Shawki A. Ibrahim

The plant/soil concentration ratio for calcium, radium, lead, and polonium: Evidence for non-linearity with reference to substrate concentration

Evidence exists from both the literature and our own observations that plant nuclide uptake for a variety of plants and elements is a non-linear function of substrate concentration. The uptake response to increasing substrate concentration is usually in the form of a single or multi-phasic saturation curve. For some plant types and elements the uptake response may also take the form in which a threshold of soil activity is necessary before uptake is measurable. We present a generic uptake response curve and the resulting concentration ratio function determined by computer simulation. Data describing the uptake response of plants to 226Ra, 210Pb and 210Po as well as for calcium and stable lead are discussed. Functions are also presented for these elements to describe the uptake response and the concentration ratio and their mathematical forms are compared to the generic model.

Plutonium concentration in human tissues: comparison to thorium.

The concentration of 238Pu, and 239,240Pu, and of 228Th, 230Th, and 232Th were measured in 10 sets of human tissues from Washington, DC, and 12 sets from Grand Junction, CO. The tissues were collected at autopsy by qualified pathologists from normal healthy persons most of whom died suddenly. The subjects had acquired plutonium from fallout of global nuclear testing and burnup of a space nuclear generator utilizing 238Pu. The median concentration of 239,240Pu was 0.08 pCi/kg in lung, 0.46 pCi/kg in tracheobronchial lymph nodes, 0.60 pCi/kg in liver, 0.02 pCi/kg in kidney and 0.17 pCi/kg in bone in Washington, DC subjects. Similarly, the concentration of 239,240Pu in Grand Junction subjects was found to be 0.17 pCi/kg in lung, 0.68 pCi/kg in lymph nodes, 0.55 pCi/kg in liver, 0.03 pCi/kg in kidney, 0.22 pCi/kg in bone and 0.08 pCi/kg in spleen. The median concentration in four gonads was 0.02 pCi/kg; the concentration in one thyroid was 0.01 pCi/kg. 238Pu was below the limit of detection in most organs except the liver where it ranged from 0.02 to 0.17 pCi/kg with a median concentration of 0.06 pCi/kg. The organ distribution pattern shows that most of the plutonium was accumulated in bone and liver with 54-60% in bone and 34-43% in liver. Only 3-6% was found in lung including lymph nodes; kidney, spleen, thyroid and gonads together contained around 1%. The analytical results show three major differences between plutonium and thorium concentrations and organ distributions: (1) for plutonium the liver is a major locus for storage (approximately 40% of that found in the total body), whereas little thorium is accumulated in the liver (around 4%); (2) the relative amounts of 230Th and 232Th are much higher in lung and lymph nodes (10-28%) than currently for plutonium (3-6%); (3) the ratio of throium concentrations in lymph nodes to lung is significantly higher than the ratio of plutonium concentration in lymph nodes to lung showing thereby that fallout plutonium is more soluble than natural thorium.

Sorption of Cs and Sr to profundal sediments of a Savannah River Site reservoir

Laboratory measurements of the sorption and desorption of 134Cs and 85Sr to sediments were conducted. These sediments were sampled from the top 1 cm of the profundal zone of Par Pond at the Savannah River Site, Aiken, South Carolina. The isotopes 134Cs and 85Sr were used to trace the sorption properties of the main contaminants found in the reservoir, which are 137Cs and 90Sr, respectively. The sorption behavior of these two elements was studied using spiked sediment/water slurries of a variable, but known, mass to volume ratio. The results reveal that Sr undergoes significant reversible sorption while a fraction of Cs irreversibly sorbs to the sediment. The Kd for 137Cs was a function of the slurry ratio, pH, conductivity, and contact time. These factors were inter-related since the sediments released ions to the slurry mixture which simultaneously decreased the pH and increased the conductivity. The calculated Kd at equilibrium was 2.8 × 104 for 134Cs after 60 days and 1 × 103 for 85Sr after 7 days at a pH ~ 6 and a slurry ratio of 1:1000 g/ml.

Comparison of 241Am, 239,240Pu and 137Cs concentrations in soil around rocky flats

Gamma spectroscopy measurements were used to estimate concentrations of 241Am and 137Cs in soil profiles to depths of 21 cm at on-site and off-site locations around the Rocky Flats Environmental Technology Site and at regional background locations east of the Front Range between Colorados borders with New Mexico and Wyoming. Concentrations of these radionuclides were compared with concentrations of (239,240)Pu in the same samples. Concentrations of 241Am in soil from depths of 0 to 3 cm decreased in an easterly direction from more than 5.3 kBq kg(-1) near the 903 pad to background levels of 1.3 Bq kg(-1) 5 to 7 km away at a rate that was nearly proportional to the inverse square of distance. Deposits of 137Cs were ubiquitous, averaging 0.12 kBq kg(-1) in soil from depths of 0 to 3 cm, but were unevenly distributed around Rocky Flats and the regional background locations. Deviations from the uniform exponential rate at which soil concentrations of 137Cs typically decreased with depth, -0.25 cm(-1) at undisturbed sites, enabled us to determine that about 10% of our sampling sites had been disturbed by erosion, tillage, or other factors. The mean rate at which (239,240)Pu decreased with depth was about the same, -0.23 cm(-1), throughout the study area. Soil concentrations of 241Am decreased with depth at a similar mean rate of -0.22 cm(-1) at locations close to the 903 pad where measurements were robust. Ratios between 241Am or (239,240)Pu and 137Cs proved more useful for delineating the extent and pattern of contamination from Rocky Flats than did activity concentrations in soil.

Thorium concentration in human tissues from two U.S. populations.

The concentrations of natural alpha-emitting isotopes of thorium (228Th, 230Th and 232Th) have been determined in 22 sets of human tissue samples obtained at autopsy from Grand Junction, CO and in 10 sets from Washington, DC. Tissues included lung, pulmonary lymph nodes, liver, kidney, bone, a few gonads, spleen and thyroid. Personal data on each individuals age, sex, smoking history and occupation were obtained whenever possible. The concentrations of 228Th, 230Th and 232Th were highest in lymph nodes for both populations with 2.6 and 5.1 pCi/kg of 228Th, 4.60 and 11.10 pCi/kg of 230Th, and 2.8 and 7.8 pCi/kg of 232Th in Washington, DC and Grand Junction, CO, respectively. The order of concentrations of all three isotopes in all other organs for both populations was as follows: (formula; see text) The data suggest that the non-mining residents who lived in the vicinity of uranium mine tailings do not have elevated 230Th concentrations in their lungs, when compared to the residents of Washington, DC who are not exposed to such tailings. However, 230Th concentration in bone of Grand Junction subjects was just significantly higher (at p less than 0.1) than that for Washington, DC subjects after suitable age adjustments. The data also suggest that 230Th is more available for accumulation in skeleton than would be supposed from its relative geochemical abundance.

Estimation of the Metabolic Rate of the Desert Iguana (Dipsosaurus dorsalis) by a Radionuclide Technique

We describe a method for measuring metabolic rates (MRs) of ectotherms using successive measurements of radionuclide body burdens, which may provide an alternative means of measuring field metabolic rate (FMR). Although MRs can be measured in the laboratory, variability in food supply and quality, temperature, activity, and other factors preclude the direct application of such data to field conditions. Recently, the doubly labeled water (DLW) technique has been successfully applied to estimate FMR in a variety of animals, but this method is expensive, requires special equipment, necessitates the sampling of blood or other body fluids, and may be unsuitable for certain species. We compared the rates of elimination of seven radionuclides with estimates of MRs (CO₂ production) from DLW measurements in the desert iguana, Dipsosaurus dorsalis. We observed temperature-dependent elimination for five of the radionuclides, and found a high correlation (r² = 0.93) between the slopes of individual 86Rb elimination curves and the MRs estimated by the DL W technique. This correlation appeared to be relatively insensitive to differences in water turnover and ingestion of the stable nutrient analog (K). The results suggest that a practical and inexpensive method for measuring FMRs of ectotherms may be derived from this relationship.

Uranium partition coefficients (Kd) in forest surface soil reveal long equilibrium times and vary by site and soil size fraction.

The environmental mobility of newly deposited radionuclides in surface soil is driven by complex biogeochemical relationships, which have significant impacts on transport pathways. The partition coefficient (Kd) is useful for characterizing the soil-solution exchange kinetics and is an important factor for predicting relative amounts of a radionuclide transported to groundwater compared to that remaining on soil surfaces and thus available for transport through erosion processes. Measurements of Kd for 238U are particularly useful because of the extensive use of 238U in military applications and associated testing, such as done at Los Alamos National Laboratory (LANL). Site-specific measurements of Kd for 238U are needed because Kd is highly dependent on local soil conditions and also on the fine soil fraction because 238U concentrates onto smaller soil particles, such as clays and soil organic material, which are most susceptible to wind erosion and contribute to inhalation exposure in off-site populations. We measured Kd for uranium in soils from two neighboring semiarid forest sites at LANL using a U.S. Environmental Protection Agency (EPA)-based protocol for both whole soil and the fine soil fraction (diameters <45 &mgr;m). The 7-d Kd values, which are those specified in the EPA protocol, ranged from 276–508 mL g−1 for whole soil and from 615–2249 mL g−1 for the fine soil fraction. Unexpectedly, the 30-d Kd values, measured to test for soil-solution exchange equilibrium, were more than two times the 7-d values. Rates of adsorption of 238U to soil from solution were derived using a 2-component (FAST and SLOW) exponential model. We found significant differences in Kd values among LANL sampling sites, between whole and fine soils, and between 7-d and 30-d Kd measurements. The significant variation in soil-solution exchange kinetics among the soils and soil sizes promotes the use of site-specific data for estimates of environmental transport rates and suggests possible differences in desorption rates from soil to solution (e.g., into groundwater or lung fluid). We also explore potential relationships between wind erosion, soil characteristics, and Kd values. Combined, our results highlight the need for a better mechanistic understanding of soil-solution partitioning kinetics for accurate risk assessment. Health Phys. 93(1):36–46; 2007

Spatial variations in natural background radiation : Absorbed dose rates in air in Colorado

Large and small-scale spatial variations in natural ambient background radiation dose rates in Colorado were investigated at 1,150 specific locations with particular attention to 40 of the more populated areas along the Front Range of the Rocky Mountains. Total dose rates (including cosmic and terrestrial components) in Front Range communities below 2,000 m elevation averaged 135 nGy h -1 . Terrestrial dose rates had a coefficient of variation of 17%. Communities above 2,000 m had a mean total dose rate of 196 nGy h -1 , and a terrestrial dose rate coefficient of variation of 17%. Across all Front Range communities, the coefficient of variation for terrestrial dose rates was 22%. Within individual communities, coefficient of variation values for terrestrial dose rates ranged from 3 to 21%. Smaller-scale spatial variability (to within a few meters) was relatively small (coefficient of variation values generally ranged from 3 to 7%). A significant linear relationship (r 2 = 0.83) between the size of area surveyed (km 2 ) and coefficient of variation value for terrestrial dose rates was found. West of the Continental Divide, the terrestrial component accounted for roughly 60% of total measured dose rates, while east of the Continental Divide, where enriched granitic source rocks and associated soils are prevalent, the terrestrial component generally accounted for two-thirds or more of total dose rates.Large and small-scale spatial variations in natural ambient background radiation dose rates in Colorado were investigated at 1,150 specific locations with particular attention to 40 of the more populated areas along the Front Range of the Rocky Mountains. Total dose rates (including cosmic and terrestrial components) in Front Range communities below 2,000 m elevation averaged 135 nGy h(-1). Terrestrial dose rates had a coefficient of variation of 17%. Communities above 2,000 m had a mean total dose rate of 196 nGy h(-1), and a terrestrial dose rate coefficient of variation of 17%. Across all Front Range communities, the coefficient of variation for terrestrial dose rates was 22%. Within individual communities, coefficient of variation values for terrestrial dose rates ranged from 3 to 21%. Smaller-scale spatial variability (to within a few meters) was relatively small (coefficient of variation values generally ranged from 3 to 7%). A significant linear relationship (r2 = 0.83) between the size of area surveyed (km2) and coefficient of variation value for terrestrial dose rates was found. West of the Continental Divide, the terrestrial component accounted for roughly 60% of total measured dose rates, while east of the Continental Divide, where enriched granitic source rocks and associated soils are prevalent, the terrestrial component generally accounted for two-thirds or more of total dose rates.

URINARY EXCRETION OF RADIONUCLIDES FROM MARSHALLESE EXPOSED TO FALLOUT FROM THE 1954 BRAVO NUCLEAR TEST

Soon after the Bravo nuclear test at Bikini Atoll in the Marshall Islands on 1 March 1954, urine samples were collected for analysis of excreted radioactivity from native residents exposed to radioactive fallout on two atolls as well as from U.S. military personnel on a third atoll. The earliest acquired samples, obtained by the Los Alamos Scientific Laboratory (LASL), were assayed for various radionuclides and provided the first known measurements of 131I in urine following exposure to fallout from a nuclear test. Over the course of 1954, many additional samples were collected by the LASL, as well as by the Atomic Energy Commission New York Operations Offices Health and Safety Laboratory and the Naval Radiological Defense Laboratory. Collectively, the groups sampled included Marshallese exposed on Rongelap and Ailinginae Atolls, American military weather observers temporarily resident on Rongerik Atoll, and sailors from the Japanese fishing vessel, the Lucky Dragon. While the bioassay measurement data and individual urine volumes have been crucial to various attempts to assess intakes of radioactivity and the related internal radiation doses among the Marshallese, those data have never been published in any peer-reviewed journal, but have been restricted to agency memoranda, laboratory reports, and summaries in some publications and book chapters. Reconstructions of internal doses to Marshallese in 1954 and in later years have depended on these data and, hence, they have considerable historical importance as well as importance to ongoing health risk projections for Marshallese. This paper presents much of the original data on urine volumes and radioactivity from the various assays of urine for radionuclides, and compares estimates of 131I intakes made in 1954, 1985, 1987, and 2008.

Plutonium concentrations in lichens of Rocky Flats environs

Xanthoparmelia spp. lichens were used to study the spatial distribution of plutonium concentrations in nonvascular plants surrounding the Rocky Flats nuclear weapons facility with respect to distance, direction, age, and washing. Plutonium concentrations in lichens were inversely related to distance from the initial contamination site with a directional component which corroborated wind-borne transport as the primary means of dispersion. Ultrasonic washing and the relative age of the lichen proved to be significant only at p = 0.21 and p = 0.96, respectively. Isotopic ratios of 239,240Pu to 238Pu were highly variable at low activities but remained consistent at 62.6 for samples with high total plutonium activity. Correlation of Xanthoparmelia spp. lichen 239,240Pu concentrations to surface soil concentrations showed a direct relationship (r = 0.767; p < 0.001). The correlation was supported by soil retention studies which revealed a lichen soil content ranging from 11 to 18% on a dry mass basis with a possible particle size selectivity in the different concentration ratios adjacent to and away from the initial contamination site. Results suggest that further study into the in situ biomonitoring of surface soil by Xanthoparmelia spp. lichens is promising.