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1 The mobility of fluids through rocks
2 Bhavik Harish Lodhia1 and Stuart Raymond Clark1
1
3 Department of Minerals and Energy Resources Engineering, University of New South Wales,
4 Sydney, 2052, Australia
6 Abstract
7 Over the last decade, there has been an irreversible shift from hydrocarbon exploration towards carbon
8 storage, low-carbon energy generation and hydrogen exploration. Whilst basin modelling techniques may be
9 used to predict the migration of hydrocarbons through sedimentary basins on geological timescales, there
10 remains little understanding of how fluids behave at the basin scale on present-day timescales. Maximum
11 vertical fluid velocity, vmax , may be calculated as the product of mobility and buoyancy. We present
12 an algorithm to determine the basin-scale mobilities of CO2 and methane with depth for sandstone and
13 carbonate. CO2 and methane mobility and buoyancy increase by an order of magnitude at gas phase
14 transitions and are significantly greater in sandstone than in carbonate. Critical properties of CO2 cause
15 fluid mobility and buoyancy to be sensitive to changes in surface temperature. vmax for CO2 and methane
16 are on scales of m/year. Our results indicate an optimal depth for CO2 storage of below 0.59 km and 1.24
17 km when surface temperature > 20◦ C and 0◦ C, respectively. vmax for hydrogen is approximately 2 − 10
18 times greater than other hydrocarbon fluids and this will have important consequences for the future use of
19 basin modelling software for determining hydrogen migration for exploration and storage.
20 1 Introduction
21 The last decade has seen an irreversible shift in research focus away from hydrocarbon exploration and towards
22 low-carbon energy production. This is reflected by the prioritisation of natural gas production over the use
23 of high-CO2 producing energy sources such as oil and coal, by many developed economies across the world
24 (e.g. United States 1 and Australia 3 ). Shifting priorities have led many of the world’s largest energy producing
25 companies to commit towards achieving carbon net-zero by 2050. 7;20 Hence, there is a growing interest across
26 industry and the scientific community at applying well known techniques for hydrocarbon exploration to low-
27 carbon technologies, such as carbon capture and storage (CCS) and green hydrogen exploration. Development
28 of these techniques is dependent on understanding how CO2 , hydrogen and other fluids migrate through rocks.
29 Traditionally, the history of fluid movement (e.g. hydrocarbons) through rocks across geologic time-scales has
30 been calculated by basin modelling: a process by which sedimentary basins and their associated fluids are
31 investigated to determine if the past conditions were appropriate to fill potential reservoirs with hydrocarbons
32 and preserve the potential reservoirs. 10 The ability to simulate the passage of fluids through rocks is of signif-
33 icant importance to both hydrocarbon exploration and low-carbon activities, such as CCS. A large portion of
34 processing time in basin modelling is used to solve Darcy flow equations in each grid cell of the model. Two-
35 and three-dimensional basin models may take several days to compute on a home computer. This could be
36 improved by assigning a fluid velocity that is dependent on properties of the carrier rock and depth. However,
37 determining the velocities of fluids through different rock types remains a significant challenge. The overwhelm-
38 ing majority of research on fluid flow through rocks is focused on laboratory studies of specific examples or case
39 studies or unsuccessful application of basin modelling software to simulate real-time fluid flow. 14 As we shall
40 see, the determination of fluid velocities in different rock types as function of depth will be of immense value
41 to both basin and future modelling studies for hydrocarbon exploration, CCS and potentially green hydrogen
42 exploration and storage.
43
44 In this study, we apply various Equations of State and bulk properties of common rock types to different fluids
45 encountered within the subsurface to calculate the variation of physical properties (e.g. volume and viscosity)
46 with depth and surface temperature. Depositional parameter values for two generalised rock types, sandstone
47 and carbonate, are applied in this study. 10 For carbonate, parameter values for micrite are used. Depositional
48 porosity (φ0 ) values are 0.41 and 0.51 and compaction wavelengths are 3.22 km and 1.92 km for sandstone and
49 carbonate, respectively. 10
50
51 We present an algorithm to calculate maximum vertical velocity, vmax , as a function of depth from the Darcy
52 flow equation (Equation 1). The results of this study may have important implications for the application of
1
53 basin modelling techniques to understand migration of non-hydrocarbon fluids and for threshold depths, below
54 which fluids have low mobilities.
64 The terms of Equation 1 include several important quantities that must be evaluated separately using the
65 appropriate relationships that describe fluid volume, viscosity, density and buoyancy.
Table 1: Component properties of hydrocarbon gases, hydrogen and CO2 . 9;10;13;17 MW = molecular weight,
TC = critical temperature, Pc = critical temperature, vc = critical volume, ω = acentric factor.
81 Whilst EoS may be applied to calculate fluid pressure, temperature and volume, viscosity is another important
82 indicator for phase property characterisations and fluid velocities within rocks and geological basins. Viscosity
83 is often modelled as a quantity dependent only on pressure, temperature, density and the amount of dissolved
84 gas. 9 Whilst advanced theories, such as the friction-theory or free-volume model match laboratory data well,
85 a lack of field data and unknown component parameters (especially for heavy hydrocarbon compounds) make
86 these unsuitable for basin modelling. 10
87
88 Compared to methods that require laboratory or field data, direct approaches such as the empirical Lohrenz–Bray–Clark
89 (LBC) model 15;5;6 are simpler to apply in basin modelling scenarios where data is often scarce. Viscosities can
90 be evaluated very fast due to the simple nature of the LBC–formulas. However, models with lower performance
91 are often not usable in fluid flow simulators. It must also be noted that the LBC-model is based on a polynomial
2
92 of degree 16. Polynomials of such a high degree are known to easily become numerically unstable and therefore
93 LBC-based models must be evaluated with care. 10 Furthermore, the pressure correction for gases in the LBC
94 method had a tabular formula and was not presented entirely. 15 Using this distinction introduces a disconti-
95 nuity between the liquid and gas viscosity. A modification to the LBC method may be made by applying the
96 Herning mixing rule. 11 This was validated to successfully model multicomponent and multiphase fluid viscosity
97 using the modified LBC approach for an example using the independent Stiel-Thodos method. 6;22 Hence, this
98 modified LBC method is preferred over the original LBC method. 6;15
99
100 The range of pressure and temperature (PT) paths in in Figure 1 defines an area of possible PT points in
101 arbitrary sedimentary basins. To simulate generic geological conditions, a geothermal gradient of 25◦ C/km and
102 PT gradient for normal conditions (0.5 MPa/K) was applied (Figure 1 10 ) to calculate the molar volume and
103 density of CO2 and methane by solving the PR78, SRK and RK EoS. 5;6 The modified-LBC method 6 was used
104 to calculate fluid viscosity (Figure 2).
105
106 The transition between phases (solid, dense liquid, liquid, gas and supercritical fluid) is controlled by a fluid’s
107 pressure and temperature relative to its critical pressure (Pc ) and temperature (Tc ). Figure 3 shows phase dia-
108 grams of CO2 and methane with PT paths for Ts = 0◦ C and 20◦ C. For CO2 , Pc = 7.3773 MPa and Tc = 30.98◦ C
109 and is encountered at 0.59 km under normal geological conditions. When Ts < 20◦ C, CO2 undergoes three
110 phase transitions at 0.36 km (gas-liquid), 0.59 km (liquid-dense liquid) and 1.24 km (dense liquid-supercritical).
111 However, when Ts ≥ 20◦ C, only one phase transition occurs at 0.59 km (gas-supercritical). For methane, all
112 conditions within the Earth irrespective of Ts place PT paths within the gas-supercritical region and only one
113 phase transition occurs at 0.36 km.
114
Figure 1: Typical pressure temperature (PT) paths in geological basins with a surface temperature of 20◦ C. 10
PT gradients are as follows: cool and overpressured = 2.5 MPa/K, overpressured = 1.0 MPa/K, normal = 0.5
MPa/K, hydrostatic = 0.3 MPa/K and hot hydrostatic = 0.1 MPa/K.
3
Figure 2: Fluid molar volume, viscosity, density and buoyancy calculated using various Equations of State and
modified-LBC method 6;5 and surface temperature of 20◦ C. Blue and black lines represent values calculated
using PR78 18 , SRK 21 and Reidlich-Kwong 26;16 EoS at Ts = 0◦ C and 20◦ C, respectively. Blue dashed lines
represent supercritical-dense liquid and dense liquid-liquid phase transitions for Ts = 0◦ C. Black dashed lines
represent gas-supercritical phase transition for Ts = 20◦ C (see Figure 3). The change from liquid to gas for all
fluids is marked by an exponential increase in molar volume and decreases in viscosity and density.
4
Figure 3: Phase diagram for CO2 , methane calculated at normal geological conditions and geothermal gradient
= 25◦ C/km. Blue and red lines represent PT paths calculated at Ts = 0◦ C and 20◦ C, respectively. Black lines
and points represent phase diagram for CO2 . grey lines and points represent the phase diagram for methane.
Tp = triple point, Cp = critical point.
φ = φ0 e−z/k (3)
121 whereby φ0 is the maximum (depositional) porosity and k is the Athy compaction parameter (Table 2).
122
123 The flow of fluids through rocks generally involves more than a single phase. The ability of one fluid to flow
124 through a rock or reservoir is affected by the presence of other fluids. Relative permeability, krp describes
125 multiphase flow in reservoirs as the ratio of the effective permeability of a fluid to the absolute permeability of
126 the rock. The effective permeability is a relative measure of conductance of the porous medium for one fluid
127 phase in the presence of other fluid phases.
128
129 Vertical and horizontal rock permeabilities may be calculated from hand-specimen measurements by using ap-
130 propriate anisotropy and upscaling factors. Anisotropy is the ratio of horizontal and vertical permeability and
131 is dependent on rock type. Basin scale values for horizontal and vertical permeabilities are calculated from hand
132 specimen values multiplied a horizontal and vertical upscaling factor, respectively. The resulting higher values
133 for larger scales are caused by macro-fractures, inhomogeneities and permeable inclusions. 10 Here, we apply
134 typical upscaling factors of 1 (vertical) and 50 (horizontal). However, greater upscaling factors (e.g. vertical =
135 10 and horizontal = 500) to basin scale elements with lengths greater > 50 m are reported in the literature for
136 sandstones. 19
137
Table 2: Rock properties. Anisotropy = ak . Porosity and permeability values used to generate multipoint
curves and rock saturation endpoint values for bulk rock. φ0 = maximum (depositional) porosity of rock. 10
These values were used to determine the rock permeability from porosity shown on Figure 4.
138 Numerous models for estimating relative permeability have been proposed over the last half century. Most
139 relative permeability models 4 assume relative permeability to be a function of connate water saturation (Sw )
5
Figure 4: Upscaled rock permeability and porosity. Values from Table 2 are used to calculate rock permeability
between maximum (depositional) porosity and zero. 10 A = sandstone, B = carbonate. Solid and dotted lines
represent vertical and horizontal permeability, respectively. C = porosity-depth relationship calculated using
Athy’s relation. 2 Gold and blue lines represent sandstone and carbonate, respectively.
140 and connate gas saturation (Sg ) respectively. The relative permeability of any fluid is zero below its critical
141 saturation, where it becomes immobile. Saturations are for often rescaled into normalised or effective satura-
142 tions (Se ) which map the saturation interval between the connate and the critical saturation to an interval of
143 0 < Se < 1. The relationships between normalised saturations of water, Swe , gas, Sge and oil-gas, Sgoe , are as
144 follows:
145
158 ❼ Sw calulations from resistivity logs and by application of a model relating Sw to porosity, φ, connate water
159 resistivity and lithology-dependent electrical properties.
160 ❼ Sw calculations from laboratory capillary pressure and saturation (Pcap /Sw ) measurements by application
161 of a model relating Sw to various rock, fluid properties and height above the free-water level.
162 ❼ Sw calculations using oil-based mud (OBM)-core-plug Dean-Stark-water-volume determinations.
163 ❼ Combinations of these methods
164 The amount of data that is available often dictates which method to use to determine Sw . For the purposes of
165 basin modelling, which requires the application of generalised lithologies and fluid types, Sw must be calculated
166 from data input by the user, e.g. rock type, fluid type and depth. Laboratory-based methods for measuring Sw
167 are not suitable for this work, as we are concerned with the properties of generalised rock types and fluids on
168 the basin-scale.
169
170 The results of early experiments 8 indicated that the product of φ and Sw is constant. The magnitude of this
171 constant was shown to be a related to rock type and indirectly to permeability, k. Better quality rocks were
172 found to correspond with low constant values. Extensive analysis of core data and petrophysical estimates of
173 porosity and irreducible water saturation 12 , from all types of reservoirs worldwide, suggests that this relation 8
174 is a unique solution to a more general equation:
φ Q × Sw = C (5)
175 whereby the value of the power function Q ranges from 0.8 to 1.3, with many reservoirs close to 1.0. For
176 sandstones, 0.02 < C < 0.10 and 0.005 < C < 0.06 for carbonates. The values of Q and constant C can be
6
177 easily derived by plotting logφ against logSw . The gradient of this linear plot = Q. Projection of the straight
178 line against φ = 1.0 gives the value of the constant, C. 12 Figure 5 shows the relationship between Sw and
179 φ calculated using Equation 5 and depth from Equation 3. Uncertainties may be calculated using the upper
180 and lower bounds of experimental constants and exponent terms from laboratory measurement. 12 Uncertainty
181 increases significantly as porosity is reduced through compaction (φ < 5%) and with depth. Uncertainties
182 increase significantly below 3 km and cover almost the entire range of possible Sw values by 4 km depth. Hence,
183 we have limited our modelling to this depth.
Figure 5: Connate water saturation (Sw ) as a function of porosity and depth calculated using parameters for
sandstone and carbonate 10;12 and Athy’s relation. 2 A-B = sandstone, C-D = carbonate. Grey regions represent
uncertainties calculated using upper and lower bounds of experimental constants for Equation 5 12 . Uncertainties
beyond depths of 4 km represent the full range of possible Sw values hence we do not extend this method beyond
this depth.
(1) Solve chemical equation of state (EoS) to calculate fluid volume from pressure and tempearature
(2) Calculate rock porosity (φ) and permeability at depth
(3) Calculate fluid-water relative permeability (krp ) and connate water saturation (Sw ) from porosity (6)
(4) Calculate fluid viscosity from pressure and temperature
(5) Calculate vertical fluid mobility and buoyancy
187 The results for fluid mobility and buoyancy calculations for CO2 and methane at normal geological conditions
188 for surface temperatures of 0◦ C and 20◦ C are shown on Figure 6. Gas phase mobility increases exponentially as
189 depth decreases, with maximum mobility at the surface. Non-gas phase mobilities for both CO2 and methane
190 in both sandstones and carbonates are significantly lower than corresponding gas phase mobilities and decrease
191 exponentially with depth. Fluid buoyancy follows a similar pattern.
192
193 The choice of EoS has a minimal impact on calculated fluid mobility and buoyancy for CO2 and methane. Fluid
194 buoyancies increase exponentially upon the transition to gas phase. Methane mobility varies little with Ts , with
195 results indistinguishable for Ts = 0◦ C and 20◦ C. Calculated vertical fluid mobilities for CO2 are particularly
196 sensitive to Ts . Fluid mobilities for both CO2 and methane are approximately double in sandstone compared to
197 carbonate. Whilst the magnitude of vertical mobilities of fluids vary little with surface temperature, the depth
198 of liquid-gas phase transitions vary considerably where critical properties are close to surface conditions (Figure
199 3).
7
Figure 6: Fluid mobility for CO2 and methane calculated according to Equation 1. Units for fluid mobility
are m2 Pa−1 S and buoyancy are m3 S kg−1 . Yellow and blue lines represent fluid mobility in sandstone and
carbonate, respectively. Grey lines represent buoyancy and shaded regions represent range of values calculated
using different EoS and lithological parameters for Equation 5. Dashed lines represent phase transitions: G =
gas, L = liquid, DL = dense liquid and SC = super-critical.
200 The equations used to relate relative permeability and normalised water saturation (Equation 4) are designed
201 for application to fluid systems with water, oil-water and gas-oil components. However, it is intriguing to ex-
202 tend this analysis to other fluids. The properties of several other important hydrocarbon fluids and hydrogen
203 are listed in Table 1. We apply the algorithm proposed in this study to calculate vertical fluid mobility and
204 buoyancy for hydrogen, dry/wet gas and various hydrocarbon fluids (Figures 8 and 7).
205
206 Unlike for CO2 , the vertical fluid mobilities and buoyancies of all other fluids considered in this study do not
207 show significant sensitivity to Ts . The magnitude of vertical fluid mobilities of hydrogen are up to twice those
208 of dry/wet gas and over an order of magnitude greater than other hydrocarbon fluids (volatile, light and black
209 oil). The buoyancy of hydrogen varies little with depth as all conditions within the Earth are beyond its crit-
210 ical parameters. Whilst above 0.36 km, the buoyancy of hydrogen is close to that of other gas phase fluids
211 (methane, dry and wet gas, Figure 8) and is > 8000 m3 S−1 kg−1 . Hence, this raises the important consideration
212 that hydrogen velocities may be 2 − 10 times greater than those for other fluids and must be accounted for
213 when evaluating hydrogen migration whilst applying conventional fluid flow modelling techniques suited for
214 hydrocarbon migration. The vertical fluid mobilities for volatile, light and black oils are an order of magnitude
215 smaller than those for other fluids, reflecting the fact that these remain in the liquid phase at all levels below
216 the surface. Whilst results for dry gas are close to those for methane, results for wet gas resemble the pattern
217 seen for CO2 when Ts = 20◦ C. This is expected, as conditions within the Earth exceed the critical properties
218 of wet gas (Table1).
219
8
Figure 7: Fluid mobility for non-hydrocarbon and hydrocarbon fluids listed in Table 1 calculated according
to Equation 1. Units for fluid mobility are m2 Pa−1 S and buoyancy are m3 S kg−1 . Yellow and blue lines
represent fluid mobility in sandstone and carbonate, respectively. Grey lines represent buoyancy and shaded
regions represent error. Wet and dry gas exhibit similar properties to CO2 and methane, respectively. Phase
transitions for CO2 and methane are plotted on wet and dry gas, respectively as dashed lines.
Figure 8: Fluid buoyancy calculated for other hydrocarbon and non-hydrocarbon fluids listed on Table 1
calculated using PR78 18 , SRK 21 and RK 5;6;16;26? EoS for dry/wet gas and hydrogen and using appropriate
EoS for hydrocarbon fluids. 24;25 Wet gas exhibits similar properties to CO2 at Ts = 20◦ C, whilst dry gas exhibits
similar properties to methane. Hydrocarbon fluid buoyancies are significantly lower than dry gas and methane
and decrease with molecular weight. Hydrogen buoyancy varies little with depth.
9
220 4 Discussion
221 The results of this study have several important implications. The velocity of fluids through rocks may be
222 calculated directly by multiplying vertical fluid mobility and buoyancy, according to Equation 1. Results indi-
223 cate maximum vertical gas-phase velocities of 1.5 − 4 m/year (sandstone) and 1 − 2.5 m/year (carbonate) for
224 CO2 and methane, respectively. As both vertical fluid mobility and buoyancy decrease exponentially below the
225 gas-supercritical or gas-liquid phase transition, our results indicate a minimum depth for CO2 storage 0.36 km
226 and 0.59 km when Ts = 0◦ C and 20◦ C, respectively.
227
228 The methodology presented in this study if combined with a directional vector, may provide a fast and compu-
229 tationally inexpensive means to calculate fluid velocities as a function of depth and angle of incidence between
230 fluid particles and geological horizons, e.g. impermeable seals. A potential method to calculate the direction of
231 fluid flow beneath geological seals is flowpath bending, which is widely used to model petroleum flow in basin
232 modelling software. A planar seal with dipping angle α in the y–direction and lateral water flow with angle β
233 to the x–axis and a hydraulic head with a dipping angle of γ are used to define the angle ψ, which indicates the
234 direction of fluid flow as 10 :
∆ρ cosαsinα
tanφ = tanβcos2 α (7)
ρw tanγcosβ
235 whereby ∆ρ = difference in density between fluid and water and ρw = water density. When water flow is also
236 assumed to follow the dipping of the seal, this becomes 10 :
∆ρ p cosαsinα
tanφ = tanβ 1 + sin2 βtan2 α (8)
ρw tanγcosβ
237 Combining calculations for vmax and directional vectors could significantly reduce fluid flow simulation process-
238 ing time compared to leading basin modelling software packages that rely on the creation of nodal meshes to
239 process fluid particle-rock interactions.
240
241 Modelling of CO2 and H2 storage are dependent on understanding the present-day velocities of fluids, however
242 there exists no direct method for calculating fluid velocities as a function of lithology and depth. Attempts to
243 apply basin modelling software to predict the effect of fluid injection on basin-scale pressure evolution have been
244 largely unsuccessful. 14 Whilst the assumptions used in this work are relevant for water, oil or gas fluid systems
245 in generalised sandstones and carbonates, our results could have important implications for future investigations
246 for carbon storage and hydrogen exploration.
247
248 Sedimentary basins around the world are often characterised by complex geological histories. The PT-path of
249 sedimentary basins will likely cross several regimes (e.g. different lines on Figure 1). The methodology outlined
250 in this study may be used to evaluate fluid velocities through different geological regimes (e.g. moving from
251 normal conditions to regions of overpressure) by choosing the appropriate PT-path for discrete depth intervals.
252 Future work should focus on expanding our understanding about the relationship between porosity and water
253 saturation 12 in different rock types. New experimental data for a wide range of rock types will improve Equation
254 5 and broaden the possibilities for the methodology described in this study.
255
256 It is widely accepted that hydrocarbons have the capability to migrate long distance through carriers on geo-
257 logical timescales, which indicative vertical fluid velocity calculations in literature reported at 180 km/Ma (0.18
258 m/year). 10 The results of this work indicate that CO2 , methane, dry gas, wet gas and H2 may migrate several
259 metres vertically per year (> 1000 km/Ma) when in the gas phase. It is very encouraging that these values are
260 consistent in magnitude with reports in the literature of hydrocarbon velocities of up to 1000 km/Ma 23 , and
261 indicate that the approximations used in this method are appropriate. Our results also indicate that future
262 application of basin modelling techniques and software to explore for hydrogen should account for hydrogen
263 fluid velocities that are approximately 2 − 10 times that of hydrocarbons at the same geological conditions. It
264 is encouraging that exponential increases in fluid velocities are concomitant with liquid-gas phase transitions
265 given that this is independent of rock type. Furthermore, the magnitudes of vertical match those reported for
266 hydrocarbon fluids that are of similar composition and molecular weights to the fluids analysed in this study
267 (excluding H2 ).
268
269
270 5 Conclusions
271 We present an algorithm to calculate vertical fluid mobility and buoyancy for CO2 and methane as a function of
272 depth for generic sandstone and carbonate by combining solutions to chemical equations of state, viscosity and
273 permeability calculations and the Darcy-Flow equation. Vertical fluid mobility and buoyancy in both sandstone
10
274 and carbonate decrease exponentially with depth and are significantly greater for gas phases compared to
275 liquid, dense liquid or supercritical phases. The depth of the phase transitions for CO2 is sensitive to surface
276 temperature, whereby gas-liquid and gas-supercritical transitions occur at 0.36 km for Ts = 0◦ C and 0.59 km
277 for Ts = 20◦ C, respectively. Surface temperatures > 0◦ C push the pressure-temperature profile of CO2 into the
278 gas-supercritical region. Hydrogen velocities may be approximately 2 − 10 times greater than those of CO2 ,
279 methane, dry and wet gas and over an order of magnitude greater than for other hydrocarbon fluids. Dry
280 and wet gas follow similar trajectories as methane and CO2 . Vertical fluid mobility and buoyancy of other
281 hydrocarbon fluids (volatile, light and black oil) are an order of magnitude smaller than those of CO2 , methane
282 and dry/wet gas.
283 6 Acknowledgements
284 This work was supported by the Australian Research Council grant number GA85582. Special thanks are given
285 to Dr Juerg Hauser (CSIRO) and Mr Zakhar Lanetc (UNSW) for their discussions during the completion of
286 this work.
11
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