Abstract
Isotopic ratios of plutonium and uranium in soil samples were investigated, in order to understand the level of contamination with plutonium and uranium released at the accident of Fukushima Daiichi nuclear power plant. At first, plutonium and uranium were recovered from the standard reference soil/sediment materials by extraction/ion-exchange chromatography, and their isotope compositions were analyzed by TIMS. By applying our analytical technique to soil samples obtained from Fukushima prefecture, a possibility of atmospheric release of nuclear fuel material during the accident of FDNPP was discussed. The contamination with uranium was under detection limit, while that with plutonium was observed.
Similar content being viewed by others
References
Zheng J, Tagami K, Uchida S (2012) Rapid analysis of U isotopes in vegetables using ICP–MS: application to the emergency U monitoring after the nuclear accident at TEPCO’s Fukushima Dai-ichi power station. J Radioanal Nucl Chem 292:171–175
Yamamoto M, Sakaguchi A, Ochiai S, Imanaka T (2014) Isotopic compositions of transuranic nuclides released by the Fukushima Daiichi nuclear power plant accident: with emphasis on Cm isotopes. J Radioanal Nucl Chem 300:1045–1052
Bu W, Zheng J, Guo Q, Aono T, Otosaka S, Tagami K, Uchida S (2015) Temporal distribution of plutonium isotopes in marine sediments off Fukushima after the Fukushima Daiichi nuclear power plant accident. J Radioanal Nucl Chem 303:1151–1154
Oikawa S, Watabe T, Takata H, Misonoo J, Kusakabe M (2015) Plutonium isotopes and 241Am in surface sediments off the coast of the Japanese islands before and soon after the Fukushima Daiichi nuclear power plant accident. J Radioanal Nucl Chem 303:1513–1518
Yamamoto M (2015) Overview of the Fukushima Daiichi nuclear power plant (FDNPP) accident, with amounts and isotopic compositions of the released radionuclides. J Radioanal Nucl Chem 303:1227–1231
Schwantes JM, Orton CR, Clark RA (2012) Analysis of a nuclear accident: fission and activation product releases from the Fukushima Daiichi nuclear facility as remote indicators of source identification, extent of release, and state of damaged spent nuclear fuel. Environ Sci Technol 46:8621–8627
Bu W, Fukuda M, Zheng J, Aono T, Ishimaru T, Kanda J, Yang G, Tagami K, Uchida S, Guo Q, Yamada M (2014) Release of Pu isotopes from the Fukushima Daiichi nuclear power plant to the marine environment was negligible. Environ Sci Technol 48:9070–9078
Shibahara Y, Kubota T, Fujii T, Fukutani S, Ohta T, Takamiya K, Okumura R, Mizuno S, Yamana H (2014) Analysis of cesium isotope compositions in environmental samples by thermal ionization mass spectrometry-1. a preliminary study for source analysis of radioactive contamination in Fukushima prefecture. J Nucl Sci Technol 51:575–579
Kubota T, Shibahara Y, Fukutani S, Fujii T, Ohta T, Kowatari M, Mizuno S, Takamiya K, Yamana H (2015) Cherenkov counting of 90Sr and 90Y in bark and leaf samples collected around Fukushima Daiichi nuclear power plant. J Radioanal Nucl Chem 303:39–46
Bohlke JK, de Laeter JR, De Bievre P, Hidaka H, Peiser HS, Rosma KJR, Taylor PDP (2005) Isotopic compositions of the elements, 2001. J Phys Chem Ref Data 34:57–68
Nishihara K, Iwamoto H, Suyama K (2012) JAEA-Data/Code 2012-018. http://jolissrch-inter.tokai-sc.jaea.go.jp/pdfdata/JAEA-Data-Code-2012-018.pdf. Accessed 30 Mar 2015
Zheng J, Tagami K, Watanabe Y, Uchida S, Aono T, Ishii Yohsida S, Kubota Y, Fuma S, Ihara S (2012) Isotopic evidence of plutonium release into the environment from the Fukushima DNPP accident. Sci Rep 2:304. doi:10.1038/srep02988
Schneider S, Walther C, Bister S, Schauer V, Christl M, Synal HA, Shozugawa K, Steinhauser G (2013) Plutonium release from Fukushima Daiichi fosters the need for more detailed investigations. Sci Rep 3:2988. doi:10.1038/srep02988
Evrard O, Pointurier F, Onda Y, Chartin C, Hubert A, Lepage H, Pottin AC, Lefevre I, Bonte P, Laceby JP, Ayrault S (2014) Novel insights into Fukushima nuclear accident from isotopic evidence of plutonium spread along coastal rivers. Environ Sci Technol 48:9334–9340
Kelley JM, Bond LA, Beasley TM (1999) Global distribution of Pu isotope and Np. Sci Total Environ 237(238):483–550
Muramatsu Y, Ruhm W, Yoshida S, Tagami K, Uchida S, Wirth E (2000) Concentrations of 239Pu and 240Pu and their isotopic ratios determined by ICP-MS in soils collected from the Chernobyl 30 km zone. Environ Sci Technol 34:2913–2917
Shibahara Y, Kubota T, Fujii T, Fukutani S, Ohta T, Takamia K, Okumura R, Mizuno S, Yamana H (2015) 235U/238U isotopic ratio in plant samples from Fukushima prefecture. J Radioanal Nucl Chem 303:1421–1424
Lindahl P, Keith-Roach M, Worsfold P, Choi MS, Shin HS, Lee SH (2010) Ultra-trace determination of plutonium in marine samples using multi-collector inductively coupled plasma mass spectrometry. Anal Chim Acta 671:61–69
Richter S, Goldberg SA (2003) Improved techniques for high accuracy isotope ratio measurements of nuclear materials using thermal ionization mass spectrometry. Int J Mass Spectrom 229:181–197
Platzner IT (1997) Modern isotope ratio mass spectrometry. Willey, Chichester
Zheng J, Yamada M (2006) Determination of U isotope ratios in sediments using ICP-QMS after sample cleanup with anion-exchange and extraction chromatography. Talanta 68:932–939
Taylor RN, Croudace IW, Warwick PE, Dee SJ (1998) Precise and rapid determination of 238U/235U and uranium concentration in soil samples using thermal ionization mass spectrometry. Chem Geol 144:73–80
Taylor SR, McLennan SM (1985) The continental crust: its composition and evolution. Blackwell, Oxford
Shinonaga T, Steier P, Lagos M, Ohkura T (2014) Airborne plutonium and non-natural uranium from the Fukushima DNPP found at 120 km distance a few days after rector hydrogen explosions. Environ Sci Technol 48:3808–3814
Steinhauser G (2014) Fukushima’s forgotten radionuclides: a review of the understudied radioactive emissions. Environ Sci Technol 48:4649–4663
Bu W, Zheng J, Guo Q, Aono T, Tazoe H, Tagami K, Uchida S, Yamada M (2014) A method of measurement of 239Pu, 240Pu, 241Pu in high U content marine sediments by sector field ICP-MS and its application to Fukushima sediment samples. Environ Sci Technol 48:534–541
Liao H, Zheng J, Wu F, Yamada M, Tan M, Chen J (2008) Determination of plutonium isotopes in freshwater lake sediments by sector-field ICP-MS after separation using ion-exchange chromatography. Appl Rad Isot 66:1138–1145
Zheng J, Tagami K, Uchida S (2013) Release of plutonium isotopes into the environment from the Fukushima Daiichi nuclear power plant accident: what is known and what needs to be known. Environ Sci Technol 47:9584–9595
Yang G, Zheng J, Tagami K, Uchida S (2015) Plutonium concentration and isotopic ratio in soil samples from central-eastern Japan collected around the 1970s. Sci Rep 5:9636. doi:10.1038/srep09636
Sources and effects of ionization radiation http://www.unscear.org/docs/reports/2008/11-80076_Report_2008_Annex_D.pdf. Accessed 30 Mar 2015
http://www.mext.go.jp/b.menu/shingi/chousa/gijyutu/017/shiryo/_icsFiles/afieldfile/2011/09/02/1310688.1.pdf. Accessed 16 Dec 2013
Acknowledgments
This work was supported by the KUR Research Program for Scientific Basis of Nuclear Safety.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Shibahara, Y., Kubota, T., Fujii, T. et al. Determination of isotopic ratios of plutonium and uranium in soil samples by thermal ionization mass spectrometry. J Radioanal Nucl Chem 307, 2281–2287 (2016). https://doi.org/10.1007/s10967-015-4551-1
Received:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10967-015-4551-1