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宮崎 加奈子*; 笛田 和希*; 門脇 正尚; 寺田 宏明; 香西 直文; 岩田 孟; 堀江 憲路*; 竹原 真美*; 山崎 信哉*; Grambow, B.*; et al.
Journal of Hazardous Materials, 511, p.142180_1 - 142180_17, 2026/06
被引用回数：0 パーセンタイル：0.00(Engineering, Environmental)Radioactive cesium-rich microparticles (CsMPs) released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) in 2011 pose a persistent environmental concern, yet their initial atmospheric dispersion has remained poorly constrained. To elucidate their release dynamics, we quantified CsMPs in 100 surface soil samples collected across Fukushima Prefecture in July 2011. CsMP abundance and radioactive fraction (RF) ranged from 0 to 52,300 particles kg
; (dry weight) and 0-61.85% of deposited 
Cs, respectively. Integrating these results with WSPEEDI atmospheric simulations reveals a major formation event of CsMPs around 03:00 JST on 15th March 2011. The plume emitted at this time was heavily enriched in CsMPs, whereas plumes released after 00:00 JST on 16th March 2011 contained no detectable CsMPs, indicating that particle formation had ceased by then. The widespread distribution of CsMPs across Fukushima Prefecture is therefore attributed primarily to this single plume on 15th March 2011. Directional differences in CsMP abundance reflect temporal variations in CsMP density within the plume, with maximum estimated concentrations of 2,070 particles m
; toward the southwest and 4,700 particles m; toward the northwest. Additionally, elevated CsMP densities coupled with relatively low RF in the northwest suggest supplementary deposition of water-soluble cesium between 17:00 and 23:00 JST on 15 March. These findings constrain the timing and mechanisms of CsMP formation and dispersion, providing essential insights for environmental reconstruction and future radiological risk assessment.
宮崎 加奈子*; 武原 政人*; 蓑毛 健太*; 堀江 憲路*; 竹原 真美*; 山崎 信哉*; 斉藤 拓巳*; 大貫 敏彦*; 高野 公秀; 塩津 弘之; et al.
Journal of Hazardous Materials, 470(15), p.134104_1 - 134104_11, 2024/05
被引用回数：4 パーセンタイル：30.48(Engineering, Environmental)Radioactive Cs contamination has been one of the central issues in Fukushima and other legacy sites; however, atomic-scale characterization of radioactive Cs has never been successful. Here we report, for the first time, the direct imaging of radioactive Cs atoms using high-resolution high-angle annular dark-field scanning transmission electron microscopy. As inclusions in Cs-rich microparticles, 27-36 wt.% of Cs (as Cs
O) occurs in a type of zeolite called pollucite. The normalized formula for pollucite are expressed as (Cs,K,Ba)
(Fe
,Zn,X
)Si
O
, (Cs,K,Ba)
(Fe
Zn
X
)
Si
O, and (Cs,K,Ba)
(Fe
ZnX
)
Si
O after normalization with 12 oxygen atoms (X includes other trace cations; Ti, Mn, Rb, Zr, Mo, and Sn). Atomic-resolution image of radioactive Cs atoms are obtained when viewing along the [111] zone axis, a view supported by image simulations using the multi-slice method. The occurrence of pollucite indicates that locally enriched Cs reacted with siliceous substances during meltdowns, presumably through hydrothermal reactions. In case of predominant occurrence of pollucite in debris, incorporation in pollucite structure retards leaching of radioactive Cs. Still, the atomic-resolution imaging of radioactive Cs is an important advance for better understanding the fate of radioactive Cs inside and outside of damaged reactors during severe accidents like Fukushima Daiichi.
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
被引用回数：7 パーセンタイル：37.65(Environmental Sciences)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.
C control rods in Fukushima Daiichi nuclear reactors during meltdown; B-Li isotopic signatures in cesium-rich microparticles笛田 和希*; 高見 龍*; 蓑毛 健太*; 諸岡 和也*; 堀江 憲路*; 竹原 真美*; 山崎 信哉*; 斉藤 拓巳*; 塩津 弘之; 大貫 敏彦*; et al.
Journal of Hazardous Materials, 428, p.128214_1 - 128214_10, 2022/04
被引用回数：18 パーセンタイル：65.73(Engineering, Environmental)Boron carbide control rods remain in the fuel debris of the damaged reactors in the Fukushima Daiichi Nuclear Power Plant, potentially preventing re-criticality; however, the state and stability of the control rods remain unknown. Sensitive high-resolution ion microprobe analyses have revealed B-Li isotopic signatures in radioactive Cs-rich microparticles (CsMPs) that formed by volatilization and condensation of Si-oxides during the meltdowns. The CsMPs contain 1518-6733 mg kg of 
B and 11.99-1213 mg kg of Li. The 
B/
B (4.15-4.21) and 
Li/
Li (213-406) isotopic ratios are greater than natural abundances (
4.05 and 12.5, respectively), indicating that B(n,
)Li reactions occurred in BC prior to the meltdowns. The total amount of B released with CsMPs was estimated to be 0.024-62 g, suggesting that essentially all B remains in reactor Units 2 and/or 3 and is enough to prevent re-criticality; however, the heterogeneous distribution of B needs to be considered during decommissioning.
宮崎 加奈子*; 山崎 信哉*; 門脇 正尚; 寺田 宏明; Law, G. T. W.*; Bernd, G.*; 宇都宮 聡*
no journal, ,
本研究は、2011年の福島第一原子力発電所(1F)事故時に大気放出された放射性物質に含まれる不溶性セシウム粒子(CsMP)に着目し、事故初期におけるCsMPの分布や放射能寄与率の分析から事故由来のCsMPの広域分布を明らかにした。文部科学省が実施した大気試料データ(100地点)からCsMPの個数と放射能寄与率を分析し、WSPEEDIによる放射性Cs大気拡散シミュレーション結果を用いて各時刻における放射性Csプルームの到達場所について検討を行い、沈着量の情報と合わせてCsMPの大気中動態を解析した。CsMPの個数および放射能寄与率値はそれぞれ最大52,300個/kgおよび最大62%であり、1F南西方向で個数、放射能寄与率ともに他の地点よりも高くなった。CsMPの個数の空間パターンはセシウム放射能マップと類似しており、特に1F北西方向における放射能の増加に対して、個数とRF値はともに減少する傾向がみられた。また、3/15の10:00頃に1F南方向に分布したプルーム(0.049-0.27個/m
)と比較して、3/15の13:00頃に1F南南西方向に分布したプルームには高濃度のCsMP(0.67個/m)が含まれたことが示唆された。さらに、3/15の22:00頃に1F北西方向に分布したプルームにはCsMPが0.10個/mが含まれたと推定され、セシウムCs放射能マップが必ずしもCsMPの降下量やプルーム中のCsMP量と対応していないこと、およびプルーム中のCsMP量は時間変動が大きいことが示された。
