Gas transfer through clay barriers

Amann-Hildenbrand, A.; Kroos, B.M.; Harrington, J.; Cuss, R.; Davy, C.; Skoczylas, F.; Jacops, E.; Maes, N.. 2015 Gas transfer through clay barriers [in special issue: Natural and engineered clay barriers] Developments in Clay Science, 6. 227-267.

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Gas transport through clay-rocks can occur by different processes that can be basically subdivided into pressure-driven flow of a bulk gas phase and transport of dissolved gas either by molecular diffusion or advective water flow (Figure 1, Marschall et al., 2005). The relative importance of these transport mechanisms depends on the boundary conditions and the scale of the system. Pressure-driven volume flow (“Darcy flow”) of gas is the most efficient transport mechanism. It requires, however, pressure gradients that are sufficiently large to overcome capillary forces in the typically water-saturated rocks (purely gas-saturated argillaceous rocks are not considered in the present context). These pressure gradients may form as a consequence of the gravity field (buoyancy, compaction) or by gas generation processes (thermogenic, microbial, radiolytic). Dissolved gas may be transported by water flow along a hydraulic gradient. This process is not affected by capillary forces but constrained by the solubility of the gas. It has much lower transport efficiency than bulk gas phase flow. Molecular diffusion of dissolved gas, finally, is occurring essentially without constraints, ubiquitously and perpetually. Effective diffusion distances are, however, proportional to the square root of time, which limits the relevance of this transport process to the range of tens to hundreds of metres on a geological time scale (millions of years). 2 Process understanding and the quantification of the controlling parameters, like diffusion coefficients, capillary gas breakthrough pressures and effective gas permeability coefficients, is of great importance for up-scaling purposes in different research disciplines and applications. During the past decades, gas migration through fully water-saturated geological clay-rich barriers has been investigated extensively (Thomas et al., 1968, Pusch and Forsberg, 1983; Horseman et al., 1999; Galle, 2000; Hildenbrand et al., 2002; Marschall et al., 2005; Davy et al., 2009; Harrington et al., 2009, 2012a, 2014). All of these studies aimed at the analysis of experimental data determined for different materials (rocks of different lithotype, composition, compaction state) and pressure/temperature conditions. The clay-rocks investigated in these studies, ranged from unconsolidated to indurated clays and shales, all characterised by small pores (2-100 nm) and very low hydraulic conductivity (K < 10-12 m·s-1) or permeability coefficients (k < 10-19 m²). Studies concerning radioactive waste disposal include investigations of both the natural host rock formation and synthetic/engineered backfill material at a depth of a few hundred meters (IAEA, 2003, 2009). Within a geological disposal facility, hydrogen is generated by anaerobic corrosion of metals and through radiolysis of water (Rodwell et al., 1999; Yu and Weetjens, 2009). Additionally, methane and carbon dioxide are generated by microbial degradation of organic wastes (Rodwell et al., 1999; Ortiz et al., 2002; Johnson, 2006; Yu and Weetjens, 2009). The focus of carbon capture and storage (CCS) studies is on the analysis of the long-term sealing efficiency of lithologies above depleted reservoirs or saline aquifers, typically at larger depths (hundreds to thousands of meters). During the last decade, several studies were published on the sealing integrity of clay-rocks to carbon dioxide (Hildenbrand et al., 2004; Li et al., 2005; Hangx et al., 2009; Harrington et al., 2009; Skurtveit et al., 2012; Amann-Hildenbrand et al., 2013). In the context of petroleum system analysis, a significant volume of research has been undertaken regarding gas/oil expulsion mechanisms from sources rocks during burial history (Tissot & Pellet, 1971; Appold & Nunn, 2002), secondary migration (Luo et al., 2008) and the capillary sealing capacity of caprocks overlying natural gas accumulations (Berg, 1975; Schowalter, 1979; Krooss, 1992; Schlömer and Kross, 2004; Li et al., 2005; Berne et al., 2010). Recently, more attention has been paid to investigations of the transport efficiency of shales in the context of oil/gas shale production (Bustin et al., 2008; Eseme et al., 2012; Amann-Hildenbrand et al., 2012; Ghanizadeh et al., 2013, 2014). Analysis of the migration mechanisms within partly unlithified strata becomes important when explaining the 3 origin of overpressure zones, sub-seafloor gas domes and gas seepages (Hovland & Judd, 1988; Boudreau, 2012). The conduction of experiments and data evaluation/interpretation requires a profound process understanding and a high level of experience. The acquisition and preparation of adequate samples for laboratory experiments usually constitutes a major challenge and may have serious impact on the representativeness of the experimental results. Information on the success/failure rate of the sample preparation procedure should therefore be provided. Sample specimens “surviving” this procedure are subjected to various experimental protocols to derive information on their gas transport properties. The present overview first presents the theoretical background of gas diffusion and advective flow, each followed by a literature review (sections 2 and 3). Different experimental methods are described in sections 4.1 and 4.2. Details are provided on selected experiments performed at the Belgian Nuclear Research Centre (SCK-CEN, Belgium), Ecole Centrale de Lille (France), British Geological Survey (UK), and at RWTH-Aachen University (Germany) (section 4.3). Experimental data are discussed with respect to different petrophysical parameters outlined above: i) gas diffusion, ii) evolution of gas breakthrough, iii) dilation-controlled flow, and iv) effective gas permeability after breakthrough. These experiments were conducted under different pressure and temperature conditions, depending on sample type, burial depth and research focus (e.g. radioactive waste disposal, natural gas exploration, or carbon dioxide storage). The interpretation of the experimental results can be difficult and sometimes a clear discrimination between different mechanisms (and the controlling parameters) is not possible. This holds, for instance, for gas breakthrough experiments where the observed transport can be interpreted as intermittent, continuous, capillary- or dilation-controlled flow. Also, low gas flow rates through samples on the length-scale of centimetres can be equally explained by effective two-phase flow or diffusion of dissolved gas.

Item Type: Publication - Article
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NORA Subject Terms: Earth Sciences
Date made live: 24 Aug 2016 15:01 +0 (UTC)

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