Investigation of molybdate melts as an alternative method of reprocessing used nuclear fuel

Hames, Amber L.; Tkac, Peter; Paulenova, Alena; Willit, James L.; Williamson, Mark A.

doi:10.1016/j.jnucmat.2017.01.027

Title: Investigation of molybdate melts as an alternative method of reprocessing used nuclear fuel

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Abstract

Here, an investigation of molybdate melts containing sodium molybdate (Na₂MoO₄) and molybdenum trioxide (MoO₃) to achieve the separation of uranium from fission products by crystallization has been performed. The separation is based on the difference in solubility of the fission product metal oxides compared to the uranium oxide or molybdate in the molybdate melt. The molybdate melt dissolves uranium dioxide at high temperatures, and upon cooling, uranium precipitates as uranium dioxide or molybdate, whereas the fission product metals remain soluble in the melt. Small-scale experiments using gram quantities of uranium dioxide have been performed to investigate the feasibility of UO₂ purification from the fission products. The composition of the uranium precipitate as well as data for partitioning of several fission product surrogates between the uranium precipitate and molybdate melt for various melt compositions are presented and discussed. The fission products Cs, Sr, Ru and Rh all displayed very large distribution ratios. The fission products Zr, Pd, and the lanthanides also displayed good distribution ratios (D > 10). A melt consisting of 20 wt% MoO₃-50 wt% Na₂MoO₄-30 wt% UO₂ heated to 1313 K and cooled to 1123 K for the physical separation of the UO₂ product from the melt, and washedmore »« less

Authors:

Hames, Amber L. ^[1];

^[2]; Paulenova, Alena ^[3]; Willit, James L. ^[2]; Williamson, Mark A. ^[2]

Oregon State Univ., Corvallis, OR (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Oregon State Univ., Corvallis, OR (United States)

Publication Date:: Tue Jan 17 00:00:00 EST 2017

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Office of Nuclear Energy (NE); USDOE Office of Nuclear Energy (NE), Reactor Fleet and Advanced Reactor Development. Office of Nuclear Energy Technologies

OSTI Identifier:: 1363800

Alternate Identifier(s):: OSTI ID: 1419390

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Nuclear Materials

Additional Journal Information:: Journal Volume: 486; Journal Issue: C; Journal ID: ISSN 0022-3115

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; modified open fuel cycle; recrystallization; uranium behavior in molybdate melts; uranium separation; uysed nuclear fuel recycle

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                    Hames, Amber L., Tkac, Peter, Paulenova, Alena, Willit, James L., and Williamson, Mark A. Investigation of molybdate melts as an alternative method of reprocessing used nuclear fuel.  United States: N. p., 2017. 
Web.  doi:10.1016/j.jnucmat.2017.01.027.

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                    Hames, Amber L., Tkac, Peter, Paulenova, Alena, Willit, James L., & Williamson, Mark A. Investigation of molybdate melts as an alternative method of reprocessing used nuclear fuel.  United States.  https://doi.org/10.1016/j.jnucmat.2017.01.027

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                    Hames, Amber L., Tkac, Peter, Paulenova, Alena, Willit, James L., and Williamson, Mark A. Tue .  
"Investigation of molybdate melts as an alternative method of reprocessing used nuclear fuel".  United States.  https://doi.org/10.1016/j.jnucmat.2017.01.027.  https://www.osti.gov/servlets/purl/1363800.

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@article{osti_1363800,

  title        = {Investigation of molybdate melts as an alternative method of reprocessing used nuclear fuel},

  author       = {Hames, Amber L. and Tkac, Peter and Paulenova, Alena and Willit, James L. and Williamson, Mark A.},

  abstractNote = {Here, an investigation of molybdate melts containing sodium molybdate (Na2MoO4) and molybdenum trioxide (MoO3) to achieve the separation of uranium from fission products by crystallization has been performed. The separation is based on the difference in solubility of the fission product metal oxides compared to the uranium oxide or molybdate in the molybdate melt. The molybdate melt dissolves uranium dioxide at high temperatures, and upon cooling, uranium precipitates as uranium dioxide or molybdate, whereas the fission product metals remain soluble in the melt. Small-scale experiments using gram quantities of uranium dioxide have been performed to investigate the feasibility of UO2 purification from the fission products. The composition of the uranium precipitate as well as data for partitioning of several fission product surrogates between the uranium precipitate and molybdate melt for various melt compositions are presented and discussed. The fission products Cs, Sr, Ru and Rh all displayed very large distribution ratios. The fission products Zr, Pd, and the lanthanides also displayed good distribution ratios (D > 10). A melt consisting of 20 wt% MoO3-50 wt% Na2MoO4-30 wt% UO2 heated to 1313 K and cooled to 1123 K for the physical separation of the UO2 product from the melt, and washed once with Na2MoO4 displays optimum conditions for separation of the UO2 from the fission products.},

  doi          = {10.1016/j.jnucmat.2017.01.027},

  journal      = {Journal of Nuclear Materials},

  number       = C,

  volume       = 486,

  place        = {United States},

  year         = {Tue Jan 17 00:00:00 EST 2017},

  month        = {Tue Jan 17 00:00:00 EST 2017}

}

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