Determination of Atto- to Femtogram Levels of Americium and Curium Isotopes in Large-Volume Urine Samples by Compact Accelerator Mass Spectrometry.

Ultralow level analysis of actinides in urine samples may be required for dose assessment in the event of internal exposures to these radionuclides at nuclear facilities and nuclear power plants. A new bioassay method for analysis of sub-femtogram levels of Am and Cm in large-volume urine samples was developed. Americium and curium were co-precipitated with hydrous titanium oxide from the urine matrix and purified by column chromatography separation. After target preparation using mixed titanium/iron oxides, the final sample was measured by compact accelerator mass spectrometry. Urine samples spiked with known quantities of Am and Cm isotopes in the range of attogram to femtogram levels were measured for method evaluation. The results are in good agreement with the expected values, demonstrating the feasibility of compact accelerator mass spectrometry (AMS) for the determination of minor actinides at the levels of attogram/liter in urine samples to meet stringent sensitivity requirements for internal dosimetry assessment.

Five-column chromatography separation for simultaneous determination of hard-to-detect radionuclides in water and swipe samples.

There is a growing demand for the rapid determination of hard-to-detect radionuclides in environmental and biological samples for environmental monitoring, radiological protection, and nuclear forensic reasons. A new method using five-column chromatography separation has been developed for the simultaneous determination of Pu, Np, Th, U, Am, Cm, Pm, Y, and Sr isotopes, as well as iron-55, by inductively coupled mass spectrometry (ICPMS), α spectrometry, Cerenkov and liquid scintillation (LS) counting. Spiked swipe and water samples as well as proficient testing water standards were analyzed to validate the separation procedure, and the results are in good agreement with the expected values. The method provides quick sample turnaround time and high analysis throughput with low analysis cost. The flexibility of the method also allows for its easy adaptation to various emergency and routine radioassays.

Optimisation of nasal swab analysis by liquid scintillation counting.

When responding to an emergency radiological incident, rapid methods are needed to provide the physicians and radiation protection personnel with an early estimation of possible internal dose resulting from the inhalation of radionuclides. This information is needed so that appropriate medical treatment and radiological protection control procedures can be implemented. Nasal swab analysis, which employs swabs swiped inside a nostril followed by liquid scintillation counting of alpha and beta activity on the swab, could provide valuable information to quickly identify contamination of the affected population. In this study, various parameters (such as alpha/beta discrimination, swab materials, counting time and volume of scintillation cocktail etc) were evaluated in order to optimise the effectiveness of the nasal swab analysis method. An improved nasal swab procedure was developed by replacing cotton swabs with polyurethane-tipped swabs. Liquid scintillation counting was performed using a Hidex 300SL counter with alpha/beta pulse shape discrimination capability. Results show that the new method is more reliable than existing methods using cotton swabs and effectively meets the analysis requirements for screening personnel in an emergency situation. This swab analysis procedure is also applicable to wipe tests of surface contamination to minimise the source self-absorption effect on liquid scintillation counting.

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.

An improved method for the rapid determination of 90Sr in cow's milk.

An improved method was developed to rapidly determine strontium-90 (90Sr) in cow's milk samples in the event of a nuclear emergency. To perform this method, no heating or ashing steps were needed and all of the material used was disposable. Stable Sr tracer was added to each 40 mL milk sample. Hydrochloric acid (HCl) and trichloroacetic acid (TCA) were added to the sample to flocculate the suspended fat and proteins in the milk. The sample was centrifuged and the strontium in the supernatant was precipitated with carbonate. The resulting precipitate was dissolved in 8 M HNO3 and the solution was passed through a Sr resin to remove potential interferents. Strontium was eluted from the resin using a small volume of water. Strontium-90 was measured by liquid-scintillation counting (LSC) and the tracer by inductively coupled plasma mass spectrometry (ICP-MS). The figures of merit of the method were determined and the method was validated using spiked samples.

Determination of 99Tc in fresh water using TRU resin by ICP-MS.

Technetium-99 (99Tc) determination at trace level by inductively coupled plasma mass spectrometry (ICP-MS) is challenging because there is no readily available appropriate Tc isotopic tracer. A new method using Re as a recovery tracer to determine 99Tc in fresh water samples, which does not require any evaporation step, was developed. Tc(VII) and Re(VII) were pre-concentrated on a small anion exchange resin (AER) cartridge from one litre of water sample. They were then efficiently eluted from the AER using a potassium permanganate (KMnO4) solution. After the reduction of KMnO4 in 2 M sulfuric acid solution, the sample was passed through a small TRU resin cartridge. Tc(VII) and Re(VII) retained on the TRU resin were eluted using near boiling water, which can be directly used for the ICP-MS measurement. The results for method optimisation, validation and application were reported.

EURADOS intercomparison on emergency radiobioassay.

Nine laboratories participated in an intercomparison exercise organised by the European Radiation Dosimetry Group (EURADOS) for emergency radiobioassay involving four high-risk radionuclides ((239)Pu, (241)Am, (90)Sr and (226)Ra). Diverse methods of analysis were used by the participating laboratories for the in vitro determination of each of the four radionuclides in urine samples. Almost all the methods used are sensitive enough to meet the requirements for emergency radiobioassay derived for this project in reference to the Clinical Decision Guide introduced by the NCRP. Results from most of the methods meet the requirements of ISO 28218 on accuracy in terms of relative bias and relative precision. However, some technical gaps have been identified. For example, some laboratories do not have the ability to assay samples containing (226)Ra, and sample turnaround time would be expected to be much shorter than that reported by many laboratories, as timely results for internal contamination and early decisions on medical intervention are highly desired. Participating laboratories are expected to learn from each other on the methods used to improve the interoperability among these laboratories.

Rapid determination of 226Ra in urine samples.

A new radiochemical separation method has been developed for rapid analysis of (226)Ra in urine samples. In this method, radium is separated from urine matrix using cation and anion exchange column chromatography. A (224)Ra tracer is added, together with its parent in the (228)Th standard, for chemical recovery correction. After separation, the sample is precipitated with hydrous titanium oxide and then prepared for counting by creating a thin-layer counting source using BaSO(4) micro-precipitation. The radium isotopes are then counted by alpha spectrometry. Replicate spike and blank samples were analysed for validation of the procedure. The detection limit was determined to be 0.22 Bq l(-1) with 4 h of counting for 20 ml of urine sample. Using this method, the results can be reported within an 8 h turn-around time. This method is suitable for quick dose assessment of (226)Ra exposure following a radiation emergency.

An emergency bioassay method for actinides in urine.

A rapid bioassay method has been developed for the sequential measurements of actinides in human urine samples. The method involves actinide separation from a urine matrix by co-precipitation with hydrous titanium oxide (HTiO), followed by anion exchange and extraction chromatography column purification, and final counting by alpha spectrometry after cerium fluoride micro-precipitation. The minimal detectable activities for the method were determined to be 20 mBq L(-1) or less for plutonium, uranium, americium and curium isotopes, with an 8-h sample turn-around time. Spike tests showed that this method would meet the requirements for actinide bioassay following a radiation emergency.