Assessing the uranium DGT-available fraction in model solutions.

The uranium speciation in humic acid (HA) and fulvic acid (FA) model solutions was investigated by diffusive gradients in thin films (DGT). A reference solution was used to normalize the DGT data from different samples. This approach was used to assess uranium DGT-available fraction (FU), which was calculated from experimental data and reflect both the mobility and lability of uranium species. FU decreased with increasing HA or FA concentrations, because more uranium was able to bind the strong binding sites of HA or FA. When copper was spiked, FU increased due to the competition between copper and uranium. In HA model solutions, an increase of ionic strength could increase FU, and when pH was greater than 7, FU increased significantly. The DGT uptake factor (φ), which can be obtained from data fitting, is the ratio of the product of diffusion coefficient and lability degree of the unknown sample to that of the reference solution. In U-HA-NaHCO3 solutions, UO2(CO3)22- had a relatively high φ value and might be the most DGT-available species. This approach allows the comparison of DGT data from different samples, and combining with a data fitting procedure, it can be used to investigate the distribution of metal species.

Measuring (210) Pb by accelerator mass spectrometry: a study of isobaric interferences of (204,205,208) Pb and (210) Pb.

RATIONALE: The measurement of (210) Pb provides an assessment of the risk an individual faces of developing lung cancer as a result of their exposure to radon and radon decay products. Existing radiometric techniques are not sensitive enough to detect (210) Pb in many exposures. This report describes the further development of a method of measuring (210) Pb using Accelerator Mass Spectrometry (AMS). METHODS: (204,205,208,) (210) Pb measurements were performed by AMS. Samples were prepared from stock solutions of (204) Pb, (205) Pb, (208) Pb and (210) Pb and measured by making PbF3 (-) ions at the IsoTrace AMS facility using a SIMS-type Cs(+) sputter source. Potential interferences in Pb(3) (+) isotope measurement and the overall efficiency of Pb beam production were determined experimentally. RESULTS: (204) Pb and (205) Pb suffer from molecular and atomic isobaric interferences that cannot be removed without sacrificing the efficiency of (210) Pb measurements whereas (208) Pb suffers from no interferences. The abundance sensitivity of (210) Pb/(208) Pb was 1.3 × 10(-12) . Keeping the (210) Pb/(208) Pb spike below this level resulted in a detection limit of 4.4 mBq of (210) Pb using the IsoTrace AMS facility. CONCLUSIONS: This study identified key interferences in the measurement of PbF3 (-) → Pb(3) (+) ions and demonstrated a new AMS method to measure (210) Pb. This new AMS technique is about five times more sensitive than gamma and beta spectroscopy measurements of (210) Pb and the measurement time is much shorter. Copyright © 2016 John Wiley & Sons, Ltd.

Detection of (135) Cs by accelerator mass spectrometry.

RATIONALE: The ability to measure both (135) Cs and (137) Cs can provide an estimate of the age and source of Cs isotopes in an environmental sample. Accelerator mass spectrometry (AMS) consistently reports lower abundance sensitivities than other techniques and, with the addition of an on-line reaction cell, simpler isobaric suppression. Therefore, an AMS methodology was developed to measure Cs isotopes using CsF2- as the initial anion. METHODS: The ion beam is passed through the Isobar Separator for Anions (ISA) where it is captured by radiofrequency quadrupoles in a gas cell before injection into the tandem accelerator. In the ISA, the beam reacts with O2 gas, selectively removing the BaF2- and leaving the Cs analyte to be reaccelerated and sent through the remainder of the AMS system. RESULTS: The BaF2- signal was attenuated by a factor of 10(5) in the ISA while 25% of the original CsF2- current was transmitted into the accelerator. (135) Cs was measured without any interference from (133) Cs to an abundance sensitivity of 1.3 × 10(-10) . The abundances of four stable Ba isotopes (masses 133, 134, 135 and 137) were measured and no isotope-dependent bias was detected using the ISA in vacuum. CONCLUSIONS: The results demonstrate the feasibility of measuring long-lived Cs isotopes without Ba interference by AMS with on-line isobar separation and the ability to use shorter lived Cs isotopes for yield tracing.

Preliminary assessment of thoron exposure in Canada.

Radon has been identified as the second leading cause of lung cancer after tobacco smoking. (222)Rn (radon gas) and (220)Rn (thoron gas) are the most common isotopes of radon. In this study, thoron exposure in Canada was assessed based on three community radon/thoron surveys conducted recently. It was confirmed that thoron was detectable in most homes and thoron progeny were present in every home surveyed. Results demonstrated that thoron concentrations varied more widely than radon. No clear correlation between (222)Rn and (220)Rn concentrations was observed in simultaneous measurements. It is estimated that thoron contributes to about 7 % of the radiation dose due to indoor radon exposure based on measurements in about 260 individual homes. Because indoor measurements and geological gamma-ray surveys did not support a reasonable association between (222)Rn and (220)Rn, thoron concentrations could not be predicted from widely available indoor radon information. In order to better assess thoron exposure in Canada and thoron risk to the Canadian population in various geographic locations, more thoron progeny measurements are required.

Preliminary evaluation of (135)Cs/(137)Cs as a forensic tool for identifying source of radioactive contamination.

Ratios of the fission products (135)Cs and (137)Cs were determined in soil and sediment samples contaminated from three different sources, to assess the use of (135)Cs/(137)Cs as an indicator of source of radioactive contamination. Soil samples from the Chernobyl exclusion zone were found to have to be heavily depleted in (135)Cs ((135)Cs/(137)Cs approximately 0.45), indicative of a high thermal neutron flux at the source. Sludge samples from a nuclear waste treatment pond were found to have a (135)Cs/(137)Cs ratio of approximately 1, whereas sediment collected downstream from a nuclear reactor was highly variable in both (137)Cs activity and (135)Cs/(137)Cs ratio. Comparison of these preliminary results of variability in radiocaesium isotope ratios with reports of Pu isotope ratios suggests (135)Cs/(137)Cs similarly varies with fuel and reactor conditions, and may be used to corroborate other methods of characterizing radioactive contamination.

Determination of 90Sr in contaminated environmental samples by tuneable bandpass dynamic reaction cell ICP-MS.

A rapid method for the extraction and determination of 90Sr in natural water, plant and sediment samples was developed using extraction chromatography and dynamic reaction cell ICP-MS, with O2 as a reaction gas. While isobaric interference from the stable isotope 90Zr was efficiently removed by this method, interferences produced from in-cell reactions with Fe+ and Ni+ required suppression by tuneable bandpass, and in sediments, additional chromatographic separation. Method detection limits were 0.1 pg g-1 (0.5 Bq g-1), 0.04 pg g-1(0.2 Bq g-1), and 3 pg L-1 (5 Bq L-1) for sediments, plant and water samples, respectively, and 90Sr concentrations determined by ICP-MS were in good agreement with activities determined by Cerenkov counting and with certified reference values. While mass spectrometric determination does not rival detection limits achievable by radiometric counting, radiometric determination of 90Sr, a pure beta-emitter, is hindered by long analysis times (several weeks); the comparatively fast analysis achieved via ICP-MS enables same-day preparation and analysis of samples, making this an important technique for the environmental monitoring of areas contaminated by radioactivity.

Tritium concentrations inside the homes of occupationally exposed workers: dosimetric implications.

The average tritiated water concentration in the indoor air of the occupationally exposed worker's residence (55 Bq m(-3), range 53-59 Bq m(-3)) was higher than the indoor air of control residences (0.7 Bq m(-3), range 0.4-0.8 Bq m(-3)). The worker had an average concentration of tritium-in-urine of 30 kBq L(-1) from chronic intakes of occupational levels of tritiated water. Higher residential concentrations of tritiated water vapor were due to tritium transferred by the worker. Urine samples from an adult co-occupant were collected and had tritiated water concentrations between 89 and 345 Bq L(-1). These concentrations were higher than for individuals (range, 6-32 Bq L(-1)) living in other residences having similar outdoor and indoor concentrations of tritiated water in air. The range of measured tritiated water in urine was in agreement with the prediction of biokinetic models for tritium intakes as recommended by the International Commission on Radiological Protection Publication 56. The tritiated water vapor in the indoor air of the exposed worker's residence contributed about 96% of the daily tritium intakes. The annual average tritium dose to the family member (7 microSv) was well below the International Commission on Radiological Protection Publication 60 recommended annual dose limit (1 mSv) for members of the public. We conclude that, for a few members of the public living near a heavy-water research reactor facility, daily intakes of tritium will relate to tritiated water dispersed by the exposed worker, as well as to tritium transported by the atmosphere from the reactor site.

129I and 36Cl concentrations in lichens collected in 1990 from three regions around Chernobyl.

129I and 36Cl were measured by accelerator mass spectrometry in 11 lichen samples (Parmelia sulcata) collected in 1990 from three regions (Novozybkov, Bragin and Ovruc) near Chernobyl. Previously measured activities of 137Cs were highest in the samples from the Novozybkov region while the measured activities of 36Cl and 129I in this study were highest in the samples from the Bragin region. The regional distribution patterns of the 36Cl and 129I show a positive correlation suggesting that these volatile radionuclides were deposited in the same manner.

The biological half-time of radioactive Cs in poikilothermic and homeothermic animals.

Literature data for the half-time of Cs in one-, two-, and three-compartment models have been collated and regressed to yield general descriptions of clearance for homeotherms (warm-blooded animals) and poikilotherms (cold-blooded animals) of different sizes. Cesium half-times increase with body weight and are longer in poikilotherms than in homeotherms. These trends and the values of the associated regression coefficients imply that Cs clearance is a function of metabolic rate. The patterns are especially visible in analyses of the larger compartments, perhaps because the curve splitting required to analyze smaller, more rapidly cleared pools is necessarily subjective. The route by which acutely contaminated animals receive their Cs also influences clearance. Inhaled Cs appears to be retained longer than injected Cs, which is in turn retained longer than ingested Cs. This suggests that Cs is discriminated against in biological transfers, so that Cs dust remains in the lungs whereas Cs in the food is less readily absorbed. These patterns of Cs clearance suggest that large animals, poikilotherms, and animals contaminated by inhalation or injection may receive a greater dose.

Hypolinimetic oxygen deficits: their prediction and interpretation.

Rates of hypolimnetic oxygen depletion can be predictedfrom a knowledge of a lake's phosphorus retention, the average hypolimnetic temperature, and the mean thickness of the hypolimnion. Areal oxygen deficits cannot be used to index lake trophic status because areal calculations do not eliminate the influence of hypo-limnetic morphometry.