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

Controlled laboratory experiments have been used to study the diagenetic chemistry of ^239,240Pu ¹³⁷Cs, and ⁵⁵Fe. 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 ⁵⁵Fe 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 ⁵⁵Fe/Fe ratios in sediments and pore waters shows that there is preferential solubilization of ⁵⁵Fe over stable Fe. The pore water activities of ^239,240Pu 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 ¹³⁷Cs 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 ^l37Cs may be.