OPTIMIZATION AND VALIDATION OF A CHEMICAL PROCESS FOR URANIUM, MERCURY AND CESIUM LEACHING FROM CEMENTED RADIOACTIVE WASTES

Abstract

Canadian Nuclear Laboratories (CNL) is developing a treatment and long-term management strategy for a legacy cemented radioactive waste that contains uranium, mercury, and fission products. Extracting the uranium would be advantageous for decreasing the waste classification and reducing the cost of long-term management. The chemical leachability of 3 key elements (U, Hg, and Cs) from a surrogate cemented waste (SCW) was studied with several lixiviants. The results showed that the most promising approach to leach and recover U, Hg, and Cs is the direct leaching of the SCW with H2SO4 in strong saline media. Operating parameters such as particle size, temperature, pulp density, leaching time, acid and salt concentrations, number of leaching/washing steps, etc. were optimized to improve key elements solubilization. Sulfuric leaching in saline media of a SCW (U5) containing 1182 ppm of U, 1598 ppm of Hg, and 7.9 ppm of Cs in the optimized conditions allows key elements solubilisation of 98.5 ± 0.4%, 96.6 ± 0.1%, and 93.8 ± 1.1% of U, Hg, and Cs, respectively. This solubilization process was then applied in triplicate to 7 other SCWs prepared with different cements, liquid ratios, and at different aging times and temperatures. Concentrated sulfuric acid is added to the slurry until the pH is about 2, which causes the complete degradation of cement and the formation of CaSO4. Sulfuric acid is particularly useful because it produces a leachate that is amenable to conventional ion exchange technology for the separation and recovery of uranium.