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Results of microbalance, pressure-volume-temperature, and mass spectrometric measurements show that a higher oxide of plutonium, PuO{sub 2+x}, and hydrogen are formed by reaction of plutonium dioxide with water at 25 C to 350 C. PuO{sub 2+x} has an intense green color consistent with the presence of Pu(VI). An oxide composition in excess of PuO{sub 2.25} is identified, but the maximum value of x is undefined. Reaction rates derived from linear mass-time and pressure-time data are described by an Arrhenius relationship that yields an activation energy of 9.4 {+-} 0.6 kcal/mol for the PuO{sub 2} + H{sub 2}O reaction. X-ray diffraction data for PuO{sub 2+x} shows that the oxide has a fluorite-related structure consistent with substitution of Pu(VI) on cationic lattice sites and accommodation of additional oxygen on interstitial sites. The cubic lattice parameter has a low, but well-defined, linear dependence on the O:Pu ratio, suggesting that PuO{sub 2+x} forms as a continuous solid solution. The failure of earlier attempts to prepare higher oxides of plutonium is attributed to slow oxidation kinetics and insensitivity of diagnostic techniques. Similarities of the PuO{sub 2+x} and UO{sub 2+x} phase are examined and relevance of the results to plutonium technology and environmental issues is discussed

Kinetics of Reaction Between Plutonium Dioxide and Water at 25 C to 350 C: Formation and Properties of the PuO{sub 2+X} Phase