On the solubility of radium sulfate and carbonate
Radium is one of the most toxic elements and its concentration in different human activities and migration from man-made wastes provokes a strong interest in environmental science. To be able to model the migration process, reliable experimental thermodynamic data of radium compounds are needed.
In this work details of the safe radium source disassembly which were previously used in brachytherapy are described and different methods for conversion of RaSO4 into aqueous solution are reviewed. The method of choice included three cycles of RaSO4 heating in 1.5 M Na2CO3 up to 85 oC, cooling and subsequent removal of supernatant. X-ray diffraction studies showed that the method allows the synthesis of amorphous RaCO3, which can be dissolved in mineral acid. Gamma spectrometric measurements showed that most of the initial RaSO4 was converted into solution and that 7 ± 1 % of the initial 210Pb was co-precipitated with RaCO3. Synthesized RaCO3 was dissolved in HCl to prepare a radium stock solution. 
The radium stock solution was used to determine the solubility of pure RaSO4 and RaCO3 from oversaturation using Na2SO4 and Na2CO3 as a source of sulfate and carbonate ions. The solubility was determined at 25.1 oC as a function of ionic strength using NaCl media. The concentration of radium was measured by gamma spectrometry after separation of the aqueous phase from the solid phase using ultracentrifugation. The extended specific ion interaction theory was used to extrapolate solubility product constants to zero ionic strength (log10 Ksp° = -10.16 ± 0.05 for RaSO4 and log10 Ksp° = -7.73 ± 0.56 for RaCO3) and to calculate ion interaction coefficients.
A comparison of the shapes of the radium solubility curves for both anions with the shapes of corresponding barium solubility curves demonstrates the similarity of the behaviour of radium and barium salts in saline solutions. It can be supposed that due to the similarity of the radium and barium effective ionic radii, and the same charge, these ions undergo similar specific ion interactions in NaCl media.
Radium and strontium binding by a modified bauxite refinery residue – isotope exchange studies of pH-dependence, reversibility and ageing
The pH-dependence and reversibility of radium (Ra) and strontium (Sr) binding to a modified bauxite refinery residue (MBRR), and the effects of sample ageing, were studied in laboratory uptake/leaching experiments. Natural 226Ra and stable strontium (Srnat) were placed in contact with the MBRR for an 8-day loading period (equilibrium pH c. 8.5). Following the addition of exchange isotopes 228Ra and 85Sr, the samples were then leached in pH-dependent experiments, where the pH was decreased incrementally from 9 to 3 over 7 h. A further suite of samples was aged at 4°, 23° and 65°C for 6 months after the initial addition of 226Ra and Srnat and then studied in a similar set of pH-dependent exchange experiments. The relative concentrations of the Ra and Sr isotope pairs (226Ra/228Ra and Srnat/85Sr) provided insights into the adsorption strength, incorporation, reversibility and ageing effects. The Srnat data showed that the amount of bound Sr released from aged MBRR samples as the pH decreases is substantially lower than the unaged sample, showing that Sr has been incorporated in less accessible phases during the ageing period. It appears that the uptake of 228Ra by the higher-temperature aged samples is somewhat stronger than the unaged samples; however, Ra isotope exchange plots for aged and unaged samples are similar. Consequently, the stronger binding of 228Ra by the higher-temperature aged samples is probably driven by translocation to kinetically less-favourable surface sites rather than a significant incorporation of Ra within the mineral solids during ageing.
Studies on the Leaching of Radium and the emanation of radon from fertilizer process sludge
Abstract Radium-226 present in rock phosphate is carried to CaCO 3 , the main process waste sludge of the fertilizer industry. Disposal of the sludge in the environment enhances the radiation background in the area. Two states of adherence of radium in the sludge have been identified, one loosely bound and the other chemically exchanged. The loosely bound fraction accounts for nearly 40% of the total activity, as demonstrated by leaching studies. Laboratory experiments show that activity leach-out by infiltration of water through the sludge is low. Lateral seepage is found to cause extensive areal contamination due to dispersal of suspended solids in the vicinity of the disposal area. The rate of emanation of radon from the sludge is found to be high, a factor of 10 over the normal background emanation rate. The radiation field in the waste disposal area also shows enhancement, with levels 4–6 times higher than natural background.