Laboratory studies of the diagenesis and mobility of 239,240 pu and 137 Cs in nearshore sediments

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Controlled laboratory experiments have been used to study the diagenetic chemistry of 239,240 Pu 137 Cs, and 55 Fe. Experiments using Buzzards Bay sediments in small tanks show that sulfate reduction is accompanied by the production of large pore water concentration gradients of alkalinity, phosphate, ammonia and dissolved organic carbon and the formation of subsurface maxima in Fe and Mn. These pore water profiles demonstrate that bacterially-mediated processes of organic matter degradation and redox reactions can be simulated in the laboratory. A vertical profile of 55 Fe in pore waters is reported for the first time: it follows the profile of stable Fe and as such has a large (200 dpm/100 kg) subsurface maximum between 2-4 cm depth. Comparison of 55 Fe/Fe ratios in sediments and pore waters shows that there is preferential solubilization of 55 Fe over stable Fe. The pore water activities of 239,240 Pu show no gradients within the large uncertainties of the counting statistics, but are two to four times higher than Buzzards Bay seawater (0.05 dpm/100 kg). The activity of 137 Cs in the pore water profile is constant (40 dpm/100 kg) within the large counting uncertainties and is twice that of Buzzards Bay seawater. Cs-137 does not appear to be involved in diagenetic chemistry but may increase in pore waters as a result of ion exchange reactions. Flux estimates based on the pore water data show that remobilization and transport of 239,240 Pu in coastal sediments are not significant processes while the transport of l37 Cs may be.

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