Field performance test of PASS,an instrument for the rapid assay of plutonium and other γ-ray emitting radionuclides

A field performance test was conducted at the INEL with the mobile Rapid Transuranic Monitoring Laboratory (RTML) that was developed for the analysis of samples from sites or facilities potentially contaminated with plutonium, other actinides, and -ray emitting activation and fission-product radionuclides. The performance test and results are described for the Photon Analysis Spectrometer System (PASS), one of three RTML assay systems. This system consists of a thin-window, n-type Ge spectrometer, that automatically analyzes soil, smear, and air particulate-filter samples for actinides emitting L x rays, and for activation and fission products that emit rays. The measurements were blind and performed with 11-g soil samples gathered from the Cold Test Pit and with spiked samples containing known mixtures of²³⁹Pu,²⁴¹Am⁶⁰Co, and¹³⁷Cs. In the spiked samples the plutonium activity concentrations ranged from 75 to 500 pCi/g while the other radionuclides ranged from 10 to 130 pCi/g. Lower limits of detection (LLDs) were verified to be 1, 5, 5, and 40 pCi/g for²⁴¹Am,⁶⁰Co,¹³⁷Cs, and²³⁹Pu, respectively. Results from the performance test are presented.     

Radionuclide contents in environmental samples as related to the Chernobyl accident

Many kinds of environmental samples including total diet samples, were collected in the Chernobyl (Ukraine) vicinity and in Ibaraki prefecture (Japan). Six radionuclides and twelve stable elements were analyzed. After samples were dry-ashed, radioactivities of¹³⁷Cs,¹³⁴Cs,⁴⁰K,⁶⁰Co and⁵⁴Mn were determined by -ray spectroscopy with a germanium detector. Strontium-90 was determined by low-background -spectrometry. Stable elements were determined by inductively coupled plasma atomic emission spectrometry (ICP-AES). Comparison of the levels of radionuclides between the Ukraine and Ibaraki showed the former were several times to a few tens of thousands of times higher than the latter, depending on the samples.     

Radiochemical determination of Caesium-137, strontium-89,90 and barium-140 in milk and bone ash

Summary A method for the determination of radiocaesium, radiostrontium, radiobarium in milk and bone ash is described. An alkaline fusion of ash followed by leaching with water provides for the preliminary separation of radiocaesium. After dissolution of leaching residue in hydrochloric acid and sorption on Dowex 50 W, X-8, radioyttrium (rare earths fission products), magnesium and calcium are eluted with 1.0 M ammonium lactate, pH 7.5. Radiostrontium, radiobarium and radium are separated by elution with 0.15 M ammonium citrate, pH 7.5. ¹³⁷Cs is isolated as Cs-dipicrylaminate, ⁸⁹Sr/⁹⁰Sr as SrCO₃, ¹⁴⁰Ba as BaCO₃ and counted on a low-background beta-counter. For determined radionuclides the average chemical yields amount to 80%. The limits of detection for ¹³⁷Cs, ⁹⁰Sr, ¹⁴⁰Ba are 0.02 pCi/g with a 10 g sample of milk ash and 0.04 pCi/g with a 4 g sample of bone ash, respectively.

---

Radiochemische Bestimmung von Caesium-137, Strontium-89,90 und Barium-140 in Milch- und Knochenasche

Zusammenfassung Zur Vorabtrennung von Radio-Caesium wird die Ascheprobe alkalisch geschmolzen und dann mit Wasser ausgelaugt. Nach Auflösung des ausgelaugten Rückstandes in Salzsäure und Sorption an Dowex 50 W, X-8 werden Yttrium (Spaltprodukte der Seltenen Erden), Magnesium und Calcium mit 1,0 M Ammoniumlactat, pH 7,5 eluiert. Radio-Strontium, Radio-Barium und Radium werden durch Elution mit 0,15 M Ammoniumcitrat, pH 7,5, abgetrennt. ¹³⁷Cs wird als Cs-Dipikrylaminat isoliert, ⁸⁹Sr/⁹⁰Sr als SrCO₃,¹⁴⁰Ba als BaCO₃; gemessen wird in einem Beta-Antikoincidenzzähler. Für die bestimmten Radio-Nuklide beträgt die durchschnittliche Rückgewinnung 80%. Die unteren Nachweisgrenzen für ¹³⁷Cs, ⁹⁰Sr, ¹⁴⁰Ba betragen bei einer 10 g-Milchasche-Probe 0,02 pCi/g und bei einer 4 g-Knochenasche-Probe 0,04 pCi/g.

     

Matrix materials for proficiency testing: optimization of a procedure for spiking soil with gamma-emitting radionuclides

The IAEA Reference Materials Group of the Chemistry Unit, Agency’s Laboratories Seibersdorf, has developed and optimized a procedure for spiking some environmental matrices with gamma-emitting radionuclides. This paper describes the spiking procedure, homogeneity testing of the spiked material, and assignment of property values and their associated uncertainties for the radionuclides ⁵⁴Mn, ⁶⁵Zn, ⁶⁰Co, ¹⁰⁹Cd, ¹³⁴Cs, ¹³⁷Cs, ²¹⁰Pb, and ²⁴¹Am. This procedure has already been successfully used in an IAEA proficiency test on the determination of ¹³⁷Cs and ²¹⁰Pb in spiked soil and has been found to be appropriate for production of soil materials for proficiency testing and internal quality control samples. The main advantage of this procedure is a low uncertainty arising from heterogeneity, which was found to be less than 1.2% for all the analytes studied.      

Modified and reverse radiometric flow injection analysis

Determination of¹³⁷Cs and⁶⁰Co by using modified and reverse radiometric flow injection analysis is described. Two component RFIA was also realized using⁶⁰Co and¹³⁷Cs radionuclides.     

Sorption of alkaline and alkaline-earth radionuclides on zirconium phosphate sorbent Termoxid-3A from aqueous solutions

Sorption kinetic behavior of¹³⁷Cs,⁸⁵Sr,¹³³Ba and²²³Ra has been studied in the system: inorganic sorbent on the base of zirconium phosphate, Temoxid-3A, and diluted aqeous solutions. Chemosorption mechanism with the limiting step of external diffusion of the reaction between radiostrontium and the sorbent was established (n=1.304±0.0). For barium, radium and cesium radionuclides this mechanism was found to have an ion-exchange character (n<1), with limiting step of external diffusion for barium and radium radionuclides and internal diffusion for radiocesium. Termoxid-3A possesses good sorption kinetic properties. Values of the equilibrium distribution coefficients of the radionuclides studied in the suggested conditions were n·10³. Time for attaining equilibrium does not exeed 40 minutes. Purification coefficient of Moscow potable water from radiostrontium was equal to 100 when 1000 column volumes passed through. Immobilized with strontium sorbent (1.5 mg equiv. of Sr/g sorbent) keeps all its good sorption kinetic characteristics towards radionuclides studied but the mechanism of radiostrontium interaction with the sorbent changes its character from chemosorption to ion exchange (n=0.75).     

Transfer of some selected radionuclides (Cs, Sr, Mn, Co, Zn and Ce) from soil to root vegetables

Transfer of radionuclides from soil to root vegetables (radish, carrot and turnip) has been studied by radiotracer experiments using Andosol, a typical soil type in Japan. The averages of the transfer factors of¹³⁷Cs,⁸⁵Sr,⁶⁰Co,⁵⁴Mn and⁶⁵Zn for edible parts of the three vegetables were 0.02, 0.14, 0.004, 0.09 and 0.13, respectively. The transfer factor of¹⁴¹Ce for the edible part of carrot was 0.0002. The transfer factors obtained for the edible part of root vegetables were markedly lower than those for leaf vegetables.     

A comparative study on environmental radioactivity in shellfish inhabiting the coasts of Korea and Japan

To examine inshore radioactive contamination caused by nuclear power plants, both gross -radioactivity and -spectrometry was measured. The measurements were taken with the sea mussels, Mytilus coruscus and Mytilus edulis, which had been collected from the four different sites of nuclear power plants (Kori, Ulchin, Wolsong, and Younggwang), and Cheju-do as a control site. As a result, the gross -radioactivity observed was similar to that in nature. Among radionuclides, only¹³⁷Cs,²⁰K,⁷Be and⁶⁰Co were detected in a very small amount, and each was also close to the natural levels.     

Radioactivity in the highly contaminated area near the Chernobyl site

Field measurements of radioactivity were performed in highly contaminated areas around Chernobyl in the summer of 1990. Six radionuclides including the most dominant¹³⁷Cs have been identified in soil samples through -ray spectrometry. The relation between the -ray dose rate above the ground and the radioactivity density in soils has been investigated. The external dose from deposited radiocesium for the period of 70 years after the deposition has been evaluated to be about 5 mSv per 1 and 0.5 Ci km^–2 of¹³⁷Cs and¹³⁴Cs deposition, respectively.     

Retention of some radionuclides in furnace lining during incineration of radioactive wastes

The incineration is one of the widely used method for treatment of solid radioactive wastes. The high volume and weight reduction coefficient (100–150 respectively 10–15) are advantages of this method. The greater part of radionuclides from solid radioactive wastes is retained in ash. From point of view of workers external irradiation, the radionuclides accumulation in furnace lining is one of risk factors. The Kalinit O 1200 is furnace lining material on NPPRIs Experimental Incineration facility. In the first step the sorption properties of this material from¹³⁷Cs,⁶⁰Co,⁵⁴Mn,⁶⁵Zn solutions were studied. The best results had⁶⁰Co, its distribution coefficient was 7036 kg · dm^–3. Cesium-137 was not absorbed on this material. The cylinders (height 5 cm, diameter 2 cm) from lining materials were made latest and were applicated inside the furnace and technological tract to study sorption properties from combustion gases. The penetration of radionuclide into lining material was studied too. The results obtained with this experiments are described in this paper.     

Assessment of intake of a complex radionuclide bearing dust formed at a nuclear power plant

The aim of this work was to provide an experimental basis for assessing intakes of an industrial actinide-bearing dust from measurements of⁶⁰Co and¹³⁷Cs in the body or urine. Whilst these radionuclides comprised 72% and 19% of the radioactivity present, greater than 90% of the committed effective dose will result from the low concentrations of the actinides present, 0.4%. To assess the dose coefficient for the dust and predict the biokinetics of⁶⁰Co and¹³⁷Cs in workers, absorption parameters for transfer from lungs to blood obtained from an animal study were combined with information on particle deposition and clearance from the ICRP human respiratory tract model and with tissue distribution and excretion data from the most recent systemic models. All other radionuclides were assumed to have Type M absorption characteristics. The dose coefficient for the dust, 1.29·10^–7 Sv·Bq^–1 was estimated to contain 113 kBq⁶⁰Co, 29 kBq¹³⁷Cs and 0.64 kBq of the actinides. The predicted retention and excretion characteristics of⁶⁰Co and¹³⁷Cs in workers after acute or chronic exposure to the dust suggested that measurements of these radionuclides in the body or urine could detect intakes equivalent to a few percent of an annual dose limit of 20 mSv·y^–1.     

Determination of137Cs and134Cs in air samples collected near Belgrade /Yugoslavia/ following the Chernobyl accident

This paper presents the results of measurements of¹³⁷Cs and¹³⁴Cs content in air sampled during May 1986. Maximum concentrations:¹³⁷Cs 2.94±0.01 Bq m^–3 and¹³⁴Cs 1.38±0.01 Bq m^–3 were registered on May 3. Several other long lived radionuclides having -energies in the region 33 keV to 1365 keV were registered in the same samples two years later. The results of measurements of the total -activity in air for the same period are also presented.     

Natural radionuclides and cesium-137 content in Arabian Gulf bottom sediments

The activity concentration of natural radionuclides and¹³⁷Cs in the bottom sediment samples from the coastal area of Kuwait on the Arabian Gulf have been determined by -ray spectrometry with REGe detector. The data for the samples are very similar to those obtained for surface soil samples in Kuwait.¹ Two parent-progeny ratios for:^23$Th–²²⁶Ra and²²⁸Ac–²⁰⁸Tl to evaluate the geochemical behavior of the radionuclides have been estimated. The existence of a serious disequilibrium between²³⁴Th and²²⁶Ra for samples taken from the vicinity of Kuwait islands and the Ras Al-Zoor area was found. The strait between the coast of Kuwait and Bubiyan island is proposed for the future sedimentation rate determinations on the basis of²¹⁰Pb measurements. No serious contamination by technogenic radionuclides for this region of Arabian Gulf was observed.     

Composite absorbers of inorganic ion-exchangers and polyacrylonitrile binding matrix

Maximum attainable self-absorption dose for cemented composite ion-exchanger, consisting of nickel hexacyanoferrate and polyacrylonitrile binding matrix, loaded with¹³⁷Cs up to repository acceptable level (1.1·10¹² Bq·m^–3) was calculated to be 10⁵ Gy. The cemented absorber with sorbed caesium was irradiated by⁶⁰Co source up to 1 MGy, and leach tests were performed to determine possible influence of self-irradiation on the caesium leachability. No radiation induced changes in caesium immobilisation in solidified ion-exchanger were observed.     

Radiocatalytic H2 production with gamma-irradiation and TiO2 catalysts

The radioactive concentrations of radionuclides were measured in the soil and groundwater below the 12 GeV proton beam-line tunnel at KEK. Various long-lived radionuclides, (⁷Be, ²²Na, ⁴⁶Sc, ⁵⁴Mn, ⁶⁰Co, ¹³⁴Cs, ¹⁵²Eu and ¹⁵⁴Eu) were observed in the soil samples by -ray spectra measurements, and ³H was also detected by liquid scintillation counting. On the other hand, ³H, ²²Na and ⁵⁴Mn, which were leached from the soil were measured in the groundwater below the EP2 beam line. ³H and ²²Na were also found in slight amounts in groundwater collected in a well dug beside the East Counter Hall. From a comparison with the radioactive concentration in soil and groundwater, the order of the leaching percentages were ³H>²²Na>⁵⁴Mn. This tendency was in agreement with an experimental result of the RI laboratory.     

Relativistic perturbation theory of molecular structure

Summary The recently developed relativistic double perturbation theory is extended to handle relativistic changes of molecular structure more easily. This is achieved by simple coordinate scalings. Accurate higher order mixed perturbation energies for H ₂ ⁺ are calculated. The relativistic changes of bond energy,DE, of bond length,R _e , and especially of force constant,k, and of anharmonicity,a, are large, up to 100%·(Z/c)². The dominant contributions tok anda are due to the indirect change of the nonrelativistick anda connected with the relativistic change of bond length. Accordingly the relativistic changes obey Badger's and Gordy's rules (–RDEk).Dedicated to Prof. Klaus Ruedenberg in appreciation of his fundamental contributions to both formal theory and physical explanations in quantum chemistry     

Laboratory standard for radionuclides in nuclear waste

A laboratory standard for the determination of long-lived radionuclides in nuclear waste has been prepared using concrete as matrix. It will be used to check sample preparation procedures, chemical separations and methods for the determination of nuclides, e.g., nuclear counting techniques or mass spectrometry. The material chosen was a fine-grained ready-to-use cement mixture, to which the following radionuclides were added:⁶⁰Co and¹³⁷Cs as -ray-emitting nuclides,⁹⁹Tc,⁹⁰Sr and⁵⁵Fe as radionuclides emitting pure -radiation or low-energy electrons, and²³³U,²³⁷Np,²³⁸Pu and²⁴¹Am as -emitters. Care was taken to attain a homogeneous distribution of the nuclides in the standard material. Pieces of about 1 g were formed as suitable and representative samples. Repeated analyses were carried out with the standard to check its homogeneity. The analytical procedures are described in brief. The pieces of the standard material have the same content of nuclides within ±5% at a 95% level of confidence.     

Distribution of137Cs,40K,238U and232Th in soils from Northern Venezuela

More than one hundred undisturbed soil samples from Northern Venezuela and the islands of Margarita and Los Roques have been analyzed for¹³⁷Cs,⁴⁰K,²³⁸U and²³²Th by -ray spectroscopy. The specimens were taken from between 5–10 cm below the earth's surface. Thus, they are valid not only for the¹³⁷Cs deposition studies but also for the estimation of the natural -ray dose from primordial radionuclides that form the terrestrial component. The concentration of⁴⁰K was directly determined from its 1461 keV -ray, while those of¹³⁷Cs,²³⁸U and²³²Th were performed using a -ray from one of their daughter radionuclides: the 661 keV -ray of^137mBa for¹³⁷Cs, the 1760 keV -ray of²¹⁴Bi for²³⁸U and the 2620 keV -ray of²⁰⁸Tl for²³²Th. Finally, the concentration values were compared with those of global estimates.     

Studies of the vertical distribution of134Cs,137Cs,238Pu,239, 240Pu,241Pu,241Am and210Pb in ombrogenous mires at mid-latitudes

Six peat cores taken from three unmodified blanket and raised bogs in Ireland were sectioned and analyzed for a range of radionuclides including¹³⁴Cs,¹³⁷Cs,²³⁸Pu,²³⁹Pu,²⁴¹Am, and²¹⁰Pb.¹³⁴Cs and¹³⁷Cs were measured by high resolution gamma-spectrometry, while the transuranium nuclides were determined after chemical separation by alpha-spectrometry.²⁴¹Pu, present on the electroplated discs together with Pu(), was measured directly by low-level liquid scintillation counting. Core chronologies were established by measuring the unsupported²¹⁰Pb component using low energy photon spectrometry (LEPS). From the resulting profiles, relaxation depths and migration rates for the above mentioned radionuclides have been determined and differences in the values of these parameters interpreted.²³⁸Pu/^239,240Pu and²⁴¹Pu/^239,240Pu ratios have been examined carefully and are discussed in some detail. Finally, the contribution from Chernobyl to the total radiocaesium inventory in each core has been established using the¹³⁴Cs/¹³⁷Cs ratio observed in the initial fallout from Chernobyl.     

Monitoring of environmental radiation on the Spratly Islets in the South China Sea

The concentration of radionuclides in environmental samples and the environmental radiation level (including cosmic rays) was monitored on Spratly Islets in South China Sea prior to the commercial operation of nearby Chinese nuclear power plants. Samples of coral sand, sea food, vegetation, water, and accumulated fallout on the islet were obtained and measured for radioactivity. Except for some exposure originating from minute amounts of⁶⁰Co and¹³⁷Cs, the radiation background is mainly emitted from naturally occurring radionuclides. Radiation levels including beta, gamma, and neutron on the islet have also monitored. Gamma dose rates for outdoor exposure averaged approximately 0.09 Sv/h; the neutron dose rate was about 0.003 Sv/h. Automatic radiation surveillance and a routine sampling program on the Spratly Islets are viewed as essential to provide an early warning in the Far East in case of a nuclear emergency.