Validating plutonium-239+240 as a novel soil redistribution tracer – a comparison to measured sediment yield

Abstract

Quantifying soil redistribution rates is a global challenge addressed with direct sediment measurements (e.g. traps), models, and isotopic, geochemical, and radionuclide tracers. The isotope of plutonium, namely 239+240Pu, is a relatively new soil redistribution tracer in this challenge. Direct validation of 239+240Pu as a soil redistribution tracer is, however, still missing. We used a unique sediment yield time series in southern Italy, reaching back to the initial fallout of 239+240Pu to verify 239+240Pu as a soil redistribution tracer. Distributed soil samples (n=55) were collected in the catchment, and at undisturbed reference sites (n=22), 239+240Pu was extracted, measured with inductively coupled plasma mass spectrometry (ICP-MS), and converted to soil redistribution rates. Finally, we used a generalized additive model (GAM) to regionalize soil redistribution estimates for the catchment. For the catchment sites, mean 239+240Pu inventories were significantly reduced (16.8 ± 10.2 Bq m−2) compared to the reference inventory (40.5 ± 3.5 Bq m−2), indicating the dominance of erosion. Converting these inventory losses into soil erosion rates resulted in an average soil loss of 22.2 ± SD 7.2 t ha−1 yr−1. The uncertainties of the approach stemmed mainly from the high measurement uncertainties of some low-activity samples where samples have been bulked over depth. Therefore, we recommend taking incremental soil samples and extracting larger soil volumes (∼ 20 g). The geographic coordinates and the flow accumulation best described the spatial pattern of erosion rates in the GAM model. Using those predictors to upscale Pu-derived soil redistribution rates for the entire catchment resulted in an average on-site loss of 20.7 t ha−1 yr−1, which corresponds very well to the long-term average sediment yield of 18.7 t ha−1 yr−1 measured at the catchment outlet and to 137Cs-derived soil redistribution rates. Overall, this comparison of Pu-derived soil redistribution rates with measured sediment yield data validates 239+240Pu as a suitable retrospective soil redistribution tracer.