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Bosbach, Dirk; Boettle, Melanie; Metz, Volker
Swedish Nuclear Fuel and Waste Management Co., Stockholm (Sweden)2010
Swedish Nuclear Fuel and Waste Management Co., Stockholm (Sweden)2010
AbstractAbstract
[en] 226Ra2+ and 133Ba2+ uptake by barite in aqueous solution is studied on the basis of batch type experiments with two different barite powders with different specific surface area (0.5 m2/g and 3.2 m2/g, respectively). The uptake of 226Ra2+ and 133Ba2+ is not only limited to adsorption reactions but proceeds significantly into the bulk of the barite crystals. 133Ba2+ uptake kinetics is affected by various parameters, such as amount of sample, specific surface area, sample type and solution composition. In the case of 133Ba2+, complete isotopic equilibration of the 133Ba2+ spiked solution with the barite powder occurs within 50 to 600 days. This information is derived by monitoring the aqueous 133Ba2+ concentration combined with simple mass balance calculations. In the case of 226Ra2+ a RaxBa1-xSO4 solid solution forms and the uptake rate drops significantly within 400 days. The observed 226Ra2+ concentration in solution is controlled by the solubility of a RaxBa1-xSO4 solid solution and several orders of magnitude below the Ra2+ solubility with respect to a pure RaSO4(s) end member. It cannot be demonstrated unambiguously that a zero exchange rate and therefore thermodynamic equilibrium has been established within the observation period. The observed concentrations may be interpreted either as (1) a partial equilibration of 20 to 50% of the barite crystals with 226Ra2+ or (2) as complete equilibration of a Ra0.000128Ba0.999872SO4 solid solution with 226Ra2+ with no pure barite left. In both cases it is concluded that equilibration between aqueous Ra2+ and barite involves the replacement of a substantial fraction of the initial barite and proceeds significantly beyond pure surface adsorption processes
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Mar 2010; 106 p; ISSN 1404-0344;
; Also available from: http://www.skb.se/upload/publications/pdf/TR-10-43webb; 31 refs., 140 figs., 40 tabs.

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ALKALINE EARTH ISOTOPES, ALKALINE EARTH METAL COMPOUNDS, ALPHA DECAY RADIOISOTOPES, BARIUM COMPOUNDS, BARIUM ISOTOPES, BETA DECAY RADIOISOTOPES, CARBON 14 DECAY RADIOISOTOPES, DAYS LIVING RADIOISOTOPES, DISPERSIONS, ELECTRON CAPTURE RADIOISOTOPES, EVEN-EVEN NUCLEI, EVEN-ODD NUCLEI, HEAVY ION DECAY RADIOISOTOPES, HEAVY NUCLEI, HOMOGENEOUS MIXTURES, INTERMEDIATE MASS NUCLEI, INTERNAL CONVERSION RADIOISOTOPES, ISOMERIC TRANSITION ISOTOPES, ISOTOPES, MANAGEMENT, MINERALS, MIXTURES, NUCLEI, OXYGEN COMPOUNDS, RADIOACTIVE WASTE MANAGEMENT, RADIOISOTOPES, RADIUM COMPOUNDS, RADIUM ISOTOPES, SOLUTIONS, SULFATE MINERALS, SULFATES, SULFUR COMPOUNDS, WASTE DISPOSAL, WASTE MANAGEMENT, YEARS LIVING RADIOISOTOPES
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