ISBN 978-983-42035-9-7

Proceedings of International Conference for Technical Postgraduates (TECHPOS 2009)

Kula Lumpur, Malaysia, 14-15December, 2009
Abstract Due to energy and environmental
issues, hydrogen becomes a more attractive
clean fuel. There is high interest to produce
hydrogen from biomass in view of
sustainability. The thermo chemical process
i.e. gasification is highlighted for hydrogen
production. This paper discusses the
mathematical modeling of hydrogen
production through steam gasification with
calcium oxide as sorbent in one gasifier. The
model framework consists of kinetics model
based on chemical reactions with few
assumptions using MATLAB. This work
investigates the influence of the temperature,
steam/biomass ratio and sorbent/biomass
ratio on the hydrogen and product gas
composition. The importance of different
reactions involved in the system is also
discussed. The model helps to predict the
product gas composition and hydrogen gas
mole fraction from biomass. It is observed
that at 1000 K temperature,3.0 steam/biomass
ratio and 1.0 sorbent/biomass ratio maximum
hydrogen mole fraction obtained in the
product gas i.e. 0.82. At sorbent /biomass 1.52,
purity of hydrogen is increased to 0.98 mole
fraction with all CO
2
present in system
absorbed.
KeywordsHydrogen, Biomass gasification, CO
2
Adsorption, Kinetics Modeling.
I. INTRODUCTION
The current main energy sources are
fossil fuels but due to the energy crisis and
environmental issues, alternative and renewable
energy sources are now under focus for
sustainable supply of energy in the future. One
of the main renewable energy sources is
biomass, which is considered for the production
of hydrogen as a clean and environment friendly
fuel [1,2]. The potential for production of
hydrogen from biomass in Malaysia is logical
due to the agricultural land and availability of
abundant biomass. Biomass can be use to
produce enriched hydrogen gas via two thermo
chemical processes, pyrolysis and gasification.
Balat [3] reported that hydrogen production via
gasification process is more economical than the
pyrolysis process. The quality of hydrogen and
product gas varies with different gasification
agents i.e. air, oxygen-steam and pure steam,
used for gasification process [4]. Moreover, the
production of hydrogen can increased to more
than 80% by using CO
2
adsorption technique in
steam gasification process [5].
Several attempts have been carried out
to evaluate for the hydrogen production from
biomass by using CaO as CO
2
sorbent. New
approach for biomass gasification to hydrogen
by using CaO as CO2 sorbent has been
introduced by Mollenstedt et al. [5]. By coupling
two fluidized beds, they have shown that
hydrogen yield can be increased in product gas
using adsorption technique from 70% to 85%.
Furthermore, Mahishi and Goswami [6] studied
steam gasification of pine bark in the presence of
CaO as sorbent. Their results showed high yield
of H
2
70% in product gas. Additionally, Florin
and Harris [7] discussed the effect of CaO in
biomass gasification and observed that CaO also
act as a catalyst as well and H
2
yield can increase
double. They also mentioned that maximum
yield of H
2
from 57% to 80% when using CO
2
sorbent.
In literature, there are numerous models
developed to explain gasification process. Some
of them are highlighted in the next few
paragraphs. Corella and Sanz [8] presented a
mathematical model for circulating fluidized bed
biomass gasifier based on hydrodynamic and
kinetics parameters. Reaction network has been
solved using heat and mass balances. In this way
they describe that temperature and some other
parameters can be calculate to optimize the
Kinetic Modeling of Biomass Steam Gasification
System for Hydrogen Production with CO
2
Adsorption
Abrar Inayat, Murni Melati Ahmad*, M Ibrahim A Mutalib and M Khairuddin Yunus
Department of Chemical Engineering,
Universiti Teknologi PETRONAS,
Bandar Seri Iskandar, Tronoh 31750, Malaysia
*Corresponding author. Tel.: +6053687588; fax: +6053656176.
E-mail address: murnim@petronas.com.my.
ISBN 978-983-42035-9-7
Proceedings of International Conference for Technical Postgraduates (TECHPOS 2009)
Kula Lumpur, Malaysia, 14-15December, 2009
design and operation of gasifier. Furthermore,
Melgar et al. [9] developed a model on thermo-
chemical equilibrium for biomass gasification
process based on equilibrium Gibbs free energy
minimization in MATLAB. The model predicted
the compositions of product with respect to
temperature. Also Mahishi et al. [10] presented a
thermodynamic equilibrium model, which
predicted the optimum temperature, pressure,
steam to biomass ratio and equivalence ratio with
respect to the composition of the product gas.
Nikoo et al. [11] has run simulation using
ASPEN PLUS based on reaction kinetics and
hydrodynamic parameters for biomass
gasification in fluidized bed reactor. The work
investigated the effect of temperature, steam to
biomass ratio and particle size of biomass on the
product gas. Sharma [12] used modeling
technique to predict the reaction temperatures,
unconverted char, and equilibrium constants for
reduction reactions and optimal energy
conversion for a downdraft fixed bed biomass
gasifier. Moreover, Shen et al. [13] simulated
for hydrogen production from biomass using
interconnected fluidized beds. The purpose of the
second fluidized bed is as a combustor to achieve
the heat required for gasification process.
Initially, Kinoshita et al. [14] presented
a model for CO
2
adsorption using CaO as
sorbent using ASPEN PLUS, but for hydrogen
production from bio oil. Proll et al. [15]
illustrated modeling approach for dual fluidized
bed gasification based on mass balances, energy
balances and thermodynamic equilibrium states.
Thus also integrated CO
2
adsorption technique
by using CaO as bed material. The results
explained the thermodynamic limits for dual
fluidized bed reactor with CO
2
adsorption
technique. As modeling approach is faster, less
expensive and can offer wide range than
experimental approach The objective of this
study to investigate the technical feasibility of
hydrogen production from biomass steam
gasification with CO
2
adsorption via
modeling approach. The kinetic behavior model
of the system developed by using MATLAB.
II. METHODOLOGY
The modeling work is carried out by using
these information. The block diagram describing
the gasification processes in one unit is shown in
Fig.1.
A. Assumptions
The following assumptions were
considered in kinetics modeling for gasification
process.
the gasifier operates under steady state
conditions.
biomass is pretreated. i.e. moisture removed
biomass is represented by char.
ash in biomass are considered as inert and
do not participate in the chemical reactions.
the reactions proceed adiabatically and at
constant volume.
carbonation reaction involved in the process
was taking as forward reaction.
B. Reaction Kinetics
In the modeling work, the following
reactions are taken for the process.
Char gasification reaction
C + H
2
O CO + H
2
(R1)
Methanation reaction
C + 2H
2
CH
4
(R2)
Boudouard reaction
C+ CO
2
2CO (R3)
Methane steam reforming reaction
CH
4
+ H
2
O CO + 3H
2
(R4)
Water gas shift reaction
CO + H
2
O CO
2
+ H
2
(R5)
Carbonation reaction
CO
2
+ CaO CaCO
3
(R6)
As there are numerous possibilities for the
kinetics rate equations, so the simplest first order
Fig. 1 Process Block Diagram
ISBN 978-983-42035-9-7
Proceedings of International Conference for Technical Postgraduates (TECHPOS 2009)
Kula Lumpur, Malaysia, 14-15December, 2009
800 900 1000 1100 1200 1300
0.8
0.802
0.804
0.806
0.808
0.81
0.812
0.814
0.816
0.818
Temperature (K)
H
y
d
r
o
g
e
n

(
M
o
l
e

F
r
a
c
t
i
o
n
)
TABLE I
KINETICS PARAMETERS FOR REACTIONS
with respect reacting species is selected for
mentioned reactions.
r

= k

C
A
C
B
(1)
where r is the rate of reaction C is the
concentration of reactant and k is the rate
constant. As water gas shift reaction is one the
very important reaction in gasification process
and also exothermic and reversible. So for the
calculation of rate of water gas shift reaction
following equation used.
r
5
= k
5
(C
C 0
C
H
2
0
+
C
C O
2
C
H
2
K
w
) (2)
where k
5
the rate constant for water gas is shift
reaction and K
w
is equilibrium constant. The
overall volumetric rate of each component is
determined by R according to chemical reaction
engineering rules.
R
H
2
= r
1
+ S r
4
+ r
5
r
2
(3)
R
C 0
= r
1
+2r
3
+r
4
r
5
(4)
R
C H
4
= r
2
r
4
(5)
R
C 0
2
= r
3
+r
5
r
6
(6)
Fig. 2- Effect of temperature on product gas. Biomass feed
rate: 0.072kg/h; Steam/Biomass ratio:3.0; Sorbent/Biomass
ratio:1.0. H2 (), CO (), CO2 (). CH4 ()
The kinetics parameters used for all above
reactions taken from literature listed in table 1.
III. RESULTS ANDDISCUSSION
Among the main variables that can affect the
performance of biomass gasification process are
temperature, steam to biomass fed ratio and
amount of sorbent. The effect of each one of
these parameters are thoroughly studied and
discussed in the following section.
A. Effect of Temperature
Fig. 2 shows the effect of temperature on the
product gas composition versus different
temperatures in the range of 800-1300 K. The
plot shows the value of hydrogen higher than 0.8
mole fraction in product gas due to usage of pure
steam and CO
2
adsorption technique. Based on
Fig.2 it also can be observed that the CO is
increasing along with the increase of
temperature. Thus observation might be due to
the exothermic and reversible behavior of water
gas shift reaction and due to the endothermic
behavior of boudouard, char gasification and
methane reforming reactions. On the other hand
CH
4
and CO
2
are found to be decreasing with the
increasing temperature. The decreasing amount
of CO
2
may be due to the slower water gas shift
reaction at high temperature and calcinations
reaction that is taken as forward reaction in
assumptions. Therefore, by increasing
temperature in gasification process the solid
yield, methane and carbon based yield decreases
and meanwhile the total gas and hydrogen
increases.
Fig. 3- Effect of temperature on hydrogen. Biomass feed rate:
0.072kg/h; Steam/Biomass ratio:3.0; Sorbent/Biomass
ratio:1.0
700 800 900 1000 1100 1200 1300 1400
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
1
Temperature (K)
P
r
o
d
u
c
t

G
a
s

(
M
o
l
e

F
r
a
c
t
i
o
n
)
Reaction Kinetics Parameters References
1 2.010
5
exp(-6000/T) [8], [16], [17]
2 0.12exp(-17921/T) [18], [19]
3 4.40 exp(-1.6210
8
/T) [18], [20]
4 3x10
5
exp(-15000/T) [8], [21], [22], [23]
5
10
6
exp(-6370/T)
Kw=520exp(-7230/T)
[8], [18], [24], [25]
6 10.20 exp(-44.5/T) [26], [27]
ISBN 978-983-42035-9-7
Proceedings of International Conference for Technical Postgraduates (TECHPOS 2009)
Kula Lumpur, Malaysia, 14-15December, 2009
0.5 1 1.5 2 2.5 3 3.5 4
0
1
2
3
4
5
6
7
8
9
10
Steam/Biomass Ratio
H
2
/
C
O

r
a
t
i
o
700 800 900 1000 1100 1200 1300 1400
0
1
2
3
4
5
6
7
8
9
10
Temperature (K)
H
2
/
C
O

r
a
t
i
o
Fig. 4- Effect of temperature on H2/CO ratio. Biomass feed
rate: 0.072kg/h; Steam/Biomass ratio:3.0; Sorbent/Biomass
ratio:1.0
The scaling up of the hydrogen
production at different temperature is clear in
Fig.3. From the figure it concluded that the
maximum hydrogen mole fraction in product gas
composition is at 950 K. The effect of
temperature on the H
2
/CO ratio for the specified
gasification process is shown in Fig.4. it is
observed that the H
2
/CO ratio is higher at lower
temperature thus its value decreases with the
increase of temperature due to the increase of
CO and decrease of hydrogen at very high
temperature, as water gas shift reaction is
reversible at high temperature. A comparison
between the developed model and literature data
is shown in Fig.5. Mahishi and Goswami [6] did
experiments with steam gasification using CaO
as sorbent. Florin and Harris [7] used CaO as
sorbent for modeling results.
Fig. 5- Effect of temperature on hydrogen. This Model (),
Florin et al [7] (), Mahishi et al [5] ()
B. Effect of steam to biomass ratio
Steam to biomass ratio has much importance in
steam gasification process, with increasing steam
to biomass ratio the hydrogen increased, CO and
CH
4
decreased.
Fig. 6- Effect of Steam/Biomass ratio on product gas.
Biomass feed rate: 0.072kg/h; Temperature:1000 K;
Sorbent/Biomass ratio:1.0. H2 (), CO (), CO2 (). CH4 ()
There are some energy losses in result
of very high steam to biomass ratio as steam loss
along the product. Fig.6 shows the result of
product gas behavior by increasing
steam/biomass ratio. Steam is the only
gasification agent being used, so the reaction
with steam, especially methane reforming and
water gas shift reaction are highly dependent on
steam feed rate. Therefore, at higher
steam/biomass ratio the hydrogen yield increases
at high extent, while CH
4
and CO is very low.
Fig.7 shows the curve for H
2
/CO ratio with effect
of steam/biomass ratio. Not like curve of H
2
/CO
ratio with effect of temperature, it shows
opposite behavior, as by increasing
steam/biomass ratio, the H
2
/CO increased, due to
rapid increase of hydrogen and decrease of CO.
At 3.5 steam/biomass ratio, the H
2
/CO ratio is
9.7.
Fig. 7- Effect of Steam/Biomass ratio on H2/CO ratio.
Biomass feed rate: 0.072kg/h; Temperature:1000 K;
Sorbent/Biomass ratio:1.0
700 750 800 850 900 950 1000
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
1
Temperature (K)
H
y
d
r
o
g
e
n
(
M
o
l
e

F
r
a
c
t
i
o
n
)
0.5 1 1.5 2 2.5 3 3.5 4
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
1
Steam/Biomass Ratio
P
r
o
d
u
c
t

G
a
s

(
M
o
l
e

F
r
a
c
t
i
o
n
)
ISBN 978-983-42035-9-7
Proceedings of International Conference for Technical Postgraduates (TECHPOS 2009)
Kula Lumpur, Malaysia, 14-15December, 2009
800
1000
1200
1400 0
1
2
3
0.72
0.74
0.76
0.78
0.8
0.82
Temperature (K)
Steam/Biomass Ratio
H
y
d
r
o
g
e
n

(
M
o
l
e

F
r
a
c
t
i
o
n
)
800
1000
1200
1400 1
2
3
4
5
5.5
6
6.5
7
7.5
8
8.5
9
9.5
Temperature (K)
Steam/Biomass Ratio
H
2
/
C
O

r
a
t
i
o
Fig. 8- Surface plot of hydrogen (mole fraction) for different
temperatures and steam/biomass ratios. Biomass feed rate:
0.072kg/h; Sorbent/Biomass ratio:1.
Fig.8 and Fig.9 show the surface plot with
effect of both temperature and steam/biomass
ratio on hydrogen mole fraction and H
2
/CO ratio.
The surface plot for hydrogen is show that
hydrogen is production increased by increasing
temperature and steam/biomass ratio. At 800 K
with lower steam/biomass 1.0 the hydrogen
amount is 0.73, and at 1300 K and high
steam/biomass ratio i.e. 3.5 the hydrogen amount
is almost 0.80. Furthermore the surface plot
show that the highest hydrogen value 0.82 occurs
at 1000K and with 3.0 steam/biomass ratio. Fig.9
shows that lower temperature and higher
steam/biomass ratio are in favor of higher value
of H
2
/CO ratio due to faster water gas shift
reaction.
Fig. 9- Surface plot of hydrogen H2/CO ratio for different
temperatures and steam/biomass ratios. Biomass feed rate:
0.072kg/h; Sorbent/Biomass ratio:1.0
Fig. 10- Effect of CaO on hydrogen and carbon dioxide
(mole fraction). Biomass feed rate: 0.072kg/h;
Sorbent/Biomass ratio: 1.0; Temperature: 1000 K;
Steam/Biomass ratio: 3.0
At lower temperature of 800 K and higher
value of steam/biomass 3.5, the H
2
/CO at ratio is
at highest i.e. 9.5.
With high temperature 1300 K and higher
steam/biomass ratio 3.5, the H
2
/CO ratio is 5.7.
Even at lower temperature 800 K and lower
steam/biomass ratio 1.0 H
2
/CO is higher 6.4.
Which shown that the high temperature is not in
favor of gasification process using steam as
gasification agent for hydrogen production, due
to increase of carbon monoxide mole fraction at
higher temperature in the product gas.
C. Effect of sorbent to biomass ratio
The presence of sorbent (CaO) in system
increased the hydrogen mole fraction in product
gas by absorbing the CO
2
present in the system.
The difference of H
2
and CO
2
mole fraction in
product gas by using CaO as sorbent is show in
Fig. 10.
Fig. 11- Effect of sorbent/biomass ratio on product gas (mole
fraction). Biomass feed rate: 0.072kg/h; Temperature: 1000
K; Steam/Biomass ratio:3.0.H2 (), CO (), CO2 (). CH4 ()
0 0.5 1 1.5
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
1
Sorbent/Biomass ratio
P
r
o
d
u
c
t

G
a
s

(
M
o
l
e

F
r
a
c
t
i
o
n
)
ISBN 978-983-42035-9-7
Proceedings of International Conference for Technical Postgraduates (TECHPOS 2009)
Kula Lumpur, Malaysia, 14-15December, 2009
Also Fig.10 shown that hydrogen can be
increased from 0.65 to 0.83 and CO
2
decreased
from 0.31 to 0.09 by using CaO as sorbent.
The amount of sorbent influenced a lot on
the production of hydrogen, as sorbent used to
increase H
2
and decrease CO
2
in product gas
composition. Fig.11 shows the effect of amount
of sorbent on product gas of gasification process.
By increasing sorbent /biomass ratio, the H
2
increases and CO
2
decreases. At 1.56
sorbent/biomass ratio, the all CO
2
absorbed by
absorbent and there is no CO
2
more in product
gas. Also along this there is maximum hydrogen
shown that is 0.99 mole fraction. But the
addition of sorbent not effect on the CO and CH
4
due to the H
2
and CO
2
are the end product of
water gas shift reaction, which is one of the main
reaction of the process.
IV. CONCLUSION
A reaction kinetics model is developed
for the prediction of the product gas composition
in a system of steam gasification integrated with
adsorption. Each reaction captured in model that
affect of performance of the biomass gasification
process. Where water gas shift reaction and
methane steam reforming reaction are the main
reactions for hydrogen production. In addition,
for temperature is the important variable, as the
hydrogen production increased by increasing
temperature initially. However, at very high
temperature, hydrogen mole fraction in the
product gas decreases due to the exothermic and
reversible behavior of water gas shift reaction.
Steam/biomass ratio is also very important in
steam gasification process because hydrogen
yield increases by increasing steam/biomass
ratio. Whereas CO and CH
4
decreases in product
gas. Both methane reforming reaction and water
gas shift reaction highly dependent on the steam
feed rate. It is very difficult to get optimum
condition for temperature and steam/biomass
ratio, which predicts the maximum hydrogen, but
an attempt has been done using 3D profiles
shows both effect of temperature and
steam/biomass ratio. It is observed 1000 K and
3.0 Steam/Biomass ratio provides maximum
hydrogen mole fraction in the product gas i.e.
0.82. Maximum H
2
/CO ratio is at lower
temperature and higher steam/biomass ratio due
to the maximum consumption of CO in water gas
shift reaction, as both conditions are in favor of
water gas shift reaction. With addition of CaO as
sorbent, the hydrogen mole fraction in product
gas can be increased from 0.65 to 0.85. At
sorbent /biomass 1.52, purity of hydrogen is 0.98
obtained with all CO
2
present in system
absorbed. Therefore, by capturing CO
2
, the
hydrogen yield increased as reaction is shifted
forward and purity increased as CO
2
is removed
from the system
ACKNOWLEDGMENT
This study has been performed with the
financial support of Petroleum Research Fund of
PETRONAS and Universiti Teknologi
PETRONAS.
NOMENCLATURE
C = Concentration (mol/m
3
)
k = Arrhenius kinetic Constant (s
-1
)
r = Rate of reaction (mol/m
3
s)
K
w
= Equilibrium Constant
R = Volumetric rate of component
(mol/m
3
s)
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