Kinetics of oxyapatite [Ca2Nd8(SiO4)6O2] and powellite [(Ca,Sr,Ba)MoO4] dissolution in glass-ceramic nuclear waste forms in acidic, neutral, and alkaline conditions

Neeway, James J.; Asmussen, R. Matthew; McElroy, Erin M.; Peterson, Jacob A.; Riley, Brian J.; Crum, Jarrod V.

doi:10.1016/j.jnucmat.2018.12.043

Title: Kinetics of oxyapatite [Ca2Nd8(SiO4)6O2] and powellite [(Ca,Sr,Ba)MoO4] dissolution in glass-ceramic nuclear waste forms in acidic, neutral, and alkaline conditions

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Authors:

;

; McElroy, Erin M.; Peterson, Jacob A.;

; Crum, Jarrod V.

Publication Date:: Fri Mar 01 00:00:00 EST 2019

Sponsoring Org.:: USDOE

OSTI Identifier:: 1547921

Grant/Contract Number:: AC05-76RL01830

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Journal of Nuclear Materials

Additional Journal Information:: Journal Name: Journal of Nuclear Materials Journal Volume: 515 Journal Issue: C; Journal ID: ISSN 0022-3115

Publisher:: Elsevier

Country of Publication:: Netherlands

Language:: English

Citation Formats


                    Neeway, James J., Asmussen, R. Matthew, McElroy, Erin M., Peterson, Jacob A., Riley, Brian J., and Crum, Jarrod V. Kinetics of oxyapatite [Ca2Nd8(SiO4)6O2] and powellite [(Ca,Sr,Ba)MoO4] dissolution in glass-ceramic nuclear waste forms in acidic, neutral, and alkaline conditions.  Netherlands: N. p., 2019. 
Web.  doi:10.1016/j.jnucmat.2018.12.043.

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                    Neeway, James J., Asmussen, R. Matthew, McElroy, Erin M., Peterson, Jacob A., Riley, Brian J., & Crum, Jarrod V. Kinetics of oxyapatite [Ca2Nd8(SiO4)6O2] and powellite [(Ca,Sr,Ba)MoO4] dissolution in glass-ceramic nuclear waste forms in acidic, neutral, and alkaline conditions.  Netherlands.  https://doi.org/10.1016/j.jnucmat.2018.12.043

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                    Neeway, James J., Asmussen, R. Matthew, McElroy, Erin M., Peterson, Jacob A., Riley, Brian J., and Crum, Jarrod V. Fri .  
"Kinetics of oxyapatite [Ca2Nd8(SiO4)6O2] and powellite [(Ca,Sr,Ba)MoO4] dissolution in glass-ceramic nuclear waste forms in acidic, neutral, and alkaline conditions".  Netherlands.  https://doi.org/10.1016/j.jnucmat.2018.12.043.

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@article{osti_1547921,

  title        = {Kinetics of oxyapatite [Ca2Nd8(SiO4)6O2] and powellite [(Ca,Sr,Ba)MoO4] dissolution in glass-ceramic nuclear waste forms in acidic, neutral, and alkaline conditions},

  author       = {Neeway, James J. and Asmussen, R. Matthew and McElroy, Erin M. and Peterson, Jacob A. and Riley, Brian J. and Crum, Jarrod V.},

  abstractNote = {},

  doi          = {10.1016/j.jnucmat.2018.12.043},

  journal      = {Journal of Nuclear Materials},

  number       = C,

  volume       = 515,

  place        = {Netherlands},

  year         = {Fri Mar 01 00:00:00 EST 2019},

  month        = {Fri Mar 01 00:00:00 EST 2019}

}

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https://doi.org/10.1016/j.jnucmat.2018.12.043

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Kinetics of oxyapatite [Ca2Nd8(SiO4)6O2] and powellite [(Ca,Sr,Ba)MoO4] dissolution in glass-ceramic nuclear waste forms in acidic, neutral, and alkaline conditions

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Solidification of chemically complex aqueous waste streams from used nuclear fuel reprocessing is achievable with glass ceramics. Glass ceramics are a desirable waste form because higher waste loading is achievable compared to borosilicate glasses. Additionally, crystalline phases with similar chemistry are more durable than their amorphous counterpart. However, during glass ceramic fabrication, mechanical stresses at crystal-glass interfaces, which are caused by thermal expansion mismatch during cooling, create locales where water is capable of accessing and reacting with the various phases in the glass ceramic and releasing radionuclides into the aqueous phase. In the present work, we build on previous chemicalmore »« less
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Synthesis and characterization of oxyapatite [Ca2Nd8(SiO4)6O2] and mixed-alkaline-earth powellite [(Ca,Sr,Ba)MoO4] for a glass-ceramic waste form

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This paper discusses the synthesis, characterization, and chemical durability assessment of oxyapatite [Ca₂Nd₈(SiO₄)₆O₂] and mixed-alkaline-earth powellite [(Ca,Sr,Ba)MoO₄]. These are the major crystalline phases that precipitate from the melt during cooling of a glass ceramic waste form currently being evaluated for immobilizing wastes produced during the aqueous reprocessing of used nuclear fuel. The oxyapatite was made at 99.7% purity using a solution-based process followed by heat treatments. The powellite, made by melting carbonates and slow-cooling the melt, formed two different phases, one rich in Ca (74.7%) and Sr (19.4%) (balance is Ba) and the other rich in Sr (25.6%) and Bamore »« less
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Six different rare-earth oxyapatites including Ca2RE8(SiO4)6O2 (RE = La, Nd, Sm, Eu, Yb) and NaLa9(SiO4)6O2 were synthesized using solution-based processes followed by heat treatments. The crystal structures of the synthesized oxyapatites were solved from X-ray powder diffraction (XRD) and electron probe microanalysis (EPMA). All the oxyapatites were isostructural with the hexagonal space group P63/m and showed similar unit cell parameters. The isolated [SiO4]4- tetrahedra in each crystal are linked by the cations at 4f and 6h sites occupied by RE3+ and Ca2+ in Ca2RE8(SiO4)6O2 or La3+ and Na+ in NaLa9(SiO4)6O2. The lattice parameters, cell volumes, and densities of the synthesizedmore »« less
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