RESUMO
Following the Fukushima Daiichi Nuclear Power Plant disaster in March 2011, the Japanese government initiated an unprecedented decontamination programme to remediate 137Cs-contaminated soils and allow population return. This programme involved the removal of topsoil under farmland and residential land, and its replacement with "fresh soil" composed of granitic saprolite. However, decontamination was limited to these two land uses, without remediating forests, which cover 70 % of the surface area in the affected region. In this unprecedented context, the specific impact of this unique decontamination programme on 137Cs transfers in river systems remains to be quantified at the catchment scale. In this study, based on the analysis of a sediment core collected in June 2021 in the Mano Dam reservoir draining a decontaminated catchment, the effects of soil decontamination on particle-bound 137Cs dynamics and sediment source contributions in response to a succession of extreme precipitation events were retrospectively assessed. The sequence of sediment layer deposition and its chronology were reconstructed through the analysis of several diagnostic properties (organic matter, elemental geochemistry, visible colourimetry, granulometry) and contextual information. During abandonment (2011-2016), cropland contribution decreased (31 %). Concurrently, 137Cs activity and deposition flux decreased (19 and 29%year-1, respectively). Following decontamination (2017), sediment transfer increased (270 %) in response to increased contributions from decontaminated cropland and "fresh soil" (625 % and 180 % respectively). Meanwhile, forest contributions remained stable. In contrast, 137Cs activity dropped (65 %), although 137Cs deposition flux remained constant. Forests acted as a stable source of 137Cs. Accordingly, 137Cs deposition flux after decontamination (2016-2021) was similar to that observed during the 5-years period of land abandonment (2011-2016), as a result of the regrowth of spontaneous vegetation over farmland, protecting soil against erosion. Future research should further investigate the impact of longer land abandonment that prevailed in some regions decontaminated lately on the 137Cs fluxes in the rivers.
RESUMO
In 2011, the Fukushima Dai-Ichi Nuclear Power Plant (FDNPP) accident released significant quantities of radionuclides into the environment. Japanese authorities decided to progressively reopen the Difficult-To-Return Zone after the decontamination of priority reconstruction zones. These areas include parts of the initially highly contaminated municipalities located to the north of the FDNPP, including Namie Town, an area drained by the Ukedo and Takase Rivers. Eleven years after the accident, research focused on the spatial distribution of plutonium (Pu) and radiocesium (Cs) isotopes at contrasted individual locations. To complement previous results, the current research was conducted on flood sediment deposits collected at the same locations after major flooding events during eleven fieldwork campaigns organised between 2013 and 2020 at the outlet of the Ukedo and Takase Rivers (n = 22). The results highlighted a global decrease of the Pu and 137Cs contents in sediment with time during the abandonment phase in the region, from 2013 (238.20 fg g-1) to 2020 (4.28 fg g-1). Furthermore, based on the analysis of the 240Pu/239Pu isotopic ratios, the plutonium transiting these rivers (range: 0.166 - 0.220) essentially originated from the global fallout (0.180 ± 0.014 (Kelley et al., 1999)). Sediment showed contrasted properties in the two investigated rivers, which is likely mainly the result of the occurrence of Ogaki Dam on upper sections of the Ukedo River as it strongly impacts the material supply from this river to the Pacific Ocean. A statistical analysis highlighted the strong correlation between Pu activity concentrations and 137Cs activities in both rivers, confirming that both radionuclides are transported with a similar pathway. Despite it was detected early after the accident (2011-2013), the current research demonstrates that plutonium originating from FDNPP is no longer detected in these rivers draining the Difficult-To-Return Zone at the onset of the reopening of the area to its former inhabitants.