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JAEA Reports

Development of stable solidification technique of ALPS sediment wastes by apatite ceramics (Contract research); FY2021 Nuclear Energy Science & Technology and Human Resource Development Project

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

JAEA-Review 2022-076, 227 Pages, 2023/03

JAEA-Review-2022-076.pdf:9.42MB

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 FY2021. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station (1F), 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 FY2019, this report summarizes the research results of the "Development of stable solidification technique of ALPS sediment wastes by apatite ceramics" conducted from FY2019 to FY2021. Since the final year of this proposal was FY2021, the results for three fiscal years were summarized. The present study aims to establish an apatite solidification process of radioactive sediment wastes, which were generated from the ALPS process manipulating the large amount of contaminated water from 1F. We selected the precipitation method and post stabilization for engineering-scale process. Investigation on composition, structure and elution properties of apatite and related phosphate waste forms fabricated from the simulated ALPS sediment wastes were implemented.

Journal Articles

Deep groundwater physicochemical components affecting actinide migration

Kirishima, Akira*; Terasaki, Mariko*; Miyakawa, Kazuya; Okamoto, Yoshihiro; Akiyama, Daisuke*

Chemosphere, 289, p.133181_1 - 133181_12, 2022/04

https://doi.org/10.1016/j.chemosphere.2021.133181

Times Cited Count：1 Percentile：5.8(Environmental Sciences)

no abstracts in English

Journal Articles

Structural characterization by X-ray analytical techniques of calcium aluminate cement modified with sodium polyphosphate containing cesium chloride

Takahatake, Yoko; Watanabe, So; Irisawa, Keita; Shiwaku, Hideaki; Watanabe, Masayuki

Journal of Nuclear Materials, 556, p.153170_1 - 153170_7, 2021/12

https://doi.org/10.1016/j.jnucmat.2021.153170

Times Cited Count：1 Percentile：15.7(Materials Science, Multidisciplinary)

Journal Articles

Adsorption behavior of cesium on hybrid microcapsules in spent fuel solution

Onishi, Takashi; Koyama, Shinichi; Mimura, Hitoshi*

Nihon Ion Kokan Gakkai-Shi, 31(3), p.43 - 49, 2020/10

https://doi.org/10.5182/jaie.31.43

Journal Articles

Influence of mixing solution on characteristics of calcium aluminate cement modified with sodium polyphosphate

Irisawa, Keita; Garcia-Lodeiro, I.*; Kinoshita, Hajime*

Cement and Concrete Research, 128, p.105951_1 - 105951_7, 2020/02

https://doi.org/10.1016/j.cemconres.2019.105951

Times Cited Count：7 Percentile：35(Construction & Building Technology)

This study investigated characteristics of a calcium aluminate cement modified with a phosphate (CAP) by changing an amount and concentration of mixing solution with sodium polyphosphate. When the amount of mixing solution was increased with a constant amount of sodium polyphosphate, an enhanced consumption of monocalcium aluminate was observed compared with gehlenite in calcium aluminate cement (CAC). Formation of gibbsite, Al(OH) $_{3}$ , was also increased as a hydration product in the CAP and the possible reduction of water in the amorphous gel phase. When the amount of mixing solution was increased with a constant concentration of sodium polyphosphate, the enhanced consumption of monocalcium aluminate was not observed. Neither gibbsite nor any other crystalline hydration products were identified in this series. In addition, unreacted sodium polyphosphate remained in the system. The increased formation of gibbsite and the possible reduction of water from the amorphous gel phase appears to contribute to the improvement of the microstructure in the products.

Journal Articles

Development of phosphate modified CAC cementitious systems with reduced water content for the immobilization of radioactive wastes

Garcia-Lodeiro, I.*; Irisawa, Keita; Meguro, Yoshihiro; Kinoshita, Hajime*

Proceedings of 15th International Congress on the Chemistry of Cement (ICCC 2019) (Internet), 10 Pages, 2019/09

The immobilization of low or intermediate-level radioactive wastes in cements is a common practise. Grout, a mixture of Portland cement and supplemental cementitious materials, is commonly used to encapsulate the wastes. However, the conventional cementing process based on portland cement has the risk of hydrogen gas generation, due to the radiolysis of the water intrinsically present in the cement matrix both in the pore solution and the hydrated products. The addition of phosphates to calcium aluminate cement (CAC) is interesting because this system sets and hardens via the acid-based reaction, between the acid phosphate solution and the basic CAC cement. Due to this different mechanism of reaction, it would be possible to generate a solid cementitious product with a reduced water content, which can be beneficial to minimize the risk of hydrogen gas generation associated with the radiolysis of water by radioactive wastes. The present study investigates the effect of water reduction on a phosphate modified CAC systems at different temperatures (35 $^{circ}$ C, 60 $^{circ}$ C, 95 $^{circ}$ C, 110 $^{circ}$ C,180 $^{circ}$ C) in the initial 7 days of curing. Experimental results indicate that these phosphate-based cements do not form the conventional CAC crystalline hydration products in the condition tested, but provide a structural integrity despite a significant amount of water loss. The results also suggest the formation of hydroxyapatite in samples cured at 95 $^{circ}$ C.

Journal Articles

Application of phosphate modified CAC for incorporation of simulated secondary aqueous wastes in Fukushima Daiichi NPP, 1; Characterization of solidified cementitious systems with reduced water content

Garcia-Lodeiro, I.*; Lebon, R.*; Machoney, D.*; Zhang, B.*; Irisawa, Keita; Taniguchi, Takumi; Namiki, Masahiro*; Osugi, Takeshi; Meguro, Yoshihiro; Kinoshita, Hajime*

Proceedings of 3rd International Symposium on Cement-based Materials for Nuclear Wastes (NUWCEM 2018) (USB Flash Drive), 4 Pages, 2018/11

Journal Articles

Reduction of water content in calcium aluminate cement with/out phosphate modification for alternative cementation technique

Garcia-Lodeiro, I.*; Irisawa, Keita; Jin, F.*; Meguro, Yoshihiro; Kinoshita, Hajime*

Cement and Concrete Research, 109, p.243 - 253, 2018/07

https://doi.org/10.1016/j.cemconres.2018.04.019

Times Cited Count：26 Percentile：68.65(Construction & Building Technology)

Journal Articles

Heat treatment of phosphate-modified cementitious matrices for safe storage of secondary radioactive aqueous wastes in Fukushima Daiichi Nuclear Power Plant

Irisawa, Keita; Taniguchi, Takumi; Namiki, Masahiro; Garca-Lodeiro, I.*; Osugi, Takeshi; Sakakibara, Tetsuro; Nakazawa, Osamu; Meguro, Yoshihiro; Kinoshita, Hajime*

Proceedings of 2017 International Congress on Advances in Nuclear Power Plants (ICAPP 2017) (CD-ROM), 6 Pages, 2017/04

A solidification technique with minimized water content is being developed using phosphate cements for the safe storage of secondary radioactive wastes in the Fukushima Daiichi Nuclear Power Plant. Conventional cement systems become solidified via hydration reactions, and need a certain water content. Phosphate cement systems, however, become solidified via an acid-base reaction, and so they only require water mainly for reasons of workability. A reduced water content of phosphate cement systems is beneficial for the immobilization of the radioactive wastes from mitigating the potential to generate hydrogen gas by the radiolysis of water by radioactive wastes. The current study investigated the water content and mineralogy of calcium aluminate cement (CAC) and phosphate-modified CAC (CAP) cured in open systems at 60, 90 and 120 $^{circ}$ C and in a closed system at 20 $^{circ}$ C as a reference case. Water contents in both the CAC and the CAP were seen to decrease as curing progressed. For 90 $^{circ}$ C, the CAP contained less water than CAC. Free water in CAC converted to structural water by heat treatment, but this was not the case for CAP. An orthophosphate hydrate salt, a precursor phase of hydroxyapatite, was found in CAP when cured at 20 and 60 $^{circ}$ C, and a mixture of the orthophosphate hydrate salt and hydroxyapatite, Ca $_{10}$ (PO $_{4}$ ) $_{6}$ (OH) $_{2}$ , were formed in the CAP when cured at 90 $^{circ}$ C. Phosphate products in CAP cured at 120 $^{circ}$ C appears to consist of a different phosphate phase compared with the CAP cured at 20, 60 and 90 $^{circ}$ C.

Journal Articles

Research on vitrification technology to immobilize radioactive sludge generated from Fukushima Daiichi Power Plant; Enhanced glass medium

Amamoto, Ippei; Kobayashi, Hidekazu; Kitamura, Naoto*; Takebe, Hiromichi*; Mitamura, Naoki*; Tsuzuki, Tatsuya*; Fukayama, Daigen*; Nagano, Yuichi*; Jantzen, T.*; Hack, K.*

Journal of Nuclear Science and Technology, 53(10), p.1467 - 1475, 2016/10

https://doi.org/10.1080/00223131.2015.1136579

Times Cited Count：4 Percentile：28.09(Nuclear Science & Technology)

The iron phosphate glass (IPG) medium is known to be a high-efficiency glass medium, therefore we try to evaluate its applicability to immobilize sludge bearing radioactive nuclides arising from treatment of contaminated water at the stricken Fukushima Daiichi Nuclear Power Plant. For this study, many physical and chemical properties of target materials are necessary to evaluate the behaviours of IPG medium and its waste forms. Inevitably, it will entail the need for many and varied types of experiments to be carried out under high temperature. It is therefore rational to apply appropriate theoretical analysis first so as to reduce the number of experimental run. For this reason, some necessary thermodynamic values for theoretical analysis were estimated by CALPHAD approach followed by making up the calculated phase diagrams. By comparison with experimental results, they were found to be reliable for evaluating the behaviours of IPG medium and its waste forms.

Journal Articles

The Spectrum and laser properties of ytterbium doped phosphate glass at low temperature

Dai, S.*; Sugiyama, Akira; Hu, L.*; Liu, Z.*; Huang, G.*; Jiang, Z.*

Journal of Non-Crystalline Solids, 311(2), p.138 - 144, 2002/11

https://doi.org/10.1016/S0022-3093(02)01365-0

Low-temperature absorption and fluorescence spectra of the Yb3+ ions were measured in phosphate glass with compositions of (60-65)P $_{2}$ O $_{5}$ -(4-8)B $_{2}$ O $_{3}$ -(5-10)Al $_{2}$ O $_{3}$ -(10-15)K $_{2}$ O-(5-10)BaO-(0-2)La $_{2}$ O $_{3}$ -(0-2)Nb $_{2}$ O $_{5}$ -(4-87)Yb $_{2}$ O $_{3}$ in mol-%. Temperature dependence of lifetime from $^{2}$ F $_{5/2}$ upper level of YB $^{3+}$ was investigated with a cryostat. The glass laser performance pumped by 940 nm laser diode was measured at different temperature range. At 8 K, glass laser oscillation had a slope efficiency of 4% and a maximum power of 2 mW at the peak laser wavelength of 1001 nm.

Journal Articles

Study of a new ytterbium doped phosphate laser glass

Dai, S.*; Hu, L.*; Sugiyama, Akira; Izawa, Yasukazu*; Liu, Z.*; Jiang, Z.*

Chinese Science Bulletin, 47(3), p.255 - 259, 2002/02

https://doi.org/10.1360/02tb9062

Times Cited Count：7 Percentile：51.71(Multidisciplinary Sciences)

A new type of ytterbium doped phosphate laser glass has been produced and studied about physical and optical properties such as thermo-mechanical properties, nonlinear properties, crystalline phase, micro defects and spectroscopic properties. In the glass forming process, newly developed OH removing technology was adopted. From the reduction of OH concentration in the glass, upper state fluorescence lifetime reached 2.2 ms. Additionally, the glass shows remarkable athermal property of 0.4210E $^{-6}$ /K, which is around one-tenth of QX/Yb glass.