Mobilization of Technetium from Reduced Sediments under Seawater Inundation and Intrusion Scenarios

摘要

Predicted sea level rise would increase the vulnerability of low lying coastal legacy nuclear sites to inundation and intrusion with oxygenated seawater. This could have a significant impact on the mobility of redox-sensitive radionuclides such as Tc. Here, batch and column experiments were used to simulate and investigate the effect of these processes on the mobilization of Tc from sediments under a range of geochemically reduced conditions. Batch experiments showed that only a small proportion of Tc was rapidly (within 5 days) released from the sediments into seawater and groundwater. The subsequent Tc release was slowest and ultimately limited to the greatest extent (17%) in initially Fe-reducing sediments, when they were reoxidized in seawater. Thus, the cycling of iron and the impact of the water chemistry on iron mineralogy were important for hindering Tc release. Column experiments showed that iron minerals were less effective at retarding Tc release under flow-through conditions. Kinetically controlled and solubility limited Fe dissolution led to ongoing Tc release from the sediments; i.e. the retarding effect of iron phases was temporary, and significantly more Tc was mobilized (79-93%) compared with the batch experiments (17-45%). These results demonstrate the potential for Tc(IV) to be oxidized and mobilized from sediments at coastal nuclear sites resulting from predicted intrusion and inundation with oxic seawater.