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Americium incorporation into studtite: a theoretical and experimental study

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Abstract

Studtite, [UO22-O2)(H2O)2]·2H2O, and metastudtite, [UO22-O2)(H2O)2], are important phase alterations of UO2 in a spent nuclear fuel repository and have previously been shown to react with Np(V). In this work we extend the study to Am(V) on a tracer scale and show spectroscopic evidence that the Am is incorporated into the structure of studtite as Am(III). A computational study on the possible mechanisms for the incorporation of Np and Am shows that protonation of the -yl oxygen is the favoured route and the calculated incorporation energies are large and positive. The results suggest that Am is less favoured compared to Np but energetically more favoured to incorporate both actinide ions into metastudtite rather than studtite. Finally, we have shown that once incorporated, Am readily leaches into water but spectroscopic measurements suggest subtle changes in the structure of studtite.

Graphical abstract: Americium incorporation into studtite: a theoretical and experimental study

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Publication details

The article was received on 09 Jul 2019, accepted on 30 Jul 2019 and first published on 01 Aug 2019


Article type: Paper
DOI: 10.1039/C9DT02848J
Dalton Trans., 2019, Advance Article

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    Americium incorporation into studtite: a theoretical and experimental study

    S. Biswas, S. J. Edwards, Z. Wang, H. Si, L. L. Vintró, B. Twamley, P. M. Kowalski and R. J. Baker, Dalton Trans., 2019, Advance Article , DOI: 10.1039/C9DT02848J

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