摘要: Plans exist to separate radioactive waste stored in underground tanks at the US Department of Energy's Hanford Site in south central Washington State into low-level and high-level fractions, and to immobilize the separate fraction... 展开 Plans exist to separate radioactive waste stored in underground tanks at the US Department of Energy's Hanford Site in south central Washington State into low-level and high-level fractions, and to immobilize the separate fractions in high-integrity vitrified forms for long-term disposal. Calcination with water dissolution has been proposed as a possible treatment for achieving low/high-level separation. Chemistry development activities conducted since 1992 with simulated and genuine tank waste show that calcination/dissolution destroys organic carbon and converts nitrate and nitrite to hydroxide and benign offgases. The process also dissolves significant quantities of bulk chemicals (aluminum, chromium, and phosphate), allowing their redistribution from the high-level to the low-level fraction. Present studies of the chemistry of calcination/dissolution processing of genuine wastes, conducted in the period October 1993 to September 1994, show the importance of sodium fluoride phosphate double salt in controlling phosphate dissolution. Peptization of waste solids is of concern if extensive washing occurs. Strongly oxidizing conditions imposed by calcination reactions were found to convert transition metals to soluble anions in the order chromate > manganate > > ferrate. In analogy with manganese behavior, plutonium dissolution, presumably by oxidation to more soluble anionic species, also occurs by calcination/dissolution. Methods to remove plutonium from the product low-level solution stream must be developed. 收起