Separation of Uranium Mixing with its Decayed Nuclides and its Activated Nuclides

Extractions of uranium from the acidic media, HCl and MNO₃ at different concentrations, by the tertiary amines, trilaurylamine, triisooctyllamine and trioctylamine were systematically investigated. In experiments, ²³²U was used as the tracer and aliquots of both phases after extractions were taken, ashed at 500°C, placed onto stainless steel planchets, and measured by a surface-barrier Si(Li) detector connected to an alpha spectrometer. One unique condition found useful for complete separation of uranium was that of the radioactive uranium present in 8 M HCl being extracted with 10% trilaurylamine in xylene. In that case, greater than 95% of the uranium could be extracted into the organic solution, whereas all of the radionuclides of a series of its decayed products, ²²⁸h, ²²⁴Ra, ²²⁰Rn, ²¹⁶Po and ²¹²Bi remained completely in the aqueous solution. The same procedure could also be used for the separation of uranium from a mixture with its activated nuclides. Plutonium-239 and Am were used as the tracers representing the activated nuclides of uranium. It was found that ²⁴¹Am was absolutely not extracted, but that ²³⁹Pu could be extracted with ≥95% efficiency from the medium of 8 M HCl into 10% trilaurylamine in xylene. However, ²³⁹Pu could be easily stripped using the solution mixture of 8 M HCl and 0.05 M NH₄I and excluded from the organic solution.     

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.     

Rapid <Superscript>224</Superscript>Ra measurements in water via multiple radon detectors

We introduce an improved on-site rapid analysis system for measuring ²²⁴Ra in natural waters. Radium isotopes are pre-concentrated on “Mn-fibers” before measurement of ²²⁰Rn. A Nafion drying system is used to lower the humidity in the detectors while maintaining a relatively constant moisture level in the Mn fiber in order to maintain a high and reproducible radon emanation. River water samples measured by this method agreed well with an analysis via RaDeCC, a very sensitive technique for measuring ²²⁴Ra. This method is recommended for fieldwork in remote areas when electricity and helium gas, required by traditional techniques, are not available.     

A new method for the determination of radium-228, thorium-228, and radium-224 in groundwaters via thoron (radon-220)

Current techniques for determining low levels of dissolved thorium involve chemical separations, generally by coprecipitation with a carrier cation, purification by ion exchange procedures, electroplating and, finally, alpha counting by alpha spectrometry. Similarly, measurements of low²²⁸Ra and²²⁴Ra activities requires concentration, by coprecipitation with barium sulfate, followed by gamma counting. An improved method for determining radium and thorium from the²³²Th decay series has been developed which measures the activity of²²⁰Rn as an assay of its parents. Although some ingrowth corrections and minor separation procedures for Th are required, the results to date show that the dynamic counting of²²⁰Rn via de-emanation and alpha counting by the alpha-scintillation method is a preferable approach for determining these radium and thorium isotopes accurately and efficiently. The method for lower limit detection depends on the emanation rate, which depends on purge-gas flow rate and sample volume analyzed. Using 50-cc and 1000-cc bubblers, and maximum effective purge gas flow rate, a lower limit of detection of 0.4 and 0.06 pCi/L²²⁰Rn can be obtained, respectively.     

Assessment of inhalation exposure potential of broken uranium ore piles in low-grade uranium mine

This paper presents the assessment of inhalation exposure potential of broken uranium ore piles in different stopes of Jaduguda uranium mines of India. ²²²Rn emanation coefficient of broken uranium ore was measured in laboratory by collecting air sample from airtight glass jar containing ore sample. An attempt was also made to correlate the emanation coefficient with ²²⁶Ra content of the ore. The ²²²Rn progeny doses estimated based on radon activity concentration of broken ore, occupancy period and equilibrium ratio in different stopes were well below the prescribed limit of International Commission on Radiological Protection. The maximum ²²²Rn progeny dose contribution from broken ore piles was worked out to be 0.22 mSv year^?1. This suggests that the broken ore piles are not the significant contributor of inhalation exposure under the existing ventilation condition of Jaduguda uranium mine.     

Radioactive contamination of the environment as a result of uranium production: a case study at the abandoned Lincang uranium mine,Yunnan Province,China

The distribution of radioactive pollutants, such as²²²Rn, U, Th and²²⁶Ra in the air, surface waters, soils and crops around the Lincang uranium mine, Yunnan Province, China, is studied. The mechanical, geochemical and biogeochemical processes responsible for the transport and fate of the radioactive elements are discussed based on the monitoring data. The pollutants concentrations of effluents from the mine tunnels were dependent on pH and which were controlled by biochemical oxidation of sulfide in the ore/host rocks. Radon anomalies in air reached 4 km from the tailings pile depending on radon release from the site, topography and climate.²³⁸U and²²⁶Ra abnormities in stream sediments and soil were 40—90 cm deep and 790—800 m away downstream. Anomalies of radioactive contaminants of surface watercourses extended 7.5—13 km from the discharge of effluents of the site mainly depending on mechanical and chemical processes. There were about 2.86 ha rice fields and 1.59 km stream sediments contaminated. Erosion of tailings and mining debris with little or no containment or control accelerated the contamination processes.

     

Radioactive contamination of the environment as a result of uranium production: a case study at the abandoned Lincang uranium mine,Yunnan Province,China

The distribution of radioactive pollutants, such as²²²Rn, U, Th and²²⁶Ra in the air, surface waters, soils and crops around the Lincang uranium mine, Yunnan Province, China, is studied. The mechanical, geochemical and biogeochemical processes responsible for the transport and fate of the radioactive elements are discussed based on the monitoring data. The pollutants concentrations of effluents from the mine tunnels were dependent on pH and which were controlled by biochemical oxidation of sulfide in the ore/host rocks. Radon anomalies in air reached 4 km from the tailings pile depending on radon release from the site, topography and climate.²³⁸U and²²⁶Ra abnormities in stream sediments and soil were 40—90 cm deep and 790—800 m away downstream. Anomalies of radioactive contaminants of surface watercourses extended 7.5—13 km from the discharge of effluents of the site mainly depending on mechanical and chemical processes. There were about 2.86 ha rice fields and 1.59 km stream sediments contaminated. Erosion of tailings and mining debris with little or no containment or control accelerated the contamination processes.     

Determination of the radon diffusion coefficient and radon exhalation rate in Moroccan quaternary samples using the SSNTD technique

Measurements have been made of radon (²²²Rn), release from diverse quaternary samples collected from different sediment deposits in the Errachidia and Beni-Mellal areas (Morocco). The radon diffusion coefficient as one of some important parameters of radon transport in the soil has been measured using solid state nuclear track detectors (SSNTD). Radon -activity, uranium content and radon exhalation rate have been determined in the studied samples. Uranium concentrations were found to vary from 0.14 to 9.52 ppm whereas the radon exhalation rate varied from 0.003 to 0.145 Bq^.m^-2.h^-1. A positive correlation has been found between radon exhalation rate and uranium content in the studied samples. The average radon diffusion coefficients were found to vary from (1.26±0.09)^.10^-6 m^2.s^-1 to (4.3±0.36)^.10^-6 m^2.s^-1. Furthermore, the correlation between ²²²Rn diffusion coefficient and porosity are also discussed.     

Determination of macroconstituents and trace elements in naturally occurring radioactive material in oil exploration waste products

Naturally occurring radioactive materials (NORM) contain radionuclides, such as radium, thorium, and uranium. The existence of NORM remains an issue for oil and gas exploration because once the material becomes concentrated through technological activity, it becomes a radioactive contamination hazard or a radioactive waste. Pipes and tanks used to handle large volumes of produced water at some oil-field sites are coated with scale deposits that contain high levels ²²⁶Ra, ²²⁸Ra and ²¹⁰Pb. Experiments were conducted using thermal and epithermal neutron activation analysis and Compton suppression for the determination of macroconstituents and trace elements in the radioactive scale sample.     

Pre-concentration of short-lived radionuclides using manganese dioxide precipitation from surface waters

Rapid determination of ²²²Rn and ²²⁰Rn progeny (²¹⁴Pb, ²¹²Pb, ²¹⁴Bi, ²¹²Bi) is achievable using manganese dioxide (MnO₂) precipitation with analysis by γ-spectrometry. This is of interest to environmental monitoring programmes that utilise gross activity methods to screen for anthropogenic radionuclides. The contribution from these naturally occurring radionuclides (NOR) varies, and is difficult to experimentally measure due to short half-lives (t _½ = 19.9 m–10.64 h) and low environmental activity (<0.1 Bq L^?1). The extraction efficiency of the technique is above 90%, and above 80% for other nuclides (²³²Th, ²³⁸U, ²³⁵U, ²²⁸Ac, ²²⁶Ra, ²²⁴Ra, ²¹⁰Pb, ⁵⁴Mn). Short-lived NOR have been measured at two surface water locations, and indicates elevated ²¹⁴Bi activity of 4.0 ± 1.1 Bq L^?1.     

Study of the Energy Resolution in Alpha-Particle Spectra from Electrodeposited Radium Sources

Electrodeposited ²²⁶Ra sources were prepared and measured in order to perform a detailed study of the energy resolutions attained with two recent electrodeposition procedures for preparing spectrometric radium sources. The values of the energy resolution for the high-energy emission of ²²⁶Ra and for the single-emissions of ²¹⁰Poand ²²²Rn were calculated by fitting the data with a curve formed by the convolution of two left-handed exponentials with a Gaussian function. Significant differences between the energy resolutions for the aforementioned radionuclides were observed. The ²¹⁰Po energy resolutions were, in general, somewhat better than those obtained for ²²⁶Ra. On the contrary, the energy resolutions found for ²²²Rn were notably poorer than those obtained for ²²⁶Ra and ²¹⁰Po. These discrepancies can be satisfactorily explained by taking into consideration the distribution of these nuclides in the sources and the effect of radon diffusion involved in this type of thin deposit.     

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.     

The determination of mercury by non-flame atomic absorption and fluorescence spectrometry.

An isotopic dilution method has been developed for the determination of ²²⁶Ra and ²²⁸Ra in sea water and sediments with ²²³Ra as a yield tracer. An alternative procedure which obviates the need for ²²³Ra is demonstrated for sediments by the assay of ²²⁴Ra and ²²⁸Th which occur naturally in sediments. In addition, a direct method for β-counting ²²⁸Ra–²²⁸Ac is proposed. Radium, polonium, thorium and uranium isotopes and ²¹⁰Pb are coprecipitated from sea water with aluminum phosphate carrier. The radium and lead-210 are coprecipitated with lead nitrate in sediment leachings. All radium procedures utilize identical chemical isolation and the cathodic electrodeposition of radium. Subsequently, the α-radiation emitted by ²²⁶Ra, ²²³Ra and ²²⁴Ra is determined by pulse-height analysis: the ²²⁸Ra-²²⁸Ac and ²¹⁰Pb-²¹⁰Bi are measured by low background anticoincidence β-counting techniques. This method was used for samples containing 10^-11–0.5 · 10^-12 g of ²²⁶Ra and 10^-13–10^-15 g of ²²⁸Ra and gave a precision of 3–6% and 5–10% respectively, even though radium levels an order of magnitude less can be measured. The ²²⁶Ra method is applicable to all environmental samples, whereas ²²⁸Ra determinations are limited to applications where the ${}^{228}\text{Ra}{}^{226}\text{Ra}$ activity ratio is greater than 0.1. This method is especially attractive for studies of parent-daughter disequilibria.     

Validation of the quantification of natural radionuclides in raw materials and by-products using gamma-ray spectrometry

The validation of a method for the indirect quantification for ²³⁸U, ²²⁶Ra, and ²³²Th activity and the direct quantification for ⁴⁰K activity using gamma-ray spectrometry was performed in view of consistency, reliability, and accuracy of the results. The gas tightness of Al containers used to confine the radon gas was verified from the establishment of the secular equilibrium between ²²⁶Ra and its indicator. To evaluate validation parameters such as linearity, range, and accuracy, it was important to verify the equilibrium state of the reference materials (RM) for U and Th, because the ingrowth of progenies in the uranium decay series can affect the quantification of ²²⁶Ra activity even if based on a certified reference material (CRM), while the ingrowth of ²²⁸Ra from the thorium decay series should be secured in order to use ²²⁸Ac as an indicator of ²³²Th. In addition, the ruggedness of the method regarding different materials was checked using two kinds of CRM, namely bauxite as an example of a raw material and coal fly ash as a by-product.     

Two new methods of determining radon diffusion in fish otoliths

Otoliths are bony structures found in the ears of fish and used in the²¹⁰Pb/²²⁶Ra dating method for age determination. This paper checks the assumption that²²²Rn is not lost from or added to orange roughy fish otoliths by diffusion, which would invalidate the technique. The first method of monitoring diffusion relies on measuring the gamma activity of daughter radionuclides. Otoliths were exposed to an atmosphere enriched in²²²Rn for 10 days, and the supported gamma activity inside them measured allowing for various decay corrections. The calculated radon addition was (0.5±0.5)% of the activity of the²²⁶Ra present. The second method used an alpha spectrometer and attempted to detect²²²Rn directly outgased from otoliths in the detector vacuum chamber. The results were consistent within errors with those of the first method and showed no loss or gain of²²²Rn, supporting previous estimates of a long life-span for the orange roughy. In contrast it was found that approximately 10% of²²²Rn formed in orange roughy fish scales was lost to an evacuated environment, (hence perhaps to an aqueous environment) and that for this species it could be difficult to base a dating method on analysis of scales. Nevertheless a preliminary minimum age of 57 years was obtained. The methods could be used with non-biological samples to determine²²²Rn diffusion rates.     

Determination of radium isotopes in soil samples by alpha-spectrometry

A sensitive and accurate method for determination of radium isotopes in soil samples by α-spectrometry has been developed ²²⁵Ra, which is in equilibrium with its mother ²²⁹Th, was used as a yield tracer. Radium in soil samples was fused together with Na₂CO₃ and Na₂O₂ at 600 °C, leached with HNO₃, HCl and HF, preconcentrated by coprecipitation with BaSO₄, separated from uranium, thorium and iron using a Microthene-TOPO chromatographic column, isolated from barium in a cation-exchange resin column using 0.05M 1,2-cyclohexylene-dinitrilo-tetraacetic acid monohydrate as an eluant, electrodeposited on a stainless steel disc, and counted by α-spectrometry. The detection limit of the method is 0.43 Bq·kg⁻¹ for ²²⁶Ra, ²²⁸Ra and ²²⁴Ra if 0.50 g of soil sample are analyzed. The method was checked with two certified reference materials supplied by the IAEA, and reliable results were obtained Fourteen soil samples collected from the refractory industry in Italy were also analyzed. The mean radiochemical yields for radium were 85.7±4.3%, and the obtained radium concentrations in the soil samples were in the range of 8.08–3878 Bq·kg⁻¹ for ²²⁶Ra, of 1.60–678 Bq·kg⁻¹ for ²²⁸Ra and 1.25–550 Bq·kg⁻¹ for ²²⁴Ra, with ²²⁸Ra/²²⁶Ra and ²²⁴Ra/²²⁶Ra ratios ranged from 0.159–0.821 and from 0.142 to 0.525, respectively.     

Selective determination of extremely low-levels of the thorium series in environmental samples by a new delayed coincidence method

An attempt was made to apply a delayed coincidence method for the absolute determination of trace quantities of the thorium series. This method is based on selective counting of the relatively short lived nuclide²¹⁶Po (half-life 145 ms) in the thorium series members. For this purpose, a list mode time analyzing system combined with a liquid scintillation counter was assembled by means of a conventional microcomputer. A multiple time analysis was employed in the processing and data compilation of delayed coincidences to distinguish them from the true coincidences due to random events.From a time spectrum, the decay component of²¹⁶Po (145 ms) can be selectively measured. Absolute activities of its progenitors,²²⁴Ra and²²⁸Th as well as²²⁰Rn, can be determined even in the presence of the background radiations of the almost equivalent activity-strength of concomitant uranium series.     

Determination of plutonium and americium in environmental samples and assessment of thorium in bone samples from normal and high background areas

The procedures developed and standardised for estimation of ultra trace quantities of Pu and Am in environmental samples involve matrix dependent sample preparation, preconcentration of the nuclides by coprecipitation on iron hydroxide and or bismuth phosphate, ion exchange, electrodeposition and counting by alpha spectrometry. Isotopic analysis of Th in chicken bone using oxalate precipitation, ion exchange, electrodeposition and alpha spectrometry has indicated higher build up of²²⁸Th in chicken bone from monazite areas possibly from metabolized²²⁸Ra.     

Radon emanometric technique for 226Ra estimation

Studies on natural background radiation show that the major contribution of radiation dose received by population is through inhalation pathway vis-à-vis contribution from radon (²²²Rn) gas. The immediate parent of radon being radium (²²⁶Ra), it is imperative that radium content is measured in the various matrices that are present in the environment. Among the various methods available for the measurement of radium, gamma spectrometry and radiochemical method are the two extensively used measurement methods. In comparison with these two methods, the radon emanometric technique, described here, is a simple and convenient method. The paper gives details of sample processing, radon bubbler, Lucas cell and the methodology used in the emanometric method. Comparison of emanometric method with gamma spectrometry has also undertaken and the results for a few soil samples are given. The results show a fairly good agreement among the two methods.     

Estimation of growth rate of hokutolite from Tamagawa hot-spring,Akita, Japan

The concentrations of radium isotopes and the progenies (²²⁶Ra; ²²⁸Ra and ²²⁸Th) in three hokutolite samples from Tamagawa hot-spring were measured. These isotopes were analyzed by a well-type HPGe γ-ray spectrometer for the 351, 911 and 583 keV γ-ray from ²¹⁴Pb, ²²⁸Ac and ²⁰⁸Tl, respectively, each being in radioactive equilibrium with precursors. Concentration of ²²⁶Ra and ²²⁸Ra were observed to be in the range of 52–85 and 7.1–85 Bq/g, respectively. The activity ratios of ²²⁸Ra/²²⁶Ra and ²²⁸Th/²²⁶Ra provided the estimation of the growth rate (0.09–0.15 mm/y). Estimated ²²⁸Ra/²²⁶Ra activity ratios in hot-spring water from surface of three hokutolite were concordant.