Potential Releases of (129)I, (236)U, and Pu Isotopes from the Fukushima Dai-ichi Nuclear Power Plants to the Ocean from 2013 to 2015.

After the Fukushima Dai-ichi nuclear accident, many efforts were put into the determination of the presence of (137)Cs, (134)Cs, (131)I, and other gamma-emitting radionuclides in the ocean, but minor work was done regarding the monitoring of less volatile radionuclides, pure beta-ray emitters or simply radionuclides with very long half-lives. In this study we document the temporal evolution of (129)I, (236)U, and Pu isotopes ((239)Pu and (240)Pu) in seawater sampled during four different cruises performed 2, 3, and 4 years after the accident, and we compare the results to (137)Cs collected at the same stations and depths. Our results show that concentrations of (129)I are systematically above the nuclear weapon test levels at stations located close to the FDNPP, with a maximum value of 790 × 10(7) at·kg(-1), that exceeds all previously reported (129)I concentrations in the Pacific Ocean. Yet, the total amount of (129)I released after the accident in the time 2011-2015 was calculated from the (129)I/(137)Cs ratio of the ongoing (137)Cs releases and estimated to be about 100 g (which adds to the 1 kg released during the accident in 2011). No clear evidence of Fukushima-derived (236)U and Pu isotopes has been found in this study, although further monitoring is encouraged to elucidate the origin of the highest (240)Pu/(239)Pu atom ratio of 0.293 ± 0.028 we found close to FDNPP.