Assessment of the global fallout of plutonium isotopes and americium-241 in the soil of the central region of Saudi Arabia

A radiochemical technique for determination of plutonium isotopes and 241Am in soil samples is tested against IAEA-standard reference materials to determine its accuracy and precision for reliable results. The technique is then used in the investigation of topsoil samples, collected from the natural environment of the central region of Saudi Arabia, to assess the effect of fallout accumulation of these radionuclides in the region. Plutonium and americium were sequentially separated from all other components of the sample by anion-exchange chromatography and co-precipitated with Nd3+ as fluorides. The precipitates were mounted on membrane filters and measured using a high-resolution alpha-spectrometer. The results of the analysis of the reference materials showed satisfactory sensitivity and precision of the technique. The results of the analyzed soil samples show activity levels ranging from < LLD to 0.089 and from 相似文献   

Isotopic composition and origin of uranium and plutonium in selected soil samples collected in Kosovo

Soil samples collected from locations in Kosovo where depleted uranium (DU) ammunition was expended during the 1999 Balkan conflict were analysed for uranium and plutonium isotopes content (234U, 235U, 236U, 238U, 238Pu, (239 + 240)Pu). The analyses were conducted using gamma spectrometry (235U, 238U), alpha spectrometry (238Pu, (239 + 240)Pu), inductively coupled plasma-mass spectrometry (ICP-MS) (234U, 235U, 236U, 238U) and accelerator mass spectrometry (AMS) (236U)). The results indicated that whenever the U concentration exceeded the normal environmental values (approximately 2 to 3 mg/kg) the increase was due to DU contamination. 236U was also present in the released DU at a constant ratio of 236U (mg/kg)/238U (mg/kg) = 2.6 x 10(-5), indicating that the DU used in the ammunition was from a batch that had been irradiated and then reprocessed. The plutonium concentration in the soil (undisturbed) was about 1 Bq/kg and, on the basis of the measured 238Pu/(239 + 240)Pu, could be entirely attributed to the fallout of the nuclear weapon tests of the 1960s (no appreciable contribution from DU).     

Radioactivity concentrations of 40K, 134Cs, 137Cs, 90Sr, 241Am, 238Pu and 239+240Pu radionuclides in Jordanian soil samples

In November 2000, surface and core soil samples were collected from different regions of Jordan. The samples were analyzed by direct gamma spectrometry and combined radiochemical separation procedure to quantify (40)K, (134)Cs, (137)Cs, (90)Sr, (241)Am, (238)Pu and (239+240)Pu radioactivity. Concentrations (Bq.kg(-1) dry weight) have been observed to vary in the range 1.5-2.6 for (134)Cs, 2.8-11.4 for (90)Sr, and 0.13-0.48 for (241)Am, 0.016-0.062 for (238)Pu, 0.28-1.01 for (239+240)Pu and 155-543 for (40)K. The typical concentration of (137)Cs found in topsoils (0-2 cm) ranged in 7.5-576 Bq.kg(-1), dry weight. These values were greater than those observed in samples taken at greater depths (up to 32 cm). Activity ratios of (134)Cs/(137)Cs, (90)Sr/(137)Cs, (239+240)Pu/(137)Cs, (238)Pu/(137)Cs, (241)Am/(137)Cs, (239+240)Pu/(238)Pu and (241)Am /(238)Pu have mean values of 0.0049 (R=1), 0.29 (R=0.76), 0.41 (R=0.90), 0.39 (R=0.85), 0.41 (R=0.88), 7.72 (R=0.97) and 16.66 (R=0.98), respectively. The underlying concentrations were correlated and relatively higher than those reported in neighboring countries. One moss sample, as a biomonitor indicator, was measured and evaluated along with the soil samples. Its data showed higher concentrations of all measured radionuclides due to accumulations over years. The depth distribution of the fission product (137)Cs and the total deposition (Bq.m(-2)) were also studied in selected samples. Estimations of the annual effective dose equivalent due to (137)Cs-soil contamination showed values up to more than 200 microSv.     

Behaviour and transport of radionuclides in soil and vegetation of a sand dune ecosystem

A sand dune ecosystem in the vicinity of the British Nuclear Fuels reprocessing plant at Sellafield, Cumbria, UK was used to examine the spatial, temporal and depth distributions of 134Cs, 137Cs, 238Pu, 239 + 240Pu and 241Am in soil and in two species of vegetation (Festuca rubra, Ammophila arenaria). Core samples showed evidence of the accumulation of radionuclides derived mainly from sea-to-land transfer. Accumulated deposits of radioactivity (0-0.1 m) lie within the range: 1.1-3.4 Bq kg-1 (134Cs), 260-440 Bq kg-1 (137Cs), 31-40 Bq kg-1 (238Pu), 150-215 Bq kg-1 (239 + 240Pu) and 190-240 Bq kg-1 (241Am). Soil profiles showed greater activity concentrations in their deeper regions and this is attributed to leaching of radionuclides in percolating drainage water accentuated by the coarse texture, low organic matter and clay mineral content of coastal sands. Radionuclide activity concentrations in F. rubra and A. arenaria were similar, in the ranges 20-70 Bq kg-1 (137Cs), 1-5 Bq kg-1 (238Pu), 10-30 Bq kg-1 (239 + 240Pu) and 10-65 Bq kg-1 (241Am). Clear temporal and spatial variations were observed in both species of vegetation, reflecting the weather conditions antecedent to the sampling period and the influence of sea-to-land transfer. Concentration ratios (vegetation:soil) for activity concentrations in the two species were similar, in the ranges: 0.05-0.14 (137Cs), 0.025-0.097 (238Pu), 0.022-0.057 (239 + 240Pu) and 0.025-0.212 (241Am).     

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.     

Plutonium and americium inventories in atmospheric fallout and sediment cores from Blelham Tarn, Cumbria (UK)

The objective of this paper is to report on the results of a study of 238Pu, 239 + 240Pu and 241Am inventories onto Blelham Tarn in Cumbria (UK). The atmospheric fallout inventory was obtained by analysing soil cores and the results are in good agreement with the literature: 101 Bq m(-2) for 239 + 240Pu; 4.5 Bq m(-2) for 238Pu and 37 Bq m(-2) for 241Am. The sediment core inventory for the whole lake is compared to the atmospheric fallout inventory. The sediment activity is 60-80% higher than the estimated fallout activity, showing a catchment area contribution and in particular the stream input.     

239+240Pu, 90Sr and 137Cs inventories in surface soils of Vietnam

Fallout 239+240Pu, 238Pu, 90Sr and 137Cs inventories in surface soils were measured for 20 locations in northern Vietnam yielding the mean values (+/- standard error) of 26.5+/-3.8 Bq m(-2) for 239+240Pu, 1048+/-143 Bq m(-2) for 137Cs and 212+/-28 Bq m(-2) for 90Sr. The concentrations of 137Cs and plutonium isotopes strongly correlate with each other resulting in a stable 239+240Pu/137Cs inventory ratio of 0.025+/-0.002. Among soil parameters, organic matter and fulvic acids strongly correlate with caesium and plutonium isotopes, especially in the 0-10 cm layer. 137Cs and 239+240Pu are distributed rather similarly over the 0-10 cm and 10-20 cm layers. At locations with high contents of sand (82-93%) along the South China Sea coast, the downward percolation by rainwater results in a higher accumulation of 239+240Pu and 137Cs in the 10-20 cm layer. The mean 137Cs/ 90Sr inventory ratio is 9.3+/-2.2, and the correlation is weak between these isotopes.     

Sector field inductively coupled plasma mass spectrometry, another tool for plutonium isotopes and plutonium isotope ratios determination in environmental matrices

The transfer of radio nuclides into the different compartments of the environment are widely studied and leads to the elaboration of transfer models in order to evaluate potential impact onto the environment and humans. Accurate experimental data are needed to validate these models for all types of matrices (air, water, sediments, soils, biota and food...). Among these radionuclides, 238Pu, 239Pu, 240Pu and 241Pu, are often mentioned. They have been released into the environment by nuclear weapon tests, nuclear facilities, reactors or satellite accidents. These different sources have different 240Pu/239Pu ratios and therefore this ratio is used to provide information on the source of contamination into the environment. The most conventional analytical tools used for plutonium isotope determination are liquid scintillation and alpha spectrometry, and thermal ionisation mass spectrometry (TIMS) is still considered as the primary method for determination of plutonium isotope ratios. During the last decade, mass spectrometers equipped with plasma ion sources and sector field analysers were developed and can offer now another alternative method for the accurate determination of isotope content and ratios of long-lived radionuclides in environmental samples. This paper presents and discusses the results obtained for 239Pu, 240Pu and 241Pu content and isotope ratios by sector field ICP-MS in different environmental matrices.     

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.     

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.     

Bioaccumulation and distribution of plutonium in fish from Gdansk Bay

In this paper, the results of 238Pu and 239 + 240Pu determinations in four representative species of Baltic fish collected in Gdansk Bay; flounder, herring, cod and sprat, are presented and discussed. The plutonium isotopes are amongst the more radiotoxic nuclides. In the marine environment, the highest concentrations of plutonium are found in the sediments, but the complex biogeochemical cycle of the element means that it is also found in all other compartments. The activities of the fish samples were measured using alpha spectrometry and the concentrations of plutonium 238Pu and 239 + 240Pu were estimated for particular organs and tissues and the whole body. The 239 + 240Pu concentrations for fish species were: flounder 0.94 mBq kg-1 w.w., herring 2.22 mBq kg-1 w.w., cod 2.35 mBq kg-1 w.w. and sprat 0.33 mBq kg-1 w.w. On the basis of the 238Pu/239 + 240Pu activity ratio in the organs and tissues, the proportion of Chernobyl-derived plutonium in the Baltic Sea was calculated. The lowest values of Chernobyl plutonium were accumulated in flounder stomach, herring skin, cod intestine, the highest in cod gills and skin.     

Plutonium concentrations in waters from the southern Baltic Sea and their distribution in cod (Gadus morhua) skin and gills

The concentrations of (238)Pu and (239+240)Pu in water samples and suspended particulate fractions, as well as in colloidal fraction from the southern Baltic Sea are presented. The (239+240)Pu concentration in surface seawater samples fall within range from 5.2 mBq.m(-3) for Gdańsk Bay to 150 mBq.m(-3) for Pomeranian Bay, most of which (from 52 to 96%) constituted filterable forms (相似文献   

Artificial radionuclides in the atmosphere over Lithuania

Measurements of airborne radioactive aerosol concentration were carried out on the basis of 1-3 days samples after the Chernobyl disaster and during the period of 1992-2003. Transport of "hot" particles of different composition resulted in the high activity concentrations of (137)Cs, (238)Pu, (239,240)Pu and (241)Am in the atmosphere in Vilnius at the end of April 1986. The (240)Pu/(239)Pu atom ratio showed clear evidence of non-global plutonium originating from the Chernobyl accident in the atmosphere over Lithuania. The (240)Pu/(239)Pu atom ratio ranged from 0.14 to 0.40 in monthly samples in Vilnius in 1995-2003. An increase in activity concentration of (137)Cs by a factor of 100 (up to 300 microBq/m(3)) was found following forest fires in the Ukraine and Belarus. However, no transport of the Chernobyl plutonium was observed and the (240)Pu/(239)Pu atom ratio in samples collected during the forest fires was found to be 0.229 and 0.185, respectively. The exponential decrease in the (240)Pu/(239)Pu atom ratio from 0.30 to 0.19 (mean values) was observed in 1995-2003.     

Residual radioactive contamination at the peaceful underground nuclear explosion sites "Craton-3" and "Crystal" in the Republic of Sakha (Yakutia)

In this paper, results are reported on the concentrations and activity ratios of 137Cs, 239+240Pu and 238Pu in soils, lichen and bottom sediments collected at the peaceful underground nuclear explosion sites "Craton-3" and "Crystal" (Republic of Sakha (Yakutia), North-East Siberia). At the "Craton-3" site, 239- 240Pu concentrations in the range 6.2 mBq/g to 5.9 Bq/g in surface soils (0-5 cm) and 239+240Pu concentrations up to 7.4 Bq/g in lichen were observed. The 137Cs concentration in measured soils range from 0.52 to 216 Bq/g for the near-plume and from 1.65 to 21.5 Bq/g for the far-plume. In lichen, 137Cs concentration varied from a global background level up to 251 Bq/g. Radioactive contamination at "Crystal" demonstrates an extremely irregular distribution of 239,240Pu and 137Cs in environmental samples taken at locations within 150 m radius of the site. Further work on compiling detailed maps of radioactive contamination of the territory around "Craton-3" and "Crystal" is discussed.     

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.     

137Cs and (239+240)Pu levels in the Asia-Pacific regional seas

137Cs and (239+240)Pu data in seawater, sediment and biota from the regional seas of Asia-Pacific extending from 50 degrees N to 60 degrees S latitude and 60 degrees E to 180 degrees E longitude based on the Asia-Pacific Marine Radioactivity Database (ASPAMARD) are presented and discussed. 137Cs levels in surface seawater have been declining to its present median value of about 3 Bq/m3 due mainly to radioactive decay, transport processes, and the absence of new significant inputs. (239+240)Pu levels in surface seawater are much lower, with a median of about 6 mBq/m3. (239+240)Pu appears to be partly scavenged by particles and is therefore more readily transported down the water column. As with seawater, (239+240)Pu concentrations are lower than 137Cs in surface sediment. The median 137Cs concentration in surface sediment is 1.4 Bq/kg dry, while that of (239+240)Pu is only 0.2 Bq/kg dry. The vertical profiles of both 137Cs and (239+240)Pu in the sediment column of coastal areas are different from deep seas which can be attributed to the higher sedimentation rates and additional contribution of run-offs from terrestrial catchment areas in the coastal zone. Comparable data for biota are far less extensive than those for seawater and sediment. The median 137Cs concentration in fish (0.2 Bq/kg wet) is higher than in crustaceans (0.1 Bq/kg wet) or mollusks (0.1 Bq/kg wet). Benchmark values (as of 2001) for 137Cs and (239+240)Pu concentrations in seawater, sediment and biota are established to serve as reference values against which the impact of future anthropogenic inputs can be assessed. ASPAMARD represents one of the most comprehensive compilations of available data on 137Cs and (239+240)Pu in particular, and other anthropogenic as well as natural radionuclides in seawater, sediment and biota from the Asia-Pacific regional seas.     

Resolving Chernobyl vs. global fallout contributions in soils from Poland using Plutonium atom ratios measured by inductively coupled plasma mass spectrometry

Plutonium in Polish forest soils and the Bór za Lasem peat bog is resolved between Chernobyl and global fallout contributions via inductively coupled plasma mass spectrometric measurements of 240Pu/230Pu and 241Pu/239Pu atom ratios in previously prepared NdF3 alpha spectrometric sources. Compared to global fallout, Chernobyl Pu exhibits higher abundances of 240Pu and 241Pu. The ratios 240Pu/230Pu and 241Pu/239Pu co-vary and range from 0.186 to 0.348 and 0.0029 to 0.0412, respectively, in forest soils (241Pu/239Pu = 0.2407 x [240Pu/239Pu] - 0.0413; r2 = 0.9924). Two-component mixing models are developed to apportion 239+240Pu and 241Pu activities; various estimates of the percentage of Chernobyl-derived 239+240Pu activity in forest soils range from < 10% to > 90% for the sample set. The 240Pu/230Pu - 241Pu/239Pu atom ratio mixing line extrapolates to estimate 241Pu/239Pu and the 241Pu/239+240Pu activity ratio for the Chernobyl source term (0.123 +/- 0.0007; 83 +/- 5; 1 May 1986). Sample 241Pu activities, calculated using existing alpha spectrometric 239+240Pu activities, and the 240Pu/230Pu and 241Pu/239Pu atom ratios, agree relatively well with previous liquid scintillation spectrometry measurements. Chernobyl Pu is most evident in locations from northeastern Poland. The 241Pu activities and/or the 241Pu/239Pu atom ratios are more sensitive than 240Pu/239Pu or 238Pu/239+240Pu activity ratios at detecting small Chernobyl 239+240Pu inputs, found in southern Poland. The mass spectrometric data show that the 241Pu activity is 40-62% Chernobyl-derived in southern Poland, and 58-96% Chernobyl in northeastern Poland. The Bór za Lasem peat bog (49.42 degrees N, 19.75 degrees E), located in the Orawsko-Nowotarska valley of southern Poland, consists of global fallout Pu.     

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).     

Determination of total content and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes by ICP-QMS

The aim of this work was to determine the concentrations and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes. An analytical method was developed with a plutonium and uranium separation procedure based on extraction chromatography (using 2 mL TEVA and UTEVA columns) and detection with a quadrupole ICP-MS applying an ultra-sonic nebulizer coupled with a membrane desolvation system. Starting from blank swipes, the background equivalent concentration (BEC) was 8 fg for ²³⁹Pu and 1 ng ²³⁸U. The method was successfully applied to certified reference materials as well as to round robin samples obtained in the framework of the inter-laboratory exercise program, promoted by the Brazilian–Argentine Agency for Accounting and Control of Nuclear Materials (ABACC), together with the US Department of Energy (USDOE). After the introduction of an additional ion-exchange separation step, the methodology was applied to the IAEA-384 sediment reference sample with precise and accurate total plutonium and uranium, ²⁴⁰Pu/²³⁹Pu, ²⁴¹Pu/²³⁹Pu, ²³⁴U/²³⁸U and ²³⁵U/²³⁸U atomic ratio results.     

Concentration and characterization of plutonium in soils of Hubei in central China

To study the Pu concentration and isotope ratio distributions present in China, the ^239+240Pu total activities and ²⁴⁰Pu/²³⁹Pu atom ratios in core soil samples from Hubei Province in central China were investigated using Accelerator Mass Spectrometry (AMS). The activities ranged from 0.019 to 0.502 mBq g⁻¹ and the ^239+240Pu inventories of 45 and ∼55 Bq m⁻² agree well with that expected from global fallout. The ²⁴⁰Pu/²³⁹Pu atom ratios in the soil ranged from 0.172 to 0.220. The ratios are similar to typical global fallout values. Hence, any close-in fallout contribution from the Chinese nuclear weapons tests, mainly conducted in the 1970s, must have either been negligible or had a similar ²⁴⁰Pu/²³⁹Pu ratio to that of global fallout. The top 10 cm layer of the soil contributes ∼90% of the total inventory and the maximum concentrations appeared in the 2-4 cm or 4-6 cm layers. It is suggested that climatic conditions and organic content are the two main factors that affect the vertical migration of plutonium in soil.