Browsing by Author "Hambley, M"

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    Characterization and leaching behavior of plutonium-bearing Synroc-C
    (Materials Research Society, 1997-04-22) Smith, KL; Lumpkin, GR; Blackford, MH; Hambley, M; Day, RA; Hart, KP; Jostsons, A
    Synroc-C containing 10wt% simulated PW-4b-D HLW including 0.62 wt% 239Pu was subjected to MCC-1 type leach tests at 70°C in deionised water, silicate and carbonate leachates for 53 d and deionised water for 2472 d. The normalised total (i.e. unfiltered leachate + vessel wall) Pu leach rates in deionised water, silicate and carbonate leachates for periods up to 53 d were found to be of the order of 10-5, 10-4 and 10-4 g m-2 d-1 respectively. After 2472 d, the differential, normalised, Pu leach rate in deionised water dropped to ∼5 × 10-6 (total) and ∼5 × 10-8 (solution - after filtration through a 1000NMW filter) g m-2 d-1. SEM and AEM were used to characterise our starting material and investigate the secondary phases on the surfaces of leached Synroc-C discs. Calculated and measured normalised Pu leach rates are compared and the partitioning of Pu between zirconolite and perovskite is discussed. © Materials Research Society 1997
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    Characterization and leaching behavior of plutonium-bearing Synroc-C
    (Cambridge University Press/Springer Nature, 1996-02-05) Smith, KL; Lumpkin, GR; Blackford, MG; Hambley, M; Day, RA; Hart, KP; Jostsons, A
    Synroc-C containing 10wt% simulated PW-4b-D HLW including 0.62 wt% 239Pu was subjected to MCC-1 type leach tests at 70°C in deionised water, silicate and carbonate leachates for 53 d and deionised water for 2472 d. The normalised total (i.e. unfiltered leachate + vessel wall) Pu leach rates in deionised water, silicate and carbonate leachates for periods up to 53 d were found to be of the order of 10-5, 10-4 and 10-4 g m-2 d-1 respectively. After 2472 d, the differential, normalised, Pu leach rate in deionised water dropped to ∼5 × 10-6 (total) and ∼5 × 10-8 (solution - after filtration through a 1000NMW filter) g m-2 d-1. SEM and AEM were used to characterise our starting material and investigate the secondary phases on the surfaces of leached Synroc-C discs. Calculated and measured normalised Pu leach rates are compared and the partitioning of Pu between zirconolite and perovskite is discussed. © Materials Research Society 1997
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    Plutonium and neptunium incorporation in zirconolite
    (Materials Research Society, 1997) Begg, BD; Vance, ER; Day, RA; Hambley, M; Conradson, SD
    The incorporation of Pu and Np in zirconolite (CaZrTi2O7) has been investigated over a range of redox conditions. Zirconolite formulations designed to favour either trivalent or tetravalent Pu and Np were prepared by limiting the amount of charge compensating additives available to maintain electroneutrality. From near-edge X-ray absorption spectroscopy the Pu valence state was found to vary with the processing atmosphere, from completely tetravalent when fired in air, and located on either the Ca or Zr sites, to trivalent, when substituted on the Ca site after annealing in 3.5% H2/N2. Np was predominantly tetravalent over the range of redox conditions examined and was readily incorporated on either of zirconolite's Ca or Zr sites. The charge compensation mechanisms at work in different zirconolites are also discussed. © Materials Research Society 1997
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    Synroc derivatives for the Hanford waste remediation task
    (Materials Research Society, 1997) Vance, ER; Hart, KP; Day, RA; Carter, ML; Hambley, M; Blackford, MG; Begg, BD
    Three wt% each of Cs and Tc were mixed with the standard Synroc precursor and the ceramic was formed by hot-pressing. Attempts were made to incorporate the Tc as either metal or Tc 4+, using different redox conditions in processing. Volatile losses of Tc during calcination were < 0.1% in all cases. Short-term Tc leach rates when the Tc was present as a metal alloy were in the order of 10−4 g/m /d at 90°C with frequently changed water, and decreased with increasing leaching time. The valence of the Tc was monitored by X-ray absorption spectroscopy at the drying and calcination stages of the production. The general viability of Synroc/glass composites for immobilising the Hanford HLW sludges is further demonstrated by using further refinements of additive schemes for the inactive “All-blend” formulation and initial studies using the U-containing “All-blend” waste formulation. © Materials Research Society 1997