"Invisible" radioactive cesium atoms revealed; Pollucite inclusion in cesium-rich microparticles (CsMPs) from the Fukushima Daiichi Nuclear Power Plant

Miyazaki, Kanako*; Takehara, Masato*; Minomo, Kenta*; Horie, Kenji*; Takehara, Mami*; Yamasaki, Shinya*; Saito, Takumi*; Onuki, Toshihiko*; Takano, Masahide; Shiotsu, Hiroyuki; et al.

Journal of Hazardous Materials, 470(15), p.134104_1 - 134104_11, 2024/05

https://doi.org/10.1016/j.jhazmat.2024.134104

Chemical species of cesium and iodine in condensed vaporized microparticles formed by melting nuclear fuel components with concrete materials

Onuki, Toshihiko*; Ye, J.*; Kato, Tomoaki; Liu, J.; Takano, Masahide; Kozai, Naofumi; Utsunomiya, Satoshi*

Environmental Science; Processes & Impacts, 25(7), p.1204 - 1212, 2023/07

https://doi.org/10.1039/D3EM00074E

To elucidate chemical forms of Cs and I in microparticles produced via the Fukushima Daiichi Nuclear Power Plant accident and released into the atmosphere, we analyzed Cs and I in condensed vaporized particles (CVP) produced by melting experiments using nuclear fuel components containing CsI with concrete. CVPs consisted of many round particles containing Cs and I of diameters less than several tens of micrometers. Two kinds of particles were present: one containing large amounts of Cs and I, suggesting the presence of CsI, and the other containing small amounts of Cs and I with large Si contents. Most of CsI from both particles were dissolved in water. On the contrary, some fractions of Cs remained from the latter particles. These results suggest that Cs was incorporated in CVPs along with Si to form water low-soluble CVPs

Iodate respiration by sp. DN11 and its potential use for removal of radioiodine from contaminated aquifers

Sasamura, Seiya*; Onuki, Toshihiko*; Kozai, Naofumi; Amachi, Seigo*

Frontiers in Microbiology (Internet), 14, p.1162788_1 - 1162788_7, 2023/04

https://doi.org/10.3389/fmicb.2023.1162788

sp. DN11 previously isolated from gasoline-contaminated groundwater contained a gene cluster involved in bacterial iodate (IO) respiration. This study determined if strain DN11 performed iodate respiration and assessed its potential use to remove and sequester radioactive iodine (I) from subsurface contaminated aquifers. Strain DN11 grew anaerobically with iodate as the sole electron acceptor. After the growth of strain DN11 on iodate, silver-impregnated zeolite was added to the spent medium to remove iodide from the aqueous phase. In the presence of 200 M iodate as the electron acceptor, more than 98% of iodine was successfully removed from the aqueous phase. These results suggest that strain DN11 is potentially helpful for bioaugmentation of I-contaminated subsurface aquifers.

An Experimental study on the degradation of UO/Fe(0) by bacteria

Liu, J.; Dotsuta, Yuma; Kitagaki, Toru; Takano, Masahide; Onuki, Toshihiko; Kozai, Naofumi

Proceedings of International Topical Workshop on Fukushima Decommissioning Research (FDR2022) (Internet), 2 Pages, 2022/10

Nuclear fuel debris, consisting primarily of nuclear fuel and structural material, was formed during the Fukushima Daiichi NPP accident and exists in the cooling water accumulated in the primary containment vessels. Microorganisms living in groundwater may come into contact with the fuel debris and react with it. To assess the degradation of fuel debris, it is necessary to evaluate the interactions between microorganisms and fuel debris. Here we performed an experimental study on bacterial degradation. A mixed powder of UO and Fe(0) was used as a fuel debris simulant. Bacillus subtilis, which is widespread bacteria in nature and thought to be present at the accident site, was used. The mixed powder was exposed to the Bacillus subtilis in a liquid medium for some days. It was found that the oxidative dissolution of the U(IV) and Fe(0) was accelerated by B. subtilis. A fraction of the dissolved U(VI) was precipitated together with iron precipitates which are probably amorphous Fe(III) hydroxides. The study indicates that microorganisms would cause the degradation of fuel debris.

Chemical species of iodine during sorption by activated carbon; Effects of original chemical species and fulvic acids

Kato, Tomoaki; Kozai, Naofumi; Tanaka, Kazuya; Kaplan, D. I.*; Utsunomiya, Satoshi*; Onuki, Toshihiko

Journal of Nuclear Science and Technology, 59(5), p.580 - 589, 2022/05

https://doi.org/10.1080/00223131.2021.1993370

This study reports the effect of fulvic acids, which is a natural organic substance generally contained in groundwater, on the oxidation states of radioactive iodine anions (iodide and iodate). Iodide and iodate are contained in the contaminated water of the Fukushima Daiichi Nuclear Power Plant and supposed to be removed by activated carbon (AC) via adsorption. When fulvic acids does not exist in the experimental system, the adsorption of iodide on AC was less than that of iodate and their oxidation states after the adsorption were not changed. When fulvic acids existed, a fraction of the adsorbed iodate was reduced to iodide. This result indicates that the reduction of the adsorbed iodate progresses during the storage of the spent AC.

Sorption of Pu(IV) on biogenic Mn oxide and complexation of Pu(IV) with organic ligands secreted by fungal cells

Tanaka, Kazuya; Tani, Yukinori*; Kozai, Naofumi; Onuki, Toshihiko

Journal of Radioanalytical and Nuclear Chemistry, 331(2), p.1109 - 1114, 2022/02

https://doi.org/10.1007/s10967-021-08178-w

We investigated the sorption of Pu(IV) on biogenic Mn oxide produced by Mn(II)-oxidizing fungus. The sorption of Pu(IV) on biogenic Mn oxide was similar to that of U(VI) and different from that of Th(IV), possibly due to oxidation of Pu(IV) to Pu(VI). When Pu(IV) was sorbed on hyphae only, it was desorbed into the solution phase over time. Pu(IV) could be solubilized by complexation with organic ligands secreted by fungal cells. In particular, Pu(IV) desorption was observed under circumneutral pH conditions.

Sewage sludge ash contaminated with radiocesium; Solidification with alkaline-reacted metakaolinite (geopolymer) and Portland cement

Kozai, Naofumi; Sato, Junya; Osugi, Takeshi; Shimoyama, Iwao; Sekine, Yurina; Sakamoto, Fuminori; Onuki, Toshihiko

Journal of Hazardous Materials, 416, p.125965_1 - 125965_9, 2021/08

https://doi.org/10.1016/j.jhazmat.2021.125965

Spectroscopic and first-principles investigations of iodine species incorporation into ettringite; Implications for iodine migration in cement waste forms

Guo, B.*; Xiong, Y.*; Chen, W.*; Saslow, S. A.*; Kozai, Naofumi; Onuki, Toshihiko*; Dabo, I.*; Sasaki, Keiko*

Journal of Hazardous Materials, 389, p.121880_1 - 121880_11, 2020/05

https://doi.org/10.1016/j.jhazmat.2019.121880

Adsorption mechanism of ReO on Ni-Zn layered hydroxide salt and its application to removal of ReO as a surrogate of TcO

Tanaka, Kazuya; Kozai, Naofumi; Yamasaki, Shinya*; Onuki, Toshihiko; Kaplan, D. I.*; Grambow, B.

Applied Clay Science, 182, p.105282_1 - 105282_8, 2019/12

https://doi.org/10.1016/j.clay.2019.105282

In this study, Ni-Zn layered hydroxide salt (LHS) was used for adsorption experiments of ReO, as a surrogate of TcO, in aqueous solutions with various initial Re and sodium salt concentrations. The maximum adsorption amount of Re was estimated at 127.7 mg/g (6.86 10 eq/g) by fitting adsorption isotherm of ReO to Langmuir plot. The adsorption of ReO at neutral pH was a reversible process by anion exchange, and decreased with increasing Cl, NO and SO in solution. EXAFS analysis indicated that ReO was adsorbed as an outer-sphere complex on Ni-Zn LHS. The Ni-Zn LHS is a more robust adsorbent for ReO than the Mg-Al LDH in terms of solution pH and tolerance to competing anions, and may be an effective alternative to the traditional and more limited method of removing aqueous TcO by reductive precipitation.

investigation of radioactive Cs mobility around litter zone in contaminated forest using spent mushroom substrata

Onuki, Toshihiko*; Sakamoto, Fuminori; Kozai, Naofumi; Yamasaki, Shinya*; Sasaki, Yoshito; Niizato, Tadafumi

Journal of Nuclear Science and Technology, 56(9-10), p.814 - 821, 2019/09

https://doi.org/10.1080/00223131.2019.1588799

We used the spent mushroom substrata (SMSs) which are a kind of by-product after growing edible mushrooms for the investigation of radioactive Cs mobility in litter zone in a forest of Fukushima prefecture, Japan. The powder SMS was filled in a plastic net bag of 0.350.55 m, then was placed in a forest for 6 months under three kinds of different conditions without treatment (No treatment), covered with wooden box (With box), and with zeolite placed on upper position of ground surface (With zeolite). We determined the ratio of radioactivity (TF) in the SMS to that of the soil and litter beneath the SMS bags. TFs of "No treatment" and of "With zeolite" were determined between 0.01 and 0.05 for 6 months. On the other hand, TFs of "With box" were lower by one order at 2 and 4 months than those of "No treatment" and of "With zeolite", and nearly the same values as TFs of "No treatment" and "With zeolite" at 6 months. These results clearly indicate that radioactive Cs accumulates in SMS mainly by throughfall. In addition, for a period of several months, fungi contribute to the accumulation of radioactive Cs in the litter zone, even though radioactive Cs was tightly associated with the soil.