Occurrence of radioactive cesium-rich micro-particles (CsMPs) in a school building located 2.8 km south-west of the Fukushima Daiichi Nuclear Power Plant

笛田 和希*; 小宮 樹*; 蓑毛 健太*; 堀江 憲路*; 竹原 真美*; 山崎 信哉*; 塩津 弘之; 大貫 敏彦*; Grambow, B.*; Law, G. T. W.*; et al.

Chemosphere, 328, p.138566_1 - 138566_12, 2023/07

https://doi.org/10.1016/j.chemosphere.2023.138566

Fukushima Daiichi Nuclear Power Plant (FDNPP) derived radioactive Cs-rich microparticles (CsMPs) present a potential health risk through inhalation. Despite their occurrence in indoor environments impacted by the FDNPP accident, little is known about their prevalence. In this study, we quantitatively analyse the distribution and number of CsMPs in indoor dust samples collected from an elementary school located 2.8 km to the southwest of FDNPP. The school had remained untouched until 2016. Then, using a modified version of the autoradiography based "quantifying CsMPs (mQCP) method," we collected samples and determined the number of CsMPs and Cs radioactive fraction (RF) values of the microparticles (defined as total Cs activity from CsMPs / bulk Cs activity of entire sample). The numbers of CsMPs were determined to be 653 - 2570 particles/g and 296 - 1273 particles/g on the first and second floors of the school, respectively. The corresponding RFs ranged between 6.85 - 38.9 % and 4.48 - 6.61 %, respectively. The number of CsMPs and RF values in additional outdoor samples near the school building were and 23 - 63 particles/g and 1.14 - 1.61 %, respectively. The CsMPs were most abundant on the School's first floor near to the entrance, and the relative abundance was high near to the stairs on the second floor, indicating a likely CsMP dispersion path through the building. Additional wetting of the indoor samples combined with autoradiography revealed that indoor dusts had a distinct absence of intrinsic, soluble Cs species like CsOH. Combined, the results indicate that a significant amount of poorly soluble CsMPs were likely contained in initial radioactive airmass plumes from the FDNPP and that the microparticles could penetrate buildings. Clean-up plans for buildings / residential areas impacted by CsMP containing plumes, and monitoring of areas re-opened to the public, should take account of CsMPs in dusts.

The Formation mechanism of radiocesium-bearing microparticles derived from the Fukushima Daiichi Nuclear Power Plant using electron microscopy

萩原 大樹; 近藤 啓悦; 日高 昭秀

Journal of Radioanalytical and Nuclear Chemistry, 331(12), p.5905 - 5914, 2022/12

https://doi.org/10.1007/s10967-022-08434-7

Radiocesium-bearing microparticles (CsMPs) were released from the Fukushima Daiichi Nuclear Power Plant during the 2011 accident. We examined the CsMP formation process by analyzing Type-A particles and conducting in situ glass fiber experiments. The results demonstrated that heating glass fibers to 450C - 800C formed spherical particles, their morphologies and elemental compositions were similar to those of actual CsMPs. The mock-up particles size was strongly dependent on the glass-fiber thickness. Our findings reveal that glass fibers can form microparticles after being exposed to high temperatures.

Accumulation mechanisms of radiocaesium within lichen thallus tissues determined by means of microscale localisation observation

土肥 輝美; 飯島 和毅; 町田 昌彦; 数納 広哉*; 大村 嘉人*; 藤原 健壮; 木村 茂*; 菅野 太志*

PLOS ONE (Internet), 17(7), p.e0271035_1 - e0271035_21, 2022/07

https://doi.org/10.1371/journal.pone.0271035

Many lichens are well known to accumulate radiocaesium and, thus acting as biomonitors of contamination levels. Here, we use autoradiography and demonstrate for the first time microscale localisation of radiocaesium within thallus tissues to investigate the radiocaesium forms and their accumulation mechanism. The radiocaesium was localised in the brown pigmented parts i.e., melanin-like substances, in the lower cortex of lichen thallus. Quantum chemical calculations showed that functional group of melanin-like substances can chelate Cs ion, which indicates that the Cs ions form complexes with the substances. Based on these findings, we suggest that radiocaesium ions may be retained stably in melanin-like substances for long periods (two to six years) due to steric factors, such as those seen in porphyrin-like structures and multimer formation in the lower cortex.

Characterization of radiocesium-bearing microparticles with different morphologies in soil around the Fukushima Daiichi Nuclear Power Plant

萩原 大樹; 舟木 泰智; 尻引 夏*; 菅野 麻里奈*; 眞田 幸尚

Journal of Radioanalytical and Nuclear Chemistry, 331(1), p.415 - 426, 2022/01

https://doi.org/10.1007/s10967-021-08061-8

Radiocesium-bearing microparticles (CsMPs) from Fukushima Daiichi Nuclear Power Plant (FDNPP) are observed in Eastern Japan. To examine their source and formation, multiple particles were isolated from soils from three sites around the FDNPP and their radioactivity, morphology, and elemental composition were analyzed. Cesium-137 radioactivity ranged from 0.23 to 8.57 Bq and particles were primarily composed of Si, Fe, Zn, C, and Cs at each site. Uranium-rich parts in certain CsMPs show their origin in the vicinity of the nuclear reactor. Our results will help characterize CsMPs and evaluate the internal dose exposure of personnel employed at the FDNPP

Microparticles with diverse sizes and morphologies from mechanical and laser cutting of fuel debris simulants and geopolymer as a covering material

Zhou, Q.*; 斉藤 拓巳*; 鈴木 誠矢; 矢野 公彦; 鈴木 俊一*

Journal of Nuclear Science and Technology, 58(4), p.461 - 472, 2021/04

https://doi.org/10.1080/00223131.2020.1869623

During the decommissioning of Fukushima Daiichi Nuclear Power Plant, the dismantling of massive fuel debris is important for the defueling process. The production and dispersion of radioactive microparticles highly depends on the cutting technique implemented. Previous studies have been conducted on the development of cutting techniques and the treatment of radioactive particles generation during the cutting process. Besides, adequate understanding of the microparticle products during the cuttings of fuel debris is of vital necessity. Nowadays, geopolymer application is proposed as a covering material during the fuel debris retrieval in order to keep the structural integrity of damaged components. In this study, the microparticle products during mechanical and laser cutting of fuel debris simulants (Hafnium oxide and Tungsten(IV) oxide pellets) and geopolymer material were investigated. The cuttings have been carried out for samples of the simulants, geopolymer, and simulants with geopolymer covering. The generated particles were collected and investigated by laser diffraction particle size analyzer and Scanning Electron Microscope with X-ray spectrometry. Particles with diverse sizes and morphologies were observed from the products of each sample. It also appears that particles with unique sizes and morphologies can generate from the laser cuttings due to the thermal effect of laser cutting.

レーザー加工により発生する微粒子の解析と核種同定手法の開発(委託研究); 令和元年度英知を結集した原子力科学技術・人材育成推進事業

廃炉環境国際共同研究センター; 東京大学*

JAEA-Review 2020-031, 69 Pages, 2021/01

JAEA-Review-2020-031.pdf:4.22MB

日本原子力研究開発機構(JAEA)廃炉環境国際共同研究センター(CLADS)では、令和元年度英知を結集した原子力科学技術・人材育成推進事業(以下、「本事業」という)を実施している。本事業は、東京電力ホールディングス福島第一原子力発電所の廃炉等をはじめとした原子力分野の課題解決に貢献するため、国内外の英知を結集し、様々な分野の知見や経験を、従前の機関や分野の壁を越えて緊密に融合・連携させた基礎的・基盤的研究及び人材育成を推進することを目的としている。平成30年度の新規採択課題から実施主体を文部科学省からJAEAに移行することで、JAEAとアカデミアとの連携を強化し、廃炉に資する中長期的な研究開発・人材育成をより安定的かつ継続的に実施する体制を構築した。本研究は、研究課題のうち、平成30年度に採択された「レーザー加工により発生する微粒子の解析と核種同定手法の開発」の令和元年度の研究成果について取りまとめたものである。レーザー加工は様々な長所を有するが、利用に際して多量の微粒子が発生することが知られており、放射性物質で汚染されている廃炉廃棄物に対する適用が躊躇されているが、その発生メカニズムは不明な点が多い。そこで、本研究は、その微粒子発生を基礎に立ち戻って検討するとともに、エアロダイナミックレンズを用いて微粒子を捕集することで粒径分布を測定し、さらに微粒子を構成する核種をレーザーによりオンラインで計測するための原理装置を開発する。

Numerical simulation of microparticles motion in two-phase bubbly flow

吉田 啓之; 上澤 伸一郎

Proceedings of 2020 International Conference on Nuclear Engineering (ICONE 2020) (Internet), 7 Pages, 2020/08

https://doi.org/10.1115/ICONE2020-16393

The radioactive aerosol removal equipment is used as one of the safety systems of nuclear reactors. In this equipment, microparticles of aerosol are removed through gas-liquid interfaces of two-phase flow. The mechanism related to the removal of microparticles through the gas-liquid interface is not precise; a numerical evaluation method of performance of aerosol removal equipment is not realized. Then, we have started to construct a numerical simulation method to simulate the removal of microparticles through gas-liquid interfaces. In this simulation method, a detailed two-phase flow simulation code TPFIT is used as the basis of this method. TPFIT adopts an advanced interface tracking method and can simulate interface movement and deformation directly. Also, to simulate the movement of particles, the Lagrangian particle tracking method is incorporated. By combining the interface tracking method, and the Lagrangian particle tracking method, the interaction between interfaces and microparticles can be simulated in detail. To solve the Lagrangian equations of particles, fluid properties and fluid velocity surrounding aerosol particles are evaluated by considering the relative position of particles and gas-liquid interface, to simulate particle movement near the interface. In this paper, we show an outline and preliminary results of this simulation method.

レーザー加工により発生する微粒子の解析と核種同定手法の開発(委託研究); 平成30年度英知を結集した原子力科学技術・人材育成推進事業

廃炉国際共同研究センター; 東京大学*

JAEA-Review 2019-034, 59 Pages, 2020/03

JAEA-Review-2019-034.pdf:3.15MB

日本原子力研究開発機構(JAEA)廃炉国際共同研究センター(CLADS)では、平成30年度英知を結集した原子力科学技術・人材育成推進事業(以下、「本事業」という)を実施している。本事業は、東京電力ホールディングス福島第一原子力発電所の廃炉等をはじめとした原子力分野の課題解決に貢献するため、国内外の英知を結集し、様々な分野の知見や経験を、従前の機関や分野の壁を越えて緊密に融合・連携させた基礎的・基盤的研究及び人材育成を推進することを目的としている。平成30年度の新規採択課題から実施主体を文部科学省からJAEAに移行することで、JAEAとアカデミアとの連携を強化し、廃炉に資する中長期的な研究開発・人材育成をより安定的かつ継続的に実施する体制を構築した。本研究は、研究課題のうち、平成30年度「レーザー加工により発生する微粒子の解析と核種同定手法の開発」について取りまとめたものである。レーザー加工は様々な長所を有するが、利用に際して多量の微粒子が発生することが知られており、放射性物質で汚染されている廃炉廃棄物に対する適用が躊躇されているが、その発生メカニズムは不明な点が多い。そこで、本研究は、その微粒子発生を基礎に立ち戻って検討するとともに、エアロダイナミックレンズを用いて微粒子を捕集することで粒径分布を測定し、さらに微粒子を構成する核種をレーザーによりオンラインで計測するための原理装置を開発する。

Extraction mechanism of lanthanide ions into silica-based microparticles studied by single microparticle manipulation and microspectroscopy

大高 稔紀*; 佐藤 辰巳*; 大野 真平; 名越 航平; 安倍 諒治*; 新井 剛*; 渡部 創; 佐野 雄一; 竹内 正行; 中谷 清治*

Analytical Sciences, 35(10), p.1129 - 1133, 2019/10

https://doi.org/10.2116/analsci.19P155

Single porous silica microparticles coated with styrene-divinylbenzene polymer (SDB) impregnated with octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) were injected into an aqueous 3 mol/L nitric acid solution containing trivalent lanthanide (Ln(III)), as a high-level liquid waste model, using the microcapillary manipulation-injection technique; and the extraction rate of Ln(III), as an Ln(III)-CMPO complex, into the single microparticles was measured by luminescence microspectroscopy. The extraction rate significantly depended on the Ln(III), CMPO, or NO concentration, and was analyzed in terms of diffusion in the pores of the microparticles and complex formation of Ln(III). The results indicated that the rate-determining step in Ln(III) extraction was the diffusion in the pore solution of the microparticles.

環境試料中からの放射性セシウム微粒子の単離; リターへの適用事例

田籠 久也; 土肥 輝美; 石井 康雄; 金井塚 清一*; 藤原 健壮; 飯島 和毅

JAEA-Technology 2019-001, 37 Pages, 2019/03

JAEA-Technology-2019-001.pdf:26.85MB

東京電力ホールディングス福島第一原子力発電所事故由来の放射性セシウム微粒子(CsMP)の空間的分布の把握や、その物理化学特性を統計的に評価するには、環境試料等からの効率的なCsMPの単離が必要となる。本報では、森林生態系のCs循環に影響する可能性のあるリターに着目し、リターからの効率的なCsMPの単離法を開発した。過酸化水素水による有機物分解処理と、電子顕微鏡学的手法を組み合わせることによって、多くの土壌鉱物粒子を含むリター中からCsMPを短時間(1粒子あたり3日)で単離することができた。この単離法は、林床のリターのみならず、生木の樹皮や葉などの植物試料をはじめ、その他の有機物試料への適用も期待される。