Caustic leaching of high-level radioactive tank sludge: A critical literature review

The Department of Energy (DOE) must treat and safely dispose of its radioactive tank contents, which can be separated into high-level waste (HLW) and low-level waste (LLW) fractions. Since the unit costs of treatment and disposal are much higher HLW than for LLW, technologies to reduce the amount of HLW are being developed. A key process currently being studied to reduce the volume of HLW sludges is called enhanced sludge washing (ESW). This process removes, by water washes, soluble constituents such as sodium salts, and the washed sludge is then leached with 2-3 M NaOH at 60-100°C to remove nonradioactive metals such as aluminum. The remaining solids are considered to be HLW while the solutions are LLW after radionuclides such as ¹³⁷Cs have been removed. Results of bench-scale tests have shown that the ESW will probably remove the required amounts of inert constituents. While both experimental and theoretical results have shown that leaching efficiency increases as the time and temperature of the leach are increased, increases in the caustic concentration above 2-3 M will only marginally improve the leach factors. However, these tests were not designed to validate the assumption that the caustic used in the ESW process will generate only a small increase (10 Mkg) in the amount of LLW; instead, the test conditions were selected to maximize leaching in a short period and used more water and caustic than is planned during full-scale operations. Even though calculations indicate that the estimate for the amount of LLW generated by the ESW process appears to be reasonable, a detailed study of the amount of LLW from the ESW process is still required. If the LLW analysis indicates that sodium management is critical, then a more comprehensive evaluation of the clean salt process or caustic recycle would be needed. Finally, experimental and theoretical studies have clearly demonstrated the need for the control of solids formation during and after leaching.