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Journal Articles

$$gamma$$-radiation and H$$_{2}$$O$$_{2}$$ induced oxidative dissolution of uranium(IV) oxide in aqueous solution containing phthalic acid

Kumagai, Yuta; Jonsson, M.*

Dalton Transactions (Internet), 49(6), p.1907 - 1914, 2020/02

 Times Cited Count:0 Percentile:100(Chemistry, Inorganic & Nuclear)

This study aims to reveal possible involvements of organic acids in the oxidative dissolution of UO$$_{2}$$. Using phthalic acid as a model compound, we have measured adsorption on UO$$_{2}$$ and investigated effects on the reaction between H$$_{2}$$O$$_{2}$$ and UO$$_{2}$$ and on oxidative dissolution induced by $$gamma$$-irradiation. Significant adsorption of phthalic acid was observed even at neutral pH. However, the reaction between H$$_{2}$$O$$_{2}$$ and UO$$_{2}$$ in phthalic acid solution induced oxidative dissolution of U(VI) similarly to aqueous bicarbonate solution. These results indicate that even though phthalic acid adsorbs on the UO$$_{2}$$ surface, it is not involved in the interfacial reaction by H$$_{2}$$O$$_{2}$$. In contrast, the dissolution of U by irradiation was inhibited in aqueous phthalic acid solution, whereas H$$_{2}$$O$$_{2}$$ generated by radiolysis was consumed by UO$$_{2}$$. The inhibition suggests that radical species derived from phthalic acid was involved in the redox reaction process of UO$$_{2}$$.

Journal Articles

A Simulation of radiolysis of chloride solutions containing ferrous ion

Hata, Kuniki; Inoue, Hiroyuki*

Journal of Nuclear Science and Technology, 56(9-10), p.842 - 850, 2019/09

 Times Cited Count:0 Percentile:100(Nuclear Science & Technology)

To investigate the effect of dissolved species from steels on the radiolysis processes of Cl$$^{-}$$, radiolysis simulations of solutions containing both Cl$$^{-}$$ and Fe$$^{2+}$$ were carried out. The results showed that the generation of radiolytic products (H$$_{2}$$O$$_{2}$$, O$$_{2}$$ and H$$_{2}$$) increased mainly by the addition of Fe$$^{2+}$$, and a drop in the pH was caused by the hydrolysis of Fe$$^{3+}$$. This pH drop enhanced the reactivity of Cl$$^{-}$$ with $$^{.}$$OH, which induced additional generation of H$$_{2}$$O$$_{2}$$ and O$$_{2}$$. These results show that low concentrations of Cl$$^{-}$$ (1 $$times$$ 10$$^{-3}$$ mol/dm$$^{3}$$ = 35ppm) in the presence of Fe$$^{2+}$$ could influence the generation of H$$_{2}$$O$$_{2}$$ and O$$_{2}$$ during water radiolysis. However, it is considered that these effects of Fe$$^{2+}$$ and low concentration of Cl$$^{-}$$ on water radiolysis are less important for corrosion of steels due to the low concentrations of H$$_{2}$$O$$_{2}$$ and O$$_{2}$$ generated. The other process, such as dissolution of iron enhanced by FeOOH, might predominantly induce corrosion under the conditions of solutions with low concentrations of H$$_{2}$$O$$_{2}$$ and O$$_{2}$$.

Journal Articles

Impact of stoichiometry on the mechanism and kinetics of oxidative dissolution of UO$$_{2}$$ induced by H$$_{2}$$O$$_{2}$$ and $$gamma$$-irradiation

Kumagai, Yuta; Fidalgo, A. B.*; Jonsson, M.*

Journal of Physical Chemistry C, 123(15), p.9919 - 9925, 2019/04

 Times Cited Count:3 Percentile:41.35(Chemistry, Physical)

Radiation-induced oxidative dissolution of uranium dioxide (UO$$_{2}$$) is one of the most important chemical processes of U driven by redox reactions. We have examined the effect of UO$$_{2}$$ stoichiometry on the oxidative dissolution of UO$$_{2}$$ induced by hydrogen peroxide (H$$_{2}$$O$$_{2}$$) and $$gamma$$-ray irradiation. By comparing the reaction kinetics of H$$_{2}$$O$$_{2}$$ between stoichiometric UO$$_{2.0}$$ and hyper-stoichiometric UO$$_{2.3}$$, we observed a significant difference in reaction speed and U dissolution kinetics. The stoichiometric UO$$_{2.0}$$ reacted with H$$_{2}$$O$$_{2}$$ much faster than the hyper-stoichiometric UO$$_{2.3}$$. The U dissolution from UO$$_{2.0}$$ was initially much lower than that from UO$$_{2.3}$$, but gradually increased as the oxidation by H$$_{2}$$O$$_{2}$$ proceeded. The $$gamma$$-ray irradiation induced the U dissolution that is analogous to the kinetics by the exposure to a low concentration (0.2 mM) of H$$_{2}$$O$$_{2}$$. The exposure to higher H$$_{2}$$O$$_{2}$$ concentrations caused lower U dissolution and resulted in deviation from the U dissolution behavior by $$gamma$$-ray irradiation.

Journal Articles

Reaction between spin-correlated triplet positronium and OH radical in water

Hirade, Tetsuya

JPS Conference Proceedings (Internet), 25, p.011022_1 - 011022_3, 2019/03

OH radicals which are very reactive are formed by radiation decomposition in water. The behavior of OH radicals is important in corrosion of materials and reactions in living bodies. Recently, the reaction occurring between positronium (Ps) formed by OH radicals formed at the end of the positron track when positron is incident and positronium (Ps) formed by reaction of excess electrons formed with OH radical formation with the thermo-positron, it is reported that quantum beat occurs due to spin correlation. This quantum beat seems to have a period depending on the hyperfine coupling constant of OH radical. It is thought that the period and intensity of the quantum beat depends on the temperature, and it seems that it reflects the state around the OH radical. From the temperature dependence of the quantum beat detected by the reaction of this spin-correlated OH radical and triplet positronium we will explain what the liquid structure might be.

Journal Articles

The Role of surface-bound hydroxyl radicals in the reaction between H$$_{2}$$O$$_{2}$$ and UO$$_{2}$$

Fidalgo, A. B.*; Kumagai, Yuta; Jonsson, M.*

Journal of Coordination Chemistry, 71(11-13), p.1799 - 1807, 2018/07

 Times Cited Count:10 Percentile:18.4(Chemistry, Inorganic & Nuclear)

In this work, we have studied the reaction between H$$_{2}$$O$$_{2}$$ and UO$$_{2}$$ with particular focus on the nature of the hydroxyl radical formed as an intermediate. Experiments were performed to study the kinetics of the reaction at different initial H$$_{2}$$O$$_{2}$$ concentrations. The results show that the consumption rates at a given H$$_{2}$$O$$_{2}$$ concentration are different depending on the initial H$$_{2}$$O$$_{2}$$ concentration. This is attributed to an alteration of the reactive interface, likely caused by blocking of surface sites by oxidized U/surface-bound hydroxyl radicals. The U dissolution yield decreases with increasing initial H$$_{2}$$O$$_{2}$$ concentration. This is expected from the mechanism of catalytic decomposition of H$$_{2}$$O$$_{2}$$ on oxide surfaces. As the experiments were performed in solutions containing 10 mM and a strong concentration dependence was observed in the 0.2 - 2.0 mM H$$_{2}$$O$$_{2}$$ concentration range, we conclude that the intermediate hydroxyl radical is surface bound rather than free.

Journal Articles

Investigation of hydrogen gas generation by radiolysis for cement-solidified products of used adsorbents for water decontamination

Sato, Junya; Kikuchi, Hiroshi*; Kato, Jun; Sakakibara, Tetsuro; Matsushima, Ryotatsu; Sato, Fuminori; Kojima, Junji; Nakazawa, Osamu

QST-M-8; QST Takasaki Annual Report 2016, P. 62, 2018/03

no abstracts in English

Journal Articles

Modern radiation chemistry (Applications), 16; Computer simulation study of initial process of radiation biological effect

Watanabe, Ritsuko*; Kai, Takeshi; Hattori, Yuya*

Radioisotopes, 66(11), p.525 - 530, 2017/11

To understand the mechanisms of radiation biological effects, modeling and simulation studies are important. In particular, simulation approach is powerful tool to evaluate modeling of mechanisms and the relationship among experimental results in different spatial scale of biological systems such as DNA molecular and cell. This article summarizes our approach to evaluate radiation action on DNA and cells by combination of knowledge in radiation physics, chemistry and biology. It contains newly theoretical approach to estimate physico-chemical process of DNA damage induction in addition to typical method of DNA damage prediction. Outline of the mathematical model for dynamics of DNA damage and cellular response is also presented.

Journal Articles

Radiolysis of mixed solutions of Cl$$^{-}$$ and Br$$^{-}$$ and its effect on corrosion of a low-alloy steel

Hata, Kuniki; Inoue, Hiroyuki*; Kojima, Takao*; Kasahara, Shigeki; Hanawa, Satoshi; Ueno, Fumiyoshi; Tsukada, Takashi; Iwase, Akihiro*

Proceedings of Symposium on Water Chemistry and Corrosion in Nuclear Power Plants in Asia 2017 (AWC 2017) (USB Flash Drive), p.304 - 314, 2017/09

A model simulation of $$gamma$$ radiolysis of mixed solutions of NaCl and NaBr was carried out. The simulation result agreed well with the experimental result, and Br$$^{-}$$ played an important role in determining the amounts of products from water radiolysis. The simulation result also showed that, in highly pure NaCl solutions, the steady-state concentration of a radolytic product, H$$_{2}$$O$$_{2}$$, was mainly controlled by three reactions (Cl$$^{-}$$ + $$^{.}$$OH $$rightarrow$$ ClOH$$^{.-}$$, ClOH$$^{.-}$$ $$rightarrow$$ Cl$$^{-}$$ + $$^{.}$$OH, and ClOH$$^{.-}$$ + H$$^{+}$$ $$rightarrow$$ Cl$$^{.}$$ + H$$_{2}$$O), which indicated that accurate evaluation of the rate constants of these reactions was very important in improving the radiolysis simulation of solutions containing Cl$$^{-}$$. An immersion test using a low-alloy steel, SQV2A, in the mixed solutions was also carried out under irradiation. The corrosion rate increased or decreased depending on the pH or the concentrations of the halide ions in a similar way to the change in concentration of H$$_{2}$$O$$_{2}$$ produced from water radiolysis, which is affected by the presence of Cl$$^{-}$$ and Br$$^{-}$$. However, at high pH values ($$>$$12), the corrosion rate was almost zero even though the concentration of H$$_{2}$$O$$_{2}$$ was high. This could be attributed to enhancement of the passivity of test specimens at higher pH values.

Journal Articles

Hydrogen production by $$gamma$$-ray irradiation from different types of zeolites in aqueous solution

Kumagai, Yuta; Kimura, Atsushi*; Taguchi, Mitsumasa*; Watanabe, Masayuki

Journal of Physical Chemistry C, 121(34), p.18525 - 18533, 2017/08

 Times Cited Count:1 Percentile:91.99(Chemistry, Physical)

H$$_{2}$$ production by irradiation of zeolite-water mixtures was studied, to investigate effect of zeolites in the reaction process for H$$_{2}$$. Four different types of zeolites were examined comparatively under anoxic and under aerated conditions. High production yields of H$$_{2}$$ were observed for the zeolites of high Al contents at low water fraction and under anoxic condition, compared to zeolites having lower Al contents. A comparison of the H$$_{2}$$ yields in connection with chemical analysis of the zeolites suggests that extraframework Al species in the zeolites are involved in a reaction pathway for H$$_{2}$$. Meanwhile, under aerated condition and at high mixing ratio of water, the difference in H$$_{2}$$ yield among the zeolites was suppressed and the yields of H$$_{2}$$ were lower than those under anoxic condition probably due to H$$_{2}$$O$$_{2}$$ produced by water radiolysis. The comparable H$$_{2}$$ yields suggest another reaction pathway for H$$_{2}$$ which is less dependent on the structure and composition of the zeolites.

Journal Articles

The Hydrogen gas generation by electron-beam irradiation from ALPS adsorbents solidified by several inorganic materials

Sato, Junya; Suzuki, Shinji*; Kato, Jun; Sakakibara, Tetsuro; Meguro, Yoshihiro; Nakazawa, Osamu

QST-M-2; QST Takasaki Annual Report 2015, P. 87, 2017/03

no abstracts in English

Journal Articles

The Hydrogen gas generation by gamma-ray irradiation from ALPS adsorbents solidified by several inorganic materials

Sato, Junya; Suzuki, Shinji*; Kato, Jun; Sakakibara, Tetsuro; Meguro, Yoshihiro; Nakazawa, Osamu

QST-M-2; QST Takasaki Annual Report 2015, P. 88, 2017/03

no abstracts in English

Journal Articles

Irradiation experiments of simulated wastes of carbonate slurry

Nagaishi, Ryuji; Motooka, Takafumi; Yamagishi, Isao

Proceedings of 2016 EFCOG Nuclear & Facility Safety Workshop (Internet), 6 Pages, 2016/09

Overflow of water from waste storage tanks of High Integrity Containers (HIC) in the multi-nuclide removal equipment (ALPS) was discovered at Fukushima Daiichi NPS in April of last year. The mechanism of overflow was not understood very much at that time. To elucidate that for chemical safety in the waste storage, irradiation experiments of simulated carbonate slurry by Co-60 $$gamma$$-rays have been conducted in CLADS, JAEA in cooperation with TEPCO, TOSHIBA and KURITA. Hydrogen molecule was the main radiolytic gas product in the slurry, and its amount was enhanced by dissolved species of not only halide ions as seawater components but also carbonate ion as an additive for co-precipitation at a basic condition. The bubbles of molecules were further formed and almost held in the slurry without stirred. These sequentially led to the expansion of slurry, and then to its separation into the shrunk one and supernatant water, which was little accumulated without irradiated.

Journal Articles

Estimation of corrosion amounts for carbon steel in $$gamma$$-ray irradiated neutral water condition

Yamamoto, Masahiro; Komatsu, Atsushi; Sato, Tomonori; Nakano, Junichi; Ueno, Fumiyoshi

Proceedings of 17th Asian Pacific Corrosion Control Conference (APCCC-17) (USB Flash Drive), 8 Pages, 2016/01

In Fukushima-Daiichi Nuclear Power Station, decommissioning procedures are continuing more than 30 years until fuel debris removal. It is important to keep soundness of primary container vessel (PCV), made of carbon steel, during these procedures. Corrosion of carbon steel is well-known to be controlled by cathodic reaction, in usual, oxygen reduction reaction. Corrosion of carbon steel could be mitigated by nitrogen injection procedure. However, a lot of radioactive materials exist in cooling water, an effect of radiolysis product on corrosion is an important problem. Clarifying an irradiation effect for corrosion of carbon steel, corrosion test was conducted in $$^{60}$$Co $$gamma$$-ray irradiated condition. Electrochemical measurements were conducted to determine cathodic current density of samples. Corrosion rates of carbon steel decrease with time in both $$gamma$$-ray irradiated and non-irradiated conditions. Measured values of cathodic current density gradually decreased with time and then stayed at constant value.

JAEA Reports

Measurement of hydrogen generating from radiolysis of highly active liquid waste and its quantitative evaluation

Yamamoto, Masahiko; Surugaya, Naoki; Mori, Eito; Taguchi, Shigeo; Sato, Soichi

JAEA-Research 2015-013, 27 Pages, 2015/10


The H$$_{2}$$ concentration generating from Highly Active Liquid Waste (HALW) of Tokai Reprocessing Plant is measured in a closed experimental system. The experimental results show that H$$_{2}$$ concentration gradually increases at first and then approaches a steady-state due to the H$$_{2}$$ consumption reaction by Pd ions. The highest H$$_{2}$$ concentration is 1200 ppm (0.1%) when the solution temperature is at 23$$^{circ}$$C. It is found that H$$_{2}$$ generating from HALW is equilibrated one order of magnitude lower than the H$$_{2}$$ combustion lower limit. Moreover, a model based on H$$_{2}$$ generation from HALW by the radiolysis and H$$_{2}$$ consumption reaction by Pd ions is proposed and applied to evaluate H$$_{2}$$ concentration behavior in the gas phase. The calculated H$$_{2}$$ concentrations from proposed model agreed well with the experimental values. It is demonstrated that the behavior of H$$_{2}$$ generating from HALW can be evaluated quantitatively by applying the proposed model in this study.

Journal Articles

Hydrogen generation by water radiolysis with immersion of oxidation products of zircaloy-4

Matsumoto, Yoshinobu*; Do, Thi-Mai-Dung*; Inoue, Masao; Nagaishi, Ryuji; Ogawa, Toru

Journal of Nuclear Science and Technology, 52(10), p.1303 - 1307, 2015/10

 Times Cited Count:3 Percentile:62.51(Nuclear Science & Technology)

Effects of zirconium oxides and oxidation products of zircaloy-4 on water radiolysis were investigated to predict the hydrogen generation from the water-immersed debris after a severe accident of a nuclear power plant. Observed yields of hydrogen in water containing the oxides were measured as a function of their weight fractions. Assuming that energies of Co-60 $$gamma$$-ray deposited to water and the oxides brought about the water radiolysis to generate hydrogen independently, the radiolysis showed an additional term of hydrogen generation due to the energy deposition to the oxides. This term seemed to be dependent on the specific surface area or particle size of oxides, but not on the crystal structure of oxides in our experimental results. The oxides in distilled water gave the strong enhancement of term. The enhancement tended to saturate with increasing the weight fraction of oxides and was not apparent in the seawater.

Journal Articles

Effect of chloride concentration on corrosion behavior of carbon steel under $$gamma$$-ray irradiation

Motooka, Takafumi; Ueno, Fumiyoshi

Zairyo To Kankyo, 64(6), p.220 - 223, 2015/06

Corrosion behavior of carbon steel in chloride aqueous solutions under a low dose rate was investigated by corrosion test using chloride aqueous solutions with different chloride concentration at a dose rate of 500 Gy/h. The corrosion rate of carbon steel increased by the irradiation, and the corrosion rate had the maximum value at a certain chloride concentration. The oxidants produced by radiolysis of chloride aqueous solution enhanced the corrosion of carbon steel. The main oxidants were oxygen and hydrogen peroxide, and the diffusion process of oxidants controlled the corrosion of carbon steel under irradiation. There was a positive correlation between the dependence of corrosion rate and chloride concentration and the dependence of oxidant concentration and chloride concentration.

Journal Articles

Effect of $$gamma$$-ray irradiation on corrosion of low alloy steel in neutral water

Yamamoto, Masahiro; Nakano, Junichi; Komatsu, Atsushi; Sato, Tomonori; Tsukada, Takashi

Proceedings of 19th International Corrosion Congress (19th ICC) (CD-ROM), 6 Pages, 2014/11

Corrosion protection of RPV and PCV is an important issue for the long term maintenance until the end of the decommissioning procedures. One of the uncertain factors for the issue is an effect of radioactivity on corrosion of LAS and CS. Corrosion tests using LAS and CS were conducted in $$gamma$$-rays irradiated condition. Oxygen and hydrogen peroxide concentrations in the water were measured after the tests. Corrosion test results indicated that the amounts of corrosion increased by $$gamma$$-rays irradiation both air and nitrogen atmosphere. And also corrosion amounts increased with $$gamma$$-ray dose rates. Electrochemical analyses indicated that cathodic reaction of Hydrogen peroxide was controlled by diffusion process. The measured diffusion constant of H$$_{2}$$O$$_{2}$$ was about 0.75 times to that of oxygen. From these results, it is estimated that corrosion of LAS and CS in $$gamma$$-ray irradiated condition was evaluated by the cathodic reduction reaction of oxidant.

Journal Articles

Revaluation of hydrogen generation by water radiolysis in SDS vessels at TMI-2 accident

Nagaishi, Ryuji; Morita, Keisuke; Yamagishi, Isao; Hino, Ryutaro; Ogawa, Toru

Proceedings of 2014 Nuclear Plant Chemistry Conference (NPC 2014) (USB Flash Drive), 9 Pages, 2014/10


Two years after Three Mile Island Unit 2 (TMI-2) loss-of-coolant accident, radioactive contaminated water has been processed by Submerged Demineralizer System (SDS) with two types of zeolite adsorbents to remove radioactive nuclides. During and after the process, adsorption amount and distribution of nuclides on the zeolites, residual water content and thermal conductivity in the SDS vessels have been measured or estimated for verification of safety in the process, subsequent transportation and disposal. Hydrogen generation has been also evaluated mainly by direct monitoring in the large-scale of vessel after the process. In this work, the revaluation of hydrogen generation was demonstrated on the basis of the open information of vessel, and the latest experimental data obtained in adsorption and radiolysis occurring in small-scale of zeolite-water mixtures. As a result, the evaluated data was found to be comparable with the reported data obtained in the large-scale of real vessel.

Journal Articles

Consideration of radiolytic behavior in diluted and concentrated systems of seawater for computational simulation of hydrogen generation

Nagaishi, Ryuji; Inoue, Masao; Hino, Ryutaro; Ogawa, Toru

Proceedings of 2014 Nuclear Plant Chemistry Conference (NPC 2014) (USB Flash Drive), 9 Pages, 2014/10

Since seawater has been used as a coolant for reactors and spent fuel pools in broken reactor buildings at Fukushima Daiichi NPS accident, radioactive contaminated water emitted following the accident has contained salt content of seawater at high concentrations, different from that at TMI-2 accident. Radiolysis of seawater leading to hydrogen generation and corrosion has been simulated and reported by several groups. However, the proposed radiolysis models cannot be always applied to water radiolysis at the wide range of salt concentrations present in the NPS, mainly because primary yields of radiolysis products of water and radiation-induced reactions are dependent on the salt concentration. In this study, the radiolytic behavior in diluted and concentrated systems of seawater was considered on the basis of results in steady state and pulse radiolysis experiments, in which the above salt effects were demonstrated from the obtained results.

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