Investigation of sorption behavior of Cs in a river-sea system boundary area after the Fukushima Dai-ichi Nuclear Power Plant accident

高田 兵衛*; 脇山 義史*; 和田 敏裕*; 平尾 茂一*; 青野 辰雄*; 中西 貴宏; 御園生 敏治; 尻引 武彦; 青山 道夫*

Marine Chemistry, 262, p.104384_1 - 104384_6, 2024/05

https://doi.org/10.1016/j.marchem.2024.104384

The radiocesium (Cs) distribution between dissolved and particulate phases was examined in river water and coastal seawater as a function of the Cs sorption behavior on suspended particles. Dissolved Cs activity concentrations in the Tomioka River (salinity 0.1) and in coastal seawater at Tomioka fishery port (salinity 30), Fukushima Prefecture, from June 2019 to October 2021 were 3.6-20 Bq/m (geometric mean 11 Bq/m) and 2.4-86 Bq/m (13 Bq/m), respectively. Although the suspended particle concentration was lower in the river (0.2-44 mg/L; geometric mean 2 mg/L) than in seawater (0.8-24 mg/L; 6.4 mg/L), the mean Cs activity on suspended particles was 11,000 Bq/kg-dry in the river versus 3,200 Bq/kg-dry in seawater. Proportions of ion-exchangeable, organically bound, and refractory fractions of Cs on suspended particles were determined by sequential extraction. The ion-exchangeable fraction accounted for 0.3-2.0% (mean 1.2%) and 0.4-1.3% (0.8%) at the river and port sites, respectively. The organically bound fraction accounted for 0.3-4.8% (1.8%) and 0.1-5.5% (2.1%) at the river and port sites, respectively. In both areas, the refractory fraction accounted for 90% of Cs. Unexpectedly, the ion-exchangeable fraction did not differ between the river and port sites, and the percentage at the river site did not vary during the sampling period. Therefore, the ion-exchangeable fraction in the river's lower reach was originally low or had decreased before the particles arrived there. The small labile Cs fraction on suspended particles indicates that the mobility of radiocesium to marine biota in this coastal region is low.

Proton diffusion in liquid 1,2,3-triazole studied by incoherent quasi-elastic neutron scattering

篠原 佑也*; 岩下 拓哉*; 中西 真大*; Osti, N. C.*; 古府 麻衣子; 楡井 真実; Dmowski, W.*; 江上 毅*

Journal of Physical Chemistry B, 128(6), p.1544 - 1549, 2024/02

https://doi.org/10.1021/acs.jpcb.3c07685

Improving the proton transport in polymer electrolytes impacts the performance of next-generation solid-state batteries. However, little is known about proton conductivity in nonaqueous systems due to the lack of an appropriate level of fundamental understanding. Here, we studied the proton transport in small molecules with dynamic hydrogen bonding, 1,2,3-triazole, as a model system of proton hopping in a nonaqueous environment using incoherent quasi-elastic neutron scattering. By using the jump-diffusion model, we identified the elementary jump-diffusion motion of protons at a much shorter length scale than those by nuclear magnetic resonance and impedance spectroscopy for the estimated long-range diffusion. In addition, a spatially restricted diffusive motion was observed, indicating that proton motion in 1,2,3-triazole is complex with various local correlated dynamics. These correlated dynamics will be important in elucidating the nature of the proton dynamics in nonaqueous systems.

Development of a radiation tolerant laser-induced breakdown spectroscopy system using a single crystal micro-chip laser for remote elemental analysis

田村 浩司; 中西 隆造; 大場 弘則; 狩野 貴宏; 柴田 卓弥; 平等 拓範*; 若井田 育夫

Journal of Nuclear Science and Technology, 8 Pages, 2024/00

https://doi.org/10.1080/00223131.2023.2298485

For the development of the remote elemental analysis method in a radiation environment based on the laser-induced breakdown spectroscopy (LIBS), the radiation effects on the laser oscillation properties of the single crystal (SC) Nd: YAG microchip laser (MCL) were investigated and compared with those of ceramics Nd: YAG MCL. The laser oscillation properties were measured under gamma-ray irradiation as a function of dose rate. The effects on the SC MCL properties were found to be very small compared to those on the ceramics, indicating minimal radiation effects on the LIBS signal when using SC MCL. Pulse energy and oscillating build-up time (BUT) were measured for a cumulative dose exceeding 1400 kGy. The pulse energy remained stable, and the laser continued to oscillate under irradiation. The BUT also remained stable, demonstrating negligible optical loss accumulation that could affect laser properties even at the demonstrated cumulative dose. The results indicate that the effects of dose rate and cumulative dose on SC MCL laser properties were minimal. The SC MCL was then integrated into the LIBS system, and the gadolinium signal of composite oxides, simulating fuel debris, was successfully measured at the dose rate of 5 kGy/hr. These findings highlight the radiation tolerance of SC MCL as a laser medium for remote LIBS applications in harsh radiation environments.

Development of an iron(II) complex exhibiting thermal- and photoinduced double proton-transfer-coupled spin transition in a short hydrogen bond

中西 匠*; 堀 優太*; 重田 育照*; 佐藤 寛泰*; 鬼柳 亮嗣; 宗像 孝司*; 大原 高志; 岡澤 厚*; 島田 林太郎*; 坂本 章*; et al.

Journal of the American Chemical Society, 145(35), p.19177 - 19181, 2023/08

https://doi.org/10.1021/jacs.3c06323

Multiple proton transfer (PT) controllable by external stimuli plays a crucial role in fundamental chemistry, biological activity, and material science. However, in crystalline systems, controlling multiple PT, which results in a distinct protonation state, remains challenging. In this study, we developed a novel tridentate ligand and iron(II) complex with a short hydrogen bond (HB) that exhibits a PT-coupled spin transition (PCST). Single-crystal X-ray and neutron diffraction measurements revealed that the positions of the two protons in the complex can be controlled by temperature and photoirradiation based on the thermal- and photoinduced PCST. The obtained results suggest that designing molecules that form short HBs is a promising approach for developing multiple PT systems in crystals.

Factors regulating the concentration of particulate iodine in coastal seawater

佐藤 雄飛*; 乙坂 重嘉*; 鈴木 崇史; 中西 貴宏

Limnology and Oceanography, 68(7), p.1580 - 1594, 2023/07

https://doi.org/10.1002/lno.12369

海水中の懸濁態ヨウ素(PI)濃度の規定要因を明らかにするため、太平洋沿岸の2つの海域で、PI、懸濁態有機炭素(POC)・窒素、溶存態ヨウ素、植物プランクトン色素を測定した。PI/POC比から、データセットは3グループ(A: 低い、B: 中間、C: 高い)に分類された。各グループは、植物プランクトンの生理状態として、それぞれ対数増殖期、静止期、衰退期に特徴付けられた。PI生産と植物プランクトンの生理状態との関係に基づき、季節的・地域的差異が一貫して説明できた。これらの結果から、植物プランクトンの生理状態が海水中のPI濃度を調節する重要な因子であることが示唆された。

Thirty-year simulation of environmental fate of Cs in the Abukuma River basin considering the characteristics of Cs behavior in land uses

池之上 翼; 嶋寺 光*; 中西 貴宏; 近藤 明*

Science of the Total Environment, 876, p.162846_1 - 162846_12, 2023/06

https://doi.org/10.1016/j.scitotenv.2023.162846

土地利用のCsの挙動特性を考慮し、阿武隈川流域におけるCsの30年間の環境動態シミュレーションを実施した。30年間で海洋へ輸送されたCsは阿武隈川流域の初期沈着量の4.6%に相当し、阿武隈川流域に沈着したCsの実効半減期はCsの半減期より3.7年(11.6%)短くなると推定された。これらの結果は事故によって沈着したCsが数十年残留し続ける可能性があることを示唆するものであった。土地利用におけるCsの挙動を分析した結果、2011年における市街地による海洋へのCsの輸送の寄与は、総輸送量の70%に相当すると推定された。一方で、2012年から2040年における農地による輸送の寄与は総輸送量の75%に相当すると推定された。事故後30年間、人間活動のある地域とない地域に残留するCsの放射性崩壊を除いた削減率は、それぞれ11.5%から17.7%、0.4%から1.4 %と推定された。これらの結果は、過去から将来にかけて人間活動が土地に残留するCsの減少を促進することを示唆するものであった。

Effect of radioactive cesium-rich microparticles on radioactive cesium concentration and distribution coefficient in rivers flowing through the watersheds with different contaminated condition in Fukushima

辰野 宇大*; 脇 嘉理*; 角間 海七渡*; 二瓶 直登*; 高瀬 つぎ子*; 和田 敏裕*; 吉村 和也; 中西 貴宏; 大手 信人*

Journal of Environmental Management, 329, p.116983_1 - 116983_13, 2023/03

https://doi.org/10.1016/j.jenvman.2022.116983

This study investigated the effect of radioactive cesium-rich microparticles (CsMPs) on the radiocesium (RCs) concentration and distribution coefficient (Kd) in two rivers, Takase River and Kami-Oguni River, flowing in the watersheds with different radioactive contaminated conditions in Fukushima Prefecture. Unlike RCs adsorbed on to the suspended solids (SS), there was no correlation between the RCs concentration derived from CsMPs and the SS concentration in both rivers. Inflow of CsMPs to the targeted rivers was contingent. CsMPs were detected only in some samples during rainfall. Furthermore, the proportion of RCs concentration derived from CsMPs in the average RCs concentrations per unit mass of SS in both rivers during rainfall were not large, which were 10% or less. As a results, CsMPs did not significantly increase particulate RCs concentration and had little effect on Kd in both river water flowing the watershed with different RCs contaminated condition.

令和3年度福島県近沿岸海域等における放射性物質等の状況調査

御園生 敏治; 中西 貴宏; 眞田 幸尚; 尻引 武彦; 卜部 嘉*; 鶴田 忠彦

JAEA-Research 2022-010, 134 Pages, 2023/02

JAEA-Research-2022-010.pdf:8.45MB

東京電力ホールディングス(株)福島第一原子力発電所(1F)の事故が発生し、多量の放射性物質が1F周辺に沈着した。日本原子力研究開発機構では、事故後、放射性物質の動態研究を継続して実施している。本報告書は、令和3年度における、近沿岸海域等における放射性物質の状況調査を実施した成果をまとめたものである。具体的には、福島沿岸域57地点において柱状試料を採取し、海底土への放射性セシウムの蓄積状況を示した。さらに海底地形・海底土分布調査を実施し、地形と堆積物の分布状況を把握した。また、河川前面における海底土表層の放射性セシウム濃度の水平分布を計測した。放射性物質の水産物への影響の基礎情報として、魚類の分布状況を調査した。さらに、無人観測船を使用した採水及び採泥の実証試験を実施した。得られた結果より1F前面海域における海底土に含まれる放射性物質の分布と動態について推定を行った。

A New approach to extracting biofilm from environmental plastics using ultrasound-assisted syringe treatment for isotopic analyses

Battulga, B.; 安藤 麻里子; 中西 貴宏; 小嵐 淳

Science of the Total Environment, 849, p.157758_1 - 157758_11, 2022/11

https://doi.org/10.1016/j.scitotenv.2022.157758

本研究では、マイクロプラスチックの表面に形成されるバイオフィルム(有機付着物)の特性を明らかにするための第一ステップとして、バイオフィルムを分離回収する手法を開発した。茨城県内の河川において、大きさ,色,組成の異なる様々なマイクロプラスチック試料を採取した。それらの試料に超音波処理を行った後、シリンジを用いた方法により有機付着物を溶液として分離回収した。バイオフィルム由来の有機物から放射性セシウムが検出され、マイクロプラスチックが河川生態系における放射性核種の輸送媒体としての役割を果たすことが示唆された。また、有機物の安定炭素・窒素同位体の分析にも成功した。本手法は、マイクロプラスチックの状態や環境中における物質循環への寄与を解明するために有効である。

Water-assisted microphase separation of cationic random copolymers into sub-5 nm lamellar materials and thin films

今井 彩帆里*; 荒川 勝利*; 中西 洋平*; 竹中 幹人*; 青木 裕之; 大内 誠*; 寺島 崇矢*

Macromolecules, 55(20), p.9113 - 9125, 2022/10

https://doi.org/10.1021/acs.macromol.2c01287

Microphase separation of copolymers is a key technique to produce polymer bulk materials or thin films with ordered nanostructures for applications in various research fields including nanotechnologies, electronic devices, among many others. Herein, we report water-assisted microphase separation of amphiphilic random copolymers bearing quaternary ammonium cations and hydrophobic alkyl or oleyl groups in the solid state and the thin films. We investigated the effects of sample preparation protocols and the hydrophobic pendants (a butyl group: C4 - octadecyl or oleyl group: C18), composition, and molecular weight of the copolymers on the microphase separation behavior. By annealing under humid conditions, the copolymers bearing alkyl groups longer than an octyl group (C8) formed sub-5 nm lamellar structures comprising cationic layers and hydrophobic layers. Water hardly remained in the resulting lamellar materials under ambient conditions. The domain spacing was controlled between 3.7 and 5.3 nm by tuning the length of the hydrophobic pendants and composition and was independent of the molecular weight and molecular weight distribution. The cationic random copolymers carrying amorphous hydrophobic pendants provided transparent or translucent polymer materials containing small lamellar structures. The random copolymers further formed multilayered lamellar thin films on silicon substrates by spin-coating the copolymer solutions, followed by a humid annealing process. The layered lamellae were directly observed as terrace structures with about 4-5 nm steps by atomic force microscopy.