Adsorption-desorption of 241Am(â ¢) on montmorillonite colloids and quartz sand: Effects of pH, ionic strength, colloid concentration and grain size.

Clay colloids in the subsurface environment have a strong adsorption capacity for radionuclides, and the mobile colloids will carry the nuclides for migration, which would promote the movability of radionuclides in the groundwater environment and pose a threat to the ecosphere. The investigations of the adsorption/desorption behaviors of radionuclides in colloids and porous media are significant for the evaluation of the geological disposal of radioactive wastes. To illustrate the adsorption/desorption behaviors of 241Am(Ⅲ) in Na-montmorillonite colloid and/or quartz sand systems at different pH (5, 7 and 9), ionic strengths (0, 0.1 and 5 mM), colloid concentrations (300 and 900 mg/L), nuclide concentrations (500, 800, 1100 and 1400 Bq/mL) and grain sizes (40 and 60 mesh), a series of batch sorption-desorption experiments were conducted. Combining the analysis of the physical and chemical properties of Na-montmorillonite with the Freundlich model, the influencing mechanism of different controlling factors is discussed. The experimental results show that the adsorption/desorption behaviors of 241Am(Ⅲ) in Na-montmorillonite colloid and/or quartz sand strongly are influenced by the pH value and ionic strength of a solution, the colloid concentration as well as quartz sand grain size. The adsorption and desorption isotherms within all the experimental conditions could be well-fitted by the Freundlich model and the correlation coefficients (R2) are bigger than 0.9. With the increase in pH, the adsorption partition coefficient (Kd) at 241Am(Ⅲ)-Na-montmorillonite colloid two-phase system and 241Am(Ⅲ)-Na-montmorillonite colloid-quartz sand three-phase system presents a trend which increases firstly followed by decreasing, due to the changes in the morphology of Am with pH. The Kd of 241Am(Ⅲ) adsorption on montmorillonite colloid and quartz sand decreases with increasing in ionic strength, which is mainly attributed to the competitive adsorption, surface complexation and the reduction of surface zeta potential. Additionally, the Kd increases with increasing colloid concentrations because of the increase in adsorption sites. When the mean grain diameter changes from 0.45 to 0.3 mm, the adsorption variation trends of 241Am(Ⅲ) remain basically unchanged. The research results obtained in this work are meaningful and helpful in understanding the migration behaviors of radionuclides in the underground environment.

Vertical distribution of 241Am in the southern Baltic Sea sediment profiles.

The contamination of the Baltic Sea with radioactive substances occurred due to the global fallout of atmospheric nuclear weapon tests and the Chernobyl disaster. The knowledge of 241Am in the sediments of the Baltic Sea is limited. Thus, this study aimed to determine 241Am in sediment cores collected from the southern Baltic Sea. Time-based distributions were derived from age-depth profiles using the 210Pb dating method and further corroborated by 137Cs profiles. The activities of 241Am were measured by alpha spectrometry after radiochemical purification. The results show divergences in the concentrations of 241Am at the local level, varying from 0.017 ± 0.001 Bq·kg-1 at the Gotland Basin station to 3.19 ± 0.23 Bq·kg-1 in the Gdansk Basin. These findings enhance our understanding of the radioactive contamination levels in the Baltic Sea and serve as a crucial reference dataset for future assessments and management strategies to mitigate the environmental impact of radionuclides in the region.

A multi-collector ICP-MS method for quantification of plutonium, uranium, and americium in hair and nails of occupationally or medically exposed individuals.

The 239Pu, 238U, and 241Am concentrations and 239Pu/240Pu, 235U/238U, and 236U/238U atom ratios were measured in the hair and nail samples using a new method utilized TEVA, UTEVA, and DGA extraction chromatography and multi-collector ICP-MS. Samples were collected from individuals who donated their bodies to the United States Transuranium and Uranium Registries. The concentration of 239Pu ranged from 0.22 to 15.8 ng/kg. The 240Pu/239Pu isotopic ratios ranged from 0.026 to 0.127 which is consistent with weapons-grade plutonium. Concentration of uranium fell between 1.84 µg/kg and 29.5 µg/kg and 235U/238U ratios ranged from 4.8 × 10-3 to 7.6 × 10-3. Elevated 236U/238U atom ratios were measured in two cases and ranged from 5.0 × 10-6 - 2.4 × 10-5 indicating exposure to spent or reprocessed uranium material. The concentration of 241Am was measured in four hair samples and ranged from 0.02 to 0.21 ng/kg.

Bioaccumulation of radionuclides in hoofed animals inhabiting the Semipalatinsk Test Site.

The article assesses the content of radionuclides in hoofed animals inhabiting the Semipalatinsk Test Site by calculation. Hoofed animals' faeces were sampled to determine the content of radionuclides in their diets. Based on values determined for the content of radionuclides in animals; diets, the content of radionuclides in the meat and milk of farm animals-cows (Bos taurus taurus), sheep (Ovis), goats (Capra hircus) and horses (Equus caballus Lin., 1758) as well as in the meat of wild animals-european moose (Alces alces Lin., 1758), argali (Ovis ammon Lin., 1758), roe deer (Capreolus pygargus Pal., 1771) and saiga (Saiga tatarica Lin., 1766) was calculated. No excess of permissible values of the content of 137Cs and 90Sr in the meat of farm animals was found to be expected, even for a conventional 'conservative' scenario, in which maxima of the radionuclide activity concentration in a vegetable feed (faeces) are taken as a basis. 241Am and 239+240Pu in the meat of farm hoofed animals are not standardized. Their predicted maxima of activity concentration are very low, and even in the 'conservative' scenario, they do not exceed 1.8×10-2 Bq kg-1, 1.4×10-1 Bq kg-1 and 1.6×10-1 Bq kg-1, respectively. In the milk of farm animals, the content of 137Cs and 90Sr does not exceed permissible values. 241Am and 239+240Pu in the milk of farm animals are not standardized. Their predicted activity concentration values in the milk of sheep and goats do not exceed 6.5×10-2 Bq l-1, for cows- 2.6×10-2 Bq l-1, for horses- 3.1×10-2 Bq l-1. Permissible values of 137Cs and 90Sr in the meat of wild hoofed animals are not exceeded either. In the meat of argali, roe deer and saigas, relatively high levels of 137Cs are predictable. 241Am and 239+240Pu in meat of wild animals are not standardized. Their predicted activity concentration values in the meat of moose and argali do not exceed 3.2×10-1 Bq kg-1 and 1.6×10-1 Bq kg-1, respectively, for roe deer and saiga-5.4×10-2 Bq kg-1. Thus, in case of free grazing in the STS territory, no excess of permissible values of standardized radionuclides (137Cs and 90Sr) in the meat and milk of hoofed animals is predictable.

THE NATIONAL RESEARCH COUNCIL OF CANADA MANGANESE BATH SYSTEM.

The manganese salt bath is considered a primary standard for determining the absolute emission rate of radionuclide neutron sources. The National Research Council of Canada has recently revived its manganese salt bath and a full description of the system is given here. The physical characteristics of the bath, as well as the methods for determining the efficiency of the bath system and the induced activity in the bath, are described. An in-depth analysis of the fraction of neutrons captured in the manganese and the correction factor for neutron losses is also provided. Finally, the results of emission rate measurements of four different sources, complete with an uncertainty budget, are given. The emission rates of three americium-beryllium neutron sources and one californium-252 neutron source were found to agree with the known values, within a standard uncertainty of 1.7%.

Vertical distribution of radionuclides in soil at the Semipalatinsk Test Site beyond its test locations.

Data on the vertical distribution of radionuclides in the soil is necessary to fully understand the radioecological situation around ecosystems, give predictive estimates to how safe crop products are and justify a rehabilitation strategy for radioactively contaminated areas. A study was conducted to investigate the vertical distribution of radionuclides in soils of the former Semipalatinsk Test Site (STS) territory beyond its testing sites, that is, in areas in which no nuclear weapons or nuclear effects of radiological warfare agents were tested. Soil was sampled layerwise all over the Semipalatinsk Test Site down to 30 cm deep at a 5-cm spacing. Most of high activity concentrations of radionuclides all over the study area were detected in the 0-5 cm soil layer. Activity concentrations of the major man-made radionuclides were determined in soil samples collected by γ-, ß and α-spectrometry. As a result, ranges of activity concentrations of 137Cs, 241Am, 90Sr and 239+240Pu were determined in 0-5, 5-10, 10-15, 15-20, 20-25, 25-30 cm soil layers. In the conventionally 'background' area, the 0-5 cm soil layer, on average, contains (the percentage of total activity concentration across the soil profile depth): 137Cs- 83%, 239+240Pu- 87% and 90Sr- 38%. For the 1953 plume, these values were 92%, 83% and 73%, respectively. Values for the 1951 plume in the 0-5 cm soil layer were: 137Cs- 93%, 239+240Pu- 93% and 90Sr- 59%. The minimum concentration of radionuclides are observed 20-30 cm deep in all areas studied. 90Sr is the most mobile radionuclide from the perspective of its ability to travel deep down the soil. The study found out that the nuclide vertical migration rates downward in soils based on detected activity were as follows (in descending order): 90Sr- 137Cs- 239+240Pu- 241Am. Coefficients that determine the ratio of the activity concentration of the radionuclide in the 0-20 and 0-30 cm soil cover layers to that of this radionuclide in the 0-5 cm topsoil were calculated. These coefficients enable to estimate the radionuclide inventory at each soil sampling point from their activity concentration in the 0-5 cm soil layer.

Experimental assessment of 241Am accumulation in Carassius gibelio from amphipods.

Accumulation of dietary 241Am in freshwater omnivorous fish (Carassius gibelio) was studied aiming to estimate the distribution and retention of 241Am in the fish body. Amphipods labeled with 241Am served as a food item. From 0.4 to 0.6% of ingested 241Am was retained in the fish body after short courses of feeding and depuration, the trophic transfer factor of 241Am for whole organism level was about 2∙10-4.

POLYETHYLENE FILTER FOR THE TNF2 THERMAL NEUTRON FACILITY.

The Standard Thermal Neutron Flux Unit, TNF2, in (LNMRI/IRD)(1,  2), was built for neutron detector and survey meter calibrations. The facility's fluence is achieved by moderation of four 241Am-Be with a graphite core and paraffin/graphite blocks surrounding it. Due to the small channel dimensions, it is impossible to calibrate personal dosemeters and survey meters for thermal neutrons. A polyethylene filter construction was carried out to allow the external irradiation of personal dosemeters and neutron survey meters. The polyethylene filter was constructed with 29 stacked discs with diameters ranging from 5 to 34 cm. Different thicknesses were simulated to provide the desired effect. This new irradiation configuration was also experimentally tested and compared with simulation results with MCNPX(3).

Assessment and clinical management of internal contamination.

Internal contamination by radionuclides may occur through inhalation, ingestion and absorption through the skin or subcutaneous tissue. The clinical management of internalized radionuclides requires the integration of clinical signs and symptoms with dose estimates in biological tissues obtained from the face, nose, sputum, urine, faeces and/or skin. The assessment of ingested radionuclides includes bioassays of urine and faeces, and if available, whole body counting for radionuclides that emit penetrating x-rays or gamma-rays. An estimate of intake dose may be made at the time of initial patient evaluation by measuring radioactivity, converting counts/minute to depositions/minute with a specific gamma-ray constant, and comparing the amount to its annual limit on intake, clinical decision guide or derived reference level. Since nobody dies from internal contamination per se, medically unstable patients should be stabilized before addressing internal contamination. Whenever possible, internal contaminants should be physically removed as soon as possible after exposure. For inhaled internal contaminants, radionuclide-specific therapy may include the administration of an ion exchange resin (i.e. Prussian blue, PB) or chelating agent (i.e. diethylenetriamine pentaacetate, DTPA, that binds toradioactiveplutonium, americium, and curium), or the physical removal of insoluble particles with a high activity radionuclide (192Ir,90Sr,210Po) by bronchioalveolar lavage. Decorporation with PB, DTPA and other agents is used to enhance excretion. The treatment of wounds contaminated with an actinide includes gentle irrigation, surgical excision of contaminated tissue and DTPA. The averted dose (i.e. the total effective dose averted by therapy) may be calculated for each exposure route.

Use of an Acellular Assay to Study Interactions between Actinides and Biological or Synthetic Ligands.

Speciation of actinides, and more particularly bioligand-binding ability, influences in vivo behavior. Understanding these interactions is essential for estimation of radiological dose and improvement of decorporation strategies for accidentally contaminated victims. Because the handling of actinides imposes overwhelming difficulties, in vitro assays carried out in physiological conditions are lacking and data regarding such interactions are scarce. In this study, we used a bi-compartmental and dynamic assay, providing physiological conditions (presence of inorganic ions, pH, temperature) to explore interactions between the actinides plutonium (Pu) and americium (Am) and endogenous (proteins transferrin and ferritin) or exogenous ligands (the chelating agent diethylenetriaminpentaacetic acid, DTPA). In this assay, an agarose gel represents the retention compartment of actinides and a dynamic fluid phase, the transfer compartment. The proportion of actinides transferred from static to dynamic phase reflects interactions between Pu/Am and various ligands. The results show differences in the formation of actinide-protein or actinide-DTPA complexes in physiologically relevant media depending on which ligand is present and where. We observed differential behavior for Pu and Am similar to in vivo studies. Thus, our assay may be used to determine the ability of various actinides to interact with specific proteins or with drug candidates for decorporation in complex physiologically relevant environments.

The use of plastic scintillation microspheres in flow scintillation analysis.

This manuscript deals with the possible utilization of plastic microspheres for radiation detection. The aim was to determine the suitability of microspheres for this application, factors that affect detection efficiency, and based on the evaluation of current state technology to design and test a constructional solution suitable for this use. Three detection cell variations and their configurations, which utilize plastic microspheres, were tested for their response to selected militarily important radionuclides during a series of static measurements. Based on the results of static measurements, the most structurally suitable cell variation was subsequently tested for flow scintillation analysis. Among the cells designed for flow scintillation counting in 2π geometry, the highest achieved detection efficiency for 241Am was 13.1 ± 0.7% using Cell #5, for 90Sr/Y was 71.2 ± 3.9% using Cell #10 and for 3H was 3.9 ± 0.2% using Cell #5 respectively. Cell #10 was evaluated to perform universally the best despite achieving slightly lower detection efficiencies for 241Am and 3H than Cell #5, as the results were easily replicable and due to the cell constructional simplicity, its application was problem-free.

YAP:CE SCINTILLATOR APPLICATION FOR 241AM COUNTING IN WOUND INJURY.

YAP:Ce scintillation probe was tested for use in a spectrometric measurement that is necessary to assess the internal dose in case of wound injuries involving radionuclide contaminant. A technique with metal filters published in the past for the determination of a depth of plutonium-contaminated wound was tested to verify the capability of the scintillator to be used for gamma-ray spectrometry counting of 241Am in a wound injury. Scintillation probe equipped with YAP:Ce scintillator showed properties sufficient for the wound counting technique tested.

Contaminant release, mixing and microbial fluctuations initiated by infiltrating water within a replica field-scale legacy radioactive waste trench.

Numerous legacy near-surface radioactive waste sites dating from the mid 20th century have yet to be remediated and present a global contamination concern. Typically, there is insufficient understanding of contaminant release and redistribution, with invasive investigations often impractical due to the risk of disturbing the often significantly radiotoxic contaminants. Consequently, a replica waste trench (~5.4 m3), constructed adjacent to a legacy radioactive waste site (Little Forest Legacy Site, LFLS), was used to assist our understanding of the release and mixing processes of neodymium (Nd) - a chemical analogue for plutonium(III) and americium(III), two significant radionuclides in many contaminated environments. In order to clarify the behaviour of contaminants released from buried objects such as waste containers, a steel drum, representative of the hundreds of buried drums within the LFLS, was placed within the trench. Dissolved neodymium nitrate was introduced as a point-source contaminant to the base of the trench, outside the steel drum. Hydrologic conditions were manipulated to simulate natural rainfall intensities with dissolved lithium bromide added as a tracer. Neodymium was primarily retained both at its point of release at the bottom of the trench (>97 %) as well as at a steel container corrosion point, simulated through the emplacement of steel wool. However, over the 8-month field experiment, advective mixing initiated by surface water intrusions rapidly redistributed a small proportion of Nd to shallower waters (~1.5-1.7 %), as well as throughout the buried steel drum. Suspended particulate forms of Nd (>0.2 µm) were measured at all depths in the suboxic trench and were persistent across the entire study. Analyses of the microbial communities showed that their relative abundances and metabolic functions were strongly influenced by the prevailing geochemical conditions as a result of fluctuating water depths associated with rainfall events. The site representing steel corrosion exhibited divergent biogeochemical results with anomalous changes (sharp decrease) observed in both dissolved contaminant concentration as well as microbial diversity and functionality. This research demonstrates that experimental trenches provide a safe and unique method for simulating the behaviour of subsurface radioactive contaminants with results demonstrating the initial retention, partial shallow water redistribution, and stability of particulate form(s) of this radioactive analogue. These results have relevance for appropriate management and remediation strategies for the adjacent legacy site as well as for similar sites across the globe.

Simulation of a new neutron calibration laboratory in Brazil using MCNP5.

Metrobras, a private company in Brazil, is developing a new laboratory for the calibration of neutron detectors in collaboration with the National Laboratory for Metrology of Ionizing Radiation (LNMRI). This work aimed at assessing neutron spectra, ambient dose equivalent rates, and neutron scattering in the calibration room of Metrobras Neutron Detectors Calibration Laboratory (LCDNM) using Monte Carlo simulation with MCNP5. Three models were simulated: vacuum, air, and the complete with the several materials employed in the actual room. Neutron spectra as a function of the distance from the source were obtained, compared, and used to calculate ambient dose equivalent at different points in the calibration room and results were compared to other neutron laboratories. Results show that LCDNM ambient dose equivalent rates are comparable to those of other neutron laboratories with 531.2 µSv . h-1 at 100 cm from the 592 GBq activity 241AmBe source. This work shows that LCDNM may be used as a calibration laboratory for neutron detectors in accordance with ISO 8529.

High-resolution records of cesium, plutonium, americium, and uranium isotopes in sediment cores from Swiss lakes.

The Aare river system in Switzerland, with two nuclear power plants on the banks of the river, and its intermediate lakes and reservoirs, provides a unique opportunity to analyze the contribution of different sources to the radioactive contamination. Sediment cores were collected from two lakes and a reservoir, all connected by the river Aare. In order to study the influence of the Chernobyl accident, one sediment core was collected from a lake in the southern part of Switzerland. The sediment cores were sliced and analyzed with gamma ray spectrometry. Plutonium, americium, and uranium were extracted radiochemically, and their concentrations were measured with a sector field ICP-MS. The uranium isotope ratios were further measured with a multi collector ICP-MS. The maximum 137Cs activity from the Chernobyl accident and the Pu and 137Cs activities associated to the 1963 global fallout maximum were well identified in sediments from all three lakes. High-resolution records of plutonium isotopes in the zone of the sediments corresponding to the period of maximum fallout from the atmospheric nuclear weapon testing showed distinct fingerprints, depending on the different test activities. Pu isotope ratios could be used to detect non-global fallout plutonium. The ratio 241Am/241Pu was used to determine the age of the plutonium. Despite of very low 241Pu and 241Am concentrations, the calculated plutonium production dates seemed to be reasonable for the sediment layers corresponding to the NWT tests. The calculated production date of the plutonium in the upper most 15 cm of the sediment core seemed to be younger. The reason for this could be additional non-global fallout plutonium. For the lake sediments, natural ratios for 235U/238U and enriched or depleted ratios for 234U/238U were measured, depending on the lake. A small increase of the 236U/238U ratio could be recognized for the NWT zone in all three lakes and, for Lake Lugano, a further distinct increase in the Chernobyl layer.

Development of a rapid technique for sequential separation of plutonium/americium in nasal swab using solvent extraction and liquid scintillation spectrometry.

A rapid radiochemical method has been developed for estimation of plutonium and americium in nasal swab using extractive liquid scintillation spectrometry. The method involves solvent extraction of plutonium and americium from pre-treated nasal swab using 0.2 M Di-(2-ethylhexyl)phosphoricacid prepared in toluene scintillator & back extraction of americium in aqueous phase using 0.35 M HNO3. Activity assessment was carried out using liquid scintillation spectrometry. Overall recovery obtained was 96% for plutonium and 76% for americium with a sample turnaround time of 3 h.

Investigation of Radionuclide Migration at Sites Adjacent to the 30-km Exclusion Zone of the Chernobyl Nuclear Power Plant.

ABSTRACT: This paper reports the study of the vertical migration of radionuclides in soils at test sites adjacent to the 30-km Chernobyl Exclusion Zone. The results of this effort demonstrate that the migration processes for studied pollution occur similarly to the fuel fallout behavior at the vicinity of the Chernobyl Nuclear Power Plant (ChNPP) Unit 4. It was also observed that the main fallout component, 137Cs, originated from aerosol fallout and was bound in the surface layer. The authors determined a significant increase of 60Co, 94Nb, and 241Am radionuclide concentrations in soils near the ChNPP Unit 4 and suggested their appearance due to the installation of the New Safe Confinement. Niobium-94 activity is proposed as a marker for monitoring the "fresh" fallout in the Chernobyl Exclusion Zone.

ESTIMATION OF SCATTERED NEUTRONS CONTRIBUTION IN A NEUTRON CALIBRATION BUNKER USING A MONTE CARLO SIMULATION.

The contribution of scattered neutrons is inevitable in neutron calibration facilities. This contribution complicates the measurements of neutron radiation, therefore, it should be estimated to correct the response of neutron probe instruments. In the present work, Monte Carlo simulation was performed for a neutron calibration bunker using the MCNP-4C code. This simulation aimed to calculate the contribution ratio of scattered neutrons to the neutron field. To simulate the neutron field, 241Am-Be neutron source defined in the ISO 8529-1 was used. The results of the simulation reported in this work were found to be consistent with those found experimentally in previous work. Additionally, the distribution of both the ambient dose equivalent rate and the contribution ratio of scattered neutrons in the bunker were mapped using this simulation.

A METHOD TO IDENTIFY AND LOCALIZE A SINGLE HOT PARTICLE IN THE LUNGS USING AN ARRAY OF HIGH-PURITY GERMANIUM DETECTORS FOR IMPROVED ESTIMATE OF THE DEPOSITED ACTIVITY.

A new method has been developed to identify and localize a single hot particle in the lungs using an array of four high-purity germanium detectors. The method is based upon calculating a set of three count rate ratios (generated by each individual detector in the array) that are evaluated in sequence to designate whether the measured deposition can be associated with a hot particle rather than the default assumption of a uniform activity distribution. Identification and localization of the hot particle are determined from a single in vivo measurement in which detectors are positioned above and below the thorax. The method was tested using an anthropomorphic thorax phantom in which point sources of 241Am, 137Cs and 60Co were individually inserted in the lungs at 15 different locations and were measured using a scanning bed whole-body counter. Depending upon source location and photon energy, a bias of -35% up to +76% could be introduced by falsely assuming a uniform activity distribution in the lungs. This bias would directly translate to an erroneous dose estimate to the lungs. It was demonstrated that by using the appropriate detector efficiencies for the single hot particle, the bias associated with the activity determination is reduced to <10% and ~2% in average.

Americium Inhalational Exposure with Successful Chelation Therapy.

Americium is a man-made metal produced in very small quantities in nuclear reactors. Americium-241 is one of the radioactive isotopes of americium and has commercial applications, including use in smoke detectors. This is a case report of an occupational inhalation of americium-241, treated with both effective external decontamination and the use of diethylenetriamine pentaacetate to promote decorporation. This experience is significant because of the potential for americium or similar radionuclides to be used in "dirty" bombs or other radiological dispersion devices to cause large-scale radioactive contamination.