Abstract
For the accurate computer simulation of the Purex process the kinetics of important chemical reactions occurring in both the aqueous and solvent phases in the process must be included in the model. One important species in the Purex process is Np(IV), and so the kinetics of the oxidation of Np(IV) by HNO 3 in TBP phases have been determined experimentally to aid the efficient modelling of Np(IV) in Purex process flowsheets. It was found that in 100% TBP solutions the oxidation is autocatalytic, with a mechanism proceeding predominantly via Np(V) reproportionation. The rate equation and rate constants have been determined for both the non-catalysed and autocatalysed components. However, there are significant departures from these kinetics as the TBP solution is diluted by n-dodecane. These differences include the retardation of the reaction and a change from an autocatalytic reaction to first-order kinetics, particularly at lower temperatures. Although this data is suitable for inclusion into computer models, the slow reaction in 30% TBP solutions means that the solvent-phase oxidation of Np(IV) will be a minor effect.
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