ABSTRACT
The structural form and elemental distribution of material originating from different Fukushima Daiichi Nuclear Power Plant reactors (Units 1 and 3) is hereby examined to elucidate their contrasting release dynamics and the current in-reactor conditions to influence future decommissioning challenges. Complimentary computed X-ray absorption tomography and X-ray fluorescence data show that the two suites of Si-based material sourced from the different reactor Units have contrasting internal structure and compositional distribution. The known event and condition chronology correlate with the observed internal and external structures of the particulates examined, which suggest that Unit 1 ejecta material sustained a greater degree of melting than that likely derived from reactor Unit 3. In particular, we attribute the near-spherical shape of Unit 1 ejecta and their internal voids to there being sufficient time for surface tension to round these objects before the hot (and so relatively low viscosity) silicate melt cooled to form glass. In contrast, a more complex internal form associated with the sub-mm particulates invoked to originate from Unit 3 suggest a lower peak temperature, over a longer duration. Using volcanic analogues, we consider the structural form of this material and how it relates to its environmental particulate stability and the bulk removal of residual materials from the damaged reactors. We conclude that the brittle and angular Unit 3 particulate are more susceptible to further fragmentation and particulate generation hazard than the round, higher-strength, more homogenous Unit 1 material.
ABSTRACT
Radioactive particles were released into the environment during the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. Many studies have been conducted to elucidate the chemical composition of released radioactive particles in order to understand their formation process. However, whether radioactive particles contain nuclear fuel radionuclides remains to be investigated. Here, we report the first determination of Pu isotopes in radioactive particles. To determine the Pu isotopes (239Pu, 240Pu and 241Pu) in radioactive particles derived from the FDNPP accident which were free from the influence of global fallout, radiochemical analysis and inductively coupled plasma-mass spectrometry measurements were conducted. Radioactive particles derived from unit 1 and unit 2 or 3 were analyzed. For the radioactive particles derived from unit 1, activities of 239+240Pu and 241Pu were (1.70-7.06) × 10-5 Bq and (4.10-8.10) × 10-3 Bq, respectively and atom ratios of 240Pu/239Pu and 241Pu/239Pu were 0.330-0.415 and 0.162-0.178, respectively. These ratios were consistent with the simulation results from ORIGEN code and measurements from various environmental samples. In contrast, Pu was not detected in the radioactive particles derived from unit 2 or 3. The difference in Pu contents is clear evidence towards different formation processes of radioactive particles, and detailed formation processes can be investigated from Pu analysis.
ABSTRACT
The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident released abundant radioactive particles into the surrounding environment. Herein, we analyzed the activity of 90Sr in these particles to estimate the contribution of this radionuclide to the overall radiation exposure and shed light on the processes that occurred during the accident. Seven radioactive particles were isolated from the dust and soil samples collected from areas surrounding the FDNPP, and the minimum/maximum 137Cs activities were determined as 224/4,100 Bq. Based on the size, specific activity, and 134Cs/137Cs activity ratios, we concluded that six of the seven radioactive particles were released from the Unit 1 reactor, while one particle was released from the Unit 3 reactor by a hydrogen explosion. Strontium-90 was detected in all radioactive particles, and the minimal/maximal 90Sr activities were determined as 0.046/1.4 Bq. 137Cs/90Sr activity ratios above 1000 were observed for all seven particles, that is, compared to 137Cs, 90Sr had negligible contribution to the overall radiation exposure. The 137Cs/90Sr activity ratios of the radioactive particles were similar to those of terrestrial environmental samples and were higher for particles released from the Unit 1 reactor than for samples collected from the Unit 1 reactor building, which indicates possibility of additional 90Sr-rich contamination after release of the particles.
