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.     

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.     

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.     

224Ra correction for determination of 226Ra in environmental materials

The most commonly available 226Ra determination was too time-consuming to be suited to 226Ra monitoring for the accidental release. The formula for determination of 226Ra was derived by 224Ra correction for WHO's equation. A rapid determination of 226Ra in environmental materials was made possible by using this formula. The 226Ra values of the soil and natural water at Ningyoh-Tohge obtained by the present method were in good agreement with those by the conventional WHO method. It was demonstrated that 226Ra of more than about 37 mBq (1 pCi) in the sample could be determined within 4 days by this method.     

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.     

226Ra, 228Ra and 210Pb Isotopes in Some Water Samples of Mines

A method for the determination of ²²⁶Ra, ²²⁸Ra and ²¹⁰Pb in water samples of mining regions by measuring the and intensities with the help of a liquid scintillation counter is presented. The high-energy part of the -particle spectrum emitted by ²¹⁰Bi is used for the determination of ²¹⁰Pb content in the samples. An attempt is also given to explain the radioactive disequilibrium between ²²⁶Ra and ²¹⁰Pb in the samples investigated.     

A new analytical approach for 226Ra and 228Ra in environmental waters

The concentration of Ra isotopes in environmental water can be determined from the amount of Ra isotopes recovered in two successive batch operations a using cation exchange resin. The present analytical method is applicable to 10 liter of sample water having a Ra concentration larger than 10 mBq/l and is also applicable to the ordinary underground water of less than 1 mBq/l by use of 50 liter of sample water. In case where Ra concentration is extremely low, Mn-impregnated acrylic fiber can be used with a larger volume of water sample as an absorbent by soaking it in the water.     

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.     

Treatment of an aqueous radioactive waste solution with elevated levels of226Ra and228Ra

Treatment of an aqueous radioactive waste solution to remove radium prior to discharge was conducted at a laboratory scale. The actual solution is mainly composed of combined radium (²²⁶Ra and²²⁸Ra) with high concentrations of manganese, iron and calcium, which are present as chlorides in dilute hydrochloric acid. Direct precipitation by sulfate anions was selected to be the more viable treatment technique. Sulfate anion concentration, free acidity, temperature and aging of the sulfate precipitate in the supernate prior to filtration are factors that were investigated for their effect on the separation efficiency. The data obtained are discussed in detail.     

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.     

Contribution to the simultaneous determination of228Ra and226Ra by using 3M's EMPORETM radium rad disks

New method for simultaneous determination of²²⁸Ra and²²⁶Ra by using 3M's EMPORE^TM Radium Rad Disks in water has been developed. Both radionuclides²²⁶Ra and²²⁸Ra were counted through their daughter products,²²⁶Ra by conventional radon emanation techniques and²²⁸Ra through its daughter²²⁸Ac by using a proportional counter. Different molarity of diammonium hydrogen citrate were used for elution of²²⁸Ac and²²⁶Ra from EMPORE^TM Radium Rad Disks. 79% of²²⁸Ac was eluted in 10 ml of 0.0003M diammonium hydrogen citrate. The recovery of²²⁶Ra was 99% by using 40 ml of 0.2M diammonium hydrogen citrate adjusted by ammonium to pH 7.8.     

Activity concentrations of 226Ra, 228Ra, 222Rn and their health impact in the groundwater of Jordan

The activity concentrations of ²²⁶Ra, ²²⁸Ra and ²²²Rn were measured in 87 groundwater samples to estimate the activity concentrations of these radionuclides and health impact due to intake of these radionuclides in groundwater of Jordan. The mean activity concentrations of ²²⁶Ra, ²²⁸Ra and ²²²Rn in groundwater were found to be 0.293?±?0.005 Bq L^?1, 0.508?±?0.009 Bq L^?1 and 58.829?±?8.824 Bq L^?1, respectively. They give a mean annual effective dose of 0.481 mSv with mean lifetime risk of 24.599?×?10^?4, exceeding the admissible limit of 10^?4. Most of the received annual effective dose (59.15% of the total) is attributed to ²²⁸Ra.

     

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.     

Factors affecting the electrodeposition of226Ra

The electrodeposition of²²⁶Ra for -spectrometry was reinvestigated to improve reproducibility and yield. Electrodeposition is from 20 ml of 90% propan-2-ol10% 0.05M HNO₃ onto stainless steel disks, using 100 mA at 35 V for 20 minutes and a platinum anode. Half deposition time is 3–4 minutes. The following factors were found important: 1. Maintaining the same anode position. 2. Rotation of cathode. 3. Exclusion of sulphate. 4. Avoiding heating the HNO₃/propan-2-ol plating solution. 5. Exclusion of solubilised resin resulting from passage through ion-exchange columns. 6. Maintaining other impurities at less than 10 g. If these precautions are followed yields are greater than 90%.     

The226Ra/Ba-ratio as indicator for phosphogypsum contributions to226Ra levels in sediments

Phosphogypsum discharges by phosphate-ore processing industries pollute sediments of the Rotterdam harbour area with²²⁶Ra. Direct measurement of this radionuclide in sediments does not provide a reliable indication of the elevation of the levels, since²²⁶Ra levels in sediments depend on the particle size. To eliminate the size effect, the²²⁶Ra/Ba ratio in sediments was tested as a possible indicator for the²²⁶Ra in the discharges. The results indicate almost a doubling of the²²⁶Ra levels in sediment samples due to phosphogypsum discharges. The contribution of phosphogypsum to the sediment mass was calculated in the order of a few percent equivalent.     

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.