Joint clarification of contaminant plume and hydraulic transmissivity via a geostatistical approach using hydraulic head and contaminant concentration data

Takai, Shizuka; Shimada, Taro; Takeda, Seiji; Koike, Katsuaki*

Mathematical Geosciences, 56(2), p.333 - 360, 2024/02

https://doi.org/10.1007/s11004-023-10084-8

To enable proper remediation of accidental groundwater contamination, the contaminant plume evolution needs to be accurately estimated. In the estimation, uncertainties in both the contaminant source and hydrogeological structure should be considered, especially the temporal release history and hydraulic transmissivity. Although the release history can be estimated using geostatistical approaches, previous studies use the deterministic hydraulic property field. Geostatistical approaches can also effectively estimate an unknown heterogeneous transmissivity field via the joint data use, such as a combination of hydraulic head and tracer data. However, tracer tests implemented over a contaminated area necessarily disturb the in situ condition of the contamination. Conversely, measurements of the transient concentration data over an area are possible and can preserve the conditions. Accordingly, this study develops a geostatistical method for the joint clarification of contaminant plume and transmissivity distributions using both head and contaminant concentration data. The applicability and effectiveness of the proposed method are demonstrated through two numerical experiments assuming a two-dimensional heterogenous confined aquifer. The use of contaminant concentration data is key to accurate estimation of the transmissivity. The accuracy of the proposed method using both head and concentration data was verified achieving a high linear correlation coefficient of 0.97 between the true and estimated concentrations for both experiments, which was 0.67 or more than the results using only the head data. Furthermore, the uncertainty of the contaminant plume evolution was successfully evaluated by considering the uncertainties of both the initial plume and the transmissivity distributions, based on their conditional realizations.

Development of an iron(II) complex exhibiting thermal- and photoinduced double proton-transfer-coupled spin transition in a short hydrogen bond

Nakanishi, Takumi*; Hori, Yuta*; Shigeta, Yasuteru*; Sato, Hiroyasu*; Kiyanagi, Ryoji; Munakata, Koji*; Ohara, Takashi; Okazawa, Atsushi*; Shimada, Rintaro*; Sakamoto, Akira*; et al.

Journal of the American Chemical Society, 145(35), p.19177 - 19181, 2023/08

https://doi.org/10.1021/jacs.3c06323

Evaluating the effectiveness of a geostatistical approach with groundwater flow modeling for three-dimensional estimation of a contaminant plume

Takai, Shizuka; Shimada, Taro; Takeda, Seiji; Koike, Katsuaki*

Journal of Contaminant Hydrology, 251, p.104097_1 - 104097_12, 2022/12

https://doi.org/10.1016/j.jconhyd.2022.104097

When assessing the risk from an underground environment that is contaminated by radioactive nuclides and hazardous chemicals and planning for remediation, the contaminant plume distribution and the associated uncertainty from measured data should be estimated accurately. While the release history of the contaminant plume may be unknown, the extent of the plume caused by a known source and the associated uncertainty can be calculated inversely from the concentration data using a geostatistical method that accounts for the temporal correlation of its release history and groundwater flow modeling. However, the preceding geostatistical approaches have three drawbacks: (1) no applications of the three-dimensional plume estimation in real situations, (2) no constraints for the estimation of the plume distribution, which can yield negative concentration and large uncertainties, and (3) few applications to actual cases with multiple contaminants. To address these problems, the non-negativity constraint using Gibbs sampling was incorporated into the geostatistical method with groundwater flow modeling for contaminant plume estimation. This method was then tested on groundwater contamination in the Gloucester landfill in Ontario, Canada. The method was applied to three water soluble organic contaminants: 1,4-dioxane, tetrahydrofuran, and diethyl ether. The effectiveness of the proposed method was verified by the general agreement of the calculated plume distributions of the three contaminants with concentration data from 66 points in 1982 (linear correlation coefficient of about 0.7). In particular, the reproduced large spill of organic contaminants of 1,4-dioxane in 1978 was more accurate than the result of preceding minimum relative entropy-based studies. The same peak also appeared in the tetrahydrofuran and diethyl ether distributions approximately within the range of the retardation factor derived from the fraction of organic carbon.

Experimental study on the localization and estimation of radioactivity in concrete rubble using image reconstruction algorithms

Takai, Shizuka; Namekawa, Masakazu*; Shimada, Taro; Takeda, Seiji

IEEE Transactions on Nuclear Science, 69(7), p.1789 - 1798, 2022/07

https://doi.org/10.1109/TNS.2022.3181241

To reduce a large amount of contaminated concrete rubble stored in the Fukushima Daiichi Nuclear Power Station site, recycling low-radioactivity rubble within the site is a possible remedy. To promote recycling while ensuring safety, not only the average radioactivity but also the radioactivity distribution of concrete rubble should be efficiently evaluated because the details of rubble contamination caused by the accident remain unclear and likely include hotspots. However, evaluating inhomogeneous contamination of thick and/or dense materials is difficult using previous measurement systems, such as clearance monitors. This study experimentally confirmed the potential applicability of image reconstruction algorithms for radioactivity distribution evaluation in concrete rubble filled in a chamber. Radiation was measured using plastic scintillation fiber around the chamber (50 50 40 cm). Localized hotspots were simulated using standard sources of Cs, which is one of the main nuclides of contaminated rubble. The radioactivity distribution was calculated for 100 or 50 voxels (voxel size: (10 cm) or 10 10 20 cm) constituting the chamber. For 100 voxels, inner hotspots were undetected, whereas, for 50 voxels, both inner and surface hotspots were reconstructible. The distribution evaluated using the maximum likelihood expectation maximization algorithm was the most accurate; the average radioactivity was estimated within 70% accuracy in all seven cases.

Evaluation of clearance level for radionuclides in asbestos-containing wastes

Shimada, Taro; Nemoto, Hiromi*; Takeda, Seiji

Hoken Butsuri (Internet), 57(1), p.5 - 29, 2022/03

https://doi.org/10.5453/jhps.57.5

Of the asbestos-containing wastes arising from the dismantling activities of nuclear facilities, those with radioactive concentrations that do not need to be treated as radioactive substances will be cleared from the nuclear regulatory control. Those will be disposed of or recycled as specially controlled industrial waste based on the Waste Management and Public Cleansing Act. The authors constructed evaluation scenarios according to the treatment manual for asbestos-containing waste and evaluated public exposure doses per year for 33 radionuclides. Based on the evaluated doses, the radioactive concentration corresponding to the dose criteria of 10 Sv/y for clearance was calculated for each radionuclide and scenario. As a result, the evaluated concentration was equal to or higher than the current clearance level. It was confirmed that the application of the current clearance level for asbestos-containing wastes did not affect safety.

Determination of Cs/Cs isotopic ratio in soil collected near Fukushima Daiichi Nuclear Power Station through mass spectrometry

Shimada, Asako; Tsukahara, Takehiko*; Nomura, Masao*; Kim, M. S.*; Shimada, Taro; Takeda, Seiji; Yamaguchi, Tetsuji

Journal of Nuclear Science and Technology, 58(11), p.1184 - 1194, 2021/11

https://doi.org/10.1080/00223131.2021.1931520

Determining the completeness of nuclear reactor decommissioning is an important step in safely utilizing nuclear power. For example, Cs from the Fukushima Daiichi Nuclear Power Station (FDNPS) accident can be treated as background radioactivity, so determining the origin of Cs is essential. To accomplish this, measuring the Cs/Cs isotope ratio can be useful, so this study optimized a solvent extraction method, with calix[4]arene-bis(t-octylbenzo-crown-6) [BOBCalixC6] in 1-octanol, to purify radioactive Cs, radiocesium, from a solution of major environmental soil elements and mass spectrometry interference elements. This optimized method was applied to Cs purification in soil samples (40 g), and the final solutions contained a total of 10g/ml of the major soil elements and ng/ml concentrations at most of interfering elements. Soil samples collected near the FDNPS were then purified, and the Cs/Cs isotope ratios were measured, using both thermal ionization mass spectrometry (TIMS) and triple quadrupole induced coupled plasma mass spectrometry (ICP-QQQ). The results of each of these measurements were compared, and we found that Cs isotope ratios obtained by TIMS were more precise, by an order of magnitude, while the ICP-QQQ results possessed good abundance sensitivities. A slightly higher Cs/Cs ratio in the northwest area of the FDNPS was observed, while other areas exhibited similar values, all within the measurement error range, which indicated different origins of radiocesium. These results agreed with previously reported Cs/Cs activity distributions, suggesting that this ratio may be useful in identifying radiocesium origins for evaluating future nuclear reactor decommissions.

Current status and issues for clearance, 5; Concept of restricted use of contaminated rubbles in the Fukushima Daiichi NPS

Shimada, Taro; Miwa, Kazuji; Takeda, Seiji

Nihon Genshiryoku Gakkai-Shi ATOMO, 61(7), p.531 - 534, 2019/07

Rubbles less than 5 Sv/h of surface dose rate, which are stored outdoor in the Fukushima Daiichi NPS (1F) site, will be recycled and applied in a restricted reuse only within 1F site in the future. However, there is no precedent for establishing the reference values such as dose and/or concentration for reuse or recycling under the existing exposure situation. In this study, we suggested a concept for establishing the reference radioactive concentration of recycling material for the restricted use in the 1F site. In addition, based on the concept, we calculated the reference radiocesium concentrations of the recycling material used for paved roads and the bases of concrete building.

Study on restricted use of contaminated rubble on Fukushima Daiichi NPS site, 1; Estimation of reference radiocesium concentration for recycling materials

Shimada, Taro; Miwa, Kazuji; Takeda, Seiji

Progress in Nuclear Science and Technology (Internet), 6, p.203 - 207, 2019/01

https://doi.org/10.15669/pnst.6.203

Rubbles less than 5 Sv/h of surface dose rate, which are stored outdoor in the Fukushima Daiichi NPS (1F) site, will be recycled and applied in a restricted reuse only within 1F site in the future. In this study, we suggested a concept for establishing the reference radioactive concentration of recycling material for the restricted use in the 1F site. Reference radiocesium concentration is calculated so that increased dose rate by restricted reuse does not exceed 1 Sv/h which is the minimum value of dose rate map in the 1F entire site. In order to justify the restricted reuse under the reference concentration calculated, additional occupational dose, dose rate at the site boundary and groundwater concentration at the outlet to the ocean are evaluated and confirmed that the values are below 2 mSv/y, 1 mSv/y and 1 Bq/cm of Cs and Cs, respectively. And then calculated the reference radiocesium concentrations of the recycling material used for paved roads and the bases of concrete building.

Evaluation of influence of splay fault growth on groundwater flow around geological disposal system

Takai, Shizuka; Takeda, Seiji; Sakai, Ryutaro*; Shimada, Taro; Munakata, Masahiro; Tanaka, Tadao

Nihon Genshiryoku Gakkai Wabun Rombunshi, 16(1), p.34 - 48, 2017/03

https://doi.org/10.3327/taesj.J16.003

In geological disposal, direct effect on geological repositories by active faults is avoided at a stage of site characterization; however, uncertainty remains for avoidance of faults derived from the active faults, which are concealed deep under the ground and difficult to detect in advance. In this research, the influence of growth of undetected splay faults on natural barrier in a geological disposal system, which will caused by attack of the faults in the future, was evaluated. We investigated examples of splay faults in Japan and set conditions for growth of splay faults. Furthermore, we assumed a disposal site composed of sedimentary rocks and made a hydrogeological model of growth of splay faults. We carried out groundwater flow analyses, changing parameters such as location and depth of repository and growth velocity of splay faults. The results indicate that main flow path from the repository is changed into upward flow along the splay fault due to its growth and the average velocity to the ground surface becomes one or two orders of magnitude higher than that before its growth. The results also suggest that the splay fault growth leads into the possibility of downward flow of oxidizing groundwater from ground surface area.

Evaluation for influence of new volcanic eruption on geological disposal site

Shimada, Taro; Takeda, Seiji; Sakai, Ryutaro*; Takubo, Kazuya; Tanaka, Tadao

MRS Advances (Internet), 1(61), p.4081 - 4086, 2016/00

https://doi.org/10.1557/adv.2017.193

Volcanic eruption which may affect geological disposal system directly depends on the regional location in Japan. It is required that the disposal site should be located far from existing volcanos. However, there are regions where it is impossible to exclude the possibility of appearance of new volcanic activity on the site even if the site is located far from existing volcanos. In order to identify the influence of volcanic eruption at disposal site to public if it occurs public exposure doses were evaluated based on the two scenarios considering types of eruption at new volcanic activity in Japan. One is the exposure by tephra widespread by Strombolian eruption and deposited on the ground surface, including radionuclides from vitrified waste forms after a volcanic conduit penetrated disposal galleries. The other is that by waste forms appeared at the surface by Merapi type pyroclastic flow. Exposure doses of the residents living on the tephra do not exceed 1mSv/y even when the eruption occurs at 1,000 years after closure of disposal site. Dose rate for the volcanic researchers temporarily approaching waste forms becomes less than 1mSv/h when the eruption occurs 100,000 years after. It indicated that attention should be paid to the impact by Merapi type pyroclastic flow on researchers approaching waste forms appeared rather than that by Strombolian eruption on residents living on the tephra widespread.