Linking heterogeneous distribution of radiocaesium in soils and pond sediments in the Fukushima Daiichi exclusion zone to mobility and potential bioavailability

During the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident in 2011 significant amounts of radiocaesium were released into the atmosphere from the reactor units 1, 2 and 3. This caused a non-uniform deposition, in composition and direction, of ¹³⁴Cs and ¹³⁷Cs in the near field (<30 km) from the reactors. In this work, we elucidate the influence of speciation, including radioactive particles, on mobility and potential bioavailability of radiocaesium in soils and sediments from sites located in different directions and distances from the FDNPP. Samples collected in September 2016 were characterized and subjected to sequential chemical extractions and simulated gastrointestinal fluid leaching, and the ¹³⁷Cs and ¹³⁴Cs activities were determined in bulk, grain-size and extracted fractions. The results show that radiocaesium was mainly irreversibly bound and in an inert form. Combined, the two forms contained >90% of the activity present in soils and ~84% in sediments. Digital autoradiography revealed that the inert fraction was predominantly associated with heterogeneities, an indication of radioactive particles. The frequency of heterogeneities was correlated with ¹³⁷Cs activity concentrations, and both were in agreement with the ambient equivalent air doses measured in situ during sampling. Moreover, in situ gamma spectrometry measurements were used in the InSiCal software tool to derive ¹³⁴Cs and ¹³⁷Cs surface contamination. Soil activity concentrations and contamination density estimations, decay-corrected to the day of the FDNPP accident, resulted in ¹³⁴Cs/¹³⁷Cs ratios that match the reported release and deposition plumes from the reactor units. Overall, these results demonstrate the persistence of the particle contamination in the Fukushima near field and highlight the importance of including radioactive particles in environmental impact assessments.