Rapid method for determination of plutonium, americium and curium in large soil samples

The analysis of actinides in environmental soil and sediment samples is very important for environmental monitoring. There is a need to measure actinide isotopes with very low detection limits. A new, rapid actinide separation method has been developed and implemented that allows the measurement of plutonium, americium and curium isotopes in large soil samples (100–200 g) with high chemical recoveries and effective removal of matrix interferences. This method uses stacked TEVA Resin®, TRU Resin® and DGA-Resin® cartridges from Eichrom Technologies (Darien, IL, USA) that allows the rapid separation of plutonium (Pu), americium (Am), and curium (Cm) using a single multi-stage column combined with alpha-spectrometry. The method combines an acid leach step and innovative matrix removal using cerium fluoride precipitation to remove the difficult soil matrix. This method is unique in that it provides high tracer recoveries and effective removal of interferences with small extraction chromatography columns instead of large ion-exchange resin columns that generate large amounts of acid waste. By using vacuum box cartridge technology with rapid flow rates, sample preparation time is minimized.     

Fast method for the determination of radiostrontium and plutonium isotopes in food samples

Rapid radioanalytical methods are important in the case of a radiological emergency and for the defence against nuclear hazards, especially for pure alpha and beta emitters like ^239/240Pu and ⁸⁹Sr/⁹⁰Sr. A new fast method was developed with an overall analysis time altogether around 11 h, for only strontium isotopes about 7 h. The method combines two extraction chromatography resins, DGA- and Sr-resin, to separate mainly strontium and plutonium. A broad variety of food samples with different fat, carbohydrate and protein contents were tested and successfully analysed. The yields obtained were typically around 95% and 70% for ⁹⁰Sr and ²⁴²Pu.

     

Rapid fusion method for determination of actinides in fecal samples

A new rapid fusion method for the determination of actinides in fecal samples has been developed at the Savannah River National Laboratory that can be used for emergency response or routine bioassay analyses. If a radiological dispersive device, improvised nuclear device or nuclear accident occur, there will be an urgent need for rapid analyses of environmental, food and bioassay matrices. If an inhalation event occurs and there is confirmed radionuclide activity present via urine analyses of individuals, fecal analyses will typically be required to determine the soluble/insoluble fraction of actinides present as a result of the event to allow a more reliable estimate of radiological dose. The new method for actinides in fecal samples uses accelerated furnace heating, a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step, and a column separation process with stacked TEVA, TRU and DGA resin cartridges. The rapid fusion method provides rugged digestion of any refractory particles present, essential for reliable analysis of actinides in fecal samples. Alpha spectrometry was used to determine the actinide isotopes, but this method can be adapted for assay by inductively-coupled plasma mass spectrometry for actinide isotopes with longer half-lives that have sufficient mass to allow measurement. The method showed high chemical recoveries and effective removal of interferences. The determination of actinides in fecal samples can be performed in less than 12 h in an emergency with excellent quality for emergency samples. The new method, which is much less tedious and time-consuming than other reported methods, can be used for emergency or routine fecal sample analyses. This enables more timely estimates of radiological dose to be performed that utilize soluble/insoluble actinide ratios.     

A combined method for the determination of the isotopic vector of plutonium isotopes in environmental samples

A combination of alpha-spectrometry, liquid scintillation counting (LSC) and accelerator mass spectrometry (AMS) was used for the determination of plutonium isotopes. ²³⁸Pu and ^239+240Pu were measured by alpha-spectrometry after separation of Pu by anion-exchange using ²³⁶Pu tracer as recovery monitor. After alpha-measurement, one part of the sample was dissolved for determining ²⁴¹Pu by LSC. Another part was used for the measurement of the ²⁴⁰Pu/²³⁹Pu atom ratio by AMS at VERA. Thus, it was possible to obtain complete information on the Pu isotopic composition of the samples. This method was applied to environmental reference samples and samples contaminated from nuclear reprocessing.     

Rapid determination of radiostrontium in large soil samples

A new method for the determination of radiostrontium in large soil samples has been developed at the Savannah River Environmental Laboratory (Aiken, SC, USA) that allows rapid preconcentration and separation of strontium in large soil samples for the measurement of strontium isotopes by gas flow proportional counting. The need for rapid analyses in the event of a radiological dispersive device or improvised nuclear device event is well-known. In addition, the recent accident at Fukushima Nuclear Power Plant in March, 2011 reinforces the need to have rapid analyses for radionuclides in environmental samples in the event of a nuclear accident. The method employs a novel pre-concentration step that utilizes an iron hydroxide precipitation (enhanced with calcium phosphate) followed by a final calcium fluoride precipitation to remove silicates and other matrix components. The pre-concentration steps, in combination with a rapid Sr Resin separation using vacuum box technology, allow very large soil samples to be analyzed for ^89,90Sr using gas flow proportional counting with a lower method detection limit. The calcium fluoride precipitation eliminates column flow problems typically associated with large amounts of silicates in large soil samples.     

A fast method for the determination of plutonium in soil and sediment samples

A so-called hour method for the determination of plutonium based on extraction chromatography is validated by its application to several certified soil and sediment samples from the International Atomic Energy Agency's Seibersdorf Laboratory. The results are in good agreement with the reference values. Chemical yields range between 47%–66%, with a mean value of (56±6)%. The possible use of this method for²⁴¹Pu determination is also demonstrated.     

Rapid method for plutonium-241 determination in soil samples

A simple and rapid procedure for the determination of plutonium isotopes in the environment is presented. The procedure combines alpha spectrometry, solvent extraction and liquid scintillation measurements to ensure that both alpha- and beta-emitting isotopes are determined. Of five tested extractants, bis-(2-ethylhexyl) phosphoric acid was found to be the best choice. The procedure was applied to soil samples contaminated with Chernobyl fallout.     

Rapid method for the analysis of plutonium isotopes in a soil sample within 60 min.

A rapid method for the determination of Pu isotopes in a soil sample within 60 min of starting sample pretreatment was developed. The large reduction in the analysis time was attained by the rapid and perfect digestion of the sample using an alkaline fusion method with an induction heating machine. Pu concentrations were then determined by flow injection/ICP-MS using a solid extraction resin after preconcentration by batch extraction with a chelate resin. The limits of detection for 239Pu and 240Pu were 9.2 fg and 4.3 fg, corresponding to 0.03 and 0.05 Bq kg(-1), respectively, under our analytical conditions, which satisfy the lower detection limits (0.5 Bq kg(-1) of 239Pu, and 2 Bq kg(-1) of 240Pu) required for rapid analysis techniques by the Ministry of Education, Culture, Sports, Science and Technology, Japan. This method provides a powerful and practical technique for emergency monitoring in and around nuclear facilities that handle large amounts of plutonium.     

Rapid method for determination of 228Ra in water samples

A new rapid method for the determination of ²²⁸Ra in natural water samples has been developed at the SRNL/EBL (Savannah River National Lab/Environmental Bioassay Laboratory) that can be used for emergency response or routine samples. While gamma spectrometry can be employed with sufficient detection limits to determine ²²⁸Ra in solid samples (via ²²⁸Ac), radiochemical methods that employ gas flow proportional counting techniques typically provide lower minimal detectable activity levels for the determination of ²²⁸Ra in water samples. Most radiochemical methods for ²²⁸Ra collect and purify ²²⁸Ra and allow for ²²⁸Ac daughter ingrowth for ~36 h. In this new SRNL/EBL approach, ²²⁸Ac is collected and purified from the water sample without waiting to eliminate this delay. The sample preparation requires only about 4 h so that ²²⁸Ra assay results on water samples can be achieved in <6 h. The method uses a rapid calcium carbonate precipitation enhanced with a small amount of phosphate added to enhance chemical yields (typically >90 %), followed by rapid cation exchange removal of calcium. Lead, bismuth, uranium, thorium and protactinium isotopes are also removed by the cation exchange separation. ²²⁸Ac is eluted from the cation resin directly onto a DGA Resin cartridge attached to the bottom of the cation column to purify ²²⁸Ac. DGA Resin also removes lead and bismuth isotopes, along with Sr isotopes and ⁹⁰Y. La is used to determine ²²⁸Ac chemical yield via ICP-MS, but ¹³³Ba can also be used instead if ICP-MS assay is not available. Unlike some older methods, no lead or strontium holdback carriers or continual readjustment of sample pH is required.     

Rapid method for determination of radiostrontium in emergency milk samples

A new rapid separation method for radiostrontium in emergency milk samples was developed at the Savannah River Site (SRS) Environmental Bioassay Laboratory (Aiken, SC, USA) that will allow rapid separation and measurement of radiostrontium within 8 hours. The new method uses calcium phosphate precipitation, nitric acid dissolution of the precipitate to coagulate residual fat/proteins and a rapid strontium separation using Sr Resin (Eichrom Technologies, Darien, IL, USA) with vacuum-assisted flow rates. The method is much faster than the previous method that use calcination or cation-exchange pretreatment, has excellent chemical recovery, and effectively removes beta-interferences. When a 100 mL sample aliquot is used with a 20 minute count time, the method has a detection limit of 0.5 Bq·L⁻¹, well below generic emergency action levels.     

Radiochemical procedure for the determination of plutonium isotopes in powdered milk

Summary A radiochemical procedure for the determination of alpha-emitting isotopes of plutonium in powdered milk is proposed. The procedure involves sample dissolution (by HNO₃ and HClO₄), separation by ionic-exchange resin, electrodeposition and alpha-spectroscopy. In order to determine the chemical recovery, ²⁴²Pu was employed as a tracer. A reference material (Marine Sediment IAEA 135) was analyzed to validate such procedure, and to show its reliability. Afterwards, some powdered milk, produced for international trade, was analyzed and chemical recovery was found to be around 95%.     

Determination of thorium,uranium and plutonium isotopes in atmospheric samples

A new procedure for the radiochemical measurements of thorium, uranium and plutonium in atmospheric samples is described. Analysis involves coprecipitation of these actinides with iron hydroxide from a 40-to 50-dm³ sample of rainwater, followed by radiochemical separation and purification procedures by the use of ion exchange chromatography (Dowex AG1×8) and solvent extraction. The new procedure enables one to determine the isotopes of thorium, uranium and plutonium, which are found in rainwater at extremely low concentrations, with a chemical yield ranging from 60 to 80%.     

Rapid dissolution of large environmental samples for the determination of fission products

The dissolution of large environmental samples was investigated using a microwave autoclave, capable of digestion conditions of 300 °C and 200 bar, for the application of rapid determination of radionuclides. Six samples of up to 5 g plant material were digested, also eliminating predigestion steps such as ashing and grinding. Batches of forty 1 g samples of plant leaves were also completely digested in 75 minutes. Quantitative recovery of ⁹⁰Sr from 5 g soil samples by leaching with 8M HNO₃ at 200 °C was achieved, whereas ¹³⁷Cs was not completely recovered from the large soil samples using total digestion or leaching (HCl:HNO₃) techniques, but quantitative recovery was achieved using fusion and sinter procedures.     

An improved method for the determination of uranium isotopes in environmental samples by alpha-spectrometry

In order to improve the selectivity of the uranium isotopes determination in environmental samples, further studies have been carried out, including (1) interference of ²¹⁰Po with uranium isotope determination, (2) distribution coefficients of polonium between 5% TOPO in toluene and aqueous hydrochloric and nitric acids, (3) decontamination factor of uranium from polonium of the recommended procedure, and (4) leaching effect comparison of two different leaching procedures in a lichen sample. Based on the new findings, a more accurate extraction chromatographic/ a-spectroscopy method has been developed. For the method's validation, four kinds of reference materials supplied by the IAEA have been tested. It is observed that nearly all the ²³⁸U, ²³⁴U and ²³⁵U concentrations obtained are in good agreement with the recommended or information values, showing that the method can give reliable results. A comparison with existing uranium determination methods has also been made. It is concluded that due to involving preconcentration and chemical separation, the extraction chromatographic/a-spectroscopy method is a more selective, very sensitive and accurate, and low cost method. This revised version was published online in July 2006 with corrections to the Cover Date.     

Rapid determination of Pu isotopes for decommission concrete samples by inductively coupled plasma mass spectrometry

Journal of Radioanalytical and Nuclear Chemistry - Plutonium is one of the key radionuclides in nuclear decommission. In this study, a rapid method was developed to analyze Pu for concrete samples...     

Rapid dissolution of plutonium in soil by fusion with ammonium hydrogen sulfate followed by plutonium determination by ion exchange and alpha spectrometry

A method was developed for the rapid dissolution of plutonium in soil by fusion with ammonium hydrogen sulfate, and the determination of plutonium content by ion exchange separation and alpha spectrometry. By this method, plutonium in environmental soil containing plutonium oxide in a soluble and/or insoluble form could successfully be determined.     

An anion exchange method for the determination of241Am and plutonium in environmental and biological samples

Irradiation and post-irradiation losses in 7 crude oils encapsulated in polyethylene and irradiated in a flux of 10¹²n·cm⁻² sec⁻¹ have been thoroughly studied. The fraction of mercury released during irradiations ranging from 10 minutes to 2 hours is proportional to the integrated flux received by the samples and does not differ substantially from one oil to another. Post-irradiation loss rates at 20°C range between 0.017 and 0.027%·hr⁻¹. Storage at−20°C reduces them by at least a factor of 2. The influence on the activity of¹⁹⁷Hg due to losses in sample weight occuring during the post-irradiation period has been examined. The fraction of radiomercury retained inside the walls of the irradiation vials versus the irradiation time has been assessed. Contamination of an inner irradiation site following prolonged irradiations of oils containing 150 μg/g of this element has been evaluated and found to have a negligible impact for trace measurements above the ng/g level.