Effects of grain size, mineralogy, and acid-extractable grain coatings on the distribution of the fallout radionuclides Be-7, Be-10, Cs-137, and Pb-210 in river sediment
Grain-size dependencies in fallout radionuclide activity have been attributed to either increase in specific surface area in finer grain sizes or differing mineralogical abundances in different grain sizes. Here, we consider a third possibility, that the concentration and composition of grain coatings, where fallout radionuclides reside, controls their activity in fluvial sediment. We evaluated these three possible explanations in two experiments: (1) we examined the effect of sediment grain size, mineralogy, and composition of the acid-extractable materials on the distribution of Be-7, Be-10, Cs-137, and unsupported Pb-210 in detrital sediment samples collected from rivers in China and the United States, and (2) we periodically monitored 7 Be, Cs-137, and Pb-210 retention in samples of known composition exposed to natural fallout in Ohio, USA for 294 days. Acid-extractable materials (made up predominately of Fe, Mn, Al, and Ca from secondary minerals and grain coatings produced during pedogenesis) are positively related to the abundance of fallout radionuclides in our sediment samples. Grain-size dependency of fallout radionuclide concentrations was significant in detrital sediment samples, but not in samples exposed to fallout under controlled conditions. Mineralogy had a large effect on Be-7 and Pb-210 retention in samples exposed to fallout, suggesting that sieving sediments to a single grain size or using specific surface area-based correction terms may not completely control for preferential distribution of these nuclides. We conclude that time-dependent geochemical, pedogenic, and sedimentary processes together result in the observed differences in nuclide distribution between different grain sizes and substrate compositions. These findings likely explain variability of measured nuclide activities in river networks that exceeds the variability introduced by analytical techniques as well as spatial and temporal differences in erosion rates and processes. In short, we suggest that presence and amount of pedogenic grain coatings is more important than either specific surface area or surface charge in setting the distribution of fallout radionuclides.