TY - JOUR
T1 - Particulate plutonium released from the Fukushima Daiichi meltdowns
AU - Kurihara, Eitaro
AU - Takehara, Masato
AU - Suetake, Mizuki
AU - Ikehara, Ryohei
AU - Komiya, Tatsuki
AU - Morooka, Kazuya
AU - Takami, Ryu
AU - Yamasaki, Shinya
AU - Ohnuki, Toshihiko
AU - Horie, Kenji
AU - Takehara, Mami
AU - Law, Gareth T.W.
AU - Bower, William
AU - W. Mosselmans, J. Frederick
AU - Warnicke, Peter
AU - Grambow, Bernd
AU - Ewing, Rodney C.
AU - Utsunomiya, Satoshi
N1 - Funding Information:
The authors are grateful to Dr. Watanabe for her assistance on SEM analyses at the Center of Advanced Instrumental Analysis, Kyushu University. This study is partially supported by JST Initiatives for Atomic Energy Basic and Generic Strategic Research and by a Grant-in-Aid for Scientific Research (KAKENHI) from the Japan Society for the Promotion of Science ( 16K12585 , 16H04634 , JP26257402 ). S.U. is also supported by The Mitsubishi Foundation /Research Grants in the Natural Sciences, Environmental Radioactivity Research Network Center ( F-19-03 ), and by ESPEC Foundation for Global Environment Research and Technology (Charitable Trust) (ESPEC Prize for the Encouragement of Environmental Studies). G.T.W.L. and W.R.B acknowledge UK NERC funding ( NE/M014088/1 ). The Diamond Light Source ( NT21211-1 ) and the Swiss Light Source ( 20181008 ) are thanked for analysis time, and Connaugh Fallon (University of Manchester) is thanked for assisting with the SR-μXRF and XANES analysis. R.C.E. was partially supported by the U.S. Department of Energy , National Nuclear Security Administration , Office of Defense Nuclear Nonproliferation Research and Development under Contract No. DE-AC02-76SF00515 . The findings and conclusions by the authors of this paper do not necessarily state or reflect those of the JST.
Funding Information:
The authors are grateful to Dr. Watanabe for her assistance on SEM analyses at the Center of Advanced Instrumental Analysis, Kyushu University. This study is partially supported by JST Initiatives for Atomic Energy Basic and Generic Strategic Research and by a Grant-in-Aid for Scientific Research (KAKENHI) from the Japan Society for the Promotion of Science (16K12585, 16H04634, JP26257402). S.U. is also supported by The Mitsubishi Foundation/Research Grants in the Natural Sciences, Environmental Radioactivity Research Network Center (F-19-03), and by ESPEC Foundation for Global Environment Research and Technology (Charitable Trust) (ESPEC Prize for the Encouragement of Environmental Studies). G.T.W.L. and W.R.B acknowledge UK NERC funding (NE/M014088/1). The Diamond Light Source (NT21211-1) and the Swiss Light Source (20181008) are thanked for analysis time, and Connaugh Fallon (University of Manchester) is thanked for assisting with the SR-?XRF and XANES analysis. R.C.E. was partially supported by the U.S. Department of Energy, National Nuclear Security Administration, Office of Defense Nuclear Nonproliferation Research and Development under Contract No. DE-AC02-76SF00515. The findings and conclusions by the authors of this paper do not necessarily state or reflect those of the JST.
Publisher Copyright:
© 2020 Elsevier B.V.
PY - 2020/11/15
Y1 - 2020/11/15
N2 - Traces of Pu have been detected in material released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) in March of 2011; however, to date the physical and chemical form of the Pu have remained unknown. Here we report the discovery of particulate Pu associated with cesium-rich microparticles (CsMPs) that formed in and were released from the reactors during the FDNPP meltdowns. The Cs-pollucite-based CsMP contained discrete U(IV)O2 nanoparticles, <~10 nm, one of which is enriched in Pu adjacent to fragments of Zr-cladding. The isotope ratios, 235U/238U, 240Pu/239Pu, and 242Pu/239Pu, of the CsMPs were determined to be ~0.0193, ~0.347, and ~0.065, respectively, which are consistent with the calculated isotopic ratios of irradiated-fuel fragments. Thus, considering the regional distribution of CsMPs, the long-distance dispersion of Pu from FNDPP is attributed to the transport by CsMPs that have incorporated nanoscale fuel fragments prior to their dispersion up to 230 km away from the Fukushima Daiichi reactor site.
AB - Traces of Pu have been detected in material released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) in March of 2011; however, to date the physical and chemical form of the Pu have remained unknown. Here we report the discovery of particulate Pu associated with cesium-rich microparticles (CsMPs) that formed in and were released from the reactors during the FDNPP meltdowns. The Cs-pollucite-based CsMP contained discrete U(IV)O2 nanoparticles, <~10 nm, one of which is enriched in Pu adjacent to fragments of Zr-cladding. The isotope ratios, 235U/238U, 240Pu/239Pu, and 242Pu/239Pu, of the CsMPs were determined to be ~0.0193, ~0.347, and ~0.065, respectively, which are consistent with the calculated isotopic ratios of irradiated-fuel fragments. Thus, considering the regional distribution of CsMPs, the long-distance dispersion of Pu from FNDPP is attributed to the transport by CsMPs that have incorporated nanoscale fuel fragments prior to their dispersion up to 230 km away from the Fukushima Daiichi reactor site.
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U2 - 10.1016/j.scitotenv.2020.140539
DO - 10.1016/j.scitotenv.2020.140539
M3 - Article
C2 - 32663681
AN - SCOPUS:85087770096
VL - 743
JO - Science of the Total Environment
JF - Science of the Total Environment
SN - 0048-9697
M1 - 140539
ER -