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Compositional and structural analysis of Fukushima-derived particulates using high-resolution X-ray imaging and synchrotron characterisation techniques

Martin, P. G.*; Jones, C. P.*; Cipiccia, S.*; Batey, D. J.*; Hallam, K. R.*; 佐藤 志彦; Griffiths, I.*; Rau, C.*; Richards, D. A.*; 末木 啓介*; et al.

Scientific Reports (Internet), 10(1), p.1636_1 - 1636_11, 2020/01

Both the three-dimensional internal structure and elemental distribution of near-field radioactive fallout particulate material released during the March 2011 accident at the Fukushima Daiichi Nuclear Power Plant is analysed using combined high-resolution laboratory and synchrotron radiation X-ray techniques. Results from this study allow for the proposition of the likely formation mechanism of the particles, as well as the potential risks associated with their existence in the environment, and the likely implications for future planned reactor decommissioning. A suite of particles is analyzed from a locality 2 km from the north-western perimeter of the site north of the primary contaminant plume in an area formerly attributed to being contaminated by fallout from reactor Unit 1. The particles are shown to exhibit significant structural similarities; being amorphous with a textured exterior, and containing inclusions of contrasting compositions, as well as an extensive internal void volume bimodal in its size distribution. A heterogeneous distribution of the various elemental constituents is observed inside a representative particle, which also exhibited a Fukushima-derived radiocesium ($$^{134}$$Cs, $$^{135}$$Cs and $$^{137}$$Cs) signature with negligible natural Cs. We consider the structure and composition of the particle to suggest it formed from materials associated with the reactor Unit 1 building explosion, with debris fragments embedded into the particles surface. Such a high void ratio, comparable to geological pumice, suggests such material formed during a rapid depressurisation and is potentially susceptible to fragmentation through attrition.


A Review of Cs-bearing microparticles in the environment emitted by the Fukushima Dai-ichi Nuclear Power Plant accident

五十嵐 康人*; 小暮 敏博*; 栗原 雄一; 三浦 輝*; 奥村 大河*; 佐藤 志彦; 高橋 嘉夫*; 山口 紀子*

Journal of Environmental Radioactivity, 205-206, p.101 - 118, 2019/09

 被引用回数:7 パーセンタイル:18.27(Environmental Sciences)

福島第一原子力発電所事故ではチェルノブイリ原発事故と異なるケイ素,酸素,鉄,亜鉛を含む放射性微粒子が発見された。この放射性微粒子は高濃度のセシウムを含むことからセシウムマイクロパーティクル(CsMP)と呼ばれることもある。またこの粒子は少なくとも2種類が見つかっており、発見された順番に、2, 3号機(放出源未確定)と1号機由来をそれぞれTypeA, TypeBと呼んでおり、Cs同位体比, 形態, 採取場所で分類されている。本レビューではこれらの背景を含むCsMPの全体像を紹介する。


Formation of radioactive cesium microparticles originating from the Fukushima Daiichi Nuclear Power Plant accident; Characteristics and perspectives

大貫 敏彦*; 佐藤 志彦; 宇都宮 聡*

Journal of Nuclear Science and Technology, 56(9-10), p.790 - 800, 2019/09

 被引用回数:0 パーセンタイル:100(Nuclear Science & Technology)

Following the identification of radioactive particulates, particularly Cs microparticles (CsMPs) in aerosol samples collected on 14-15 March 2011 at Tsukuba, $$sim$$ 170 km south of the Fukushima Daiichi Nuclear Power Plant (FDNPP), numerous reports on CsMPs have been published. This paper reviews recent progress in the measurement and characterization of CsMPs by advanced analytical techniques, including advanced transmission electron microscopy (TEM) and synchrotron X-ray analysis. These analyses revealed that the CsMPs contained Si, Fe, Zn, Cs, and minor quantities of U together with some fission products. Uranium in the CsMPs was identified as being in the form of uraninite and (U,Zr)O$$_{2}$$. Detailed advanced TEM analysis has clarified some of the processes resulting in alteration of constituents of the nuclear fuels and containment vessel materials during this severe accident. In addition, the Tokyo Electric Power Company in cooperation with the Japan Atomic Energy Agency and the International Research Institute for Nuclear Decommissioning issued a detailed report on the elemental compositions and structures of the fuel debris fragments collected inside and outside of the primary containment vessel. This report highlighted the fact that the fuel debris fragments contained nanoparticles with the U and Zr components having similar structures to that of the CsMPs. This similarity in structures has stimulated further research on the structure and elemental constituents, especially for U and Zr in the CsMPs, and has opened up new avenues for studying the chemical characteristics of the fuel debris.


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

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*

Scientific Reports (Internet), 9(1), p.11807_1 - 11807_10, 2019/08



DNA damage induction during localized chronic exposure to an insoluble radioactive microparticle

松谷 悠佑; 佐藤 志彦; 浜田 信行*; 伊達 広行*; 石川 正純*; 佐藤 達彦

Scientific Reports (Internet), 9(1), p.10365_1 - 10365_9, 2019/07

 被引用回数:2 パーセンタイル:41.98(Multidisciplinary Sciences)

不溶性放射性微粒子(Cs含有粒子)は、呼吸器系に吸引された後、長期にわたって気管に付着し、微粒子周辺の正常組織に不均一な線量分布をもたらすと考えられている。このような微粒子によってもたらされる生物影響は不明なままであるため、本研究では、均一な被ばくとの比較の中で、微粒子による局所的慢性被ばく下において蓄積される核内DNA損傷を研究した。我々は、微粒子を含むマイクロキャピラリーを、正常肺細胞を含む培養皿に配置し、24時間もしくは48時間被ばく後に核内誘発$$gamma$$-H2AX focusの有意な変化を観察した。モンテカルロ計算と均一被ばくとの比較から、微粒子による局所被ばく下では、遠位細胞に対する細胞間シグナル誘発DNA損傷と近位細胞に対するDNA損傷誘発の低減(防御効果)の両者が誘発されることが示唆された。微粒子による臓器線量は微量であることから、従来の放射線リスク評価で十分であると思われる。本研究により、不溶性Cs含有粒子による不均一暴露下でのDNA損傷の空間分布を定量化することに初めて成功した。


Provenance of uranium particulate contained within Fukushima Daiichi Nuclear Power Plant Unit 1 ejecta material

Martin, P. G.*; Louvel, M.*; Cipiccia, S.*; Jones, C. P.*; Batey, D. J.*; Hallam, K. R.*; Yang, I. A. X.*; 佐藤 志彦; Rau, C.*; Mosselmans, J. F. W.*; et al.

Nature Communications (Internet), 10(1), p.2801_1 - 2801_7, 2019/06

 被引用回数:2 パーセンタイル:29.22(Multidisciplinary Sciences)



Activity of $$^{90}$$Sr in fallout particles collected in the difficult-to-return zone around the Fukushima Daiichi Nuclear Power Plant

Zhang, Z.*; 五十嵐 淳哉*; 佐藤 志彦; 二宮 和彦*; 末木 啓介*; 篠原 厚*

Environmental Science & Technology, 53(10), p.5868 - 5876, 2019/05

 被引用回数:3 パーセンタイル:19.27(Engineering, Environmental)




太田 祐貴*; 末木 啓介*; 笹 公和*; 高橋 努*; 松中 哲也*; 松村 万寿美*; 戸崎 裕貴*; 本多 真紀*; 細谷 青児*; 高野 健太*; et al.

JAEA-Conf 2018-002, p.99 - 102, 2019/02

福島第一原子力発電所事故により放出された放射性核種に長寿命の$$^{36}$$Cl(半減期: 30.1万年)がある。$$^{36}$$Clは放射性廃棄物の処理の際に土壌中における高い移動能と相まって重要な核種である。しかし、土壌中では無機塩素(Clinorg)が有機塩素(Clorg)に変換・保持されることで、その移動の機構は不明である。本研究では、汚染地域の無機$$^{36}$$Clの深度分布を得ることで$$^{36}$$Clの動態を検討し、事故による$$^{36}$$Cl汚染の程度を検討した。また、5cm表土に含まれる$$^{36}$$Clについても検討した。2017年における深度分布では、$$^{36}$$Cl濃度は表層で最も高くなり、深度とともに緩やかに減少した。一方で、$$^{36}$$Cl/Clはほぼ一定(平均値: 3.24$$pm$$0.55 ($$times$$10$$^{-12}$$))の値を示した。事故前の$$^{36}$$Cl/Clと比べると$$^{36}$$Cl/Clの増加を示し、事故由来の$$^{36}$$Clは土壌3.6g/cm$$^{2}$$(=5cm深)より深く移動していることが分かった。


Radiocarbon variations in tree rings since 1960 near the Tokai nuclear facility, Japan

松中 哲也*; 笹 公和*; 高橋 努*; 細谷 青児*; 松村 万寿美*; 佐藤 志彦; Shen, H.*; 末木 啓介*

Nuclear Instruments and Methods in Physics Research B, 439, p.64 - 69, 2019/01

 被引用回数:1 パーセンタイル:34.57(Instruments & Instrumentation)



Isotope-selective microscale imaging of radioactive Cs without isobaric interferences using sputtered neutral mass spectrometry with two-step resonant ionization employing newly-developed Ti:Sapphire lasers

坂本 哲夫*; 森田 真人*; 金成 啓太*; 富田 英生*; Sonnenschein, V.*; 齊藤 洸介*; 大橋 雅也*; 加藤 弘太郎*; 井口 哲夫*; 河合 利秀*; et al.

Analytical Sciences, 34(11), p.1265 - 1270, 2018/11

 被引用回数:3 パーセンタイル:57.52(Chemistry, Analytical)

Characterization of radionuclides in Fukushima is important to determine their origins and current state in the environment. Radionuclides exist as fine particles and are mixed with other constituents. A measurement method with both micro-imaging capability and highly selective element detection is necessary to analyze these particles. We developed such an imaging technique using a time-of-flight secondary ion mass spectrometry and wavelength tunable Ti:Sapphire lasers for resonance ionization of target elements without mass interference. This is called resonant laser ionization sputtered neutral mass spectrometry. The instrument has high lateral resolution and higher ionization selectivity using two-step resonance excitation of Cs with two lasers at different wavelengths. Optimization of the wavelength for resonance ionization using a Cs compound was performed, and a real environmental particle containing radioactive Cs was analyzed. Isotope images of three kinds of Cs were successfully obtained without interfere from Ba isotopes for the first time.


Analysis of two forms of radioactive particles emitted during the early stages of the Fukushima Dai-ichi Nuclear Power Station accident

佐藤 志彦; 末木 啓介*; 笹 公和*; 吉川 英樹; 中間 茂雄; 箕輪 はるか*; 阿部 善也*; 中井 泉*; 小野 貴大*; 足立 光司*; et al.

Geochemical Journal, 52(2), p.137 - 143, 2018/00

 被引用回数:19 パーセンタイル:1.73(Geochemistry & Geophysics)

Two types of radioactive particles have been isolated from environmental samples collected at various distances from the Fukushima Dai-ichi Nuclear Power Station. "Type A" particles are 2-10 $$mu$$m in diameter and display characteristic Cs X-ray emissions when analysed by energy-dispersive X-ray spectrometry (EDS). "Type B" particles are considerably larger, up to 400 $$mu$$m in diameter, with Cs concentrations too low to be detectable by EDS. These larger particles were isolated from the region to the north of the nuclear reactor site, which was contaminated on March 12, 2011. The specific activity of Type B particles is much lower than Type A, and the mean $$^{134}$$Cs$$/^{137}$$Cs ratios are $$sim$$0.93 and 1.04, respectively. The Type B ratio indicates power station Unit 1 as the source, implying that these larger radioactive particles were discharged on March 12. This study found that different type of radioactive particle was released not only on March 15 but also on March 12.



二宮 和彦*; 佐藤 志彦; 他53名*

KEK Proceedings 2017-6, p.31 - 34, 2017/11



Analysis of external surface irregularities on Fukushima-derived fallout particles

Martin, P. G.*; 佐藤 志彦; Griffiths, I.*; Richards, D.*; Scott, T.*

Frontiers in Energy Research (Internet), 5, p.25_1 - 25_9, 2017/09

 被引用回数:6 パーセンタイル:61.53(Energy & Fuels)

Three large high radioactivity particulate fragments, each several 100 $$mu$$m in diameter, have been recovered from the region immediately surrounding the Fukushima Daiichi Nuclear Power Plant. Through the application of high-resolution electron and ion-beam methods, this work has sought to investigate the structure and composition of this fibrous surface morphology. By evaluating this, a potential material source can be determined, alongside important information relating to the conditions/events at the time of the reactor explosions and catastrophic release of radioactive materials. The results of this study show that the fibrous features associated with these large radiocesium-containing particles share a common elemental composition. With respect to the surrounding particle, the fibers are enriched in Si, Cl, and Fe, while depleted in both Zn and Al. Based on composition, these fibers are ascribed to thermal insulating material used within the plant, which was sufficiently heated during the loss of coolant incident at the plant to be incorporated into the molten ejecta material that rapidly solidified upon quenching in air. Elemental analysis of these fibers does not reveal any evidence of leaching or the presence of actinide materials.



杉浦 広幸*; 酒井 創*; 佐藤 志彦; 末木 啓介*

Radioisotopes, 66(9), p.311 - 319, 2017/09




松中 哲也*; 笹 公和*; 高橋 努*; 細谷 青児*; 松村 万寿美*; 末木 啓介*; 佐藤 志彦

第19回AMSシンポジウム・2016年度「樹木年輪」研究会共同開催シンポジウム報告集, p.76 - 79, 2017/06

原子力施設の稼働に伴い放出する$$^{14}$$C放出量を松の木の年輪に含まれる$$^{14}$$Cを測定することで評価した。結果、(1)東海原子力施設周辺における1967-2010年単年輪内の$$^{14}$$C濃度は、北半球バックグラウンドに比べ2.6-70Bq kg$$^{-1}$$C高かった。(2)単年輪内の余剰$$^{14}$$C濃度は、2つの原子力発電所からの$$^{14}$$C放出量変動の影響を受けて、稼働開始時期と終了時期におよそ応答して増加傾向と減少傾向を示した。(3)再処理施設からの$$^{14}$$C放出量が比較的多かった3つの時期(1980年, 1985年, 1992年付近)に余剰$$^{14}$$C濃度の増大が認められた。(4)主として東海原子力施設に由来すると考えられる単年輪内余剰$$^{14}$$Cは、食物摂取による実効線量に換算すると最大で3.9$$mu$$Sv yr$$^{-1}$$程度であった。



小野 貴大*; 飯澤 勇信*; 阿部 善也*; 中井 泉*; 寺田 靖子*; 佐藤 志彦; 末木 啓介*; 足立 光司*; 五十嵐 康人*

分析化学, 66(4), p.251 - 261, 2017/04

 被引用回数:14 パーセンタイル:19.34(Chemistry, Analytical)



学位論文要録; 福島第一原発事故で生じた帰還困難区域における放射性物質の沈着と放射性粒子の関係の研究

佐藤 志彦

放射化学, (34), p.59 - 61, 2016/09




佐藤 志彦*; 末木 啓介*; 箕輪 はるか*; 中間 茂雄; 吉川 英樹

no journal, , 




佐藤 志彦*; 末木 啓介*; 笹 公和*; 箕輪 はるか*; 吉川 英樹; 藤原 健壮; 中間 茂雄; 足立 光司*; 五十嵐 康人*

no journal, , 




佐藤 志彦*; 末木 啓介*; 笹 公和*; 箕輪 はるか*; 吉川 英樹; 藤原 健壮; 中間 茂雄

no journal, , 


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