Catalytic reduction of U(VI) to U(IV) using hydrogen with platinum loaded on alumina and silica

Abstract

During the reprocessing of spent nuclear fuel, uranium (U) and plutonium (Pu) are together extracted by employing tri-n-butyl phosphate (TBP)/dodecane mixture and their partitioning is achieved by adding uranous nitrate. The partitioning agent, uranous is conventionally produced by the electrolytic reduction of uranyl nitrate. An alternate route for the reduction of U from (VI) to (IV) using hydrogen (H₂) as reductant was developed using platinum (Pt) based catalyst. Improvements in the development of the catalyst have been carried out in order to reduce the requirement of Pt without affecting the reduction performance. Experiments using 2 wt% Pt loaded on alumina beads and alumina powder have been performed and results are discussed. As the catalyst supported on alumina was found to be unstable in acidic environment, Pt loaded on silica powder has also been developed. Pt loaded on alumina and silica substrates have been tried to envisage the reduction behaviour using H₂ as reductant in presence of hydrazine nitrate which acts as U(IV) stabiliser as well as reductant. Parametric studies have been carried out to optimise the process parameters namely pressure, temperature, U concentration, free acidity, hydrazine concentration and catalyst to U (C/U) ratio. 2 wt% Pt loaded on silica has been selected for further scale up studies for making uranous.