A neutron monitor for in-situ real-time determination of transuranics in a processed waste effluent stream

A pilot plant operation at the Savannah River Site will remove ⁹⁰Sr, ¹³⁷Cs, and transuranics from a high-level liquid waste stream prior to encapsulation in a Saltstone Facility. Monitors are required to determine the concentrations of all radionuclides, including transuranics, in real-time on this processed waste stream. A neutron counter used to measure the concentration of each actinide isotope present in the stream is described. The neutron counter assembly consists of nested annular layers of shielding, reflectors, detectors, and moderators. On-line, live-time system control and calibration is provided by a time-tagged neutron source embedded in the moderator assembly.     

Development of field portable sampling and analysis systems

A portable, field rugged, sampling and analysis system has been developed for the rapid screening of aqueous samples during scoping and remediation studies. Using field portable equipment, water is pumped through ion selective solid phase extraction (SPE) disks, at a flow rate of 150-250 ml/min, and counted for the radionuclide of interest in the field using portable detectors. SPE disks are currently available to selectively concentrate ⁹⁹Tc, ⁹⁰Sr, radiocesium (¹³⁴Cs and ¹³⁷Cs) and radium isotopes. In the field the radiocesium concentration is determined by gamma-spectrometry, ⁹⁰Sr and ⁹⁹Tc are determined by beta-counting. A one-liter sample can be processed and ready for counting within ten minutes. Using a 5-minute counting time, a detection limit of <50 pCi/l for ⁹⁹Tc or ⁹⁰Sr and ~50 pCi/l for ¹³⁷Cs has been achieved. Up to 10 liters of water have been processed for the analysis of ⁹⁹Tc and ¹³⁷Cs when lower limits of detection were required. The sampling and analysis system has been field tested at the Savannah River Site (SRS), Aiken SC, and the Hanford Site, Richland WA. The SRS H-area tank farm storm water runoff system was analyzed for ⁹⁰Sr and ¹³⁷Cs. Groundwater from the SX tank farm at the Hanford Site was analyzed for ¹³⁷Cs and ⁹⁹Tc. Groundwater from seeps below the 100-H area at Hanford was analyzed for ⁹⁰Sr and ⁹⁹Tc.     

Synthesis and characterization of Nb–Ge doped titanosilicate nanoparticles and study of their selectivity for absorption of 137Cs and 90Sr

In this research, for the first time Nb and Ge were doped into titanosilicate nanoparticles up to 25% simultaneously. Crystalline phases and morphology of the synthesized samples were studied by X-ray diffraction (XRD) method and scanning electron microscope (SEM), respectively. Elemental analysis of the samples was performed using X-ray fluorescence (XRF) and Energy dispersive X-ray (EDX) techniques. Surface area of the samples was measured by BET method. Ion exchange potential of the synthesized samples for Sr²⁺ and Cs⁺ and effective parameters such as concentration, temperature, time, and pH were investigated. In addition,¹³⁷Cs and ⁹⁰Sr radio nuclides absorption in the best appropriate sample was examined. The selectivity of the samples for absorption of ¹³⁷Cs and ⁹⁰Sr was studied by gamma spectroscopy, liquid scintillation spectrometry, and atomic absorption spectroscopy methods. The obtained results showed that the prepared samples had good potential for absorption of ¹³⁷Cs and ⁹⁰Sr from the model solution. The sample containing equal amount of niobium and germanium, removed completely the ¹³⁷Cs within the waste water of Tehran nuclear reactor and ⁹⁰Sr in the desired solution.     

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

The concentrations of¹³⁷Cs were determined by in 11 sediment samples, collected along the Romanian sector of the Danube river and the Black Sea coast during 1994 γ-ray spectrometry. The concentrations of⁹⁰Sr in the same sediment samples were determined by β-counting of the⁹⁰Y oxalate, precipitated after strontium separation using a strontium extraction chromatography column. The concentration distributions of¹³⁷Cs and⁹⁰Sr are compared with the²³⁸Pu and^239,240Pu concentration distributions in the same samples, reported in a previous paper. The accumulation potential of¹³⁷Cs,⁹⁰Sr and plutonium isotopes in the river and sea sediments analysed is discussed.     

Determination of137Cs,90Sr and fallout Pu in the volcanic soil of Korea

The cumulative depositions of¹³⁷Cs,⁹⁰Sr and fallout Pu in the volcanic ash soil of Korea were determined. The average accumulated depositions of¹³⁷Cs,⁹⁰Sr and fallout Pu in the volcanic soil were much higher than those in other forest sites of Korea. From depth profiles, it was found that¹³⁷Cs,⁹⁰Sr and^239,240Pu in the volcanic soil are more mobile than those in other forest sites of Korea, and that the downward movement of⁹⁰Sr is faster than¹³⁷Cs and^239,240Pu. A significant correlation was found between the concentration of¹³⁷Cs and those of⁹⁰Sr and^239,240Pu. The activity ratios of²³⁸Pu/^239,240Pu and²⁴¹Pu/^239,240Pu in soils are close to those observed in the cumulative deposit from the global fallout of nuclear weapon testings.     

Migration processes of <Superscript>137</Superscript>Cs and <Superscript>90</Superscript>Sr in compartments of a lake ecosystem

Summary The dispersion of radioactive substances in the environment following nuclear weapon tests in atmosphere since 1954 and accidents to nuclear plants, like that in Chernobyl in 1986, have allowed us to study the migration processes of some radionuclides in complex ecosystems such as lakes are. In the present paper the behavior of ¹³⁷Cs and ⁹⁰Sr in different compartments of the Monterosi Lake (central Italy) was assessed. The ¹³⁷Cs concentration was measured in lake water as well as sediment, stream water, aquatic plant and fish samples. ⁹⁰Sr concentration in water and sediments was also determined. A total inventory of 4206±76 Bq ^. m^-2 and 958±79 Bq ^. m^-2 (on 27/6/01) has been found for ¹³⁷Cs and ⁹⁰Sr, respectively. The experimental data presented here allow to calibrate theoretical models predicting the temporal trend of radionuclide concentration in similar ecosystems. Moreover, information on cesium and strontium migration processes can be extended to other pollutants having similar environmental behavior.     

Uptake of cesium and strontium by crystalline silicotitanates from radioactive wastes

Crystalline silicotitanate inorganic ion exchanger, with a sitinakite structure is candidate material for remediation of aqueous nuclear waste streams. The syntheses of crystalline silicotitanate (CST) and Nb-substituted crystalline silcotitanate (Nb-CST) were carried out under hydrothermal conditions and the products were characterized using techniques viz., XRD, SEM/EDS, DTA/TGA, surface area respectively. Batch experiments were carried out to study the kinetics of uptake of ¹³⁷Cs and ⁹⁰Sr, to estimate the decontamination factor (DF) values and distribution coefficients (K _d) for the above synthesized CST and Nb-CST samples from actual radioactive waste solutions. The DF values for uptake of Cs and Sr by Nb-CST after 24 h of equilibration was 355 and 136 whereas for CST it was found to be 40 and 176 respectively. The K _d values for uptake of Cs and Sr for Nb-CST after 24 h of equilibration was found to be 35,490 and 13,500 mL/g respectively whereas the K _d values for uptake of Cs and Sr for CST was found to be 4,025 and 17,525 mL/g respectively. The ion exchange capacity of Nb-CST towards ⁹⁰Sr and ¹³⁷Cs was estimated to be 11.8 and 3.2 meq/g respectively whereas the ion exchange capacity of CST towards ⁹⁰Sr and ¹³⁷Cs was estimated to be 14.6 and 4.4 meq/g respectively.     

Determination of radioactive pollution from an open landfill

Summary This paper presents a case study of radioactive pollution of groundwater caused by leachate from an open landfill. Alpha- and beta-radioactivity analysis of the leachate from different points in the region and associated fountain water from a village down stream were carried out during four seasons. The alpha- and beta-radioactivity concentrations were under the detection limit in all samples and ranged between 0.07 and 2.17 Bq/l, respectively. The beta-radioactivity concentration from ¹²⁹I, ¹³⁷Cs and ⁹⁰Sr individual radioisotopes were determined and their annual effective dose was calculated.     

The Effect of Carbonate Soil on Transport and Dose Estimates for Long-Lived Radionuclides at a U.S. Pacific Test Site

The United States conducted a series of nuclear tests from 1946 to 1958 at Bikini, a coral atoll, in the Marshall Islands (MI). The aquatic and terrestrial environments of the atoll are still contaminated with several long-lived radionuclides that were generated during testing. The four major radionuclides found in terrestrial plants and soils are cesium-137, strontium-90, plutonium-239+240 and americium-241. Cesium-137 in the coral soils is more available for uptake by plants than ¹³⁷Cs associated with continental soils of North America or Europe. Soil-to-plant ¹³⁷Cs median concentration ratios (CR) (kBq·kg^-1 dry weight plant/kBq·kg^-1 dry weight soil) for tropical fruits and vegetables range between 0.8 and 36, much larger than the range of 0.005 to 0.5 reported for vegetation in temperate zones. Conversely, ⁹⁰Sr median CRs range from 0.006 to 1.0 at the atoll versus a range from 0.02 to 3.0 for continental silica-based soils. Thus, the relative uptake of ¹³⁷Cs and ⁹⁰Sr by plants in carbonate soils is reversed from that observed in silica-based soils. The CRs for ^239+240Pu and ²⁴¹Am are very similar to those observed in continental soils. Values range from 10^-6 to 10^-4 for both ^239+240Pu and ²⁴¹Am. No significant difference is observed between the two in coral soil. The uptake of ¹³⁷Cs by plants is enhanced because of the absence of mineral binding sites and the low concentration of potassium in the coral soil. Cesium-137 is bound to the organic fraction of the soil, whereas ⁹⁰Sr, ^239+240Pu and ²⁴¹Am are primarily bound to soil particles. Assessment of plant uptake for ¹³⁷Cs and ⁹⁰Sr into locally grown food crops was a major contributing factor in: (1) reliably predicting the radiological dose for returning residents and (2) developing a strategy to limit the availability and uptake of ¹³⁷Cs into locally grown food crops.     

Determination of long-lived fission products and actinides in Savannah River Site HLW sludge and glass for waste acceptance

Savannah River Site (SRS) is immobilizing the radioactive, high-level waste sludge in Tank 51 into a borosilicate glass for disposal in a geologic repository. A requirement for repository aceeptance is that SRS report the concentrations of certain fission product and actinide radionuclides in the glass. This paper presents measurements of many of these concentrations in both Tank 51 sludge and the final glass. The radionuclides were measured by inductively coupled plasma mass spectrometry and α, β, and γ counting methods. Examples of the radionuclides are⁹⁰Sr,¹³⁷Cs,²³⁸U and,²³⁹Pu. Concentrations in the glass are 3.1 times lower due to dilution of the sludge with a nonradio-active glass forming frit in the vitrification process. Results also indicated that in both the sludge and glass the relative concentrations of the long lived fission products insoluble in caustic are in proportion to their yields from the fission of²³⁵U waste in the SRS reactors. This allowed the calculation of a fission yield scaling factor. This factor in addition to the sludge dilution factor can be used to estimate concentrations of waste acceptance radionuclides that cannot be measured in the glass. Examples of these radionuclides are⁷⁹Se,⁹³Zr, and¹⁰⁷Pd.     

Determination of137Cs and90Sr in milk by the static method with an ion exchanger

This paper presents the method of⁹⁰Sr and¹³⁷Cs determination from 10 litres of milk. The preconcentration is made by the static method with a strong acid cation exchanger (OSTION KS).¹³⁷Cs from the eluent (8M HCl) is selectively eliminated with ammonium molybdophosphate and then the^137mBa gamma activity measured, using NaI(T1) detector.⁹⁰Sr as⁹⁰Y is determined after achievement of the radioactive equilibrium and measured by flow proportional counter. The method appears to be accurate, reproducible and permits to determine³² mBq¹³⁷Cs and 13 mBq⁹⁰Sr in the samples.     

Determination of90Sr and137Cs in mushrooms following the Chernobyl fallout

After the Chernobyl accident high concentrations of radionuclides were found in Sweden in mushrooms and the contents of⁹⁰Sr and¹³⁷Cs were measured. The level of⁹⁰Sr was generally low and, in proportion to¹³⁷Cs, 2–3 orders of magnitude lower than in the fallut. The contents of¹³⁷Cs varied among species and extreme local variations occurred. The ratio¹³⁴Cs/¹³⁷Cs diverged from other biological samples leading to the conclusion that old fallout was involved in the uptake.     

Analysis of 99Tc in the radioactive liquid waste after extraction into suitable solvent

⁹⁹Tc is one of the long lived fission product with high fission yield. From radioactive waste management point of view it is very much essential to evaluate the concentration of technetium in the radioactive liquid waste in order to finalise the treatment process to extract/isolate it from the stream which is discharged to the environment. For the estimation of ⁹⁹Tc in the radioactive liquid waste stream, extraction of the stable complex of technetium-tetraphenyl arsonium chloride (TPAC) into chloroform followed by beta counting was studied. Various parameters like pH, time of equilibration, concentration of TPAC in chloroform, use of other solvent for extraction as well as interference of various other radionuclides present in the waste were also studied. The radioactive liquid waste being handled in plant contains high concentrations of salts in the form of sodium nitrate. Hence effect of salt concentration on the percentage extraction was also evaluated. The extraction behavior does not dependent on change in the pH of the solution. Almost 99.5% extraction was observed in the pH range of 1?C13.0. High concentration of salt is affecting the extraction. However, this can be taken care by diluting the radioactive waste. It takes almost 90?min time for maximum extraction. Presence of radionuclides like ¹³⁷Cs, ⁹⁰Sr are not interfering the extraction of ⁹⁹Tc. However, ¹⁰⁶Ru is getting slightly extracted along with ⁹⁹Tc. The error due to ¹⁰⁶Ru can be eliminated by taking gamma spectrum and deducting the activity from the total beta activity to get ⁹⁹Tc activity. Nitrobenzene can be used for extraction of Tc?CTPAC complex in place of chloroform.     

Rapid determination of 89Sr and 90Sr in radioactive waste using Sr extraction disk and beta-ray spectrometer

A rapid determination method in which beta-ray spectrometry was combined with solid phase extraction using Sr Rad Disk was developed for the determination of ⁸⁹Sr and ⁹⁰Sr in low-level radioactive waste. Various amounts of ⁸⁹Sr, ⁹⁰Sr, and ⁹⁰Y retained by the Sr Rad Disk was measured by a beta-ray spectrometer, and it was found that both ⁸⁹Sr and ⁹⁰Sr were simultaneously determined with <30% error (2σ) at ⁸⁹Sr/⁹⁰Sr radioactivity ratio of 0.3 to 45. The present method was successfully applied to actual radioactive liquid waste samples arising from nuclear facilities in Japan Atomic Energy Agency. Strontium was simply separated from interfering nuclides such as ¹³⁷Cs and ¹⁵⁴Eu, and matrix components by the Sr Rad Disk, and the results obtained by beta-ray spectrometry was in good agreement with that of the conventional analysis.     

Physical and chemical investigation of water and sediment of the Keban Dam Lake, Turkey:

Summary The gross alpha- gross beta-activity, ¹³⁷Cs and ⁹⁰Sr in the water and sediment samples taken from the Keban Dam Lake, Uluova Region, was investigated in 2003 and 2004. We have found that in spring the concentration of ¹³⁷Cs in the surface water and deep sediment changed between 0.001-0.01 Bq/l (0.4-2.5 Bq^.kg^-1) that of ⁹⁰Sr between 0.0001-0.009 Bq/l (0.1-9 Bq^.kg^-1) and in autumn the values were 0.0001-0.009 Bq/l (0.4-8 Bq^.kg^-1) for ¹³⁷Cs and 0.0002-0.005 Bq/l (0.6-4 Bq^.kg^-1) for ⁹⁰Sr, respectively. The results were presented in form of iso-curves.     

Plutonium measurements in Hanford DOE site waste samples

This paper describes development work to prepare a method to measure absolute²³⁹Pu content and Pu-isotopics by ICP-MS in acidified Hanford DOE-site samples which are very high in⁹⁰Sr,⁹⁹Tc, and¹³⁷Cs radioactivity and which are frequently high in organic carbon content. Samples with very large⁹⁰Sr and¹³⁷Cs contents have historically been difficult to analyze for Pu content by each of three alpha-counting techniques in use at SRS, and analysis by ICP-MS in these samples is complicated by the high organics content. We report an ion exchange chemical preparation to obtain fraction of Pu that does not contain any fission product contribution and no interfering organics to allow measure of absolute²³⁹Pu and of²³⁹Pu through²⁴¹Pu isotopics by ICP-MS. The method uses a²⁴²Pu spike to measure Pu recovery and is demonstrated in this paper with three distinct commercially available resins and with over 300 samples. Measured absolute²³⁹Pu contents in sixty-three spiked/unspiked duplicates have agreed within 15% precision. Overall²⁴²Pu recoveries were near 90% with 25% precision. Comparisons of absolute²³⁹Pu contents measured directly on three samples agreed within the quoted 25% uncertainty.     

Depth distribution of137cesium,90strontium and210lead in sediments of lake Mondsee,Austria

¹³⁷Cs,⁹⁰Sr and²¹⁰Pb were determined in sediment cores from lake Mondsee /Austria/. The depth profiles show that¹³⁷Cs remains undisturbed, i.e. its distribution corresponds to the fallout deposition pattern.⁹⁰Sr, however, has been transported into the upper sediment layers. In this upper zone nearly constant levels of⁹⁰Sr and also of²¹⁰Pb/²¹⁰Po/were found. Comparison of the⁹⁰Sr and¹³⁷Cs profiles indicates that chemical processes must be responsible for the translocation of⁹⁰Sr as well as²¹⁰Pb, and not bioturbation, i.e. mixing of upper sediment layers by benthic organisms.Dedicated to Prof. Dr. Karl Schlögl, University of Vienna, for his 60th birthday.     

The transfer of natural (226Ra,?232Th, 40K) and artificial (137Cs, 90Sr) radionuclides from soil to the wood of a Scots pine (Pinus sylvestris L.)

On the Stabatishke site near to Ignalina Nuclear Power Plant a near surface repository for low and intermediate-level short-lived radioactive waste is being constructed to store the waste which was produced during the decommissioning of the Ignalina Nuclear Power Plant. A possible spread of radionuclides from the near surface repository and the radiation level of expression are one at the most important aspects while evaluating the safety of the repository. The article examines the specific activity of artificial (¹³⁷Cs, ⁹⁰Sr) and natural (²²⁶Ra, ²³²Th, ⁴⁰K) radionuclides in the soil of Stabatishke site of Ignalina NPP in pinewood; the spread of these radionuclides is determined in the system “soil-tree”. The change of long term soil pollution with artificial radionuclides was estimated. This is a background soil pollution which had been there before the exploitation of the near surface waste repository. The transfer factors of natural (²²⁶Ra, ²³²Th, ⁴⁰K) and artificial (¹³⁷Cs, ⁹⁰Sr) radionuclides from the 0-to-20-cm soil layer to different annual pinewood rings were measured. After estimation of the position of pine roots in accordance to the soil vertical and the annual change of the plant biomass, the transfer factor of ¹³⁷Cs movement to different annual pinewood rings from the separate 0 to 20-cm soil layers was determined.     

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.     

Separation of137Cs and90Sr from mineralizates of biological materials by dicarbolide of cobalt

The distribution of some radionuclides in the course of¹³⁷Cs and⁹⁰Sr extraction and scrubbing between organic and water phase was determined.¹³⁷Cs and⁹⁰Sr were isolated from the mixture of radionuclides in mineralized biological materials. Dicarbolide of cobalt i. e. 3,3′-commo-bis[undecahydro-1,2-dicarbo-3-closo-dodecaborate] was used as an extracting agent. Quantities of the extracted radionuclides were determined by gamma spectrometric technique. Single and repeated extraction of⁹⁰Sr with 0.01M resp. 0.1M dicarbolide of cobalt in nitrobenzene and scrubbing of coextracted radionuclides by 0.5M HNO₃ were studied. The extraction of⁹⁰Sr was investigated from solutions of a hydrofobizing agent in the same way. Finally, the quantitative extraction of¹³⁷Cs followed by the extraction of⁹⁰Sr from mixtures of radionuclides in a mineralized biological material was studied. Extraction yields from dry and wet mineralizates of biological tissues, from urine and milk were compared. Suitable working conditions for the separation procedures were selected.