DOE OSTI2014
Cementitious materials are used to solidify and stabilize aqueous based radioactive waste containing sodium salts. The types and proportions of cementitious ingredients used to treat aqueous radioactive waste streams containing sodium salts depend on the performance objectives for the waste forms and the compositions of the waste streams. Matrix phases can stabilize certain contaminants (co-precipitation, substitution, ion exchange, and / or sorption), influence processing properties, and are responsible for physical properties and durability of the cured waste forms. Consequently, characterization of the matrix (binder) mineralogy (chemical compositions and crystalline / non crystalline structures) is important for predicting contaminant leaching and evolution of the materials as a function of time and changing conditions This report documents sample preparation and x-ray diffraction results for a series of mixtures of sodium salt waste and cementitious binders. The objective of this study was to provide initial phase characterization for the CBP reference case cementitious salt waste form. This information can be used to: 1) generate a base line for the evolution of the waste form as a function of time and conditions, 2) potentially to design new binders based on mineralogy of the binder, 3) understand and predict anion and cation leaching behavior of contaminants of concern, and 4) predict performance of the waste forms for which phase solubility and thermodynamic data are available. Characterization of the mineralogy is also important for understanding the buffering effects that the waste form has on infiltrating water / leachates. More specifically, identification of hydrated phases capable of sequestering anions in the structures and crystallinity of the calcium silicate binder phases were of particular interest. The intent was to use this characterization data as a starting point for more detailed phase characterization using neutron diffraction techniques in addition to quasi-elastic neutron scattering techniques for characterization of water at the ORNL Spallation Neutron Source, Oak Ridge, TN. The initial characterization is complete. Due to extensive substitutions of cations and anions in the layered double hydroxide phases and the very fine intermixing of poorly crystalline hydrated phases in the reference case blend (10 : 45 : 45 cement : slag : fly ash), electron diffraction and transmission electron spectroscopy are recommended as the next step for characterization. In summary, the hydrated mixtures of Type II portland cement, Grade 100 ground granulated blast furnace slag (GGBFS) and carbon burn-out (CBO) Class F Fly ash contained hydrated phase assemblages which were typical of those reported in the literature. Based on x-ray diffraction results, no significant differences were detected in samples cured 2 months and 14 months in sealed containers at ambient indoor temperatures.