Estimation of <Superscript>90</Superscript>Sr activity in reprocessed uranium from the PUREX process

⁹⁰Sr estimation in reprocessed uranium was carried out by a series of solvent extraction and carrier precipitation techniques using strontium and lanthanum carriers. Fuming with HClO₄ was used to remove ¹⁰⁶Ru as RuO₄. Three step solvent extraction with 50% tri-n-butyl phosphate in xylene in presence of small amounts of dibutyl phosphate and thenoyl trifluoro acetone was carried out to eliminate uranium, plutonium, thorium and protactinium impurities. Lanthanum oxalate precipitation in acid medium was employed to scavenge the remaining multivalent ions. Strontium was precipitated as strontium oxalate in alkaline pH and ¹³⁷ Cs was removed by washing the precipitate with water. A strontium recovery well above 70% was obtained. Final estimation was carried out by radiometry using end window GM counter after drying the precipitate under an infra red lamp. The same procedure was extended to the estimation of ⁹⁰Sr in a diluted sample of the actual spent fuel solution. An additional lanthanum oxalate precipitation step was required to remove the entire ¹⁴⁴Ce impurity from this sample. This modified procedure was employed in the determination of ⁹⁰Sr in a number of reprocessed uranium samples and the over all precision of the method was found to be well within ±10%. An additional barium chromate precipitation step was necessary for the analysis of reprocessed uranium samples from high bumup fuels to eliminate trace amounts of short lived ²²⁴Ra produced during the decay of ²³²U and its daughters as they interfere in the estimation of ⁹⁰Sr.     

Separation and purification of 90Sr from PUREX HLLW using N,N,N′,N′-tetra(2-ethylhexyl) diglycolamide

This paper describes a method for the separation and purification of ⁹⁰Sr from PUREX–HLLW employing solvent extraction and precipitation techniques. 30 % TBP in n-dodecane was used for the removal of residual uranium, plutonium and neptunium from HLLW. Trivalent actinides and lanthanides were subsequently removed using N,N,N’,N’-tetra(2-ethylhexyl) diglycolamide (TEHDGA, 0.20 M in 30 % isodecyl alcohol and n-dodecane). ⁹⁰Sr was selectively extracted from actinides and lanthanides depleted HLLW using 0.3 M TEHDGA in 5 % isodecyl alcohol and dodecane. Loaded strontium was stripped using 0.01 M HNO₃ and further purified by radiochemical precipitation technique after adding Fe and natural strontium as carriers. Based on the experimental results, a flow-sheet was formulated and mCi levels of ⁹⁰Sr recovered.     

Strontium isolation from natural samples with Sr resin and subsequent determination of 90Sr</p> </p>

The reliability of an ⁹⁰Sr determination method was tested using an Sr extraction chromatographic resin for strontium isolation. The ⁹⁰Sr-content in samples of vegetables, soil and water (obtained from Environmental Measurement Laboratory, USA) were determined and the results were controlled by classical methods and by using an anion-exchanger and an alcohol solution of nitric acid for the strontium isolation. These methods were previously tested by determining ⁹⁰Sr in IAEA 326 and 327 samples of soil. It is shown that the isolation process with Sr resin is simpler and faster than the classical and mixed solvent anion-exchange methods. The efficiency of isolation on a Sr column depends on the resin quantity and separation conditions; and is the highest with a Sr column, compared to the classical and anion-exchange methods. Experimental data and theoretical models were used to calculate the parameters that enable the estimation of optimum dimensions of the column for isolation. A simple relation is proposed for the calculation of breakthrough volume, which defines the sample and eluent volumes for an optimal strontium isolation.</p> </p>     

The solvent extraction of carrier-free90Y from90Sr with crown ethers

A simple solvent extraction method has been developed for the separation of⁹⁰Y from⁹⁰Sr. Crown ether dissolved in chloroform was used as a selective reagent and organic picrate anion was chosen as a counter ion. The effect of various factors on the extraction separation of strontium and yttrium in the system have been studied. The extraction equilibrium constant of strontium logK _ex=9.15 was obtained from the study of the distribution coefficient versus the crown ether concentration. The separation method was simple, resulted high purity (>99.9%) and quantitative yield, and took less than half an hour.     

An improved method FO the determination of90Sr in large samples of seawater

The determination of⁹⁰Sr in large sample of seawater by its daughter product⁹⁰Y by means of solvent extraction with bis-2-ethylhexyl-phosphoric acid (HDEHP) ini n-heptane leads to²³⁴Th contamination. Two methods are described by which the²³⁸U daughter product²³⁴Th is separated from the Y³⁺ samples, either by a cation exchanger procedure or by a co-recipitation with Zr₃(PO₄)₄.     

Separation of radioactive strontium from natural samples by means of mixed-solvent anion exchange

A new procedure for isolation and determination of⁹⁰Sr in real natural samples is presented. It consists of bringing natural samples in a soluble form suitable for separation on an ion-exchange column, separation of calcium from strontium by means of the anion exchanger Amberlite CG-400 and 0.25M HNO₃ in methanol as eluent for calcium, and the determination of⁹⁰Sr using a low level -counter after elution with H₂O, scavenging steps and SrCO₃ precipitation. The method was tested with IAEA standards of natural samples with known contents of⁹⁰Sr, and water samples, where the concentration of⁹⁰Sr was previously determined by the standard IAEA procedure. The results obtained show that it is possible to isolate and determine low levels of⁹⁰Sr in natural samples. The procedure is favorable because of the simple separation of radioaactive strontium without using fuming nitric acid.     

New method for90Sr determination in liquid samples

A method has been developed for measuring⁹⁰Sr activity in liquid samples. After concentrating strontium from the sample by coprecipitation with calcium phosphate, the residue is dissolved in 8N HNO₃ and passed through an extraction chromatographic column (Sr.Spec) containing a new material that selectively retains strontium. This is eluted from the column with 0.05N HNO₃ and counted by liquid scintillation. Measurement is performed using a double window method, that allows a rapid and single determination of⁹⁰Sr.     

Separation of microamounts of yttrium from strontium by using nitrobenzene solution of sodium dicarbollylcobaltate in the presence of 18-crown-6

A rapid extraction separation of trace amounts of yttrium from strontium with a nitrobenzene solution of sodium dicarbollylcobaltate (NaDCC) and 18-crown-6 in the presence of tetrasodium salt of ethylenediamine-N,N,N",N"- tetraacetic acid (Na₄L) in the aqueous phase was developed. The separation factor a(Sr/Y) was substantially higher than 10⁶. This water-nitrobenzene extraction system can be applied for efficient separation of carrier-free ⁹⁰Y from ⁹⁰Sr/⁹⁰Y generator.     

Sequential radiochemical separations from Alpine Wetland soils (Boréon, France) with emphasis on 90Sr measurement

A radiochemical procedure to extract plutonium, americium and strontium from soils is presented. Strontium was separated from americium and plutonium fraction at the beginning of the method to increase the Sr recovery. The studied soils coming from an Alpine wetland site contain a big amount of iron which was eliminated by an oxalate precipitation before the column step. The hydroxide precipitation should be made by adding iron of known quantity to avoid interference. The procedure was validated by reference soils from IAEA. Plutonium-238, 239, 240, ²⁴¹Am, ⁹⁰Sr and ¹³⁷Cs activities are given and some isotopic ratios are calculated in order to know the origin of the radionuclides.     

Bestimmung von90Sr auf der Ionex-Säule in Milch und Knochen Unter Berücksichtigung der Komplexen Eigenschaften Einiger Reagenzien

The determination of⁹⁰Sr is extremely difficult in biological materials by chemical meth ods owing to the quantity of calcium associated. The problem consists of the quantitative removal of calcium and of the selective extraction of⁹⁰Sr using strontium carrier. It can be solved by precipitation and extraction methods, or by ion exchange chromatography. Following our previous works, experimental evidence is presented using ion exchange technique for these purposees, where complex compounds are used as eluents for calcium removal. For the determination of⁹⁰Sr in milk and bones, calcium was removed with 1,2-diamino-cyclohexane-N,N,N′,N′-tetraacetic acid (CyDTA) eluent from Amberlite IR-120 column. Our results show that compounds of chelatone type used as eluents with a strong acidic cation exchanger column are the most convenient, for they prefer to compound with ligands of weaker or mean complexibility (hydrochloric acid, citric acid and lactic acid).      

Separation of microamounts of yttrium from strontium by using sodium dicarbollylcobaltate, Slovafol 909 and ethylenediamine - N, N, N', N'-tetraacetic acid in the water - nitrobenzene extraction system

Summary A rapid extraction separation of trace amounts of yttrium from strontium by a nitrobenzene solution of sodium dicarbollylcobaltate (NaDCC) in the presence of p-nonylphenylnonaethylene glycol (Slovafol 909) and tetrasodium salt of ethylenediamine - N,N,N',N' - tetraacetic acid (Na₄L) in the aqueous phase was developed. The separation factor a(Sr/Y) was substantially higher than 10⁵. This water-nitrobenzene extraction system can be applied for the efficient separation of carrier-free ⁹⁰Y from ⁹⁰Y/⁹⁰Sr generator.     

Bestimmung des Gehaltes an90Sr und89Sr in Proben tierischer und pflanzlicher Herkunft

A method is described for the determination of⁸⁹Sr and⁹⁰Sr in samples of plant and animal origin. The Rehak-Feddersen method was modified to measure⁹⁰Sr. Modification was made in the sample preparation and in the toluene-HDEHP [di(2-ethylhexyl)phosphoric acid] extraction. After the extraction of yttrium, strontium is separated with nitric acid and—calculating with a correction factor—⁸⁹Sr can directly be determined. Namely,⁸⁹Sr can be measured in an aqueous solution by a liquid scintillation technique with an efficiency of 30% while⁹⁰Sr with 1.4% only. Quenching of the solution—depending on the composition—which may influence the measurement of⁹⁰Y and⁸⁹Sr was also examined. Detection limits and reproducibilities are given. Finally, evaluation of the experimental data is reported.      

The Comprehensive Nuclear Test-Ban-Treaty and the radiological risk to on-site inspection teams

The solvent extraction behavior of thorium traces from the hydrochloric acid media with 1-phenyl-3-methyl-4-benzoyl-5-pyrazolone (PMBP) is described using ²³⁴Th as a tracer. The influence of certain variables such as extractant concentration, acidity, equilibrium time as well as UO₂ ²⁺ ions on the extraction of thorium has been investigated systematically. The back-extraction behavior of thorium from the organic phase has also been tested. The results reveal that the percent extraction of ²³⁴Th decreases with increasing hydrochloric acid concentration and thorium is easily back-extracted with an 4-6 mol/l aqueous HCl solution. At the same time, the effect of thorium extraction with PMBP was tested employing radioisotopes as multi-tracers in the irradiation of natural uranium with 14-15 MeV neutrons. The results show that thorium can be completely separated from a large amount of uranium and most of the other main reaction products.     

Studies on soil samples mineralization conditions preceding the determination of 90Sr

Some results of the extraction of strontium and yttrium from soil samples by concentrated nitric acid are described. The concentration of Sr and Y in the solid was determined by XRF method. The results obtained allowed to elaborate the conditions of acid leaching and to propose an analytical procedure for the determination of ⁹⁰Sr in samples without their total dissolution.     

Separation of strontium-90 and yttrium-90 in the presence of thorium-234 by dynamic ion chromatography

A relatively rapid (<20 min) technique is described for the analysis of ⁹⁰Sr and ⁹⁰Y in the presence of ²³⁴Th. The method joins ion-chromatography and on-line scintillation detection. Experiments were performed to characterize separation of the three radionuclides in an Ion Pac CS5 ion-exchange column under the influence of the following eluents: oxalic acid, diglycolic acid (DGA), -hydroxy isobuteric acid (HIBA), and a mixture of hydrochloric acid and ammonium sulfate. Ammonium sulfate was the most effective of the eluents tested, yielding a resolution of 2.04 for strontium/yttrium and 1.03 for strontium/thorium. Within the limits of experimental uncertainty, the recoveries were quantitative for ⁹⁰Sr and ⁹⁰Y in the presence of 17 to 262 Bq·ml of ²³⁴Th.The authors thank Professor Dr R. A. Fjeld, Department of Environmental and Engineering Science, Clemson University, USA, for his helpful support and discussion.     

Characterization and application of SuperLig<Superscript>®</Superscript> 620 solid phase extraction resin for automated process monitoring of <Superscript>90</Superscript>Sr

Characterization of SuperLig^® 620 solid phase extraction resin was performed in order to develop an automated on-line process monitor for ⁹⁰Sr. The main focus was on strontium separation from barium, with the goal of developing an automated separation process for ⁹⁰Sr in high-level wastes. High-level waste contains significant ¹³⁷Cs activity, of which ^137mBa is of great concern as an interference to the quantification of strontium. In addition barium, yttrium and plutonium were studied as potential interferences to strontium uptake and detection. A number of complexants were studied in a series of batch K_d experiments, as SuperLig^® 620 was not previously known to elute strontium in typical mineral acids. The optimal separation was found using a 2 M nitric acid load solution with a strontium elution step of ~0.49 M ammonium citrate and a barium elution step of ~1.8 M ammonium citrate. ⁹⁰Sr quantification of Hanford high-level tank waste was performed on a sequential injection analysis microfluidics system coupled to a flow-cell detector. The results of the on-line procedure are compared to standard radiochemical techniques in this paper.     

Separation of strontium-90 and yttrium-90 in the presence of thorium-234 by dynamic ion chromatography

A relatively rapid (<20 min) technique is described for the analysis of ⁹⁰Sr and ⁹⁰Y in the presence of ²³⁴Th. The method joins ion-chromatography and on-line scintillation detection. Experiments were performed to characterize separation of the three radionuclides in an Ion Pac CS5 ion-exchange column under the influence of the following eluents: oxalic acid, diglycolic acid (DGA), -hydroxy isobuteric acid (HIBA), and a mixture of hydrochloric acid and ammonium sulfate. Ammonium sulfate was the most effective of the eluents tested, yielding a resolution of 2.04 for strontium/yttrium and 1.03 for strontium/thorium. Within the limits of experimental uncertainty, the recoveries were quantitative for ⁹⁰Sr and ⁹⁰Y in the presence of 17 to 262 Bq·ml of ²³⁴Th.The authors thank Professor Dr R. A. Fjeld, Department of Environmental and Engineering Science, Clemson University, USA, for his helpful support and discussion.     

Simultaneous determination of uranium and plutonium isotopes in soils by means of single alpha-spectrometry

A simple, rapid and reliable method was developed for the simultaneous determination of uranium and plutonium isotopes by alpha-spectrometry using a single source. A new uranium tracer²³⁰U was applied as well as the²³⁶Pu tracer to determine overall yields of uranium and plutonium isotopes throughout the entire procedure employed. The analytical procedure consists of sample leaching with 8N HNO₃ solution, purification by solvent extraction, simultaneous electrodeposition of U and Pu, and subsequent alpha-spectrometry with a silicon detector. In the solvent extraction using TOA/xylene from 8N HNO₃ solution, the preferential extractability of Pu rather than U permits to purify simultaneously the trace amounts of Pu and the macro amounts of U, as in the case of ordinary soil samples, resulting in favourable peak heights for both isotopes. From a single alpha-spectrum, the determinations of²³⁸U,²³⁴U (and their ratio of²³⁴U/²³⁸U),^239+240Pu, and²³⁸Pu contents were conveniently carried out after correcting the overall yields obtained from²³⁰U and²³⁶Pu activities in the same spectrum. This analytical method was satisfactorily applied to the determination of U and Pu isotope contents in some soils.     

The simple radiochemical determination of 90Sr in environmental solid samples by solvent extraction

Determination of ⁹⁰Sr in environmental solid samples is a challenging task because of the presence of so many other radionuclides in samples of interest. This problem was dealt with by radiochemical separation of strontium followed by yttrium separation and Cerenkov counting of the high-energy ??-particle emissions of ⁹⁰Y in order to quantitate ⁹⁰Sr. In this work, an improved method is described for the determination of ⁹⁰Sr in soil samples, through the separation of the daughter ⁹⁰Y at equilibrium. The procedure is based on the HDEHP solvent extraction in combination with liquid scintillation spectrometry (LSS). A low background Quantulus has been optimized for low level counting of Cerenkov radiation emitted by the hard ??-emitter ⁹⁰Y. The analytical quality of the method has been checked by analyzing IAEA Soil-375 reference materials. The analytical method has also been successfully applied to the determination of ⁹⁰Sr for moss-soil samples in inter-laboratory exercises through IAEA??s ALMERA network. The chemical recovery for ⁹⁰Y extraction ranged from 80 to 85% and the counting efficiency was 73% in the window 25?C400 keV.     

Sequential Isotopic Determination of Strontium, Thorium, Plutonium, Uranium, and Americium in Bioassay Samples

A procedure is presented to provide sequential determination of isotopic strontium, thorium, plutonium, uranium, and americium in a single biological sample. The method begins with digestion and dissolution of the sample. Tracers and/or carriers are added to the sample for the purpose of chemical yield monitoring. Strontium is first separated from the actinides and from most of the interfering constituents of the sample by precipitation as carbonates. Strontium isotopes are purified, and ⁸⁹Sr and ⁹⁰Sr are measured by gas proportional counting. Actinides are separated and purified by ion exchange chromatography, co-precipitated with neodymium fluoride, filtered, and counted by alpha-particle spectrometry.