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

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 CO 2 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 CO 2, H 2, CH 4 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 modeled diffusion coefficientsmore » show good agreement, differing generally by less than factor 5. Furthermore, 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.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [4];  [4]; ORCiD logo [5]; ORCiD logo [6];  [7];  [8];  [8]
  1. Heriot-Watt Univ., Edinburgh (United Kingdom)
  2. Shell Global Solutions International B.V., Rijswijk (The Netherlands)
  3. RWTH Aachen Univ., Aachen (Germany)
  4. Forschungszentrum Jülich GmbH (Jülich Centre for Neutron Science, JCNS) at Heinz Maier-Leibnitz Zentrum (MLZ), Garching (Germany)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  6. Keyworth, British Geological Survey, Nottingham (United Kingdom)
  7. Imperial College London, London (United Kingdom)
  8. Belgian Nuclear Research Centre (SCK-CEN), Mol (Belgium)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1515688
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Water Resources Research
Additional Journal Information:
Journal Volume: 54; Journal Issue: 9; Journal ID: ISSN 0043-1397
Publisher:
American Geophysical Union (AGU)
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; mudrock; fractal; diffusion; small‐angle neutron scattering; tortuosity

Citation Formats

Busch, Andreas, Kampman, Niko, Bertier, Pieter, Pipich, Vitaliy, Feoktystov, A., Rother, Gernot, Harrington, J., Leu, Leon, Aertens, M., and Jacops, E. Predicting Effective Diffusion Coefficients in Mudrocks Using a Fractal Model and Small-Angle Neutron Scattering Measurements. United States: N. p., 2018. Web. doi:10.1029/2018WR023425.
Busch, Andreas, Kampman, Niko, Bertier, Pieter, Pipich, Vitaliy, Feoktystov, A., Rother, Gernot, Harrington, J., Leu, Leon, Aertens, M., & Jacops, E. Predicting Effective Diffusion Coefficients in Mudrocks Using a Fractal Model and Small-Angle Neutron Scattering Measurements. United States. doi:10.1029/2018WR023425.
Busch, Andreas, Kampman, Niko, Bertier, Pieter, Pipich, Vitaliy, Feoktystov, A., Rother, Gernot, Harrington, J., Leu, Leon, Aertens, M., and Jacops, E. Tue . "Predicting Effective Diffusion Coefficients in Mudrocks Using a Fractal Model and Small-Angle Neutron Scattering Measurements". United States. doi:10.1029/2018WR023425. https://www.osti.gov/servlets/purl/1515688.
@article{osti_1515688,
title = {Predicting Effective Diffusion Coefficients in Mudrocks Using a Fractal Model and Small-Angle Neutron Scattering Measurements},
author = {Busch, Andreas and Kampman, Niko and Bertier, Pieter and Pipich, Vitaliy and Feoktystov, A. and Rother, Gernot and Harrington, J. and Leu, Leon and Aertens, M. and Jacops, E.},
abstractNote = {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 modeled diffusion coefficients show good agreement, differing generally by less than factor 5. Furthermore, 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.},
doi = {10.1029/2018WR023425},
journal = {Water Resources Research},
number = 9,
volume = 54,
place = {United States},
year = {2018},
month = {9}
}

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