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論文

Pore connectivity influences mass transport in natural rocks; Pore structure, gas diffusion and batch sorption studies

Yuan, X.*; Hu, Q.*; Lin, X.*; Zhao, C.*; Wang, Q.*; 舘 幸男; 深津 勇太; 濱本 昌一郎*; Siitari-Kauppi, M.*; Li, X.*

Journal of Hydrology, 618, p.129172_1 - 129172_15, 2023/03

 被引用回数:0 パーセンタイル:0(Engineering, Civil)

Mass transport in geomedia as influenced by the pore structure is an important phenomenon. Six rocks (granodiorite, limestone, two chalks, mudstone, and dolostone) with different extents of heterogeneity at six different particle sizes were studied to describe the effects of pore connectivity on mass transport. The multiple methods applied were porosity measurement, gas diffusion test, and batch sorption test of multiple ions. Porosity measurement results reveal that with decreasing particle sizes, the effective porosities for the "heterogenous" group (granodiorite and limestone) increase, whereas the porosities of "homogeneous" group (chalks, mudstone, and dolostone) roughly remain constant. Gas diffusion results show that the intraparticle gas diffusion coefficient among these two groups, varying in the magnitude of 10$$^{-8}$$ to 10$$^{-6}$$ m$$^{2}$$/s. The batch sorption work displays a different affinity of these rocks for tracers, which are related to their mineral components. For granodiorite, mudstone, and dolostone, the adsorption capacity increases as the particle size decreases, due to higher specific surface area in smaller particle-size. In general, this integrated research of grain size distribution, rock porosity, intraparticle diffusivity, and ionic sorption capacity gives insights into the pore connectivity effect on both gas diffusion and chemical transport behaviors for different lithologies and/or different particle sizes.

論文

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.*; 舘 幸男

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

 被引用回数:3 パーセンタイル:72.03(Energy & Fuels)

To understanding the spatial heterogeneity of mineral and pore structure variations in fine-grained shale, microscale X-ray fluorescence (micro-XRF) mapping, (ultra-) small-angle X-ray scattering [(U)SAXS] and wide-angle X-ray scattering were applied for two samples from a piece of Eagle Ford Shale in South Texas. Thin section petrography and field emission-scanning electron microscopy, X-ray diffraction (XRD), total organic carbon, and pyrolysis were also utilized to investigate the potential spatial heterogeneity of pore types, mineral and organic matter compositions for both samples. Overall, the siliceous-carbonate mineral contents in these carbonate-rich Eagle Ford Shale vary between laminations at mm scales. By analyzing six selected sub-samples on each of two samples with X-ray scattering and XRD techniques, nm-sized pores are mainly interparticle ones in the higher calcite regions, where the porosity is also relatively lower, while the lower calcite regions consist of both interparticle and intraparticle pore types with higher porosity. Finally, the micro-XRF and (U)SAXS are combined to generate porosity distribution maps to provide more insights about its heterogeneity related to the laminations and fractures at our observational scales.

口頭

Pore connectivity of clay materials implicated in fluid flow and chemical diffusion

Hu, Q.*; Wang, Q.*; Zhao, C.*; 舘 幸男; 深津 勇太

no journal, , 

低透水粘土バリア材料中の低拡散性は、放射性廃棄物処分場の長期性能評価において、重要な安全機能と認識されている。間隙の連結性が低い低透水粘土材料は、特異な拡散特性を示し、このことが長期拡散挙動に影響を及ぼす可能性が報告されている。日本の幌延URLの稚内層の泥岩、スイスのモンテリURLのオパリナス粘土岩、さまざまな頁岩や粘土鉱物の関連研究において、間隙構造の評価手法(水銀圧入法や中性子小角散乱法など)と、レーザーアブレーションICP-MSによるマイクロスケールでの元素分布分析を組合せたトレーサー試験手法が適用された。これらの試験結果から、間隙の連続性と拡散挙動の特異性との関係が得られた。間隙のサイズは低い透水性や拡散性の主要な要因ではなく、特異な拡散挙動は間隙の連結性に起因していることを明らかにした。

口頭

Fluid flow and chemical transport in shallow and deep mudrocks being implicated by pore geometry and connectivity

Hu, Q.*; Wang, Q.*; Zhao, C.*; Zhang, T.*; 舘 幸男; 深津 勇太

no journal, , 

Fine-grained and clay-rich mudrocks play an important role in the long-term performance of a geological repository for storing high-level nuclear wastes and petroleum production in shale formations. However, low-permeability mudrocks whose pores are poorly interconnected are known to have anomalous diffusion properties that strongly impact long-term net diffusion. The complex pore structure involving predominantly nano-sized pore space is related to compaction and diagenesis from the maturation process of organic matter-rich mudrocks at deep depths, leading to a much smaller effective porosity which could be further partitioned by water- or oil-wet pore networks. Working with shallow clayey sediments of Wakkanai formation around Horonobe underground research center in Hokkaido of Japan and Opalinus clay of Mt. Terri Underground Research Laboratory in Switzerland, as well as various deep shales (Barnett, Eagle Ford and Wolfcamp from Texas, Bakken from North Dakota), using a wide range of sample sizes, this multi-approach and -scale work utilizes a complementary suite of approaches for pore structure characterization (e.g., helium pycnometry, mercury intrusion porosimetry, small angle/X-ray neutron scattering, field emission-scanning electron microscopy), gas diffusion and liquid (including water-, oil-, and bi-wetting) imbibition involving custom-designed tracer recipe followed with micro-scale mapping with laser ablation-ICP-MS. The experimental results show that deep mudrocks has a much smaller effective porosity than the total porosity (as a result of poor pore connectivity) and associated diffusion coefficient, and the effective porosity and diffusion coefficients are also dependent upon the sample sizes used in the measurement.

口頭

Fluid flow and chemical transport in clay-rich media implicated by pore geometry and connectivity

Hu, Q.*; Wang, Q. M.*; Zhao, C.*; Zhang, T.*; Iltaf, H.*; 舘 幸男; 深津 勇太

no journal, , 

Fine-grained and clay-rich mudrocks play an important role in the long-term performance of a geological repository for storing high-level nuclear wastes and petroleum production in shale formations. However, low-permeability mudrocks whose pores are poorly interconnected are known to have anomalous diffusion properties that strongly impact long-term net diffusion. The complex pore structure involving predominantly nano-sized pore space is related to compaction and diagenesis from the maturation process of organic matter-rich mudrocks at deep depths, leading to a much smaller effective porosity. Working with various clay minerals, shallow clayey sediments of Wakkanai formation around Horonobe URL in Japan and Opalinus clay of Mt. Terri URL in Switzerland, as well as various deep shales (Barnett, Eagle Ford and Wolfcamp from Texas), using a wide range of sample sizes, this multi-approach and -scale work utilizes a complementary suite of techniques for pore structure characterization (e.g., mercury intrusion porosimetry, small angle X-ray/neutron scattering, scanning electron microscopy), gas diffusion, batch sorption and column transport. The experimental results show that deep mudrocks has a much poor pore connectivity than the shallow ones, and the effective porosity, diffusion coefficients, sorption coefficients are also dependent upon the sample sizes used in the measurement.

口頭

Decimeter-scale laboratory studies of thermal, mechanical, hydrological and chemical processes in near-field systems of generic geological waste repositories

Hu, Q. H.*; Zhang, T.*; Shen, Y. Q.*; 舘 幸男; 深津 勇太; Borglin, S.*; Chang, C.*; Hampton, J.*

no journal, , 

In a deep geological repository of high-level nuclear wastes, the near-field systems consist of waste packages, buffer materials, and natural barrier systems. It is expected that the initial thermal loading after waste emplacement will last several hundred years. It is important to investigate the effects of this thermal loading on the near-field components under in situ stress conditions, in terms of thermal-hydrological-mechanical-chemical (THMC) processes and subsequent radionuclide retention and migration. Preliminary tests have been performed via integrated combinations of buffer materials and host rocks, at nm-dm scales, subjected to a range of elevated temperatures under true-triaxial conditions, which is complemented by a suite of nano-petrophysical characterization approaches such as small-angle neutron/X-ray scattering techniques to quantify total pore space and sample size-dependent effective porosity. For multiple-approach radionuclide retention and migration tests before- and after-THMC experiments, a complementary range of tests will include batch, column, and gas diffusion for granular samples, as well as gas/liquid diffusion and fractured core transport tests for intact rock samples under different temperature and pressure conditions.

口頭

Microscopic pore structure and macroscopic fluid flow-chemical transport in host rocks and barrier materials

Wang, Q. M.*; Hu, Q.*; Zhao, C.*; Zhang, T.*; 深津 勇太; 舘 幸男

no journal, , 

Fluid flow and chemical transport in porous media are the macroscopic consequences of pore structure, which integrates geometry (e.g., pore size and surface area, pore-size distribution) and topology (e.g., pore connectivity). Low-permeability geological media whose pores are poorly interconnected will exhibit the characteristics of anomalous diffusion and sample size-dependent effective porosity, which will strongly impact long-term net diffusion and retention of radionuclides in geological repository settings. A suite of experimental approaches is utilized to study the microscopic pore structure and macroscopic fluid flow and chemical transport for a range of natural rocks (such as clay/shale, crystalline rock, salt), in addition to clay minerals. With a particular focus on quantifying the presence and magnitude of isolated pores for a reduced effective porosity in low-permeability geomedia, the integrated methodologies for basic properties and pore structure characterization include X-ray diffraction, thin section petrography, grain size distribution, water immersion porosimetry, mercury intrusion porosimetry, nitrogen physisorption, scanning electron microscopy, X-ray computed tomography, and (ultra-)small angle neutron (or X-ray) scattering. In addition, custom-designed gas diffusion, tracer recipe involving a range of anionic and cationic chemicals with subsequent analyses by laser ablation and inductively coupled plasma-mass spectrometry, along with batch sorption, column transport, and imbibition tests were conducted for coupled effects of pore structure and chemical retention/transport.

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