Rapid separation of actinides and radiostrontium in vegetation samples

A new rapid method for the determination of actinides and radiostrontium in vegetation samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used in emergency response situations or for routine analysis. The actinides in vegetation method utilizes a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step, and a streamlined column separation process with stacked TEVA, TRU and DGA Resin cartridges. Lanthanum was separated rapidly and effectively from Am and Cm on DGA Resin. Alpha emitters are prepared using rare earth microprecipitation for counting by alpha spectrometry. The purified ⁹⁰Sr fractions are mounted directly on planchets and counted by gas flow proportional counting. The method showed high chemical recoveries and effective removal of interferences. The actinide and ⁹⁰Sr in vegetation sample analysis can be performed in less than 8 h with excellent quality for emergency samples. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory actinide particles or vegetation residue after furnace heating is effectively digested.     

In situ neutron activation analysis of and the neutron capture cross-section for90Sr+

Neutron activation analysis has been investigated as an in situ method for determination of⁹⁰Sr. The thermal neutron capture cross-section for the⁹⁰Sr(n, γ)⁹¹Sr reaction has been measured to be 14.0±2.4 mb which is in disagreement with the currently accepted literature value. The suitability of this reaction and the fast neutron reactions⁹⁰Sr(n, p)⁹⁰Rb and⁹⁰Sr(n, α)⁸⁷Kr, for the in situ determination of⁹⁰Sr is discussed.     

Feasibility study of an analytical method for detecting <Superscript>90</Superscript>Sr in soil using DGA resin and Sr resin

This study investigated an analytical method for detecting ⁹⁰Sr in soil samples for the routine monitoring of environmental radioactivity. Mineral acid leaching and fusion methods were first used to digest the soil sample, and the analytical results were compared. DGA resin was employed to separate ⁹⁰Y, being a daughter of ⁹⁰Sr. Then, ⁹⁰Y was analyzed by liquid scintillation counter (LSC). These analytical results were compared with those obtained using Sr resin, which is a well-known, simple and reliable separation method. With the DGA resin approach a minimum detectable activity of ~0.28 Bq kg^?1 was detected in a 50 g sample, with 180 min of counting time, 70% recovery and ~97% counting efficiency using a LSC.     

Co-precipitation of plutonium(IV) and americium(III) from nitric acid–oxalic acid solutions with bismuth oxalate

This study presents analytical methods for the determination of gross beta, ⁹⁰Sr, ²²⁶Ra and Pu isotopes using samples in the IAEA-TEL-2015-04 ALMERA Proficiency Test exercise. Samples for gross beta were prepared by evaporation and then analyzed using a gas proportional counter. ⁹⁰Sr in the liquid sample was concentrated as SrCO₃ precipitates and purified by Sr resin. Pu isotopes and ⁹⁰Sr in the soil sample were extracted from the sample by mineral acid leaching and separated using TEVA and Sr resin, respectively. Pu isotopes were determined by alpha spectrometry and ⁹⁰Sr were determined with a liquid scintillation counter. Radium in the soil sample was extracted by LiBO₂ fusion, and the radon-emanation method using LSC was applied for the determination of ²²⁶Ra.     

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.     

Radiochemical separation of Pu, U, Am and Sr isotopes in environmental samples using extraction chromatographic resins

This study presents a rapid and quantitative sequential radiochemical separation method for Pu, U, Am and Sr isotopes in environmental samples with extraction chromatographic resins. After radionuclides were leached from the samples with 6 M HNO₃, Pu and U isotopes were adsorbed onto the UTEVA column and Am isotopes were adsorbed onto the TRU column connected with the UTEVA column. Also, ⁹⁰Sr was adsorbed onto the Sr column connected with the TRU column. Pu and U isotopes were purified from other nuclides through the UTEVA column. In addition, Am isotopes were separated from other nuclides with the TRU column. Finally, ⁹⁰Sr was purified with the Sr resin. After α source preparation for the purified Pu, U and Am isotopes with micro-coprecipitation method, Pu, U and Am isotopes were measured using alpha spectrometry. On the other hand, ⁹⁰Sr was measured using a low level liquid scintillation counter. The radiochemical procedure for Pu, U, Am and Sr nuclides investigated in this study has been applied to environmental samples after validating the simulated samples.     

Simultaneous determination of Cs and Sr in the high level waste by ion-chromatography

A method based on ion-chromatography has been developed for determination of Cs and Sr in high level waste (HLW) without matrix separation. The acidity of HLW (3 M HNO₃) was decreased to 0.01 M by addition of NaOH. Chromatographic separation of Cs⁺ and Sr⁺⁺ in presence of bulk Na⁺ has achieved using methane sulphonic acid as mobile phase in isocratic and gradient mode. The calibration plot was linear for the concentration range of 0.5–12 mg/L for Cs and 0.025–6 mg/L for Sr with regression coefficients close to 1. RSD obtained for Cs and Sr was 1 and 5 % respectively. Detection limit calculated as 3(S/N) was found to be 20 μg/L for Cs and 30 μg/L for Sr. The standard addition procedure was used to validate the developed method. The samples received from PREFRE, Tarapur and WIP, BARC were analyzed by the new method and the results are presented.     

Standardization of multi-nuclide mixtures by a new spectrum unfolding method

A new spectrum unfolding method has been applied to double-labeled mixtures with excellent results, while the CIEMAT/NIST method has been used for gels. The convenience of applying both methods has been demonstrated with mixtures containing more than three components.⁹⁰Sr+⁹⁰Y,⁸⁹Sr,²⁰⁴TI,⁴⁵Ca and³⁵S nuclides were combined as three, four and five components, and the different quench values and activity ratios were assayed. The discrepancies between computed and experimental activities were also obtained. Mixtures with some of their components below background have been prepared in order to test low-level activities.     

Removal of 90Sr and 241Am from concentrated Hanford chelate-bearing waste by precipitation with strontium nitrate and sodium permanganate

The Hanford Nuclear Site, near Richland, Washington, is developing a method to simultaneously remove chelated ⁹⁰Sr and ²⁴¹Am from the liquid phase of high-level nuclear waste using sodium permanganate and cold strontium nitrate. This method has been reported previously for treating diluted waste in the Hanford Waste Treatment and Immobilization facility (WTP) that is currently under construction. This method had not been verified previously for treating the more concentrated waste as it sits in the tank farm. There are a number of logistical advantages to performing this process in the tank farm. Therefore, the present study was undertaken to compare the removal of ⁹⁰Sr and ²⁴¹Am in diluted waste (WTP conditions) and more concentrated waste (tank farm conditions). Both diluted and more concentrated waste from Hanford tank AN-107 was treated with 3.0 M Sr(NO₃)₂ and 3.8 M NaMnO₄, at a constant cold chemical to radionuclide ratio. The amount of ⁹⁰Sr and ²⁴¹Am removed was monitored through alpha and beta counting. The removal of ⁹⁰Sr was essentially identical at both levels of dilution. The removal of ²⁴¹Am was slightly better in the diluted sample than in the tank farm sample, but the difference was not large (77 % versus 67 % removed). These results indicate that it is reasonable to expect this ⁹⁰Sr and ²⁴¹Am removal process can be employed in the tank farm.     

Analytical method for determining colour intensities based on Cherenkov radiation colour Quenching

In the present work a study was made for determining colour intensities using as luminous non-monochromatic source the Cherenkov emission produced in the walls of a glass capillary which acts as luminous source itself inside of a coloured solution to be evaluated. The reproducibility of this method has been compared with the spectrophotometric assay; the relative errors of both analytical methods have been calculated for different concentrations of congo red solution in the range of minimal error, according to Ringbom's criterion. The sensitivity of this analytical method has been studied for the two β-emitters employed:⁹⁰Sr/⁹⁰Y and²⁰⁴Tl.     

Seasonal variations of atmospheric210Pb and7Be concentrations at Kumamoto, Japan and their removal from the atmosphere as wet and dry depositions</p> </p>

Summary A relatively simple chemical separation procedure has been developed for the simultaneous determination of⁸⁹Sr and ⁹ 0Sractivities in water samples and on aerosol-filters of the Nuclear Power Plant (NPP) Paks origin. The procedure combines the cation-exchange chromatographic (Dowex 50 WX 8 resin) and solid phase extraction (EIChroM Sr.Spec?, DC18C6 crown ether) steps. The beta-radiation of radionuclides can be measured directly after the chemical separation by LSC. The activities of⁸⁹Sr,⁹⁰Sr and⁹⁰Y are calculated from an over determined set of equations using a method of constrained optimization technique. The equations are based on LSC measurements performed in three counting windows plus the⁹⁰Sr-⁹⁰Y decay law. The chemical yield of strontium is determined by ICP-AES. The lowest limits of detectable activity, for the measurement time of 600 minutes, are 30 mBq/sample and 18 mBq/sample for⁸⁹Sr and⁹⁰Sr, respectively.     

Analytical Methods for the Determination of 90Sr and 239,240Pu in Environmental Samples

Artificial long-lived radionuclides such as ⁹⁰Sr and ^239,240Pu have been long released into the environment by human nuclear activities, which have a profound impact on the ecological environment. It is of great significance to monitor the concentration of these radionuclides for environmental safety. This paper summarizes and critically discusses the separation and measurement methods for ultra-trace determination of ⁹⁰Sr, ²³⁹Pu, and ²⁴⁰Pu in the environment. After selecting the measurement method, it is necessary to consider the decontamination of the interference from matrix elements and the key elements, and this involves the choice of the separation method. Measurement methods include both radiometric methods and non-radiometric methods. Radiometric methods, including alpha spectroscopy, liquid scintillation spectrometry, etc., are commonly used methods for measuring ^239+240Pu and ⁹⁰Sr. Mass spectrometry, as the representative of non-radiometric measurement methods, has been regarded as the most promising analytical method due to its high absolute sensitivity, low detection limit, and relatively short sample-analysis time. Through the comparison of various measurement methods, the future development trend of radionuclide measurement is prospected in this review. The fully automatic and rapid analysis method is a highlight. The new mass spectrometer with ultra-high sensitivity shows strong analytical capabilities for extremely low concentrations of ⁹⁰Sr, ²³⁹Pu, and ²⁴⁰Pu, and it is expected to develop determination methods with higher sensitivity and lower detection limit.     

Implementation of a Sequential Injection Pre-Treatment Method for Simultaneous Radium and Strontium Determination

A semi-automatic procedure for the simultaneous determination of Ra and Sr in two steps has been developed. In the first step, separation and pre-concentration of both analytes is performed by using a sequential injection procedure. In the second step, the activities of ²²⁶Ra and ⁹⁰Sr, alpha and beta emitters, respectively, are determined using a low background proportional counter at the corresponding plateau potentials. ²²⁶Ra concentration is obtained by a single measurement of the precipitate. ⁹⁰Sr activity is determined by means of its daughter ⁹⁰Y carrying out two different measurements along the first day after the separation process; the solution of the Bateman radioactivity decay equations allows to obtain the initial ⁹⁰Sr-⁹⁰Y activities. The activities analysed in the present work have been ranged between 0-14 Bq/L for ²²⁶Ra and 0-175 Bq/L for ⁹⁰Sr.     

Problems in obtaining precise and accurate Sr isotope analysis from geological materials using laser ablation MC-ICPMS

This paper reviews the problems encountered in eleven studies of Sr isotope analysis using laser ablation multicollector inductively coupled plasma mass spectrometry (LA-MC-ICPMS) in the period 1995–2006. This technique has been shown to have great potential, but the accuracy and precision are limited by: (1) large instrumental mass discrimination, (2) laser-induced isotopic and elemental fractionations and (3) molecular interferences. The most important isobaric interferences are Kr and Rb, whereas Ca dimer/argides and doubly charged rare earth elements (REE) are limited to sample materials which contain substantial amounts of these elements. With modern laser (193 nm) and MC-ICPMS equipment, minerals with >500 ppm Sr content can be analysed with a precision of better than 100 ppm and a spatial resolution (spot size) of approximately 100 μm. The LA MC-ICPMS analysis of ⁸⁷Sr/⁸⁶Sr of both carbonate material and plagioclase is successful in all reported studies, although the higher ⁸⁴Sr/⁸⁶Sr ratios do suggest in some cases an influence of Ca dimer and/or argides. High Rb/Sr (>0.01) materials have been successfully analysed by carefully measuring the ⁸⁵Rb/⁸⁷Rb in standard material and by applying the standard-sample bracketing method for accurate Rb corrections. However, published LA-MC-ICPMS data on clinopyroxene, apatite and sphene records differences when compared with ⁸⁷Sr/⁸⁶Sr measured by thermal ionisation mass spectrometry (TIMS) and solution MC-ICPMS. This suggests that further studies are required to ensure that the most optimal correction methods are applied for all isobaric interferences.     

Etude des generateurs de strontium-87m

A method is proposed for the determination of chemical and radionuclidic purity of^87mSr generator eluates. Two generators of different origins have been studied. The presence of the radionuclides⁸⁷Y,⁸⁵Sr,⁸⁸Y,⁶⁰Co,⁵⁸Co has been shown in the eluates. Fe and Sr were not found in the eluates in concentrations higher than 10 mg/l and 100 mg/l, respectively. A recommendation is made for the use of these generators.      

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.     

Artificial radioactive contamination of sediments along the Romanian sector of the Danube river and the Black Sea coast

The concentrations of⁹⁰Sr,²³⁸Pu,^239,240Pu and²⁴¹Am were determined in 12 sediment samples, collected from the bed of the Romanian sector of the Danube river and the Black Sea coast during 1996–1997. The samples were dissolved using a microwave digestion technique which left the refractory part of the samples undissolved. Part of the samples were also dissolved totally by alkaline fusion. The results obtained after radiochemical separations and measurement of the radionuclides by the two dissolution methods were compared recommending the optimum method. The radioactive contamination of the investigated sector in 1996–1997 is compared with the results obtained for the same locations in 1994–1995 reported in previous papers.     

Improved method for the separation of radioactive strontium from various samples by mixed solvent anion exchange

Procedures for the separation and determination of⁹⁰Sr in liquid samples, with cation and anion exchangers have been described. Strontium, yttrium and other cations bind to the cation exchanger and are eluted from the column by means of nitric acid. Separation of yttrium and strontium from other cations is carried out on columns filled with strong base anion exchangers in nitrate form with alcoholic solutions of nitric acid. This separation method enables the determination of⁹⁰Sr through yttrium on a low-level gas flow α, β-counter, as well as through strontium on a lowlevel liquid scintillation counter by means of Cherenkov counting. Such procedures have been tested by the determination of⁹⁰Sr in water, wine, medium radioactive liquid waste samples, milk and clover samples. For comparison, the determination has also been carried out by the standard method. It has been showed that the developed procedures might produce a high efficiency in strontium separation and a satisfactory accuracy of determination.     

Rapid determination of radiostrontium in seawater samples

A new method for the determination of radiostrontium in seawater samples has been developed at the Savannah River National Laboratory (SRNL) that allows rapid pre-concentration and separation of strontium and yttrium isotopes in seawater samples for measurement. The new SRNL method employs a novel and effective pre-concentration step that utilizes a blend of calcium phosphate with iron hydroxide to collect both strontium and yttrium rapidly from the seawater matrix with enhanced chemical yields. The pre-concentration steps, in combination with rapid Sr Resin and DGA Resin cartridge separation options using vacuum box technology, allow seawater samples up to 10 L to be analyzed. The total ⁸⁹Sr + ⁹⁰Sr activity may be determined by gas flow proportional counting and recounted after ingrowth of ⁹⁰Y to differentiate ⁸⁹Sr from ⁹⁰Sr. Gas flow proportional counting provides a lower method detection limit than liquid scintillation or Cerenkov counting and allows simultaneous counting of samples. Simultaneous counting allows for longer count times and lower method detection limits without handling very large aliquots of seawater. Seawater samples up to 6 L may be analyzed using Sr Resin for ⁸⁹Sr and ⁹⁰Sr with a minimum detectable activity (MDA) of 1–10 mBq/L, depending on count times. Seawater samples up to 10 L may be analyzed for ⁹⁰Sr using a DGA Resin method via collection and purification of ⁹⁰Y only. If ⁸⁹Sr and other fission products are present, then ⁹¹Y (beta energy 1.55 MeV, 58.5 day half-life) is also likely to be present. ⁹¹Y interferes with attempts to collect ⁹⁰Y directly from the seawater sample without initial purification of Sr isotopes first and ⁹⁰Y ingrowth. The DGA Resin option can be used to determine ⁹⁰Sr, and if ⁹¹Y is also present, an ingrowth option with using DGA Resin again to collect ⁹⁰Y can be performed. An MDA for ⁹⁰Sr of <1 mBq/L for an 8 h count may be obtained using 10 L seawater sample aliquots.     

Sequential estimation of106Ru,137Cs,and90Sr in urine

A sequential method has been developed for the estimation of¹⁰⁶Ru,¹³⁷Cs, and⁹⁰Sr in urine using beta counting. After completely destroying the organic matter in urine,¹⁰⁶Ru is oxidized to volatile ruthenium tetroxide and allowed to reactin-situ with polyethylene powder;¹³⁷Cs is concentrated on ammonium phosphomolybdate and estimated as tetraphenylborate;⁹⁰Sr is coprecipitated as strontium sulphate and converted to carbonate. The recoveries have been found to be better than 83% for all of the radionuclides. The minimum detection limits are 0.16, 0.85, and 0.14 Bq/dm³ for¹⁰⁶Ru,¹³⁷Cs, and⁹⁰Sr, respectively. Yttrium-90 fraction of⁹⁰Sr is also estimated using sodium nitroprusside as reagent, after allowing it to grow for 14 days.This work forms part of the doctoral work of SRIM.V.R. PRASAD to be submitted to the University of Madras, under the supervision of DR. O.M. SREEDHARAN.