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451

A mathematical modeling approach to improve


the point estimation of landll gas surface
emissions using the ux chamber technique
M.D.N. Perera, J.P.A. Hettiaratchi, and G. Achari

Abstract: The accurate determination of gas emissions from sanitary landfills is necessary to assess the contribution of
landfill gas emissions to global warming and to develop optimum techniques to control emissions from individual landfills.
The most popular method available for point measurement of landfill gas, the closed or static flux chamber technique,
has inaccuracies associated with the technique itself. A new mathematical modeling approach is presented to estimate
the errors caused by changes to the flow pattern of gases within the soil cover when a closed flux chamber is placed
on top of the cover to measure gas emissions. The proposed two-dimensional numerical model considers both advective
and dispersive processes of gas migration. The model was calibrated and verified using data from controlled laboratory
experiments. The model was able to predict the fluxes with 95% accuracy. Based on laboratory experiments and model
predictions, our analysis showed that a closed flux chamber technique would underestimate actual gas flux by as much
as 65% depending on the configuration of the flux chamber, the actual flux rate, and the characteristics of the soil in the
landfill cover.
Key words: landfill gas, methane, global warming, mathematical modeling, landfill cover, simulation, environmental
monitoring, flux chamber.
Rsum : Il est ncessaire de dterminer prcisment les missions gazeuses provenant des lieux denfouissement afin
dvaluer la contribution de ces missions au rchauffement de la Terre et de dvelopper des techniques optimales de
contrle des missions provenant des lieux denfouissement individuels. La mthode la plus populaire disponible pour
les points de mesure des gaz de lieux denfouissement, la technique de la chambre de flux dbit statique ou ferm,
prsente des imprcisions associes la technique elle-mme. Une nouvelle approche de modlisation mathmatique est
prsente afin destimer les erreurs causes par les changements au cheminement du dbit des gaz dans la couverture
de sol lorsquune chambre de flux dbit ferm est place sur le dessus de cette couverture pour mesurer les missions
gazeuses. Le modle numrique deux dimensions propos considre les procds dadvection et de dispersion de la
migration des gaz. Le modle a t talonn et vrifi en utilisant des donnes provenant dexpriences contrles en
laboratoire. Il peut prdire les dbits avec une prcision de 95 %. Notre analyse, base sur des expriences en laboratoire
et des prdictions de modles, montre que la technique par chambre dbit ferm sous-estimerait le dbit rel de gaz par
autant que 65 %, selon la configuration de la chambre dbit, le dbit rel ainsi que les caractristiques du sol dans la
couverture.
Mots cls : gaz denfouissement, mthane, rchauffement de la Terre, modlisation mathmatique, couche de couverture,
simulation, surveillance environnementale, chambre de flux.
[Traduit par la Rdaction]

Introduction
Sanitary landfills accepting biodegradable organic waste are
known to produce significant quantities of methane (CH4 ) and
carbon dioxide (CO2 ). Although both CH4 and CO2 are green-

house gases, CH4 is more of a concern on a per unit of emission


basis because it has a global warming potential (GWP) of 23
with reference to a 100-year time horizon (IPCC 2001), as compared to CO2 with a GWP of 1. According to some estimates,
sanitary landfills contribute up to 12% of global anthropogenic

Received 11 October 2001. Revision accepted 7 October 2002. Published on the NRC Research Press Web site at http://jees.nrc.ca/ on
4 December 2002.
M.D.N. Perera. Stantec Consulting Ltd., 1122 - 4th Street S.W., Calgary, AB T2R 1M1, Canada.
J.P.A. Hettiaratchi1 and G. Achari. Department of Civil Engineering, The University of Calgary, 2500 University Drive N.W., Calgary,
AB T2N 1N4, Canada.
Written discussion of this article is welcomed and will be received by the Editors until 31 March 2003.
1

Corresponding author (e-mail: jhettiar@ucalgary.ca).

J. Environ. Eng. Sci. 1: 451463 (2002)

DOI: 10.1139/S02-033

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452

CH4 emissions into the atmosphere (Bogner et al. 1997). Considering the importance of controlling atmospheric CH4 emissions from landfills, there is renewed interest in quantifying
surface emissions from individual landfills. Accurate quantification of surface gas emissions is required for three purposes:
(i) to assess the magnitude of the problem created by individual landfills and the global problem posed by land disposal
of biodegradable organic waste, (ii) to identify and implement
methods to control atmospheric emissions, and (iii) to evaluate
the effectiveness of methods to control atmospheric emissions
of landfill gases.
Although several techniques are available for measuring surface gas emissions from landfills, the closed, or static, flux
chamber method is the most popular (Bogner et al. 1997; Czepiel
et al. 1996; Livingston and Hutchinson 1995). A closed flux
chamber is used to measure the landfill gas flux at a selected
point on the surface of a landfill. The flux is measured at the
point of emission into the atmosphere, after the gas generated
within the landfill had the opportunity to travel across the landfill cover layer. Although this method is simple and applicable
in almost all landfill situations, various researchers have identified errors in surface flux calculations based on closed flux
chamber measurements (Reinhart et al. 1992).
The closed flux chamber technique involves trapping the gas
in an enclosed chamber as it leaves the soil surface and allowing
the gas concentration to build up within this chamber. The rate of
gas emission into the chamber, F in mol m2 s1 , is calculated
using
 
V dC
[1]
F =
A dt
where V (m3 ) and A (m2 ) are volume and area of the flux chamber, respectively, and C (mol m3 ) is the concentration of the
component gas inside the chamber.
Since gas collected inside the closed flux chamber is not being
continually diluted with external air (as is the case with the open
flux chamber technique), even small fluxes can be measured
with this method. However, the main drawback of the closed
chamber technique is the influence of the chamber itself on the
flux rate. As gas accumulates in the chamber, the increase in
concentration decreases the flux rate. Therefore, this technique
tends to underestimate the gas fluxes. According to Matthias et
al. (1978), the actual flux could be as much as 55% higher than
the flux calculated from flux chamber measurements.
Several researchers have proposed error correction methods
to improve the calculated surface flux using closed flux chamber measurements. Hutchinson and Mosier (1981) proposed
the use of three chamber measurements as a correction. Since
their correction considers only diffusive gas flow, it has limited
use in a landfill situation where flow may be controlled by advection, mechanical dispersion, and molecular diffusion. Other
researchers (e.g., Matthias et al. 1978; Hutchinson and Mosier
1981; Healy et al. 1996) have attempted to use mathematical
models to improve the accuracy of gas flux determinations.

J. Environ. Eng. Sci. Vol. 1, 2002

Matthias et al. (1978) and Hutchinson and Mosier (1981) proposed the use of separate nonlinear models, each based on the
theory of molecular diffusion in soils. The model proposed by
Matthias et al. (1978) is capable of simulating nitrous oxide
(N2 O) flux from homogeneous soil in the presence of a closed
flux chamber. It is a two-dimensional diffusion model under the
Cartesian coordinate system, but it does not consider advective
or mechanical dispersion induced flow of gas in soils. The most
extensive numerical modeling effort was by Healy et al. (1996).
They considered three-dimensional molecular diffusion but also
neglected advective flow as well as flow due to mechanical dispersion. Their model is applicable only to diffusion of a single
gas in a porous medium under ambient pressure.
Since most of the past modeling efforts are directed at low
fluxes of N2 O from soils by diffusive flow alone, the resulting models cannot be applied in landfill situations where high
fluxes could be encountered. Pressures in landfills could be
much higher than atmospheric pressure, and therefore both advective and dispersive (i.e., molecular diffusion and mechanical
dispersion) processes govern gas flow behavior across a landfill cover. There have been instances where the pressure inside
landfills exceeded 2 kPa (Hartless 1995). Furthermore, landfill
gas is a mixture of gases, including CH4 and CO2 as well as a
variety of other gases in trace quantities.
In this paper, a mathematical modeling approach is introduced that can be used to estimate the errors associated with
calculating landfill surface flux from closed flux chamber measurements. The approach requires the collection of data using
the closed flux chamber and applying a new two-dimensional
advectivedispersive gas migration model. The mathematical
model formulation is presented first. The two-dimensional gas
migration model was solved numerically using the Alternating
Implicit Direction (ADI) method. Model calibration, sensitivity analysis, and verification using laboratory data sets are then
presented. The paper concludes with a description of potential
model applications, strengths, and limitations.

Theoretical formulations
The errors associated with the determination of surface gas
fluxes using flux chambers can be quantified by modeling gas
migration in soil in the vicinity of the flux chamber considering gas flow across a landfill cover to be multicomponent and
unsteady. The theoretical aspects of the mathematical model
that accommodates the two physical processes of importance,
advection and dispersion, are discussed below.
Landfill cover systems are usually layered structures, with
different layers serving different purposes. In this analysis, for
simplicity, it is assumed that a landfill cover consists of a single
layer of soil. Gas migration in the soil cover is modeled assuming soil is a continuum. Since flux chambers considered in this
study are cylindrical, perturbations in the soil atmosphere are
radial. However, it can further be simplified to an axisymmetric
case assuming the soil properties are isotropic on the horizontal
plane.
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453

Fig. 1. Gas flow patterns adjacent to a flux chamber.

Landfill Cover

It is assumed that there are no sources of gas or sinks of gas in


the soil (Note: soil respiration that could be a source of CO2 is
neglected). Since the intent of this paper is to assess the effects
of only the physical processes (i.e., advection and diffusion) on
flux chamber measurements, the sourcesinkreaction term S
will not be used in subsequent equations. In addition, the model
development has been further simplified by using only two gas
components, CO2 and air, with the air component representing CH4 , N2 , O2, and other trace gases. The reason behind this
simplification is that a single nonreactive gas (i.e., CO2 ) is sufficient to assess the effects of advective and dispersive processes
on flux chamber measurement, and these processes are the only
ones contributing to errors in gas measurement.
Gas velocities are determined from Darcys law
[3]

Waste Layer

Figure 1 depicts the soil gas migration patterns in the vicinity


of a closed flux chamber. In this analysis, only gas migration is
considered and the moisture migration is neglected. Moisture
migration is neglected for a number of reasons. These include
the short time frame of flux chamber measurement (typically,
flux chamber measurements are taken quickly to minimize perturbations in the soil atmosphere) and the relatively low moisture flux because of low hydraulic head and hydraulic conductivity of landfill cover soils. However, the effect of pore water
on gas permeability is taken into account during mechanistic
modeling. At a landfill cover, the gas phase may include CH4 ,
CO2 , oxygen (O2 ), nitrogen (N2 ), and water vapour. In model
development, the potential dissolution of gases in pore water
and the presence of water vapour in gas phase are neglected.
Advective flows due to gravity and differential density are also
neglected because of the small vertical distances considered in
modeling.
The axisymmetric relationship to describe the fate and transport of a fluid in a uniform soil is given in eq. [2] (Mendoza and
Frind 1990). When applied to gas movement in the presence
of a flux chamber, the z direction is vertically downwards and
the r direction is radially outwards from the centre of the flux
chamber.


Cm
(ur Cm ) (uz Cm ) Dr
Cm
[2]

+
r
t
r
z
r r
r
+ Dz

2 Cm
S
z2

krel kj P
j

where krel is the relative permeability; kj is the intrinsic permeability in j direction (m2 ); is the gas mixture viscosity (Pa s);
P is the pressure (Pa); and j = r, z.
The gas mixture viscosity () is calculated using viscosities
of the individual gases (m ) and their mole fraction (Ym ).
[4]

2


m

2 

m=1 1 +
ml YYml
l=1
m=l

in which
0.5

ml = 8


Mm 0.5
1+
Ml



 2

m 0.5
Ml 0.25
1+

l
Mm

where Ym , Yl = mole fraction of gas m and l, respectively and


Mm and Ml = molecular weight of gas m, and l, respectively.
Gas migration modeling is complex because of the interdependence of flow and transport equations. The solution procedure is therefore iterative for any time step (Mendoza and Frind
1990). In the process, the flow and transport equations are combined by deriving the pressures from concentrations of the component gases using the equation of state for gases (Findikakis
and Leckie 1979). It results in a single nonlinear equation with
concentrations of different gases as the variables.
From the equation of state for gas
[5]

P = RT

2


Cm

m=1

m3 );

where Cm is the concentration of gas m (mol


m = CH4 ,
CO2 , O2 , N2 (all these gases should be considered when simulating landfill gas emissions); Dj is the coefficient of dispersion
in j direction (m2 s1 ); uj is the gas velocity in j direction (m
s1 ); j = r, z; is the gas porosity; S is the source, sink, or
reaction (decay or production rate) (mol s1 m3 ).

uj =

where R is the universal gas coefficient (Pa m3 K1 mol1 ), T


is the absolute temperature (K), and m represents the two gas
components, CO2 and air.
[6]

D = D + |u|
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where D is the dispersion coefficient (m2 s1 ), D* is the molecular diffusion (m2 s1 ), is the dispersivity (m), and u is the
gas velocity (m s1 ).
The complete equation for a component gas i is
[7]

Cm
krel kr P Cm
krel kr 2 P
=
+
Cm
t
r r
r 2
krel kz P Cm
krel kz 2 P
+
+
Cm
z z
z2
2 Cm
2 Cm
Dr Cm
+
D
+ Dr
+
z
r 2
r r
z2

Such equations can be derived for each of the gas component


(CO2 and air). In the steady state case, the left-hand side of
eq. [7] becomes zero, and on the right-hand side all terms with
r are dropped because all of the variations are in the vertical
z direction. The steady state solution is used to determine the
initial conditions for the transient (axisymmetric) case.

[8]

n+1
Ci,j

n
Ci,j

t



n+1
n+1
Ci+1,j
Ci1,j

Boundary conditions
The boundary conditions are illustrated in Fig. 3. There are
N + 1 nodes in the r direction and M + 2 nodes in the z direction.
The number of grid points inside the chamber is defined as M1.

Top boundary: outside the chamber

[9]

The governing equations were solved using the finite difference method. For higher accuracy, space derivatives of concentrations and pressures were determined by central difference
method. The nonlinear problem was linearized prior to solving
by lagging the coefficients. The linearization was achieved by
taking the pressures and viscosities from the earlier time step.
For the axisymmetric case, the Alternating Implicit Direction
(ADI) method was used (Aziz and Settari 1979).
The finite difference equation for a particular gas component
is given in eq. [8]. In this equation, n and n + 1 represented the
time step of that particular variable.
Variable grid spacings were used to reduce the number of
grid points without compromising representation of the actual
conditions. This is because a thin layer of grid points is required
to represent gas transport adjacent to the atmosphere and flux
chamber, and a thin column of grid points is required to simulate
transport in soil adjacent to the chamber wall. Figure 2 shows
the finite difference grid system simulated in the model. The
entire depth of the landfill cover was modeled.

n
n
Pi,j
Pi+1,j

n Pn
Pi,j
i1,j

krel kr

ri1 + ri
ri1 + ri

ri
ri1



n+1
n+1
n
n
Ci,j
Pi,j
Pi,j
Ci,j
+1
+1
1
1
2
k
k
rel z

C n+1 +
ri1 + ri i,j

zj 1 + zj
zj 1 + zj
 


n
n
n
n
2
krel kz Pi,j +1 Pi,j Pi,j Pi,j 1

+
C n+1

zj
zj 1
zj 1 + zj i,j
 




n+1
n+1
n
n
n Cn
Ci+1,j
Ci,j
Ci,j

C
C
i+1,j
i1,j
i1,j
2
Dr

+ Dr
+
ri
ri1
ri1 + ri
r
ri1 + ri
 


n
n
n Cn
Ci,j
Ci,j
+1 Ci,j
i,j 1
2

+ Dz
zj
zj 1
zj 1 + zj

krel kr

n
n
Pi1,j
Pi+1,j

Numerical solution

Ci,1 = Catm at any time t

where i = M1 + 1, M + 2. This boundary condition is common


to both transient and steady state cases. The CO2 and air concentrations were determined considering the atmospheric gas
composition of 0.03% CO2 , 21% O2 , 78% N2 , and 1% Ar.
Top boundary: inside the chamber
Since gases accumulate with time, the gas concentrations
inside the chamber are transient. Therefore, this boundary condition is a time dependent one. The boundary condition was
determined by considering advective and diffusive flows into
the chamber until a particular time is elapsed. The flow was
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455

Bottom boundary

Fig. 2. Finite difference grid.


Flux
Chamber

Centre Line

Finite
Difference
Grid
r-Direction

In a landfill, the bottom of the soil cover is in contact with


the top of the waste layer. Therefore, the bottom boundary condition should characterize gas emissions from the waste layer.
To incorporate this situation, the bottom boundary condition is
given as a gas flux. The advective and diffusive fluxes at the
bottom were set to constant values.

z-Direction

[14]
Landfill
Cover

n+1
DN
v N CN

C
= QBottom
z

Therefore,
Waste

considered quasi steady for this calculation.



qm dAdt
[10]
Cm,z=0,t=t = Cm,atm +
R 2 H

where
qm dA dt is the volume of component m entering
the chamber during time t (mol m2 s1 ), R is the radius of the
chamber (m), and H is the height of the chamber (m).
The finite difference form of this equation can be written as
[11]

n+1
n
Ci,1
= Ci,1
+


n Cn
  Ci,2
i,1
n+1
D
+ v1,1/2 Ci,1
z1

(ri + ri+1 )
2ri t
/ R 2 H
2

where i = 2, M1; v is the Darcy velocity (m s1 ).


Left and right boundary conditions
The central axis of the chamber is characterized by the left
boundary of the domain. Due to symmetry, the concentration
gradient at this point is zero.


C
[12]
=0
r r=0
Therefore, C1,j = C3,j at any time where j = 1, N + 1.
The right boundary is selected such that there is no perturbation due to the chamber at this boundary point. Therefore, this
boundary was defined as a zero concentration gradient.


C
[13]
=0
r r=L
where L is the distance to the right boundary from the center
of the chamber (m).
Therefore, CM+1,j = CM,j at any time where j = 1, N + 1.

[15]

n+1
CN+1
=

QBottom (zN + zN1 )


DN
vN (zN + zN1 ) n+1
n+1
+ CN1
+
CN
DN

In these eqs. [14] and [15], QBottom is the gas flux rate at the
bottom boundary. The bottom boundary in the finite difference
grid is represented by the Nth row. QBottom is a negative value
(mol m2 s1 ) for CO2 and 0.0 for air (in a landfill setting,
fluxes for CH4 and CO2 were specified and fluxes for O2 and
N2 are set to zero).

Initial conditions
For the transient case, initial conditions are required. Since
the initial condition is the concentration at steady state, the required concentrations were determined from steady state modeling. Assuming there was no spatial heterogeneity, the steady
state was modeled as a one-dimensional situation. The top and
the bottom boundaries were similar to the two-dimensional case
outside the chamber. The governing equation for steady state
gas transport was derived from eq. [2]. It is the one-dimensional
gas migration equation in the z direction.
Removing the terms in the radial direction, the following
equation was obtained:
[16]

0=




Cm
vz Cm D
+S
z
z

Similar equations were written for both gas components and


solved.
Finite difference equations for steady state were derived from
a transient one-dimensional model when there was negligible
difference between the concentrations in two consecutive time
steps. For high accuracy, the Crank-Nicholson scheme was used
in the steady state solution.
The steady state equation is given in eq. [17]
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[17]


vj +1/ 2
vj 1/ 2
Dj +1/ 2
Dj 1/ 2

+
Cjn 1
2(zj + zj +1 ) 2(zj + zj +1 ) zj (zj + zj +1 ) zj 1 (zj + zj +1 ) t




vj +1/ 2
vj 1/ 2
Dj +1/ 2
Dj 1/ 2
+
=

+
Cjn+1
+
Cjn1
+1
2(zj + zj +1 ) zj (zj + zj +1 )
2(zj + zj +1 ) zj 1 (zj + zj +1 )

Laboratory experiments: materials and


methods
For model calibration and verification, known landfill gas
fluxes were needed. Such data could not be obtained from actual
landfills. Field experiments that simulated actual landfill conditions are difficult to control. Because of these difficulties, laboratory experiments were undertaken to generate experimental
data for model calibration and verification. The laboratory experimental data were generated using three gas flux rates and
with three flux chambers of different configurations. Since our
interest was on evaluating advective and dispersive gas migration patterns on the flux chamber measurements (as mentioned
in the model development section), it was sufficient to use one
type of gas that is nonreactive (i.e., CO2 ) to generate laboratory
data.

The pressure gauge (Cole-Parmer) had a range of 015 in. of


water (04 kPa) with an accuracy of 3% full scale. It measured
low gauge pressure using a phosphor bronze diaphragm.
Three 3/8-in. nylon tubes were installed vertically within the
soil to obtain gas samples from different depths. The tubes
reached depths of 16.5, 36, and 54 cm (see Fig. 4). The tubes
were perforated at the bottom (up to a length of 38 mm), and
a fine steel mesh was wrapped as a screen around the perforated tube to prevent entry of fine soil particles. Swagelok fittings were attached to the top of these tubes to measure the gas
concentrations. Three probes were also installed at three levels in the soil to monitor moisture content and the temperature.
Pressure inside the chamber was measured using an inclined
micromanometer.

Data collection
Experimental setup
Laboratory experiments were conducted under controlled
conditions using a soil cell constructed of a 159-L steel barrel with a height of 1 m (see Fig. 4). The bottom of the cell was
filled with a gravel layer overlying a perforated pipe bent into a
circle of diameter 25 cm. The gravel layer and a fine mesh (sieve
size 30) support the soil above and distribute the gas uniformly
within the soil cell. A port was attached to the bottom to supply
gas. This experimental setup was thoroughly checked for any
gas leaks before filling the soil. The top of the cell was kept open
to the atmosphere to enable measurement of flow rates using
a flux chamber. The soil used was a sandy loam (according to
USDA classification) with 63% sand, 22% silt, and 6% clay
.The soil was placed in three layers and compacted following
the modified Proctor compaction test procedure. The difference
in pore sizes, and therefore the contrast in gas permeabilities
between soil and gravel, result in uniform gas concentrations at
the boundary. Ultrahigh purity CO2 gas (supplied by Praxair)
was used as feed gas.

Instrumentation
The gas flow rate at the base of the cell was regulated using
needle valves and measured with a Cole-Parmer 65 mm direct
reading flow metre with a range of 0100 mL/min (accuracy
of 5% full scale). The feed gas was sent to the bottom of the
cell via TygonTM tubing. A pressure gauge was connected to
measure the gas pressure inside the cell using a Y connector.

The laboratory experiments were conducted to generate data


for the following reasons: (i) to allow the assessment of the accuracy of closed flux chamber measurements (under different
flux rates and with different configurations of flux chambers)
and (ii) to calibrate the mathematical model. Both of these objectives were accomplished using the same data sets.
For model calibration in the steady state and transient state,
two types of data were collected. In the steady state, the gas flow
was assumed to be one dimensional. The test gas was sent from
the bottom of the cell for several weeks to allow equilibrium
to take place before actual readings were taken. During experimentation, the gas concentrations were measured at various
depths within the soil cell. At each depth, gas samples (2 mL)
were collected and analyzed using a Hewlett Packard MicroGas Chromatograph with thermal conductivity detectors. The
carrier gas used was helium (He). All peaks were quantified on a
personal computer with Hewlett Packard EZ-Chrom integration
software.
Once steady state was achieved within the test cell, flux chamber measurements were taken. Three flux chambers of dimensions 25 cm diameter and 16.5 cm height, 10 cm diameter and
5 cm height, and 20 cm diameter and 12 cm height were used
to generate transient case data. The use of flux chambers with
different dimensions allowed the assessment of the effect of
chamber configuration on the flux measurement. During flux
measurements, the flux chambers were placed on the soil surface at the center of the cell to ensure axisymmetry. After a
flux chamber was placed on the soil surface, the soil around the
edge was pressed to ensure a good seal. The concentrations of
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457

Fig. 3. Boundary conditions for the model.


Inside the
Chamber
Time Dependent
Concentration

Chamber

C = Catmospheric
j=1

Right
Boundary

Left
Boundary

C =0
r

C
=0
r

i=1

i=M+2

j=N+1

Imaginary
Grid
Points

Bottom Boundary
Const. Flux

gas inside the chamber were monitored for a period of time to


develop concentration vs. time graphs. The CO2 concentrations
inside the flux chamber were measured using an EGM2-CO2
analyzer. This instrument used a nondispersive infrared analyzer to measure CO2 concentration. The measurement range
was 050 000 ppm by volume. Within this range, the precision
of the instrument was 0.5% of full scale.

assumption because dry CO2 gas was sent through the soil for
several weeks before readings were taken (the dry gas removes
moisture from the soil and makes it almost completely dry).
The total porosity ( t ) was determined using the estimated dry
density of the soil at the time of compaction. The following
equation (American Society of Agronomy 1982) was used for
this purpose:

Model calibration

[18]

The results from laboratory experiments conducted at different gas flow rates were used for model calibration. The data
generated consisted of gas concentrations at different depths of
the soil cell and gas concentrations inside the flux chamber at
different time intervals.
During model calibration, selected model input parameters
were adjusted until there was agreement between the model
output results and the experimentally determined values.
Model calibration for steady state
The parameters used for model calibration for steady state
included soil porosity, soil diffusion coefficient, vertical and
horizontal dispersivities, and vertical and horizontal permeabilities. The model outputs included CO2 concentrations at various
locations within the soil cell. At the beginning of the calibration, the best estimates of input parameters were used. Some of
the parameter values were determined from laboratory analysis,
whereas the others were obtained from the literature.
The soil porosity was determined from the total porosity
and assuming almost completely dry soil conditions (with only
34% volumetric water content). It was possible to make this

t = 1

d
s

where d is the soil dry density (kg m3 ) and s is the particle


density (kg m3 ).
Assuming a particle density of 2650 kg m3 , and using the
measured dry density of 1634 kg m3 , the total porosity was
found to be 0.383. Therefore, the gas porosity was determined
to be 0.35 (assuming a volumetric water content of 34%).
The gas diffusion coefficient values available in the literature
are primarily for gas diffusion in air (Reid et al. 1987) but not
for porous media. To determine the coefficient of molecular
diffusion in soil, an empirical equation proposed by Millington
and Quirk (1961) was used
10/3

[19]

Dsoil = Dair

a
t2

where Dsoil is the molecular diffusion coefficient in soil (m2 s1 ),


Dair is the molecular diffusion coefficient in air (m2 s1 ), a
is the gas porosity, and t is the total porosity. Using a binary
diffusion coefficient for CO2 in air of 1.8 105 m2 s1 (Reid
et al. 1987), the soil gas diffusion coefficient was determined
to be 3.7 106 m2 s1 .
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Fig. 4. Laboratory experimental setup.

Compacted
Soil

To the Flow
Meter/Cylinder

100 cm

Nylon
Pipes

Soil Column 80 cm

Thermocouples

Fine Screen
Perforated
Ring
Pressure Gauge

Gravel

45 cm

When parameter values were changed during the model calibration process, the sensitivity of the individual parameters was
also considered. When the uncertainty of a parameter was low,
the parameter was kept unchanged. That was the case with gas
porosity and the coefficient of molecular diffusion. The other
parameters (e.g., vertical and horizontal dispersivities and vertical and horizontal permeabilities) showed high sensitivity and,
therefore, were varied within the ranges reported in the literature
until the simulated concentrations matched the experimentally
determined CO2 concentrations.
Laboratory results showed a high dispersion of gas within the
system.Although dispersion is caused by molecular diffusion as
well as mechanical dispersion, the contribution from molecular
diffusion was too small to account for this dispersion. When the
gas velocities are comparatively large, in the range of 1 m d1 ,
mechanical dispersion becomes important. Therefore, the dispersivity value was changed until the simulated results matched
the experimentally determined CO2 concentration values. The
resulting calibrated dispersivity value was 0.5 m, which lies on
the high side of the dispersivity range reported in the literature,
i.e., 0.011.0 m for the scale of this experiment (Mendoza and
Frind 1990). The lateral dispersivity was assumed to be 0.05 m.
Gas permeability did not affect the concentration profile significantly. However, it affected the flux rates due to advection
and gas pressure within the soil cell. At the bottom of the cell,
gas pressures were low (510 Pa), indicating a high intrinsic
permeability of soil. The selected intrinsic vertical permeability for calibration was 1 1010 m2 , which is equivalent to a
gas permeability of 2 104 m s1 . This value is reasonable
for sandy loam (Zheng and Bennett 1995). Horizontal permeability was assumed to be five times higher than the vertical
permeability, or 5 1010 m2 .

Table 1. Parameters used to calibrate the model.


Parameter

Value

Intrinsic permeability vertical


Intrinsic permeability horizontal
Molecular diffusion coefficient
Dispersivity vertical
Dispersivity horizontal
Volumetric air content

1 1010 m2
5 1010 m2
5.46 105 m2 s1
0.5 m
0.05 m
0.35

The parameter values selected for calibration of the model are


presented in Table 1. The resulting experimental and simulated
steady state CO2 concentration profiles along the test cell are
presented in Fig. 5. The concentration profiles were generated
for the CO2 flux rate of 199 g m2 d1 (without a flux chamber).
The model simulated results and experimental data show good
agreement.
Model calibration for transient state
The calibration for transient state was carried out in conjunction with the calibration for steady state. In the transient case,
the input parameter values were varied to obtain a reasonable
agreement between the experimentally derived CO2 concentrations within the flux chamber (as a function of time) and
the model simulated values. The set of input parameter values
presented in Table 1 provided a reasonable match.
The set of experimental data generated during the use of the
medium-sized flux chamber with a flux rate of 199 g m2 d1
was selected for the transient state model calibration. The model
simulations and experimental results are compared in Fig. 6.
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459

Fig. 5. Steady state CO2 concentration profiles from experimental


and model results.

Fig. 7. Sensitivity on grid size.


35
30

30

CO2 Concentration (%)

CO 2 Concentration (%)

35

25
20
15
Experimental

10

20
15
dz = 2 cm
dz = 1 cm

10

dz = 6 cm

Simulated

25

0
0

0
0

0.2

0.4

0.1

0.2

0.6

0.3

0.4

0.5

Depth (m)

Depth (m)
Fig. 8. Sensitivity on intrinsic permeability.

500

1000

35
CO2 Concentration (%)

CO 2 Concentration (%)

Fig. 6. CO2 concentrations over time in the medium-sized flux


chamber.
0.9
0.8
0.7
0.6
0.5
0.4
Simulated
0.3
Experimental
0.2
0.1
0.0

30
25
20
15
k = 1E-10

10

k = 1E-11
k = 1E-9

5
0
0

0.1

0.2

0.3

0.4

0.5

0.6

Depth (m)

1500

Time (s)

The model simulations show good agreement with experimental


data (< 5% error between the two sets of results) until the CO2
concentration within the chamber reaches about 0.5%. Beyond
this gas concentration (which corresponds to a time of about
10 min), the model fails to simulate the experimental results.

Sensitivity analysis
A sensitivity analysis was undertaken to evaluate the sensitivity of model results to the following key model input parameters: grid size, intrinsic permeability (k), dispersion coefficient
(D), gas porosity (a ), and dispersivity (). During this analysis, calibrated values of all the parameters were systematically
changed (one parameter at a time) within an established plausible range. The magnitude of change in model output CO2 concentration due to a change in one of the parameters is a measure
of the sensitivity of the solution to that particular parameter. The
sensitivity analysis was undertaken for the steady state model
because the transient model took a relatively long time to run
(sometimes more than 10 h). The resultant gas concentration
profiles could be compared with either the calibrated model results or the experimental results. Since calibrated model results
showed excellent agreement with experimental results, in this
case comparisons were made with the calibrated model results.

The effect of varying model grid sizes (1, 2, and 6 cm) on gas
flux is presented in Fig. 7. There is no discernible change in CO2
concentration along the cell depth as the grid size was varied.
The low sensitivity indicates the possibility of decreasing the
number of grid points in the model, thereby reducing the model
run time. However, a larger grid spacing was not preferred for
the two-dimensional model. Since the flux chamber wall has
to be simulated in the r direction, a large grid spacing is not
appropriate. The grid spacing used for the model was 2 cm.
The sensitivity analysis result for intrinsic permeability is
shown in Fig. 8. The intrinsic permeability was varied by two
orders of magnitude, between 109 and 1011 m2 , but the model
results indicate minimal effect. The minimal significance indicates that advection could be a less important mechanism than
dispersion under the test conditions and the time interval considered during simulations.
Figure 9 illustrates the sensitivity of gas flux to the diffusive
properties by plotting the CO2 concentration profile against the
molecular diffusion coefficient, D*. The sensitivity of the model
output to D* is significant, and indicates the importance of diffusion as a process controlling gas flux rates. The sensitivity
increases with depth where the CO2 concentrations are higher.
The sensitivity of the CO2 concentrations to gas porosity is also
high (Fig. 10). Since Dsoil (a )10/3 , the high sensitivity is
expected. The parameter that exhibited the highest impact on
model outputs is dispersivity, (Fig. 11). Therefore, the sen2002 NRC Canada

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J. Environ. Eng. Sci. Vol. 1, 2002


Fig. 12. CO2 concentrations over time in the large flux chamber.

Fig. 9. Sensitivity on molecular dispersion.

CO2 Concentration ( %)

CO2 Concentration (%)

35
30
25
20
15
D* = 3.7E-5

10

D* = 3.7E-4
D* = 3.7E-6

5
0
0

0.1

0.2

0.3

0.4

0.5

0.6

0.8
0.7
0.6
0.5
0.4
0.3

Simulated
Experimental

0.2
0.1
0.0

Depth (m)

40

1500

Fig. 13. CO2 concentrations over time in the small flux chamber.

35

1.2

30
25
20
15

phi = 0.35

10

phi = 0.45

phi = 0.25

0
0

0.1

0.2

0.3

0.4

0.5

0.6

Depth (m)

alfa = 0.65
alfa = 0.1

60
50
40
30
20
10
0

0.6
Simulated

0.4

Experimental

0.2

500

1000

1500

Time (s)

alfa = 0.35

70

0.8

alfa = 0.50

80

1.0

0.0

Fig. 11. Sensitivity on dispersivity.

90

CO2 Concentration (%)

CO 2 Concentration (%)

1000
Time (s)

Fig. 10. Sensitivity on gas porosity.

CO2 Concentraction (%)

500

0.2

0.4

0.6

Depth (m)

sitivity analyses confirm that dispersion is the dominant flow


mechanism under the test conditions and the time interval considered during simulations.

Model verication
For verification of the model, the calibrated model was used
to reproduce a set of experimental observations independent of
those observations used in model calibration. The experimental
results generated during the use of the large-sized flux chamber
(i.e., 25 cm diameter and 16.5 cm height) were selected for this
purpose. The simulated and experimental results are presented

in Fig. 12. A close agreement exists between the model results


and the experimental data.
For further verification of the model, a second data set obtained using the small chamber (i.e., volume 400 mL and height
5 cm) was also compared with the model results (see Fig. 13).
In this case, the model over-estimated the CO2 concentrations
within the chamber after 10 min. Thus, if the flux chamber
size is large, the model and experimental results agree up to
20 min, which is the total duration of the experiment, whereas
if the chamber size is small, the model and experimental results
agree only up to about 10 min.

Model applications, strengths, and


limitations
Table 2 presents a comparison of flux rates calculated from
closed flux chamber measurements and the actual flux rates
used in the experimental component of the study. The percentage errors of measurement for the three types of flux chamber
configurations and the three flux rates are also presented in this
table. The results clearly show that the errors in the flux chamber measurement largely depend on the chamber size and the
flux rate. The errors associated with the measurement technique
within the flux ranges tested varied from approximately 15%
to 65% of the actual flux rate. The large flux chamber and the
smaller flux rates produce the least error in measurement. Since
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461
Table 2. Actual flux rates and measured flux rates.
Chamber
configuration

Actual CO2 flux


rated (mol m2 d1 )

Measured CO2 flux


rate (mol m2 d1 )

Error in
measurement (%)

Smalla

2.25
4.5
2.25
4.5
4.5
6.75

0.78
1.62
1.81
3.37
3.83
4.77

65.5
64.0
19.4
25.1
14.9
29.4

Mediumb
Largec
a

10 cm diameter and 5 cm height.


Chamber dimensions: 20 cm diameter and 12 cm height.
c
25 cm diameter and 16.5 cm height.
d
Measured as the gas enters the test cell (N.B. the model predicted all of these
values within a 5% error margin).
b

Fig. 14. CO2 concentration contours after 1 min and 20 min (values are in mol/L).

(a)
the model could effectively reproduce the actual flow rates, the
model is being used here to estimate the errors in flux chamber
measurements. It should be noted that the comparison of model
outputs and experimentally derived concentrations within the
flux chamber have shown that the mathematical model is capable of predicting the actual gas flux rates with a maximum error
of 5%.
In a field situation, if the model input parameters are known,
the flux chamber measurements can be corrected using the
model simulations to determine the actual flux rate of gas emissions from the surface of a landfill cover. If large-sized flux
chambers are used, the model can be used to correct the values

(b)
obtained within the first 20 min. On the other hand, with smallsized flux chambers the model can be used to increase accuracy
of measurements within the first 10 min. The experimental and
model simulation results also imply the need to use large-sized
flux chambers in the field to obtain accurate gas measurements.
An example of further model simulation is shown in Fig. 14.
This figure shows the effect of flux chamber on individual velocity vectors of gas at times 1 and 20 min. As gas pressure builds
up within the flux chamber, the flow lines of CO2 are significantly affected. The effect is small at the beginning (at time 1
min) but high after 20 min. A further strength of the model is
its potential to be used to develop sets of curves to determine
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462

errors for any type of closed flux chamber and a range of possible flux rates. Such curves could be used to eliminate errors
(without running the model) and select the best configuration
of the flux chamber for a given range of flux rates.
At this stage of the development of the model, several limitations exist. First, the model cannot be directly applied in a
field situation where local nonhomogeneities exist in the landfill cover. Most landfill covers encountered in practice consist
of several layers of soil with variable soil properties. Consideration of flow of landfill gas through multiple layers of soil could
further enhance the predictive capabilities of the model. Second,
the application of the model requires accurate determination of
model parameters. Uncertainties in model parameter values affect the accuracy of the results. Third, inclusion of other gases,
such as CH4 , may require consideration of other processes impacting gas flow in landfill cover soils. In the case of CH4 ,
methanotrophic bacteria in landfill cover soil are known to biologically oxidize CH4 to CO2 (Stein and Hettiaratchi 2001).
This may require inclusion of a reactive term, S, in the model.
However, if advection and dispersion are the primary mechanism governing flow, biological oxidation may not provide
changes to flow patterns. Since changes to flow patterns determine the errors associated with flux chambers, consideration of
a single gas (such as CO2 ) may be sufficient to eliminate errors
associated with most flux chamber measurements.

Conclusions
The lack of sufficiently accurate and convenient surface gas
emission measurement techniques limits the capacity to estimate surface emissions of gases from landfills. The simplest and
the most popular technique for point estimation of landfill gas
fluxes, the closed flux chamber technique, provides inaccurate
results under certain situations. The closed flux chamber, once
placed on top of a landfill cover during a measurement, alters the
concentration gradient in the soil and thereby underestimates
the actual emission rate. The errors largely depend on the configuration of the flux chamber and the flux rate. The smaller the
chamber and higher the flux rate, the higher the percentage error in measurement. To minimize the errors associated with this
technique, a mathematical modeling approach is proposed. The
application of the two-dimensional advectivedispersive mathematical model will help maintain the simplicity of the flux
chamber technique, but still provide accurate estimates of CH4
emissions. The model is capable of predicting the actual flux
rates within an accuracy level of 5% and, therefore, could be
used to determine the error in a point estimate of landfill gas flux
calculated from closed flux chamber measurements. The laboratory experiments and mathematical model simulations show
that the model is sensitive to gas porosity and dispersivity, but
is fairly insensitive to grid size and intrinsic permeability.

J. Environ. Eng. Sci. Vol. 1, 2002

Acknowledgements
Funding for this research was received from the Natural Sciences and Engineering Research Council (NSERC) of Canada
and the University of Calgary.

References
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Bogner, J.E., Meadows, M., and Czepiel, P. 1997. Fluxes of methane
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IPCC (Intergovernmental Panel on Climate Change). 2001. Technical
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Perera et al.

List of symbols
A
C
Cm
CO2
D
Dj
D*
Dair
Dsoil
F
H
kj
krel
L

area of the flux chamber (m2 )


concentration of the component gas inside the chamber
(g m3 )
concentration of gas m (mol m3 )
concentration of O2 (mol m3 )
dispersion coefficient (m2 s1 )
coefficient of dispersion in j direction (m2 s1 )
molecular diffusion (m2 s1 )
diffusion coefficient in air (m2 s1 )
diffusion coefficient in soil (m2 s1 )
rate of gas emission into the chamber (g m2 s1 )
height of the chamber (m)
intrinsic permeability in j direction (m2 )
relative permeability
distance to the right boundary from the chamber centre
(m)

463
Mm
P
R
Rc

QBottom
qm
S

T
u
uj
V
X
Ym

molecular weight of gas m (g mol1 )


pressure (Pa)
universal gas coefficient (8.314 J K1 mol1 )
radius of the chamber (m)
gas flux rate at the bottom boundary (mol m2 s1 )
gas flux for component m (mol m2 s1 )
source, sink, or reaction (decay, or production rate)
(mol s1 m3 )
absolute temperature (K)
gas velocity (m s1 )
gas velocity in j direction (m s1 )
volume of the flux chamber (m3 )
concentration of organisms (g m3 )
mole fraction of gas m
dispersivity (m)
gas mixture viscosity (Pa s)
porosity

2002 NRC Canada

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