Microbially formed Mn(IV) oxide as a novel adsorbent for removal of Radium

Tanaka, Kazuya; Yamaji, Keiko*; Masuya, Hayato*; Tomita, Jumpei; Ozawa, Mayumi*; Yamasaki, Shinya*; Tokunaga, Kohei; Fukuyama, Kenjin*; Ohara, Yoshiyuki*; Maamoun, I.*; et al.

Chemosphere, 355, p.141837_1 - 141837_11, 2024/05

https://doi.org/10.1016/j.chemosphere.2024.141837

In this study, biogenic Mn(IV) oxide was applied to remove Ra from mine water collected from a U mill tailings pond in the Ningyo-toge center. Just 7.6 mg of biogenic Mn(IV) oxide removed more than 98% of the Ra from 3 L of mine water, corresponding to a distribution coefficient of 10 mL/g for Ra at pH 7. The obtained value was convincingly high for practical application of biogenic Mn(IV) oxide in water treatment.

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.

Improvement of the stability of IO-, SeO-, and SeO-coprecipitated barite after treatment with phosphate

Tokunaga, Kohei; Tanaka, Kazuya; Takahashi, Yoshio*; Kozai, Naofumi

Environmental Science & Technology, 57(8), p.3166 - 3175, 2023/02

https://doi.org/10.1021/acs.est.2c08939

Coprecipitation of radionuclides with barite has been studied to remove radionuclides from radioactive liquid waste because of its excellent removal efficiency; however, little information exists concerning the stability of the ions coprecipitated with barite. This study systematically investigated the stability of iodate, selenite, and selenate coprecipitated with barite via leaching tests. These oxyanions were gradually leached from the oxyanion-bearing barite into ultrapure water over time. Leaching of the oxyanions significantly increased in leaching solutions containing NaCl (pH5.3), NaNO (pH5.9), and NaSO (pH5.7). Conversely, leaching of the oxyanions was suppressed in KHPO solution (pH8.5), indicating that phosphate stabilized the oxyanion-bearing barite. The effect of phosphate treatment on oxyanion-bearing barite was further investigated. The results showed that the barite surface was modified with phosphate, and a thin surface layer of a barium phosphate-like structure was formed. The amount of oxyanions leached from the phosphate-treated samples into leaching solutions containing NaCl or NaNO was much lower than the amounts leached from the untreated barite samples into ultrapure water. The barite coprecipitation combined with subsequent phosphate treatment may be a promising method to efficiently remove iodate, selenite, and selenate from wastewater and stabilize them as barite coprecipitates.

Arsenic and iron speciation and binding in the surface soils in Ningyo-toge mill tailings pond using X-ray absorption fine spectroscopy

Tokunaga, Kohei; Takahashi, Yoshio*; Kozai, Naofumi

Journal of Nuclear and Radiochemical Sciences (Internet), 23, p.14 - 19, 2023/00

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.

Fe, Mn and U accumulations in naturally growing at the mill tailings pond; Iron plaque formation possibly related to root-endophytic bacteria producing siderophores

Nakamoto, Yukihiro*; Doyama, Kohei*; Haruma, Toshikatsu*; Lu, X.*; Tanaka, Kazuya; Kozai, Naofumi; Fukuyama, Kenjin; Fukushima, Shigeru; Ohara, Yoshiyuki; Yamaji, Keiko*

Minerals (Internet), 11(12), p.1337_1 - 1337_17, 2021/12

https://doi.org/10.3390/min11121337

Mine drainage is a vital water problem in the mining industry worldwide because of the heavy metal elements and low pH. Rhizofiltration using wetland plants is an appropriate method to remove heavy metals from the water via accumulation in the rhizosphere. is one of the candidate plants for this method because of metal accumulation, forming iron plaque around the roots. At the study site, which was the mill tailings pond in the Ningyo-toge uranium mine, has been naturally growing since 1998. The results showed that accumulated Fe, Mn, and U in the nodal roots without/with iron plaque compared with other plant tissues. Among the 837 bacterial colonies isolated from nodal roots, 88.6% showed siderophore production activities. Considering iron plaque formation around roots, we hypothesized that microbial siderophores might influence iron plaque formation because bacterial siderophores have catechol-like functional groups. The complex of catechol or other phenolics with Fe was precipitated due to the networks between Fe and phenolic derivatives. The experiment using bacterial products of root endophytes, such as spp. and spp., showed precipitation with Fe ions, and we confirmed that several spp. and spp. produced unidentified phenolic compounds. In conclusion, root-endophytic bacteria such as spp. and spp., isolated from metal-accumulating roots of , might influence iron plaque formation as the metal accumulation site. Iron plaque formation is related to tolerance in , and spp. and spp. might indirectly contribute to tolerance.

Effect of bacterial siderophore on cesium dissolution from biotite

Kimura, Tatsuki*; Fukutani, Satoshi*; Ikegami, Maiko*; Sakamoto, Fuminori; Kozai, Naofumi; Grambow, B.*; Yoneda, Minoru*

Chemosphere, 276, p.130121_1 - 130121_7, 2021/08

https://doi.org/10.1016/j.chemosphere.2021.130121

The adsorption of cesium (Cs) on biotite and dissolution of Cs from Cs-bearing biotite using a siderophore were investigated aiming to contribute to the elucidation of radiocesium migration mechanisms in the soil environment. Cs was adsorbed on a hardly weathered biotite powder sample. A siderophore was extracted and purified from the bacterial culture medium, and the purified siderophore was used in five consecutive dissolution experiments of the biotite samples. The major components of the biotite (Al, Fe, and Mg) were dissolved almost stoichiometrically, strongly suggesting that the siderophore selectively dissolves the broken edges of the biotite. The Cs adsorbed on the broken edges was dissolved rapidly as the siderophore dissolved the broken edges, and then, the Cs adsorbed on the outer planar surface of the biotite particles was slowly dissolved.

Carbonated nanohydroxyapatite from bone waste and its potential as a super adsorbent for removal of toxic ions

Sekine, Yurina; Nankawa, Takuya; Yamada, Teppei*; Matsumura, Daiju; Nemoto, Yoshihiro*; Takeguchi, Masaki*; Sugita, Tsuyoshi; Shimoyama, Iwao; Kozai, Naofumi; Morooka, Satoshi

Journal of Environmental Chemical Engineering, 9(2), p.105114_1 - 105114_12, 2021/04

https://doi.org/10.1016/j.jece.2021.105114

Remediating toxic ion contamination is crucial for protecting human health and the environment. This study aimed to provide a powerful strategy for effectively utilizing bone waste from the food production and preparation industries for removal of toxic ions. Here, we show that immersing pig bone in NaHCO solution produced a carbonated nanohydroxyapatites (C-NHAP). The C-NHAP exhibited high adsorptivity for Sr, Cd, Pb, and Cu. The strontium adsorptivity was about 250 and 4,500 times higher than that of normal bone and synthetic HAP, respectively. The C-NHAP is an eco-friendly, high-performance material that is simple to prepare and should be useful for tackling problems of food waste disposal and environmental pollution.