Separation of critical radioactive and non-radioactive species from aqueous waste streams

The separation of radioactive and non-radioactive species from the simulated DOE neutralized current acid waste (NCAW) stream was studied. Cation and anion species were referred to their possible basic compounds, and divided into seven groups (nitrate, phosphate, sulfate, fluoride, nitrite, carbonate, and hydroxide). The nitrate group (the major anion in the DOE waste streams) contains several cations species, while the rest of the groups are only in the form of sodium. The precipitation measurements were conducted in three experimental stages. In the first stage, the precipitation of sodium sulfate, sodium phosphate, sodium-sulfate-phosphate, and aluminum nitrate systems were studied using isopropylamine (IPA) as a precipitation solvent. The objectives of this stage were to evaluate the precipitation ability of IPA in precipitating these compounds individually, and to validate the consistency of the analytical instruments and the employed experimental procedure. Tests performed on the acquired data indicated a high level of experimental consistency. The removal of phosphate, sulfate and aluminum were very high. In the second stage, the precipitation studies were conducted on the: (1) nitrate group alone; (2) binary groups containing the groups of nitrate-phosphate, nitrate-sulfate, nitrate-fluoride, nitrate-nitrite, and nitrate-carbonate; (3) combined nitrate, phosphate, sulfate, and fluoride groups and (4) combined nitrate, phosphate, sulfate, fluoride, nitrite, and carbonate groups. IPA was used as a precipitation solvent. The objectives of this stage were to evaluate the interactions of these groups in the absence of the hydroxide group (e.g. DOE acid-dissolved sludge and acidified supernate streams), and the influence of such interactions on the individual removal of the targeted species. The removal of the aluminum, phosphate, fluoride, and alkaline cations were significantly high (reached 99.9%). The removal of sulfate were moderately high (reached 87%), and the removal of nitrate and alkali cations including cesium were to some extent low (reached about 50%). In the third stage, the precipitation of inorganic species from the simulated NCAW stream was studied using IPA and ethylamine (EA). The precipitation process is very feasible for reducing the radioactivity contents of alkaline cations. However, the process is less effective in separating alkali cations including cesium. The removal of polyvalent transition metals such as aluminum ion is negatively influenced by the significant presence of hydroxide. While the process is effectively capable of separating phosphate, fluoride, and sulfate, it is significantly less effective in separating nitrate and nitrite. A previously derived thermodynamics framework was used to model the precipitation measurements. The framework provided two predictive equations (the 2-Suffix and 3-Suffix equations). Both equations were reasonably adequate for predicting the solubility phase behavior of tested inorganic species in a mixed-solvents mixture as well as for estimating optimum interaction parameters. However, the 3-Suffix equation was better than the 2-Suffix equation. The parameters were useful for estimating the: (1) precipitation fractions (%P) of the studied species, for instance, at different concentration levels of similar targeted species, or in different waste streams with similar or approximate abundance of species, or at different solvents volume ratio (V(r)) where no experimental data are available.