FRACTIONAL CRYSTALLIZATION OF HANFORD SINGLE-SHELL TANK WASTES FROM CONCEPT TO PILOT PLANT

The Hanford site has 149 underground single-shell tanks (SST) storing mostly soluble, multi-salt mixed wastes resulting from Cold War era weapons material production. These wastes must be retrieved and the salts immobilized before the tanks can be closed to comply with an overall site-closure consent order entered into by the US Department of Energy, the Environmental Protection Agency, and the State of Washington. Water will be used to retrieve the wastes and the resulting solution will be pumped to a proposed pretreatment process where a high-curie (primarily 137Cs) waste fraction will be separated from the other waste constituents. The separated waste streams will then be vitrified to allow for safe storage as an immobilized high-level waste, or low-level waste, borosilicate glass. Fractional crystallization, a common unit operation for production of industrial chemicals and pharmaceuticals, was proposed as the method to separate the salt wastes; it works by evaporating excess water until the solubilities of various species in the solution are exceeded (the solubility of a particular species depends on its concentration, temperature of the solution, and the presence of other ionic species in the solution). By establishing the proper conditions, selected pure salts can be crystallized and separated from the radioactive liquid phase. The aforementioned parameters, along with evaporation rate, proper agitation, and residence time, determine nucleation and growth kinetics and the resulting habit and size distribution of the product crystals. These crystals properties are important considerations for designing the crystallizer and solid/liquid separation equipment. A structured program was developed to (a) demonstrate that fractional crystallization could be used to pre-treat Hanford tank wastes and (b) provide data to develop a pilot plant design