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First determination of Pu isotopes ($$^{239}$$Pu, $$^{240}$$Pu and $$^{241}$$Pu) in radioactive particles derived from Fukushima Daiichi Nuclear Power Plant accident

福島第一原子力発電所事故に由来する放射性粒子中のPu同位体($$^{239}$$Pu, $$^{240}$$Pu and $$^{241}$$Pu)の最初の決定

五十嵐 淳哉*; Zheng, J.*; Zhang, Z.*; 二宮 和彦*; 佐藤 志彦  ; 福田 美保*; Ni, Y.*; 青野 辰雄*; 篠原 厚*

Igarashi, Junya*; Zheng, J.*; Zhang, Z.*; Ninomiya, Kazuhiko*; Satou, Yukihiko; Fukuda, Miho*; Ni, Y.*; Aono, Tatsuo*; Shinohara, Atsushi*

TEPCO福島第一原子力発電所(福島原発)事故によって放射性微粒子が放出された。この粒子の生成過程を解明するために、この粒子中の化学組成に関してこれまで多くの研究が行われてきた。しかし、この粒子中に核燃料由来の放射性物質が含まれているかまで、明らかにされていなかった。そこで、放射化学法とICP-MSを用いて、粒子中のプルトニウム(Pu)の測定を行った。結果、放射性粒子中の$$^{239+240}$$Puと$$^{241}$$Pu濃度範囲は、それぞれ(1.70-7.06)$$times$$10$$^{-5}$$Bqと(4.10-8.10)$$times$$10$$^{-3}$$Bqであった。$$^{240}$$Pu/$$^{239}$$Puと$$^{241}$$Pu/$$^{239}$$Puの同位体原子比は、ORIGENコードを用いたシミュレーションの結果やこれまでに福島原発事故後に様々な環境試料の測定結果の範囲にあった。また土壌中の放射性微粒子(SP)は、$$^{134}$$Cs/$$^{137}$$Cs放射能比等から2と3号機由来の粒子と特定できたが、Puは検出されなかった。ダスト中の放射性微粒子(DP)は、$$^{134}$$Cs/$$^{137}$$Cs放射能比から福島原発1号機由来と特定でき、さらにDP3粒子中2粒子からPuが検出され、これは福島原発事故由来のPuであった。

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 ($$^{239}$$Pu, $$^{240}$$Pu and $$^{241}$$Pu) 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 $$^{239+240}$$Pu and $$^{241}$$Pu were (1.70-7.06)$$times$$10$$^{-5}$$ Bq and (4.10-8.10)$$times$$10$$^{-3}$$ Bq, respectively and atom ratios of $$^{240}$$Pu/$$^{239}$$Pu and $$^{241}$$Pu/$$^{239}$$Pu 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.

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パーセンタイル:100

分野:Multidisciplinary Sciences

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