Yttrium-90 adsorption on various soils of successive horizons in Poland

The adsorption of ⁹⁰Y on various types of soil samples representing successive horizons was studied. The adsorption process can be described by a Freundlich isotherm and was influenced by the soil type and the horizon's depth. Hydrogen ions did not have a significant influence on the adsorption of ⁹⁰Y. This revised version was published online in July 2006 with corrections to the Cover Date.     

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.     

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.     

A rapid and accurate method for the determination of strontium-90 in environmental soil

A rapid and accurate method for the determination of⁹⁰Sr in environmental soil has been developed; the procedure includes soil leaching by hydrochloric acid, oxalate precipitation, decontamination from²¹⁰Bi, separation by HDEHP extraction chromatography column, yttrium oxalate precipitation and -counting. The interference of²¹⁰Bi was found and studies have been made for the decontamination of⁹⁰Y from²¹⁰Bi by Bi₂S₃ precipitation giving a decontamination factor of 1.05·10³. The analytical results obtained by the improved rapid method for 12 soil samples were comparable to that obtained by a previous method within a relative error of 20%. Studies of vertical distribution of⁹⁰Sr in an environmental soil profile have shown that 90% of the⁹⁰Sr deposits in the 30 cm surface soil of the earth with a highest concentration of 3.40 Bq/kg. When 50 g soil was analyzed, the yield of yttrium was 73±17% with a detection limit of 0.26 Bq/kg.     

Strontium-90 determination in biological and environmental samples by direct milking of its daughter product, yttrium-90

A method is presented for the determination of ⁹⁰Sr in environmental samples by direct milking of ⁹⁰Y. Pyridine-2,6-dicarboxylic acid forms an anionic complex with yttrium which is retained on an anionic resin. Most of the matrix elements are washed out of the column as neutral or uncomplexed species and yttrium is eluted by increasing the ionic force of the eluent solution. This method gives yttrium recoveries between 65% to 85% for soil, grass, milk and bone samples with very high radiochemical purity (⁹⁰Y average half-life of 66±4 hours) and a detection limit of 0.3 Bq/kg of soil. The method supports a calcium content up to 3 g per sample without any decrease in yttrium yield, allowing the measurement of milk, milk-teeth and bone samples with no concentration step in one day.     

Adaptation of a radioanalytical method for strontium-90 to different kinds of environmental samples and its application for the investigation of some samples in the Riyadh region

A relatively simple and rapid radioanalytical method, limited to milk, is adapted for investigating soil, biological and water samples for⁹⁰Sr. The method is based on a selective separation and successive counting of equilibrium quantities of its daughter 90Y, which can be extracted by tributyl phosphate from nitrate medium and stripped by conc. ammonia solution. 90Y is separated from possible iron and measured by Cerenkov counting. The procedure is thoroughly tested with certified reference materials and used lately for determining⁹⁰Sr in some environmental samples in the Riyadh region. The results obtained are given and discussed.     

Sequential separation and determination of plutonium, americium-241 and strontium-90 in soils and sediments

A sensitive and reliable metbod for the sequential separation and determination of plutonium,²⁴¹Am and⁹⁰Sr in soil samples was developed. Plutonium was separated by a Microthene-TNOA column. Then⁹⁰Y (for⁹⁰Sr determination) was separated from americium by a HDEHP column after elimination of large amounts of interfering stable or radioactive nuclides (iron,²¹⁰Bi and²¹⁰Po etc.) by an oxalate precipitation and a Microthene-TNOA column. Finally americium was purified by another HDEHP column and a PMBP-TOPO extraction. A special attention was paid to the decontamination of Pu and Am from²¹⁰Po and of⁹⁰Y from²¹⁰Bi; the relevant decontamination factors resulted greater than 10⁵, 10⁶ and 10⁴ respectively. The detection limits were 1.2 mBq/kg for Pu and 1.7 mBq/kg for²⁴¹Am and 0.32 Bq/kg for⁹⁰Sr. The procedure was checked by analyzing three certified samples supplied by IAEA. Some Italian soil samples were also analyzed giving average yields of 84.9±7.2% for Pu, 57.8±3.2%for Am and 96.7±1.6% for Y; the^239+240Pu,²³⁸Pu,²⁴¹Am and⁹⁰Sr contents (Bq/kg) ranged from 0.347 to 1.53, from 0.013 to 0.048, from 0.126 to 0.556 and from 2.89 to 11.6 respectively and the average ratios were 0.037±0.017 for²³⁸Pu/^239+240Pu, 0.357±0.040 for²⁴¹Am/^239+240Pu and 7.0±1.2 for⁹⁰Sr/^239+240Pu.     

Separation of Y from Sr by zirconium vanadate gel ion-exchanger sorbent: kinetics and thermodynamic study

A new zirconium vanadate (Zr–V) ion-exchanger was synthesized and characterized for fast and selective separation procedure of ⁹⁰Y from ⁸⁹Sr. The method was based on ⁹⁰Y(III) sorption from aqueous HCl solution containing ⁸⁹Sr(II) onto Zr–V gel exchanger. The kinetics of Y(III) sorption from HCl solution by Zr–V exchanger was subjected to Weber–Morris, Lagergren, Bhattacharya and Venkobachar, and Bt models. Initially, the uptake of Y(III) onto the exchanger was fast followed by kinetically first-order sorption with an overall rate constant, K _Lager = (3.55 ± 0.03) × 10^?4 min^?1. Film and intraparticle transport are the two steps that might influence Y(III) sorption. The negative values of ΔG of ⁹⁰Y retention dictate that, the process is a spontaneous. The negative values of ΔH and ΔS reflect the exothermic nature of ⁹⁰Y(IIsorption and the random uptake of ⁹⁰Y(III) onto Zr–V sorbent. Zr–V exchanger offers unique advantages of ⁹⁰Y(III) retention over conventional solid sorbents in rapid and effective separation of traces of ⁹⁰Y(III) from Sr. The exchanger was successfully packed in column for an effective separation of ⁹⁰Y.     

Separation of yttrium-90 from strontium-90 via colloid formation

No-carrier-added ⁹⁰Y was separated from ⁹⁰Sr via colloid formation of ⁹⁰Y in basic media. The mixture was passed through glass wool or membrane filter. The filtrate contained ⁹⁰Sr, while ⁹⁰Y was retained on glass wool/membrane filter. Yttrium-90 was extracted with 0.1 M HCl. Contamination of ⁹⁰Sr was <0.0001%. More than 98% labeling yield of ⁹⁰Y-EDTMP was confirmed by paper chromatography.     

Evaluation of interferences on measurements of 90Sr/90Y by TDCR Cherenkov counting technique

A study to evaluate conditions affecting the determination of ⁹⁰Sr/⁹⁰Y activities in liquid samples by the triple-to-double coincidence ratio (TDCR) Cherenkov counting technique was conducted. The Cherenkov radiation produced by the ⁹⁰Y beta decay was determined using a commercially available Hidex 300 SL liquid scintillation counter. The interferences of sample geometry, including sample counting vial type and volume composition, and sample colour on the TDCR were investigated. The effects of potentially interfering beta and mixed beta–gamma emitters on the TDCR Cherenkov counting of ⁹⁰Sr/⁹⁰Y activities were also examined. The TDCR values were used to quantify counting efficiencies of ⁹⁰Y under different experimental conditions. The results demonstrated that the Cherenkov counting efficiency of ⁹⁰Y is independent of sample volume and counting vial size. The effect of colour quenching was examined using yellow and brown food-grade dyes. The TDCR correction for colour quenching was found to be effective. An evaluation of counting efficiency of different beta-emitting radionuclides demonstrated that strong gamma emissions can contribute to the Cherenkov counting efficiency. Overall, measured radioactivity values deviated from reference values by ≤7.5 %, which is acceptable for screening applications in emergency situations.     

Radiochemical determination of 90Sr and 86Sr in soil

Summary A modified HCl-leach method for the radiochemical ⁹⁰Sr and ⁸⁹Sr determination in soil has been developed. The sample is leached by HCl in the presence of the Sr-carrier. Then bi- and trivalent ions are separated by a combination of complexation and ion exchange. The separation of strontium and calcium is performed by fuming nitric acid. After further purification, strontium carbonate is precipitated and the activity of ⁹⁰Sr and ⁸⁹Sr is measured. ⁹⁰Sr determined by the isolation of ⁹⁰Y and by measuring its activity. The ⁹⁰Sr and ⁸⁹Sr content in soil is calculated from the measured activities of yttrium oxide and strontium carbonate by considering the counting efficiencies for ⁹⁰Y, ⁹⁰Sr and ⁸⁹Sr beta rays, the chemical yields of strontium and yttrium and the time of ⁹⁰Y growth from ⁹⁰Sr.

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Radiochemische Bestimmung von ⁹⁰Sr und ⁸⁹Sr in Boden

Zusammenfassung Eine modifizierte Auslaugungsmethode für die radiochemische Bestimmung von ⁹⁰Sr und ⁸⁹Sr im Boden wurde entwickelt. Die Probe wird in HCl in Gegenwart des Sr-Trägers ausgelaugt und die zwei- und dreiwertigen Ionen dann durch eine Kombination von Komplexierung und Ionenaustausch getrennt. Die Strontiumtrennung von Calcium erfolgt mit rauchender Salpetersäure. Nach weiterer Reinigung wird SrCO₃ gefällt und die Aktivität von ⁹⁰Sr und ⁸⁹Sr bestimmt. ⁹⁰Sr wird durch Isolierung und Zählung von ⁹⁰Y ermittelt. Der ⁹⁰Sr- und ⁸⁹-Sr-Gehalt im Boden wird aus der Aktivität von Y₂O₃ und SrCO₃ unter Berücksichtigung der Zählausbeute für ⁹⁰Y-, ⁹⁰Sr- und ⁸⁹-Sr-beta-Strahlen, aus der gravimetrischen Bestimmung von Strontium und Yttrium und aus der Zeit der ⁹⁰Y-Entstehung aus ⁹⁰Sr bestimmt.

     

Validation of an extraction paper chromatography (EPC) technique for estimation of trace levels of 90Sr in 90Y solutions obtained from 90Sr/90Y generator systems

While the extraction paper chromatography (EPC) technique constitutes a novel paradigm for the determination of few Becquerels of ⁹⁰Sr in MBq quantities of ⁹⁰Y obtained from ⁹⁰Sr/⁹⁰Y generator, validation of the technique is essential to ensure its usefulness as a real time analytical tool. With a view to explore the relevance and applicability of EPC technique as a real time quality control (QC) technique for the routine estimation of ⁹⁰Sr content in generator produced ⁹⁰Y, a systematic validation study was carried out diligently not only to establish its worthiness but also to broaden its horizon. The ability of the EPC technique to separate trace amounts of Sr²⁺ in the presence of large amounts of Y³⁺ was verified. The specificity of the technique for Y³⁺ was demonstrated with ⁹⁰Y obtained by neutron irradiation. The method was validated under real experimental conditions and compared with a QC method described in US Pharmacopeia for detection of ⁹⁰Sr levels in ⁹⁰Y radiopharmaceuticals.     

Rapid determination of 90Sr/90Y in water samples by liquid scintillation and Cherenkov counting

Strontium-90 (⁹⁰Sr) is a ubiquitous contaminant at nuclear facilities, found at high concentrations in spent nuclear fuel and radioactive waste. Due to its long half-life and ability to be transported in groundwater, an accurate method for measuring ⁹⁰Sr in water samples is critical to the monitoring program of any nuclear facility. To address this need, a rapid procedure for sequential separation of Sr/Y was developed and tested in groundwater samples collected from an area of riverbed affected by a ⁹⁰Sr groundwater plume. Sixteen samples, plus spike and water blanks, were analyzed. Five different measurements were performed to determine the ⁹⁰Sr and yttrium-90 (⁹⁰Y) activities in the samples: direct triple-to-double-coincidence ratio (TDCR) Cherenkov counting of ⁹⁰Y, liquid scintillation (LS) counting for ⁹⁰Sr following radiochemical separation, LS counting for ⁹⁰Y following radiochemical separation, Cherenkov counting for ⁹⁰Y following radiochemical separation and LS counting of the Sr samples for ⁹⁰Y in-growth. The counting was done using a low-level Hidex 300SL TDCR counter. Each measurement method was compared for accuracy, sensitivity and efficiency. The results following Cherenkov counting and radiochemical separation were in very good agreement with one another.     

Determination of90Sr in environmental and biological materials with combined HDEHP solvent extraction-low liquid scintillation counting technique

Low level⁹⁰Sr in environmental and biological samples is determined using a combined HDEHP solvent extraction-liquid scintillation procedure. Yttrium-90 is selectively extracted from nitric acid solution into 5% di(2-ethylhexyl) phosphoric acid (HDEHP) in toluene, and⁹⁰Y in the organic phase is measured directly using an ultra low level liquid scintillation spectrometer.The working program of the Quantulus counter has been optimized. As the counting efficiency using liquid scintillation counting is high and the stripping and precipitation of Yttrium-90 oxalate is omitted, this procedure is simpler and more timesaving than traditional methods. The chemical recoveries of⁹⁰Y were 85.1% for soil, 75.7% for milk and 65.3% for bone. The detection limit is 8 mBq.     

Adsorption and migration of <Superscript>241</Superscript>Am in aerated zone soil

As an important radioisotope in nuclear industry and other fields, ²⁴¹ Am is one of the most serious contamination concerns due to its high toxicity and long half-life. In order to supply useful reference for disposal of ²⁴¹Am waste with low-medium radioactivity, the adsorption and migration behavior of ²⁴¹Am on aerated zone soil were investigated by the static experimental method and column experiments. The results showed that more than 98% of the total ²⁴¹Am could be adsorbed from ²⁴¹Am solution of 0.32·10⁻⁷−1.1·10⁻⁷ mol/l by the soil at pH 4–9. The adsorption of ²⁴¹Am on the soil was a pH-dependent process at pH<4, but for pH>4, the adsorption rate of ²⁴¹Am on the soil changed minutely. The adsorption equilibrium was achieved within 24 hours and no significant effect on adsorption of ²⁴¹Am was observed at liquid-solid ratios of 50:1–500:1. The relationship between concentration of ²⁴¹Am and adsorption capacities of ²⁴¹Am can be described by the Freundlich adsorption equation. Adsorption of ²⁴¹Am on the soil can be inhibited by humic acid, ferric hydroxide colloid, or some anions, such as citric acid anion, saturated EDTA solution, C₂O₄ ²⁻ and CO₃ ²⁻. It was also noted that the adsorption rate of ²⁴¹Am drops in solutions containing Eu³⁺ or Nd³⁺, even 0.5 times above the ²⁴¹Am concentration. A migration distance of 8 mm for ²⁴¹Am(III) is observed only in the aerated zone soil containing ferric colloid, while a migration distance of less than 2 mm is noted in other soil samples after more than 250 days. All these results indicate that the aerated zone soil is an efficient sorbent for ²⁴¹Am and can inhibit the migration of ²⁴¹Am.     

Separation of yttrium from strontium in the aqueous phase of the water/nitrobenzene system

A rapid separation of carrier-free ⁹⁰Y in the aqueous phase of the water/nitrobenzene extraction system from an ⁹⁰Y/⁹⁰Sr generator is proposed. After a three-stage extraction, the chemical yield of ⁹⁰Y in the final aqueous phase was almost 90%, while the ⁹⁰Sr radionuclide impurity in this phase containing carrier-free ⁹⁰Y was about 10^–10%.     

The use of liquid scintillation spectrometry for the determination of radionuclidic purity of 90Y from a radiochemical 90Y/90Srgenerator

Summary An extraction technique for the separation of ⁹⁰Sr from a high excess of⁹⁰Y has been developed. This procedure can be used for the determination of trace amounts of⁹⁰Sr in⁹⁰Y prepared by a radiochemical⁹⁰Y/⁹⁰Sr generator by liquid scintillation.     

Preparation of 90Y by the 90Sr-90Y Generator for Medical Purpose

The production of ⁹⁰Y by ⁹⁰Sr-⁹⁰Y generator was studied. ⁹⁰Sr was adsorbed on a column with Aminex A-5 resin. The daughter radionuclide ⁹⁰Y was eluted with 0.7M -hydroxyisobutyrate (-HIB, pH 5.4). Radionuclidic, radiochemical and chemical purities were >98% and yield >85%. After converting into chloride form ⁹⁰YCl₃-solution (pH:1) was used for preparing injectable yttrium citrate and labeling some other radiopharmaceuticals. Furthermore, a fast ITLC-method for the determination of ⁹⁰Sr in ⁹⁰Y-eluate was developed.     

Research on extracted <Superscript>90</Superscript>Y with P204 in lipiodol for liver cancer

Research on extracted ⁹⁰Y with di(2-ethylhexyl) orthophosphoric acid (P204) in lipiodol for liver cancer was made to evaluate the stability of extracted ⁹⁰Y with P204 in lipiodol (⁹⁰Y-P204-lipiodol) in serum of newly-born cattle and human’s blood. At first, P204 (extractant) was dissolved in lipiodol (organic phase). Secondly, ⁹⁰Y was extracted to organic phase after adding ⁹⁰Y solution into test tube with P204 and lipiodol in it. The extracting efficiency with 0.01 mol/l P204 could reach 99.4%. The stability of ⁹⁰Y-P204-lipiodol has been experimented in physiological saline solution as preparation for further stability experiment. The result indicated that the extracted ⁹⁰Y lost 0.02%–0.36% in physiological saline solution. The results of further stability experiment showed that loss efficiencies of extracted ⁹⁰Y after adding newly-born cattle serum 1 hour, 1 day, 3 and 7 days are 3.38%, 3.12%, 4.29% and 6.62%, respectively, and loss efficiencies of extracted ⁹⁰Y after adding human’s blood 1 hour, 1 day, 3 and 7 days are 2.55%, 5.91%, 7.88% and 5.63%, respectively. Our data also indicated that ⁹⁰Y is the most possible radioisotope for being extracted with P204 in lipiodol to treat hepatocellular carcinoma, particularly in cases of unresectable liver tumors, since ⁹⁰Y is available from several commercial sources in clinical quality. We conclude that the stability of ⁹⁰Y-P204-lipiodol tested with newly-born cattle serum and human’s blood attained great results. ⁹⁰Y-P204-lipiodol is a kind of potential and exciting pharmaceutical in inerventional therapy for liver cancer and we can carry on the further animal test and clinical trial.     

Adsorption and desorption of Am(III) on calcareous soil and its parent material

Summary The adsorption and desorption of Am(III) on a calcareous soil (sierozem) and its parent material (loess) were studied by batch technique. The molarities of the Am(III) aqueous solutions were less than 5 ^. 10^-9 mol/l. High adsorbability was found of Am(III) on the calcareous soil and its parent material. In order to decrease the adsorption and, hence, to investigate the adsorption characteristics properly, stable Eu³⁺ as hold back carrier and analogue was added to the aqueous solution. The relative contributions of CaCO₃, organic matter (OM) to the Am(III) adsorption on calcareous soil and its parent material were investigated. The adsorption and desorption isotherms of Am(III) on untreated soil and loess and the three kinds of treated soils and three kinds of treated loesses to remove CaCO₃, OM and both CaCO₃ and OM were determined, respectively. It was found that all isotherms were linear, the average distribution coefficients (K^-_d) for the untreated soil and for the untreated loess were almost equal, while there was an obvious difference between the values of the average distribution coefficients (K^-_d) for the treated soil and the treated loess to remove CaCO₃ or OM. The adsorption-desorption hysteresis on the untreated and treated soils and loesses actually occurred and there was an obvious difference between the hysteresis coefficients on both the corresponding treated soil and loess. It can be concluded that the adsorbability of Am(III) on calcareous soil is similar to that on its parent material, and that the contributions of CaCO₃ and OM to the Am(III) adsorption by the untreated soil are different from those by the untreated parent material.