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     

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%.     

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

A rapid separation for carrier-free ⁹⁰Y in the aqueous phase of the water/nitrobenzene extraction system from an ⁹⁰Y/⁹⁰Sr generator was proposed. After two-stage extraction separation, chemical yield of ⁹⁰Y in the final aqueous phase was roughly 80%, while ⁹⁰Sr radionuclide impurity in this phase containing carrier-free ⁹⁰Y was 10^-6%.     

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.     

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.     

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.     

Studies on Separation of 90Y and 90Sr Separation from Hydrochloric Acid Solutions Using TODGA as the Extractant by SLM Method

Yttrium-90 is an important radionuclide known for its therapeutic application in nuclear medicine. Solvent extraction studies with N,N,N’,N’-tetra-octyldiglycolamide (TODGA) has shown that Y(III) is well extracted in 6 M HCl while at the same time, extraction of Sr(II) is very low leading to a separation factor (DY/DSr = 60,000). This property of TODGA can be exploited for the separation of Y from Sr. The aim of this present work is to produce carrier free ⁹⁰Y by using Supported Liquid Membrane (SLM) based separation of Y and Sr with TODGA as the carrier. Solvent extraction studies with various diluents viz. 1-decanol, xylene, MIBK, chloroform etc. indicated that xylene and n-dodecane are most suitable as S.F. >50,000 are obtained. Based on the results, a SLM based separation scheme was developed using 0.1 M TODGA in xylene loaded on a microporous PTFE membrane as a polymeric support and 6 M HCl as feed and 0.01 M HCl as strip phase. The results appear promising for the development of SLM based Y-90 generator. The purity of the product was ascertained by the half life method.     

Quinolinephosphomolybdate as ion exchanger: synthesis,characterization, and application in separation of <Superscript>90</Superscript>Y from <Superscript>90</Superscript>Sr

An inorganic ion exchanger, quinolinephosphomolybdate has been synthesized and characterized by elemental analysis, infrared (IR) and X-ray diffraction (XRD) spectroscopy. This compound is highly stable toward thermal, chemical and radiation dose. This has been employed in the separation of carrier-free ⁹⁰Y from its parent ⁹⁰Sr from an equilibrium mixture. The absorbed daughter was recovered by using 0.0284 mol L⁻¹ ascorbic acid solutions at pH 5.0 as eluting agent.     

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.     

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 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.     

Diffusion dialysis aided electrodialysis process for concentration of radionuclides in acid medium

A study on the separation of the long-lived heat generating fission products¹³⁷Cs and⁹⁰Sr from acidic solutions has been carried out using a specially fabricated electrodialytic cell equipped with a pair of cation and anion exchange membranes forming a catholyte and anolyte, respectively, and a radioactive feed chamber. The studies were done with feed solutions containing different concentrations of Na⁺, Cs⁺ and Sr²⁺ individually and with a mixture of these cations in 0.3 M HNO₃. In all the cases, the transfer of Cs and Sr was found to be greater than 90%. To facilitate the separation of the above radionuclides from higher acidity (∼3.0M HNO₃), diffusion dialysis was taken as a possible pretreatment step using a two compartment diffusion cell with an anion exchange membrane in between. All the experiments were done under non-stirring mode.     

Separation of carrier-free 90Y from 90Sr using flat sheet supported liquid membranes containing multiple diglycolamide-functionalized calix[4]arenes

Abstract

Five diglycolamide-appended calix[4]arene (C4DGA) ligands, viz. C4DGA with no substituent (L-I), n-propyl (L-II), 3-pentyl (L-III), n-octyl (L-IV) and both side (L-V) substituents were evaluated for the separation of carrier free ⁹⁰Y from a ⁹⁰Y–⁹⁰Sr mixture using the flat sheet supported liquid membrane technique. Based on the results of earlier batch studies, the transport properties of the C4DGA ligands towards Y(III) and Sr(II) were monitored at two different feed acidities. The transport rates were significantly lower for 6 M HNO₃ as compared to 3 M HNO₃ as the feed. After 6 h, the observed trend of Y(III) transport with the C4DGA ligands using a feed of 3 M HNO₃ was: L-I ~ L-III > L-V > L-IV > L-II which changed to L-III > L-I > L-IV > L-V > L-II for 6 M HNO₃ as the feed. With 3 M HNO₃ as feed, >97% Y(III) transport was obtained with L-I and L-III in 6 h. Comparative Sr(II) transport was negligible resulting in high decontamination factors. In a one-step separation process, using L-I as the carrier ligand, pure ⁹⁰Y was obtained as the respective complex with either EDTA or DOTA. The highlights of this liquid membrane-based separation method comprise: its easiness, one-step separation, low ligand inventory, relatively pure product and continuous method.     

A simple and quick method for the preparation of radionuclide <Superscript>87</Superscript>Y/<Superscript>87m</Superscript>Sr generator using the <Superscript>nat</Superscript>Rb(α,xn)<Superscript>87</Superscript>Y reaction

A rapid method for the preparation of ⁸⁷Y/^87mSr radionuclide generator from a rubidium chloride target irradiated with 35 MeV α-particles is described. A simple two-step procedure is used to obtain a carrier-free ^87mSr isotope with a high enough radiochemical yield and high purity in the final aqueous fraction.     

Investigation and characterization of PVA-g-AAc/Zol membranes for possible practical use in separation processes

Poly(vinyl alcohol) films were grafted with two monomers (acrylic acid and N-vinyl imidazole) using the gamma irradiation technique. The melting temperature (T_m) and glass transition temperature (T_g) of the grafted membranes were determined with respect to the grafting yield. The ability of these membranes to separate cobalt from nickel has been investigated. The diffusion of cobalt and nickel ions from the feed compartment to the receiver compartment depends on the grafting yield and the pH of the feed solution. Cobalt ions do not diffuse through the membrane when the pH of the feed solution is >4.5. Thus, the prepared membranes could be considered for the separation of cobalt ions from nickel ions. The temperature of thermal decomposition of pure PVA-g-AAc/Zol membrane, PVA-g-AAc/Zol membranes containing cobalt ions, and PVA-g-AAc/Zol membranes containing nickel ions are determined using TGA analyzer; it was shown that the presence of cobalt and nickel increases the decomposition temperature. Also the membranes bonded with cobalt ions are more stable than the membranes containing nickel ions.     

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.     

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.     

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.     

Prompt gamma activation analysis (PGAA) and short-lived neutron activation analysis (NAA) applied to the characterization of legacy materials

The ⁹⁰YCl₃ radionuclide precursor (solution of ⁹⁰Y³⁺ in diluted HCl) of high purity and high specific activity is already commercially produced and successfully used in nuclear medicine. At the Nuclear Physics Institute ASCR, the ⁹⁰YCl₃ radionuclide precursor is prepared using extraction ⁹⁰Sr/⁹⁰Y generator (technology of centrifuge extractors with di-2-ethylhexylphosphoric acid, D2EHPA).¹ Its radionuclidic, radiochemical, and chemical purity were examined and specified. The procedure developed for labeling of DOTA-Tyr³-octreotide (DOTATOC) with carrier-free ^86/90Y by Rösch ² at the Institute of Nuclear Chemistry of the University Mainz was optimized and modified in our Department of Radiopharmaceuticals at NPI ASCR as standard labeling test (SLT) for analytical purposes. The SLT as a method for ⁹⁰YCl₃ radionuclide precursor quality control determining its labeling efficiency using ITLC SG chromatography is described and proposed thereinafter. The labeling-efficiency of the tested batches of our product reached more than 95%.     

Dünnschichtchromatographie an Salzen von Heteropolysäuren

Zusammenfassung In Fortsetzung einer früheren Arbeit wurde die Verwendbarkeit von Ammoniumphosphordodekamolybdat (APM), Ammoniumgermanododekamolybdat (AGM), Oxingermanododekamolybdat (OGM), Pyridingermanododekamolybdat (PGM), Oxinsilicododekamolybdat (OSM) und Pyridinsilicododekamolybdat (PSM) für Dünnschichtchromatographie untersucht und die Abhängigkeit derR _f -Werte der Alkalimetallionen von der Laufmittelkonzentration (Ammoniumnitrat und Wasser) bestimmt. Gleichzeitig wurden Vorversuche angestellt, eine spezifische Abtrennung des Cäsiums von den Spaltprodukten⁹⁵Zr/⁹⁵Nb,¹⁰⁶Ru,⁹⁰Sr/⁹⁰Y und¹⁴⁴Ce durchzuführen.

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Summary As continuation of an earlier study, ammonium phosphododeoa molybdate (APM), ammonium germanododecamolybdate (AGM), oxinegerdodecamolybdate (OGM), pyridinegermanododecamolybdate (PGM), oxininesilicododecamolybdate (OSM), and pyridinesilicododecamolybdate (PSM) were investigated for thin layer chromatography and the relation of theR _f -values of the alkali metal ions to the concentration of the carrier concentration (ammonium nitrate and water) was determined. At the same time, preliminary studies were made with respect to a specific separation of cesium from the fission products⁹⁵Zr/⁹⁵Nb,¹⁰⁶Ru,⁹⁰Sr/⁹⁰Y and¹⁴⁴Ce.

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Résumé Comme suite à une publication antérieure, on a étudié les possibilités d'application en chromatographie en couche mince du phosphododécamolybdate d'ammonium (APM), du germanidodécamolybdate d'ammonium (AGM), du germanidodécamolybdate d'oxinium (OGM), du germanidodécamolybdate de pyridinium (PGM), du silicomolybdate d'oxinium (OSM) et du silicododécamolybdate de pyridinium, en déterminant la dépendance des valeurs duR _f des ions métalliques alcalins avec la concentration de l'éluant (nitrate d'ammonium et eau). On a commencé simultanément l'étude de la séparation spécifique du césium d'avec les produits de fission⁹⁵Zr/⁹⁵Nb,¹⁰⁶Ru,⁹⁰Sr/⁹⁰Y et¹⁴⁴Ce.

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Herrn Prof. Dr.A. A. Benedetti-Pichler mit herzlichen Wünschen zum 70. Geburtstag gewidmet.