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Journal Articles

Study on the relation between the crystal structure and thermal stability of FeUO$$_{4}$$ and CrUO$$_{4}$$

Akiyama, Daisuke*; Kusaka, Ryoji; Kumagai, Yuta; Nakada, Masami; Watanabe, Masayuki; Okamoto, Yoshihiro; Nagai, Takayuki; Sato, Nobuaki*; Kirishima, Akira*

Journal of Nuclear Materials, 568, p.153847_1 - 153847_10, 2022/09

FeUO$$_{4}$$, CrUO$$_{4}$$, and Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ are monouranates containing pentavalent U. Even though these compounds have similar crystal structures, their formation conditions and thermal stability are significantly different. To determine the factors causing the difference in thermal stability between FeUO$$_{4}$$ and CrUO$$_{4}$$, their crystal structures were evaluated in detail. A Raman band was observed at 700 cm$$^{-1}$$ in all the samples. This Raman band was derived from the stretching vibration of the O-U-O axis band, indicating that Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ was composed of a uranyl-like structure in its lattice regardless of its "x"' value. M$"o$ssbauer measurements indicated that the Fe in FeUO$$_{4}$$ and Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ were trivalent. Furthermore, Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ lost its symmetry around Fe$$^{mathrm{III}}$$ with increasing electron densities around Fe$$^{mathrm{III}}$$, as the abundance of Cr increased. These results suggested no significant structural differences between FeUO$$_{4}$$ and CrUO$$_{4}$$. Thermogravimetric measurements for UO$$_{2}$$, FeUO$$_{4}$$, and CrUO$$_{4}$$ showed that the temperature at which FeUO$$_{4}$$ decomposed under an oxidizing condition (approximately 800 $$^{circ}$$C) was significantly lower than the temperature at which the decomposition of CrUO$$_{4}$$ started (approximately 1250 $$^{circ}$$C). Based on these results, we concluded that the decomposition of FeUO$$_{4}$$ was triggered by an ``in-crystal'' redox reaction, i.e., Fe$$^{mathrm{III}}$$ $${+}$$ U$$^{mathrm{V}}$$ $$rightarrow$$ Fe$$^{mathrm{II}}$$ $${+}$$ U$$^{mathrm{VI}}$$, which would not occur in the CrUO$$_{4}$$ lattice because Cr$$^{mathrm{III}}$$ could never be reduced under the investigated condition. Finally, the existence of Cr$$^{mathrm{III}}$$ in FexCr$$_{1-x}$$UO$$_{4}$$ effectively suppressed the decomposition of the Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ crystal, even at a very low Cr content.

Journal Articles

Irradiation growth behavior and effect of hydrogen absorption of Zr-based cladding alloys for PWR

Kakiuchi, Kazuo; Amaya, Masaki; Udagawa, Yutaka

Annals of Nuclear Energy, 171, p.109004_1 - 109004_9, 2022/06

 Times Cited Count:0 Percentile:0.02(Nuclear Science & Technology)

Journal Articles

Predictive modeling of a simple field matrix diffusion experiment addressing radionuclide transport in fractured rock. Is it so straightforward?

Soler, J. M.*; Neretnieks, I.*; Moreno, L.*; Liu, L.*; Meng, S.*; Svensson, U.*; Iraola, A.*; Ebrahimi, K.*; Trinchero, P.*; Molinero, J.*; et al.

Nuclear Technology, 208(6), p.1059 - 1073, 2022/06

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

The SKB Task Force is an international forum on modelling of groundwater flow and solute transport in fractured rock. The WPDE experiments are matrix diffusion experiments in gneiss performed at the ONKALO underground facility in Finland. Synthetic groundwater containing several conservative and sorbing tracers was injected along a borehole interval. The objective of Task 9A was the predictive modelling of the tracer breakthrough curves from the WPDE experiments. Several teams, using different modelling approaches and codes, participated in this exercise. An important conclusion from this exercise is that the modelling results were very sensitive to the magnitude of dispersion in the borehole opening, which is related to the flow of water. Focusing on the tails of the breakthrough curves, which are more directly related to matrix diffusion and sorption, the results from the different teams were more comparable.

Journal Articles

Sorption of Cs$$^{+}$$ and Eu$$^{3+}$$ ions onto sedimentary rock in the presence of gamma-irradiated humic acid

Zhao, Q.*; Saito, Takeshi*; Miyakawa, Kazuya; Sasamoto, Hiroshi; Kobayashi, Taishi*; Sasaki, Takayuki*

Journal of Hazardous Materials, 428, p.128211_1 - 128211_10, 2022/04

 Times Cited Count:0 Percentile:0.01(Engineering, Environmental)

The influence of humic acid and its radiological degradation on the sorption of Cs$$^{+}$$ and Eu$$^{3+}$$ by sedimentary rock was investigated to understand the sorption process of metal ions and humic substances. Aldrich humic acid (HA) solution was irradiated with different doses of gamma irradiation using a Co-60 gamma-ray source prior to the contact between the metal ions and the solid sorbent. The HA molecule decomposed to smaller molecules with a lower complexation affinity. Batch sorption experiments were performed to evaluate the effect of gamma-irradiated HA on the sorption of Cs$$^{+}$$ and Eu$$^{3+}$$ ions. The addition of non-irradiated HA weakened the sorption of Eu because of the lower sorption of the neutral or negatively charged Eu-HA complexes compared with free Eu ions. The sorption of monovalent Cs ions was barely affected by the presence of HA and its gamma irradiation. The concentration ratio of HA complexed species and non-complexed species in the solid and liquid phases was evaluated by sequential filtration and chemical equilibrium calculations. The ratios supported the minimal contribution of HA to Cs sorption. However, the concentration ratio for Eu$$^{3+}$$ in the liquid phase was high, indicating that the complexing ability of HA to Eu$$^{3+}$$ was higher than that of HA to Cs$$^{+}$$ ions. Therefore, the sorption of free Eu$$^{3+}$$ would predominate with the gamma irradiation dose applied to the HA solution under a radiation field near the HLW package.

JAEA Reports

Development of JAEA sorption database (JAEA-SDB); Update of sorption/QA data in FY2021

Sugiura, Yuki; Suyama, Tadahiro*; Tachi, Yukio

JAEA-Data/Code 2021-017, 58 Pages, 2022/03

JAEA-Data-Code-2021-017.pdf:1.98MB

Sorption behavior of radionuclides (RNs) in buffer materials (bentonites), rocks and cementitious materials is one of the key processes in a safe geological disposal of radioactive waste because RNs migration in these materials is expected to be retarded by the sorption process. Therefore, it is necessary to understand the sorption process and develop a database compiling reliable data and mechanistic/predictive models so that reliable parameters can be set under a variety of geochemical conditions relevant to a performance assessment (PA). For this purpose, Japan Atomic Energy Agency (JAEA) has developed the database of sorption parameters in bentonites, rocks and cementitious materials. This sorption database (SDB) was firstly developed as an important basis for the H12 PA of a high-level radioactive waste disposal, and have been provided through the Web. JAEA has continued to improve and update the SDB in the view of potential future needs of data focusing on assuring the desired quality level and testing the usefulness of the databases for possible applications to the PA-related parameter setting. This report focuses on updating of the sorption database (JAEA-SDB) as a basis of integrated approach for the PA-related distribution coefficient (Kd) setting and development of mechanistic sorption models. This report also includes an overview of the database structure and contents. Kd data and their quality assurance (QA) results were updated from literature collected with wider ranges. As a result, 8,503 Kd data from 70 references related to the above-mentioned systems were added and the total number of Kd values in JAEA-SDB reached 79,072. The QA/classified Kd data reached about 75.4% for all Kd data in JAEA-SDB. The updated JAEA-SDB is expected to make it possible to give a basis for the next-step PA-related Kd setting.

JAEA Reports

Quantitative evaluation of long-term state changes of contaminated reinforced concrete considering the actual environments for rational disposal (Contract research); FY2020 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; The University of Tokyo*

JAEA-Review 2021-047, 127 Pages, 2022/01

JAEA-Review-2021-047.pdf:5.57MB

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 "Quantitative evaluation of long-term state changes of contaminated reinforced concrete considering the actual environments for rational disposal" conducted in FY2020. The present study aims to construct a database for quantitative prediction of contaminated reinforced concrete inside the reactor building. In FY2020, in chapter 3.1, in order to obtain the data for the evaluation of mesoscale cracking behavior, the equipment for the making and the measurement of the test specimens were prepared, the evaluation method was confirmed, and preliminary experiments were carried out. And, for the prediction of cracking on the surface of thick concrete wall, the rigid-body spring network model associated with heat and moisture

Journal Articles

Decrease of radionuclide sorption in hydrated cement systems by organic ligands; Comparative evaluation using experimental data and thermodynamic calculations for ISA/EDTA-actinide-cement systems

Ochs, M.*; Dolder, F.*; Tachi, Yukio

Applied Geochemistry, 136, p.105161_1 - 105161_11, 2022/01

 Times Cited Count:0 Percentile:0.01(Geochemistry & Geophysics)

Various types of radioactive wastes and environments contain organic substances that can stabilize the aqueous complexes with radionuclides and therefore lead to a decrease of sorption. The present study focuses on testing a methodology to quantify sorption reduction factors (SRFs) in the presence of organic ligands for cement systems. Three approaches for the estimation of SRFs; (1) analogy with solubility enhancement factors, (2) radionuclide speciation based on the thermodynamic calculations, and (3) experimental sorption data in ternary systems, were coupled and tested for the representative organic ligands (ISA and EDTA) and selected key radionuclides (actinides). Our approach allows to critically evaluate the dependence of SRFs for various systems on the chosen method of quantification, in accordance with the data availability for a given systems. The reliable SRFs can only be derived from the sorption measurements in ternary systems. SRF often need to be derived in the absence of such direct evidence, and estimations need to be made based on analogies and speciation information. However, such estimates may be subject to substantial uncertainties.

Journal Articles

Chemical interaction between Sr vapor species and nuclear reactor core structure

Mohamad, A. B.; Nakajima, Kunihisa; Miwa, Shuhei; Osaka, Masahiko

Journal of Nuclear Science and Technology, 8 Pages, 2022/00

 Times Cited Count:0

Journal Articles

A Scaling approach for retention properties of crystalline rock; Case study of the in-situ long-term sorption and diffusion experiment (LTDE-SD) at the $"A$sp$"o$ Hard Rock Laboratory in Sweden

Tachi, Yukio; Ito, Tsuyoshi*; Gylling, B.*

Water Resources Research, 57(11), 20 Pages, 2021/11

 Times Cited Count:0 Percentile:0.04(Environmental Sciences)

This paper focuses on the scaling approach for sorption and diffusion parameters from laboratory to in-situ conditions using the dataset of LTDE-SD experiment performed at the $"A$sp$"o$ HRL. The near-surface heterogeneities at both fracture surface and rock matrix could be evaluated by conceptual model with high porosity and diffusivity, and sorption capacity, and their gradual change at the near-surface zones. The modelling results for non-sorbing Cl-36 and weak-sorbing Na-22 could validate the model concept and the parameter estimation of porosity and diffusivity, by considering the disturbed zone of 5 mm thickness with gradual parameter changes. The De values of these cationic and anionic tracers showed typical cation excess and anion exclusion effects. The modelling results for high sorbing tracers (Cs-137, Ra-226, Ni-63 and Np-237) with different sorption mechanism could confirm the validity of the scaling approaches of Kd values as a function of particle size and their relation to the near-surface disturbances.

Journal Articles

Experimental study on modeling of Pu sorption onto quartz

Hemmi, Ko; Walker, A.*; Yamaguchi, Tetsuji

Radiochimica Acta, 109(7), p.539 - 546, 2021/07

 Times Cited Count:0 Percentile:0.01(Chemistry, Inorganic & Nuclear)

Plutonium(IV) sorption onto quartz in carbonate solutions was systematically investigated under anaerobic conditions to analyze the sorption behaviors of Pu(IV) with a non-electrostatic model (NEM). Pu(IV) sorption data was obtained from batch sorption experiments as a function of pH and carbonate concentration. The Pu(IV) sorption onto quartz showed similar tendencies to Th(IV), which is considered to be chemically analogous as a tetravalent actinoid. The distribution coefficient, ${it K}$d, of Pu(IV) onto quartz showed inverse proportionality to the square of the total carbonate concentration under the investigated pH conditions of 8 to 11. The modeling study, however, revealed a Th(IV) sorption model, which is $$equiv$$SOTh(OH)$$_{4}$$$$^{-}$$ and $$equiv$$SOThOH(CO$$_{3}$$)$$_{2}$$$$^{2-}$$, could not be applied to simulate the Pu(IV) sorption onto quartz. It was inferred that the electrostatic repulsion between negatively charged ligands limited the formation of $$equiv$$SOM(OH)$$_{4}$$$$^{-}$$ and $$equiv$$SOMOH(CO$$_{3}$$)$$_{2}$$$$^{2-}$$ for Pu(IV) with smaller ionic radii than Th(IV). The Pu(IV) sorption model was developed as $$equiv$$SOPu(OH)$$_{3}$$ and $$equiv$$SOPu(OH)$$_{4}$$$$^{-}$$. In addition, data of Pu(IV) sorption onto muscovite was obtained in order to be compared with data for quartz.

Journal Articles

Evaluation report of Task 9B based on comparisons and analyses of modelling results for the $"A$sp$"o$ HRL LTDE-SD experiments

Soler, J. M.*; Meng, S.*; Moreno, L.*; Neretnieks, I.*; Liu, L.*; Kek$"a$l$"a$inen, P.*; Hokr, M.*; $v{R}$$'i$ha, J.*; Vete$v{s}$n$'i$k, A.*; Reimitz, D.*; et al.

SKB TR-20-17, 71 Pages, 2021/07

Task 9B of the SKB Task Force on Modelling of Groundwater Flow and Transport of Solutes in fractured rock focused on the modelling of experimental results from the LTDE-SD in situ tracer test performed at the $"A$sp$"o$ Hard Rock Laboratory in Sweden. Ten different modelling teams provided results for this exercise, using different concepts and codes. Three main types of modelling approaches were used: (1) analytical solutions to the transport-retention equations, (2) continuum-porous-medium numerical models, and (3) microstructure-based models accounting for small-scale heterogeneity (i.e. mineral grains and microfracture distributions). The modelling by the different teams allowed the comparison of many different model concepts, especially in terms of potential zonations of rock properties (porosity, diffusion, sorption), such as the presence of a disturbed zone at the rock and fracture surface, the potential effects of micro- and cm-scale fractures.

Journal Articles

Microparticles with diverse sizes and morphologies from mechanical and laser cutting of fuel debris simulants and geopolymer as a covering material

Zhou, Q.*; Saito, Takumi*; Suzuki, Seiya; Yano, Kimihiko; Suzuki, Shunichi*

Journal of Nuclear Science and Technology, 58(4), p.461 - 472, 2021/04

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

JAEA Reports

Investigation and consideration on evaluation of radiation doses to residents in the case of a nuclear emergency

Hashimoto, Makoto; Kinase, Sakae; Munakata, Masahiro; Murayama, Takashi; Takahashi, Masa; Takada, Chie; Okamoto, Akiko; Hayakawa, Tsuyoshi; Sukegawa, Masato; Kume, Nobuhide*; et al.

JAEA-Review 2020-071, 53 Pages, 2021/03

JAEA-Review-2020-071.pdf:2.72MB

In the case of a nuclear accident or a radiological emergency, the Japan Atomic Energy Agency (JAEA), as a designated public corporation assigned in the Disaster Countermeasures Basic Act and the Armed Attack Situation Response Law, undertakes technical supports to the national government and local governments. The JAEA is requested to support to evaluate radiation doses to residents in a nuclear emergency, which is specified in the Basic Disaster Management Plan and the Nuclear Emergency Response Manual. For the dose evaluation, however, its strategy, target, method, structure and so on have not been determined either specifically or in detail. This report describes the results of investigation and consideration discussed in the "Working Group for Radiation Dose Evaluation at a Nuclear Emergency" established within the Nuclear Emergency Assistance and Training Center to discuss technical supports for radiation dose evaluation to residents in the case of a nuclear emergency, and aims at contributing to specific and detailed discussion and activities in the future for the national government and local governments, also within the JAEA.

Journal Articles

Incorporation of U, Pb and rare earth elements in calcite through crystallisation from amorphous calcium carbonate; Simple preparation of reference materials for microanalysis

Miyajima, Yusuke*; Saito, Ayaka*; Kagi, Hiroyuki*; Yokoyama, Tatsunori; Takahashi, Yoshio*; Hirata, Takafumi*

Geostandards and Geoanalytical Research, 45(1), p.189 - 205, 2021/03

 Times Cited Count:2 Percentile:28.61(Geochemistry & Geophysics)

Uncertainty for elemental and isotopic analyses of calcite by LA-ICP-MS is largely controlled by the homogeneity of the reference materials (RMs) used for normalization and validation. In order to produce calcite RMs with homogeneous elemental and isotopic compositions, we incorporated elements including U, Pb, and rare earth elements into calcite through heat- and pressure-induced crystallization from amorphous calcium carbonate that was precipitated from element-doped reagent solution. X-ray absorption spectra showed that U was present as U(VI) in the synthesized calcite, probably with a different local structure from that of aqueous uranyl ions. The uptake rate of U by our calcite was higher in comparison to synthetic calcite of previous studies. Variations of element mass fractions in the calcite were better than 12% 2RSD, mostly within 7%. The $$^{207}$$Pb/$$^{206}$$Pb ratio in the calcite showed $$<$$1% variations, while the $$^{238}$$U/$$^{206}$$Pb ratio showed 3-24% variations depending on element mass fractions. Using the synthetic calcite as primary RMs, we could date a natural calcite RM, WC-1, with analytical uncertainty as low as $$<$$3%. The method presented can be useful to produce calcite with controlled and homogeneous element mass fractions, and is a promising alternative to natural calcite RMs for U-Pb geochronology.

Journal Articles

Consideration on modeling of Nb sorption onto clay minerals

Yamaguchi, Tetsuji; Ohira, Saki; Hemmi, Ko; Barr, L.; Shimada, Asako; Maeda, Toshikatsu; Iida, Yoshihisa

Radiochimica Acta, 108(11), p.873 - 877, 2020/11

 Times Cited Count:0 Percentile:0.01(Chemistry, Inorganic & Nuclear)

Journal Articles

Key factors controlling radiocesium sorption and fixation in river sediments around the Fukushima Daiichi Nuclear Power Plant, 2; Sorption and fixation behaviors and their relationship to sediment properties

Tachi, Yukio; Sato, Tomofumi*; Takeda, Chizuko*; Ishidera, Takamitsu; Fujiwara, Kenso; Iijima, Kazuki

Science of the Total Environment, 724, p.138097_1 - 138097_10, 2020/07

 Times Cited Count:7 Percentile:59.98(Environmental Sciences)

To understand and predict radiocesium transport behaviors in the environment, sorption and fixation behaviors of radiocesium on river sediments from Ukedo and Odaka rivers around the Fukushima Daiichi Nuclear Power Plant were investigated systematically focusing on Cs sorption and fixation mechanisms and their relationship with Cs concentrations and sediment properties including clay mineralogy and organic matter.

Journal Articles

Development of fission product chemistry database ECUME for the LWR severe accident

Miwa, Shuhei; Nakajima, Kunihisa; Miyahara, Naoya; Nishioka, Shunichiro; Suzuki, Eriko; Horiguchi, Naoki; Liu, J.; Miradji, F.; Imoto, Jumpei; Afiqa, B. M.; et al.

Mechanical Engineering Journal (Internet), 7(3), p.19-00537_1 - 19-00537_11, 2020/06

We constructed the fission product (FP) chemistry database named ECUME for LWR severe accident. This version of ECUME is equipped with dataset of the chemical reactions and their kinetics constants for the reactions of cesium(Cs)-iodine(I)-boron(B)-molybdenum(Mo)-oxygen(O)-hydrogen(H) system in gas phase, the elemental model for the high temperature chemical reaction of Cs with stainless steel applied as the structural material in a reactor, and thermodynamic data for CsBO$$_{2}$$ vapor species and solids of Cs$$_{2}$$Si$$_{4}$$O$$_{9}$$ and CsFeSiO$$_{4}$$ for these chemical reactions. The ECUME will provide estimation of Cs distribution due to the evaluation of effects of interaction with BWR control material B and stainless steel on Cs behavior in the Fukushima Daiichi Nuclear Power Station.

Journal Articles

Study on chemisorption model of cesium hydroxide onto stainless steel type 304

Nakajima, Kunihisa; Nishioka, Shunichiro*; Suzuki, Eriko; Osaka, Masahiko

Mechanical Engineering Journal (Internet), 7(3), p.19-00564_1 - 19-00564_14, 2020/06

A large amount of cesium (Cs) chemisorbed onto stainless steel is predicted to be present especially in the upper region of reactor pressure vessel (RPV) during light water reactor severe accident (LWR SA) and a chemisorption model was developed for estimation of such amounts of Cs for stainless steel type 304 (SS304). However, this existing chemisorption model cannot accurately reproduce experimental results. Therefore, in this study, a modified Cs chemisorption model which accounts for silicon content in SS304 and concentration of cesium hydroxide (CsOH) in gaseous phases was constructed by combining penetration theory for gas-liquid mass transfer with chemical reaction and mass action law for CsOH decomposition at interface between gaseous and solid phases. As a result, it was found that the modified model was able to reproduce the experimental data more accurately than the existing model.

Journal Articles

Sorption behavior of selenide on montmorillonite

Sugiura, Yuki; Tomura, Tsutomu*; Ishidera, Takamitsu; Doi, Reisuke; Francisco, P. C. M.; Shiwaku, Hideaki; Kobayashi, Toru; Matsumura, Daiju; Takahashi, Yoshio*; Tachi, Yukio

Journal of Radioanalytical and Nuclear Chemistry, 324(2), p.615 - 622, 2020/05

 Times Cited Count:2 Percentile:43.05(Chemistry, Analytical)

JAEA Reports

Development of JAEA sorption database (JAEA-SDB); Update of sorption/QA data in FY2019

Sugiura, Yuki; Suyama, Tadahiro*; Tachi, Yukio

JAEA-Data/Code 2019-022, 40 Pages, 2020/03

JAEA-Data-Code-2019-022.pdf:2.22MB

Sorption behavior of radionuclides (RNs) in buffer materials, rocks and cementitious materials is one of the key processes in a safe geological disposal. This report focuses on updating of JAEA sorption database (JAEA-SDB) as a basis of integrated approach for the performance assessment (PA)-related distribution coefficient (K$$_{rm d}$$) setting and development of mechanistic sorption models. K$$_{rm d}$$ data and their quality assurance (QA) results were updated by focusing on the following systems as potential needs extracted from our recent activities on the K$$_{rm d}$$ setting and development of mechanistic models, i.e., clay minerals, sedimentary rocks and cementitious materials. As a result, 6,702 K$$_{rm d}$$ data from 60 references were added and the total number of K$$_{rm d}$$ values in JAEA-SDB reached 69,679. The QA/classified K$$_{rm d}$$ data reached about 72% for all K$$_{rm d}$$ data in JAEA-SDB.

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