Transport mechanism for Pb-210, Cs-137 and Pu fallout radionuclides through fluvial-marine systems

Pb-210, Cs-137 and Pu-239,240 sediment-depth profiles in an anoxic, unbioturbated, estuarine depositional regime at the head of the Saguenay Fjord, Que. exhibit a seasonally-modulated component caused by pulsed inputs of silts and sands during high energy, spring river discharge events superimposed on an ambient depositional pattern of finer grained clays and organic matter. A precise sediment timestratigraphy has been determined by the inverse correlation of the Pb-210 activity with the rate of river discharge during the period, 1963–1976. The historical record of Cs-137 and Pu-239,240 sediment fluxes has been reconstructed through the normalization of fallout radionuclide activities to the excess Pb-210 activity profile. Radionuclide flux geochronologies have been interpreted on the basis of a fluvial-marine transport model which distinguishes between inputs due to direct adsorption of radionuclides onto particles in the water column and inputs resulting from the erosion of particle-associated radionuclides from the drainage basin. Rate constants corresponding to residence times of one year for Cs-137 and Pu-239,240 in the water column and 1500 years for each radionuclide in the drainage basin provide reasonable agreement between the model and experimental results, although there is some evidence for a slightly longer drainage basin residence time for plutonium. Both the threshold for the initial appearance of Pu-238, derived from the atmospheric burnup of a SNAP-9A satellite reactor in 1964, and the magnitude of its isotopic dilution by drainage basin inputs of Pu-239,240 are also in agreement with model predictions.