~(137)Cs Activities and ~(135)Cs/~(137)Cs Isotopic Ratios from Soils at Idaho National Laboratory: A Case Study for Contaminant Source Attribution in the Vicinity of Nuclear Facilities

摘要

Radiometric and mass spectrometric analyses of Cs contamination in the environment can reveal the location of Cs emission sources, release mechanisms, modes of transport, prediction of future contamination migration, and attribution of contamination to specific generator(s) and/or process(es). The Subsurface Disposal Area (SDA) at Idaho National Laboratory (INL) represents a complicated case study for demonstrating the current capabilities and limitations to environmental Cs analyses. ~(137)Cs distribution patterns, ~(135)Cs/~(137)Cs isotope ratios, known Cs chemistry at this site, and historical records enable narrowing the list of possible emission sources and release events to a single source and event, with the SDA identified as the emission source and flood transport of material from within Pit 9 and Trench 48 as the primary release event These data combined allow refining the possible number of waste generators from dozens to a single generator, with INL on-site research and reactor programs identified as the most likely waste generator. A discussion on the ultimate limitations to the information that ~(135)Cs/~(137)Cs ratios alone can provide is presented and includes (1) uncertainties in the exact date of the fission event and (2) possibility of mixing between different Cs source terms (including nuclear weapons fallout and a source of interest).