Experimental study on modeling of Pu sorption onto quartz

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

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

https://doi.org/10.1515/ract-2020-0068

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, 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 SOTh(OH) and SOThOH(CO), 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 SOM(OH) and SOMOH(CO) for Pu(IV) with smaller ionic radii than Th(IV). The Pu(IV) sorption model was developed as SOPu(OH) and SOPu(OH). In addition, data of Pu(IV) sorption onto muscovite was obtained in order to be compared with data for quartz.

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

https://doi.org/10.1515/ract-2020-0006

Evaluation and modelling report of Task 9A based on comparisons and analyses of predictive modelling results for the REPRO WPDE experiments; Task 9 of SKB Task Force GWFTS - Increasing the realism in solute transport modelling based on the field experiments REPRO and LTDE-SD

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

SKB R-17-10, 153 Pages, 2019/01

The SKB Task Force is an international forum on modeling 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 modeling of the tracer breakthrough curves from the WPDE experiments. Several teams, using different modelling approaches, participated in this exercise. An important conclusion from this exercise is that the modeling 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. The modeling results have also been finally compared to the measured breakthroughs.

Evaluation of effective dose coefficient with variation of absorption fraction in gastrointestinal system for ingestion of radiocesium

Pratama, M. A.; Takahara, Shogo; Hato, Shinji*

Hoken Butsuri, 52(3), p.200 - 209, 2017/09

https://doi.org/10.5453/jhps.52.200

The purpose of this study is to identify the significance of the change in the intestinal absorption rate values the ( value) to the change of dose coefficient as well as to provide a list of dose coefficients which each of the value corresponds to a specific intestinal absorption rate and age groups. In the range of 0-1, 10 different values of for 1 year, 5 years old, and adult group were chosen and used in a separate calculation by using, a biokinetic compartment model, DCAL. It was found that the lower values of intestinal absorption rate lead to a significant decrease of the committed effective coefficient for adult. Oppositely for children, the decrease of committed effective coefficient was not as significant. This study also suggests that the significance of dose coefficient change due to the variation of substantially depends on the biological half-life of the radionuclide and the mass of organs and tissues in human body.

Clay-based modeling approach to diffusion and sorption in the argillaceous rock from the Horonobe URL; Application to Ni(II), Am(III), and Se(IV)

Tachi, Yukio; Suyama, Tadahiro; Yotsuji, Kenji; Ishii, Yasuo; Takahashi, Hiroaki*

CMS Workshop Lectures, Vol.21, p.241 - 250, 2016/00

https://www.clays.org/other-cms-publications-wrksh21/

Sorption and diffusion of radionuclides in argillaceous rocks are key processes in the safe geological disposal. The diffusion and sorption behavior of Ni(II), Am(III) and Se(IV) in mudstone from the Horonobe URL were investigated by experimental and modeling approaches. Effective diffusivities obtained by the through-diffusion experiments were in the sequence of Cs, Ni, HTO, I, Se(SeO), Am(Am(CO)) by comparison with the previous study. The distribution coefficient values were consistent with those obtained by batch sorption tests. These results were interpreted by the clay-based modeling approach coupling the thermodynamic sorption model assuming key contributions of clays (smectite and illite) and the diffusion model assuming the electrical double layer theory and the simplified pore model with size distribution. This clay-based model could provide reasonable account of observed trends and could be basically applicable for various radionuclides.

JENDL photonuclear data file

Kishida, Norio*; Murata, Toru*; Asami, Tetsuo*; Kosako, Kazuaki*; Maki, Koichi*; Harada, Hideo*; Lee, Y.*; Chang, J.*; Chiba, Satoshi; Fukahori, Tokio

AIP Conference Proceedings 769, p.199 - 202, 2005/05

https://doi.org/10.1063/1.1944989

Nuclear data for photonuclear reactions are required in the field of shielding design of high-energy electron accelerators and high-energy -ray therapy. The JENDL Photonuclear Data File was prepared by a working group on nuclear data evaluations for photonuclear reactions in Japanese Nuclear Data Committee. From a survey of many literatures, it is difficult to construct the photonuclear data file by using only measured data, since there are not sufficient experimental data. We were therefore evaluating with theoretical calculations based on statistical nuclear reaction models. The photonuclear cross sections that are to be contained in the file are as follows: photoabsorption cross sections, yield cross sections and DDX for neutrons, protons, deuterons, tritons, He-particles and alpha-particles, and isotope production cross sections. For the actinide nuclides, photofission cross sections are also included. The maximum energy of incident photons is 140 MeV and stored are the photonuclear data for 68 nuclides from H to Np.

Adsorption mechanisms and models of Sr, Np, Pu and Am in loess media (Joint research)

Tanaka, Tadao; Mukai, Masayuki; Maeda, Toshikatsu; Matsumoto, Junko; Ogawa, Hiromichi; Li, S.*; Wang, Z.*; Wang, J.*; Guo, Z.*; Zhao, Y.*

JAERI-Research 2002-034, 20 Pages, 2002/12

JAERI-Research-2002-034.pdf:1.1MB

Adsorption mechanisms and models of Sr(II), Np(V), Pu(IV) and Am(III) on the loess were investigated from their adsorption and desorption properties. The distribution coefficient of Sr and Np was 2 - 3 orders of magnitude smaller than that of Pu and Am. The adsorption of Sr and Np was mainly controlled by the ion exchange reaction. On the other hand, the adsorption of Pu and Am was mostly controlled by the selective chemical reactions with Fe and Mn oxyhydroxide/oxide and humic substances. On the basis of the experimental results, several types of adsorption models of the radionuclides, considering elemental concentrations, adsorption mechanisms and kinetics, were proposed for setting up the analytical systems of radionuclide migration in the loess media.

Dynamic behaviors of fragments ejected from the surface of carbon materials by laser ablation

Yoda, Osamu; Miyashita, Atsumi; *; *

JAERI-M 92-173, 27 Pages, 1992/10

JAERI-M-92-173.pdf:1.22MB

no abstracts in English

The GTS-LTD MONOPOLE-2 experiment at grimsel; Predictive modeling and comparison with monitoring data

Soler, J. M.*; Martin, A. J.*; Lanyon, G. W.*; Havlov, V.*; Siitari-Kauppi, M.*; Tachi, Yukio

no journal, , 

An in-situ long-term diffusion (LTD) project has been performed at the Grimsel Test Site, Switzerland, to realistically evaluate matrix diffusion of radionuclides in crystalline rock with minimal disturbance to in-situ conditions. A second in situ diffusion experiment (monopole 2) has been performed. Predictive calculations for the monopole-2 experiment, based on results from monopole 1 or from through-diffusion experiments have been compared to monitoring data from the injection and observation boreholes. For the non-sorbing tracers (HTO, Cl), the diffusion parameters from the through-diffusion experiments provide a better match for the measurements, especially in the injection borehole. The initial drop in activities for Cs and Ba shows clearly the effect of sorption. Bulk rock parameters for Cs from monopole 1 seem to be applicable to monopole 2. However, Ba seems to sorb more strongly than expected.

Effects of heterogeneity at fracture surface for tracer migration in a fractured crystalline rock from the Grimsel Test Site

Tachi, Yukio; Ito, Tsuyoshi; Akagi, Yosuke*; Sato, Hisao*; Martin, A. J.*

no journal, , 

The effects of heterogeneity at fracture surface on radionuclides migration in fractured crystalline rocks was investigated by laboratory migration experiments, microscopic observations and detailed modelling, using a single fractured granodiorite sample from the Grimsel Test Site (GTS), Switzerland. The tracer migration behaviors in fracture and matrix parts were evaluated by series of laboratory experiments including through-diffusion and flow-through experiments. Mineral distributions from fracture surface to matrix were evaluated by X-ray CT, and were validated by comparing the elemental mapping measured by EPMA. Based on the microscopic observations by X-ray CT and EPMA, the aperture and connectivity in fracture and minerals distribution near fracture surface were quantitatively evaluated. The heterogeneous multi-layered model assuming a weathered vermiculite zone, a foliated mica zone and rock matrix was possible to provide a reasonable interpretation for measured breakthrough curves of all tracers.