Americium incorporation into studtite: a theoretical and experimental study
Abstract
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.
- Authors:
-
[1];
[2];
[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)
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1700514
- Report Number(s):
- PNNL-SA-143797
Journal ID: ISSN 1477-9226
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Dalton Transactions
- Additional Journal Information:
- Journal Volume: 48; Journal Issue: 34; Journal ID: ISSN 1477-9226
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Biswas, Saptarshi, Edwards, Samuel J., Wang, Zheming, Si, Hang, Vintró, Luis León, Twamley, Brendan, Kowalski, Piotr M., and Baker, Robert J. Americium incorporation into studtite: a theoretical and experimental study. United States: N. p., 2019.
Web. doi:10.1039/c9dt02848j.
Biswas, Saptarshi, Edwards, Samuel J., Wang, Zheming, Si, Hang, Vintró, Luis León, Twamley, Brendan, Kowalski, Piotr M., & Baker, Robert J. Americium incorporation into studtite: a theoretical and experimental study. United States. https://doi.org/10.1039/c9dt02848j
Biswas, Saptarshi, Edwards, Samuel J., Wang, Zheming, Si, Hang, Vintró, Luis León, Twamley, Brendan, Kowalski, Piotr M., and Baker, Robert J. Thu .
"Americium incorporation into studtite: a theoretical and experimental study". United States. https://doi.org/10.1039/c9dt02848j. https://www.osti.gov/servlets/purl/1700514.
@article{osti_1700514,
title = {Americium incorporation into studtite: a theoretical and experimental study},
author = {Biswas, Saptarshi and Edwards, Samuel J. and Wang, Zheming and Si, Hang and Vintró, Luis León and Twamley, Brendan and Kowalski, Piotr M. and Baker, Robert J.},
abstractNote = {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.},
doi = {10.1039/c9dt02848j},
journal = {Dalton Transactions},
number = 34,
volume = 48,
place = {United States},
year = {Thu Aug 01 00:00:00 EDT 2019},
month = {Thu Aug 01 00:00:00 EDT 2019}
}
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