Stabilization of Rocky Flats Pu-contaminated ash within chemically bonded phosphate ceramics

摘要

A feasibility study was conducted on the use of chemically bonded phosphate ceramics for stabilization of combustion residue of high transuranic (TRU) wastes. Using a matrix of magnesium potassium phosphate formed by the room-temperature reaction of MgO and KH_2PO_4 solution, we made waste forms that contained 5 wt% Pu to satisfy the requirements of the Waste Isolation Pilot Plant. The waste forms were ceramics whose compression strength was twice that of conventional cement grout and whose connected porosity was approx = 50% that of cement grout. Both surrogate and actual waste forms displayed high leaching resistance for both hazardous metals and Pu. Hydrogen generation resulting from the radiolytic decomposition of water and organic compounds present in the waste form did not appear to be a significant issue. Pu was present as PuO_2 that was physically microencapsulated in the matrix. In the process, pyrophoricity was removed and leaching resistance was enhanced. The high leaching resistance was due to the very low solubility of PuO_2 coupled with superior microencapsulation. As a result, the waste forms satisfied the current Safegurad Termination Limit requirement for storage of TRU combustion residues.