Skip to main content
SpringerLink
Log in

Synthesis and Characterization of Brannerite Compositions for MOX Residue Disposal

  • Published:
MRS Advances Aims and scope Submit manuscript

Abstract

Due to their high actinide content MOX residues require immobilization within a robust host matrix. Although it is possible to immobilize actinides in vitreous wasteforms; ceramic phases, such as brannerite (UTi2O6), are attractive due to their high waste loading capacity and relative insolubility. Brannerites Gd0.1U0.9Ti2O6, Ce0.1U0.9Ti2O6 and Gd0.1U0.81Ce0.09Ti2O6 were prepared using an oxide route. Charge compensation of trivalent cations was expected to occur via the oxidation of U (IV) to higher valence states (U (V) or U (VI)). Gd was added to act as a neutron absorber in the final Pu bearing wasteform and Ce was used as a structural surrogate for Pu. X-ray absorption spectroscopy showed that Ce (IV) was reduced to Ce (III) in all cases. X-ray powder diffraction of synthesized specimens found that the final phase assemblage was strongly affected by processing atmosphere (air or argon). Prototypical brannerite was formed in all compositions, secondary phases observed were found to vary according to processing atmosphere and stoichiometry. Microstructural analysis (SEM) of the sintered samples confirmed the results of the X-ray powder diffraction.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Similar content being viewed by others

References

  1. N. C. Hyatt, “Plutonium management policy in the United Kingdom: The need for a dual track strategy,” Energy Policy, 99, (In press, 2016).

  2. P. D. Wilson, The Nuclear Fuel Cycle: From Ore to Waste, 1st ed (Oxford University Press, Oxford, 1996).

    Google Scholar 

  3. J. T. Szymanski and J. D. Scott, “A Crystal Structure Refinement of Synthetic Brannerite, UTi2O6 , and Its Bearing on Rate of Alkaline-Carbonate Leaching of Brannerite in Ore,” Can. Mineral., 20, 271–279 (1982).

    CAS  Google Scholar 

  4. F. J. Ryerson and B. Ebbinghaus, “Pyrochlore-Rich Titanate Ceramics for the Immobilization of Plutonium : Redox Effects on Phase Equilibria in Cerium- and Thorium- Substituted Analogs,” Lawrence Livermore National Laboratory Report, UCRL-ID-139092 (2000).

  5. Y. Zhang, G. R. Lumpkin, H. Li, M. G. Blackford, M. Colella, M. L. Carter, and E. R. Vance, “Recrystallisation of amorphous natural brannerite through annealing : The effect of radiation damage on the chemical durability of brannerite,” J. Nucl. Mater., 350, 293–300 (2006).

    Article  CAS  Google Scholar 

  6. F. A. Charalambous, R. Ram, M. I. Pownceby, J. Tardio, and S. K. Bhargava, “Chemical and microstructural characterisation studies on natural and heat treated brannerite samples,” Miner. Eng., 39, 276–288 (2012).

    Article  CAS  Google Scholar 

  7. G. R. Lumpkin, “Alpha-decay damage and aqueous durability of actinide host phases in natural systems,” J. Nucl. Mater., 289 (1–2), 136–166 (2001).

    Article  CAS  Google Scholar 

  8. M. C. Stennett, C. L. Freeman, A. S. Gandy, and N. C. Hyatt, “Crystal structure and nonstoichiometry of cerium brannerite: Ce0.975Ti 2O5.95,” J. Solid State Chem.,192, 172–178 (2012).

    Article  CAS  Google Scholar 

  9. E. R. Vance, J. N. Watson, M. L. Carter, R. A. Day, and B. D. Begg, “Crystal Chemistry and Stabilization in Air of Brannerite, UTi2O6,” vol. 44, pp. 141–144, 2001.

  10. M. James and J. N. Watson, “The Synthesis and Crystal Structure of Doped Uranium Brannerite Phases U1−xMxTi2O6 (M=Ca2+, La3+, and Gd3+),” J. Solid State Chem., 165, 261–265 (2002).

    Article  CAS  Google Scholar 

  11. B. Ravel and M. Newville, “ATHENA, ARTEMIS, HEPHAESTUS: Data analysis for X-ray absorption spectroscopy using IFEFFIT,”Journal of Synchrotron Radiation, 12 (4), 537–541 (2005).

    Article  CAS  Google Scholar 

  12. J. E. Patchettt and E. W. Nuffield, “Studies of Radioactive Compounds X- The Synthesis and Crystallography of Brannerite,” Can. Mineral., 6, 483–490 (1960).

    Google Scholar 

  13. D. J. Bailey, M. C. Stennett, and N. C. Hyatt, “Synthesis and Characterization of Brannerite Wasteforms for the Immobilization of Mixed Oxide Fuel Residues,” Procedia Chem., 21, 371–377 (2016).

    Article  Google Scholar 

Download references

Author information

Authors and Affiliations

  1. Immobilisation Science Laboratory, Department of Materials Science and Engineering, Univeristy of Sheffield, Mappin Street, Sheffield, S1 3JD, United Kingdom

    D. J. Bailey, M. C. Stennett & N. C. Hyatt

Authors
  1. D. J. Bailey
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. M. C. Stennett
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. N. C. Hyatt
    View author publications

    You can also search for this author in PubMed Google Scholar

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Bailey, D.J., Stennett, M.C. & Hyatt, N.C. Synthesis and Characterization of Brannerite Compositions for MOX Residue Disposal. MRS Advances 2, 557–562 (2017). https://doi.org/10.1557/adv.2016.631

Download citation

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1557/adv.2016.631

Search

Navigation