Mechanism of gas flow through coal

F. S. Karn, R. A. Friedel and A. G. Sharkey, Jr

Spectra-Physics, Pittsburgh Energy Research Center, U.S. Energy Research and Develop-
men t Administration, 4800 Forbes Avenue, Pittsburgh, Pa. 752 13, USA
(Received 25 February 7975)
(Revised June 1975)

Coals are fossilized plant material plus inorganic silt deposited in irregular layers and
containing l-20% void space which provides a medium which is porous to gas flow.
Gas flows have been measured using discs of coal cut from several coal seams. Observed
flow phenomena include molecular diffusion (low gas pressure, small pores) and bulk dif-
fusion (higher gas pressure, larger pores). In the examples investigated, methane flows
ranged from 1.2 X lo-lo cm* s-l atm-l for Pittsburgh-seam attrital coal to 2.0 cm* s-l
atm-’ for Oklahoma Hartshorne coal. Flow characteristics have been compared with gas
flows observed by Knudsen through glass capillaries. This information can be applied to
mine safety and to coal utilization studies.

Since methane has been found in most coal deposits and
constitutes a serious fire hazard to miners, many studies
have been made of methane flow through the voids in
coa11-3. In the present study discs or cylinders of coal were
cut from several coal seams and tested in the laboratory
for methane diffusivity. Since the voids in coal include
micropores, macropores and cracks, it was expected that
gas flow data would vary between individual samples from
the same seam. A variety of flow phenomena were
observed.
(a) A very slow gas flow through the fine-pore structure
of coal has been described as molecular or Knudsen dif-
fusion4. It is characterized by low pressure and small pores;
the mean free path of the gas molecule approaches the
diameter of the pore. The rate of flow in such a system is
independent of both the gas viscosity and the gas pressure
but is proportional to [molecular weight] -I/2 and to
pressure differential. Diffusion of a single gas can be
described by equation (1):
Q is the volume of gas flowing per second (cm3 s-l); A is the
area of the coal face (cm2); D is the diffusion constant (cm2
s-l atm-l); Q is the gas concentration gradient (atm*); dx
is the thickness of the coal sample (cm).
This relation was shown by Knudsen’ to describe the gas
flow at low pressures through glass capillaries. In the present
work the geometric measurements of the face area and the
sample thickness are normally used. These are empirical
values since gases obviously flow through the void system of
the coal, but the values calculated using equation (1) are
particularly useful in estimating flow through a coal seam.
Gas flow mechanisms can be more accurately defined if pore
dimensions are available for coals.
(b) More rapid flow at higher gas pressures has been
described as permeability, bulk-diffusion or Poiseuille
flowb. The flow is proportional to the average pressure of
--___- -------
* 1 atm = 101.3 kPa
the system and the pressure differential. Thi s type of gas
flow is inversely proportional to gas viscosity. For a single
gas, permeability can be described by equation (2):
Q=AKp 2 (2)
dx
where K is the permeability constant (cm s-l atm-*) and
p is the average pressure (atm). This flow phenomenon was
also observed by Knudsen’ using gases at higher pressures
flowing through glass capillaries of measured radius and
length.
EXPERIMENTAL WORK
In this study, coal samples were cut in the form of plugs
1.3 cm in diameter and varying between 0.1 and 10 cm
thick. The plugs were sealed into glass or metal tubes (using
epoxy cement) to form a gas reservoir on one side and a
sampling cavity on the other. The coal samples were evacu-
ated and many successive measurements were made on each
sample to obtain data representing steady state conditions.
Diffused gases were analysed by mass spectrometry as
described previously’.
Coals tested were:
1. Pittsburgh seam (hvAb) attrital coal. A very dense coal
with only a trace of a bedding plane; sometimes known as
splint coal.
2. Pittsburgh seam (hvAb) non-attrital coal. A less dense
coal with a well-defined bedding plane.
3. Pocahontas No. 3 (lvb) non-attrital coal.
4. Oklahoma Hartshorne (lvb) non-attrital coal.
5. Illinois No. 5 (hvCb) non-attrital coal.
6. Illinois No. 6 (hvBb) non-attrital coal.
R ESU LTS
Diffusion coefficients have been calculated as the volume of
gas (standard temperature and pressure) flowing at a rate of

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Mechanism of gas flow through coal: F. S. Karn, R. A. Friadel and A. G. S,barkey

Table 1 Methane flow through various coals at 25’C, 0.5 would be expected along the bedding plane of any undisturb-
atm average pressure and I.0 atm pressure differential ed coal seam. A generally slower flow across the bedding
plane might be interrupted by a fast flow at a natural or
Coal Flow (cm* s-’ atm-‘) man-made crack in the coal. Contrary to this expectation,
-~- -__ the two coals examined here were much alike with reference
Pittsburgh attrital 1.2 x IO-10 to their bedding planes (Table 3). Since mining proceeds
Pittsburgh non-attrital 3.0 x IO-5 along the bedding plane, the remaining samples in this study
Illinois No. 6 7.1 x 10-4 were similarly oriented.
Illinois No. 5 4.0 x 1o-3
Pocahontas No. 3 O-1 Molecular weight af gas
Oklahoma Hartshorne 2.0 Methane is the gas of primary interest in coal mines but
by comparing methane with other gases some diffusion
chararacteristics become obvious. Coals of widely vary-
Tab/e 2 Comparison of methane flows through duplicate
ing porosity were tested and several gases were caused to
samples from various locations in a coal bed
flow along the bedding plane of each coal. Gas flows
were reported (Table 4) in cm2 s-l atmet at a pressure
Flow through sample
drop of one atm. Hydrocarbon flows through the dense
Coal Location (cm* s-l atm-‘1
-- Pittsburgh attrital coal have the characteristics of molecular
---
diffusion. That is, their flow rates decrease as the square
Pittsburgh
roots of their molecular weights increase. In sharp contrast
non-attrital Bottom O-46 m 3.2 X 10v5
is the gas flow through the less dense Pittsburgh non-attrital
(18 in) 6.4 X 1O-5
and Pocahontas No. 3 coals. Not only are these flows much
9.8 X 1O-5
faster but they are independent of the gas. This is in agree-
046-1*22m 2,8X 10e5
ment with the theory of gas permeability. The high flow
(18-48 in)
rate for helium through Pittsburgh attrital coal has not been
Top 0.46 m 2*4X 1O-5 explained. One suggestion (based on the work of Barrer and
(18 in) 2.2 x 10-S Barrie using porous giass7) is that the lower sorptivity of
helium may maintain a more porous micropore system.
Oklahoma Top, east face 1.48 3.10
Top, north face 2.92 2.66
Temperature
Middle, west 3.56 3.25
face The effect of temperature on the flow rate of several
Middle, east 4.20 gases through Pittsburgh-attrital coal is shown in Table 5.
face
Middle, north 2.27 1.58 Tab/e 3 Methane flow along and across the bedding planes
face of two coats (cm* s-l atm-‘)

1 cm/s through 1 cm2 of coal cross-section with a pressure Along bedding Across bedding
gradient of one atm. Coefficients are characteristic of the Coal plane plane
coal bed and vary widely between coals, as shown in Table 1. _~____
Other independent variables are the location of the sample Pittsburgh attrital 1.2 x 10-10 0.6 X IO-lo
within the bed, the direction of gas flow with respect to Pocahontas No. 3 0.10 0.14
the bedding plane of the coal sample, the molecular weight
of the gas, the temperature and the pressure of the system.
Table 4 Flow of various gasesalong the bedding planes of
three coals (cm* s-’ atm-‘1
Location of sample
Gas flow might vary from coal sample to sample and thus Pittsburgh Pittsburgh Pocahontas
make data unreliable. To test reproducibility methane flow Gas attrital non-attrital No. 3
was measured on several samples from each coal mine. A ----~
special effort wasmade to inspect coal from several locations 8.81 x 10-8 2.4 X 1O-4 7.5 x IO-2
He
within the mine and particularly to compare the coal from 1.26 X lo-” 2.1 x 10-4 7.0x 10-2
CH4
the top and the bottom of the seam. Methane flows were 0.54 x 10-10 7.7 x 10-2
C2’-‘6
measured on fifteen samples of Pittsburgh non-attrital coal 0.36 X lo-lo
C4ho
and Oklahoma Hartshorne coal as shown in Table 2. Flows
are in cm2 s-l atm-l at an average pressure of one atmo-
sphere. These measurements show a consistency between Tab/e 5 Activation energies for the flow of several gases
individual coal samples. The 3 to 4 fold variations are small over Pittsburgh attrital coal (kJ mol-‘)
when compared with the differences in magnitude of values
between coal seams. There is little difference between Flow across Flow along
samples from the top and bottom of the bed and between Gas bedding plane bedding plane
locations within these mines. --- ___-
Helium 16.3 16.3
Bedding plane Methane 57.0 57.0
Differences in flow rate were measured as a function of Ethane 60
bedding plane or the orientation of the coal sample as it was Butane 55.5
cut and mounted in the sample holder. The major gas flow

280 FUEL, 1975, Vol 54, October

 F. S. Karn, R. A. Friedel and A. G. Sharkey: Mechanism of gas flow through coal

1
6X10-~*- of free gas molecules in the coal pores and non-mobile

I \ 0
0 0, Pfttsburgh attritus
molecules adsorbed on the walls. The high activation energy
found for methane flow through Pittsburgh-attrital coal
might be an example of this mechanism. The zero activa-
tion energies observed with the more porous coals may be
justified by the Poisseuille equation4 where observed flow
rates are a function of temperature but only indirectly
through gas density and viscosity. In the case of methane
flow the observed effect is 0.0 kJ/mol; that due to density

-
3xlo-lo~
:zJ:,::r \ :\
is 1.7 kJ/mol; and that due to viscosity is -2.1 kJ/mol 9.
The net effect of temperature on methane flow should
therefore be approximately zero as observed.

B 1 \ \ I
PRESSURE

Pressure is the most complex independent variable in these

gas flow measurements. Several pressure effects are illustrat-
ed in Figure 2 which are reproduced from Knudsen’s data’
”
0.5 for carbon dioxide flow through a glass capillary. As the
3
0
pressure decreases, the flow as measured by Knudsen is
CL Pocahontas
0.4
first (a) proportional to pressure, (b) passes through a mini-
mum and becomes inversely proportional to pressure, and
finally becomes (c) independent of pressure. Methane flows
through coals show similar phenomena (Figure 3) although
coal is obviously a more complex diffusion medium.
Knudsen’s data give Q/(Pl - P2) as a function of pressure
where Q/(Pl - P2) 1s . a volume (STP) of gas flowing per
second through a capillary at a pressure differential of one
atm. Methane flows through coals (Figure 3) were plotted
as Q&/,4@, or Knudsen-type data compensated for the
geometric area and thickness of the coal plug. Methane
flow through Pittsburgh-seam attrital coal (Figure 3)
I I I I is independent of absolute pressure in accordance with
0,7 x lo-s2$
2.8 3.0 3.2 3.1 3% molecular flow theory. The pressure dependence of
10’1 temperature I KS’ I Pittsburgh-seam non-attrital coal indicates molecular flow
at lower pressures, but above 100 kPa the flow approaches
Figure 1 Methane flow through solld coal at 1 atm differential
pressure as a function of temperature
permeability-type. Illinois No. 5 shows this transition
more clearly and Pocahontas No. 3 shows permeability
with a minimum and transition. Although these pressure
dependencies are consistent with Knudsen’s models, a
complete evaluation of gas flow through coal requires
measurements of pore-radius distribution and pore length.
Coal diffusivities have been calculated on the basis of coal-
face area and coal thickness but these are only approxima-
tions since the gases pass through pores in the coal and the
pores probably represent a tortuous path. To compare gas
flow data for coal more precisely with the capillary data of
Knudsen the pore system of the coal should be examined.

Figure 2 CO2 flow through a capillary according to Knudsen

Activation energies of hydrocarbons are similar to each

other; heiium flow rates are much Iess sensitive to tempera-
ture changes. The effect of temperature on methane flow
rate has been measured for several coal samples over a
temperature range from 25 to 100°C. Arrhenius plots
(figure 1) are shown for Pittsburgh-attrital coal (slope 57
kJ mol-l) and for both Pittsburgh non-attrital coal and
Pocahontas No. 3 coal (zero activation energy). Nandi and
Walker8 have suggested that the effect of temperature on
flow rate should help to identify the type of gas flow Figure3 Methane flow along the bedding plane of various coals
through coal. They postulate a two-phase system consisting per atm differential pressure as a function of average pressure

FUEL, 1975, Vol 54, October 287

Mechanism of gas flow through coal: F. S. Karn, R. A. Fritdel and A. G. Sharkey

Table 6 Open pore volumes determined by immersion of The pressures used in these coal experiments (20-200
coal cubes in water kPa) are higher than the pressures used by Knudsen
(O-30 kPa). However, flow is not controlled by pressure
Coal density Open-pore volume alone but by a combination of pressure and pore radius.
(g crnm3) (cm3 g-’ ) (cm3 cmm3) It has been observed that coal contains a wide distribution
-- of pore sizes13 and it appears that this is responsible for the
Pittsburgh attrital 1.328 0.0056 0.0076 wide range of methane flow rates as well as the temperature
Pittsburgh 1 a268 0.0217 0.0277 and pressure effects reported here.
non-attrital
Oklahoma, 1.246 0.0338 0.0421
Hartshorne CONCLUSIONS
Illinois No.611 1.25 0.042 0.0525
Pocahontas No. 3 1.236 0.0454 0.0467 Knudsen flows(independent of pressure) have been observed
in the fine pore system of coals and Poiseuille flows (pro-
portional to pressure) have been observed through the larger
pores. Knudsen flows have a strong temperature effect
Table7 Methane flow through coal and through glass (>.50 kJ mol-l) but the primary forces controlling activa-
capillaries (cm* s-l atm-l) tion energy for Poiseuille flow approximately cancel. The
wide variation in methane flows between coals (Pittsburgh
Based on Based on attrital 1.2 X 1 O-lo cm2 S-I atm-l, Oklahoma Hartshorne
sample geometry porosity 2.0 cm2 s-l atm-l) correspond generally to the void space
~-____ in the solid coal (Pittsburgh attrital 0.8 vol.%, Oklahoma
Pittsburgh seam attrital 1.2x 10-10 1.6X 1OA Hartshome 4.2 vol.%). If the methane flow rate is calculated
Pittsburgh seam non- 3.0x 10-S 1.1 x 10-S on the basis of the available porosity measurements, it is
attrital found that flow rates in coal approximate to flow rates
Illinois No. 6 7.1 x 10-4 1.4 x 10-2 through suitably sized glass capillaries. Illinois No. 6 with
Knudsen (capillary 7.3 x 10-2 a pore flow of 0.014 cm2 s-l atm-l can be compared with
radius 30 urn) a 30 pm capillary which has a flow of O-073 cm2 s-l atm-l.
Knudsen (capillary 3.3 x 10-l Pocahontas No. 3 with a flow of l-8 cm2 s-l atm-l can be
radius 110 pm) compared with a 140pm capillary which has a methane flow
Knudsen (capillan/ 8.5 X lo-’ rate of 1.5 cm2 s-1 atm-l. Although it is interesting to
radius 110 pm) compare flow through such models with gas flow through
Knudsen (capillary 1.5 coal, the authors believe that the value of this paper lies
radius 140 pm) chiefly in the new flow data, and the relatively simple
Pocahontas No. 3 0.1 1.8 method which is readily available for use on almost all ranks
Oklahoma Hartshorne 2.0 47.5 of coal.

Pore volumes for coal have been estimated in several ways

REFERENCES
including mercury versus helium densities and mercury
penetration. Karn, F. S., Friedel, R. A., Thames, B. M. and Sharkey, A. G.,
1
These methods were applied to the present samples but Jr Fuel, Lond. 1970,49, 249
the macropore structure (>lOO nm) was sometimes lost. 2 Karn, F. S., Friedel, R. A. and Sharkey, A. G., Jr Rep. Invest.
To duplicate massive coal samples, coal cubes were carefully U.S. Bur. Mines 7441,197O
cut, measured, and immersed in distilled water until they 3 Cervik, J.MiningCongr. J. 19, July 1967, pp 52-57
4 Loeb, L. B. The Kinetic Theory of Gases, Dover Publications,
reached a maximum weight gain. As reported by Franklinto, New York, 1961
liquid water filled the pore space of the coal samples; these 5 Knudsen, M. Annalen der Physik 1909,28,75
pore volumes are shown in Table 6. From these data an 6 Anderson, W. A. Carbon 1966,4,107
estimate was made of the methane diffusivity through the I Barrer, R. M. and Barrie, J. A. Proc. Roy.Soc. 1952, A213,
250
pore area and geometrical thickness in contrast with the
8 Nandi, S. P. and Walker, P. L., Jr Fuel, Lond. 1970,49, 309
diffusivity based on the geometrical total area and thickness 9 Handbook of Chemistry and Physics, 48th edn
of the coal sample. These values are shown in Table 7. On 10 Franklin, R. E. Trans. Farad. Sot. 1949,45,214
a porosity basis, methane flow rates through Knudsen 11 Machin, J. S., Staplin, F. and Deadmore, D. L. IllinoisState
Geol. Surv. Circ. 350, 1963
capillaries of 30 and 140 I.tm respectively are similar to the
12 Mercury penetration measurements through the courtesy of
observed flows through Illinois No. 6 and Pocahontas No. 3 Karl H. van Heek, Bergbau-Forschung, Essen
coals. Samples of these coals gave pore-radius distributions 13 Zwietering, P. and van Krevelen, D. W. Fuel, Lond. 1954,33,
by mercury penetration ranging from 1 0e2 up to 100 pm”. 331

282 FUEL, 1975, Vol 54, October