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JAEA Reports

Development of coupled mass-transport and chemical-reaction calculation code for alteration of engineered barrier

Sasagawa, Tsuyoshi; Mukai, Masayuki; Sawaguchi, Takuma

JAEA-Data/Code 2021-012, 122 Pages, 2022/01


Reducing public dose is required when radioactive wastes such as high-level and from reactor core internals etc. are disposed of by means of multi barrier system consist of engineered and natural barriers. In these barriers, engineered barrier is expected to bring out confinement function of waste's radionuclides in the barrier. Materials used as the engineered barriers are altered and performances of the barrier materials are degraded in course of time. To estimate properly the degraded performances, analytical evaluation of long-term change of the engineered barrier state is important. Change state of the engineered barrier is given by mass-transport and geochemical-reaction inside the barrier materials and these phenomena are interrelated, it is necessary to calculate the state by means of coupled analysis procedure. We have developed a coupled mass-transport and geochemical-reaction calculation code (MC- BUFFER) to evaluate alteration of engineered barrier specially targeted for water permeability of bentonite buffer material as one of most important performances to engineered barrier. This report describes functions expected for the engineered barrier, influence parameters for the functions, implementation models in MC-BUFFER, structure and functions of MC-BUFFER, input file format and output examples, execution method of MC-BUFFER, and sample run with MC-BUFFER.

Journal Articles

Erratum; Effects of OH$$^{-}$$ activity and temperature on the dissolution rate of compacted montmorillonite under highly alkaline conditions [Clay Minerals, vol.51, p.275 (2016), Corrected Fig. 7.]

Sawaguchi, Takuma; Tsukada, Manabu; Yamaguchi, Tetsuji; Mukai, Masayuki

Clay Minerals, 51(5), P. 815, 2016/12

ERRATUM; Effects of OH$$^{-}$$ activity and temperature on the dissolution rate of compacted montmorillonite under highly alkaline conditions [Clay Minerals, vol.51, p.275 (2016), Corrected Fig. 7.]

Journal Articles

Effects of OH$$^{-}$$ activity and temperature on the dissolution rate of compacted montmorillonite under highly alkaline conditions

Sawaguchi, Takuma; Tsukada, Manabu; Yamaguchi, Tetsuji; Mukai, Masayuki

Clay Minerals, 51(2), p.267 - 278, 2016/05

 Times Cited Count:6 Percentile:24.25(Chemistry, Physical)

The dependences of the dissolution rate of compacted montmorillonite on activity of OH$$^{-}$$ (a$$_{rm OH}$$-) and temperature (T) were investigated. The dissolution rate of montmorillonite ($$R_{rm A}$$) in compacted pure montmorillonite, which was formulized as $$R_{rm A}$$ = 10$$^{4.5}$$ (a$$_{rm OH}$$-)$$^{1.3}$$ e$$^{-55000/RT}$$, was higher than that in the compacted sand-bentonite mixtures: $$R_{rm A}$$ = 3500 (a$$_{rm OH}$$-)$$^{1.4}$$ e$$^{-51000/RT}$$. The difference can be explained by considering the decrease in a$$_{rm OH}$$- in the mixtures accompanied by dissolution of accessory minerals such as quartz and chalcedony. The dissolution rate model developed for pure montmorillonite is expected to be applied to bentonite mixtures if quantification of the decrease in a$$_{rm OH}$$- is achieved somehow.

JAEA Reports

Development of ESRAD2 program for estimation of spatial radioactivity distribution based on Kriging; User's manual

Ishigami, Tsutomu; Shimada, Taro; Seki, Masaya; Mukai, Masayuki

JAEA-Data/Code 2015-019, 122 Pages, 2015/12


In ensuring compliance with the criterion of site release as the final stage of termination of decommissioning of nuclear facilities, it is supposed to confirm the radioactivity concentration obtained by measurement in the site is less than or equal to the concentration corresponding to the criterion. It is needed to estimate the distribution and mean of radioactivity concentration in the evaluation unit using a number of measured data. It is further needed to compare the estimated result with the concentration corresponding to the criterion of site release and to decide if the evaluation unit should comply with the criterion. The estimated result exhibits uncertainty depending on the number of measurement points, which results in a certain probability of the occurrence of decision error according to the uncertainty. It is important to decide the number of measurement points required by revealing a relationship of the error probability to the number of measurement points for site security. We have developed the ESRAD2 (Estimation of Spatial RadioActivity Distribution program version 2), which is an extended version of the existing ESRAD, for estimating the mean of radioactivity concentration and calculating the number of measurement points required according to the error probability. This report describes a method for ensuring compliance with the criterion of site release, structure and functions, input file format, output examples, execution method of ESRAD2, and sample run with ESRAD2.

JAEA Reports

Study on the evaluation method to determine the radioactivity concentration waste generated from post-irradiation examination facilities

Hoshino, Yuzuru; Sakamoto, Yoshiaki; Muroi, Masayuki*; Mukai, Satoru*

JAEA-Technology 2015-015, 96 Pages, 2015/07


In order to dispose of the radioactive waste which generates from post-irradiation examination (PIE) facilities, the common evaluation method of radioactivity in wastes from PIE should be established by the actual data such as radioactivity values and the theoretical calculation. In this study, the radioactivity concentrations of 17 nuclides (H-3, C-14, Co-60, Ni-63, Sr-90, Tc-99, Cs-137, Eu-154, U-234, U-235, U-238, Pu-238, Pu-239, Pu-240, Pu-241, Am-241, Cm-244) in combustible wastes stored in NUCLEAR DEVELOPMENT CORPORATION were measured from 3 samples and the radioactivity was calculated by ORIGEN-2 based on initial contents and operation record of the spent fuel. From the comparison of the obtained data by the radiological measurement with the calculated values, the subject to be solved for establishment of the radioactivity evaluation method for PIE was extracted.

Journal Articles

Analysis of radionuclide migration with consideration of spatial and temporal change of migration parameters due to uplift and denudation

Shimada, Taro; Takeda, Seiji; Mukai, Masayuki; Munakata, Masahiro; Tanaka, Tadao

Materials Research Society Symposium Proceedings, Vol.1744, p.229 - 234, 2015/04

Integrated safety assessment methodology which analyzes radionuclide migration reflecting the spatial and temporal changes of disposal systems was developed for a geological disposal site with uplift and denudation, and then some case analyses for an assumed site with sedimentary rocks were carried out. The combination of uniform uplift and denudation has the most effect on the radionuclide migration because the groundwater flow velocity increases with decreasing the depth from the ground surface. In the case without denudation, tilted uplift has more effect than uniform uplift because flow velocity in tilted uplift increase with increasing hydraulic gradient. The long-term change of the geological structures including the uplift and denudation, the hydraulic conditions, and the recharge and outlet of the groundwater around a candidate site should be carefully investigated to determine the appropriate the place,depth and layout of the repository.

Journal Articles

Alkaline dissolution behavior of montmorillonite under compacted condition

Sawaguchi, Takuma; Kadowaki, Mitsushi*; Yamaguchi, Tetsuji; Mukai, Masayuki; Tanaka, Tadao

Genshiryoku Bakkuendo Kenkyu (CD-ROM), 20(2), p.71 - 78, 2013/12

The dissolution rate for montmorillonite under compacted condition was studied in order to evaluate long-term alteration behavior of bentonite buffer materials by highly alkaline groundwater. The dissolution rate of compacted montmorillonite was found to be larger than that of montmorillonite in compacted sand-bentonite mixtures at 130 $$^{circ}$$C, which revealed that the dissolution of montmorillonite was inhibited by decreasing the activity of hydroxide ions (${it $alpha$$_O$$_H$$^-$}$) in the compacted mixtures including accessory minerals such as silica. In order to provide reliability for the analysis of bentonite-alteration using a formula of dissolution rate of montmorillonite, it is important to quantify the decrease of ${it $alpha$$_O$$_H$$^-$}$ in the compacted mixtures and to formulate the dissolution rate of compacted montmorillonite.

JAEA Reports

Evaluation of uncertainties in model parameters for evaluating decommissioning project management data based on JPDR decommissioning experience data

Ishigami, Tsutomu; Sukegawa, Takenori*; Mukai, Masayuki

JAEA-Technology 2013-027, 124 Pages, 2013/10


In order to safely and efficiently implement decommissioning of nuclear installations, it is important to beforehand predict decommissioning project management data (PMD) and to develop a decommissioning plan based on the predicted results. The PMD prediction is made with PMD evaluation equations including model parameters such as unit work activity coefficients. Although model parameter values developed so far include uncertainties, little evaluation of the uncertainties and resulted uncertainties in predicted PMD has been made. However information on the uncertainties is valuable in flexibly studying and developing a decommissioning plan. We therefore studied and evaluated uncertainties in model parameters by analyzing the JPDR decommissioning experience data. This report describes an evaluation method of the model parameter uncertainties and their evaluated results.

Journal Articles

Development of a reactive transport code MC-CEMENT ver.2 and its verification using 15-year ${it in-situ}$ concrete/clay interactions at the Tournemire URL

Yamaguchi, Tetsuji; Kataoka, Masaharu; Sawaguchi, Takuma; Mukai, Masayuki; Hoshino, Seiichi; Tanaka, Tadao; Marsal, F.*; Pellegrini, D.*

Clay Minerals, 48(2), p.185 - 197, 2013/05

 Times Cited Count:3 Percentile:10.43(Chemistry, Physical)

Highly alkaline environments induced by cement based materials are likely to deteriorate the physical and/or chemical properties of the bentonite buffer materials in radioactive waste repositories. Predicting long-term alteration of concrete/clay systems requires physico-chemical models and a number of input parameters. In order to provide reliability to the long-term prediction of bentonite buffer performance under disposal conditions, it is necessary to develop and verify reactive transport codes for concrete/clay systems. In this study, a PHREEQC-based, reactive transport analysis code (MC-CEMENT ver.2) was developed and was verified by comparing results of the calculations with ${it in situ}$ observations of the mineralogical evolution at the concrete/argillite interface. The calculation reproduced the observations such as the mineralogical changes limited within one cm in thickness, formation of CaCO$$_{3}$$ and CSH, dissolution of quartz, decrease of porosity in argillite and increase in concrete. These agreements indicate possibility that the models based on lab-scale ($$sim$$ 1 y) experiments can be applied to longer time scale. The fact that the calculation did not reproduce the dissolution of clays and the formation of gypsum indicates that there is still room for improvement in our model.

JAEA Reports

Development of ESRAD program for estimation of spatial radioactivity distribution based on Kriging; User's manual

Ishigami, Tsutomu; Mukai, Masayuki; Sukegawa, Takenori; Matsubara, Takeshi*

JAEA-Data/Code 2012-023, 83 Pages, 2012/11


Verification for site release is one of procedures to confirm termination of decommissioning of nuclear installations. The verification procedure would need to confirm that the radioactive concentration at the site is lower than the criterion value by measurement. Then to efficiently perform the measurement and verification it is one of important issues how to efficiently estimate and evaluate overall spatial radioactivity distribution using a sampling method. For the efficient estimation and evaluation we have applied a Kriging technique which in the geostatistics, and have developed a computer program ESRAD (Estimation of Spatial RadioActivity Distribution). The ESRAD program is designed to support sample selection, calculate a variogram, and estimate a radioactivity distribution for the area concerned. This report describes the Kriging technique, structure and functions of ESRAD, input file format, output examples, execution procedure of ERSAR, and sample run with ESRAD.

JAEA Reports

Study on experimental models to analyze radionuclide migration behaviors through porous geologic media

Tanaka, Tadao; Mukai, Masayuki

JAEA-Research 2011-053, 41 Pages, 2012/08


To understand the migration phenomenon of radionuclide, actual migration data are experimentally acquired by a batch test, a column test and field trial. In the present study, experimental models about the interactions of radionuclide between the solid phase and the liquid phase were discussed systematically to interpret the migration data acquired by the various techniques and conditions. Equilibrium, reversibility, linearity, mechanism and chemistry in the interactions were considered in discussion of the experimental models. A calculation program, which can analyze migration data obtained under various conditions by applying the selected 9 types of experimental models, was maintained. The calculation program makes it be able to predict the migration behavior of radionuclide under various conditions and to decide the important parameter by a fitting analysis of the migration data.

Journal Articles

Irradiation history of Itokawa regolith material deduced from noble gases in the Hayabusa samples

Nagao, Keisuke*; Okazaki, Ryuji*; Nakamura, Tomoki*; Miura, Yayoi*; Osawa, Takahito; Bajo, Kenichi*; Matsuda, Shintaro*; Ebihara, Mitsuru*; Ireland, T.*; Kitajima, Fumio*; et al.

Science, 333(6046), p.1128 - 1131, 2011/08

 Times Cited Count:121 Percentile:95.46(Multidisciplinary Sciences)

A steroid surface materials record regolith processes and a history of cosmic-ray irradiation. Noble gas isotopes in three rocky grains from Itokawa have been determined. High concentrations of solar He, Ne, and Ar, as high as those in lunar soils, are released at variable temperatures from each sample. The isotopic compositions are essentially identical to those of solar wind but distinguishable in He relative abundance. These noble gas characteristics can be explained by repeated implantation and preferential loss of solar He by removal of weathered He-rich rim on the grain surface through friction among regolith grains on Itokawa. Residence time of regolith materials on Itokawa is alculated to be shorter than 10 Myr, suggesting that regolith materials of small asteroids would escape easily to space.

Journal Articles

Numerical simulation of the influence of humic-complexation on the migration of radionuclide through porous media; A Consideration of the sensitivity of analytical parameters

Tanaka, Tadao; Mukai, Masayuki

Humic Substances Research, 5-6(1), p.35 - 43, 2009/00

The present paper describes a theoretical evaluation of the influence of humic-complexation on migration of cationic radionuclides through porous media, where it is assumed that complexation reactions between radionuclides and natural organics, such as humic acid and fulvic acid, can be regarded to follow an instantaneous equilibrium or a first-order kinetic reaction. The calculation results revealed that radionuclide migration in the presence of humic substance was predominantly controlled by relative magnitude of distribution coefficients between the cationic radionuclides and the complexed radionuclides. Radionuclide migration was also affected significantly by the stability of the complexes or the rate constants of the complexation reaction.

Journal Articles

The H-Invitational Database (H-InvDB); A Comprehensive annotation resource for human genes and transcripts

Yamasaki, Chisato*; Murakami, Katsuhiko*; Fujii, Yasuyuki*; Sato, Yoshiharu*; Harada, Erimi*; Takeda, Junichi*; Taniya, Takayuki*; Sakate, Ryuichi*; Kikugawa, Shingo*; Shimada, Makoto*; et al.

Nucleic Acids Research, 36(Database), p.D793 - D799, 2008/01

 Times Cited Count:51 Percentile:72.68(Biochemistry & Molecular Biology)

Here we report the new features and improvements in our latest release of the H-Invitational Database, a comprehensive annotation resource for human genes and transcripts. H-InvDB, originally developed as an integrated database of the human transcriptome based on extensive annotation of large sets of fulllength cDNA (FLcDNA) clones, now provides annotation for 120 558 human mRNAs extracted from the International Nucleotide Sequence Databases (INSD), in addition to 54 978 human FLcDNAs, in the latest release H-InvDB. We mapped those human transcripts onto the human genome sequences (NCBI build 36.1) and determined 34 699 human gene clusters, which could define 34 057 protein-coding and 642 non-protein-coding loci; 858 transcribed loci overlapped with predicted pseudogenes.

Journal Articles

Development and verification of a reactive transport model for long-term alteration of bentonite-cement-seawater systems

Yamaguchi, Tetsuji; Yamada, Fumika; Negishi, Kumi*; Hoshino, Seiichi; Mukai, Masayuki; Tanaka, Tadao; Nakayama, Shinichi

Physics and Chemistry of the Earth, 33(Suppl.1), p.S285 - S294, 2008/00

It is important to assess long-term alteration of engineered barrier composed of bentonite and cement for the safety assessment of radioactive waste disposal. In order to promote our development of the assessment methodologies, we developed a secondary mineral formation model for cement based materials and a hydraulic conductivity model for bentonite buffer materials. These models were verified by comparing with experimental observations. We also calculated changes in mineralogy of bentonite buffer materials and accompanying changes in the hydraulic conductivity over 10,000 y. We identified the temperature as an important factor dominating the alteration of the buffer. We also identified that the alteration is limited by slow kinetics of the dissolution of montmorillonite and by the diffusive mass transfer. Our calculation showed that the mineralogical change proceeds rather fast during the initial 1,000 y and slows down afterwards, and that salinity of the groundwater has both positive and negative effects on the hydraulic conductivity.

Journal Articles

Field tests on Ce transfer in natural loess environments

Tanaka, Tadao; Mukai, Masayuki; Bamba, Tsunetaka

Proceedings of International Symposium on Environmental Modeling and Radioecology, p.275 - 278, 2007/03

Migration behavior of Ce, one of redox-sensitive elements, was studied in natural aquifer loess zone in P.R.China. Migration parameters such as distribution coefficient were obtained by column migration and batch sorption tests. The batch sorption test indicates Ce is irreversibly incorporated near loess surface as Ce(IV). Cerium showed large retardation in migration in the aquifer loess zone. Predicted migratory mobility of Ce in the aquifer, which was calculated by using the distribution coefficient determined by the batch and column tests, could reproduce that in the field test conservatively.

Journal Articles

Study on evaluation method of colloidal migration of radionuclides; Models on colloid transport in porous media

Mukai, Masayuki; Tanaka, Tadao; Yukawa, Kazuhiko; Suryantoro*

Genshiryoku Bakkuendo Kenkyu, 12(1-2), p.41 - 51, 2006/03

To evaluate radionuclides migration through geologic media coexistent with colloids in groundwater, a model has been coded. To evaluate an applicability of four models to colloid transport through porous media, breakthrough curves (BTCs) from column experiments using sand and reddish soil have been analyzed. Instantaneous equilibrium model could not explain both timings of breakthrough and reach to C$$_{c}$$/C$$_{co}$$=1 concurrenyly, however 1st order kinetic reaction model successfully simulate them well. BTCs from the reddish soil column have a particular feature that shows step-wise rising pattern in response to alternately inflow of colloid. Both the instantaneous equilibrium, the 1st order kinetic reaction and filtration models could not simulate this feature, however a 1st order kinetic reaction with filtration capacity model reasonably simulates the feature. The model for colloid transport, given an important role as a part of colloidal migration model of radionuclide, has been validated on the basis of the laboratory experiments.

Journal Articles

Sorption and migration of neptunium in porous sedimentary materials

Tanaka, Tadao; Mukai, Masayuki; Nakayama, Shinichi

Proceedings of International Conference on Nuclear Energy System for Future Generation and Global Sustainability (GLOBAL 2005) (CD-ROM), 6 Pages, 2005/10

no abstracts in English

Journal Articles

Influences of humid substances, alkaline conditions and colloids on radionuclide migration in natural barrier

Mukai, Masayuki; Ueda, Masato; Inada, Daisuke; Yukawa, Kazuhiko; Maeda, Toshikatsu; Iida, Yoshihisa

Proceedings of International Symposium NUCEF 2005, p.219 - 224, 2005/08

For better quantitative understanding of radionuclide migration for safety assessment of geologic disposal, JAERI has been conducting experimental and modeling studies on influences of humic substances, highly alkaline conditions and colloids on sorptive and diffusional behavior of TRU in geologic materials. In the absence of fulvic acid, one of humic substances, diffusion of Am through a tuff sample was not detected. By adding fulvic acid, Am was detected in the downstream cell, which indicates the diffusion through the sample. Highly alkaline conditions arisen from cementitious materials may spread by altering chemical and physical properties of geologic materials. Through-diffusion experiments of alkaline species in granite showed that the effective diffusion coefficient of Ca$$^{2+}$$ and OH$$^{-}$$ in a cement-equilibrated aqueous solution were found to be higher by almost two orders of magnitude than Na$$^{+}$$ and OH$$^{-}$$ in a NaOH solution. Radionuclide migration can be enhanced by colloids, and thus a calculation code describing the effect of colloids on radionuclide migration has been required.

Journal Articles

Influence of humic substances on the $$^{63}$$Ni migration through crushed rock media

Tanaka, Tadao; Sakamoto, Yoshiaki; Mukai, Masayuki; Maeda, Toshikatsu; Nakayama, Shinichi

Radiochimica Acta, 92(9-11), p.725 - 729, 2004/12

 Times Cited Count:1 Percentile:10.23(Chemistry, Inorganic & Nuclear)

Migration experiments of $$^{63}$$Ni for crushed rocks, granite and tuff, were performed under the coexistent condition with a humic acid and a fulvic acid of 0-30 mg/l in concentration, which are Nordic humic substances supplied from International Humic Substance Society. Migration experiments of Ni had been performed by a column system, to investigate migration behavior of Ni through a column packed crushed rock. The Ni concentration in the effluent passed through the column was corresponding to the fractional percentage of Ni complexing with humic substance in influent solution. This result suggests that the Ni complexing with humic substance in influent solution was flowed out from the column without any effective interactions with the rock media. The migration behavior of Ni could be expressed by a migration model taking account of the complexation kinetics of Ni with humic substance in the aqueous phase.

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