Reference material for radionuclides in sediment IAEA-384 (Fangataufa Lagoon sediment)

A reference material designed for the determination of anthropogenic and natural radionuclides in sediment, IAEA-384 (Fangataufa Lagoon sediment), is described and the results of certification are presented. The material has been certified for 8 radionuclides (⁴⁰K, ⁶⁰Co, ¹⁵⁵Eu, ²³⁰Th, ²³⁸U, ²³⁸Pu, ^239+240Pu and ²⁴¹Am). Information values are given for 12 radionuclides (⁹⁰Sr, ¹³⁷Cs, ²¹⁰Pb (²¹⁰Po), ²²⁶Ra, ²²⁸Ra, ²³²Th, ²³⁴U, ²³⁵U, ²³⁹Pu, ²⁴⁰Pu and ²⁴¹Pu). Less reported radionuclides include ²²⁸Th, ²³⁶U, ²³⁹Np and ²⁴²Pu. The reference material may be used for quality management of radioanalytical laboratories engaged in the analysis of radionuclides in the environment, as well as for the development and validation of analytical methods and for training purposes. The material is available from IAEA in 100 g units. Retired from IAEA in 2003.     

A certified reference material for radionuclides in the water sample from Irish Sea (IAEA-443)

A new certified reference material (CRM) for radionuclides in sea water from the Irish sea (IAEA-443) is described and the results of the certification process are presented. Ten radionuclides (³H, ⁴⁰K, ⁹⁰Sr, ¹³⁷Cs, ²³⁴U, ²³⁵U, ²³⁸U, ²³⁸Pu, ^239+240Pu and ²⁴¹Am) have been certified, and information values on massic activities with 95% confidence intervals are given for four radionuclides (²³⁰Th, ²³²Th, ²³⁹Pu and ²⁴⁰Pu). Results for less frequently reported radionuclides (⁹⁹Tc, ²²⁸Th, ²³⁷Np and ²⁴¹Pu) are also reported. The CRM can be used for quality assurance/quality control of the analysis of radionuclides in water samples, for the development and validation of analytical methods and for training purposes. The material is available in 5 L units from IAEA (http://nucleus.iaea.org/rpst/index.htm).     

The NIST natural-matrix radionuclide standard reference material program for ocean studies

In 1977, the Low-level Working Group of the International Committee on Radionuclide Metrology met in Boston, MA (USA) to define the characteristics of a new set of environmental radioactivity reference materials. These reference materials were to provide the radiochemist with the same analytical challenges faced when assaying environmental samples. It was decided that radionuclide bearing natural materials should be collected from sites where there had been sufficient time for natural processes to redistribute the various chemically different species of the radionuclides. Over the succeeding years, the National Institute of Standards and Technology (NIST), in cooperation with other highly experienced laboratories, certified and issued a number of these as low-level radioactivity Standard Reference Materials (SRMs) for fission and activation product and actinide concentrations. The experience of certifying these SRMs has given NIST the opportunity to compare radioanalytical methods and learn of their limitations. NIST convened an international workshop in 1994 to define the natural-matrix radionuclide SRM needs for ocean studies. The highest priorities proposed at the workshop were for sediment, shellfish, seaweed, fish flesh and water matrix SRMs certified for mBq per sample concentrations of ⁹⁰ Sr, ¹³⁷ Cs and ²³⁹ Pu + ²⁴⁰ Pu. The most recent low-level environmental radionuclide SRM issued by NIST, Ocean Sediment (SRM 4357) has certified and uncertified values for the following 22 radionuclides: ⁴⁰ K, ⁹⁰ Sr, ¹²⁹ I, ¹³⁷ Cs, ¹⁵⁵ Eu, ²¹⁰ Pb, ²¹⁰ Po, ²¹² Pb, ²¹⁴ Bi, ²²⁶ Ra, ²²⁸ Ra, ²²⁸ Th, ²³⁰ Th, ²³² Th, ²³⁴ U, ²³⁵ U, ²³⁷ Np, ²³⁸ U, ²³⁸ Pu, ²³⁹ Pu + ²⁴⁰ Pu, and ²⁴¹ Am. The uncertainties for a number of the certified radionuclides are non-symmetrical and relatively large because of the non-normal distribution of reported values. NIST is continuing its efforts to provide the ocean studies community with additional natural matrix radionuclide SRMs. The freeze-dried shellfish flesh matrix has been prepared and recently sent to participating laboratories for analysis and we anticipate receiving radioanalytical results in 2000. The research and development work at NIST produce well characterized SRMs that provide the world's environment-studies community with an important foundation component for radionuclide metrology.     

The natural radioactivity of Brazilian phosphogypsum

Phosphogypsum is a high volume by-product from the phosphoric acidindustries containing naturally occurring radionuclides. Envisaging the usesof phosphogypsum, a characterization of this material in terms of spatialdistribution of radionuclides was carried out by core samples taken from stacksof two important Brazilian phosphoric acid facilities. Samples were analyzedfor ²³⁸U, ²³⁴U, ²³²Th, ²²⁶Ra, ²²⁸Ra, ²¹⁰Pb and ²¹⁰Po using alpha- and gamma-spectrometryand UV-VIS spectrophotometry. Specific activities of ²³⁸U, ²³⁴U, ²²⁶ Ra and ²¹⁰Po obtained were comparablewith data reported in the phosphogypsum literature, while higher values werefound for ²³² Th and ²²⁸Ra.     

Distribution of environmental radionuclides in sediment cores of the Jinheung catchment

Sediment core samples taken from the Jinheung catchment located in the middle of the Korean Peninsula were used to know environmental radionuclide distribution. The grain sizes of the sediment cores were found at depth of about 17 cm suggesting that it might have occurred during a dry period of 1969. The radionuclides, ¹³⁷Cs, ²³⁷Np, ²³⁹Pu, ²⁴⁰Pu, ²³⁴U, ²³⁸U, ²²⁸Th, ²³⁰Th, ²³²Th, were analyzed by sector type ICP-MS and gamma-spectrometry. The Cs and Pu distribution changed with the depth, in which the maximum ranged from 14 to 22 cm. This was due to the high activity of the results of nuclear bomb tests in the air from 1960s and showed different distribution pattern on the soil surface. The average activity ratio of ²⁴⁰Pu/²³⁹Pu and ²³⁷Np/²³⁹Pu was 0.173 and 0.45, respectively. These values were similar to the north hemisphere global fallout ratio of ²⁴⁰Pu/²³⁹Pu (0.18) and ²³⁷Np/²³⁹Pu (0.45). The ²³⁷Np/²³⁹Pu ratio showed a higher value than the global fallout ratio above 14 cm depth. The U, Th and their daughter radionuclides kept secular equilibrium in the sediment core because the average activity ratios were nearly 1.     

Multifarious application of well-type germanium detector

A low-background well-type high-purity germanium detector system, with high counting efficiencies for X-rays and low-energy g-rays, was used to determine several radionuclides of environmental, biomedical, or geological interest. These included ¹²⁵I, ¹²⁹I, ²¹⁰Pb, ²²⁶Ra, ²³⁴Th (daughter of ²³⁸U), ²³⁹Pu, ²⁴⁰Pu and ²⁴¹Am. Methods were devized for their determinations in diverse environmental matrices or under laboratory procedural conditions. Counting efficiencies and minimum detectable activities for each nuclide were determined under the experimental conditions. These methods are being applied to our service analysis. This revised version was published online in July 2006 with corrections to the Cover Date.     

Polonium (210Po), uranium (238U) and plutonium (239+240Pu) in the biggest Polish rivers

In the paper the results of determination of ²¹⁰Po, ²³⁸U and ^239+240Pu radionuclides in the biggest Polish rivers are presented. Our results show the Vistula and the Oder as well as three Pomeranian Rivers are important sources of these radionuclides for the southern Baltic Sea.     

Inflow of polonium, uranium and plutonium radionuclides in Odra River catchment area assessment by environmetric expertise

The study deals with the application of cluster analysis (CA) and non-parametric tests (Shapiro–Wilk, Kruskal–Wallis, Dunn, U Mann–Whitney) to classify and interpret of a monitoring data set for Odra River water quality assessment based on concentration values of radiochemical parameters. The data set represents results for 3 alpha emitters (²¹⁰Po, ²³⁸U and ^239+240Pu) measured in surface water samples collected at 13 different sampling locations (5 in major Odra stream while 8 in Odra tributaries) within four seasons: winter, spring, summer and autumn, in the framework of 1 year-term quality monitoring research. The correlation analysis of polonium, uranium and plutonium data indicates that significant values of Spearman’s correlation coefficient appears between ²¹⁰Po and ^239+240Pu (r = 0.55 in autumn and 0.77 in winter as well as 0.49 in all year), while statistical significant correlation between uranium and plutonium as well as uranium and polonium were not found. In the Odra drainage basin, the biggest differences were observed in the case of ²³⁸U. The hypothesis about possible geographic and seasonal differences between concentration of ²¹⁰Po, ²³⁸U and ^239+240Pu in the Odra River catchment area was verified by cluster analysis (CA). Finally, to asses if there are statistically significant differences in mean concentration value of ²¹⁰Po, ²³⁸U and ^239+240Pu for Vistula and Odra Rivers drainage basins were obtained by used of the non-parametric tests. Comparing to Vistula catchment area, statistically different concentration of ²¹⁰Po and ^239+240Pu in all year was observed for river samples collected on Odra drainage basin.     

Certified reference material for radionuclides in seawater IAEA-381 (Irish Sea Water)

A certified reference material (CRM) for radionuclides in seawater, IAEA-381 (Irish Sea Water), is described and the results of certification are presented. The material has been certified for nine radionuclides (⁴⁰K, ⁹⁰Sr, ¹³⁷Cs, ²³⁷Np, ²³⁸Pu, ²³⁹Pu,²⁴⁰Pu, ^239,240Pu and ²⁴¹Am). Information on massic activities with the corresponding 95% confidence intervals are given for eight radionuclides (³H, ¹²⁵Sb, ²³⁴U, ²³⁵U, ²³⁶U, ²³⁸U, ²⁴¹Pu and ²⁴⁴Cm). Less reported radionuclides include ⁶⁰Co, ⁹⁹Tc, and ²⁴²Pu. The CRM may be used for quality assurance/quality control of the analysis of radionuclides in environmental water samples, for the development and validation of analytical methods and for training purposes. The material is available from the IAEA in 5 kg units.     

Natural radionuclide-free phosphoric acid production

High-uranium phosphate rock from Itataia, Brazil, was milled for wet-process phosphoric acid production using the dihydrate method. Uranium contained in the phosphoric acid was recovered by solvent extraction. The distribution of long-lived natural radionuclides of the ²³⁸U and ²³²Th decay series involved in these operations was evaluated. ²²⁶Ra, ²²⁸Ra and ²¹⁰Pb were found to predominate in the phosphogypsum, while ²²⁸Th, ²³⁰Th and ²³²Th in the uranium-free phosphoric acid. Thorium is removed from the phosphoric acid by solvent extraction to produce a NORM-free phosphoric acid.     

Cerenkov counting technique

A review is presented on the progress made in the Cerenkov counting technique. History, theory, and applications have shown that this technique is simple, easy, and can be used for the determination of low levels of radionuclides with a low background liquid scintilation counter. It has been applied to the measurement of radioactive biological tracers, fission products (⁹⁰sr,⁸⁹Sr) and natural radionuclides (²²²Rn,²²⁶Ra,²²⁴Ra,²¹⁰Pb,²²⁴Th,²²⁸Th,²³⁸U) in various types of samples. Advantages and disadvantages of this technique are summarized.     

Radioactive series disequilibria in underground uranium deposits of the Singhbhum Shear Zone, Eastern India

Radionuclides of the ²³⁸U series (²²⁶Ra, ²¹⁰Pb, ²³⁴Th and ²³⁴U), ²³⁵U series (²²⁷Ac and ²³¹Pa) and ²³²Th series (²²⁸Th and ²²⁸Ra) series were measured by High Resolution Gamma Spectrometry system in twenty-five uranium ore samples from underground uranium deposits in the Singhbhum Shear Zone of Eastern India. The activity concentrations were observed to vary within a wide range in most of the deposits, as is the case in most rocks of crustal origin. The uranium ore from these deposits were not of high ore grade (U concentrations ranged from 0.015 to 0.082%). Activity ratios of key daughter–parent pairs from the decay chains, viz. ²²⁶Ra/²³⁸U, ²²⁶Ra/²¹⁰Pb, ²³¹Pa/²³⁵U, ²²⁷Ac/²³⁵U, ²³⁰Th/²³⁸U, ²³⁴U/²³⁸U, ²²⁶Ra/²³⁰Th and ²²⁸Th/²²⁸Ra indicated migration/accumulation of uranium and radium in some samples. The ²²⁶Ra/²³⁰Th ARs suggested that the deposits were not closed to groundwater movement for a maximum time period of 8ky. Thiel plot of the ²³⁴U/²³⁸U vs. ²³⁰Th/²³⁸U activity ratios indicated uranium accumulation and complex processes of uranium redistribution.     

Use of combined alpha-spectrometry and fission track analysis for the determination of240Pu/239Pu ratios in human tissue

Plutonium and other actinides were determined in human autopsy tissues of occupationally exposed workers who were registrants of the United States Transuranium and Uranium Registries (USTUR). In this study, Pu was purified and isolated from Am, U and Th, after drying and wet-ashing of the tissues, and the addition of²³⁸Pu as a radiotracer. After electrodeposition onto vanadium planchets the^239+240Pu activity was determined by alpha-spectrometry. A fission track method was developed to determine²³⁹Pu in the presence of²³⁸Pu and²⁴⁰Pu, using Lexan^TM polycarbonate detectors. Combining the two techniques allowed the determination of the²⁴⁰Pu/²³⁹Pu activity and atom ratios. Data from selected USTUR cases are presented.     

Hokutolite collected from riverbed at Peitou Hot Spring in Taiwan: With emphasis on radiochemical studies

Summary Hokutolite, and hot spring water and river water collected recently at Peitou Hot Spring in Taiwan were analyzed for U, Th, Ra and ²¹⁰Pb isotopes. Concentrations of major chemical elements were also measured. Hokutolite had its typical chemical composition make-up for this area. The concentrations of ²³⁸U, ²³⁴U, ²³² Th, ²³⁰ Th, ²²⁸ Th, ²²⁶Ra, ²²⁸Ra and ²¹⁰Pb in samples scrapped into 7 layers from the surface to the bottom of a hokutolite specimen were 0.0021-0.0068, 0.0022-0.0075, 1.47-2.07, 1.00-1.29, 1.56-1.97, 56.7-68.6, 1.46-2.06 and 25.9-36.0 Bq/g, respectively. All the radionuclides exhibited a relatively uniform distribution, and radioequilibrium was confirmed among ²³² Th, ²²⁸Ra and ²²⁸ Th. From the relationship between the decay and growth of Th-series nuclides it was considered that the hokutolite studied was isolated from the stream water at least 70-80 years ago. The U/Th-series radionuclides in the hot spring water were in rather high concentrations and the enrichment of ²²⁸Ra and ²²⁸ Th to ²³² Th was the most prominent feature. Evaluation of the distribution coefficients (K_d) using the data on hot spring water or river water and hokutolite indicated that Th (K_d = 10⁴-10⁵) in water was likely to be precipitated (and/or co-precipitated) with BaSO₄ as Th(SO₄)₂ with a relatively high concentration into hokutolite, together with Ra (K_d = 10⁶-10⁷).     

Radioactivity of coals and fly ashes

The level and the behavior of the naturally occurring primordial radionuclides ²³⁸U, ²²⁶Ra, ²¹⁰Pb, ²³²Th, ²²⁸Ra and ⁴⁰K in coals and fly ashes are described. The activity concentrations of the examined coals and originated from coal mines in Greece ranged from 117 to 435 Bq·kg⁻¹ for ²³⁸U, from 44 to 255 Bq·kg⁻¹ for ²²⁶Ra, from 59 to 205 Bq·kg⁻¹ for ²¹⁰Pb, from 9 to 41 Bq·kg⁻¹ for ²²⁸Ra and from 59 to 227 Bq·kg⁻¹ for ⁴⁰K. These levels are comparable to those appeared in coals of different countries worldwide. The activity concentrations of the examined fly ashes and produced in coal-fired power plants in Greece ranged from 263 to 950 Bq·kg⁻¹ for ²³⁸U, from 142 to 605 Bq·kg⁻¹ for ²²⁶Ra, from 133 to 428 Bq·kg⁻¹ for ²¹⁰Pb, from 27 to 68 Bq·kg⁻¹ for ²²⁸Ra and from 204 to 382 Bq·kg⁻¹ for ⁴⁰K. The results showed that there is an enrichment of the radionuclides in fly ash relative to the input coal during the combustion process. The enrichment factors (EF) ranged from 0.60 to 0.76 for ²³⁸U, from 0.69 to 1.07 for ²²⁶Ra, from 0.57 to 0.75 for ²¹⁰Pb, from 0.86 to 1.11 for ²²⁸Ra and from 0.95 to 1.10 for ⁴⁰K.     

Comparison of transfers for natural radionuclides (238U, 234Th, 226Ra, 210Pb & 210Po) from five different soils to four different barley genotypes

Transfer Factors (Fv) of ²³⁸U, ²²⁶Ra, ²³⁴Th, ²¹⁰Po and ²¹⁰Pb from five different agricultural soils in semi-arid region (Syria) to four different barley genotypes were studied in an agricultural potted experiment. The geometric mean of the Fv values were (0.08) for ²¹⁰Pb, and (0.02) for ²¹⁰Po, while it ranged from 0.18 to 0.42 ,from 0.08 to 0.15 and from 0.22 to 0.4 for ²³⁸U, ²³⁴Th and ²²⁶Ra, respectevily. The Fv values of ²³⁸U and ²²⁶Ra were within the recommended global medians, while the Fv values of ²³⁴Th, ²¹⁰Pb and ²¹⁰Po were higher. There is no clear relationship between the soil properties and Fv of all studied radionuclides to barley genotypes. Moreover, the expression of glutathione (GSH) gene, which is belived to be involoved in heavy metal removal was generally low in all studied varieties grown in all soil types.

     

Measurement of non-separated U/Pu samples: optimization of TIMS procedures for safeguards purposes at Rokkasho on-site laboratory

The on-site laboratory (OSL) at Rokkasho Reprocessing Plant (RRP) is jointly operated by the Japanese authority Nuclear Material Control Centre and the International Atomic Energy Agency (IAEA) and provides, together with the Nuclear Material Laboratory (NML) at Seibersdorf, analytical services to the IAEA’s inspectorate. OSL deals with a variety of samples typical to a reprocessing plant including pure product solutions of uranium and plutonium but also mixed U/Pu solutions originating from various stages of the chemical process. For a significant proportion of the samples, the requirement on measurement accuracy and precision from the Inspectorate makes the use of thermal ionization mass spectrometry (TIMS) indispensible. Until recently, all samples intended for TIMS had to undergo time-consuming U/Pu separation before isotope dilution measurement. The need for rapid reporting of analytical results for certain safeguards samples evoked the idea of performing TIMS measurements without prior U/Pu separation for mixed U/Pu products as they are obtained from the PUREX process at RRP. For this purpose, a systematic study was initiated to probe the figure of merits and limitations of conducting TIMS analyses on mixed U/Pu samples and, in particular, whether the accuracy and precision of the main ratios of interest, n(²³⁵U)/n(²³⁸U) and n(²⁴⁰Pu)/n(²³⁹Pu), are influenced by the presence of larger amounts of the other element. A series of synthetic mixtures with U/Pu ratios ranging from 1:10 up to 100:1 were prepared and measured in both laboratories—OSL and NML—using ThermoFisher TRITON multi-collector TIMS instruments. For the n(²³⁵U)/n(²³⁸U) ratio, interference due to ²³⁸Pu was observed which can be significant depending on the U/Pu ratio and the ²³⁸Pu abundance. However, for the n(²⁴⁰Pu)/n(²³⁹Pu) ratio, which is of premier importance for safeguarding RRP, no significant interference arising from the concomitant U was detected independently of enrichment. Even in samples with an excess of U (U/Pu ratio of 100:1), compliance with International Target Values (ITV2010) was demonstrated for n(²⁴⁰Pu)/n(²³⁹Pu) results with a relative difference to certified not exceeding 0.01 %.     

A simple radiochemical method for determining bone-seeking radionuclides in bone and teeth: 90Sr in teeth of children from Ukraine and Germany

Bone is a critical organ for the accumulation of ⁹⁰Sr but also of other “bone-seeking” radionuclides such as Ra, Pb, Th, U and Pu. That's why a simple radiochemical procedure to separate ⁹⁰Sr, ²¹⁰Pb, ²²⁶Ra, Th_nat. U_nat., ²³⁸Pu and ^239/240Pu from bone and teeth was developed. The separation scheme is based on extraction chromatography. Deciduous teeth, extracted from children born in 1982-1991 were collected in various regions of Germany and in Northwest Ukraine and analyzed for ⁹⁰Sr concentrations with regard to the Chernobyl accident in 1986. The teeth were grouped into samples according to the year of birth and the residence of the donors. The ⁹⁰Sr content in teeth from the Ukraine (mean = 63.8 mBq/g Ca) averaged more than twice as much as that found in teeth from Germany (mean = 28.4 mBq/g Ca). The obvious explanation for this effect is that the concentration of ⁹⁰Sr decreased with increasing distance from the damaged Chernobyl nuclear power plant. The measured levels of ⁹⁰Sr concentrations, however, were much lower than ⁹⁰Sr concentrations determined in the mid-60s and mid-70s. This revised version was published online in July 2006 with corrections to the Cover Date.     

Distribution of radionuclides and elements in Cubatão River sediments

Summary Cubat?o River is located in Santos Basin, S?o Paulo State, Brazil. This region is characterized by the occurrence of estuaries and mangrove. Due to its location, near the coastal line, it is also an important industrial area, where phosphate fertilizer plants, petrol refineries, and chemical and steel industries are present. Such human activities contribute to the enhancement of elemental composition in sediments and, in some cases, also increase the radionuclide concentrations, the so called Technologically Enhanced Natural Occurring Radioactive Materials (TENORM). The contamination of land and sediments by TENORM is of major concern. The activity concentration of U and Th series radionuclides was determined in five sediment samples from Cubat?o River. The activity concentration ratio was also determined. Equilibrium was observed for the ratio ²³⁴U/²³⁸U. The activity ratios of Th/²³⁸U, ²²⁸Ra/²²⁶Ra and ²¹⁰Pb/²²⁶Ra were higher than the unity. In the first two cases, the observed values are due to the higher activity of Th in the sediment and in the last case are probably due to the atmospheric deposition of ²¹⁰Pb.     

Development of a sequential method for the determination of238U,234U,232Th,230Th,228Th,228Ra,226Ra,and210Pb. in environmental samples

A sequential analytical method for the determination of²³⁸U,²³⁴U,²³²Th,²³⁰Th,²²⁸Th,²²⁸Ra,²²⁶Ra and²¹⁰Pb in environmental samples was developed. Uranium and thorium isotopes are first chromatographically sepaaated using tri-n-octyl phosphine oxide (TOPO) supported on silica gel. The uranium isotopes are determined by alpha-spectrometry following extraction with TOPO onto a polymeric membrane. Thorium isotopes are co-precipitated with lanthanum fluoride before counting in an alpha spectrometer. Radium isotopes and²¹⁰Pb are separated by co-precipitation/precipitation with mixed barium/lead sulphate. Radium-226 is determined by gross alpha counting of the final BaSO₄ precipitate and²²⁸Ra by gross beta counting of the same source. Lead-210 is determined through beta counting of its daughter product²¹⁰Bi.