Recovery and purification of Sr(II) in perchloric acid medium

Perchloric acid was found to be a suitable medium for the quantitative leaching of Sr(II) from homogeneous and calcined (Th,Sr)O₂ particularly with respect to the contamination from Th(IV). ⁹⁰Sr is a cause of major concern to the environment due to its long half life (28.6 years), significant abundance in large inventory of spent nuclear fuels (~350 thousand tons) awaiting geological disposal and its chemical similarity to Ca(II), an essential element for the living beings. Application of ⁹⁰Sr as a parent radionuclide for ⁹⁰Y (used in therapy radiopharmaceuticals) is possible provided it can be made available at desired high purity. In this context, the distribution coefficients of Sr(II), Th(IV), Zr(IV), Y(III), ¹⁵²Eu(III) and ¹³⁷Cs(I) were determined using Sr selective crown ether 4,4′(5′)-di-tert-butyl-dicyclohexano-18-crown-6 by solid–liquid extraction in perchloric acid medium. Feasibility of employing extraction chromatography using Sr selective resin for the recovery and purification of Sr(II) from leached perchloric acid medium was explored. Perchloric acid medium is better than nitric acid medium for the uptake of Sr by Sr selective chromatographic resin under varying loading conditions of Sr(II). Similarly pH 2 solution appears better eluent of Sr(II) than distilled water. Present work offers a novel approach for setting up a ⁹⁰Sr–⁹⁰Y generator.     

Studies on the separation of 90Y from 90Sr by solvent extraction and supported liquid membrane using TODGA: role of organic diluent

Solvent extraction and supported liquid membrane transport studies on Y(III) and Sr(II) were carried out using both nitric as well as hydrochloric acid feed conditions using N,N,N′,N′-tetra-octyldiglycolamide (TODGA) in several organic diluents. The solvent extraction studies indicated extremely large separation factor (SF) values with chloroform, carbon tetrachloride, 1-decanol and hexone when 6 M HNO₃ was used as the feed. On the other hand, the SF values were 1–2 orders of magnitude lower when the nitric acid concentration was 3 M HNO₃. Significantly large SF values were also obtained from 6 M HCl when xylene, carbon tetrachloride, n-dodecane and hexone were used as the diluent. Though mass transfer was not very promising in the supported liquid membrane studies with most of the diluent systems, quantitative Y(III) transport was observed with 0.1 M TODGA in xylene with negligible Sr(II) transport suggesting possibility of obtaining carrier free ⁹⁰Y. The purity of the radiotracer was checked by half-life method.     

Estimation of 90Sr in reprocessed uranium oxide samples

Summary A method has been developed for the estimation of ⁹⁰Sr in reprocessed uranium oxide samples obtained from the Purex processing of natural uranium spent fuel discharged from the research reactor. The method employs a combination of precipitation and solvent extraction procedure to eliminate other beta-impurities prior to resorting to the estimation of ⁹⁰Sr by beta-counting. ¹⁰⁶Ru was eliminated by volatalizing with perchloric acid, uranium was removed by carrier precipitation with strontium as sulphate. The sulphate precipitate was converted to carbonate and dissolved in nitric acid. ²³⁴Th and ²³⁴Pa were eliminated by synergistic solvent extraction using tri-n-butyl phosphate and thenoyl trifluoroacetone extractant mixture in xylene. An iron scavenging step was included to remove any residual impurities. Finally, strontium is precipitated as SrC₂O₄^. H₂O. The separated ⁹⁰Sr activity was followed to check the equilibrium growth of ⁹⁰Y.     

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.     

Study of HDEHP-PAN solid extractants for the determination of <Superscript>90</Superscript>Sr

Solid extractants containing di-(2-ethylhexyl)phosphoric acid (HDEHP) in the support based on modified polyacrylonitrile (PAN) were studied for the determination of ⁹⁰Sr by means of measuring the activity of its separated ⁹⁰Y daughter. In this paper, ¹⁵²Eu and ¹³³Ba were used as chemical homologues of ⁹⁰Y and ⁹⁰Sr. For these radionuclides, dependences of mass distribution coefficients (D _g) on the nitric acid concentration were measured for several types of HDEHP-PAN solid extractants. The mechanism of the Eu³⁺ and Ba²⁺ ions extraction was confirmed to follow the theoretical two-phase equation for the chelating extractants. Further, the influences of the presence of nitrates, calcium and iron ions on the values of D _g(Ba, Eu) were determined concentrating on the possibility of masking the iron ions by the addition of the ascorbic acid. This method was tested on the solution simulating the leachate of ashed green plant sample. The results obtained make the application of solid extractants containing HDEHP in PAN support prospective for ⁹⁰Sr determination.     

Preparation and quality control and biodistribution studies of [90Y]-DOTA-cetuximab for radioimmunotherapy

Yttrium-90 is a useful radionuclide for radioimmunotherapy (RIT) and the anti-epidermal growth factor receptor (anti-EGFR) antibody cetuximab is clinicsally approved for the treatment of EGFR-expressing metastatic colorectal cancer and advanced head and neck cancer. Thus in this work radiolabeling of monoclonal anti-EGFR with ⁹⁰Y for radioimmunotherapy (RIT) is targetted. Cetuximab was successively labeled with [⁹⁰Y] chloride (74 MBq) 2 mCi after conjugation with macrocyclics bifunctional chelating agent, 1,4,7,10-tetraazacyclododecane-N,N′,N″,N″′-tetraacetic acid mono-(N-hydroxysuccinimidyl) ester (DOTA-NHS), purified and concentrated by centrifugation using an Amicon Ultra-15 filter (Millipore, MWCo, 30000). ⁹⁰Y chloride was obtained by ⁹⁰Sr/⁹⁰Y generator. Radiolabeling was completed in 2 h by the addition of DOTA-cetuximab conjugate at 42 °C. The stability of radiolabeled was studied in human serum. Biodistribution studies in normal rats were carried out to determine the radioimmunoconjugate distribution up to 96 h. Radiochemical purity of 92 % (using ITLC) was obtained for final radioimmunoconjugate (Specific activity = 0.55 GBq/mg). Stability of radiolabeled protein in presence of human serum was tested at 37 °C for up to 24 h. Biodistribution studies demonstrated the highest ID/g % in the blood (2.62 ± 0.005 at 24 h) and the liver (2.19 ± 0.001). This study demonstrated that ⁹⁰Y-DOTA-cetuximab is a potential compound for the treatment of EGFR-expressing cancers.     

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.     

Extraction of Microamounts of Yttrium from Strontium in a Water-Nitrobenzene System

A rapid extraction separation of trace amounts of yttrium from strontium with a nitrobenzene solution of sodium dicarbollylcobaltate (NaDCC) in the presence of polyethylene glycol having mean relative molecular weight 400 (PEG 400) and tetrasodium salt of ethylenediamine-N,N,N,N-tetraacetic acid (Na₄L) in the aqueous phase was developed. The separation factor (Sr/Y) was substantially higher than 10⁶. This water-nitrobenzene extraction system can be applied for the efficient separation of carrier-free ⁹⁰Y from a ⁹⁰Y/⁹⁰Sr generator.     

Variations in the gross alpha and beta activity in surface waters at the Atomic Weapons Establishment Aldermaston (UK)

N,N,N′,N′-tetra-2-ethylhexyldiglycolamide (T2EHDGA) has been used for the preferential extraction of ⁹⁰Y from its mixture with ⁹⁰Sr from HNO₃ as well as HCl medium. The separation efficiencies have been found out under varying experimental conditions. The extracted species were determined from T2EHDGA concentration variation experiments carried out at 3 M nitric acid as well as HCl and were found out to be Y(X₃)₃·3(TEHDGA)_(o) for both the extraction systems, where X = NO₃ ⁻ and Cl⁻, respectively. Comparison of the T2EHDGA and TODGA based separation methods is also made. In order to avoid third phase formation, iso-decanol has been used as the modifier in all the studies. The modifier content was optimized to 30% for 4 M HCl and 20% for 6 M HNO₃ as the feed aqueous phases. Separation schemes were developed for the separation of carrier free ⁹⁰Y and the purity was checked by the half-life measurement method.     

Atmospheric depositional fluxes of cosmogenic <Superscript>32</Superscript>P, <Superscript>33</Superscript>P and <Superscript>7</Superscript>Be in the Sevastopol region

⁹⁰Y was separated from ⁹⁰Sr using an extraction chromatographic resin consisting of 4, 4′(5′)-bis-t-butylcyclohexano-18-crown-6 (DtBuCH₁₈C₆), 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl) amide (C₂mimNTf₂), and a polymer (Amberlite XAD-7). Ionic liquid was introduced into the column to improve the separation efficiency. The column showed an excellent performance for the separation of Y from Sr. After the separation, the ratio of ⁹⁰Sr/⁹⁰Y was <2.0 × 10^?5; the column was recycled for >18 times. This study provides preliminary results on columns to produce ⁹⁰Y with a high purity in radiopharmaceuticals.     

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.     

Extraction chromatographic separation of carrier-free90Y from90Sr/90Y generator by crown ether coated silica gels

A remarkable extraction chromatographic method for the preparation of⁹⁰Y of high radiochemical purity has been developed. The generator consists of silica gel coated crown ether. It functions as a strong adsorber for⁹⁰Sr and in the meantime high purity of⁹⁰Y is eluted with a dilute solution of picric acid after a suitable period. The experiments indicated that DC18C6 coated silica gel is better than that of DB18C6 coated. The extraction capacity of strontium on 3.8% DC18C6 coated silica gel is 5.6 mg Sr/g silica gel. Yttrium is obtained with more than 95% milking yield with radionuclide purity greater than 99.9%. The extraction chromatographic generator does not change its characteristics even after 5 elutions.     

The separation of daughter nuclides from90Sr−90Y and140La−140Ba systems by thin-layer chromatographic methods

The separation of daughter nuclides in the carrier-free state from⁹⁰Sr?⁹⁰Y and¹⁴⁰Ba?¹⁴⁰La aqueous solution systems was performed by thin-layer chromatographic methods. (1) When a silica gel adsorbent and a developer of 1N NaCl, KCl, NH₄Cl, CaCl₂, SrCl₂ or BaCl₂ solutions was employed,⁹⁰Y and¹⁴⁰La were retained at the origin, while⁹⁰Sr and¹⁴⁰Ba advanced with the developer front. Addition of gypsum as binder to the silica gel prevented the separation of the¹⁴⁰Ba?¹⁴⁰La system, retaining both components at the origin. (2) When the¹⁴⁰Ba?¹⁴⁰La system was developed with water on a silica gel adsorbent containing 5% of gypsum, which was treated with various concentrations of nitric acid, the Rf value of¹⁴⁰La increased with the concentration of nitric acid used, reaching a maximum of 0.98 at 0.1 N. The Rf value then decreased on the further increase of the concentration of nitric acid. When the same process was applied to the⁹⁰Sr?⁹⁰Y system, there was no separation. The radiochemical purities of⁹⁰Y and¹⁴⁰La obtained in the above two ways were more than 99%.     

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.     

Rapid determination of strontium-90 in seawater

It is shown that Y₂O₃, YF₃, LaF₃, and CeF₃ help concentrate ⁹⁰Y from seawater. To determine ⁹⁰Sr, YF₃ is the best reagent because the effect of interfering lead and thorium radioisotopes is minimum in this case. It is proposed to preconcentrate ²¹⁰Bi on PbS to eliminate its interference. To determine ⁹⁰Sr we measure the Cherenkov radiation of ⁹⁰Y concentrated on YF₃ without prior elution.     

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.     

A new method for the carrier-free production of 90y from 90sr-90y mixture and 89sr from neutron-irradiated y2o3

The extraction of strontium(II) and yttrium(III) ions from aqueous solutions at various pH values into methyl isobutyl ketone containing I-phenyl-3-methyl-4-caprylpyrazolone-5 is described. Quantitative extraction of Sr and Y at pH 8.6–10 and pH 2.8–5.4 respectively is utilized for the carrier-free production of ⁹⁰Y from ⁹⁰Sr–⁹⁰Y mixtures and ⁸⁹Sr from neutron-irradiated yttrium oxide. A clean separation of these elements from each other and more than 95% calculated activities were recovered     

An electrochemical pathway to prepare circular planar 90Sr/90Y sources for the calibration of surface contamination monitors

In this communication, we describe a novel method to prepare circular planar ⁹⁰Sr/⁹⁰Y sources (? = 16 mm) exploiting the intrinsic properties of the anodized titanium to electro-deposit predicted quantity of ⁹⁰Sr activity from an aqueous solution. The influences of various experimental parameters such as pH of the electrolyte, applied current density, electrodeposition time and carrier strontium concentration were thoroughly investigated to arrive at a condition resulting optimal deposition of the ⁹⁰Sr/⁹⁰Y activity on the substrate. An optimized electrochemical procedure to prepare ~3.7 MBq (~0.1 mCi) of circular planar ⁹⁰Sr/⁹⁰Y sources commensurate with regulatory safety requirement has been the positive outcome.     

Tuning the diglycolamides for modifier-free minor actinide partitioning

The unsymmetrical diglycolamides (DGAs) such as N,N-dihexyl-N′,N′-dioctyl-3-oxapentane-1,5-diamide (DHDODGA), N,N-didecyl-N′,N′-dioctyl-3-oxapentane-1,5-diamide (D²DODGA), N,N-didodecyl-N′,N′-dioctyl-3-oxapentane-1,5-diamide (D³DODGA), were synthesized, and characterized by IR, NMR, and mass spectroscopic techniques. The extraction behaviour of Am(III), Eu(III), and Sr(II) by the solutions of these unsymmetrical DGAs in n-dodecane was studied as a function of concentration of nitric acid and DGA. The distribution ratio of Am(III) and Eu(III) increased with increase in the concentration of nitric acid; whereas, the distribution ratio of Sr(II) reached a maximum at 4 M nitric acid followed by decrease at higher acidities. The extraction of Am(III) and Eu(III) in 0.1 M DGA/n-dodecane decreased in the order DHDODGA > D²DODGA > D³DODGA. However, the order changed upon lowering the concentration of DGA. The third-phase formation behaviour of nitric acid and neodymium(III) in 0.1 M DGA/n-dodecane was studied as a function of concentration of nitric acid. The limiting organic concentration of nitric acid and neodymium increased with increase in the chain length of alkyl group attached to amidic nitrogen. Near stoichiometric amount of neodymium(III) was loaded in 0.1 M D³DODGA/n-dodecane without the formation of third-phase from 3 to 4 M nitric acid medium. The study revealed that the unsymmetrical diglycolamides D²DODGA and D³DODGA are superior candidates for partitioning the minor actinides from high-level liquid waste.     

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.