Remobilisation of radiocaesium from bottom sediments to water column in reservoirs in Fukushima, Japan

Abstract

Reservoir sediments generally act as a sink for radionuclides derived from nuclear accidents, but under anaerobic conditions, several radionuclides remobilise in bioavailable form from sediments to water columns, which may contribute to the long-term contamination of aquatic products. This study systematically investigated the ¹³⁷Cs activities of sediment-pore water, providing a direct evidence of the remobilisation of bioavailable ¹³⁷Cs from sediments in two highly contaminated reservoirs affected by the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. We observed that the dissolved ¹³⁷Cs activity concentration of pore water (3.0-65.8 Bq L^-1) was one to two orders of magnitude higher than that of reservoir water. Moreover, the distribution coefficient (K_d) values for the ¹³⁷Cs of sediment-pore water (2.6-14 × 10³ L kg^-1) decreased with depth. The K_d values were significantly and negatively correlated with the concentration of the major ¹³⁷Cs competing cation NH₄⁺. Our results strongly indicate a competitive ion exchange process between ¹³⁷Cs and NH₄⁺ via a highly selective interaction with the frayed edge sites of phyllosilicate minerals, which is the major reason for the variability of K_d values of sediment-pore water, even in the Fukushima case. Additionally, the sediment accumulation rates were relatively high, and the annual depositional rate of exchangeable ¹³⁷Cs prevailed over the annual diffusive flux of ¹³⁷Cs from the sediment to the overlying water. This finding indicates that even after 10 years since the FDNPP accident, the bioavailable ¹³⁷Cs is still continuously supplied from the catchment covered by mountainous forests, and reservoir sediments are a long-term important source of bioavailable ¹³⁷Cs in the riverine system. Our findings provide important parameter values for mid- and long-term assessments of the radiation impact of radionuclide discharges to freshwater environments.

Keywords: Fukushima; Pore water; Radiocaesium; Reservoir; Sediment.