Recrystallization of 223Ra with barium sulfate

In this work, the kinetics of barium sulfate recrystallization has been studied in acidic 0.01 mol dm^?3 sodium sulfate solution using ²²³Ra and ¹³³Ba tracers at very low total radium concentration, i.e. less than 10^?13 mol dm^?3. It was found that the system follows the homogeneous recrystallization model and that recrystallization rates, inferred by the decrease of ²²³Ra and ¹³³Ba in the aqueous solution, are fast. Therefore, even at very low concentrations, below the solubility limit, radium will be retained by barium sulfate—a mineral present in the deep underground repository.     

Separation and electrodeposition of226Ra

The chemical behavior of calcium, barium and radium in the ion exchange resins Dowex 50W-X8, AG 50W-X8 and Merk I in the presence of ammonium tartrate, EDTA, and citrate has been studied. No differences were observed in results while using any one of the three resins. Calcium, barium and radium were fixed to the exchange column at pH 4.8 EDTA solution. Calcium was eluted in an EDTA solution at pH 5.3, barium and radium between pH 8–11. Elution in citrate media for calcium was achieved at pH 6.1 and for radium at pH 10. In ammonium tartrate, calcium was eluted at pH 6, barium and radium at pH 11.5. Radium was also eluted from the ion exchange resins with a 2M nitric acid solution. The radium free of calcium was electrodeposited onto a stainless steel disc cathode using a 0.1 M potassium fluoride solution, pH 12–14, with a yield of >50%. The energies of²²⁶Ra were analyzed through high resolution -spectra. The²²⁶Ra utilized for these experiments was separated from Mexican carnotite.     

Marine radioactivity concentration in the Exclusive Economic Zone of Peninsular Malaysia: 226Ra, 228Ra and 228Ra/226Ra

The present occurrence of ²²⁶Ra and ²²⁸Ra in marine sediment core and fish from the Exclusive Economic Zone in the east coast of Peninsular Malaysia were studied. Sediment core and biota in respectively was collected using multicorer device and purchased from local fishermen at identified stations during the cruise expedition conducted in 2008. The purpose of this study was to determine and to make available an inventory of activity concentration levels and activity ratio for these radionuclides in this region. The activity concentrations of ²²⁶Ra and ²²⁸Ra in sediment core and edible part of fish were ranged between 15.9–46.5 and 27.7–87.1 Bq/kg dry wt and; 0.80–2.13 and <0.95–3.57 Bq/kg fresh wt, respectively. Meanwhile, the activity ratios of ²²⁸Ra/²²⁶Ra in sediment core and fish were varied with the range between 1.63–2.09 and 0.45–2.38, respectively. Refer to those ranges the activity concentrations of radium isotopes were comparable with other region. Thus, it can be concluded that the occurrence of radium isotopes mainly supplied from terrestrial sources and the factors of assimilation efficiency and transfer coefficient of radium may probably effect to the variation activity concentration of ²²⁶Ra and ²²⁸Ra and its activity ratio in edible part of pelagic and demersal fish obtained in this study.     

Assessment of 226Ra and 228Ra activity concentration in west coast of India

An investigation on the distribution of ²²⁶Ra and ²²⁸Ra activity concentration in coastal surface sea water from Okha in Gujarat to Ratnagiri in Maharashtra state along the west coast of India was carried out. In-situ pre-concentration technique was used to measure radium isotopes by passing 1,000 L of seawater through MnO₂ impregnated polypropylene filter cartridges at all the locations. ²²⁶Ra was estimated using gamma ray peak of its daughter radionuclides ²¹⁴Bi and ²¹⁴Pb. ²²⁸Ra was estimated from its daughter ²²⁸Ac. In the coastal waters, ²²⁶Ra and ²²⁸Ra activity concentration were observed to be in the range of 1.5–2.9 and 2.5–8.6 Bq m^?3 with a mean of 2.2 and 4.9 Bq m^?3 respectively. The activity of ²²⁸Ra was observed to be more than ²²⁶Ra in all the locations. The variation in spatial distribution of the radium isotopes activity concentration and its ratio with respect to location is discussed in the paper. The radioactive database obtained represents reference values for coastal environment of India.     

On the use of232U and its daughters for the determination of226Ra in water samples

The authors propose a method to determine 226Ra by using a solution of²³²U and its daughters in equilibrium as a tracer.²²⁴Ra of the²³²U solution can be used as yield determinant for²²⁶Ra. The growth of²¹⁴Po from²²⁶Ra and of²¹²Po from²²⁴Ra is measured at different times after the isolation of the radium fraction.     

Removal of 226Ra from aqueous media and its thermodynamics and kinetics

The composite adsorbent prepared by mixing of polyacrylonitrile and clinoptilolite was used for investigating the adsorption behaviour of ²²⁶Ra in column system. The effective parameters like initial activity concentration, pH of the solution, contact time and temperature for adsorption behaviour of ²²⁶Ra were studied. Adsorption efficiency of ²²⁶Ra on composite adsorbent from aqueous solution was determined to 98.73 ± 0.59 % at pH 5.0 and 30 °C in a short time. The isotherm models were studied to evaluated adsorption characteristics of ²²⁶Ra onto composite adsorbent. The thermodynamic parameters were showing that the processes for ²²⁶Ra were exothermic. Adsorption kinetics of the radium is also studied.

     

Determination of228Ra in drinking water

A procedure for the analysis of²²⁸Ra in drinking water has been developed. The procedure involves separation of radium by an initial coprecipitation with lead sulfate. The isolated Pb(Ra)SO₄ is then dissolved in sodium diethylenetriamine pentaacetate (DTPA). Radium-228 is co-precipitated from this solution with barium sulfate while the DTPA supernate which contains pre-existing²²⁸Ac is discarded. The purified Ba(Ra)SO₄ precipitate is then allowed to ingrow, generating²²⁸Ac, which is then dissolved in DTPA, isolating both²²⁶Ra and²²⁸Ra in the precipitate while²²⁸ Ac remains in the aqueous supernate. The supernate is partitioned against di-(2-ethylhexyl phosphoric acid), HDEHP, dissolved in n-heptane, which retains the²²⁸Ac. Actinium-228 is then stripped from the organic phase by partitioning against 1M HNO₃. Finally, the²²⁸Ac is coprecipitated onto cerium oxalate. The precipitate is collected on a filter and counted in a low-background beta counter. Radium-228 standards with concentrations ranging from 0.044 to 1.6 Bq were used to establish the detector counting efficiency for²²⁸Ac in cerium oxalate samples, as well as monitoring the chemical yield and absorption factors. The resultant average value of 30.3±2.1 cpm/Bq (uncertainty given at 95% level of confidence) was obtained. Various²²⁸Ra cross checks from U. S. Environmental Protection Agency (EPA) with concentrations of 0.063–0.52 Bq/l were analyzed in order to assess the performance of the procedure. The minimum detectable concentration (MDC) of²²⁸Ra in water with this procedure is 0.015 Bq/l. This is based on a one liter aliquot of sample, a 100 min couting period, and a 3 hour decay interval between the end of²²⁸Ac ingrowth and midpoint of counting. Decontamination factor studies were performed to determine the extent of the carry-over of²³⁸U,²²⁶Ra,²¹⁰Po, and⁹⁰Sr into the final fraction.     

Rapid method for 226Ra and 228Ra analysis in water samples

Summary The measurement of radium isotopes in natural waters is important for oceanographic studies and for public health reasons. Radium-226 (T_1/2 = 1620 y) is one of the most toxic of the long-lived alpha-emitters present in the environment due to its long life and its tendency to concentrate in bones, which increases the internal radiation dose of individuals. The analysis of ²²⁶Ra and ²²⁸Ra in natural waters can be tedious and time-consuming. Different sample preparation methods are often required to prepare ²²⁶Ra and ²²⁸Ra for separate analyses. A rapid method has been developed at the Savannah River Environmental Laboratory that effectively separates both ²²⁶Ra and ²²⁸Ra (via ²²⁸Ac) for assay. This method uses MnO₂ Resin from Eichrom Technologies (Darien, IL, USA) to preconcentrate ²²⁶Ra and ²²⁸Ra rapidly from water samples, along with ¹³³Ba tracer. DGA Resin^ò (Eichrom) and Ln-Resin^ò (Eichrom) are employed in tandem to prepare ²²⁶Ra for assay by alpha-spectrometry and to determine ²²⁸Ra via the measurement of ²²⁸Ac by gas proportional counting. After preconcentration, the manganese dioxide is dissolved from the resin and passed through stacked Ln-Resin-DGA Resin cartridges that remove uranium and thorium interferences and retain ²²⁸Ac on DGA Resin. The eluate that passed through this column is evaporated, redissolved in a lower acidity and passed through Ln-Resin again to further remove interferences before performing a barium sulfate microprecipitation. The ²²⁸Ac is stripped from the resin, collected using cerium fluoride microprecipitation and counted by gas proportional counting. By using vacuum box cartridge technology with rapid flow rates, sample preparation time is minimized.     

Measurement of 222Rn and 226Ra in municipal supply tap water to evaluate their radiological impacts

ABSTRACT

Radon (²²²Rn) and its parent radionuclide Radium (²²⁶Ra) are classified as carcinogen. Human exposes to radon in water via inhalation and ingestion, although ingestion is the only way for radium to enter the human body. In this research, tap water collected from Bornova distinct was studied to determine the concentration of radon (²²²Rn) and radium (²²⁶Ra) for evaluating their radiological impact. For this reason, the annual effective doses for ingestion and inhalation were estimated. The measurements were performed using a collector chamber method. The mean concentrations of ²²²Rn and ²²⁶Ra were determined as 0.85 and 0.76 Bq/L, respectively. It can be stated that the ²²²Rn and ²²⁶Ra concentrations of tap waters here are lower than the international reference levels. Obtained concentration levels were applied to estimate annual effective dose due to the inhalation and ingestion. The dose values are also found to be lower than the recommended maximum values. On the other hand, it should be considered that consumption of these waters (2 L) and average radon and radium concentrations of water are the significant factors for estimating doses.     

226Ra, 228Ra and 228Ra/226Ra in surface marine sediment of Malaysia

Surface sediment samples were collected at the West (east coast and west coast of Peninsular Malaysia) and East (Sabah and Sarawak) Malaysia in several expeditions within August 2003 until June 2008 for determining the level of natural radium isotopes. Activity concentrations of ²²⁶Ra and ²²⁸Ra in surface marine sediment at 176 sampling stations were measured. The activity concentrations of both radionuclides in Malaysia (East and West Malaysia) display varied with the range from 9 to 158 Bq/kg dry wt. and 13 to 104 Bq/kg dry wt., respectively. Meanwhile, the ratio distributions of ²²⁸Ra/²²⁶Ra were ranged from 0.62 to 3.75. This indicated that the ratios were slightly high at west coast of Peninsular Malaysia compared to other regions (east coast of Peninsular Malaysia, Sabah and Sarawak). The variation of activity concentrations of ²²⁶Ra and ²²⁸Ra and its ratios were also supported by the statistical analyses of one-way ANOVA and t test at 95 % confidence level, whereby there were proved that the measured values were different between the regions. These different were strictly related to their half-life, potential input sources (included their parents, ²³⁸U and ²³²Th), parent’s characteristic, the geological setting/formation of the study area, environment origin and behavior.     

Rapid determination of 226Ra in environmental samples

A new rapid method for the determination of ²²⁶Ra in environmental samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used for emergency response or routine sample analyses. The need for rapid analyses in the event of a Radiological Dispersive Device or Improvised Nuclear Device event is well-known. In addition, the recent accident at Fukushima Nuclear Power Plant in March, 2011 reinforces the need to have rapid analyses for radionuclides in environmental samples in the event of a nuclear accident. ²²⁶Ra (T1/2?=?1,620?years) is one of the most toxic of the long-lived alpha-emitters present in the environment due to its long life and its tendency to concentrate in bones, which increases the internal radiation dose of individuals. The new method to determine ²²⁶Ra in environmental samples utilizes a rapid sodium hydroxide fusion method for solid samples, calcium carbonate precipitation to preconcentrate Ra, and rapid column separation steps to remove interferences. The column separation process uses cation exchange resin to remove large amounts of calcium, Sr Resin to remove barium and Ln Resin as a final purification step to remove ²²⁵Ac and potential interferences. The purified ²²⁶Ra sample test sources are prepared using barium sulfate microprecipitation in the presence of isopropanol for counting by alpha spectrometry. The method showed good chemical recoveries and effective removal of interferences. The determination of ²²⁶Ra in environmental samples can be performed in less than 16?h for vegetation, concrete, brick, soil, and air filter samples with excellent quality for emergency or routine analyses. The sample preparation work takes less than 6?h. ²²⁵Ra (T1/2?=?14.9?day) tracer is used and the ²²⁵Ra progeny ²¹⁷At is used to determine chemical yield via alpha spectrometry. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory radium particles are effectively digested. The preconcentration and column separation steps can also be applied to aqueous samples with good results.     

Study of the immobilization of226Ra

A study of the immobilization for²²⁶Ra waste has been carried out. Cement-based concrete was used as a matrix for the solidification of radium waste. The experimental results show that the cement mixture with water/cement between 0.46–0.54 has higher strengh (above 20 MPa), and the compressive strength was not reduced by addition of 1% barite or the radium waste (RaSO₄) into the concrete solid.Sponsored by the National Nuclear Corporation of China.     

Separation of Ra and Th from rock matrices for alpha-spectrometry

Dating rocks using²²⁶Ra/²³⁰Th isochrons demands radiochemical purification of radium and thorium. This paper presents an improved method. Rocks are solubilised by nitric/nydrofluoric digestion followed by dissolution of insoluble fluorides by boric/nitric acids, and Th is extracted by passing the 8M nitric solution through an anion column in nitrate form. The eluant contains Ra and Ba which are precipitated as sulphate and redissolved in alkaline EDTA. Complete separation of Ba and Ra from sulphate is on an AG 1×8 anion column in EDTA form, which was found better than the chloride form. The Ba+Ra is separated on an AG 50W×8 cation column, and uses CDTA as an eluant for Ba. Careful pH control is essential. Ra elutes later with EDTA or 4M HCl and is precipitated with 125 g barium as sulphate to yield a source suitable for -spectrometry, or further treated to electroplate the Ra. The yield tracers used are²²⁸Th and²²⁴Ra. Because the sample contains natural²²⁴Ra a correction must be applied, calculated from the amount of natural²³²Th in the Th spectrum. Th may be precipitated with 100 g of ferric iron and gives a spectrometry-quality source, but further purification and electrodeposition was found to be preferable. Variations on the method for the case of analysis of calcium-rich fish otoliths are described.     

<Superscript>226</Superscript>Ra and <Superscript>228</Superscript>Ra determination in environmental samples by alpha-particle spectrometry

A complete methodology for ²²⁶Ra and ²²⁸Ra determination by alpha-particle spectrometry in environmental samples is being applied in our laboratory using ²²⁵Ra as an isotopic tracer. This methodology can be considered highly suitable for the determination of these nuclides when very low absolute limits of detection need to be achieved. The ²²⁶Ra determination can be performed at any time after the isolation of the radium isotopes from the analyzed samples while the ²²⁸Ra determination needs to be carried out at least six months later through the measurement of one of its grand-daughters. The method has been validated by its application to samples with known concentrations of these Ra nuclides, and by comparison with other radiometric methods.     

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.     

Improvement of quality in the evaluation of radium isotopes 224,226,228Ra in oil scale samples

Elevated concentrations of the radium isotopes ^224,226,228Ra exist in the scale and produced water in oil exploration. The activity concentration of ²²⁶Ra was calculated from 186.2 keV peak with no usual spectral interference of 185.7 from ²³⁵U. The activity concentration of ²²⁸Ra was calculated from its first daughter product ²²⁸Ac using the 911.2 keV gamma rays since it is a pure beta emitter. The activity concentration of ²²⁴Ra was calculated from ²¹²Pb using the 238.6 keV gamma-ray and the secular equilibrium equation with ²²⁸Ra. The IAEA 448 (oil contaminated field soil) reference material was used as a quality control for ^226,228Ra and but was unreliable for ²²⁴Ra using ²¹²Pb.

     

Separation of228Ra from natural thorium oxalate

A simple and efficient method to isolate²²⁸Ra from natural thorium oxalate was developed. It consists in the coprecipitation of radium by hydrolysis of saturated solutions of ammonium thoroxalate followed by ion-exchange chromatography on Amberlite IR-120. The final product is carrier-free and pure enough for the preparation of thin sources for alpha and conversion electrons spectrometry. The radium coprecipitation utilized in the first step of this method, could be used to separate thorium from most of its radioactive daughters, decreasing the hazards of manipulation of large quantities of thorium.     

MSFIA-LOV system for Ra isolation and pre-concentration from water samples previous radiometric detection

An automatic system based on multisyringe flow injection analysis (MSFIA) and lab-on-valve (LOV) flow techniques for separation and pre-concentration of ²²⁶Ra from drinking and natural water samples has been developed. The analytical protocol combines two different procedures: the Ra adsorption on MnO₂ and the BaSO₄ co-precipitation, achieving more selectivity especially in water samples with low radium levels.     

Partition coefficient of Ra in gypsum

A partition coefficient (λ) for Ra in gypsum was determined from coprecipitation experiment using oversaturation method. The λ-value derived for Ra was: λ _Ra = 0.32±0.15. Saturation state was estimated with the initial concentration of Ca and SO₄²⁻ in an experiment of the present study. Saturation index was calculated to be (0.49±0.02). This value was similar to those corresponds to analogous case where slow precipitation rate was kept in coprecipitation experiment for Sr in gypsum. Therefore, derived λ-value is thought to describe partition of Ra and Ca in solid phase and solution under an equilibrium condition without the effect of kinetic of precipitation. Determined λ-value was compared with those of other alkaline elements in sulfate minerals. The derived λ-value is smaller than that of Ra in barite and is similar to those of Sr in gypsum. This trend agrees with mechanical understanding for the size effect against partition coefficient.     

On the determination of226Ra in soils and uranium ores by direct gamma-ray spectrometry

The evaluation of the source term in facilities related to the first stages of nuclear fuel involves the determination of radium concentration, as well as those from other radionuclides members of the uranium series. These activities are often required within a short time period, making impossible the use of radiochemical methods or the gamma-ray spectrometry of radium daughters. In those situations it can be very convenient to determine the²²⁶Ra activity by means of its 186 keV gamma-ray line. For this purpose it is necessary to estimate the interference due to²³⁵U, also present in natural samples. This method has been applied successfully to several soil samples from an old uranium factory in Southern Spain.