Predicting Effective Diffusion Coefficients in Mudrocks Using a Fractal Model and Small‐Angle Neutron Scattering Measurements

Andreas Busch, Niko Kampman, Pieter Bertier, Vitaliy Pipich, Artem Feoktystov, Gernot Rother, Jon F. Harrington, Leon Leu, Marc Aertens, Elke Jacops

Research output: Contribution to journalArticle

Abstract

The determination of effective diffusion coefficients of gases or solutes in the water-saturated pore space of mudrocks is time consuming and technically challenging. Yet, reliable values of effective diffusion coefficients are important to predict migration of hydrocarbon gases in unconventional reservoirs, dissipation of (explosive) gases through clay barriers in radioactive waste repositories, mineral alteration of seals to geological CO2 storage reservoirs and contaminant migration through aquitards. In this study, small angle and very small angle neutron scattering techniques have been utilized to determine a range of transport properties in mudrocks, including porosity, pore size distributions and surface and volume fractal dimensions of pores and grains, from which diffusive transport parameters can be estimated. Using a fractal model derived from Archie’s Law, we calculate effective diffusion coefficients from these parameters and compare them to laboratory-derived effective diffusion coefficients for CO2, H2, CH4 and HTO on either the same or related mudrock samples. The samples include Opalinus Shale from the underground laboratory in Mont Terri, Switzerland; Boom Clay from a core drilled in Mol, Belgium and a marine claystone cored in Utah, USA. The predicted values were compared to laboratory diffusion measurements. The measured and modelled diffusion coefficients show good agreement, differing generally by less than factor 5. Neutron or X-ray scattering analysis is therefore proposed as a novel method for fast, accurate estimation of effective diffusion coefficients in mudrocks, together with simultaneous measurement of multiple transport parameters including porosity, pore size distributions and surface areas, important for (reactive) transport modelling.
LanguageEnglish
Pages7076-7091
Number of pages16
JournalWater Resources Research
Volume54
Issue number9
Early online date4 Sep 2018
DOIs
Publication statusPublished - Sep 2018

Fingerprint

neutron scattering
mudstone
porosity
gas
Boom clay
mineral alteration
aquitard
reactive transport
claystone
pore space
repository
radioactive waste
explosive
solute
dissipation
shale
surface area
scattering
hydrocarbon
clay

Cite this

Busch, Andreas ; Kampman, Niko ; Bertier, Pieter ; Pipich, Vitaliy ; Feoktystov, Artem ; Rother, Gernot ; Harrington, Jon F. ; Leu, Leon ; Aertens, Marc ; Jacops, Elke. / Predicting Effective Diffusion Coefficients in Mudrocks Using a Fractal Model and Small‐Angle Neutron Scattering Measurements. In: Water Resources Research. 2018 ; Vol. 54, No. 9. pp. 7076-7091.
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abstract = "The determination of effective diffusion coefficients of gases or solutes in the water-saturated pore space of mudrocks is time consuming and technically challenging. Yet, reliable values of effective diffusion coefficients are important to predict migration of hydrocarbon gases in unconventional reservoirs, dissipation of (explosive) gases through clay barriers in radioactive waste repositories, mineral alteration of seals to geological CO2 storage reservoirs and contaminant migration through aquitards. In this study, small angle and very small angle neutron scattering techniques have been utilized to determine a range of transport properties in mudrocks, including porosity, pore size distributions and surface and volume fractal dimensions of pores and grains, from which diffusive transport parameters can be estimated. Using a fractal model derived from Archie’s Law, we calculate effective diffusion coefficients from these parameters and compare them to laboratory-derived effective diffusion coefficients for CO2, H2, CH4 and HTO on either the same or related mudrock samples. The samples include Opalinus Shale from the underground laboratory in Mont Terri, Switzerland; Boom Clay from a core drilled in Mol, Belgium and a marine claystone cored in Utah, USA. The predicted values were compared to laboratory diffusion measurements. The measured and modelled diffusion coefficients show good agreement, differing generally by less than factor 5. Neutron or X-ray scattering analysis is therefore proposed as a novel method for fast, accurate estimation of effective diffusion coefficients in mudrocks, together with simultaneous measurement of multiple transport parameters including porosity, pore size distributions and surface areas, important for (reactive) transport modelling.",
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Busch, A, Kampman, N, Bertier, P, Pipich, V, Feoktystov, A, Rother, G, Harrington, JF, Leu, L, Aertens, M & Jacops, E 2018, 'Predicting Effective Diffusion Coefficients in Mudrocks Using a Fractal Model and Small‐Angle Neutron Scattering Measurements', Water Resources Research, vol. 54, no. 9, pp. 7076-7091. https://doi.org/10.1029/2018WR023425

Predicting Effective Diffusion Coefficients in Mudrocks Using a Fractal Model and Small‐Angle Neutron Scattering Measurements. / Busch, Andreas; Kampman, Niko; Bertier, Pieter; Pipich, Vitaliy; Feoktystov, Artem; Rother, Gernot; Harrington, Jon F.; Leu, Leon; Aertens, Marc; Jacops, Elke.

In: Water Resources Research, Vol. 54, No. 9, 09.2018, p. 7076-7091.

Research output: Contribution to journalArticle

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T1 - Predicting Effective Diffusion Coefficients in Mudrocks Using a Fractal Model and Small‐Angle Neutron Scattering Measurements

AU - Busch, Andreas

AU - Kampman, Niko

AU - Bertier, Pieter

AU - Pipich, Vitaliy

AU - Feoktystov, Artem

AU - Rother, Gernot

AU - Harrington, Jon F.

AU - Leu, Leon

AU - Aertens, Marc

AU - Jacops, Elke

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N2 - The determination of effective diffusion coefficients of gases or solutes in the water-saturated pore space of mudrocks is time consuming and technically challenging. Yet, reliable values of effective diffusion coefficients are important to predict migration of hydrocarbon gases in unconventional reservoirs, dissipation of (explosive) gases through clay barriers in radioactive waste repositories, mineral alteration of seals to geological CO2 storage reservoirs and contaminant migration through aquitards. In this study, small angle and very small angle neutron scattering techniques have been utilized to determine a range of transport properties in mudrocks, including porosity, pore size distributions and surface and volume fractal dimensions of pores and grains, from which diffusive transport parameters can be estimated. Using a fractal model derived from Archie’s Law, we calculate effective diffusion coefficients from these parameters and compare them to laboratory-derived effective diffusion coefficients for CO2, H2, CH4 and HTO on either the same or related mudrock samples. The samples include Opalinus Shale from the underground laboratory in Mont Terri, Switzerland; Boom Clay from a core drilled in Mol, Belgium and a marine claystone cored in Utah, USA. The predicted values were compared to laboratory diffusion measurements. The measured and modelled diffusion coefficients show good agreement, differing generally by less than factor 5. Neutron or X-ray scattering analysis is therefore proposed as a novel method for fast, accurate estimation of effective diffusion coefficients in mudrocks, together with simultaneous measurement of multiple transport parameters including porosity, pore size distributions and surface areas, important for (reactive) transport modelling.

AB - The determination of effective diffusion coefficients of gases or solutes in the water-saturated pore space of mudrocks is time consuming and technically challenging. Yet, reliable values of effective diffusion coefficients are important to predict migration of hydrocarbon gases in unconventional reservoirs, dissipation of (explosive) gases through clay barriers in radioactive waste repositories, mineral alteration of seals to geological CO2 storage reservoirs and contaminant migration through aquitards. In this study, small angle and very small angle neutron scattering techniques have been utilized to determine a range of transport properties in mudrocks, including porosity, pore size distributions and surface and volume fractal dimensions of pores and grains, from which diffusive transport parameters can be estimated. Using a fractal model derived from Archie’s Law, we calculate effective diffusion coefficients from these parameters and compare them to laboratory-derived effective diffusion coefficients for CO2, H2, CH4 and HTO on either the same or related mudrock samples. The samples include Opalinus Shale from the underground laboratory in Mont Terri, Switzerland; Boom Clay from a core drilled in Mol, Belgium and a marine claystone cored in Utah, USA. The predicted values were compared to laboratory diffusion measurements. The measured and modelled diffusion coefficients show good agreement, differing generally by less than factor 5. Neutron or X-ray scattering analysis is therefore proposed as a novel method for fast, accurate estimation of effective diffusion coefficients in mudrocks, together with simultaneous measurement of multiple transport parameters including porosity, pore size distributions and surface areas, important for (reactive) transport modelling.

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