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.     

Mixing of atmospheric <Superscript>210</Superscript>Pb and <Superscript>7</Superscript>Be and <Superscript>137</Superscript>Cs and <Superscript>90</Superscript>Sr fission products in four characteristic soil types

Depth distribution of atmospheric ²¹⁰Pb and ⁷Be and ⁹⁰Sr and ¹³⁷Cs fission products was measured in two types of aeolian soils (desert dust and volcanic ash), irrigated paddy soil and strongly acidic soil. The depth dependence of ²¹⁰Pb, ⁷Be and ¹³⁷Cs show that these radionuclides have been diffused as solid soil particles in surface soil layers. In aeolian soil layers, about 50% of ⁹⁰Sr were diffused in surface soil layer and the remaining 50% had penetrated to deeper layers. The half of the fission particles containing ⁹⁰Sr were shown to have decomposed over the past 35 years.     

Quality assessment of hydrosphere in the vicinity of Czech nuclear power plants by radioanalytical methods

Summary The paper deals with the impact of nuclear plants and radioactive waste disposal on surface and ground water quality in their vicinity using various radiometric and radioanalytical methods. The impact of nuclear power plant Temelin on activation concentrations and fission products in hydrosphere, including tritium, was detected. The annual average tritium concentrations in Vltava River correspond to the previously calculated estimates for average and minimal quaranteed flow rates. The concentrations histories of ⁹⁰Sr and ¹³⁷Cs in surface water show a decreasing trend. This trend was not influenced by the nuclear power plant pilot operation. In the case of tritium, a concentration increase trend has been already observed since the startup of pilot operation. An attempt has made interpreting the sorption and diffusion data for radionuclides of cesium, strontium and tritium and technetium as representatives of multivalent elements. Sorption and diffusion data of ¹³⁷Cs and ⁹⁰Sr in contact with natural sorbent bentonite lead to the conclusion that both diffusion and batch sorption experiments can be simulated by an exchange model. Sorption of technetium on various bentonites plus additives materials is described. Retention of technetium on these solid phases is driven by sorption of reduced form of technetium Tc(IV).     

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.     

Application of radiochemical methods and dispersion model in the study of environmental pollution in Brazil

Methodologies for analysis of anthropogenic and natural radionuclides in marine samples were developed and applied in environmental samples. Results of systematic measurements of these radionuclides have showed that artificial radioactivity levels are in agreement with the values from the regions not affected directly by nuclear accidents or nuclear reprocessing plant discharges and are due to the global fallout. The average concentration of¹³⁷Cs is of 1.4 Bq·m⁻³ in seawater, ranges from 13 to 220 mBq·kg⁻¹ in fish, and from 0.4 to 1.8 Bq·kg⁻¹ for sediments.⁹⁰Sr levels in seawater are of 1.8 Bq·m⁻³ and in fish vary from 19 to 75 mBq·kg⁻¹. Sediments present concentrations of⁹⁰Sr lower than 0.8 Bq·kg⁻¹ and for^239+240Pu of 0.03 to 0.18 Bq·kg⁻¹.²¹⁰Po levels in fish range from 0.5 to 5.3 Bq·kg⁻¹. The data generated represent reference values for our country and are used to estimate the intake levels of these radionuclides by consuming of marine products.     

Production of radionuclides for nuclear therapy and environmental studies

This work is devoted to the production of the radionuclides used in nuclear medicine and as radiotracers for environmental research. Production methods for high LET radionuclides (⁶⁷Ga, ⁷⁷Br, ¹¹¹In, ²¹¹At) that are promising for radioimmunotherapy are proposed. Production techniques for short-lived analogues of highly radiotoxic long-lived fission products (Tc, Se, Sr) are developed. The techniques are based on extraction and chromatographic separation from a cyclotron target irradiated by α-particles and deuteron beams.     

A new reference material for radionuclides in the mussel sample from the Mediterranean Sea (IAEA-437)

A new Reference Material (RM) for radionuclides in mussel (Mytilus galloprovincialis) from the Mediterranean Sea (IAEA-437) is described and the results of the certification process are presented. Four radionuclides (⁴⁰K, ²³⁴U, ²³⁸U, and ^239+240Pu) have been certified, and information values on massic activities with 95% confidence intervals are given for nine radionuclides (¹³⁷Cs, ²¹⁰Pb(²¹⁰Po), ²²⁶Ra, ²²⁸Ra, ²²⁸Th, ²³⁰Th, ²³²Th, ²³⁵U, and ²⁴¹Am). Results for less frequently reported radionuclides (⁹⁰Sr, ¹²⁹I, ²³⁸Pu, ²³⁹Pu, and ²⁴⁰Pu) are also reported. The RM can be used for quality assurance/quality control of the analysis of radionuclides in mussel samples, for the development and validation of analytical methods and for training purposes. The material is available in 200 g units.     

Recent Development on Determination of Low-Level 90Sr in Environmental and Biological Samples: A Review

In the context of the rapid development of the world’s nuclear power industry, it is vital to establish reliable and efficient radioanalytical methods to support sound environment and food radioactivity monitoring programs and a cost-effective waste management strategy. As one of the most import fission products generated during human nuclear activities, ⁹⁰Sr has been widely determined based on different analytical techniques for routine radioactivity monitoring, emergency preparedness and radioactive waste management. Herein, we summarize and critically review analytical methods developed over the last few decades for the determination of ⁹⁰Sr in environmental and biological samples. Approaches applied in different steps of the analysis including sample preparation, chemical separation and detection are systematically discussed. The recent development of modern materials for ⁹⁰Sr concentration and advanced instruments for rapid ⁹⁰Sr measurement are also addressed.     

Measurement of 90Sr in Marine Biological Samples

Strontium-90 (⁹⁰Sr) is one of the most hazardous radionuclides, and it contributes to radiation exposure by ingestion. The routine determination of ⁹⁰Sr in marine biological samples is highly desirable given the development of the nuclear power industry. A fast, simple, and low-detection-limit method was developed for the measurement of ⁹⁰Sr in marine biological samples based on determining ⁹⁰Y by means of coprecipitation and solvent extraction with bis-2-ethylhexyl-phosphoric acid (HDEHP) in n-heptane. The interfering ²¹⁰Bi is removed using Bi₂S₃ precipitation. The separation and purification of eight samples per day can be accomplished through this method. The detection limit of ⁹⁰Sr for this method is 0.10 Bq/kg (ash weight). The radiochemical procedure was validated by fitting the decay curve of the sample source and by the determination of ⁹⁰Sr standards.     

Analytical Methods for the Determination of 90Sr and 239,240Pu in Environmental Samples

Artificial long-lived radionuclides such as ⁹⁰Sr and ^239,240Pu have been long released into the environment by human nuclear activities, which have a profound impact on the ecological environment. It is of great significance to monitor the concentration of these radionuclides for environmental safety. This paper summarizes and critically discusses the separation and measurement methods for ultra-trace determination of ⁹⁰Sr, ²³⁹Pu, and ²⁴⁰Pu in the environment. After selecting the measurement method, it is necessary to consider the decontamination of the interference from matrix elements and the key elements, and this involves the choice of the separation method. Measurement methods include both radiometric methods and non-radiometric methods. Radiometric methods, including alpha spectroscopy, liquid scintillation spectrometry, etc., are commonly used methods for measuring ^239+240Pu and ⁹⁰Sr. Mass spectrometry, as the representative of non-radiometric measurement methods, has been regarded as the most promising analytical method due to its high absolute sensitivity, low detection limit, and relatively short sample-analysis time. Through the comparison of various measurement methods, the future development trend of radionuclide measurement is prospected in this review. The fully automatic and rapid analysis method is a highlight. The new mass spectrometer with ultra-high sensitivity shows strong analytical capabilities for extremely low concentrations of ⁹⁰Sr, ²³⁹Pu, and ²⁴⁰Pu, and it is expected to develop determination methods with higher sensitivity and lower detection limit.     

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.     

Determination of long-lived radionuclides in radioactive wastes from the IEA-R1 nuclear research reactor

Ion-exchange resins and activated charcoal beds are employed for purification of the cooling water that is pumped through the core of pool type nuclear research reactors. Once expended, these media are replaced and become radioactive wastes that contain low concentrations of long-lived fission and activation products, uranium isotopes and transuranium elements. Determination of the radioactive inventory is of paramount importance in the management of such radioactive wastes, which, besides high-energy photon emitters that can be identified and quantified directly by gamma-ray spectrometry, also contain pure alpha, pure beta and low-energy photon emitters whose quantitative determination require radiochemical separation. These later are collectively known as difficult to measure (DTM) radionuclides. A characterization program embracing the DTM radionuclides is currently in progress for spent ion-exchange resins and activated charcoal beds that were definitively withdrawn from the water cleanup system of the IEA-R1 nuclear research reactor. Radiochemical methods used in the characterization program include separations with specific anionic resins, chromatographic extractions and co-precipitation, which enabled the measurement of the activity concentrations of ⁹⁰Sr, ²³⁴U, ²³⁵U, ²³⁸U, ²³⁸Pu, ^239+240Pu, ²⁴¹Pu, ²⁴¹Am and ²⁴⁴Cm. An enhanced retention of uranium and transuranium elements was observed in the activated charcoal compared to the ion-exchange resins as a result of the tendency of actinides to undergo hydrolysis in aqueous solutions.     

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.     

Separation of Ba and Pb from aqueous solutions of Sr with commercially available “precipitated active manganese dioxide”

Ba and Pb radionuclides can be removed from Sr in aqueous solution in both sodium acetate and acetic acid, containing 20 mg Sr carrier, by stirring with small (0.1–0.5 g) amounts of solid manganese dioxide. In tracer experiments⁸⁵Sr was separated with only small losses from¹³³Ba and²¹⁰Pb by separation factors of 87 and 135, respectively. The separation factor is defined here as the % of the initial⁸⁵Sr activity/ % of the initial¹³³Ba or²¹⁰Pb activity remaining in the aqueous phase after MnO₂ contact. The applicability of this technique for removing Ba and Pb radionuclides in the analysis of⁹⁰Sr in environmental samples (especially milk) is discussed.     

Liquid-liquid extraction methods for the production of carrier-free 115cd and 89,90sr from fission products

The extraction of fission product elements with 1-phenyl-3-methyl-4-caprylpyrazolone-5 at various pH values has been investigated. The quantitative extraction of cadmium at pH 5.4 and that of strontium at pH 9.0 is utilised in devising procedures for the recovery of ¹¹⁵Cd and ^89,90Sr from the fission products. Good decontamination factors and more than 90% ¹¹⁵Cd and 80% ^89,90Sr activities were recovered.     

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.     

Methodology for determination of 89Sr and 90Sr in radiological emergency: I. Scenario dependent evaluation of potentially interfering radionuclides

Early determination of ⁸⁹Sr and ⁹⁰Sr in radiological emergency is hampered by the presence of interfering short-lived fission products. In this study, three commonly used radioanalytical strategies for ⁸⁹Sr and ⁹⁰Sr were evaluated theoretically considering their suitability in a nuclear explosion scenario. The methods were evaluated with respect to the need for decay time of interfering short-lived strontium and yttrium isotopes, and reduction of other known interfering nuclides prior to measurement. The strategy shown to be most successful included initial separation of strontium and determination of ⁸⁹Sr, followed by an yttrium separation and counting of ⁹⁰Y. ⁸⁹Sr and ⁹⁰Sr could be determined about 5 and 9 days after a nuclear explosion, respectively.     

Occurrence of natural radionuclides and fallout cesium-137 in dry-season agricultural land of South Western Nigeria

The radioactivity of the Opa river — irrigated farmlands in the south western Nigeria was determined using an HpGe based, low-level passive gamma-counting system. With the exception of two isotopes, the main radionuclides analysed in the sample were the progenies of²³⁸U and²³²Th. The other two isotopes were the naturally occurring⁴⁰K and the anthropogenic¹³⁷Cs. The result obtained showed elevated levels of radioactivity from all detected radionuclides compared to the published data for this area. Enhanced levels of naturally occurring radionuclides is attributed to the use of phosphatic fertilizers for dry season vegetable cultivation along this river banks. The presence of the fission product¹³⁷Cs could be traced to the fallouts occasioned by the various French nuclear tests in the Sahara desert, and probably, some effect of the more recent nuclear reactor accident at Chernobyl in 1986.     

Proficiency test exercise on the determination of natural levels of radionuclides in mushroom reference material

The results from a proficiency test exercise for the determination of natural levels of radionuclides in mushroom reference material carried out by laboratories in six different countries are discussed. These laboratories submitted data on seven radionuclides, namely ¹³⁴Cs, ¹³⁷Cs, ⁴⁰K, ⁹⁰Sr, ²⁴¹Am, ²²⁶Ra, and ²¹⁰Po. However, only the data received for three of these radionuclides could be statistically evaluated to obtain consensus mean values and confidence intervals (at a significance level of 0.05). The contents of ¹³⁴Cs, ¹³⁷Cs and ⁴⁰K were quantified as 4.4, 2,899 and 1,136 Bq/kg, respectively.     

Methodology for determination of <Superscript>89</Superscript>Sr and <Superscript>90</Superscript>Sr in radiological emergency: II. Method development and evaluation

In this work a method for the determination of both ⁸⁹Sr and ⁹⁰Sr is presented. The method can potentially be used in radiological emergency and deliver results shortly after an incident. The method development was based on theoretical calculations of potential interferences from other fission products and how these could be discriminated when applying different chemical separation schemes. Validation was done on reactor coolant water containing short-lived fission products, and on a reference material. The results indicate that correct results of ⁸⁹Sr and ⁹⁰Sr can be obtained 4 and 9 days, respectively, after an incident.