International Journal of Coal Geology 86 (2011) 342–348

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International Journal of Coal Geology

j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / i j c o a l g e o

Gas diffusion behavior of coal and its impact on production from coalbed
methane reservoirs
Mallikarjun Pillalamarry, Satya Harpalani ⁎, Shimin Liu
Department of Mining and Mineral Resources Engineering, Southern Illinois University, Carbondale, Illinois 62901-6603, United States

a r t i c l e i n f o a b s t r a c t

Article history: This paper discusses the results of an experimental study carried out to study and evaluate the sorption and
Received 4 January 2011 diffusion properties of methane in Illinois basin coals. As a first step, sorption results were modeled using the
Received in revised form 25 March 2011 Langmuir isotherm model and the Langmuir Constants were estimated. Next, the diffusion coefficient, D, was
Accepted 25 March 2011
estimated by modeling experimental data using the unipore diffusion theory and Fick's law of diffusion. The
Available online 31 March 2011
results clearly indicated a negative correlation between D and pressure for pressures below 3.5 MPa. The
Keywords:
overall trend of the variation was found to be bi-modal, its value remaining constant at high pressures,
Methane diffusion followed by a sharp increase below this critical pressure. Finally, a comparison of the sorption and diffusion
Fick's law results revealed that D depended on the surface coverage, which exhibits a positive relationship with
Unipore model pressure. The trend of diffusion variation with pressure appeared to be in good agreement with the results
Sorption isotherms reported in the past studies using the bi-disperse diffusion model. The practical implication of the results is
that the movement of methane is eased significantly at low pressures. Given the low in situ pressure typically
encountered in the Illinois basin, this is a positive finding. Finally, this behavior may be responsible, at least in
part, for the increased gas production rates encountered in the San Juan basin after several years of
production.
© 2011 Elsevier B.V. All rights reserved.

1. Introduction and background
Coalbed methane is as an abundant, low cost, energy fuel that has
significant long-term potential for discovery and development.
Methane production from virgin coal seams in the US, almost zero
in 1980, increased to 91 Bcf (billion cubic feet) in 1989 and 2 Tcf
(trillion cubic feet) in 2008, contributing almost 10% of the US natural
gas production (US EIA, 2009). The estimated gas-in-place in the US
coals has increased from 400 Tcf (Bell and Rakop, 1986) to more than
700 Tcf (USGS, 2000).
Coal has unique characteristics, such as, pore structure, gas storage
and flow mechanisms that require a different production approach
than that employed in conventional gas reservoirs. First, the pore
structure of coal is highly heterogeneous, with pore size varying from
a few Angstroms to frequently over a micrometer in size (IUPAC,
1982). Second, coal is characterized as a dual porosity system (Warren
and Root, 1963), where the primary porosity consists of micropores
associated with the coal matrix and secondary porosity system of
macropores. The micropores occur as a part of the coal matrix,
providing extremely large internal surface area with a strong affinity
to certain gasses, like methane, ethane and CO2. The coal matrix stores
~ 95% of the total gas available in adsorbed form (Gray, 1987). The
⁎ Corresponding author. Tel.: +1 618 453 7918; fax: +1 618 453 7455.
E-mail address: satya@engr.siu.edu (S. Harpalani).
secondary porosity system, on the other hand, consists of a naturally
occurring network of closely spaced fractures, surrounding the matrix
blocks of coal, called the cleat system, and provides the flow paths for
gas and water. The cleat spacing is fairly uniform, ranging from a
fraction of an inch to several inches (Rogers, 1994).
Typically, virgin coalbeds in the US are saturated with water, that
is, cleats are filled with water and water pressure holds the methane
in place. De-pressurization of the coalbed by pumping out water from
the cleats results in release of adsorbed methane. Subsequently, the
released gas moves to the depressurized zone. Commonly, gas
transport in coal is considered to occur in two stages: gas flow within
the coal matrix and flow in the cleat system. Flow through the cleat
system is believed to be pressure-driven, and described using Darcy's
law. Flow through the matrix is assumed to be concentration
gradient-driven and is usually modeled using Fick's Second Law of
Diffusion (Harpalani and Chen, 1997). The general process of gas
transport in coal is schematically shown in Fig. 1.
Although micropore diffusion is considered a single process, it is
usually a combination of three types of diffusion: Knudsen (where
molecule–wall collisions dominate), surface (transport through
physically adsorbed layer) and bulk (molecule–molecule collisions
dominate) (Shi and Durucan, 2003). When the mean free path of the
gas molecules is greater than the molecular diameter, or when the
pressure is very low, Knudsen diffusion takes place, and gas molecules
flow from higher to lower gas concentration (Collins, 1991; Zhao,
1991). In this mechanism, the gas molecules collide more frequently

0166-5162/$ – see front matter © 2011 Elsevier B.V. All rights reserved.
doi:10.1016/j.coal.2011.03.007
 M. Pillalamarry et al. / International Journal of Coal Geology 86 (2011) 342–348 343

Fig. 1. Gas transport mechanisms in CBM reservoirs (King, 1985).

with the walls of the flow paths than with other molecules
(Thorstenson and Pollock, 1989). Broadly, the resistance to flow is
not due to the intermolecular collisions, but rather due to gas
molecules colliding with pore walls. Bulk diffusion, on the other hand,
is the opposite of Knudsen diffusion, occurring at higher pressures
(Collins, 1991), or where the pore diameter is larger than the mean
free path of gas molecules. The resistance to diffusion comes primarily
from collision between gas molecules. Finally, surface diffusion of gas
occurs when adsorbed gas molecules move along the micropore
surface like a liquid (Collins, 1991). At room temperature, surface
diffusion is much smaller than the Knudsen diffusion and is typically
ignored in CBM production. Overall, the micropore diffusion can be a
complex parameter, which often includes more than one type of
diffusion.
A significant amount of work has been completed in the area of
modeling diffusion coefficient (D) for methane and CO2 in coal (Busch
et al., 2004; Charrière et al., 2010; Clarkson and Bustin, 1999b; Cui et
al., 2004; Kumar, 2007; Mavor et al., 1990; Nandi and Walker, 1970;
Saghafi et al., 2007; Shi and Durucan, 2003; Siemons et al., 2007).
Clarkson and Bustin (1999b) showed that the kinetics of adsorption at
low and high pressures depends on the nature of the gas, moisture
content, and temperature. Furthermore, diffusion of CO2 in coal is
higher than methane and this is attributed to the physico-chemical
properties of the molecules, such as, size and polarity as well as gas
interaction in coal. Cui et al. (2004) used the bi-disperse diffusion
model to calculate the diffusion coefficient for coal and methane,
carbon dioxide and nitrogen systems at varying gas pressures and
found a negative correlation between diffusion coefficient and reservoir
pressure. Similar studies were conducted by Busch et al. (2004), Kumar
(2007), Saghafi et al. (2007) and Shi and Durucan (2003). Both unipore
and bi-disperse pore methods were used successfully to model diffusion
in coal and it was concluded that both models can be used effectively
for modeling of methane diffusion in coal.
This paper describes a study carried out to characterize methane
diffusion properties of coals in the Illinois basin. Since the primary
objective of the study was to establish the variation trend in the
diffusion coefficient with gas depletion, the unipore model was used
rather than the bi-disperse model to avoid complex mathematical
calculations. A comparison of the results obtained in this study, and
the study carried out by Cui et al. (2004) using bi-disperse model, is
presented at the end.
average radius of 0.0143 cm. Although crushing the coal changes the
surface area for gas adsorption, the increase for 40–100 mesh coal size
is between 0.1 and 0.3%, which is not believed to affect the accuracy of
the experiment (Jones et al., 1988). Furthermore, the effect of grain
size on diffusion was studied by Busch et al. (2004), Nandi and Walker
(1970), and Siemons et al. (2003). The results showed that there is no
effect of grain size when the particle radius is greater than 0.1 mm. In
this study, the average particle radius was 0.143 mm. Moreover, the
purpose of grinding the coal to this size is to reduce the diffusion time
and to eliminate the effect of cleats on diffusion since, flow through the
cleat system is believed to be pressure-driven. Prior to starting an
experiment, approximately 90 g of pulverized sample was placed in
environmental chamber for ~ 48 h at reservoir temperature (73 °F)
and humid conditions (99%) for moisture equilibrium. Six grams of
sample was used for moisture and ash analysis following the ASTM
procedures (ASTM D3173-87, 1987; ASTM D3174-04, 2004), and the
rest was used for the sorption/diffusion experiment.
2.2. Experimental setup and procedure
The experimental setup consisted of a sample cylinder and a
reference volume, both capable of withstanding high pressures. The
sample cylinder was connected to the reference volume through a
two-way valve and a micro-filter to prevent movement of coal
particles with sudden changes in pressure. Since the diffusion/
sorption is extremely sensitive to temperature, the entire setup was
placed in a constant-temperature bath, capable of maintaining the
temperature to within 0.2 °C of the desired temperature. This not only
ensured constant temperature throughout the experiment, but also
allowed carrying out the experiment at in situ temperature. A
schematic of the experimental setup is shown in Fig. 2. Precise

2. Experimental setup and procedure

2.1. Sample procurement and preparation

Blocks of coal were obtained from two different seams in the Illinois
basin. The most commonly used technique, particle method, was used
to estimate the diffusion coefficient. This involves grinding the coal to
eliminate the cracks and macropores completely, ensuring that the
movement of gas is purely diffusive in nature. In order to prepare
appropriate samples, coal was first broken into lumps approximately
half-inch in size. These were then ground and sieved to obtain the
desired sample size of 40–100 mesh (0.0425–0.0149 cm), giving an Fig. 2. Schematic of experimental setup used for diffusion/sorption experiments.
344 M. Pillalamarry et al. / International Journal of Coal Geology 86 (2011) 342–348
monitoring of pressure variation in the sample container is critical in
order to calculate the amount of gas diffusing from within the coal
matrix. Hence, a highly sensitive pressure transducer was connected
to the reference volume which was subsequently connected to a data
acquisition system (DAS), capable of recording pressure data at very
short time intervals.
Prior to starting a diffusion experiment, calibration of the setup
was carried out. This involved determining the volume of the void
space in the sample container using a non-adsorbing gas, like helium.
Diffusion tests were performed for increasing and decreasing pressure
steps and designated as adsorption/desorption steps. Initially, the
pressure in the sample container was set to zero. The reference
volume was subjected to a pressure of 1 MPa and allowed to
equilibrate. The valve between the sample container and reference
volume was then opened. The DAS was programmed to take readings
at half-second intervals at this stage since methane adsorption rate is
extremely high during the initial period. Acquiring data at this pace
continued until the pressure variation became insignificant, in this
case, 0.7 kPa/h. Readings were then taken at 50 s intervals and
continued for approximately 20 h, after which, there was negligible
change in the pressure and the sample was believed to have attained
equilibrium. The coal sample was now believed to be fully saturated
with methane at the equilibrium pressure. The procedure was
repeated for a step-wise pressure increment of ~1 MPa, to a final
pressure of ~7 MPa. Following this, the entire procedure was repeated
for decreasing pressure steps of 1 MPa.
3. Measurement technique
3.1. Ad/de-sorption isotherm
The pressure data recorded during each step of the experiment
was used to establish the adsorption isotherm, a natural by-product of
the diffusion experiment. The amount of gas adsorbed at a given
pressure was calculated using the Gibbs isotherm principle. Gibbs
adsorption isotherm calculation assumes constant void volume
within the coal throughout the pressure steps. It neglects the volume
occupied by the adsorbed gas at each pressure step when calculating
the amount of “free” gas. The difference between Gibbs and absolute
adsorption is significant at high pressures, and the relationship used
to calculate the absolute volume is given as (Sudibandriyo et al.,
2003):
VGibbs
Vabs = ρgas
1

ρads
where, Vabs and VGibbs are the absolute and Gibbs sorption respectively,
and ρgas and ρads are gas densities in gaseous and adsorbed phases
respectively. The phase density for adsorbed methane used to calculate
the absolute adsorption was 0.421 g/cm3 (Sudibandriyo et al., 2003).
The isotherm was established using the Langmuir isotherm model,
given as:
PVL
V=
P + PL
where, P is the equilibrium gas pressure, V is the volume of gas
adsorbed, VL is the Langmuir Volume representing the maximum
volume that can be sorbed at infinite pressure, and PL is the Langmuir
Pressure at which the sorbed volume is half the Langmuir Volume.
3.2. Estimation of diffusion coefficient
Various approaches have been used by past researchers to model
kinetics of gas sorption on coal. Two diffusion models, based on the
pore structure of coal, that have been successfully used in prior studies
are the ‘unipore’ and ‘bi-disperse’ models (Busch et al., 2004; Nandi
and Walker, 1970; Ruckenstein et al., 1971; Shi and Durucan, 2003). In
this study, the data was modeled using the unipore approach, since
most CBM/ECBM reservoir simulators are based on a single-step
unipore diffusion model.
As the name suggests, unipore model assumes that all the pores in
the coal matrix are of the same size (Crank, 1975). The basis of this
model is the Fick's Second Law of Diffusion for spherically symmetric
flow. The model also assumes a constant gas concentration at the
surface of the spheres throughout the sorption process. Although this
method does not provide a perfect fit of the measured data, it is
considered adequate as a first-order approximation for the purpose of
making a first estimate of the sorption rates in a specific coal reservoir.
For homogeneous spherical particles with a constant surface
concentration and isothermal conditions, Fick's Second Law, is given
as (Crank, 1975):
" #
Mt 6 ∞ 1
2 2
Dn π t
= 1− 2 ∑ 2 exp − ð3Þ
M∞ π n=1 n r2p
where, Mt is the total mass of the diffusing gas that has desorbed in
time t, M∞ is the total desorbed mass in infinite time, and D is the
diffusion coefficient, and rp is diffusion path length. After a step
change in the surface concentration, the relationship for desorbed gas
can be expressed as (Clarkson and Bustin, 1999b):
" #
Vt 6 ∞ 1 Dn2 π2 t
= 1− 2 ∑ 2 exp − ð4Þ
V∞ π n=1 n r2p
where, Vt is the total volume of gas ad/de-sorbed in time t and V∞ is
the total gas adsorbed or desorbed after infinite time. For short times
(t b 600 s) and when the fraction of gas desorbed (Vt/V∞) is less than
0.5, the Eq. (4) can be approximated to:
sffiffiffiffiffiffiffiffiffi
Vt Dt
=6 : ð5Þ
V∞ πr2p
Several researchers have used the unipore approach to fit their
experimental sorption data (Clarkson and Bustin, 1999b; Mavor, et al.,
1990; Smith and Williams, 1984). They concluded that the unipore
diffusion model is more applicable at high pressure steps of the
ð1Þ
isotherm rather than all of the steps.
4. Results and discussion
4.1. Ad/de-sorption isotherms
The experiments were performed on both samples at in situ
temperature of 73 °F and pressures up to 9 MPa. Experimental
isotherms for adsorption and desorption steps are shown for the
two coal types in Fig. 3 (Ref: Table 1). The isotherm shows that
desorption hysteresis is insignificant. Ideally, desorption isotherm for
ð2Þ
coal and methane should not deviate from the adsorption isotherm
since the sorption process is purely physical in nature and is reversible
(Ruthven, 1984). Laboratory based isotherms typically exhibit some
hysteresis due to the fact that the moisture content of the sample
varies somewhat between the two isotherms (Dutta et al., 2008;
Harpalani et al., 2006). A part of the sample moisture is removed
during desorption every time gas is bled out. Another reason for the
hysteresis, pointed out by previous researchers, is that there may be a
change in the properties of the adsorbate. When the adsorbent/
adsorbate system is in a metastable state, a decrease in pressure does
not release the gas as readily (Busch et al., 2003).
 M. Pillalamarry et al. / International Journal of Coal Geology 86 (2011) 342–348
16
12
Sorption, ml/g
8 8
Sample1-Adsorption
4 Sample1-Desorption
Sample2-Adsorption
Sample2-Desorption
0 0
0 1 2 3 4 5 6 7
Pressure, MPa
Fig. 3. Experimental absolute ad/de-sorption isotherms for methane.
Since it is the desorption part of the experiment that truly
replicates the CBM operations, only desorption data was modeled
using the Langmuir isotherm. Langmuir isotherms for the two coal
types are shown in Fig. 4. The Langmuir parameters obtained for the
samples, along with proximate analysis results, of the two coal types
are presented in Table 1. It is apparent that all isotherms are of Type 1,
according to Brunauer's classification (Brunauer et al., 1940). The
relative errors of deviation of Langmuir-predicted values were
calculated to be 2.5%. These levels of error are acceptable (Dutta et
al., 2008).
Gas sorption capacity of coal is typically influenced by pressure
and temperature, the actual moisture content, composition of the
organic material, mineral content, coal rank and meceral composition
(Crosdale et al., 1998; Hildenbrand et al., 2006; Krooss et al., 2002). It
is evident from Fig. 4 that Sample 1 has a higher sorptive affinity for
methane than Sample 2 although the depth from which these were
retrieved was almost the same. The volatile matter and fixed carbon
content are also fairly close. Hence, the slight difference in the results
obtained for the two samples may very well be the result of other
controlling factors, such as, ash content, volatile matter and meceral
composition.
4.2. Estimation of diffusion coefficient
Compared to measurements for sorption isotherm, where only the
final equilibrium pressure is required, measurement of diffusion
coefficient requires precise and continuous change in pressure in the
sample container over time, especially during the initial period of
desorption when the rate of diffusion is extremely fast. This was
repeated for every pressure step, that is, every time pressure in the
sample container was changed to ad/de-sorb the gas. Decrease/
increase in the gas pressure of the sample container was converted to
the amount of gas ad/de-sorbed. The frequency of data collection was
decreased as equilibrium approached. Also, for calculation of the
diffusion coefficient, only the initial sorption period (Vt/V∞ ~ 0.5) was
considered, when the gas sorbs at a relatively fast pace. The change in
gas content was calculated for each time interval during a pressure
step. The fraction of gas (Vt/V∞) desorbed over time for the desorption
steps of Sample 2 is shown in Fig. 5. The model, derived from Fick's
Table 1
Langmuir constants for desorption isotherms.
Sample Depth Volatile Fixed
(m) matter (%) carbon (%)
Sample 1 154 35 48
Sample 2 145 37 46
345
16
12
Sorption, ml/g
Sample1-Experimental Data
4 Sample1-Langmuir Isotherm
Sample2-Experimental Data
Sample2-Langmuir Isotherm
8 0 1 2 3 4 5 6 7 8
Pressure, MPa
Fig. 4. Langmuir isotherm models for desorption data.
Law, and described by Eq. (4), was used to calculate the diffusion
coefficient for each step. The results depicting the variation in the
value of diffusion coefficient for adsorption and desorption steps with
pressure for the samples are shown in Fig. 6. The overall trend
exhibited by all the results is very similar.
It is apparent from the figures that there is a negative correlation
between diffusion coefficient and pressure below 3.5 MPa, both for
increasing as well as decreasing pressure steps. This suggests that the
ease with which methane moves in the coal matrix improves with
pressure reduction, or with continued gas production in the reservoir.
However, since desorption part of the experiment truly replicates a
CBM operation, the diffusion variation trend analysis was carried out
for this alone. This is shown in Fig. 7. The diffusion variation trend is
consistent with other diffusion results that have been reported by
Clarkson and Bustin (1999a, 1999b), Cui et al. (2004), Wei et al.
(2007) who studied the diffusion/adsorption of methane at different
pressures using the bi-disperse model. Cui et al. (2004) observed that
both micropore and macropore diffusions decrease with increasing
adsorption. Reduction in diffusion coefficient with increased adsorp-
tion may be attributed to two reasons: (1) the effect of coal matrix
swelling on pore size because adsorption swelling may narrow some
micropore entrances and increase the resistance to diffuse the gas
molecule through (Cui et al., 2004); and (2) strong repulsive force
between adsorbed molecules with increase in surface coverage (Chen
and Yang, 1991). However, a few researchers have reported that
pressure is not directly related to the rate of adsorption or desorption
for coals, Nandi and Walker (1970) for pressures below 2 MPa, and
Sevenster (1959) for pressures below 0.1 MPa. Moreover, the results
of this study contrast the observation made by Nandi and Walker
(1970) stating that the diffusion coefficient increases with average
methane concentration at high surface coverage.
Finally, Charrière et al. (2010) and Nandi and Walker (1970)
observed a surface cover dependency of the diffusion coefficient for
methane and CO2 on coals. Their results showed a positive correlation
between the diffusion coefficient and surface coverage (sorbed
volume). To test this conclusion, desorption isotherm was plotted
along with the variation in the value of diffusion coefficient for one of
the samples. This is shown in Fig. 8. There is clear indication that the
two are almost mirror images of each other. The observed trend was
similar for the second coal type tested. Moreover, it is also apparent
Ash Moisture Temperature Desorption
(%) (%) (°F)
VL (ml/g) PL (MPa)
9.3 2.3 73 16.5 1.84
13 1.1 73 15.4 2.7
346 M. Pillalamarry et al. / International Journal of Coal Geology 86 (2011) 342–348

Diffusion Coeffcient, x10-10 cm2/sec

1 45
40 Sample1
0.8 Sample2
35
Fraction Sorbed

30
0.6
25
38.2E-10 cm2/sec
26.7E-10 ,, 20
0.4 12.5E-10 ,,
4.70E-10 ,, 15
3.10E-10 ,,
2.40E-10 ,, 10
0.2 2.10E-10 ,,
5
0
0 0 1 2 3 4 5 6 7 8
0 10 20 30 40 50
Pressure, MPa
Time, Hours
Fig. 7. Variation of diffusion coefficient for desorption data (gray band is a free-plot
Fig. 5. Fraction of gas desorbed with time for Sample 2. trend line to emphasize the general trend).

from Fig. 6 that the diffusion coefficient for adsorption steps is slightly 4.3. Effect of varying diffusion coefficient on gas production
higher than for desorption steps. A similar observation was reported
by other researchers (Dutta et al., 2008; Harpalani et al., 2006) during A preliminary and basic simulation study, using the simulator
the sorption process, where adsorption isotherm was slightly higher package COMET3, was carried out to investigate the effect of varying
than the desorption isotherm. Hence, this corroborates the findings diffusion coefficient on continued gas production for a period of
that both diffusion and surface coverage are related, and in this case, 10 years. Since the permeability and diffusion coefficient influence the
negatively related below 3.5 MPa. gas transport in coal, both parameters were considered as variables.
The overall diffusion versus pressure trend established suggests The simulation results are shown in Fig. 10. The results show that, for
that the variation in the value of diffusion coefficient with pressure is a high permeability reservoir (25 md), increase in diffusion coefficient
bi-modal in nature. At high pressures, its value remains fairly from 2.4 × 10− 10 cm2/s to 38.2 × 10− 10 cm2/s resulted in increased
constant. However, after a certain pressure, the value of diffusion production. The value of D remained constant throughout the period
coefficient starts to increase, the rate of increase being almost simulated since the simulator is not capable of handling a variable D. It
exponential, suggesting that substantial desorption is responsible is apparent from Fig. 10 that the increase in gas production is not
for the increase in the value of diffusion coefficient. Alternatively, significant for a low permeability reservoir (14 md), suggesting that
desorption is the result of a significant increase in the value of the diffusion is not the controlling mechanism in gas production for low
diffusion coefficient. This finding can have a significant impact on permeability reservoirs. Nevertheless, this is inconclusive since the
projecting methane production from coals at low pressures, that is, simulator used in the modeling exercise is not very sensitive to
after substantial depletion. The finding would also have a significant diffusion coefficient. This may very well be due to the well accepted
impact on our understanding of the release of methane from belief in the past that production of methane in CBM reservoirs is
abandoned mines and release of methane in worked out and sealed permeability controlled rather than diffusion controlled. Although
coal mining gob operations. this is believed no longer to be the case, most simulators have not
As a final exercise to evaluate the difference between using the been modified to reflect this change. The ideal simulation would be
unipore versus the bi-disperse theory when estimating diffusion possible only if a variable value of D could be used, perhaps something
coefficient in the laboratory, results obtained by Cui et al. (2004) were that the developers of the various simulator packages need to
compared with those obtained in this study. Fig. 9 shows the two consider.
trends together. It is apparent that, for the purpose of establishing
variation trends, the two theories give almost identical results.

16 50
Diffusion Coeffcient, x10-10 cm2/sec
Diffusion Coeffcient, x10-10 cm2/sec

60
40
12
Sample1Adsorption Step
50
Sorption, ml/g

Sample1 Desorption Step

Sample2 Adsorption Step Desorption Data Points 30
Sample2 Desorption Step Langmuir Isotherm
40
8 Diffusion Coefficient Data Points

30 20

20 4
10
10
0 0
0 0 1 2 3 4 5 6 7 8
0 1 2 3 4 5 6 7 8 Pressure, MPa
Pressure, MPa
Fig. 8. Desorption isotherm and variation in D with pressure for one sample (gray band
Fig. 6. Variation in the diffusion coefficient with pressure. is a free-plot trend line to emphasize the general trend).
 M. Pillalamarry et al. / International Journal of Coal Geology 86 (2011) 342–348 347

9 prolific basin in the world, is that diffusion might be playing a

Apparent Diffusivity x10-6, Sec-1
8 Bi-disperse Model
significant role in later stages of the life of a CBM reservoir and
7 Unipore Model might even explain the increased production rates typically
observed in the basin during the later part of the reservoir's life.
6
• The analysis of the adsorption and diffusion results revealed that the
5 diffusion coefficient also depends on adsorption or surface coverage.
4 These results support the observations made by Clarkson and Bustin
(1999a, 1999b), Cui et al. (2004) who used bi-disperse methods to
3
model the experimental data. Since adsorption is different for
2 different gasses, variation in the value of diffusion coefficient should
1 be measured as a function of gas-in-place composition. For the same
reason, the value of D should be measured for coal–CO2 system as
0
0 1 2 3 4 5 6 7 8 9 well. In a scenario where CO2 is injected in coalbeds to enhance the
Pressure, MPa CBM production, or CO2 sequestration, there is counter-diffusion in
the matrix, with CO2 diffusing in to, and methane diffusing out of,
Fig. 9. Comparison of results using the unipore and bi-disperse models (re-constructed the matrix. An effort was initiated by Wei et al. (2007) to develop
after Cui et al., 2004) (gray band is a free-plot trend line to emphasize the general
trend).
this theoretically but no studies have been reported to date to do so
effectively, nor have there been studies to validate any theoretical
models.
5. Summary and conclusions • The pore-size distribution within coal varies with coal type, basin,
rank, etc. and is highly heterogeneous (Clarkson and Bustin, 1999a).
Methane adsorption and diffusion characteristics of Illinois basin Hence, no model can perfectly fit the experimental data unless it
coals were established using the volumetric method. The Langmuir considers all pores of different sizes that exist in coal, which may not
equation was used to model sorption data and unipore model to be possible due to mathematical complications. Although unipore
estimate the behavior of diffusion coefficient. Based on the work method used in this study does not provide a perfect fit of the
completed, the following conclusions are made: measured data, the results showed that it may be adequate for
making a first-estimate of the trend of this gas transport
• The value of diffusion coefficient is not constant over the life of a phenomenon in CBM reservoirs. Hence, the use of the unipore
CBM reservoir. There is a negative correlation between diffusion model of diffusion is definitely justified even if the bi-disperse
coefficient and pressure in the low pressure range. This finding has a model of diffusion represents the coal particle properties better. The
significant practical implication. First, since the pressures encoun- unipore model is simpler and easy to use and gives very similar
tered in Illinois coals are typically low, this can have a positive results for the variability of diffusivity as a function of reservoir
impact on methane production from coals in the basin. Second, pressure.
current simulators incorporate the diffusion parameter using the • Based on the preliminary simulation study, gas production from low
‘sorption time’, which is considered to be constant for the entire permeability reservoirs is not controlled by diffusion although this
production period and this is simply not the case. Therefore, may be due to the simulator algorithm, which underplays the
sorption time should be treated as a variable when simulating long/ importance of diffusion. However, for high permeability reservoirs,
short-term production. Modification of the simulators to incorpo- application of varying diffusion characteristics can become a
rate this change should not be much of a challenge since controlling factor in methane production. The authors do believe
permeability is already considered a dynamic parameter in several that the philosophy that methane production from coalbeds is
simulators. In fact, using the diffusion coefficient as a direct input permeability-controlled should be re-evaluated.
parameter would make more sense rather than impacting its impact
using sorption time.
• The value of diffusion coefficient can be represented by a dual Acknowledgments
model, its value remaining constant at high pressures, and
increasing continuously when accompanied by substantial desorp- This study was carried out with support, in part by grants made
tion of gas. An important extrapolation of this finding to other possible by the Illinois Department of Commerce and Economic
basins, particularly the San Juan, which is considered the most Opportunity (DCEO) through the Office of Coal Development and the
Illinois Clean Coal Institute (ICCI). The authors wish to thank these
organizations for the financial support.
50
25 md Permeability, 2.40E-10 cm2/sec DC
Production per Well, MSCFD

25 md Permeability, 38.2E-10 cm2/sec DC

2
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