Valette-Silver, & Robertson, 1999; Kelley et al., 1999). While this potentially suggests another plutonium source, such as high burn-up nuclear reactor fuel, rather than underground nuclear tests, the uncertainties in analyses and environmental processes need to be fully assessed before any conclusion can be reached. Further work is needed to evaluate these findings and to support any radiological assessment of the marine environment surrounding Amchitka. Based on geohydrological testing and modeling, leakage from the Amchitka Underground Nuclear Tests is projected to occur to the marine environment (Claassen, 1978; Fenske, 1972; Wheatcraft, 1995).     

Plutonium contamination from accidental release or simply fallout: study of soils at Palomares (Spain)

The activity concentration of plutonium in an environmental sample does not usually constitute sufficient information to determine if it is due only to fallout. Alpha and gamma spectrometry are used here conjointly in the study of environmental soil samples to distinguish between samples showing plutonium contamination due to fallout exclusively, and samples contaminated with plutonium from another source. The method was applied to soil samples collected in Palomares (Spain), where an accidental release of aerosols contaminated with plutonium occurred. The two contributions (fallout and accidentally released plutonium) were separated by means of the activity ratios between various radionuclides present in the samples analyzed. The fallout level was estimated from the 239 + 240Pu/137Cs activity ratio. For samples showing contamination due to the accident, the 238Pu/239 + 240Pu and 239Pu/240Pu activity ratios were also calculated to determine the grade of plutonium of this contamination.     

The distribution of plutonium,Americium and curium isotopes in pond and stream sediments of the Savannah river plant,South Carolina,USA

The concentrations of ²³⁸Pu, ^239,240Pu, ²⁴¹Am and ²⁴⁴Cm were determined in sediment samples from five streams and two ponds on the Savannah River Plant (SRP) and in four sediment samples from the Savannah River above and below the plant site. The following concentration ranges were determined: ²³⁸Pu, 0·07–386 fCi g⁻¹; ^239,240Pu, 0·37–1410 fCi g⁻¹; ²⁴¹Am, 0·1–4360 fCi g⁻¹; ²⁴⁴Cm, <0·01–392 fCi g⁻¹. Comparisons of the elemental and isotopic ratios of the sediments show that the majority of the sediments studied have been impacted upon by plant operations and that sediments outside the plant boundary in the Savannah River have only been influenced by aerial releases. Atom ratios of ²⁴⁰Pu/²³⁹Pu indicate that up to 86% of the Pu in these sediments is derived from plant operations. However, comparisons of the concentration data with values for other impacted sediments near nuclear facilities indicate that the levels are relatively small. Finally, <13% of the Pu, Am or Cm in pond sediments is associated with humic or fulvic acids, indicating that little of the material should be remobilized in oxic environments through organic complexation.     

Studies of Np and Pu in the marine environment of Swedish-Danish waters and the North Atlantic Ocean

The long-lived anthropogenic radionuclides (237)Np, (239)Pu and (240)Pu were determined in marine environmental samples (seaweed and seawater) collected from Swedish-Danish waters and the North Atlantic Ocean at various locations on different occasions during the period 1991-2001. The measurements were performed with sector field Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and conventional alpha spectrometry. The (237)Np activity concentrations in Fucus vesiculosus and surface seawater from the Swedish west coast and Danish waters ranged from 0.16+/-0.02 to 1.02+/-0.09 mBq kg(-1) (dry weight) and 0.65+/-0.02 to 1.69+/-0.02 mBq m(-3), respectively, depending on the location and sampling year. Most of the (237)Np in these waters is believed to originate from the Sellafield nuclear reprocessing plant, with some contribution from global fallout. The (240)Pu/(239)Pu atomic ratios in F. vesiculosus samples are reported in this study with an overall average of 0.17+/-0.03. The (237)Np and (239)Pu activity concentrations observed in surface seawater collected in North Atlantic waters ranged from 0.16+/-0.01 to 0.62+/-0.08 mBq m(-3) and from 0.64+/-0.05 to 4.27+/-0.08 mBq m(-3), respectively, and the (237)Np/(239)Pu atomic ratios were a good indicator of conservative behaviour of Np in marine waters.     

Upward movement of plutonium to surface sediments during an 11-year field study

An 11-year lysimeter study was established to monitor the movement of Pu through vadose zone sediments. Sediment Pu concentrations as a function of depth indicated that some Pu moved upward from the buried source material. Subsequent numerical modeling suggested that the upward movement was largely the result of invading grasses taking up the Pu and translocating it upward. The objective of this study was to determine if the Pu of surface sediments originated from atmosphere fallout or from the buried lysimeter source material (weapons-grade Pu), providing additional evidence that plants were involved in the upward migration of Pu. The ²⁴⁰Pu/²³⁹Pu and ²⁴²Pu/²³⁹Pu atomic fraction ratios of the lysimeter surface sediments, as determined by Thermal Ionization Mass Spectroscopy (TIMS), were 0.063 and 0.00045, respectively; consistent with the signatures of the weapons-grade Pu. Our numerical simulations indicate that because plants create a large water flux, small concentrations over multiple years may result in a measurable accumulation of Pu on the ground surface. These results may have implications on the conceptual model for calculating risk associated with long-term stewardship and monitored natural attenuation management of Pu contaminated subsurface and surface sediments.     

Plutonium isotopes in the lower reaches of the River Rhône over the period 1945-2000: fluxes towards the Mediterranean Sea and sedimentary inventories

Plutonium isotopes in the Rh?ne River originate from both the weathering of the catchment basin contaminated by global atmospheric fallout, and the liquid effluents released from the Marcoule reprocessing plant since 1961. Due to a new treatment process applied to the liquid effluents, a decrease of two orders of magnitude in the industrial plutonium discharged into the River Rh?ne has been registered from 1991. Today, 238Pu industrial inputs to the River Rh?ne are still about 10 times higher than those derived from global fallout, while 239+240Pu inputs from industrial and global fallout sources are of similar importance, i.e. 1 GBq y(-1). Our results indicate that the river sedimentary compartment act either as a sink or a delayed-source term of plutonium for the freshwaters depending on the hydraulic regime and flood events. This compartment may then represent an important industrial delayed-source term for the River Rh?ne freshwaters in the coming years as the Marcoule reprocessing plant is being dismantled. These results were obtained from samples collected from the lower course of the River Rh?ne over the 1987-1998 period and analysed for 238Pu and 239+240Pu activities. Both river sedimentary inventories of plutonium isotopes and effective outputs from the River Rh?ne towards the Gulf of Lions have been estimated for each year over the 1945-2000 period. Regarding 239+240Pu, the sedimentary inventory accumulated since 1945 is estimated to be 172+/-35 GBq. If mobile, this amount represents a significant delayed-source term of plutonium on the scale of the Rh?ne watershed.     

Modelling the distribution of plutonium in the Pacific Ocean

An Oceanic General Circulation Model (OGCM) including a plutonium scavenging model as well as an advection-diffusion model has been developed for modelling the distribution of plutonium in the Pacific Ocean. Calculated 239, 240Pu water profile concentrations and 239, 240Pu inventories in water and sediment of the Pacific Ocean have showed a reasonable agreement with the experimental results. The presence of local fallout plutonium in central North Pacific waters has been confirmed. The observed 240Pu/239Pu mass ratios confirm that plutonium originating from local fallout from nuclear weapons tests carried out at Bikini and Enewetak Atolls is more rapidly removed from surface waters to deeper waters than plutonium originating from global fallout. The developed OGCM can be used for modelling the dispersion of other non-conservative tracers in the ocean as well.