Beruflich Dokumente
Kultur Dokumente
www.elsevier.com/locate/enconman
Abstract
Equilibrium modeling has been used to predict the gasication process in a downdraft gasier. The
composition of the producer gas and, hence, the caloric value have been determined. The eects of initial
moisture content in the wood and the temperature in the gasication zone on the caloric value have been
investigated. The predicted values compare reasonably well with experimental data. The caloric value of
the producer gas decreases with increase in moisture content in the raw material. The caloric value of the
producer gas decreases as the gasication temperature increases in the range of temperatures investigated. 2001 Elsevier Science Ltd. All rights reserved.
Keywords: Renewable energy; Biomass; Gasication; Modeling
1. Introduction
Concern over the depletion of fossil fuels in the near future and an increasing awareness of
energy conservation have drawn worldwide attention. Present energy resources, such as coal, oil
and gas, are being used at an accelerating rate with fear of depletion in the next century, although
coal might be an exception. Apart from this fear, there is also an increasing awareness about
environmental pollution and ways of minimizing the same. There are nine general sources of
energy on Earth. They are: solar, biomass, wind, wave, hydro, tidal, geothermal, nuclear and
fossil. Except for the last three the remaining six are generally called renewable sources of energy,
as they are not depleted with time. One of the most promising renewable sources of energy is the
*
0196-8904/01/$ - see front matter 2001 Elsevier Science Ltd. All rights reserved.
PII: S 0 1 9 6 - 8 9 0 4 ( 0 0 ) 0 0 0 7 8 - 9
1500
energy from biomass. It is, however, appropriate at this juncture to emphasize conservation of
energy. Energy conserved is energy available for other uses. Energy is not utilized properly in the
world. It is, therefore, imperative to educate people to be more energy conscious and to treat
conservation of energy as important as nding an alternative form of energy. Many countries
have already started programs to recycle waste materials. Similarly, the utilization of waste
material to form fuel sources is most welcome and appreciated. Biomass materials constitute the
greatest proportion of waste materials.
Biomass material does not only arise from wastes. Energy plantations have been a subject of
study by many researchers to form a continuous supply of energy. Suitable crops that grow
rapidly have been tested, such as willow trees that are being used and tested in the United
Kingdom. Other similar fast growing crops are also being studied, such as the Euphorbia
Characias [1]. In the Netherlands, poplar and miscanthus are the two most promising types of
specically grown biomass for energy generation [2]. Miscanthus and other species, such as
Sorghum, are C4 crops characterized by high rates of carbon assimilation. Sims [3] comments that
the greatest potential source of biomass fuels in New Zealand comes from energy plantations of a
species known as Pinus Radiata.
Most of the biomass materials are found in the developing countries in Africa and Asia whose
main sources of revenue are agriculture, timber logging, animal rearing etc., where biomass is the
main byproduct. The rst impression is that biomass energy would be the most viable form of
energy in the developing countries. However, in recent years, the developed countries in Europe in
particular have promoted the importance of biomass energy [48]. Hence, biomass energy is not
only essential in the developing countries but has also aroused great interest in Europe. Sweden
has continued to invest in the biomass energy program as a renewable energy source [9]. The
diculties faced during the Second World War have always been a constant reminder to the
Swedes and should be for most countries in the world whose prime dependence is on imported
fossil fuel.
Utilization of biomass is a very important source of energy in many parts of the world, especially for areas remote from a supply of high quality fossil fuels, such as natural gas, liqueed
petroleum gas (LPG) etc. For small installations producing less than 1.5 MW thermal, coal is not
a popular fuel owing to its high sulphur content (typically 0.52%) and the resulting necessity for
expensive removal of SO2 from the stack. Biomass gasication treats the solid feed material in a
reactor such that virtually all of it is converted into fuel gas with caloric values typically 35 MJ/
m3 (natural gas is 34 MJ/m3 ) with most of the energy being available from H2 and CO. After
cleaning, this gas can be used to run small reciprocating engines, boilers, process heaters etc.
Narvaez et al. [10] have studied biomass gasication with air in a small pilot plant in a bubbling
uidized bed, and the eect of several variables on the performance of the gasier has been investigated. Brookes [11] discussed a gasier for biomass waste and related volatile solids. Delgado
et al. [12] discussed upgrading (cleaning) the raw hot gases from a bubbling uidized bed biomass
gasier using cheap calcined minerals or rocks downstream from the gasier. Goldman et al. [13]
demonstrated the possibility of a two phase counterow concept as a means of providing super
adiabatic conditions, which are expected to enhance weak exothermic reactions and endothermic
gasication reactions in the reforming zone. They have also developed a mathematical model
based on a simplied case with a single source of reaction liberated energy to obtain temperature
proles in the gasication process. The United States Department of Energy (DOE) has a major
1501
goal in the development of cost competitive technologies for the production of power from renewable biomass crops. Paisley and Anson [14] discussed the development and commercial
demonstration of the Battelle high through-put gasication process power generating system.
Hughes et al. [15] use a modeling approach to simulate the eect of varying moisture content in
the gasier feed biomass. Jorapur et al. [16] report the commercial scale (1080 MJ/h) development
of a gasication system using low density biomass (sugar cane leaves and bagasse, bajra stalks,
sweet sorghum stalks). Ergudenler et al. [17] validated a mathematical model for uidized bed
gasication of biomass using experimental data from a 400 kW thermal dual distributor type
uidized bed gasier. They also showed that the model predictions improved substantially when
the tar formation is included in the model. The amount of tar formed in a downdraft gasier is
very low, and it is ignored in our mathematical model. Beenackers [18] presents a critical review of
the moving bed biomass gasier system presently commercially available or under development in
the European Union. A spectacular increase in interest in biomass gasication technology is
hosted as catalyzed by the EC JOULE and AIR programs.
In view of the considerable interest in the gasication process world wide, it is necessary to
model and predict the performance of the gasier before the design of a gasier can be undertaken. In this paper, an equilibrium modeling of the gasication process is performed to predict
the composition of the fuel gas produced and the associated caloric values.
2. Analysis
The equilibrium model assumes that all the reactions are in thermodynamic equilibrium. It is
expected that the pyrolysis product burns and achieves equilibrium in the reduction zone before
leaving the gasier, hence an equilibrium model can be used in the downdraft gasier. The reactions are as follows:
C CO2 2CO
C H2 O CO H2
C 2H2 CH4
Eqs. (1) and (2) can be combined to give the shift reaction
CO H2 O CO2 H2
PCH4
PH2 2
PCO2 PH2
:
PCO PH2 O
The typical chemical formula of woody material, based on a single atom of carbon, is
1502
CH1:44 O0:66
The global gasication reaction can be written as follows:
CH1:44 O0:66 wH2 O mO2 3:76mN2 x1 H2 x2 CO x3 CO2 x4 H2 O x5 CH4
3:76mN2
where w is the amount of water per kmol of wood, m, the amount of oxygen per kmol of wood, x1 ,
x2 , x3 , x4 and x5 , the coecients of constituents of the products.
Note:
mass of water
18w
100% ) MC
100%:
mass of wet biomass
24 18w
Therefore,
w
24MC
:
181 MC
Hydrogen balance:
2w 1:44 2x1 2x4 4x5 ) w 0:72 x1 x4 2x5 :
Oxygen balance:
w 0:66 2m x2 2x3 x4 :
Equilibrium constant from methane formation (Eq. (5)):
x5
K1 2 :
x1
10
11
x1 x3
:
x2 x4
The equation for the heat balance for the gasication process, assumed to be adiabatic, is:
12
1503
x1 Hf0H2 x2 Hf0CO x3 Hf0CO2 x4 Hf0H2 Ovap x5 Hf0CH4 DT x1 CpH2 x2 CpCO
x3 CpCO2 x4 CpH2 O x5 CpCH4 3:76mCpN2 :
Since Hf0H2 , Hf0N2 and Hf0O2 are zero at ambient temperature, Eq. (13) reduces to:
Hf0wood w Hf0H2 Ol Hvap x2 Hf0CO x3 Hf0CO2 x4 Hf0H2 Ovap x5 Hf0CH4
DT x1 CpH2 x2 CpCO x3 CpCO2 x4 CpH2 O x5 CpCH4
3:76mCpN2 ;
13
14
where Hf0wood , is the heat of formation of wood, Hf0H2 Ol , the heat of formation of liquid water,
Hvap , the heat of vaporization of water, Hf0H2 Ovap , the heat of formation of water vapor, Hf0CO ,
Hf0CO2 , Hf0CH4 , are heats of formation of the gaseous products, CpH2 , CpCO , CpCO2 , CpH2 O , CpCH4 , CpN2 ,
are specic heats of the gaseous products, DT T2 T1 , T2 , the gasication temperature at the
reduction zone; T1 , the ambient temperature at the reduction zone.
Eq. (13) can be simplied to be:
dHwood w dHH2 Ol x1 dHH2 x2 dHCO x3 dHCO2 x4 dHH2 Ovap x5 dHCH4
3:76m dHN2 ;
15
DH DT Cpg ;
16
x2
x3 :
17
x1
2x5 :
18
x1
21
x2 x3 ) x4
x1 2x2 2x3 w
1:28:
19
1504
m 1=2x2 2x3 x4
0:66:
20
x1 2x2 2x3 w
1:28
0:66
1:94:
21
22
x3 x21 K1 ) x21 K1 x2 x3
x2
1 0:
23
24
x2 x1 2x2 2x3 w
K2 x1 x2 w
1:28K2 0
1:28K2 x2 2K2 x2 2
x1 x3 2K2 x2 x3 0:
25
Substitution of Eqs. (17), (19) and (21) into Eq. (15) gives:
x1 dHH2 x2 dHCO x3 dHCO2 x1 2x2 2x3 w
1
x2
) dHH2
dHH2 Og
1:94 dHN2
dHCO2 2 dHH2 Og
1:28 dHH2 Og
1:28 dHH2 Og
3:6472 dHN2
dHwood
w dHH2 Ol 0
dHwood 0:
26
dHH2 Og
1:88 dHN2 ;
B dHCO 2 dHH2 Og
C dHCO2 2 dHH2 Og
D dHH2 Og
E dHCH4
dHH2 Ol ;
1:28 dHH2 Og
3:6472 dHN2
dHwood :
27
The systems of remaining equations are 3, two nonlinear equations (23) and (25), and one linear
equation (27). The set of equations is solved using the NewtonRaphson method.
The heat of formation equation for the formation of 1 mol of solid biomass wood CH1:44 O0:66
from solid carbon, hydrogen and oxygen is:
Csol 0:72H2g 0:33O2g ! CH1:44 O0:66
28
1505
and in reality, the reaction cannot occur. The formation of CH1:44 O0:66 is based on the following
reactions:
DHc 393 509
C O2 ! CO2
0:72H2 0:36O2 ! 0:72H2 O
DHc 0:72 241 818
CO2 0:72H2 O ! CH1:44 O0:66 2:06O2
C 0:72H2 0:33O2 ! CH1:44 O0:66
Therefore, the heat of formation of wood is 118 050 kJ/kmol. Hence, the heat of formation
for any biomass material can be determined if the ultimate analysis and the heating value of the
material are known. The heating value can be determined experimentally by a bomb calorimeter,
and according to Reed and Levie [19], the heat of formation of any biomass material can be
calculated with good accuracy from the following:
DHc HHV kJ=kmol 0:2326146:58C 56:878H
51:53O
6:58A 29:45;
29
where C, H, O and A are the mass fractions of carbon, hydrogen, oxygen and ash, respectively, in
the dry biomass. The ultimate analyses and the heating values for various biomass materials are
shown in Table 1. The chemical formula of any biomass material can be determined if the ultimate
analysis is known.
At constant pressure, the specic heat can be written as:
oH
30
Cp
oT p
or
dH Cp dT
Z
DH
T2
T1
31
Cp dT ;
32
T1 ;
33
where Cpmh is the average specic heat over the temperature change
R T2
Cp dT
T
:
Cpmh 1
T2 T1
34
Table 1
Ultimate analyses for various biomass materials chosen (dry basis, weight percentage) [20]
Material
Ash
HHV (kJ/kmol)
Wood
Paddy husk
Paper
Municipal waste
50.0
38.5
43.4
47.6
6.0
5.7
5.8
6.0
0.0
0.5
0.3
1.2
0.0
0.0
0.2
0.3
44.0
39.8
44.3
32.9
15.5
6.0
12.0
449 568
402 133
454 864
433 034
1506
The dependence of specic heat on temperature is given by an empirical equation and the most
simplied version is [20]:
C
D
2
;
35
4Tam T1 T2
Cpmh R A BTam
3
T1 T2
where Tam T1 T2 =2 is the arithmetic mean temperature and A, B, C and D are the constants
for the properties of the gases concerned (the values of the constants are shown in Table 2) and R
is the universal gas constant (8.314 J/mol K).
For example, take the gasication temperature, T2 750C (1023 K) and the ambient temperature, T1 25C (298 K)
)
36
Substituting the values of A, B, C and D for the gases concerned, the specic heat of the gas can be
obtained as follows:
CpH2 O 37:14 kJ=kmol K;
CpH2 29:55 kJ=kmol K;
CpCO 31:04 kJ=kmol K;
CpCO2 47:96 kJ=kmol K;
CpN2 30:64 kJ=kmol K;
CpCH4 55:39 kJ=kmol K:
Therefore, after the gasication process, the temperature of the gas increases from T1 298C
to the gasication temperature T2 1023C. The enthalpy change DH can be obtained using Eq.
(33),
Table 2
Heat capacities (constants A, B, C and D) [20]
Chemical species
Formula
Tmax
103 B
Methane
Hydrogen
Carbon monoxide
Carbon dioxide
Nitrogen
Water
Carbon
CH4
H2
CO
CO2
N2
H2 O
C
1500
3000
2500
2000
2000
2000
2000
1.702
3.249
3.376
5.457
3.280
3.470
1.771
9.081
0.422
0.557
1.047
0.593
1.450
0.771
106 C
2.164
10 5 D
0.083
0.031
1.157
0.040
0.121
0.867
DH Cpmh T2
T1 ;
T2
T1 1023
1507
298 725;
37
where DG0 is the standard Gibbs function of formation, and the values for the gases involved are
shown in Table 3 and DH0 is the heat of formation. The dependence of DG0 with temperature T
can be written as follows:
dDG0 =RT
DH 0
dT
RT 2
with reference to Eq. (37),
DG0
RT
38
ln K
therefore,
d ln K DH 0
:
dT
RT 2
39
The above equation gives the eect of temperature on the equilibrium constant. If DH0 is negative,
that is if the reaction is exothermic, the equilibrium constant will be reduced if the temperature
increases. On the contrary, K increases with T for an endothermic reaction.
Since the heat of formation is a function of T, Eq. (39) can be integrated as follows:
Table 3
Gibbs functions of formation at 298.15 K (kJ/kmol) [20]
Chemical species
Formula
Phase
Water
Water
Carbon dioxide
Carbon monoxide
Methane
Hydrogen
Oxygen
Nitrogen
H2 O
H2 O
CO2
CO
CH4
H2
O2
N2
g
l
g
g
g
g
g
g
DG0f 298
0
0
0
228 572
237 129
394 359
137 169
50 460
1508
Z
ln K
DH 0
dT I;
RT 2
40
where I is the constant of integration. DH0 is given in the following equation [20]:
DH 0 J
DB 2 DC 3 DD
T
T
;
41
DAT
R
2
3
T
R
where J is a constant.
DA, DB, DC, DD are the coecients for determining specic heat. Substitution of Eq. (41) into
Eq. (40) and integrating gives:
J
DB
DC 2 DD
DA ln T
T
T 2 I:
RT
2
6
2T
0
From Eq. (37), DG RT ln K and multiplying Eq. (42) with
DB
DC 2 DD
0
T
T 2I :
DG J RT DA ln T
2
6
2T
42
ln K
RT gives:
43
Eqs. (41)(43) will be used to nd the equilibrium constant for any reaction temperature T. For
this purpose, knowledge of the specic heat is sucient to determine the constants J and K. The
constant J can be determined using Eq. (41) at the temperature of 298.15 K where the value DH0 is
known. Similarly, the constant I is determined using Eq. (42) or Eq. (43) at the temperature at
which the values of ln K or DG0 are known, normally at 298.15 K.
In this paper, two equilibrium equations are required to determine the equilibrium constants K1
and K2 . K1 is the equilibrium constant for the reaction of Eq. (3) and is solved as follows: DA, DB,
DC and DD can be obtained from the data of heat capacity. For the reaction from Eq. (3),
C 2H2 CH4
D CH4 C 2H2
The equations to determine the values of DA, DB, DC and DD can be written as [20]:
DA ACH4
AC
2AH2 ;
DB BCH4
BC
2BH2 ;
DC CCH4
CC
2CH2 ;
DD DCH4
DC
2DH2 :
1:771
0:771
0
0:867
23:249
6:567;
20:422 10
20 10
7:466 10 3 ;
2:164 10 6 ;
Calculation of the constants J and I for Eqs. (41) and (43) at 298.15 K requires the values for
0
and DG0298 . This data is available from the heat of formation data (Table 4) and the Gibbs
DH298
function of formation (Table 3).
1509
Table 4
Heats of formation at 25C (kJ/kmol) [20]
Chemical species
Formula
Phase
Water
Water
Carbon dioxide
Carbon monoxide
Methane
Hydrogen
Oxygen
Nitrogen
H2 O
H2 O
CO2
CO
CH4
H2
O2
N2
g
l
g
g
g
g
g
g
0
0
DH298
DH298
CH4
0
DH298
DG0298
74520 0
DG0298 CH4
DG0298
50460
0
DH298
C
0
2 DH298
H2
0
DH298
(kJ/kmol)
0
0
0
241 818
285 830
393 509
110 525
74 520
20 74520 J=mol;
DG0298 C 2 DG0298 H2 ;
0
50460:
Substituting the known values into Eq. (40) for T 298:15 K gives
74520 J
7:466 10
6:657298:15
2
8:314
R
298:152
2:164 10
3
298:153
0:701 105
298:15
)
)J
7082:848
58886:8:
Substituting the known values into Eq. (43) for T 298:15 K gives
50460
58886:8
8:314298:15
2:164 10
298:152
6:567 ln 298:15
0:701 10
2298:152
7:466 10
2
298:15
) I 32:541:
Therefore, the general equation for ln K1 (using Eq. (42)) is:
ln K1
7082:848
7:466 10
6:567 ln T
T
2
5
0:701 10
32:541:
2T 2
2:164 10
6
T2
44
1510
The equilibrium constant K1 for any temperature T can be obtained by substituting the temperature T into Eq. (44). A similar procedure is used to determine the equilibrium constant K2 for
the reaction of Eq. (6), that is
CO H2 O CO2 H2
After going through the calculation steps, the general equation ln K2 is obtained as follows:
5870:53
58200
18:007:
45
1:86 ln T 2:7 10 4 T
T
T2
Similarly, the equilibrium constant K2 for any temperature T can be obtained by substituting the
temperature T into Eq. (45).
ln K2
Fig. 1. Eect of moisture content in the wood chips on gas composition at 800C.
1511
Fig. 2. Concentration of H2 against moisture content at 800C for dierent biomass materials.
Fig. 3. Concentration of CO against moisture content at 800C for dierent types of biomass material.
Fig. 2 shows the composition of hydrogen plotted against the moisture content for various raw
materials, like paper, wood, municipal waste and paddy husk. It is surprising to nd that the
percentage of hydrogen in the fuel gas increases almost linearly with moisture content. At any
given moisture content, the composition of hydrogen in the fuel gas is highest for paper and
minimum for paddy husk with wood and municipal waste lying between these two compositions.
It is not surprising that the hydrogen in the fuel gas produced by the raw material paper is
maximum as it contains only carbon, hydrogen and oxygen.
Fig. 3 shows the variation of carbon monoxide in the producer gas as a function of the raw
materials moisture content. We observe a reduction in the percentage of carbon monoxide with
moisture content for all the raw materials. At any given moisture content, the percentage of
carbon monoxide is highest for wood and minimum for paddy husk. The reduction in the percentage of carbon monoxide with moisture content is almost linear.
1512
Fig. 4. Concentration of CH4 against moisture content at 800C for dierent biomass materials.
Fig. 5. Caloric value against moisture content at 800C for dierent biomass materials.
Fig. 4 shows the percentage variation of methane with moisture content. It is seen from the
gure that the highest percentage of methane is associated with paper followed by wood, municipal waste and paddy husk. The variations of methane percentage in all the raw materials
increase linearly with increase in moisture content. However, it is to be noted that the methane
content in the producer gas is very small compared to those of hydrogen and carbon monoxide.
Fig. 5 shows the variation of caloric values for several raw materials against moisture content.
This is expected in view of the greater reduction in carbon monoxide content compared to the
increase in the hydrogen content as moisture content increases, as shown in Fig. 1. It is seen that
the caloric values decrease with increase in moisture content. Paper and wood have the highest
caloric values and paddy husk the minimum with municipal waste lying between.
1513
Fig. 6. Caloric value against temperature for wood at 20% moisture content.
Table 5
Comparison between model and experimental results for wood at 20% moisture content and gasication temperature of
800C
Hydrogen (%)
Carbon monoxide (%)
Methane (%)
Carbon dioxide (%)
Nitrogen (%)
Oxygen (%)
Caloric value (MJ/m3 )
Model
Experiment [21]
21.06
19.61
0.64
12.01
46.68
0
4.72
15.23
23.04
1.58
16.42
42.31
1.42
4.85
Table 6
Iteration results
k
x1
x2
x3
kxk
0
1
2
3
4
5
0.6
0.549 668
0.574 508
0.574 642
0.574 643
0.574 643
0.6
0.825 641
0.798 702
0.798 437
0.798 437
0.798 437
0.3
0.151 526
0.17 619
0.176 397
0.176 397
0.176 397
xk
0.24 413
0.054 225
0.000 445
0.000 001
0
k1
1514
Fig. 6 shows the variation of caloric value against gasication temperature for the raw material wood with an initial moisture content of 20%. It can be observed that the predicted caloric
value reduces with increase in temperature. The experimental points [21] corresponding to this
temperature are also marked on the same gure. It can be observed that a good agreement exists
between the predicted values and the experimental data, indicating that the equilibrium model
predicts reasonably well the caloric value for a downdraft gasier.
Table 5 shows the composition of the producer gas at a gasication temperature of 800C for a
wood with 20% moisture content. It can be observed from the table that the predicted combined
percentage of hydrogen and carbon monoxide content (which are responsible for the caloric
value of fuel) is predicted as 40.67% against an experimental value of 38.27%. The hydrogen
percentage predicted is more than the experimental value, while the carbon monoxide percentage
predicted is lower than the experimental result. The predicted caloric value 4.72 MJ/m3 compares
reasonably well with the experimental value of 4.85 MJ/m3 .
4. Conclusion
The modeling of a gasication process in a downdraft gasier is performed using an equilibrium model. The calculations of the composition and the caloric value of the producer gas with
wood as a raw material are illustrated. In addition to wood, the predictions are also determined
for paddy husk, paper and municipal waste. The predicted caloric values compare reasonably
well with the experimental values available in the literature for wood. The equilibrium model
predicts the caloric value reasonably well for the downdraft gasier. With known ultimate
analysis of any biomass and its caloric value, the model can predict the composition and the
caloric value of the producer gas.
From the analysis, the following conclusions are made:
1. The content of hydrogen in the producer gas increases with moisture content for all the materials considered, almost in a linear fashion.
2. The carbon monoxide content in the producer gas decreases with moisture content for all the
materials considered, almost in a linear variation.
3. The methane content in the producer gas increases linearly with moisture content, however, the
percentage of methane in the producer gas is quite small and is of the order of 1%.
4. The caloric value of the producer gas decreases with the increase in moisture content for all
the raw materials studied.
5. The caloric value reduces as the gasication temperature increases in the range of temperatures studied.
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