Radium-based estimates of cesium isotope transport and total direct ocean discharges from the Fukushima Nuclear Power Plant accident

Abstract

Radium has four naturally occurring isotopes that have proven useful in constraining water mass source, age, and mixing rates in the coastal and open ocean. In this study, we used radium isotopes to determine the fate and flux of runoff-derived cesium from the Fukushima Dai-ichi Nuclear Power Plant (FNPP). During a June 2011 cruise, the highest cesium (Cs) concentrations were found along the eastern shelf of northern Japan, from Fukushima south, to the edge of the Kuroshio Current, and in an eddy ~ 130 km from the FNPP site. Locations with the highest cesium also had some of the highest radium activities, suggesting much of the direct ocean discharges of Cs remained in the coastal zone 2–3 months after the accident. We used a short-lived Ra isotope (223Ra, t1/2 = 11.4 d) to derive an average water mass age (Tr) in the coastal zone of 32 days. To ground-truth the Ra age model, we conducted a direct, station-by-station comparison of water mass ages with a numerical oceanographic model and found them to be in excellent agreement (model avg. Tr = 27 days). From these independent Tr values and the inventory of Cs within the water column at the time of our cruise, we were able to calculate an offshore 134Cs flux of 3.9–4.6 × 1013 Bq d−1. Radium-228 (t1/2 = 5.75 yr) was used to derive a vertical eddy diffusivity (Kz) of 0.7 m2 d−1 (0.1 cm2 s−1); from this Kz and 134Cs inventory, we estimated a 134Cs flux across the pycnocline of 1.8 × 104 Bq d−1 for the same time period. On average, our results show that horizontal mixing loss of Cs from the coastal zone was ~ 109 greater than vertical exchange below the surface mixed layer. Finally, a mixing/dilution model that utilized our Ra-based and oceanographic model water mass ages produced a direct ocean discharge of 134Cs from the FNPP of 11–16 PBq at the time of the peak release in early April 2011. Our results can be used to calculate discharge of other water-soluble radionuclides that were released to the ocean directly from the Fukushima NPP.