Evolution of radionuclide transport and retardation processes in uplifting granitic rocks, Part 2; Modelling coupled processes in uplift scenarios

Metcalfe, R.*; Benbow, S. J.*; Kawama, Daisuke*; Tachi, Yukio

Science of the Total Environment, 958, p.177690_1 - 177690_17, 2025/01

https://doi.org/10.1016/j.scitotenv.2024.177690

Uplifting fractured granitic rocks occur in substantial areas of countries such as Japan. A repository site would be selected in such an area only if it is possible to make a safety case, accounting for the changing conditions during uplift. The safety case must include robust arguments that chemical processes in the rocks around the repository will contribute sufficiently to minimise radiological doses to biosphere receptors. To provide confidence in the safety arguments, numerical models need to be sufficiently realistic, but also parameterised conservatively (pessimistically). However, model development is challenging because uplift involves many complex couplings between groundwater flow, chemical reactions between water and rock, and changing rock properties. The couplings would affect radionuclide mobilisation and retardation, by influencing diffusive radionuclide fluxes between groundwater flowing in fractures and effectively immobile porewater in the rock matrix and radionuclide partitioning between water and solid phases, via: (i) mineral precipitation/dissolution; (ii) mineral alteration; and (iii) sorption/desorption. It is difficult to represent all this complexity in numerical models while showing that they are parameterised conservatively. Here we present a modelling approach, illustrated by simulation cases for some exemplar radioelements, to identify realistically conservative process conceptualisations and model parameterisations.

Evolution of radionuclide transport and retardation processes in uplifting granitic rocks, Part 1; Key processes, conceptual models and scenario

Metcalfe, R.*; Tachi, Yukio; Sasao, Eiji; Kawama, Daisuke*

Science of the Total Environment, 957, p.177375_1 - 177375_17, 2024/12

https://doi.org/10.1016/j.scitotenv.2024.177375

A safety case for an underground radioactive waste repository must show that groundwater will not in future transport radionuclides from the repository to the near-surface environment (the biosphere) in harmful quantities. Safety cases are developed step-wise throughout a programme to site and develop a repository. At early stages, before a site is selected, safety cases are generic and based on simplified safety assessment models of the disposal system that have conservative parameter values. Later, when site-specific conditions are known, more realistic models are needed for the long-term geo-environmental evolution and their impacts on radionuclide migration/retention. Uplift is one such environmental change, which may be particularly important in countries near active tectonic plate boundaries, such as Japan. Here we review the state of knowledge about how the properties of fractured granitic rocks evolve during uplift, based on studies in Japan. Hence, we present conceptual models and a generic scenario for mass transport and retardation processes in uplifting granitic rocks as a basis for realistic numerical models to underpin safety assessment.

Evaluation of thermodynamic model of Pd(II) complex formation with isosaccharinic acid

Kimuro, Shingo; Taneichi, Yayoi; Iwata, Hajime; Ishidera, Takamitsu; Kitamura, Akira; Tachi, Yukio; Tanaka, Takeru*; Hirano, Kana*; Hieda, Manami*; Miyabe, Shunsuke*; et al.

Journal of Solution Chemistry, 53(6), p.854 - 868, 2024/06

https://doi.org/10.1007/s10953-023-01352-6

Archie's cementation factors for natural rocks; Measurements and insights from diagenetic perspectives

Yuan, X.*; Hu, Q. H.*; Fang, X.*; Wang, Q. M.*; Ma, Y.*; Tachi, Yukio

Sedimentary Geology, 465, p.106633_1 - 106633_14, 2024/05

https://doi.org/10.1016/j.sedgeo.2024.106633

Predictive and inverse modeling of a radionuclide diffusion experiment in crystalline rock at ONKALO (Finland)

Soler, J. M.*; Keklinen, P.*; Pulkkanen, V.-M.*; Moreno, L.*; Iraola, A.*; Trinchero, P.*; Hokr, M.*; ha, J.*; Havlov, V.*; Trpkoov, D.*; et al.

Nuclear Technology, 209(11), p.1765 - 1784, 2023/11

https://doi.org/10.1080/00295450.2023.2209234

Paleoclimatic controls on natural tracer profiles in biogenic sedimentary formations of the Horonobe area, Japan

Arthur, R.*; Sasamoto, Hiroshi; Alt-Epping, P.*; Tachi, Yukio

Applied Geochemistry, 155, p.105707_1 - 105707_8, 2023/08

https://doi.org/10.1016/j.apgeochem.2023.105707

The experience gained in modeling the evolution, from past to present, of natural tracer profiles in geologic media can help support safety assessment of disposal concepts for radioactive wastes in deep geologic repository. Solute-transport models were developed in the present study using a forward modeling approach constrained by boundary conditions inferred from the paleo-hydrogeological evolution of the Horonobe area in Hokkaido, Japan. Apparent differences in transport behavior at the two boreholes location considered in this study, which were situated only about 1 km apart, appear to have resulted from relatively small differences in accessible porosity and hydraulic conductivity, which in turn may have been controlled by local differences in fracture density and fracture connectivity.

None

Hamamoto, Takafumi*; Ishida, Keisuke*; Tachi, Yukio

NUMO-TR-22-02, p.62 - 64, 2023/03

https://www.numo.or.jp/technology/technical_report/NUMO-TR-22-02.pdf

no abstracts in English

New approach to understanding the experimental Cs NMR chemical shift of clay minerals via machine learning and DFT-GIPAW calculations

Okubo, Takahiro*; Takei, Akihiro*; Tachi, Yukio; Fukatsu, Yuta; Deguchi, Kenzo*; Oki, Shinobu*; Shimizu, Tadashi*

Journal of Physical Chemistry A, 127(4), p.973 - 986, 2023/02

https://doi.org/10.1021/acs.jpca.2c08880

The identification of adsorption sites of Cs on clay minerals has been studied in the fields of environmental chemistry. The nuclear magnetic resonance (NMR) experiments allow direct observations of the local structures of adsorbed Cs. The NMR parameters of Cs, derived from solid-state NMR experiments, are sensitive to the local neighboring structures of adsorbed Cs. However, determining the Cs positions from NMR data alone is difficult. This paper describes an approach for identifying the expected atomic positions of Cs adsorbed on clay minerals by combining machine learning (ML) with experimentally observed chemical shifts. A linear ridge regression model for ML is constructed from the smooth overlap of atomic positions descriptor and gauge-including projector augmented wave (GIPAW) ab initio data. The Cs chemical shifts can be instantaneously calculated from the Cs positions on any clay layers using ML. The inverse analysis from the ML model can derive the atomic positions from experimentally observed chemical shifts.

Micro- to nano-scale areal heterogeneity in pore structure and mineral compositions of a sub-decimeter-sized Eagle Ford Shale

Wang, Q.*; Hu, Q.*; Zhao, C.*; Yang, X.*; Zhang, T.*; Ilavsky, J.*; Kuzmenko, I.*; Ma, B.*; Tachi, Yukio

International Journal of Coal Geology, 261, p.104093_1 - 104093_15, 2022/09

https://doi.org/10.1016/j.coal.2022.104093

Evolution of the reaction and alteration of granite with Ordinary Portland cement leachates; Sequential flow experiments and reactive transport modelling

Bateman, K.*; Murayama, Shota*; Hanamachi, Yuji*; Wilson, J.*; Seta, Takamasa*; Amano, Yuki; Kubota, Mitsuru*; Ouchi, Yuji*; Tachi, Yukio

Minerals (Internet), 12(7), p.883_1 - 883_20, 2022/07

https://doi.org/10.3390/min12070883