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Synroc containing 20 wt% simulated high level waste (HLW) was subjected to
two sets of leach tests at 150°C where the leachant was and was not replaced
during the test (replacement and non-replacement testing). The leachant was
a KH-phthalate buffered solution (pH 4.2). Samples were characterised before
and after leach testing using SEM, AEM and SIMS. Elemental concentrations in
leachates were measured using ICP-MS. In concert with the findings of i) a
dissolution study of perovskite in a flowing leachant and ii) a previous
Synroc dissolution study (wherein Synroc containing 10 wt% simulated HLW was
subjected to periodic replacement, leach testing in deionised water at
150°C), the results of this study show that when the leachant replacement
frequency is varied from 7 d to the duration of the test, there is no effect
on leach rate or leaching mechanisms.
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.
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