Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling

Burns, Jonathan D.; Moyer, Bruce A.

doi:10.1021/acs.inorgchem.6b01430

Title: Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling

Journal Article · Wed Aug 17 00:00:00 EDT 2016 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.6b01430· OSTI ID:1325476

Burns, Jonathan D. ^[1]; Moyer, Bruce A. ^[2]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Nuclear Security and Isotope Technology Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division

Hexavalent Np, Pu, and Am individually, and as a group, have all been cocrystallized with UO₂(NO₃)₂∙ 6H₂O, constituting the first demonstration of an An(VI) group cocrystalliza- tion. The hexavalent dioxo cations of Np, Pu, and Am cocrystallize with UO₂(NO₃)₂∙ 6H₂O in near proportion with a simple reduction in temperature, while the lower valence states, An(III) and An(IV), are only slightly removed from solution. A separation of An(VI) species from An(III) ions by crystallization has been demonstrated, with an observed separation factor of 14. Separation of An(VI) species from key fission products, ⁹⁵Zr, ⁹⁵Nb, ¹³⁷Cs, and ¹⁴⁴Ce, has also been demonstrated by crystallization, with separation factors ranging from 6.5 to 71 in the absence of Am(VI), while in the presence of Am(VI), the separation factors were reduced to 0.99 7.7. One interesting observation is that Am(VI) shows increased stability in the cocrystallized form, with no reduction observed after 13 days, as opposed to in solution, in which >50% is reduced after only 10 days. The ability to cocrystallize and stabilize hexavalent actinides from solution, especially Am(VI), introduces a new separations approach that can be applied to closing the nuclear fuel cycle.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1325476

Journal Information:: Inorganic Chemistry, Vol. 55, Issue 17; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 20 works

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Effective separation of Am(III) and Cm(III) using a DGA resin via the selective oxidation of Am(III) to Am(V) Kazi, Zakir; Guérin, Nicolas; Christl, Marcus Journal of Radioanalytical and Nuclear Chemistry, Vol. 321, Issue 1 https://doi.org/10.1007/s10967-019-06571-0	journal	May 2019
X-Ray crystallographic and computational study on uranyl–salophen complexes bearing nitro groups Valkonen, Arto; Lombardo, Giuseppe M.; Rissanen, Kari Dalton Trans., Vol. 46, Issue 16 https://doi.org/10.1039/c6dt04773d	journal	January 2017
Kinetics of Ion Exchange of Zr/Sn(IV) Phosphonate–Phosphate Hybrid Materials for Separation of Lanthanides from Oxidized Actinides Burns, Jonathan D.; Clearfield, Abraham Solvent Extraction and Ion Exchange, Vol. 36, Issue 7 https://doi.org/10.1080/07366299.2018.1542971	journal	November 2018
Solid state characterization of oxidized actinides co-crystallized with uranyl nitrate hexahydrate Einkauf, Jeffrey D.; Burns, Jonathan D. Dalton Transactions, Vol. 49, Issue 3 https://doi.org/10.1039/c9dt04000e	journal	January 2020

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