A sequential method for the determination of 210Pb, 226Ra,and uranium and thorium radioisotopes by LSC and alpha-spectrometry

A procedure for the determination of ²¹⁰Pb, and alpha-emitting radioisotopes of uranium, thorium, and radium from the same aliquot of a sample has been proposed. The key step consisted in the recovery of Pb(II) and Ra by precipitation of insoluble Pb(NO₃)₂, the uranium and thorium radioisotopes remaining in solution. Afterwards, the fractions were handled by specific, well consolidated procedures. Lead-210 was determined by the LSC technique while the uranium, thorium, and radium radioisotopes were measured with silicon alpha-spectrometers. The procedure was applied to a reference sample and several environmental samples obtaining satisfactory results.     

Characteristics of NORM in the oil industry from eastern and western deserts of Egypt.

Naturally occurring radionuclides (NORs) from the 232Th- and 238U-series, which are omnipresent in the earth's crust, can be concentrated by technical activities, particularly those involving natural resources. Although, a great deal of work has been done in the field of radiation protection and remedial action on uranium and other mines, recent concern has been devoted to the hazard arising from naturally occurring radioactive materials (NORM) in oil and gas facilities. NORM wastes associated with oil and gas operations from scale deposits, separated sludge and water at different oil fields in the eastern and western deserts were investigated. Concentrations of the uranium, thorium, and potassium (40K) series have been determined from high-resolution gamma-ray spectrometry. Total uranium content of samples was determined using laser fluorimetry. The levels of radioactivity were mainly due to enhanced levels of dissolved radium ions. Only minute quantities of uranium and thorium were present. The disequilibrium factor for 238U/226Ra has been determined.     

Improvement of a method for the sequential determination of Pb, Ra, and uranium isotopes by LSC and alpha-particle spectrometry

In a previous paper the authors proposed a sequential method for the determination of isotopes of uranium, thorium, radium, and lead from environmental samples using alpha-particle spectrometry and LSC techniques. Although the radiochemical yields were suitable when the assays were performed on synthetic samples, application to real environmental samples caused a major decrease in the radiochemical yield, especially for uranium in inorganic samples (soils). A modification of the procedure is described that overcomes this drawback.     

Sequential extraction for radionuclide fractionation in soil samples: a comparative study.

Two sequential extraction procedures, Tessier's method (Anal. Chem. 51(7) (1979) 844), and a current version known as Schultz's method (J. Environ. Radioact. 40(2) (1998) 155), were compared. The two procedures were applied to a natural soil sample that presents high activity concentrations in natural radionuclides of the 238U series. Reproducibility studies of each method and a comparison between the two sets of results were performed for uranium, thorium, and radium. The results were different for each radionuclide. Analysis of the extracted fractions was carried out by alpha spectrometry.     

Radon escape from New Zealand speleothems

When calculating the environment radiation absorbed dose rate in ESR or TL dating, it is usual to allow for the possibility of dissequilibrium in the uranium-series decay chain, due to the escape of the radioactive gas, radon, from the sample before its decay to non-gaseous daughter products. Partial or complete radon escape may reduce the internal radiation dose to less than half that which would be received if no radon escaped. In this study a number of speleothems from a temperate climate, varying in age from 6 ka to more than 730 ka (ages determined by ²³⁴U/²³⁰Th and ²³⁵U/²³¹Pa dating and by paleomagnetic analysis) have been analysed for thorium and polonium isotopes. As radon lies between thorium and polonium in the uranium decay chain, a comparison of thorium and polonium activities with the expected values, derived from the age of the sample and the initial concentrations, gives an estimate of the radon escape factor and its impact on environmental dose rates. The activity rates of thorium, uranium and polonium were measured separately by counting their α particle emissions after electroplanting the elements onto rotating stainless steel discs. Polonium was plated directly after dissolution of the sample and before loading the solution onto a heated cation column to separate the uranium and thorium fractions. The uranium fraction was further purified on an anion before plating. The recovery rates of uranium and thorium were monitored by spiking but the recovery rate of polonium must be regarded as a minimum; estimates of radon escape are therefore likely to be overestimates rather than underestimates. Of 19 speleothems studied, only two gave results inconsistent with values predicted on the basis of no radon loss (Chauvenet's test): one, a relatively young sample of 6 ka, showed evidence of radium coprecipitation with uranium, and one, a dog-tooth spar with an open crystal structure and a high porosity showed evidence for radon escape. A third sample, also a flowstone/spar with a higher porosity than normal, was marginally significant. As the degree of radon escape will vary from sample to sample, the environment dose rate must be regarded as having a high level of uncertainty for samples of this type, unless radon escape is determined experimentally. The remaining samples (12 stalagmites, 3 stalactites and 1 flowstone), of a more massive structure, showed no significant radon escape (Student's t-test), and therefore the environmental dose rate for such samples should be calculated on the basis of radon retention.     

A method for preparation and purification of 234Th.

An improved method to recover 234Th from depleted uranium has been developed. The method is based on solvent extraction and ion-exchange separations. The final thorium fraction has a high specific activity, about 1-3 PBq/mol Th, which makes it well suited for investigations, where a low thorium concentration is essential. The method is comparably fast, with a total processing time of 2 days. Another advantage is that the uranium fraction can be used as a 234Th generator for several years.     

Determination of natural radioactivity in building materials used in the Rawalpindi/Islamabad area by gamma-ray spectrometry and instrumental neutron activation analysis.

Samples of sand and manufactured building materials collected from the Rawalpindi/Islamabad area have been analyzed for the primordial natural radionuclides 238U, 232Th and 40K using gamma-ray spectrometry. The uranium and thorium contents have also been determined by instrumental neutron activation analysis (INAA). The specific activities of these radionuclides in the samples are compared with those of the world averages for soil. The comparison shows that, of the nine samples analyzed, only the three brick samples have higher activities than the world averages for soil. The specific activities in these materials, having a radium equivalent activity of less than 370 Bq kg-1, when evaluated for radiological effects show that all materials meet the external gamma-ray dose limitation of 1.5 mSv y-1. The gamma-spectrometric and INAA techniques complemented each other well in this study.     

Uranium and thorium series disequilibrium in quaternary carbonate deposits from the Serra da Bodoquena and Pantanal do Miranda, Mato Grosso do Sul State, central Brazil.

Activities of gamma-ray emitting members of the uranium (238U) and thorium (232Th) series were measured in a quaternary limestone deposit that outcrops in the southeastern Pantanal Matogrossense Basin and in quaternary tufas deposited at the drainage of the Serra da Bodoquena. It is a first step in a study of the mobilization of uranium and thorium series and its relation to surface hydrology, in a region where carbonate deposits are being continuously dissolved and reprecipitated. The obtained results show that all these deposits are characterized by very low concentrations of uranium and thorium. The 238U/226Ra and 228Th/228Ra activity ratios are significantly different than 1.0, indicating that both series are in radioactive disequilibrium. Although the Serra da Bodoquena deposits seem to be very recent, their very fine granulation and high porosity suggest that they behave as open systems for geochemical exchanges of uranium and thorium series members. The Pantanal do Miranda limestone has a radiocarbon age of 3900 yr BP. Since the thorium series is in disequilibrium it is also concluded that this deposit behaves as an open system for geochemical exchanges.     

Rapid non-destructive quantitative estimation of urania/ thoria in mixed thorium uranium di-oxide pellets by high-resolution gamma-ray spectrometry

A non-destructive technique using high-resolution gamma-ray spectrometry has been standardised for quantitative estimation of uranium/thorium in mixed (ThO₂–UO₂) fuel pellets of varying composition. Four gamma energies were selected; two each from the uranium and thorium series and the time of counting has been optimised. This technique can be used for rapid estimation of U/Th percentage in a large number of mixed fuel pellets from a production campaign.     

Alpha-spectrometric analysis of uranium and thorium using solid-phase extraction for sample preparation

A method is presented here for the preparation of thin uniform samples of naturally occurring uranium and thorium which are highly suitable for α-spectrometric analysis. The solid-phase extraction procedure simultaneously achieves a complete separation of the analytes from the sample matrix and a high enrichment factor for uranium and thorium, so that the ensuing eluate is ideally suited for either electrodeposition or ICP-MS, without the need for complicated and painstaking sample preparation. In contrast to conventional liquid–liquid phase-extraction methods, no organic waste solutions are produced, and the process can be easily automated.     

Influence of the soil bioavailability of radionuclides on the transfer of uranium and thorium to mushrooms.

The soil-mushroom transfer of thorium and uranium was analyzed in two ecologically similar but geographically separated Spanish ecosystems by means of the transfer factor, TF. Uranium TF values were in the range 0.043-0.49, and thorium TF values in the range 0.030-0.62. These values were similar to those of (90)Sr, (239+240)Pu, and (241)Am found previously in the same ecosystems. Given the low availability of uranium and thorium, the available transfer factors, ATF, were also determined. These were higher than the TF values by one order of magnitude for (234, 238)U, and by 2-3 orders of magnitude for (228, 230, 232)Th. The ATF value of thorium was similar to that of (137)Cs, and that of uranium similar to that of (40)K. Hebeloma cylindrosporum presented the highest uranium and thorium transfer factors, confirming this species as a good bioindicator of a soil's radioactive content.     

Preconcentration of radium isotopes from natural waters using MnO2 Resin.

We have characterized "MnO2 Resin," a new resin developed by the PG Research Foundation, for radium adsorption over wide ranges of pH, reaction times and salt concentrations. We show that the sorption of 133Ba (used as a proxy for Ra) is highly dependent on pH with the most useful range from pH 4 to 8. The surface layers of the Mn oxides apparently become more positively charged under acidic conditions (below pH 4), which prevents diffusion of positively charged alkaline earth species (e.g. Ba2+, Ra2+) into the sorption sites. Adsorption at higher pH is thought to be inhibited because of carbonate complexation.We found that the sorption characteristics for radium onto MnO2 Resin are especially favorable for low-salinity waters but the sorption is still very satisfactory for highly salted solutions (KD=2.8x10(4) in both cases) but with slower kinetics. For analytical purposes, both column and pump experiments showed high recoveries with no measurable discrimination between Ra and Ba regardless of flow rates in fresh water. Seawater tests showed that recoveries of Ra and Ba are lower than fresh water at elevated flow rates with Ra adsorption higher than Ba at flow rates above 10 ml/min.     

Leaching of technologically enhanced naturally occurring radioactive materials.

A form of waste associated with mining activities is related to the type of deposit being mined and to the procedure of exploitation and enrichment adopted. The wastes usually contain relatively large amounts of technologically enhanced naturally occurring radioactive materials (TENORM). The TENORM are often stored on the surface. Consequently, they can be leached as a result of interaction with aqueous solutions of different chemical composition. This further leads to pollution of water and soil in the vicinity of the stored wastes. The paper presents the results of laboratory investigation aimed at quantifying the leaching process of samples originating from uranium dumps and storage reservoirs associated with brine pumped from coal mines. The leaching process was investigated with respect to selected elements: uranium isotopes, radium isotopes, iron, barium and sodium. The samples were exposed to aqueous solutions of different chemical composition. The experiments revealed that TENORM in form of sulphate compounds are the most resistant against leaching. The leaching coefficient for radium isotopes varies from a few thousandth percent to a few hundredth percent. On the other hand, for TENORM occurring in sand or sludge, the leaching coefficient for uranium and radium isotopes ranged from a few hundredth percent to a few percent.     

A method for the rapid radiochemical analysis of uranium and thorium isotopes in impure carbonates.

A simple method combining solvent extraction and electrodeposition procedures is described for the determination of the isotopic composition and content of uranium and thorium in travertine samples. The actinide elements are extracted with diethyl ether from a calcium nitrate solution. The isolation of the elements and the alpha source preparation are performed in two steps after the sample digestion. The acid leaching of samples is performed using both partial and total dissolution methods. High recoveries of both uranium and thorium and good alpha-spectra are obtained with both partial and total dissolution methods.     

Sequential isotopic determination of plutonium, thorium, americium, strontium and uranium in environmental and bioassay samples.

A procedure has been developed to provide sequential analysis of 238Pu, 230Th, 241Am, 238U, and 90Sr in environmental and bioassay samples. Tracers and/or carriers (242Pu, 243Am, 232U, and stable strontium) are added into the sample as chemical yield monitors, and then, plutonium, thorium, strontium, americium, and uranium are sequentially separated and purified by Dowex ion-exchange resin, EiChroM Sr-resin, EiChroM TRU-resin, and Chelate-100 resin, respectively. The radioactivities of 90Sr and the actinides are measured using the liquid scintillation counter and alpha-particle spectrometer, respectively. Acidified water, glass-fiber air filter, soil, synthetic urine and synthetic feces samples of US National Institute of Standard and Technology Radiochemical Intercomparison Program(NRIP) were analyzed to verify this method. All the analytical results of 238Pu, 230Th, 90Sr, 241Am and 238U meet the traceability limit per ANSI N42.22, and when appropriate, evaluation of radiobioassay measurement bias and precision per ANSI N13.30.     

Pioneers of nuclear medicine, Madame Curie

Among those who have made important discoveries in the field of radioactivity and thus helped in the development of nuclear medicine as an identical entity are: Heinrich Hertz who in 1886 demonstrated the existence of radiowaves. In 1895 Wilhelm R?ntgen discovered the X-rays. In 1896 H. Becquerel described the phenomenon of radioactivity. He showed that a radioactive uranium salt was emitting radioactivity which passing through a metal foil darkened a photographic plate. An analogous experiment performed by S.Thomson in London was announced to the president of the Royal Society of London before the time H.Becquerel announced his discovery but Thomson never claimed priority for his discovery. Muarie Sklodowska Curie (1867-1934) was undoubtedly the most important person to attribute to the discovery of radioactivity. In 1898 she discovered radium as a natural radioactive element. This is how she describes the hard time she had, working with her husband Pierre Curie (1859-1906) for the discovery of radium and polonium: "During the first year we did not go to the theater or to a concert or visited friends. I miss my relatives, my father and my daughter that I see every morning and only for a little while. But I do not complain...". In presenting her discovery of radium, Madame Curie said: " ...in the hands of a criminal, radium is very dangerous. So we must often ask ourselves: will humanity earn or lose from this discovery? I, myself belong to those who believe the former...". The notebooks that Madame Curie had when she was working with radium and other radioactive elements like polonium, thorium and uranium are now kept in Paris. They are contaminated with radioactive materials having very long half-lives and for this reason anyone who wishes to have access to these notes should sign that he takes full responsibility. There are some more interesting points in Madame Curie's life which may not be widely known like: Although her full name is Maria Sklodowska-Curie, she is not known neither by that full name nor as Maria Sklodowska but as Marie Curie. Madame Curie was the second of five children. At the age of 24 she went to Sorbonne-Paris after being invited by her sister Bronja to study for about 2-3 years; instead she stayed in Paris for her whole life. Her doctorate was on the subject: "Research on radioactive substances" which she completed in six years under the supervision of H. Becquerel. Pierre Curie was Director of the Physics Laboratory of the Ecole Municipale of Physics and Industrial Chemistry when he married M. Curie in 1895. Pierre Curie left his other research projects and worked full time with his wife. In this laboratory M. Curie and her husband Pierre discovered radium and polonium. In 1901 Pierre Curie induced a radiation burn on his forearm by applying on his skin radiferous barium chloride for 10 hours. During World War I, M.Curie organized for the Red Cross a fleet of radiological ambulances each with X-ray apparates which were called "Little Curies". The X-ray tubes of these apparates were unshielded and so M.Curie was exposed to high doses of radiation. Once an ambulance fell into a ditch and M.Curie who was inside the ambulance was badly bruised and stayed at home for 3 days. M. Curie with her daughters, Irene and Eve, was invited and visited America in 1921. She led a successful campaign to collect radium for her experiments. Before leaving America, President Harding donated through her to the Radium Institute of Paris 1 g of radium for research purposes. At that time the process to obtain 0.5 g of pure radium bromide required 1 ton of ore and 5 tons of chemicals. No measures of radiation protection were taken back then. In 1929 Madame Curie visited the United States for a second time. She met with President Hoover and with the help of the Polish women's association in America collected funds for another gram of radium. Madame Curie died of leukemia on July 4, 1934. Sixty years after her death her remnants were laid to rest under the dome of the Pantheon. Thus she became the first woman under her own merit, to rest in the Pantheon. In 1934 at the Institute of Radiology in Paris, Frederique Joliot and Irene Curie-Joliot discovered artificial radiation. They studied alpha particles and beta;-radiation.     

食品中天然铀和钍的三正辛胺萃取-分光光度法联合测定研究

目的 建立食品中天然铀和钍联合测定的方法。 方法 基于N235萃取-分光光度法和三正辛胺(TOA)与N235的化学类似性,通过以TOA代替N235完成了必要的条件实验研究并获得了主要分析步骤的最佳条件。集合所获各项最佳条件,建立了本法的实验程序的方法学依据并对所建方法进行了验证。 结果 本方法对Th和U的最低探测限分别为3.47×10^-8 g/g灰和 9.47×10^-8 g/g灰。Th和U的加标回收率分别为98.7%和96.7%,相对标准偏差分别为±5.95%和±6.31%。对主要种类食品样品的铀、钍含量进行了测定,其化学回收率为70%～90%。结论 首次建立了食品中三正辛胺萃取-分光光度法作为天然铀、钍联合测定的方法。本法简便快速、准确度和精密度好。     

Gamma absorptiometric technique employing high resolution gamma spectrometry

Gamma absorptiometric method was used to determined uranium and thorium concentration in both aqueous and organic solutions. The complete computer-based γ-spectroscopy system includes a coaxial Ge(Li) detector used to measure the absorption of γ-rays from ²⁴¹Am through the solutions. The absolute concentration of natural uranium and thorium can be determined within 1–200 g U/L and 1–360 g Th/L concentration ranges with a precision of ± 1% for a counting time of up to 100 s with the result that the method is suitable for on-line measurement in fuel element fabrications.     

Use of three new SSNTD methods for evaluating thorium contents in different building materials and measuring thoron and its progeny concentrations inside dwellings.

Three new methods based on using CR-39 and LR- 115 type II solid state nuclear track detectors (SSNTD) were used for measuring thorium concentrations (in 10(-6)g/g (ppm)) inside different building materials and evaluating the resulting concentrations of thoron and its progenies in dwellings built by the studied materials. The first technique consists of determining the probabilities for alpha-particles emitted by the uranium and thorium series inside the building materials or by the radon and thoron groups inside the dwelling atmosphere to reach and be registered as tracks on the SSNTD utilized and exploiting the resulting track density rates. The second method consists of evaluating the mean critical angles of etching of the CR-39 and LR-115 II SSNTD and measuring the resulting track densities registered on the detectors utilized. The third technique is based on calculating the detection efficiencies of the CR-39 and LR-115 II SSNTD for a-particles emitted by the uranium and thorium series in the building materials or by the radon and thoron groups in air and measuring track density rates registered on these detectors. The influence of the building material's nature and ventilation rate on the thoron and its decay products inside the dwelling rooms studied has been investigated.     

Automated measurement of 224Ra and 226Ra in water.

We present a new simple approach for automated, non-destructive measurement of the alpha-emitting radium isotopes ((223)Ra, (224)Ra, and (226)Ra) in water based on the emanation of their respective radon daughters ((219)Rn, (220)Rn, and (222)Rn). The method combines the high adsorption uptake of MnO(2) Resin for radium (K(d)=2.4 x 10(4)ml/g) over a wide pH range with the simplicity of the activity registration using a commercial radon-in-air analyzer (RAD7, DURRIDGE Company, Inc). Radium is first adsorbed onto the MnO(2) Resin by passing a water sample through the resin packed in a gas-tight glass cartridge. The same cartridge is then connected to the radon analyzer via a simple tubing system to circulate air through the resin and a drying system. The efficiency of the proposed system is determined by running standards prepared in the same manner. Our results indicate that the efficiency for (226)Ra is >22% if both (218)Po and (214)Po counts are collected. This is comparable with typical efficiencies for alpha spectrometry but with much less sample preparation. We estimate that an MDA of 0.8 pCi/L for (226)Ra may be obtained with this new approach using a 1L water sample and less than 4h of counting.