Kumagai, Yuta; Nagaishi, Ryuji; Kimura, Atsushi*; Taguchi, Mitsumasa*; Nishihara, Kenji; Yamagishi, Isao; Ogawa, Toru
Insights Concerning the Fukushima Daiichi Nuclear Accident, Vol.4; Endeavors by Scientists, p.37 - 45, 2021/10
Zeolite adsorbents are to be used for decontamination of radioactive water in Fukushima Dai-ichi Nuclear Power Station. Evaluation of hydrogen production by water radiolysis during decontamination is important for safe operation. Thus hydrogen production from the mixture of zeolite adsorbents and seawater was studied because seawater was urgently used as a coolant for the fuels. The hydrogen yield from the mixture decreased at a high weight fraction of zeolites. However, the measured yield was higher than the yield expected from the direct radiolysis of seawater in the mixture, which would decrease proportional to the weight fraction of seawater. The result suggests that the radiation energy deposited to zeolites was involved in the hydrogen formation. From the results, the hydrogen production rate was evaluated to be 3.6 mL/h per ton of radioactive water before decontamination. After the process, it was evaluated to be 1.5 L/h per ton of waste adsorbents due to the high dose rate.
Horita, Takuma; Yamagishi, Isao; Nagaishi, Ryuji; Kashiwaya, Ryunosuke*
JAEA-Technology 2021-012, 34 Pages, 2021/07
Waste mainly consisting of carbonate precipitates (carbonate slurry) from the Advanced Liquid Processing System (ALPS) and the improved ALPS at the Fukushima Daiichi Nuclear Power Station of Tokyo Electric Power Holdings, Inc. have been storing in the High Integrity Container (HIC). The supernatant solution of carbonate slurry contained in some of HICs were overflowed in April of 2015. The all of level of liquid in the HICs were investigated; however, almost of the HICs were under the level of overflow. The mechanism of overflow suggested to be depending on the difference of the properties of the carbonate slurry such as the retention/release characteristics of the bubbles. Therefore, in order to clarify the mechanism of leakage, the repeatability experiment was carried out by using simulated carbonate slurry. The simulated carbonate slurry was perpetrated by using the same cross-flow filter system of the actual ALPS. Moreover, the preparative conditions for the simulated carbonate slurry were the same as Mg/Ca concentration ratio in inlet water of the ALPS (raw water) and the ALPS operating conditions. The chemical characteristics of simulated carbonate slurries were revealed by ICP-AES, pH meter, etc. The density of the settled slurry layer tended to increase depending on the calcium concentration in the raw water. The bubble injection test was conducted in order to investigate the bubble retention/release behavior in the simulated carbonate slurry layer. The simulated carbonate slurry with high settling density, which was generated by high calcium concentration solution was revealed to retain the injected bubbles. Since the ratio of concentration calcium and magnesium during the carbonate slurry generation is assumed to affect the retention of bubbles in the slurry layer, the information on the composition of raw water is one of important factor for overflow of HICs.
Cantarel, V.; Lambertin, D.*; Labed, V.*; Yamagishi, Isao
Journal of Nuclear Science and Technology, 58(1), p.62 - 71, 2021/01
The gas production of wasteforms is a major safety concern for encapsulating active nuclear wastes. For geopolymers and cements, the H produced by radiolytic processes is a key factor because of the large amount of water present in their porous structure. Herein, the gas composition evolution around geopolymers was monitored on line under Co gamma irradiation. Transient evolution of the hydrogen production yield was measured for samples with different formulations. The rate of its evolution and the final values are consistent with the presence of a chemical reaction of the pseudo-first order consuming hydrogen in the samples. The results show this phenomenon can significantly reduce the hydrogen source term of geopolymer wasteform provided their diffusion constant remains low. Lower hydrogen production rates and faster kinetics were observed with geopolymers formulations in which pore water pH was higher. Besides hydrogen production, a steady oxygen consumption was observed for all geopolymers samples. The oxygen consumption rates are proportional to the diffusion constants estimated in the modelization of hydrogen recombination by a pseudo first order reaction.
Cantarel, V.; Arisaka, Makoto; Yamagishi, Isao
Journal of the American Ceramic Society, 102(12), p.7553 - 7563, 2019/12
The hydrogen gas (H) production of wasteforms is a major safety concern for encapsulating nuclear wastes. For geopolymers, the H 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 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 (1.910 mol/J) than a sample in powder form (2.210 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.
Cantarel, V.; Arisaka, Makoto; Yamagishi, Isao
Proceedings of 3rd International Symposium on Cement-based Materials for Nuclear Wastes (NUWCEM 2018) (USB Flash Drive), 4 Pages, 2018/10
Geopolymers were successfully synthesized with different water content and loading of zeolites (0 to 40%wt). Zeolite A, geopolymer and their composites were then irradiated by a Co source (1.5 to 2.5 kGy/h) up to 10 kGy. The hydrogen was measured by GC after irradiation. Yields of radiolitic hydrogen were obtained for individual components. Obtained yields suggested a recombination process during irradiation. The system was then modelled to explain the observed behavior and predict the hydrogen production under ray irradiation of larger samples.
Cantarel, V.; Motooka, Takafumi; Yamagishi, Isao
JAEA-Review 2017-014, 36 Pages, 2017/06
After a necessary decay time, the zeolites used for the water decontamination will eventually be conditioned for their long-term storage. Geopolymer is considered as a potential matrix to manage radioactive cesium and strontium containing waste. For such applications, a correct comprehension of the binder structure, its macroscopic properties, its interactions with the waste and the physico-chemical phenomena occurring in the waste form is needed to be able to judge of the soundness and viability of the material. Although the geopolymer is a young binder, a lot of research has been carried out over the last fifty years and our understanding of this matrix and its potential applications is progressing fast. This review aims at gathering the actual knowledge on geopolymer studies about geopolymer composites, geopolymer as a confinement matrix for nuclear wastes and geopolymer under irradiation. This information will finally provide guidance for the future studies and experiments.
Morita, Yasuji; Yamagishi, Isao
JAEA-Research 2017-006, 27 Pages, 2017/06
Separation of Pd by extraction with 5,8-diethyl-7-hydroxy-6-dodecanone oxime (DEHDO) was examined by batch and continuous tests for the purpose of developing Pd separation process. Batch extraction tests using n-dodecane solution of DEHDO revealed that Pd, Zr and Mo were extracted from simulated high-level radioactive liquid wastes (HLLW) and other elements were not, and also showed that the extraction rate was a little slow and a white precipitate appeared in the aqueous phase but its formation could be avoided by raising temperature. The extracted Pd was found to be back-extracted with sodium nitrite. In the continuous extraction tests with simulated HLLW without Zr and Mo, about 98% of Pd were extracted with DEHDO-n-dodecane and 95% of the extracted Pd were back-extracted with sodium nitrite and nitric acid. Continuous extraction test with simulated HLLW with Zr and Mo showed the possibility of the simultaneous separation of Pd and Mo by DEHDO extraction.
Motooka, Takafumi; Yamagishi, Isao
JAEA-Review 2017-004, 157 Pages, 2017/03
Collaborative Laboratories for Advanced Decommissioning Science (CLADS) is responsible to promote international cooperation in the R&D activities on the decommissioning of Fukushima Daiichi Nuclear Power Station and to develop the necessary human resources. CLADS held the Research Conference on Post-accident Waste Management Safety (RCWM2016) was held on November 7th, 2016 and the Technical Seminar on Safety Research for Radioactive Waste Storage was held on November 8th, 2016. This report compiles the abstracts and the presentation materials in the above conference and seminar.
Motooka, Takafumi; Nagaishi, Ryuji; Yamagishi, Isao
QST-M-2; QST Takasaki Annual Report 2015, P. 95, 2017/03
We conducted ray irradiation test using simulated carbonate slurry to investigate the cause of stagnant water over the high integrity container (HIC). This test was performed at Co-60 irradiation facility in Takasaki Advanced Radiation Research Institute. We observed a rise in water level, air bubbles in the slurry, a supernatant when the carbonate slurry with 95 g/L density was irradiated by ray at a dose rate of 8.5 kGy/h. The cause of the rise in water level was regarded as the volume expansion by the gas retention of the carbonate slurry. It was suggested that the cause of stagnant water over the high integrity container might be the volume expansion by the gas retention.
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 -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.
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 HO 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 HO by the zeolites. A clear relationship was observed between ESP and the HO 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.
Kato, Chiaki; Sato, Tomonori; Nakano, Junichi; Ueno, Fumiyoshi; Yamagishi, Isao; Yamamoto, Masahiro
Nihon Genshiryoku Gakkai Wabun Rombunshi, 14(3), p.181 - 188, 2015/09
In relation to the consideration for long-term storage of spent Cs adsorption vessels containing zeolites in the Fukushima Daiichi Nuclear Power Station, corrosion of the vessel material in the spent Cs adsorption vessel is one of important issues. We performed electrochemical tests of stainless steel (SUS 316L) in the zeolites containing artificial seawater under -ray irradiation. The spontaneous potential () and critical pitting potential (), of SUS 316L were measured to understand the corrosion resistance of the stainless steel in this study. The rest potential of the stainless steel increased with increasing time after -ray irradiation. The , defined as the steady rest potential, increased with increasing dose rate, while increasing was suppressed by contact with the zeolites. Concentration of HO in bulk water increased with increasing dose rate. The concentration increasing was suppressed by contact with the zeolites due to decomposition of HO. There was good relationship between and the concentration of HO. The of SUS 316L contacted with the zeolites decreased with increasing Cl ion concentration and is slightly smaller than the in the bulk water. The contact with the zeolites causes the suppressant of increasing under the irradiation. The contact with the zeolite can reduce probability in the localized corrosion for SUS 316L.
Yamagishi, Isao; Odakura, Makoto; Ichige, Yoshiaki; Kuroha, Mitsuhiko; Takano, Masahide; Akabori, Mitsuo; Yoshioka, Masahiro*
Proceedings of 21st International Conference & Exhibition; Nuclear Fuel Cycle for a Low-Carbon Future (GLOBAL 2015) (USB Flash Drive), p.1113 - 1119, 2015/09
The characteristics of insoluble residues in fine suspension at the Rokkasho Reprocessing Plant were analyzed. The insoluble residues were washed with oxalic acid solution to dissolve zirconium molybdate residues. XRD profiles of unwashed residues showed the presence of a noble metal alloy, zirconium molybdate, and zirconia, but zirconium molybdate was not found after washing. More than 50% of the Sb-125 and Pu in thee residues was washed out as well. The noble metal alloy composed of Mo, Tc, Ru, Rh, and Pd occupied more than 90% of the total weight of 12 elements (Ca, Cr, Fe, Ni, Zr, Mo, Tc, Ru, Rh, Pd, Te, and U) found in the residues. In consideration of the chemical forms of 12 elements, the alloy-to-residue weight ratio was evaluated to be 64% and 78% with and without 18% of an unknown component, respectively.
Kato, Chiaki; Sato, Tomonori; Ueno, Fumiyoshi; Yamagishi, Isao; Yamamoto, Masahiro
Zairyo To Kankyo 2015 Koenshu (CD-ROM), p.83 - 86, 2015/05
In relation to the consideration for long-term storage of spent Cs adsorption vessels containing zeolites in the Fukushima Daiichi Nuclear Power Station, corrosion of the vessel material in the spent Cs adsorption vessel is one of important issues. We performed electrochemical tests of stainless steel (SUS 316L) in the zeolites containing artificial seawater under gamma-ray irradiation. The spontaneous potential (ESP) and critical pitting potential (VC), of SUS316L were measured to understand the corrosion resistance of the stainless steel in this study. The rest potential of the stainless steel increased with increasing time after gamma-ray irradiation. The ESP, defined as the steady rest potential, increased with increasing dose rate, while increasing ESP was suppressed by contact with the zeolites. Concentration of HO in bulk water increased with increasing dose rate. The concentration increasing was suppressed by contact with the zeolites due to decomposition of HO. There was good relationship between ESP and the concentration of HO. The VC of SUS316L contacted with the zeolites decreased with increasing Cl ion concentration and is slightly smaller than the VC in the bulk water. The contact with the zeolites causes the suppressant of increasing ESP under the irradiation. The contact with the zeolites can reduce probability in the localized corrosion for SUS316L.
Nishihara, Kenji; Yamagishi, Isao; Yasuda, Kenichiro; Ishimori, Kenichiro; Tanaka, Kiwamu; Kuno, Takehiko; Inada, Satoshi; Goto, Yuichi
Journal of Nuclear Science and Technology, 52(3), p.301 - 307, 2015/03
After the severe accident at the Fukushima-1 nuclear power plant, large amounts of contaminated stagnant water have accumulated in turbine buildings and their surroundings. This rapid communication reports calculation of the radionuclide inventory in the core, collection of measured inventory in the stagnant water, and estimation of radionuclide release ratios from the core to the stagnant water. This evaluation is based on data obtained before June 3, 2011. The release ratios of tritium, iodine, and cesium were several tens of percent, whereas those of strontium and barium were smaller by one or two orders of magnitude. The release ratios in the Fukushima accident were equivalent to those in the TMI-2 accident.
Mimura, Hitoshi*; Yamagishi, Isao
Zeoraito, 31(4), p.115 - 124, 2014/12
Massive tsunami caused by the Great East Japan Earthquake attacked the Fukushima Daiichi Nuclear Power Plant and caused the nuclear accident of level 7 to overturn the safety myth of nuclear power generation. The domestic worst accident does not yet reach the convergence, and many inhabitants around the power plant are forced to double pains of earthquake disaster and nuclear accident. At present, large amounts of high-activity-level water over 500,000 tons are stored in Fukushima NPP-1 site, which is a serious obstacle to take measures for the nuclear accident. For the decontamination of high-activity-level water containing seawater, the circulating injection cooling system using packed columns with inorganic ion-exchangers is operated and the cold shutdown is accomplished. However, the advancement of operating system and the safety management of secondary solid wastes are very important subject. In this paper, the adsorption properties and solidification characteristics are compared for Cs and Sr selective adsorbents mainly composed of zeolites and the enhancement of adsorption properties are reported. Especially, naturally occurring zeolites abundant in Japan have high selectivity towards Cs, and also have excellent functions of gas trapping and self sintering for stable solidification. Zeolites are thus expected for the treatment and disposal of contaminated water in future. This paper also reports the present situation of safety management of solid wastes and the development of stable solidification methods, and summarizes the future subjects considering the safety disposal.
Morita, Keisuke; Yamagishi, Isao; Nishihara, Kenji; Tsubata, Yasuhiro
Proceedings of 2014 Nuclear Plant Chemistry Conference (NPC 2014) (USB Flash Drive), 11 Pages, 2014/10
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.
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 -ray irradiation. Steady spontaneous potential (Esp) and pitting potential (VC), of type 316L was measurement. Co -rays source was used under irradiation. Dose rate of -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 -ray irradiation. The Esp was shifted to nobler by -rays irradiation, while increasing Esp was suppressed by contacted with zeolite.
Yamagishi, Isao; Nagaishi, Ryuji; Kato, Chiaki; Morita, Keisuke; Terada, Atsuhiko; Kamiji, Yu; Hino, Ryutaro; Sato, Hiroyuki; Nishihara, Kenji; Tsubata, Yasuhiro; et al.
Journal of Nuclear Science and Technology, 51(7-8), p.1044 - 1053, 2014/07
For safe storage of zeolite wastes generated by treatment of radioactive saline water at the Fukushima Daiichi Nuclear Power Station, properties of the Herschelite adsorbent were studied and its adsorption vessel was evaluated for hydrogen production and corrosion. Hydrogen production depends on its water level and dissolved species because hydrogen is oxidized by radicals in water. It is possible to evaluate hydrogen production rate in Herschelite submerged in seawater or pure water by taking into account of the depth effect of the water. The reference vessel of decay heat 504 W with or without residual pure water was evaluated for the hydrogen concentration by thermal hydraulic analysis using obtained fundamental properties. Maximum hydrogen concentration was below the lower explosive limit (4 %). The steady-state corrosion potential of a stainless steel 316L increased with absorbed dose rate but its increase was repressed by the presence of Herschelite. At 750 Gy/h and 60C which were values evaluated at the bottom of the vessel of 504 W, the localized corrosion of SUS316L contacted with Herschelite would not immediately occur under 20,000 ppm of Cl concentration.