1. Introduction
Unconventional natural gas, especially shale gas, has become increasingly important in the global energy supply in the past decade [
1,
2]. Hydraulic fracturing technology has been successfully applied to the exploitation of unconventional natural gas for the permeability enhancement of shale gas reservoirs. The fracturing fluid retains in the target formation and changes the flow mechanism in a longer production time [
3,
4]. In this flow regime, the relative permeability, as an essential parameter for characterizing the behavior of two-phase flow in a complex porous medium, plays a critical role in shale gas production and CO
2 geological storage [
5,
6]. Previous studies focused on the flow characteristics of gas in porous media and ignored the significant effect of water in complex micropores on gas effective permeability. This behavior is harmful to understanding the mechanism of gas-water displacement in complex pore structures. For instance, it may lead to an inaccurate prediction of fracturing fluid flowback in shale gas production. Therefore, it is meaningful to study the gas-water relative permeability in complex fractal porous media for gas-water displacement.
The gas-water relative permeability has been investigated through experiments, theoretical modeling, and numerical simulations.
Figure 1 summarizes some classical relative permeability models and provides a brief introduction to the development of relative permeability model in recent years. The Purcell model calculated the permeability through capillary pressure data and formulated a relatively primitive permeability model [
7]. This model assumes that the sum of the gas and water relative permeability is equal to 1, which does not agree with the actual fluid flow in porous media. Subsequently, this model was further modified by many scholars. Gates and Leitz [
8] integrated the relative permeability from the capillary pressure. Burdine [
9] thought that the assumption of capillary parallelism was not accurate and introduced the tortuosity factor into the Purcell model. Mualem [
10] proposed an integration method based on the Purcell model. For simplicity, Romm [
11] developed a relative permeability model which ignored the phase interference between the gas and water phases. This model is also called the X model. Brooks and Corey [
12] introduced a pore-size distribution index to modify the capillary pressure function and proposed a more generalized gas-water relative permeability model. The Brooks–Corey model has been widely used in modeling two-phase flow in complex porous media. Fourar and Lenormand [
13] derived a viscous coupling model after integrating Stokes’ equation and the effect of viscosity. Combined with momentum balance, viscosity, and cubic law, Chima and Geiger [
14] developed a new relative permeability model. After ignoring the capillary pressure, Chima’s model became a unique form of the viscous coupling model. Li et al. [
15] improved Chima’s model through the consideration of the influences of capillary tortuosity and irreducible water saturation on relative permeability. The above relative permeability models have made significant contributions to the prediction of two-phase flow in porous media. They also found that the relative permeability of the gas phase is more susceptible to the geometry of flow channels. However, these relative permeability models did not thoroughly consider the effects of complex pore microstructures on fluid flow.
Complex nanoscale pore structures of shale gas reservoirs can be directly observed by the advanced image technology such as focused ion beam-scanning electron microscopes (FIB-SEM) and broad ion beam-scanning electron microscopes (BIB-SEM), but the inclusion of these complex microstructures into the relative permeability model has become a challenging problem. There are several mathematical and physical issues to be solved. The first issue is the description of complex microstructures. Mandelbrot [
16] first developed the fractal theory for self-similarity in complex porous media. The fractal theory has been regarded as a useful tool to describe nanoscale pore structures [
17,
18,
19]. The second issue is the interaction between complex microstructures and fluid flow in porous media. Many scholars have discussed the influence of the complex pore structure on the flow mechanism in the relative permeability model [
20,
21,
22]. For example, Li et al. [
23] considered some non-interconnected tortuous capillaries in fractal-like porous media and proposed a novel gas-water displacing model. Lei et al. [
17] developed a relative permeability model in multiscale porous media, which takes lognormal distribution function and residual water saturation into consideration. Ghanbarian et al. [
21] developed a relative permeability model to consider the tortuosity-connectivity factor and effective saturation. The influences of drawdown pressure on the relative permeability of water and gas phase were experimentally investigated by Mo et al. [
24]. Their experimental results indicated that gas relative permeability increases with drawdown pressure. Additionally, the increase in drawdown pressure can reduce irreducible water saturation. Huo and Benson [
25] experimentally investigated the dependence of relative permeability on stress. They found that both irreducible water saturation and endpoint gas phase relative permeability decrease with the increase of effective stress at the same flow rate. Li et al. [
1] stated that the interface effect plays a significant role in gas-water relative permeability. When the contact angle is higher than 90 °, the surface of hydrophobic material decreases the resistance of fluid flow, and the relative permeability correspondingly increases with the contact angle. Lei et al. [
26] proposed a fractal model for the prediction of gas-water relative permeability in fractures. They found that increasing the complexity of pore structure (fractal dimension) would result in a decrease of water relative permeability, while the gas relative permeability has a corresponding increase with the ratio of fluid viscosity. Geng et al. [
18] deduced a fractal apparent permeability model for shale gas flow in the heterogeneous matrix (organic and inorganic matters). If the organic matter in the matrix is ignored, the apparent permeability will be overestimated up to 24.1%. Therefore, pore shape, maximum pore size, and porosity are primary factors that have significant effects on apparent permeability [
27]. Cai et al. [
28] proposed an improved permeability model to consider viscous flow, molecular diffusion, and surface diffusion. However, this model uses a uniform diffusion coefficient to deduce gas permeability, ignoring the effect of water on the transport mechanism. Wang et al. [
29] considered surface effects (hydrogen bond, double layer repulsive force, Vander Waals force, and structure repulsive force) into the gas-water relative permeability model. They found that the effect of hydrogen bond can significantly enhance fluid flow in porous media. However, the interaction of microstructures and fluid flow regimes has not been well-described in relative permeability models.
Because of the extremely low permeability of shale and complex pore structure, the relative permeability is difficult to measure in experiments. Thus, an analytical method for deriving gas-water relative permeability is critical. In the above-mentioned relative permeability models, the complexity of the pore structure, geometric correction factor, water film, and real gas effect are not comprehensively considered. It is still not clear how the irreducible water in the shale gas reservoir affects the gas flow in the complex pore structure. In this paper, an improved gas-water relative permeability model was proposed based on fractal theory. This improved fractal model takes the complexity of pore structure, geometric correction factor, water film, and real gas effect into consideration. Then, the improved fractal model was compared with two classical models and verified against available experimental data. Finally, the effects of structural parameters, geometric correction factor, water film, and real gas effect on gas-water relative permeability were investigated.
2. Proposed Gas-Water Relative Permeability Model
In this section, the two-phase flow mechanism in complex pore structures is investigated. The threshold pressure gradient and the critical capillary radius are depicted in a conceptual model to emphasize the influence of capillary size on the gas-water displacing process. Then, the fractal dimensions are introduced to describe the complexity of porous media. Finally, an improved gas-water relative permeability model is derived from accounting for the influences of the complex pore structure, geometric correction factor, water film and the real gas effect.
2.1. Two Classical Relative Permeability Models
2.1.1. Brooks–Corey Model
In the Corey model, relative permeability is a function of capillary pressure as
where
is a constant,
is the capillary pressure in porous media,
is a correction coefficient, and
is the water relative permeability.
For complex pore structures, this equation cannot predict the relative permeability with sufficient accuracy. Researchers have found that relative permeability is sensitive to pore-size distribution. The classical Brooks–Corey model introduces a macroscopic parameter of pore-size distribution index
to describe the heterogeneity of pore structure. Their relative permeability model is
where
represents the effective water saturation and is a function of capillary pressure
.
2.1.2. Viscous Coupling Model
Considering the effect of viscosity on fluid flow, Fourar and Lenormand [
13] developed a gas-water relative permeability model as
where
is the water saturation.
is the viscosity ratio of gas to water and is
.
2.2. Gas-Water Displacement and the Variation of Capillary Pressure with Water Saturation
Figure 2 presents a simplified conceptual diagram to express the variation of capillary pressure with water saturation. The solid red line represents the process of gas displacing water. The initial state of the rock formation is fully water-saturated, and the pressure increases with gas injection. When the capillary entry pressure is overcome, the front of two-phase flow starts to move. The accumulated pressure will cause the gas to break through the upper boundary of the rock formation. This pressure is called breakthrough pressure. Finally, the increase of pressure does not further reduce water saturation in the fracture. This minimum water saturation is irreducible water saturation (IRWS). The blue dotted line represents the process of water imbibition. As the capillary pressure decreases, a portion of the gas is trapped in tinny pores or fractures under the wetting phase pressure. This minimum capillary pressure is often termed as snap-off pressure. The corresponding saturation is irreducible gas saturation (IRGS).
Both the pore-size distribution index and the capillary entry pressure are macroscopic parameters. They can express the complexity of rock pore structure. Such a model can macroscopically match the experimental data of permeability but does not describe the interaction of gas and water from the microscopic mechanism. In fact, the effects of pore-size distribution and tortuosity on permeability should be discussed from the viewpoint of fractal dimension. From a capillary theoretical model to the integration of capillaries in different radius sizes, fractal theory can better explore the effects of complex pore structure on permeability. Besides, the capillary entry pressure is usually regarded as a fixed value in the classical Brooks–Corey model. However, this value is difficult to determine using experimental tests. In this paper, we defined the critical capillary radius, which corresponds to the capillary entry pressure. When the capillary tube size is smaller than the critical radius of the capillary, the gas cannot displace the water, and the water flow fills the entire capillary flow channel. On this sense, this part of water is the irreducible water and its saturation is called the irreducible water saturation in the two-phase flow.
2.3. Irreducible Water Saturation and Threshold Pressure Gradient
This concept of irreducible water saturation is very similar to the threshold pressure gradient (TPG) that was mentioned in our previous study [
6]. From the macroscopic view, the residual water in the target reservoir blocks the pore-throat. Only when the capillary pressure is higher than the capillary entry pressure, the two-phase flow can be observed, as shown in
Figure 3a. TPG is a vital parameter in describing the gas starting flow against viscous forces. This TPG makes the Darcy flow gradually transform to a low-velocity, non-Darcy flow when water saturation is gradually increasing. Many researchers have indicated that permeability, water saturation, and pore pressure are controlling parameters for TPG in tight gas reservoirs [
23,
25,
30]. On this sense, we proposed the following formula for TPG:
where
is the intrinsic permeability,
is the pore pressure,
is a correction coefficient for water saturation, and
and
are correction coefficients for pore pressure. These correction coefficients are also linked with shale permeability.
The accuracy of Equation (6) was checked using the experimental data from Ding et al. [
30]. Their comparison is shown in
Figure 4.
Figure 4a presents the rise of TPG with the increase of water saturation.
Figure 4b shows the effect of different permeabilities on TPG. Although TPG describes the gas-water displacement in capillary tubes, it does not consider the complex pore structure of porous media.
2.4. Calculation of Water Saturation and Irreducible Water Saturation
Based on the Laplace formula, capillary pressure can be expressed as
where
is the capillary pressure,
represents the surface tension, and
is the contact angle of gas-water-rock interface.
If the surface tension and contact angle are constant, the capillary pressure has an inverse proportional relationship with the pore radius. There is a critical capillary radius
in the complex distribution of capillary pore size. When the pore size is larger than the critical capillary radius, the gas flow can occur in the capillary tube, and the water film is attached to the capillary wall. If the capillary tube size is smaller than the critical radius
, the capillary tube is fully saturated with water and gas flow does not occur. Therefore, from the microscopic view, the gas can displace water only when the capillary tube radius is greater than the critical capillary tube radius, as described in
Figure 3b.
The water sources come from two parts: One is a single water flow
, and the other is the gas-water two-phase flow
. According to the area ratio of pores, the water saturation can be calculated by pore-size distribution and water film as [
20]
When the pore size is less than the critical capillary tube radius, there is not enough capillary pressure to further displace the water in pores. At this time, the water saturation is the irreducible water saturation and is calculated by
Figure 5 shows the variation of irreducible water saturation with critical capillary tube radius. No linear relationship was observed between the critical capillary radius and irreducible water saturation. When the critical capillary radius is large enough, the irreducible water saturation grows slowly and tends to be stable. In the case of the same capillary critical tube radius, the increase in the maximum capillary radius leads to a decrease in irreducible water saturation. The water flow is enhanced by the increase of capillary tube radius rather than being sealed in the capillary tube. When the critical capillary tube radius is small relative to the capillary tube size, the difference is not obvious. However, the irreducible water saturation changes from 0.2 to 0.4 when the critical capillary tube radius is 10 nm.
2.5. Fractal Distribution of Pores
Porous media have numerous capillary tubes with different pore sizes and tortuous lengths. These inter-pore structures are of self-similarity and can be described by fractal theory. The number of pore sizes greater than
can be expressed as
where
represents the scale of length,
and
are the maximum pore radius and pore radius, respectively, and
is the pore-size distribution (PSD) fractal dimension and in the range of
in two dimensions. Yu and Li [
31] found that this fractal dimension is related to the porosity
and the radius ratio
.
where
represents the Euclidean dimension.
Differentiating Equation (10) with respect to
obtains the following expression:
Thus, the probability density function of pore-size distribution is expressed as
Due to the tortuosity, the length of the capillary tube is higher than the straight capillary tube in complex porous media. Capillary length is related to the radius size with following fractal law [
31]:
where
and
represent the actual capillary length and representative capillary length, respectively.
is the fractal dimension of the tortuosity, and its range is between 1 and 2 in two-dimensional space. Therefore, the cross-sectional area of all pores could be written as [
20]
Thus, the representative capillary length can be expressed as
2.6. Two-Phase Flow Model in Nanopores
2.6.1. Flow Rate of Gas
The flow channels in
Figure 6 were assumed to be capillary tubes with tortuosity. SEM images showed that the pore shape was not only circular, but also slit. Ignoring the influence of pore shape will affect the understanding of the fluid flow mechanism in complex porous media. Mortensen et al. [
32] stated that the capillary channel with a circular cross-section does not reflect the complexity of various cross-sectional shapes, such as elliptic, rectangular, triangular, and harmonic-perturbed circles. We introduced a geometrical correction factor to describe different cross-sectional shapes in a unified form.
When a steady-state laminar flow occurs within capillary tubes,
Figure 7 gives the flow distribution of the gas and water phases. This conceptual model has three different regions: The gas flow region, the typical viscosity water flow region, and a high-viscosity water film region. The fluid flow in these three regions has different flow mechanisms. They are mathematically described below.
Based on the Hagen–Poiseuille equation, the gas flow rate in a capillary tube is obtained below if slip flow and free molecular flow are considered in the continuum flow regime.
where
and
are the capillary tube radius and capillary tube length, respectively,
is the pressure difference applied to the external capillary tube,
is the gas viscosity, and
represents a dimensionless rarefaction coefficient. When
changes from 0 to
, a slip flow regime transforms into a free molecular flow regime.
represents the slip coefficient and can be obtained from the linearized Boltzmann solution or velocity distribution given by the Poiseuille flow in a cylindrical tube [
35].
is the modified Knudsen number, which is the ratio of the mean free path of gas flow to the characteristic size of gas flow channel. Details are provided in the next section.
2.6.2. Geometrical Correction Factor and Real Gas Effect
Shale formation has various shapes of pores. This study introduced a geometric correction factor to express the deviation of pore shape from a circular pore channel [
36,
37].
where
is the geometric correction factor. The
is 1 for the circular pore, 1.094 for the square pore, and is 1.1186 for the equilateral triangle pore [
18].
is the gas mean free path.
where
is the gas pressure,
is the universal gas constant,
is the reservoir temperature,
is the gas molecule mass, and
is the gas compressible factor, which expresses the real gas effect on gas density and viscosity. It was noted that previous models usually neglected this real gas effect (that is
Z = 1), but this effect becomes more notable at high pressure and temperature.
can be expressed as [
38]:
where
and
are the gas critical pressure and temperature, respectively, and
–
are tuned coefficients.
Jarrahian and Heidaryan [
39] developed a generalized gas viscosity model with a range of pressures (0.1–137.8 MPa) and temperatures (241–473 K). This study described their expression of gas viscosity as
where
is the gas viscosity under the standard condition, and
,
, and
are temperature, pressure, and molar weight independently tuned coefficients, respectively.
Beskok and Karniadakis [
40] found that gas flow is in the slip flow regime when
. Combining Equations (17)–(21), we extended the gas flow rate to consider the geometric correction factor and real gas effect in a capillary tube and obtain the flow rate as
Integrating Equation (22), the total gas volumetric flow rate is expressed as
where
is the distance from the center of the circular pore to the gas-water interface and
is the critical capillary tube radius.
.
2.6.3. Water Film Effect
The water with normal viscosity occupies the most of capillary channels. Due to influences of the hydrophilicity of the matrix, the high-viscosity water forms a water film on the surface of capillary tubes. For the flow region of normal viscosity water, the governing equation can be obtained based on the Hagen–Poiseuille equation.
The governing equation of water film region is
where
and
are the water viscosity for the typical viscosity water region and water film region, respectively,
is the correction factor of the vapor flow rate, and
represents the vapor flow rate.
The ratio of these two viscosities is related to the contact angle
[
41]:
With the combined effects of temperature, pressure, and gas flow rate, the water film adhering to the surface of the channel will diffuse into the gas under evaporation reaction and be extracted with the gas. The influence of water vapor on the pressure of the gas is small and was thus ignored. However, the evaporation of the water film directly affects the flow rate of the water film. If the effect of water vapor flow rate on the water film flow rate is not considered, the water film flow rate will be overestimated. This vapor flow rate could be calculated as [
42]
where
is the molecule mass of vapor,
is the diffusion coefficient, and
is the pressure difference of vapor.
The boundary conditions for water flow and water film regions are as follows:
By substituting Equations (26)–(28) into Equations (24) and (25), the final flow velocities are obtained as
By integrating Equations (29) and (30) on the cross-section of the circular tube, the volumetric flow rate of the water are obtained as
When only water flows in the capillary tube (
), the volumetric flow rate of water can be simplified as
Similarly, combining with fractal theory obtains the volumetric flow rate of water as
where
.
2.7. Intrinsic Permeability
Intrinsic permeability is an inherent property of rock. It is only related to the rock microstructures and is thus independent of fluid type. For two-phase flow, the effective permeability of each phase depends on its saturation and intrinsic permeability. Experimental results have suggested that the effective permeability of non-wetting phase tends to be higher than the effective permeability of wetting phase [
43]. Relevant literature has summarized following reasons [
44]: (1) The rock is rich in swelling clay minerals. When the effective permeability of the wetting phase is measured, the clay mineral in the matrix absorbs water and swells. This leads to the reduction of the flow channel of fractures; (2) The existence of a water film on the structure surface reduces the effective radius of the flow channel; (3) The high viscosity of the movable water film zone increases the viscous force of normal flowing water. Thus, higher shear stress is required to start the water flow.
Figure 8 compares several sets of experimental data on the relationship between water and gas permeability. These experimental data were obtained from Busch and Hildenbrand [
43]. These data showed that the gas effective permeability is slightly higher than the water effective permeability. This is related to the complex micropore structure and the flow mechanism of two-phase flow.
Two mainstream methods are usually used to calculate the intrinsic permeability of rock. The first is the Kozeny–Carman equation or its modified form. The intrinsic permeability of rocks, especially with high permeability, is expressed as
where
is a constant,
is the average radius of grains.
represents the Kozeny–Carman constant and has
where
is the dimensionless Kozeny constant and
is the tortuosity of rock.
Another method was proposed by Yang and Aplin. This method does not only consider the pore size and porosity, but also includes the effect of mineral composition (clay content) in the intrinsic permeability:
where
is the volume ratio of pores to matrix and is the volume ratio of pores to matrix at the effective stress of 0.1 MPa, is the clay mineral content, and represents the angle between the average pore alignment angle and bedding direction.
2.8. Gas-Water Relative Permeability Model
The water flow velocity is expressed in Darcy’s law:
By substituting Equation (33) into Equation (38), the effective permeability of water is obtained as
Similarly, the effective permeability of gas is
Thus, the relative permeability for water is
and the relative permeability for gas is
In this study, our intrinsic permeability was calculated by Yang and Aplin’s method. The clay content was 0.1 and the porosity of rock was 0.2.
3. Model Validation
The above-improved fractal relative permeability model for gas and water was compared with the classic Brooks–Corey model and viscous coupling model. Our fractal model was further verified against experimental data. The parameters used in this validation are listed in
Table 1.
The comparison of our fractal model with the classic Brooks–Corey model and the viscous coupling model is presented in
Figure 9. The residual water saturation of the Brooks–Corey model was 0.2, and the pore-size distribution index was infinite.
The viscous coupling model takes the viscosity ratio of the gas and water phase into account. When the viscosity difference between the gas and liquid phase is significant, the viscous coupling model is similar to the Brooks–Corey model. Our fractal model had similar trends to the two classic models. However, our fractal model had some features that the classic models missed: (1) The pore-size distribution index in the classical model is constant and difficult to measure. However, pore-size distribution fractal dimension and tortuosity fractal dimension can be calculated by the capillary pore distribution and pore size. Through fractal dimensions, complex porous media can be better expressed; and (2) The real gas effect and water film flow are not considered in the classical models. These factors are particularly important in high-temperature, pressure, and humidity formations. Further, our fractal model was compared with experimental data, and the results are presented in
Figure 10. These experimental data were measured by Mahiya [
45] for the relative permeability of water and vapor at 120 °C. The permeability and porosity of Berea core samples used in this experiment were 1200 md and 0.24. Subsequently, the relative permeability of nitrogen and water were measured by Li and Horne [
46]. Diomampo et al. [
47] conducted drainage experiments for the rough-walled fractures, and relative permeability data of nitrogen and water were obtained. In their experiments, the fracture was initially saturated with water, and the non-wetting phase was injected with a constant flow rate. Wang et al. [
48] measured the relative permeability of oil and water in carbonate core samples. The permeability and porosity of this sample were 33.9 md and 0.18. Our fractal relative permeability model is in a good agreement with these experimental data. This indicates that this improved fractal model can describe the evolution of gas-water relative permeability in complex porous media.