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JAEA Reports

Development of the Sintering Solidification Method for Spent Zeolite to Long-term Stabilization (Contract research); FY2019 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Shibaura Institute of Technology*

JAEA-Review 2020-049, 78 Pages, 2021/01

JAEA-Review-2020-049.pdf:5.85MB

JAEA/CLADS had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project. Among the adopted proposals in FY2018, this report summarizes the research results of the "Development of the Sintering Solidification Method for Spent Zeolite to Long-term Stabilization" conducted in FY2019.

JAEA Reports

Development of the sintering solidification method for spent zeolite to long-term stabilization (Contract research); FY2018 Center of World Intelligence Project for Nuclear Science/Technology and Human Resource Development

Collaborative Laboratories for Advanced Decommissioning Science; Shibaura Institute of Technology*

JAEA-Review 2019-028, 71 Pages, 2020/03

JAEA-Review-2019-028.pdf:6.46MB

JAEA/CLADS, had been conducting the Center of World Intelligence Project for Nuclear Science/Technology and Human Resource Development (hereafter referred to "the Project") in FY2018. Among the adopted proposals in FY2018, this report summarizes the research results of the "Development of the Sintering Solidification Method for Spent Zeolite to Long-term Stabilization". The present study aims to develop the sintering solidification method for zeolites (spent zeolites) that adsorbs continuously generated radionuclides such as cesium. The sintering solidification method is able to stabilize adsorbed radionuclides such as cesium in zeolites by adding a glass as a binder to spent zeolite and sintered it. It is expected that the sintering solidification method is significantly reduce the volume of the solidified body compare with the glass solidification method and to form a stable solidified body equivalent to the calcination solidification method. In this project, we planned to select a glass suitable for the sintering solidification method and optimize the sintering temperature, etc. using non-radioactive nuclides (cold tests), and verify it by using radioactive nuclides (hot tests). In FY2018, we investigated the thermal properties of candidate glasses for binder and the effect of heating atmosphere on the sintering solidification method. Irradiated fuel for preparing simulated contaminated water containing radionuclides was selected and the condition of it was observed. In addition, we surveyed existing research results and latest research trends about solidification of zeolite, calcination solidification and so on.

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:5 Percentile:48.77(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

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:1 Percentile:17.98(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

Effects of gamma-ray irradiation on spontaneous potential of stainless steel in zeolite-containing diluted artificial seawater

Kato, Chiaki; Sato, Tomonori; Ueno, Fumiyoshi; Yamagishi, Isao

Proceedings of 17th International Conference on Environmental Degradation of Materials in Nuclear Power Systems - Water Reactors, Vol.2, p.1357 - 1374, 2016/05

With respect to the long-term storage of the zeolite-containing spent Cs adsorption vessels used at the Fukushima Daiichi Nuclear Power Station, the corrosion of the vessel material is one of the most important issues. In this study, we performed electrochemical tests on stainless steel specimens in zeolite-containing artificial seawater under gamma-ray irradiation. The spontaneous potential ESP and critical pitting potential VC of the type 316L steel in systems in contact with various zeolites were measured in order to evaluate the corrosion resistance of the steel. In addition, the water sample was analyzed after being irradiated, in order to determine the concentrations of various dissolved oxidants such as oxygen and hydrogen peroxide, which can accelerate the corrosion process. The steady-state rest potential increased with an increase in the dose rate; however, the increase was suppressed in contact with the zeolites. The VC value of the steel when in contact with the zeolites was slightly smaller than the VC value in bulk water; however, the choice of the zeolite used as herschelite, IE96 and IE911 hardly affect the VC value. The concentration of H$$_{2}$$O$$_{2}$$ in the bulk water under irradiation also increased with the increase in the dose rate. This increase was suppressed in the systems in contact with the zeolites, owing to the decomposition of the H$$_{2}$$O$$_{2}$$ by the zeolites. A clear relationship was observed between ESP and the H$$_{2}$$O$$_{2}$$ concentration. As contact with the zeolites caused the increase in ESP under irradiation to be suppressed, it can be concluded that the presence of zeolites in the spent Cs adsorption vessels can reduce the probability of the localized corrosion of the stainless steel in the vessels.

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

Local structure around cesium in montmorillonite, vermiculite and zeolite under wet condition

Tsuji, Takuya; Matsumura, Daiju; Kobayashi, Toru; Suzuki, Shinichi; Yoshii, Kenji; Nishihata, Yasuo; Yaita, Tsuyoshi

Clay Science, 18(4), p.93 - 97, 2014/12

Journal Articles

Corrosion of the stainless steel in the zeolite containing diluted artificial seawater under $$gamma$$-ray irradiation

Kato, Chiaki; Sato, Tomonori; Nakano, Junichi; Ueno, Fumiyoshi; Yamagishi, Isao

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

As a part of consideration for long-term storage of spent zeolite adsorption vessels in the Fukushima Daiichi Nuclear Power Station, corrosion of vessel material in the spent zeolite adsorption vessel is one of important issue. We performed electrochemical tests of stainless steel (type 316L) in the zeolite containing artificial seawater under $$gamma$$-ray irradiation. Steady spontaneous potential (Esp) and pitting potential (VC), of type 316L was measurement. $$^{60}$$Co $$gamma$$-rays source was used under irradiation. Dose rate of $$gamma$$-ray irradiation was controlled for 5 kGy/h and 400 Gy/h. In anode polarization curves, there was no clear difference under irradiation and non-irradiation. The corrosion potential of type 316L increased with increasing time after $$gamma$$-ray irradiation. The Esp was shifted to nobler by $$gamma$$-rays irradiation, while increasing Esp was suppressed by contacted with zeolite.

Journal Articles

Alteration-phase formation and associated cesium release during alteration of R7T7 waste glass

Inagaki, Yaohiro*; Idemitsu, Kazuya*; Arima, Tatsumi*; Maeda, Toshikatsu; Ogawa, Hiromichi; Itonaga, Fumio

Materials Research Society Symposium Proceedings, Vol.713, p.589 - 596, 2002/00

A large number of studies on HLW glass corrosion have shown that the glass reacts with water to form more stable mineral phases (alteration phases) during the long-term geological disposal. The phase formation is essential to evaluate the radionuclide release from the glass during the long-term disposal. The purpose of this study is to evaluate, experimentally, the mineral phase formation from HLW glass and the associated cesium release. Static corrosion tests were performed on powdered R7T7 glass in alkalline solutions at elevated temperatures to accelerate the reaction, and mineral phases formed were analyzed by XRD. The results showed that analcime (zeolite) is formed as the dominant phase coexisting with SiO$$_{2}$$(am), and beidellite(smectite) or gibbsite coexists dependiting on the conditions. The solution analysis indicated that most of the cesium is retained in the phases of beidellite and analcime by sorption.

Journal Articles

Radiolytic hydrogen gas formation from water adsorbed on type Y zeolites

Nakashima, Mikio;

Radiation Physics and Chemistry, 47(2), p.241 - 245, 1996/00

no abstracts in English

Journal Articles

Radiolytic hydrogen gas formation from water adsorbed on type A zeolites

Nakashima, Mikio; Aratono, Yasuyuki

Radiation Physics and Chemistry, 41(3), p.461 - 465, 1993/00

 Times Cited Count:19 Percentile:84.69(Chemistry, Physical)

no abstracts in English

Journal Articles

A Simplified method for preparation of $$^{1}$$$$^{3}$$$$^{7}$$Cs pollucite $$gamma$$-ray source

*; ;

Int.J.Appl.Radiat.Isot., 32, p.595 - 599, 1981/00

 Times Cited Count:3 Percentile:55.98(Nuclear Science & Technology)

no abstracts in English

Journal Articles

Dissolution and solidification of aluminum capsule in production of Mo-99 by sublimation from neutron-irradiatedUO$$_{2}$$

; ; ; *

Journal of Nuclear Science and Technology, 17(1), p.83 - 85, 1980/00

 Times Cited Count:0 Percentile:0.29(Nuclear Science & Technology)

no abstracts in English

Journal Articles

ESR and NMR study of the $$gamma$$-ray-induced postpolymerization of vinyl monomers adsorbed on zeolite

J.P.Quaegebeur*; Seguchi, Tadao; H.Lebail*; C.Chachaty*

Journal of Polymer Science; Polymer Chemistry Edition, 14(11), p.2703 - 2724, 1976/11

no abstracts in English

Oral presentation

Hydrogen and hydrogen peroxide productions by $$gamma$$-irradiation of A-, X-, Y- and mordenite type zeolites in aqueous solution

Kumagai, Yuta; Kimura, Atsushi; Taguchi, Mitsumasa

no journal, , 

Zeolite minerals are suitable adsorbents for removal of radioactive cesium in water, because of their high radiation resistances. However, irradiation of zeolites results in decomposition of water adsorbed on the zeolites. Water decomposition produces hydrogen (H$$_{2}$$) and hydrogen peroxide (H$$_{2}$$O$$_{2}$$). H$$_{2}$$ production has a risk of making an explosive gas mixture. H$$_{2}$$O$$_{2}$$ causes corrosion of metals and alloys. Therefore, the radiation effects are required to be assessed and controlled. In this study, H$$_{2}$$ and H$$_{2}$$O$$_{2}$$ production by irradiation of zeolites in aqueous solution are comparatively studied among different types of zeolites, A-, X-, Y- and mordenite-types. The mixtures of the zeolites and aqueous solution were irradiated by $$^{60}$$Co $$gamma$$-rays. The A-type and the X-type zeolites produced more H$$_{2}$$ than the Y-type and the mordenite-type. In contrast, the H$$_{2}$$O$$_{2}$$ production was inhibited by the addition of zeolites. The A-type and the X-type zeolites showed remarkable inhibition. The A-type and the X-type contains more aluminum in their frameworks than the others do. Therefore, the results suggest that aluminum sites have an important role in the reactions induced by irradiation.

Oral presentation

Behavior of radiolytic gas in zeolite bed under $$gamma$$-ray irradiation

Motooka, Takafumi; Yamagishi, Isao

no journal, , 

Mixtures of zeolite IE96 and artificial seawater (ASW) were poured in cylindrical tubes, and irradiated by Co-60 $$gamma$$-rays. In the case of a zeolite bed which was fully immersed in ASW, the zeolite bed level increased slightly (1.8%) and an ASW phase formed onto the bed. The ASW level increased with the irradiation dose. In the case of a partial immersion, which simulates a drained zeolite vessel, the zeolite bed level was un-changed (0.0%).

Oral presentation

Study on wet waste storage; Irradiation behavior of carbonate slurry and wet zeolite

Yamagishi, Isao; Motooka, Takafumi

no journal, , 

Highly radioactive wastes such as carbonate slurry and zeolite are generated from the contaminated water treatment system at Fukushima Daiichi Nuclear Power Station. We have studied radiolytic gas generation in wet wastes for their safe storage. Carbonate slurry or wet zeolite as a simulated waste was irradiated by $$gamma$$-ray. Radiolytic gas generation resulted in the slurry expansion and supernatant separation from the slurry. The supernatant was observed during irradiation of the zeolite immersed fully in seawater but not in case of the partial immersion.

Oral presentation

Selective uranium adsorption from liquid waste using zeolites

Matsuura, Haruaki*; Aso, Hiroki*; Toyosaki, Ayaka*; Asanuma, Noriko*; Takahatake, Yoko; Hoshino, Takanori; Watanabe, So; Watanabe, Masayuki

no journal, , 

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