Hydrolysis reactions of actinide oxides play an important role in the initial steps of the conversion of actinide oxides to compounds containing OH groups. These reactions are important in the design of new nuclear fuels as well as environmental cleanup. Experimentally, these type of reactions are being studied in the gas phase at Lawrence Berkeley National Laboratory where the actinide cations and anions are identified using a mass spectrometer. Although the experimental work determines reaction products, it does not determine their structures or the overall energetics. Our results using electronic structure calculations provide a structural and energetic background which explains the experimental results providing us with unique insights into the chemistry of the +III/+IV/+V oxidation state of the actinides, especially the transuranics about which little is known because of their radioactivity and the cost to synthesize these atoms. The potential energy surfaces for the reactions of H2O with actinide dioxides with the An in the +IV oxidation states for all the actinides and AnO(NO3)3- with H2O and HNO2 for An = Th, - Bk have been predicted at the DFT and CCSD(T) levels. The energetic results are correlated with oxidation states and electronic populations.

Hydrolysis reactions of actinide oxides and actinide oxides nitrates

255th National Meeting (2018)

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