Americium incorporation into studtite: a theoretical and experimental study

Biswas, Saptarshi; Edwards, Samuel J.; Wang, Zheming; Si, Hang; Vintró, Luis León; Twamley, Brendan; Kowalski, Piotr M.; Baker, Robert J.

doi:10.1039/c9dt02848j

Americium incorporation into studtite: a theoretical and experimental study

Journal Article · Thu Aug 01 00:00:00 EDT 2019 · Dalton Transactions

DOI:https://doi.org/10.1039/c9dt02848j· OSTI ID:1700514

Biswas, Saptarshi ^[1]; ^[1]; ^[2]; Si, Hang ^[3]; Vintró, Luis León ^[4]; Twamley, Brendan ^[1]; ^[3]; ^[1]

Univ. of Dublin Trinity College (Ireland)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Forschungszentrum Juelich (Germany). Inst. for Energy and Climate Research (IEK)
Univ. College Dublin (Ireland)

Studtite, [UO₂(η₂-O₂)(H₂O)₂]·2H₂O, and metastudtite, [UO₂(η₂-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.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1700514

Report Number(s):: PNNL-SA--143797

Journal Information:: Dalton Transactions, Journal Name: Dalton Transactions Journal Issue: 34 Vol. 48; ISSN 1477-9226

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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