Experimental investigation of cesium mobility in the course of secondary mineral formations in Hanford sediment columns at 50°C

Formation of secondary minerals and Cs mobility in Hanford sediments were investigated under conditions similar to the Hanford tank leak in a dynamic flow system at 50°C. The objectives were to (1) examine the nature and locations of secondary mineral phases precipitated in the sediments and (2) quantify the amount of Cs retained by the sediment matrix at 50°C. To this end, Hanford sediments were packed into 10-cm long columns and leached with simulated tank waste consisting of 1.4 M NaOH, 0.125 M NaAlO₂, 3.7 M NaNO₃, and 1.3 × 10^???4 M Cs at 50°C. Compositions of outflow solution were monitored with time for up to 25 days, and the columns were then segmented into four 2.5-cm long layers. The colloidal fraction in these segments was characterized in terms of mineralogy, particle morphology, Cs content, and short-range Al and Si structure. It was observed that cancrinite and sodalite precipitated at 50°C. Approximately 53% Cs was retained in the column treated by the simulated tank waste at this temperature. Cesium retention in the column was lowered in the high ionic strength solution due to competition from Na for the exchange sites. This can be explained by alteration of distribution and number of sorption sites which reduces the selectivity of Cs for Na, and through the formation of cancrinite and sodalite. The formation of hydroxide complexes in highly alkaline solutions could also contribute to relatively poor retention of Cs by hindering ion exchange mechanism.     

The influence of pH and temperature on the aqueous geochemistry of neodymium in near surface conditions

Geochemical calculations were employed for the solubility and speciation of neodymium in a model soil solution as a function of pH. The calculations were based on the recently determined stability constants for Nd and solubility product for the Nd end-member of mineral monazite (NdPO(4)). Simulations were carried out at near neutral pH (pH 6.0 to pH 7.5) and 25 degrees C at the atmospheric CO(2) partial pressure. Additional calculations were also performed to assess Nd mobility at the extreme temperature conditions (300 degrees C) at neutral pH. Our results suggest that relatively dilute (Ionic Strength, I = 0.1), low-temperature waters may transport very small quantities of rare earth elements and actinides to the surficial environment at near neutral pH conditions. Evidently, higher temperature or extreme fluid composition may have a greater potential for mobilization of these elements. The results are pertinent to researchers interested in engineering applications for the precipitation of Nd and surrogate actinides from aqueous nuclear wastes.     

Geochemical and radionuclide profile of Tuzla geothermal field, Turkey

Tuzla geothermal basin is situated in north-western Turkey on the Biga Peninsula, which is located at the west end of the Northern Anatolian Fault system. Soil and water samples were collected between August 2003 and June 2004 to initiate development of a geochemical profile of surface and subsurface waters in the geothermal basin and radionuclide concentrations in soils. All water samples were found to fall within Turkish Water Quality Class 4, meaning they were remarkably contaminated for any water consumption sector (industrial, human use or agricultural) based on sodium and chloride ions. Such waters could be used only after appropriate water treatment. The water samples are of the chloride type in terms of geochemical evaluation. Preliminary geochemical evidence shows that the N-S flowing part of the Tuzla River acts as a natural barrier within the basin. Heavy metal concentrations in the soil samples show slight elevations, especially those obtained from the east part of the basin where thermal springs are dominant. Geochemical calculations were carried out with PHREEQC software to determine equilibrium concentration of chemical species and saturation indices, by which it is suggested that chloride is the most important ligand to mobilize the heavy metals in the studied system. In addition, the activity concentration and gamma-absorbed dose rates of the terrestrial naturally occurring radionuclides were determined in the soil using gamma-ray spectrometry. The soil activity ranged from 42.77 to 988.66 Bq kg(-1) (averaging 138 Bq kg(-1)) for ( 238 )U, 13.27 to 106.31 Bq kg(-1) (averaging 32.42 Bq kg(-1)) for ( 232 )Th, and 99.28 to 935.36 Bq kg(-1) (averaging 515.44 Bq kg(-1)) for ( 40 )K. The highest value of ( 238 )U was found in the soil samples obtained from an area close to the hot spring.