ABSTRACTOne of the most complex problems concerning nuclear waste management and the restoration of plutonium production sites is the treatment and disposition of mixed and TRU wastes. Hydrothermal oxidation, which has been shown to be effective in oxidizing a wide variety of organic material to CO2, water, salts and other nonhazardous oxides, is a promising new technology for the treatment and volume reduction of actinide-containing waste. Information on the speciation and solubility of plutonium under process effluent conditions will facilitate the development of separation techniques for removing it from the treated solutions. Such a strongly oxidizing environment will generate plutonium(VT); and upon the destruction of organics, hydrothermal reactor solutions will contain carbonate. We are investigating the solubility and speciation of the plutonium(VI) carbonate system as a function of ionic strength (0.1 to 5.0 M). Formation constants for the tris- and biscarbonato complexes of plutonium(IV) were determined to be, log β130= 17.7 and log β120= 13.6, respectively, by spectrophotometry. These formation constants indicate that PuO2CO3(aq)is the plutonium (VI) carbonate solution species with the largest relevant stability range. We prepared and characterized the corresponding solid using XRD, EXAFS, and diffuse reflectance, and initiated solubility experiments in 0.1, 0.2, 0.5, 1,2, and 5 M NaCl at 22±1°C under 100% CO2. Data collected thus far yield the solubility products, log Kspmol2/kg2= -12.9 (0.1 m NaCl), -12.4 (0.2 m NaCl), -12.5 (0.5 m NaCl), -12.3 (1 m NaCl), -12.2 (2 m NaCl), -12.3 (5 m NaCl).