Migration of239Pu in soluble and insoluble forms in soil

A field experiment study was performed at the rural site of South-East Lithuania. The main tasks of the study included an evaluation of the peculiarities of partition of²³⁹Pu in soluble (²³⁹Pu(NO₃)₄,²³⁹PuCl₃) and insoluble (²³⁹PuO₂) forms in soddy and forest soil horizons. The results of durable experiments (418 and 326 days) have shown that from 44.1% to 92.2% of²³⁹Pu of investigated chemical forms were accumulated in the top (0–5 cm) soil layer. Some share (5.7–39.2%) of plutonium from studied chemical forms was found in the 5–20 cm layers of studied soil samples (columns). Obtained distribution of plutonium in soil layers may be attributed to the consideration that the migration rate to the soil depth for plutonium is 0.1–1.0 cm·y⁻¹ but for some part of plutonium 10 times higher migration rate is characteristic as well. Plutonium transfer factor (TF) to the grassland plants was calculated, the values ranged from 10⁻² to 10⁻¹.     

Isotopic composition of plutonium immissions in Austria after the Chernobyl accident

Alpha-spectrometric Pu determinations in aerosol samples collected after the Chernobyl accident in Austria show a²³⁸Pu/²³⁹ (240)Pu ratio in the range of 0.33–0.76 with a most reliable value of 0.47. From²⁴¹Am measurements in old Pu preparations and air filter analyses also²⁴¹Pu activities have been calculated. The ratio²⁴¹Pu/^{239 (240)}Pu during the main contamination period is 74.6±5.7, when maximum²⁴¹Pu concentrations in air achieved 4.5–6.0 mBq/m³.     

<Superscript>239, 240, 241</Superscript>Pu fingerprinting of plutonium in western US soils using ICPMS: solution and laser ablation measurements

Sector field inductively coupled plasma mass spectrometry (SF-ICPMS) has been used with analysis of solution samples and laser ablation (LA) of electrodeposited alpha sources to characterize plutonium activities and atom ratios prevalent in the western USA. A large set of surface soils and attic dusts were previously collected from many locations in the states of Nevada, Utah, Arizona, and Colorado; specific samples were analyzed herein to characterize the relative contributions of stratospheric fallout vs. Nevada Test Site (NTS) plutonium. This study illustrates two different ICPMS-based analytical strategies that are successful in fingerprinting Pu in environmental soils and dusts. Two specific datasets have been generated: (1) soils are leached with HNO₃-HCl, converted into electrodeposited alpha sources, counted by alpha spectrometry, then re-analyzed using laser ablation SF-ICPMS; (2) samples are completely dissolved by treatment with HNO₃-HF-H₃BO₃, Pu fractions are prepared by extraction chromatography, and analyzed by SF-ICPMS. Optimal laser ablation and ICPMS conditions were determined for the re-analysis of archived alpha spectrometry “planchette” sources. The best ablation results were obtained using a large spot size (200 μm), a defocused beam, full repetition rate (20 Hz) and scan rate (200 μm s⁻¹); LA-ICPMS data were collected with a rapid electrostatic sector scanning experiment. Less than 10% of the electroplated surface area is consumed in the LA-ICPMS analysis, which would allow for multiple re-analyses. Excellent agreement was found between ^239+240Pu activities determined by LA-ICPMS vs. activity results obtained by alpha spectrometry for the same samples ten years earlier. LA-ICPMS atom ratios for ²⁴⁰Pu/²³⁹Pu and ²⁴¹Pu/²³⁹Pu range from 0.038–0.132 and 0.00034–0.00168, respectively, and plot along a two-component mixing line (²⁴¹Pu/²³⁹Pu = 0.013 [²⁴⁰Pu/²³⁹Pu] – 0.0001; r ² = 0.971) with NTS and global fallout end-members. A rapid total dissolution procedure, followed by extraction chromatography and SF-ICPMS solution Pu analysis, generates excellent agreement with certified ^239+240Pu activities for standard reference materials NIST 4350b, NIST 4353, NIST 4357, and IAEA 385. ^239+240Pu activities and atom ratios determined by total dissolution reveal isotopic information in agreement with the LA-ICPMS dataset regarding the ubiquitous mixing of NTS and stratospheric fallout Pu sources in the regional environment. For several specific samples, the total dissolution method reveals that Pu is incompletely recovered by simpler HNO₃-HCl leaching procedures, since some of the Pu originating from the NTS is contained in refractory siliceous particles.     

Radioactivity of plutonium isotopes, <Superscript>137</Superscript>Cs and their ratio in sediment,seawater and biota from the east coast of Peninsular Malaysia

This study with sampling expeditions of marine sediment, seawater and biota were performed at 30 stations within Malaysian Exclusive Economic Zone (EEZ). A total of >400 samples were collected to determine the activity concentration of anthropogenic radionuclides (^239+240Pu, ¹³⁷Cs) and their activity ratio (^239+240Pu/¹³⁷Cs) in sediments, seawater and biota. The purpose of this study was to determine the concentration levels for these radionuclides and to evaluate any occurrence of radioactive contamination. Sediment cores were obtained using multicorer device, while water samples via co-precipitation techniques and biota was purchased from local fishermen. The activity concentrations of ^239+240Pu in sediment, seawater and biota were ranged 0.21–0.45 Bq/kg dry wt., 2.33–7.95 mBq/m³ and <0.008 Bq/kg fresh wt., respectively. Meanwhile, the values of ¹³⁷Cs were ranged <1.00–2.71 Bq/kg dry wt. in sediment, 3.40–5.89 Bq/m³ in seawater and <0.05–0.41 Bq/kg fresh wt. in biota, respectively. Activity ratios of ^239+240Pu to ¹³⁷Cs obtained seem to confirm that these artificial radioactivities were mainly due to global nuclear fallout.     

Pu isotopes and137Cs in the surrounding areas of the former Soviet Union's Semipalatinsk nuclear test site

Field missions were sent to Semipalatinsk City and several settlements near the former Semipalatinsk nuclear test site to investigate the current radioactive contamination levels of the land coming from long-lived radionuclides. The soil was sampled at about 20 sites, including some settlements such as Mostik, Dolon and Chagan, forest and pasture areas, along the roads from Semipalatinsk City to Kurchatov City and to Korosteli settlement in the direction of the Altai District. The radioactivities of¹³⁷Cs,²³⁸Pu and^239,240Pu as well as²⁴⁰Pu/²³⁹Pu atomic ratios in the soil were determined by non-destructive γ-ray spectrometry and radiochemical separation followed by α-ray spectrometry and/or ICP-MS, respectively. The results showed a distinction of¹³⁷Cs and^239,240Pu inventories in soil depending on the site where we visited. While the overall¹³⁷Cs levels were as same as or slightly lower than the domestic global fallout level (3·10³–7·10³ Bq/m²),^239,240Pu levels at some sites were several to a few ten times higher than the domestic level (40–120 Bq/m²). The atomic ratios of²⁴⁰Pu/²³⁹Pu in the soil were in the range of 0.024–0.125, which were significantly lower than the value of 0.18 commonly accepted for global fallout Pu.     

Behavior and distribution of <Superscript>239+240</Superscript>Pu and <Superscript>241</Superscript>Am in the east coast of Peninsular Malaysia marine environment

The present distributions of ^239+240Pu, ²⁴¹Am and activity ratio of ²⁴¹Am/^239+240Pu in surface seawater of the Peninsular Malaysia east coast were studied. The surface seawater samples were collected at 30 identified stations during the expedition conducted in 2008. ^239+240Pu activity concentrations in surface seawater of the studied area were in the range of 2.33 ± 0.20–7.95 ± 0.68 mBq/m³, meanwhile ²⁴¹Am activity concentrations ranged from MDA to 1.90 ± 0.23 mBq/m³. The calculated activity ratios of ²⁴¹Am/^239+240Pu were varied and disperse distributed with the ranged of 0.12–0.53. The relationships between anthropogenic radionuclide and oceanographic parameters such as turbidity and salinity were examined. The linearly relationships between ^239+240Pu and oceanographic parameters are important for better understanding of its transport processes and behavior in the east coast of Peninsular Malaysia marine environment. Thus, the differ of distribution of ^239+240Pu, ²⁴¹Am and ²⁴¹Am/^239+240Pu in the studied area mainly due to high affinity of ^239+240Pu to associate with sinking particles, mobility nature of ²⁴¹Am, degree of particle reactive of both anthropogenic radionuclides, scavenging and removal process; and others.     

Evaluation of measurements of 238Pu, 239Pu and 240Pu in urine at the microbecquerel level using thermal ionization mass spectrometry and alpha-spectrometry at Los Alamos National Laboratory: Results of a two year comparison test (LA-UR-06-8055)

The Intercomparison Studies Program (ISP) at the Oak Ridge National Laboratory (ORNL, Oak Ridge, TN, USA) provides natural-matrix urine quality-assurance/quality-control (QA/QC) samples to radiobioassay analysis laboratories. In 2003, a single laboratory (Los Alamos National Laboratory LANL, Los Alamos NM USA) requested a change in the test-samples provided previously by the ISP. The change was requested to evaluate measurement performance for analyses conducted using thermal-ionization mass spectrometry (TIMS). Radionuclides included ²³⁹Pu at two activity levels (75–150 μBq^·sample⁻¹ and 1200–1600 μBq^·sample⁻¹) and ²³⁸Pu (3700–7400 μBq^·sample⁻¹). In addition, ²⁴⁰Pu was added to the samples so that the ^239+240Pu specific activity was 3700–7400 μBq^·sample⁻¹. In this paper, the results of testing during the period May, 2003 through September, 2005 are presented and discussed.     

Inflow of polonium, uranium and plutonium radionuclides in Odra River catchment area assessment by environmetric expertise

The study deals with the application of cluster analysis (CA) and non-parametric tests (Shapiro–Wilk, Kruskal–Wallis, Dunn, U Mann–Whitney) to classify and interpret of a monitoring data set for Odra River water quality assessment based on concentration values of radiochemical parameters. The data set represents results for 3 alpha emitters (²¹⁰Po, ²³⁸U and ^239+240Pu) measured in surface water samples collected at 13 different sampling locations (5 in major Odra stream while 8 in Odra tributaries) within four seasons: winter, spring, summer and autumn, in the framework of 1 year-term quality monitoring research. The correlation analysis of polonium, uranium and plutonium data indicates that significant values of Spearman’s correlation coefficient appears between ²¹⁰Po and ^239+240Pu (r = 0.55 in autumn and 0.77 in winter as well as 0.49 in all year), while statistical significant correlation between uranium and plutonium as well as uranium and polonium were not found. In the Odra drainage basin, the biggest differences were observed in the case of ²³⁸U. The hypothesis about possible geographic and seasonal differences between concentration of ²¹⁰Po, ²³⁸U and ^239+240Pu in the Odra River catchment area was verified by cluster analysis (CA). Finally, to asses if there are statistically significant differences in mean concentration value of ²¹⁰Po, ²³⁸U and ^239+240Pu for Vistula and Odra Rivers drainage basins were obtained by used of the non-parametric tests. Comparing to Vistula catchment area, statistically different concentration of ²¹⁰Po and ^239+240Pu in all year was observed for river samples collected on Odra drainage basin.     

Development of a bipolar electrolysis system for tritium accumulation in HTO

Due to the different ²⁴⁰Pu/²³⁹Pu atom ratios from different sources of Pu in the environment, Pu isotopes have been widely used for source identification of radionuclides in sediments. In this work, using sector-field ICP-MS, we investigated Pu inventory and its isotopic composition in a lacustrine sediment core collected in Chenghai Lake, SW China. The ²⁴⁰Pu/²³⁹Pu atom ratios in this sediment core ranged from 0.166 to 0.271 with a mean of 0.195±0.021, which was slightly higher than that of global fallout. The ^239+240Pu/¹³⁷Cs activity ratios ranged from 0.0155 to 0.0411, with a mean of 0.0215, and the ^239+240Pu inventory was 35.4 MBq/km²; both ^239+240Pu/¹³⁷Cs activity ratio and Pu inventory were close to those values of global fallout at 20–30 °N. Three peaks were observed for both ¹³⁷Cs and ^239+240Pu activities in the examined sediment core; they most probably indicated the maximum deposition of global fallout between 1963 and 1964, the fallout from a series of Chinese nuclear tests during the 1970s, and the deposition of resuspended Pu-bearing particles from the Chernobyl accident. Therefore, the vertical profile of Pu isotopes should provide useful time markers for rapid dating of recent sediments. These authors contributed equally to this work.     

Distribution of uranium,plutonium, and <Superscript>241</Superscript>Am in soil samples from Idaho National Laboratory

Soil materials used were collected in the early 1970s at Idaho National Laboratory near the Subsurface Disposal Area (SDA). Samples from a depth of 0–4 and 4–8 cm at two different sites located on the northeast corner of the SDA perimeter were analyzed. The concentration of ²³⁴U, ²³⁵U, ²³⁶U, and ²³⁸U in soil digests were measured by mass spectrometry. Uranium isotopic composition of the soil at the two sample sites and depths is compared to previously measured concentrations of ²³⁸Pu, ²³⁹Pu, ²⁴⁰Pu, ²⁴¹Pu, and ²⁴¹Am. Implications for remediation of contaminated soils surrounding the SDA are discussed.     

Current levels and distribution of 137Cs and Pu isotopes in soil on the Kazakhstan territory of the Kazakhstan-Chinese border: Semipalatinsk and Lob Nor nuclear test sites detonation

More than 100 soil samples were collected from 46 sites along roads and some settlements connecting Alma-Ata to Semipalatinsk City of the Kazakhstan-Chinese border and analyzed for ¹³⁷Cs and Pu isotopes (²³⁸Pu, ²³⁹Pu and ²⁴⁰Pu). The mean ¹³⁷Cs inventory at each site was within the range of 1,000-3,000 Bq/m² for most of the sites. The ^239,240Pu concentration and its inventories were observed in the wide range of 0.18-2.6 Bq/kg and 28-677 Bq/m², respectively. At the most northern sites in the areas studied, higher^239,240Pu inventories were found corresponding to the increase of ^239,240Pu fraction which was not leached by hot digestion with conc. HNO₃+H₂O₂. The ^239,240Pu/¹³⁷Cs activity ratios for the soil samples from the southern areas lie in the narrow range of 0.016–0.039 (most of data being 0.02–0.03), probably indicative of global fallout origin. On the other hand, a little or several higher ratios (0.05 to 0.22) were found for soil samples from the northern areas. These higher ratios demonstrate strongly that there was additional Pu input of local fallout due to the atomic explosions. From ²⁴⁰Pu/²³⁹Pu atomic ratios measured, contribution of local fallout ^239,240Pu, probably from the SNTS, was found to be higher (60–86%) in the sites around the northern areas than the southern ones. The present data might serve not only as a current baseline information on distribution and contamination levels of the long-lived fallout radionuclides in the Kazakhstan areas of the Kazakhstan-Chinese border, but also as a aid of selection of control area for epidemiological projects.     

Determination of plutonium isotopes in marine particles collected by the large volume in situ filtration and concentration system

An analytical method for the determination of ²³⁹Pu and ²⁴⁰Pu in marine particle samples by sector field high-resolution ICP-MS was developed. The method was applied for large and small particle samples (particle diameter: >70 μm and 1–70 μm, respectively, collected with a large volume in situ filtration and concentration system at different depths in the water column off Rokkaho, Japan, where the spent nuclear fuel reprocessing plant of Japan Nuclear Fuel Ltd. has started test operation since March 2006.     

Determination of plutonium and other transuranic elements by inductively coupled plasma mass spectrometry: A historical perspective and new frontiers in the environmental sciences

Inductively coupled plasma mass spectrometry (ICPMS), particularly with sector field mass analyzers (SF-ICPMS), has emerged in the past several years as an excellent analytical technique for rapid, highly sensitive determination of transuranic elements (TRU) in environmental samples. SF-ICPMS has advantages of simplicity of sample preparation, high sample throughput, widespread availability in laboratories worldwide, and relatively straightforward operation when compared to other competing mass spectrometric techniques. Arguably, SF-ICPMS is the preferred technique for routine, high-throughput determination of ²³⁷Np and the Pu isotopes, excepting ²³⁸Pu, at fg-pg levels in environmental samples. Many research groups have now demonstrated the SF-ICPMS determination of ^239 + 240Pu activities, ²⁴⁰Pu/²³⁹Pu and other Pu atom ratios in several different application areas. Many studies have examined the relative contribution of global fallout vs. local/regional Pu sources in the environment through measurement of ²⁴⁰Pu/²³⁹Pu and, in some cases, ²⁴¹Pu/²³⁹Pu and ²⁴²Pu/²³⁹Pu. “Stratospheric fallout”, which was deposited from thermonuclear tests, conducted largely during the 1952–1964 time period, is characterized by a well-defined ²⁴⁰Pu/²³⁹Pu of ~ 0.18, while most other sources have different ratios. Examples of local/regional Pu sources are the Nevada Test Site, the Chernobyl plume, and accidents at Palomares, Spain and Thule, Greenland. The determination of Pu activities and atom ratios has stimulated much interest in the use of Pu as a marine tracer; several studies have shown that Pu is transported over long distances by ocean currents. ²⁴⁰Pu/²³⁹Pu ratios > 0.20 in sediments and seawater of the North Pacific are ascribed to ocean current transport of fallout from the Pacific Proving Ground. In nuclear forensics, much effort is focused on detection and fingerprinting of small amounts of TRU in environmental samples consisting of bulk material or individual isolated particles. Activity measurements of ^239 + 240Pu, determined by SF-ICPMS, have the potential to supplement and/or replace ¹³⁷Cs as a tracer of erosion, deposition, and sedimentation. Undoubtedly, the application of SF-ICPMS in TRU analysis will continue to expand, witness new developments, and generate interesting unforeseen applications in upcoming years.     

Large volume preconcentration and purification for determining the240Pu/<Superscript>239</Superscript>Pu isotopic ratio and <Superscript>238</Superscript>Pu/<Superscript>239+240</Superscript>Pu alpha-activity ratio in seawater

Summary The present paper describes a new analytical method for determining the ²⁴⁰Pu/²³⁹Pu isotopic ratio and ²³⁸Pu/^239+240Pu α -activity ratio in seawater, both of which are important parameters for determining Pu sources in the ocean. Plutonium isotopes were preconcentrated from a large volume of seawater (4700-10800 liter) by solid phase extraction using MnO₂-impregnated fibers and eluted into 3M HCl. After the elution, the Pu species of all oxidation states were converted to Pu(IV) using NaNO₂, purified by solvent extraction using thenoyltrifluoroacetone (TTA)-benzene, and concentrated in 5 ml of 0.2M HNO₂. The ²⁴⁰Pu/²³⁹Pu and ²³⁸Pu/^239+240Pu ratios in the 5-ml final solution were determined by inductively coupled plasma-mass spectrometry (ICP-MS) and α-spectrometry, respectively. A pg level of Pu, which was a sufficiently large amount for the determination, was obtained by the solid phase extraction. Through the redox conversion and solvent extraction, the Pu species, such as Pu(III), Pu(IV) and Pu(VI), were collected at a high recovery of 96±2% (n=3) despite the presence of large amounts of Mn, and interfering ²³⁸U (3.3 μg^. l^-1in seawater) was effectively removed with a decontamination factor of 1.7·10⁷. The accuracy of the method for the ²⁴⁰Pu/²³⁹Pu ratio was verified using reference materials of seawater and a terrestrial soil sample. The present technique was applied to the determination of the ²⁴⁰Pu/²³⁹Pu and ²³⁸Pu/^239+240Pu ratios in coastal and oceanic water.     

Refinement of Pu parent–daughter isotopic and concentration analysis for forensic (dating) purposes

Plutonium (Pu) metal samples from an interlaboratory exchange exercise and simulated swipe samples were dated using plutonium–uranium (Pu–U) and plutonium–americium (Pu–Am). Metal data were evaluated for consistency and the swipe data against its source material. Metal ages based on ²³⁹Pu versus ²³⁵U and ²⁴⁰Pu versus ²³⁶U agreed to within a few percent, while the ²³⁸Pu–²³⁴U and ²⁴¹Pu–²⁴¹Am measurements had larger uncertainties. Swipe ages compared favorably with the material’s known history. Neptunium (²³⁷Np) analyses were examined in the context of the ²⁴¹Pu–²⁴¹Am–²³⁷Np system to estimate whether Np can provide insights on material from which Am, Np, and U were removed.     

Dynamic surface tension and dilational viscoelasticity of adsorption layers of alkylated chitosans and surfactant–chitosan complexes

The kinetics of the adsorption at the air-water interface and the processes of the structure formation inside the adsorption layers of hydrophobically modified systems [alkylated chitosans and sodium dodecyl sulfate (SDS)–chitosan (Ch) complexes] have been studied by the tensiometric method based on the axisymmetric rising-bubble-shape analysis as a function of the bulk concentration of polymers and the ageing time of their adsorption layers. The kinetics of the adsorption of chitosan, alkylated chitosans (ChC₃, ChC₈, and ChC₁₂), and surfactant–polyelectrolyte (PE) complexes formed by the chitosan and the polysoaps with oppositely charged anionic surfactant SDS is characterized by an induction time (the so-called lag time), τ_lag, corresponding to the diffusion stage of the formation of adsorption layers. During this time, the decrease in the surface tension (or the increase in the surface pressure π) does not exceed several millinewtons per meter that corresponds to the “gaseous” state of adsorption layers. The postlag stage of the formation of the adsorption layer is characterized by the remarkable rate of increase in the surface pressure π that corresponds to the conformational rearrangement of PEs inside the adsorption layer by increasing the number of hydrophobic groups (adsorbing centres) in contact with the non-polar phase at the interface. It has been found that during the lag time, the adsorption of alkylated chitosans (cationic polysoaps) increases with increasing alkyl chain length, whereas during the postlag time, the adsorption of the ChC₃ is maximal with regard to other polysoaps. It has been confirmed that at equal content of alkyl groups in the system, the surface activity of the SDS–Ch complexes is much higher with regard to that of the polysoaps. The viscoelasticity of adsorption layers of individual PEs and their complexes continuously increases with the ageing time, giving evidence for the interaction between the polymers inside the adsorption layers. It has been found that the rate of increase in the dilational storage module E′ of the adsorption layers of SDS–Ch complexes is much higher than for the polysoaps that correlates with the higher surface activity of the former with regard to the latter. For the mentioned systems, the module E′ is much higher than the loss module E″ that confirms the solid-like properties of their adsorption layers. On the other hand, the adsorption layers of the chitosan are liquid-like, while E′<<E′′.     

<Superscript>237</Superscript>Np in peat and lichen in Finland

Activity concentrations of ²³⁷Np in peat and lichen samples in Finland were determined and contributions from nuclear weapons testing in 1950–1960s and the Chernobyl accident were estimated. ²³⁷Np was determined with ICP-MS using ²³⁵Np as a tracer. Activity concentrations of ²³⁷Np in peat samples varied between 1.98 ± 0.05 and 14.1 ± 0.3 mBq/m². The contribution from the Chernobyl accident to the total ²³⁷Np deposition in peat was 0.1–13%, the Chernobyl-derived fraction of total ²³⁷Np in peat being much lower than the previously determined corresponding Chernobyl-derived fractions of ^239+240Pu, ²⁴¹Pu, ²⁴¹Am and ²⁴⁴Cm.     

Improved method for the quantitative determination of ultra trace level of Pu-239+240 in siliceous base samples using microwave assisted dissolution

Mobilisation of alpha emitting radionuclides from silicious base sample is one the challenging task for environmental radiochemist. During this study, rapid and complete dissolution of the siliceous base samples were carried out by optimizing temperature, pressure and power of the microwaves. The Pu-239+240 in digested samples was pre-concentrated by scavenging Fe as Fe(OH)₃. Pu-239+240 was isolated from the Fe(OH)₃ by co-precipitating Pu with Bi(PO₄) in HNO₃ medium at pH 2. Pu-239+240 was separated from Bi(PO₄) and other transuranics by passing through cation and anion exchange resin. Pu-239+240 was counted by alpha spectrometry after electroplating on stainless steel planchet. The detection limits achieved for Pu-239+240 was 60 μBq/g (2.6 × 10⁻¹⁴ g/g). Pu-242 was used as a tracer for the evaluation of recovery of Pu-239+240. Samples prepared after complete destruction of matrix in microwave, showed 10–20% higher concentration of Pu-239+240 compared to conventional acid leached. Consistent recovery in the range of 97–99% for Pu-242 were observed in microwave digested samples whereas inconsistent results were observed in acid leached samples where the recoveries were in the range of 75–86%. Siliceous matrix degradation was tracked by monitoring the surface morphology and composition of the residue left at various stages of digestion using Scanning Electron Microscope (SEM) coupled with Energy dispersive X-ray spectrometer (EDS).     

Actinide targets for neutron cross section measurements

The Advanced Fuel Cycle Initiative (AFCI) and the Generation IV Reactor Initiative have demonstrated a lack of detailed neutron cross sections for certain “minor” actinides. For some closed-fuel-cycle reactor designs more than 50% of reactivity will, at some point, be derived from “minor” actinides that currently have poorly known or in some cases not measured (n,γ) and (n,f) cross sections. Using a combination of resurrected techniques and new developments, we have made a series of targets including highly enriched ²³⁹Pu, ²⁴⁰Pu, and ²⁴²Pu. Thus far, we have electrodeposited these actinide targets. The chemical purification and electodeposition techniques will be described.     

Evaluation of 239+240Pu, 137Cs and natural 210Pb fallout in agricultural upland fields in Rokkasho, Japan

The background distributions of ^239+240Pu and ¹³⁷Cs fallout in agricultural soil were investigated in Rokkasho where Japan's first commercial nuclear fuel reprocessing plant is now being constructed. The mean inventories of ^239+240Pu and ¹³⁷Cs in three fields with non-yam-cultivation history were 116 Bq·m⁻² and 3.4 kBq·m⁻², respectively. The mean atomic ratio of ²⁴⁰Pu/²³⁹Pu for all studied fields was 0.18±0.04, and was similar to that of global fallout. The ^239+240Pu concentrations correlated very well with ¹³⁷Cs (r = 0.97) in spite of heavy disturbance of the soil, and the activity ratio of ^239+240Pu/¹³⁷Cs was 0.037±0.007, which is a typical value for global fallout. These results showed that the nuclides had similar behavior in agricultural upland fields in Rokkasho. Since ²¹⁰Pb is steadily deposited from the atmosphere to the land, this nuclide could be an index for the degree of disturbance of a field and of soil lost from the field. The ratio of excess ²¹⁰Pb inventory in the soil to the equivalent inventory of atmospheric ²¹⁰Pb deposition was 96%, and indicated that soil was not lost from the cultivated fields. This revised version was published online in July 2006 with corrections to the Cover Date.