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JAEA Reports

Development of a new corrosion mitigation technology using nanobubbles toward corrosion mitigation in PCV system under the influence of $$alpha$$/$$beta$$/$$gamma$$-rays radiolysis (Contract research); FY2020 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Tohoku University*

JAEA-Review 2022-002, 85 Pages, 2022/06


The Collaborative Laboratories for Advanced Decommissioning Science (CLADS), Japan Atomic Energy Agency (JAEA), had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project (hereafter referred to "the Project") in FY2020. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. (TEPCO). For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2020, this report summarizes the research results of the "Development of a new corrosion mitigation technology using nanobubbles toward corrosion mitigation in PCV system under the influence of $$alpha$$/$$beta$$/$$gamma$$-rays radiolysis" conducted in FY2020. In this work, in order to ensure the long-term reliability of steel structures that ensure important confinement functions in the debris removal process, such as existing PCVs and newly constructed negative pressure maintenance systems and piping, corrosion phenomena in wet environments where $$alpha$$- and $$beta$$-ray emitting nuclides come into contact with steel are clarified for the first time. At the same time, we will develop a new corrosion prevention technology that has excellent basic applicability to PCVs and has

Journal Articles

Radiation-induced effects on the extraction properties of hexa-$$n$$-octylnitrilo-triacetamide (HONTA) complexes of americium and europium

Toigawa, Tomohiro; Peterman, D. R.*; Meeker, D. S.*; Grimes, T. S.*; Zalupski, P. R.*; Mezyk, S. P.*; Cook, A. R.*; Yamashita, Shinichi*; Kumagai, Yuta; Matsumura, Tatsuro; et al.

Physical Chemistry Chemical Physics, 23(2), p.1343 - 1351, 2021/01

 Times Cited Count:4 Percentile:71(Chemistry, Physical)

The candidate An(III)/Ln(III) separation ligand hexa-$$n$$-octylnitrilo-triacetamide (HONTA) was irradiated under envisioned SELECT (Solvent Extraction from Liquid waste using Extractants of CHON-type for Transmutation) process conditions using a solvent test loop in conjunction with cobalt-60 gamma irradiation. We demonstrate that HONTA undergoes exponential decay with increasing gamma dose to produce a range of degradation products which have been identified and quantified by HPLC-ESI-MS/MS techniques. The combination of HONTA destruction and degradation product ingrowth, particularly dioctylamine, negatively impacts the extraction and back-extraction of both americium and europium ions. The loss of HONTA was attributed to its reaction with the solvent (${it n}$-dodecane) radical cation of ${it k}$(HONTA + R$$^{.+}$$) = (7.61 $$pm$$ 0.82) $$times$$ 10$$^{9}$$ M$$^{-1}$$ s$$^{-1}$$ obtained by pulse radiolysis techniques. However, when this ligand is bound to either americium or europium ions, the observed ${it n}$-dodecane radical cation kinetics increase by over an order of magnitude. This large reactivity increase to additional reaction pathways occurring upon metal-ion binding. Lastly nanosecond time-resolved measurements showed that both direct and indirect HONTA radiolysis yielded the short-lived ($$<$$100 ns) HONTA radical cation as well as a longer-lived ($$mu$$s) HONTA triplet excited state. These HONTA species are important precursors to the suite of HONTA degradation products observed.

Journal Articles

Study on the mechanism of radiolytic degradation of an extractant for minor actinides separation

Toigawa, Tomohiro; Murayama, Rin*; Kumagai, Yuta; Yamashita, Shinichi*; Suzuki, Hideya; Ban, Yasutoshi; Matsumura, Tatsuro

UTNL-R-0501, p.24 - 25, 2020/12

This report summarizes the results obtained in FY2019 at Electron Linac Facility of University of Tokyo. The radiolysis process of a diglycolamide extractant, which is expected to be used in the separation process of minor actinides (MA), in dodecane and octanol solutions was investigated by pulse radiolysis. As a result, it was suggested that by adding alcohol, the decomposition process of the diglycolamide extractant was different from the decomposition processes in the single solvent of dodecane considered that the decomposition occurred via a radical cation species of the extractant.

Journal Articles

On the hydrogen production of geopolymer wasteforms under irradiation

Cantarel, V.; Arisaka, Makoto; Yamagishi, Isao

Journal of the American Ceramic Society, 102(12), p.7553 - 7563, 2019/12

 Times Cited Count:6 Percentile:44.2(Materials Science, Ceramics)

The hydrogen gas (H$$_{2}$$) production of wasteforms is a major safety concern for encapsulating nuclear wastes. For geopolymers, the H$$_{2}$$ produced by radiolytic processes is a key factor because of the large amount of water present in their porous structure. Herein, the hydrogen production was measured under $$^{60}$$Co gamma irradiation. The effect of water saturation and sample size were studied for pure geopolymers, or using zeolites as an example waste. When geopolymer monolithic samples were large and saturated by water, the hydrogen released was measured up to two orders of magnitude lower with a 40 cm long cylinder samples (1.9$$times$$10$$^{-10}$$ mol/J) than a sample in powder form (2.2$$times$$10$$^{-8}$$ mol/J). To interpret results, a simple model was used, considering only hydrogen production, a potential recombination and its diffusion in the geopolymer matrix. Knowing the diffusion constant of the matrix, the model was able to reproduce the evolution of the hydrogen release as a function of the water saturation level and predict the evolution when sample size is increased up to 40 cm.

Journal Articles

Preliminary verification of water radiolysis and ECP calculation models by in-pile ECP measurements

Hanawa, Satoshi; Hata, Kuniki; Chimi, Yasuhiro; Kasahara, Shigeki

Proceedings of 21st International Conference on Water Chemistry in Nuclear Reactor Systems (Internet), 12 Pages, 2019/09

Journal Articles

Radiation-induced degradation of aqueous 2-chlorophenol assisted by zeolites

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

Journal of Radioanalytical and Nuclear Chemistry, 316(1), p.341 - 348, 2018/04

 Times Cited Count:2 Percentile:27.95(Chemistry, Analytical)

We studied effect of adsorption and condensation by zeolites on radiation-induced degradation of aqueous 2-chlorophenol (2-ClPh). This study aims to demonstrate that the solid-phase extraction using zeolites has potential advantage in treatments of aqueous organic pollutants. Among three zeolites examined in this study, a mordenite type zeolite (HMOR) that has a high Si to Al ratio (127 $$pm$$ 3) exhibited preferable performance as the matrix for the 2-ClPh degradation. HMOR adsorbed far more 2-ClPh than the other zeolites, which have lower Si/Al ratios. The irradiation of HMOR induced degradation of adsorbed 2-ClPh into Cl$$^{-}$$ and organic by-products. We found a significant increase in Cl$$^{-}$$ production by HMOR. The yield of Cl$$^{-}$$ production in the presence of HMOR was as high as the yield in aqueous solution of 2-ClPh at a concentration 10 times higher. The increased Cl$$^{-}$$ production indicates that the high concentration of adsorbed 2-ClPh led to effective use of the adsorbed energy of HMOR.

Journal Articles

A Modelling study on water radiolysis for primary coolant in PWR

Mukai, Satoru*; Umehara, Ryuji*; Hanawa, Satoshi; Kasahara, Shigeki; Nishiyama, Yutaka

Proceedings of 20th International Conference on Water Chemistry of Nuclear Reactor Systems (NPC 2016) (USB Flash Drive), 9 Pages, 2016/10

In Japanese PWR, the concentration of dissolved hydrogen in the primary coolant is controlled in the range from 25 cc/kg-H$$_{2}$$O to 35 cc/kg-H$$_{2}$$O for suppression of water decomposition. However this concentration is desired to reduce for the purpose of radiation source reduction in Japan. So, the concentration due to water radiolysis in primary coolant was evaluated at lower hydrogen concentration by the water radiolysis model in consideration of $$gamma$$ ray, fast neutron and alpha ray due to the reaction $$^{10}$$B(n,$$alpha$$)$$^{7}$$Li. The results of evaluation showed that the water radiolysis was suppressed even if the hydrogen concentration was decreased to 5 cc/kg-H$$_{2}$$O. The effects of the different G-value and the rate constants of major reaction on the concentration of H$$_{2}$$O$$_{2}$$ and O$$_{2}$$ were studied under hydrogen addition. We also focused on the effect of the alpha radiolysis in boron acid water.

Journal Articles

Study of irradiation effect on ECP using in-pile loops in the JMTR

Hanawa, Satoshi; Uchida, Shunsuke; Hata, Kuniki; Chimi, Yasuhiro; Kasahara, Shigeki*; Nishiyama, Yutaka

Proceedings of 20th Nuclear Plant Chemistry International Conference (NPC 2016) (USB Flash Drive), 10 Pages, 2016/10

The authors proposed and ECP evaluation model introducing irradiation-induced diffusion in the oxide layer to simulate neutron irradiation effect, and predicted with this model that ECP is started to depress from the neutron flux of about ten to the fourteenth per square meter. As the JMTR has in-pile loops applicable to water chemistry experiments, degree of irradiation effect on ECP appears in the in-pile loop was estimated by the model. Under oxygen injected condition, ECP in a capsule becomes constant along the vertical direction due to the presence of high amount of oxygen and hydrogen peroxide in a capsule. However, if neutron irradiation depress ECP, ECP in a capsule along vertical direction wouldn't become constant, and the degree to the decrement is detectable by experiments.

Journal Articles

Simulation for radiolytic products of seawater; Effects of seawater constituents, dilution rate, and dose rate

Hata, Kuniki; Sato, Tomonori; Motooka, Takafumi; Ueno, Fumiyoshi; Hanawa, Satoshi; Kasahara, Shigeki; Tsukada, Takashi

Journal of Nuclear Science and Technology, 53(8), p.1183 - 1191, 2016/08

 Times Cited Count:5 Percentile:49.98(Nuclear Science & Technology)

Journal Articles

Radiolysis of boiling water

Yang, S.*; Katsumura, Yosuke*; Yamashita, Shinichi*; Matsuura, Chihiro*; Hiroishi, Daisuke*; Lertnaisat, P.*; Taguchi, Mitsumasa

Radiation Physics and Chemistry, 123, p.14 - 19, 2016/06

 Times Cited Count:2 Percentile:23.29(Chemistry, Physical)

$$gamma$$-radiolysis of boiling water has been investigated. The G-value of H$$_{2}$$ evolution was found to be very sensitive to the purity of water. In high-purity water, both H$$_{2}$$ and O$$_{2}$$ gases were formed in the stoichiometric ratio of 2:1; a negligible amount of H$$_{2}$$O$$_{2}$$ remained in the liquid phase. The G-values of H$$_{2}$$ and O$$_{2}$$ gas evolution depend on the dose rate: lower dose rates produce larger yields. To clarify the importance of the interface between liquid and gas phase for gas evolution, the gas evolution under Ar gas bubbling was measured. A large amount of H$$_{2}$$ was detected, similar to the radiolysis of boiling water. The evolution of gas was enhanced in a 0.5 M NaCl aqueous solution. Deterministic chemical kinetics simulations elucidated the mechanism of radiolysis in boiling water.

Journal Articles

Effects of constituents of seawater on formation of volatile iodine by aqueous phase radiation chemistry

Hata, Kuniki; Kido, Kentaro; Nishiyama, Yutaka; Maruyama, Yu

NEA/CSNI/R(2016)5 (Internet), p.196 - 203, 2016/05

Journal Articles

Hydrogen peroxide production by $$gamma$$ radiolysis of sodium chloride solutions containing a small amount of bromide ion

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

Nuclear Technology, 193(3), p.434 - 443, 2016/03

 Times Cited Count:10 Percentile:75.38(Nuclear Science & Technology)

Journal Articles

Effects of $$alpha$$-radiation on a direct disposal system for spent nuclear fuel, 1 Review of research into the effects of $$alpha$$-radiation on the spent nuclear fuel, canisters and outside canisters

Kitamura, Akira; Takase, Hiroyasu*

Journal of Nuclear Science and Technology, 53(1), p.1 - 18, 2016/01

 Times Cited Count:3 Percentile:14.58(Nuclear Science & Technology)

Not only geological disposal of vitrified waste generated by spent fuel (SF) reprocessing, but also the possibility of disposing of SF itself in deep geological strata (hereinafter "direct disposal of SF") may be considered in the Japanese geological disposal program. In the case of direct disposal of SF, the radioactivity of the waste is higher and the potential effects of the radiation are greater. Specific examples of the possible effects of radiation include: increased amounts of canister corrosion; generation of oxidizing chemical species in conjunction with radiation degradation of groundwater and accompanying oxidation of reducing groundwater; and increase in the dissolution rate and the solubility of SF. Focusing especially on the effects of $$alpha$$-radiation in safety assessment, this study has reviewed research into the effects of $$alpha$$-radiation on the spent nuclear fuel, canisters and outside canisters.

Journal Articles

Effects of $$alpha$$-radiation on a direct disposal system for spent nuclear fuel, 2; Review of research into safety assessments of direct disposal of spent nuclear fuel in Europe and North America

Kitamura, Akira; Takase, Hiroyasu*; Metcalfe, R.*; Penfold, J.*

Journal of Nuclear Science and Technology, 53(1), p.19 - 33, 2016/01

 Times Cited Count:1 Percentile:7.29(Nuclear Science & Technology)

Not only geological disposal of vitrified waste generated by spent fuel (SF) reprocessing, but also the possibility of disposing of SF itself in deep geological strata (hereinafter "direct disposal of SF") may be considered in the Japanese geological disposal program. In the case of direct disposal of SF, the radioactivity of the waste is higher and the potential effects of the radiation are greater. Specific examples of the possible effects of radiation include: increased amounts of canister corrosion; generation of oxidizing chemical species in conjunction with radiation degradation of groundwater and accompanying oxidation of reducing groundwater; and increase in the dissolution rate and the solubility of SF. Therefore, the influences of radiation, which are not expected to be significant in the case of geological disposal of vitrified waste, must be considered in safety assessments for direct disposal of SF. Focusing especially on the effects of $$alpha$$-radiation in safety assessment, this study has reviewed safety assessments in countries other than Japan that are planning direct disposal of SF. The review has identified issues relevant to safety assessment for the direct disposal of SF in Japan.

Journal Articles

Degradation of 2-chlorophenol by $$gamma$$-ray irradiation in zeolite/water mixtures

Kumagai, Yuta

Hoshasen Kagaku (Internet), (99), p.53 - 56, 2015/04

Radiation-induced degradation of 2-chlorophenol (2-ClPh) in zeolite/water mixtures was studied in order to consider a possibility of adsorption on zeolites to improve efficiencies of irradiation treatments of water contaminated by organic compounds. The degradation of 2-ClPh by $$gamma$$-ray irradiation was investigated as a model compound. The degradation was evaluated by chloride ion (Cl$$^{-}$$) production. A high concentration of Cl$$^{-}$$ was observed after the irradiation of a mixture with a mordenite-type zeolite (NaMOR), whereas A-type and X-type zeolites showed no significant effect. Therefore, for the mixture with NaMOR, effects of pH of the solution and of the 2-ClPh concentration were examined. At pH 5.7, the excess production of Cl$$^{-}$$ was induced by the addition of NaMOR. Concurrently, adsorption of 2-ClPh on NaMOR was observed. When the mixture contained a higher concentration of 2-ClPh at pH 5.7, the Cl$$^{-}$$ production increased. The adsorption of 2-ClPh also increased with increasing concentration. The results suggest that organics adsorbed on zeolites are decomposed by irradiation effectively at high adsorption concentrations.

Journal Articles

Influence of radiolysis and gas-liquid partition of I-131 in accumulated water on late phase source terms at Fukushima NPP accident

Hidaka, Akihide

Proceedings of 2014 Nuclear Plant Chemistry Conference (NPC 2014) (USB Flash Drive), 12 Pages, 2014/10

During core cooling at Fukushima Daiichi NPP accident, large amount of contaminated water was accumulated in the basements of reactor buildings at Units 1 to 4. The estimated ratios of I-131 and Cs-137 quantities in water to the core inventories are 0.51%, 0.85% at Unit 1, 74%, 38% at Unit 2 and 26%, 18% at Unit 3, respectively. According to the Henry's law, certain fraction of iodine in water could be released to atmosphere. Many evaluations for I-131 release have been performed so far by MELCOR or the reverse estimation with SPEEDI. The SPEEDI reverse predicted significant release until March 26 while no prediction in MELCOR after March 17. The present study showed that iodine release from accumulated water due to radiolytic conversion from I$$^{-}$$ to I$$_{2}$$ and gas-liquid partition of I$$_{2}$$ may explain the release between March 17 and 26. This strongly suggests a need for improvement of current MELCOR approach which treats the release only from containment breaks.

Journal Articles

Safety handling characteristics of high-level tritiated water

Hayashi, Takumi; Ito, Takeshi*; Kobayashi, Kazuhiro; Isobe, Kanetsugu; Nishi, Masataka

Fusion Engineering and Design, 81(8-14), p.1365 - 1369, 2006/03

 Times Cited Count:18 Percentile:77.84(Nuclear Science & Technology)

In a fusion reactor, high-level tritiated water of more than GBq/ml will be generated and stored temporally in the various areas. High level tritiated water decomposes by itself and generates hydrogen and oxygen, and becomes to tritiated hydrogen peroxide water, however, effective G-values from tritiated water are different from those obtained $$gamma$$-ray experiments in our previous report. Furthermore, tritiated water of about 250GBq/ml has been stored for several years safely and checked its characteristics. Using the above experiences, this paper summarizes safety requirements for storage of high-level tritiated water and discusses design issues of the safety storage system. Concerning gaseous species, storage tank should be maintained at negative pressure and purged periodically or constantly to dedicated tritium removal system. Specially, it is important that the G-value of high-level tritiated water is increasing with decreasing the tritium concentration. The pH and ORP (Oxidation Reduction Potential) of tritiated water have been also changed depending on the tritium concentration and maintained for more than several years in glass vessel. High-level tritiated water of more than GBq/ml was acid and became to be corrosive depending on the dissolved species. Large amount of tritiated water will be stored in the various tanks of stainless steel, therefore, it should be monitored so that the liquid situation is maintained not to be corrosive.

Journal Articles

Time-dependence of differential G-values of OH radicals in water under Ne ion radiolysis

Taguchi, Mitsumasa; Kojima, Takuji

JAEA-Review 2005-001, TIARA Annual Report 2004, p.181 - 182, 2006/01

The yields of OH radicals in water containing phenol have been investigated for several ten MeV/n C ion and Ne ion having the same LET value, as a function of the residual ion energy at the specific depth in water. In this study, beside such energy dependence, the dependence of reaction time of OH radical yield was examined by changing the concentration of phenol as solute. The defferential G'-values of OH radicals, those G-values per kinetic energy of ions increase with specific energy of Ne ions. The G'-value just after irradiation(1.5ns) is relatively high but become lower with reaction time to be the value (2.7) obtained for $$^{60}$$Co $$gamma$$-rays. It suggests the diffusion behavior of OH radicals locally induced in water.

Journal Articles

Study of radiation-induced primary process by ion pulse radiolysis

Yoshida, Yoichi*; Yang, J.*; Kondo, Takafumi*; Seki, Shuhei*; Kozawa, Takahiro*; Tagawa, Seiichi*; Shibata, Hiromi*; Taguchi, Mitsumasa; Kojima, Takuji; Namba, Hideki

JAEA-Review 2005-001, TIARA Annual Report 2004, p.183 - 185, 2006/01

A heavy-ion-pulse radiolysis technology was developed using a single-photon-counting system. In the system, the ion beam was injected a thin scintillator before irradiating the sample. The light emitted from the scintillator by the ion irradiation was used as analyzing source to detect the absorption of primary species in water. Measurement of time-dependent absorption of hydrated electrons in water was achieved using the system, which demonstrates the usefulness of this technique.

JAEA Reports

Numerical analysis on deflagration-to-detonation transition of a hydrogen-oxygen mixture in a smooth tube

Inaba, Yoshitomo; Kotchourko, A.*; Breitung, W.*

JAERI-Tech 2005-053, 24 Pages, 2005/09


The Flow and Combustion Engineering Division at the Forschungszentrum Karlsruhe carried out the explosion experiments of hydrogen-oxygen mixtures in a smooth tube made of stainless steel after two radiolysis gas explosion accidents occurred in Japanese and German BWRs. In these experiments, stoichiometric hydrogen-oxygen mixtures with different initial pressures were used. The pressure in the tube and the strain of the tube were measured, and then the structural response during the detonation and the Deflagration-to-Detonation Transition (DDT) process were investigated. In the present study, a numerical analysis was performed to simulate one of the experiments by the use of the 3-dimensional turbulent combustion analysis code COM3D, which has been developed in FZK, and a DDT process was calculated. The COM3D code contains a reaction rate constant, which must be obtained empirically from experimental results. In the present calculation, the reaction rate constant was assumed to be an exponential function. As a result, it was found that the COM3D code can simulate the DDT process.

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