ROUTINE METHOD FOR THE DETERMINATION OF TRACE AMOUNTS OF 226Ra IN URINE BY ALPHA SPECTROMETRY.

226Ra is considered one of the most radiotoxic naturally occurring radionuclides. A new routine method was developed to measure traces of 226Ra in urine. Radium was pre-concentrated from a 2 l urine sample using manganese oxide (MnO2) particles. The MnO2 precipitate was dissolved and the organic matter was broken down. Then, potential radiological interferents were removed using DGA and AGMP1 stacked resin columns. A barium sulphate (BaSO4) micro-precipitation was performed before measuring the sample by alpha spectrometry. A good recovery of 60 ± 10% and excellent alpha resolution were obtained. The minimum detectable activity (MDA) was 0.2 ± 0.1 mBql-1. The method was validated using spiked samples and can be completed in 5 hours.

Determination of 226Ra at low levels in environmental, urine, and human bone samples and 223Ra in bone biopsy using alpha-spectrometry and metrological traceability to 229Th/225Ra or 226Ra.

226Ra is a natural radioelement emitting α and γ radiations. It can be highly concentrated in TENORM materials from the petroleum or fertilizer industries. In Switzerland, 226Ra is currently a radioactive inheritance problem from the watch industry. Furthermore, 223Ra is a radium isotope used in nuclear medicine to treat bone metastasis. There exist several methods to measure radium using alpha or gamma spectrometry or using 222Rn emanation technique. The limitations of these methods are due to the required detection limits and the nature of the samples. When using alpha spectrometry to reach very low detection limits, critical technical hitches often arise because of the difficulties in separating radium from barium, in removing organics eluted from the separating chromatography column, and in plating radium. Moreover, overall chemical recovery of radium is often not reproducible, depending on the studies. Here we propose a method that separates radium from other alkaline-earth cations using cation exchange chromatography and selective complex formation by EDTA and DCTA. Radium is completely free of the 229Th tracer and its daughter products, particularly 225Ac. Organics from the column are removed in a further purification step so that radium can be plated with acceptable yields in a HCl/HNO3/ethanol solution. We successfully applied the method to soil, water, urine and human bone samples and further extended it to the determination of 223Ra in a bone biopsy, using 226Ra as an internal tracer.

Emergency Radiobioassay Method for Determination of 9°Sr and ²²6Ra in a Spot Urine Sample.

A new radiobioassay method has been developed for simultaneous determination of (90)Sr and (226)Ra in a spot urine sample. The method is based on a matrix removal procedure to purify the target radionuclides from a urine sample followed by an automated high performance ion chromatographic (HPIC) separation of (90)Sr and (226)Ra and offline radiometric detection by liquid scintillation counting (LSC). A Sr-resin extraction chromatographic cartridge was used for matrix removal and purification of (90)Sr and (226)Ra from a urine sample prior to its introduction to the HPIC system. The HPIC separation was carried out through cation exchange chromatography using methanesulfonic acid (75 mM) as the mobile phase at 0.25 mL/min flow rate. The performance criteria of the method was evaluated against the American National Standard Institute ANSI/HPS N13.30-2011 standard for the root mean squared error (RMSE) of relative bias (Br) and relative precision (SB) at two different spiked activity levels. The RMSE of Br and SB for (90)Sr and (226)Ra were found to be satisfactory (≤0.25). The minimum detectable activity (MDA) of the method for (90)Sr and (226)Ra are 2 Bq/L and 0.2 Bq/L, respectively. The MDA values are at least 1/10th of the concentrations of (90)Sr (190 Bq/L) and (226)Ra (2 Bq/L) excreted in urine on the third day following an acute exposure (inhalation) that would lead to an effective dose of 0.1 Sv in the first year. The sample turnaround time is less than 8 h for simultaneous determination of (90)Sr and (226)Ra.

Determination of 226Ra in urine samples by alpha spectrometry.

A radiation protection system to assess the internal contamination of workers during decontamination activities in an abounded fertilizer industry in the region of Attika, Greece, has been implemented. This system concerns, among other radionuclides, 226Ra. Because of the low 226Ra activities in urine, alpha spectrometry was used as the determination method after radiochemical separation. Radium was co precipitated with lead sulphate and purified using anion and cation exchange techniques. The source for the alpha spectrometric measurement was prepared by the electrodeposition of radium, from an aqueous/ethanol solution, onto stainless steel. The tracer used was 229Th. The chemical yield and the activity concentration were calculated via its daughter radionuclide 217At. Using the time-evolution formulas to calculate the 217At growth from its parent radionuclide 225Ra, a computer software was developed. This software was incorporated in a database, which automatically calculates and stores the results.

Daily uranium excretion in German peacekeeping personnel serving on the Balkans compared to ICRP model prediction.

An investigation was performed to assess a possible health risk of depleted uranium (DU) for residents and German peacekeeping personnel serving on the Balkans. In order to evaluate a possible DU intake, the urinary uranium excretions of volunteers were collected and analysed using inductively coupled plasma mass spectrometry (ICP-MS). In total, more than 1300 urine samples from soldiers, civil servants and unexposed controls of different genders and ages were analysed to determine uranium excretion parameters. All participating volunteers, aged 3-92 y, were grouped according to their gender and age for evaluation. The results of the investigation revealed no significant difference between the unexposed controls and the peacekeeping personnel. In addition, the geometric means of the daily urinary excretion in peacekeeping personnel, ranging from 3 to 23 ng d(-1) for different age groups, fall toward the lower end of renal uranium excretion values published for unexposed populations in literature. The measured data were compared with the International Commission on Radiological Protection prediction for the intake of natural uranium by unexposed members of the public. The two data sets are in good agreement, indicating that no relevant intake of additional uranium, either natural or DU, has appeared for German peacekeeping personnel serving on the Balkans.

The metabolism of radium-226 during pregnancy in the rat.

Metabolism of radium including the transfer to the fetus through the placenta was studied during three successive pregnancies 92, 155, and 213 days after injection of 226Ra in young female rats. The cumulative fecal and urinary excretions of 226Ra in a 213-day period following injection were about 30 and 15% injected dose (%ID), respectively, most of them occurring during the first 42 days. The excretions were similar in both the pregnant and control (unmated) rats. The whole-body burden of radium (mostly in the skeleton) determined by actual analysis of the entire body was similar in the two groups and was about 53, 48, and 44 %ID at the first, second, and third pregnancy, respectively. Pregnancy alone, therefore, did not significantly affect metabolism of radium. At 20 days of gestation the mean placental content of radium was 0.005, 0.0045, and 0.0036 %ID in the first, second, and third litter, respectively; the corresponding mean fetal content was 0.01, 0.008, and 0.005 %ID. The radium burden of the full-term neonate (21-22 days) was 0.014 and 0.011 %ID for the first and second delivery, respectively. The total amount calculated of radium transferred from the mother to the 8-10 fetuses in a litter did not exceed about 0.3% of the maternal content per each pregnancy. Comparison of the ratio of radium and calcium in the fetus and maternal skeleton shows that there is a Ra-Ca discrimination during their passage from the mother to the fetus.

Radium retention and dosimetry in the St. Bernard.

The percentage total-body retention (R) of 226Ra was determined in 14 young adult St. Bernards for the first 4 years after injection to be represented by the equation, R = 34.8 e-0.165t + 24.6 e-0.00537t + 40.6 e-0.000503t, where t is the time after injection in days. It was found that the 222Rn/226Ra ratio in the skeleton was similar to that measured previously for young adult beagles given 226Ra. Excretion of injected 226Ra averaged about 32% in the first 2 weeks, with about 2/3 of the total appearing in the feces. St. Bernards appear to retain more 226Ra than do beagles injected at the same age. The last two terms of the retention equation were used to calculate the average skeletal radiation dose rate and cumulative radiation dose normalized to each dog's individual retention measurements. Allowance was made in the calculations for the changing skeletal retention of 222Rn and its radioactive daughters as a function of time.

The metabolism of radium in dairy cows.

1. The isotopes (45)Ca and (224)Ra were administered simultaneously, both orally and intravenously, to two pairs of cows. 2. The first pair of animals received large doses of (224)Ra and (45)Ca, which produced clinical and metabolic disturbances. 3. The second pair of animals received much smaller doses and showed no clinical disturbances. The mean recoveries in these animals of (45)Ca and (224)Ra in the 8 days after the oral administration were respectively: from faeces, 63.2 and 103.8%; from urine, 0.26 and 0.44%; from milk, 15.8 and 0.35% of the dose; and in the 8 days after intravenous administration: from faeces, 20.5 and 36.5%; from urine, 1.56 and 17.6%; from milk, 49.3 and 11.8% of the dose. 4. Calculation of discrimination factors shows that absorptive discrimination played the most important part in the overall discrimination between the calcium and radium in their passage from diet to milk, but that mammary discrimination plays a more important role than in the overall discrimination between calcium and strontium or barium. 5. In its treatment by the kidney radium is more like strontium than barium, but radium is actively secreted by the gut in the same way as barium. 6. In its skeletal metabolism radium is indistinguishable from calcium and strontium except in its rate of resorption, which is similar to that of barium.