Chemical Engineering and Processing 44 (2005) 717–736

Experimental investigation and modeling of gasification of

sewage sludge in the circulating fluidized bed
I. Petersen, J. Werther∗
Technical University Hamburg-Harburg, Denickestr. 15, D-21073 Hamburg, Germany

Received 31 October 2003; received in revised form 1 September 2004; accepted 1 September 2004
Available online 12 October 2004

Abstract

Experiments of sewage sludge gasification were performed in a circulating fluidized bed of pilot plant scale (15 m height, 0.1 m i.d.). For
the examination of the influence of the air ratio, gasification temperature, feeding height and fluidization velocity several screening tests were
conducted. To understand better the results from the screening experiments, axial profiles of the gas composition were measured. As the most
influencing factor for the heating value of the gasification gas the air ratio was found. Additionally, a low feeding height is recommended for
good gas quality. While feeding into the lower dense zone of a circulating fluidized bed (CFB), mixing of the fuel particles is better. With low
feeding ports, high velocities are attainable and therefore high fuel throughput can be achieved.
In a second step a model of the CFB gasifier was developed. The fluid dynamics of a CFB were included as well as the complete reaction
network of gasification. With the measured axial profiles of gas composition during pyrolysis, and gasification with air and a CO2 /N2 -mixture
kinetic rate expressions for sewage sludge gasification under fluidized-bed conditions were determined which may now be used for reactor
scale-up calculations.
© 2004 Elsevier B.V. All rights reserved.

Keywords: Gasification; Circulating fluidized bed; Reaction kinetics; 1.5-dimensional model

1. Introduction In Germany nowadays the sewage sludge on one hand

Combustion was the primary method of generating heat
and also power (by a using the heat from the combustion in
a steam turbine) from renewable fuels. More recently, gasi-
fication of wood, as well as wastes and also sewage sludge
has come into the discussion. The efficiency of the gasifica-
tion process is better, in principle, because the produced gas
can be used directly in a power generation process. The only
drawback to date for this technology is the high tar and dust
content of the synthesis gas produced. Typical tar content for
wood gasification is in the range of 1–30 g/m3 STP [1]. For
the use in gas-motors or gas-turbines a tar content of only
50 mg/m3 STP is permitted [2,3].
∗ Corresponding author. Tel.: +49 40 428783039; fax: +49 40 428782678.
E-mail address: werther@tu-harburg.de (J. Werther).
is used energetically in mono-combustion plants; it is co-
combusted in coal fired power stations and in municipal solid
waste combustion. On the other hand, sewage sludge is used
as landfill and in agriculture [4]. From 1 June 2005 on, use as
landfill will no longer be permitted. Only pre-treated wastes
can be deposited. The facilities for pre-treatment have only
sufficient capacity for the “normal” wastes. Additional treat-
ment of sewage sludge is problematic [5]. But agricultural
recycling of sewage sludge is controversial. In some German
states, a ban is being drawn up. Agricultural recycling will
probably cease by 2020 [6]. Therefore operators of wastewa-
ter treatment plants are looking for new and reliable disposal
paths for the sewage sludge having high acceptance by the
population and also by the operators of co-combustion facil-
ities.
In Germany utilization of biomass as renewable en-
ergy source is regulated by the German government in the

0255-2701/$ – see front matter © 2004 Elsevier B.V. All rights reserved.
doi:10.1016/j.cep.2004.09.001
718 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736
Renewable Energy Law (EEG) and the Biomass Ordinance
(BiomasseV). The objective of the EEG was to increase the
contribution of renewable energies for the total power con-
sumption, and consequently to reach the goal set by the Euro-
pean Union to double the contribution of renewable energies
for the total power consumption until the year 2010. The def-
inition of “biomass” according to the EEG is given in the
Biomass Ordinance (BiomasseV). The possible processes to
generate power from biomass are also fixed in the Biomas-
seV. Sewage sludge itself is not accepted as “biomass” ac-
cording to the BiomasseV. But in the processes, which are
defined in the ordinance to be possible for power generation
from biomass, it is allowed to add synthesis gas from sewage
sludge gasification to a portion of up to 10% of the total en-
ergy content. In this case a gas with as high as possible energy
content is to be produced in the gasification plant rather than
a real tar-free gas.
But besides the use of sewage sludge as renewable en-
ergy, gasification of sewage sludge is also interesting for co-
combustion in fossil-fired power generation facilities [7]. The
addition of sewage sludge directly to the combustor is some-
times problematic due to the high ash content of the sludge
and the high amount of contaminants (e.g. heavy metals) in
its ash. If sewage sludge gasification is performed before co-
combusting the produced gas in the utility burner, the coal ash
bed is prevented from being polluted by the sewage sludge
ash. In this case, too, the tar amount in the low calorific value
gas from gasification is unimportant as are some unconverted
char particles from the gasifier. Some coal is replaced by
sewage sludge, and additionally the entering gas from the
gasifier produces a reburning-effect, which results in a re-
duction of nitrogen oxides (NOx ) [8,9].
The objective of the present paper is the examination of
sewage sludge gasification. The circulating fluidized bed was
chosen as the gasification reactor, because fluidized beds
are already used mostly in sewage sludge mono-combustion
plants due to the good gas-solid contact, mixing and its
flexibility as far as the fuel composition and condition is
concerned. To understand more deeply the reactions in the
gasification of sewage sludge and to prove the feasibility of
sewage sludge gasification in the circulating fluidized bed, an
experimental examination was carried out at the circulating
fluidized bed pilot plant (0.1 m riser diameter, 15 m high) at
TUHH. To get information about the drying and pyrolysis,
experiments in an inert atmosphere (only nitrogen present)
were performed. CO2 gasification and air gasification were
examined thereafter at different operating conditions. From
these measurements supported by a 1.5-dimensional mathe-
matical model of a fluidized-bed gasifier, the kinetics of py-
rolysis and the main gasification reactions were determined
based on kinetics available in the literature. An equilibrium
calculation for the whole gasification reaction network in the
temperature range commonly used in fluidized-bed combus-
tion and gasification technology was also performed.
A major goal of the present work was to derive a quan-
titative description of the gasification kinetics which should
be applicable under fluidized-bed conditions since a major
drawback of kinetic informations about gasification reaction
networks available in the literature is that they have been ob-
tained from single-particle or fixed bed reactor experiments.
Since heat and mass transfer in a fluidized bed are quite dif-
ferent and since furthermore it is well known from pyrolysis
experiments that the pyrolysis gas yield and the composition
of the pyrolysis gas are strongly dependent on the heating rate
it is highly desirable to obtain information about the gasifica-
tion kinetics directly from fluidized-bed experiments. In the
present work a set of kinetic equations is coupled with a fluid-
dynamic model of a circulating fluidized-bed riser. Numerical
values of three kinetic parameters are then determined not by
simply comparing measured and calculated reactor exit con-
centrations but by fitting the model to measured axial profiles
of the species concentration over the full 15 m of height the
gasification reactor. Although, admittedly, inaccuracies of the
complex fluid-dynamical model will also affect the thus de-
termined values it is believed that the fluidized-bed conditions
are essential for the determination of reaction kinetics which
are to be used for the simulation of fluidized-bed gasifiers.
2. Experimental
Experimental examination was conducted on pyrolysis
and gasification of sewage sludge in order to observe the ki-
netics and the mechanism of devolatilization and the reaction
network. The facility used for the gasification experiments is
the circulating fluidized bed at TUHH (Fig. 1). The circu-
lating fluidized-bed riser is made of stainless steel (German
material number 1.4841) without refractory lining for fast
start-up of the facility. The inner diameters of the riser and
downcomer are 100 and 80 mm, respectively. The riser has a
total height of 15 m. The plant is heated electrically from the
outside. The distributor plate is a bubble-cap distributor with
one bubble cap. The fluidizing gas is preheated electrically
before entering the windbox up to a maximum temperature
of 800 ◦ C.
The gas and some fly ash leaving the facility pass the final
measurement position for the gas quality after the cyclone,
and enter an after-burning chamber where the energy-gas is
completely burned. The after-burning chamber has an inner
diameter of 300 mm and a total length of 4.3 m and is heated
by electrical radiation heating to 850 ◦ C. The residence time
in the after-burning chamber is at minimum 3.3 s. The after-
burning air can be preheated electrically, too.
The plant is equipped with ports for temperature and pres-
sure measurement. In addition there are several ports for in-
serting gas measurement probes. At four positions along the
riser height there are ports for fuel feeding (positions: 1.75,
2.5, 3.5 and 4.6 m). The feeding system is a screw feeder. It
is positioned next to the facility and connected to the plant
by a tube into which the fuel particles are dosed. The tube
is approximately 1.5 m long, and the particles enter the flu-
idized bed due to gravity with their falling velocity. On top
 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736 719

Fig. 1. Flowsheet of the gasification facility.

of the screw feeder the storage is located with enough space
for fuel to operate the plant for one whole day.
Temperature measurement is carried out with Ni–Cr–Ni
thermocouples. Only in the after-burning chamber where
higher temperatures were expected, Pt–Rh–Pt thermocouples
were used. The riser pressure drop is measured with sensors
for differential pressures. The mean total riser pressure drop
during the experiments was held at 7000 Pa. The operation of
the fluidized bed as a gasifier is controlled with gas composi-
tion measurements. The complete combustion of the synthe-
sis gas in the after-burning chamber is also controlled by gas
concentration measurement. In the after-burning chamber an
air ratio of λ = 1.23 was chosen.
Two basically different sampling locations were used: The
measurement ports along the riser height enable gas sam-
pling from inside the riser to probe the axial profile of the gas
composition. In order to separate the sample gas from the
fluidized-bed particles, the gas sampling probe is equipped
with a ceramic filter at the tip of the probe. This ceramic filter
prevents the particles from entering the probe. The ceramic
filter is located inside a stainless steel tube to save the fil-
ter from erosion. The measured gas concentration is a mean
average concentration for the cross section. The other mea-
surement position is directly after the cyclone at the exit of
the plant. Because the particles are already separated from
the gas flow by the cyclone, only some fly ash particles are
720 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736

Fig. 2. Sampling probes for use inside the riser (left) and for position the measurement after cyclone (right).

expected. Therefore the gas sampling probe is designed dif-
ferently. It is just a stainless steel tube with an inner diameter
of 4 mm (suction velocity 4–20 m/s). The fly ash that is sucked
out is separated from the sample gas by a small measurement
cyclone. So at this measurement position not only a gas sam-
ple is taken but also a sample of the fly ash is withdrawn.
To prevent the particles not separated by this small measure-
ment cyclone from plugging the adjacent gas sampling line,
an additional filter is positioned behind the measurement cy-
clone. The measurement cyclone and filter are heated to 250
and 200 ◦ C, respectively. In Fig. 2 both sampling probes are
shown.
Directly after the gas sampling probe and cyclone plus
filter, respectively, is the tar trap. Following the tar trap is the
gas sampling line (Fig. 3). The gas sampling duct is made of
Teflon-tubing, which is electrically heated from the outside
to a temperature of 160 ◦ C to prevent the temperature inside
from dropping below the dew point of water.
The analyzers are fed via a membrane pump. The analyzer
for the water content does not need any more pretreatment of
the sample gas. For the rest of the analyzers, a tar condenser
with glass wash bottles in an ice bath is put in this place. Af-
terwards, the gas passes a cooler and the dry gas is distributed
to the analyzers. The flow to the analyzers is adjusted to one
liter per minute. The analyzers are supplied in series (Fig. 3).
All the main components, which are O2 , CO, CO2 , H2 , CH4 ,
C2 H4 , and H2 O, could be measured online. The oxygen an-
alyzer measures with the paramagnetic effect. The analyzers
for CO, CO2 , CH4 , C2 H4 , and H2 O have a non-dispersive in-
frared (NDIR) detector. The instrument for the measurement
of the H2 concentration has a thermal conductivity detector
(TCD) with cross compensation for CH4 , CO, and CO2 .
The solid materials used in the experiments were the fuel
and silica sand as bed material. No additional catalyst or
limestone was used in the riser. The fuel examined was dried
pelletized sewage sludge from a municipal waste-water treat-
ment plant. In Table 1 the composition (proximate and ulti-
mate analysis) is given.
The particle size distribution was measured before and
after the feeder. The mean particle diameter before was
x3,50 = 2.9 mm. After the feeder the mean particle diameter
was slightly reduced to x3,50 = 2.8 mm. The density of the
sewage sludge was experimentally determined by helium py-
cnometer to 1728 kg/m3 .
As bed material silica sand was used. This sand was avail-
able with two different particle size distributions. The 50%
value of the cumulative mass distribution was found to be

Table 1
Proximate and ultimate analysis of the dried sewage sludge
Mean
Proximate analysis
Volatiles, wt% (waf) 83.4
Combustibles,a wt% (raw) 50.6
Water, wt% (raw) 7.3
Ash, wt% (raw) 42.1
Ultimate analysis
C, wt% (waf) 50.5
H, wt% (waf) 6.6
O,a wt% (waf) 34.5
S, wt% (waf) 1.2
N, wt% (waf) 7.1
Lower heating value (LHV), MJ/kg (raw) 10.0
Fig. 3. Gas measurement system. a By difference.
 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736
x3,50 = 180 ␮m and x3,50 = 203 ␮m, respectively. In most of
the experiments finer sand was used. After each experiment,
the sand from the facility was completely retained. For the
next experiment a mixture of this retained activated bed ma-
terial and new sand was used at the start. The retained bed
material to be reused in the next experiment was sieved to
have particle diameters smaller than 70 ␮m only. The density
of the bed material was experimentally determined by helium
pycnometer as 2687 kg/m3 . The minimum fluidization veloc-
ity umf was determined as 4.4 cm/s for the original sand, and
6.5 cm/s for the mixture of fresh and activated bed material
under ambient conditions with air.
In the experiments the following factors were examined:
• As fluidizing agent air, a CO2 /N2 -mixture, and pure N2
were used, respectively.
• The temperature was varied between 1023 and 1123 K.
• To determine the influence of the air ratio, experiments
with λ = 0.3 and λ = 0.6 were carried out.
• As superficial gas velocities 3.5 and 5 m/s were adjusted,
respectively.
• As feeding height 2.5 and 4.6 m, respectively, above the
distributor plate were examined.
In several screening tests the gas composition was measured
at the measuring position directly after the cyclone at the exit
of the riser. For each of the four influencing factors, which are
air ratio, temperature, feeding height, and superficial gas ve-
locity, two conditions were chosen (two-level factorial design
[10,11]), and experiments with all 16 combinations (24 = 16)
were run. For the air ratio λ = 0.3 and λ = 0.6 were chosen, the
desired temperature was adjusted to 750 and 850 ◦ C, the su-
perficial gas velocity at the top of the riser was 3.5 and 5 m/s,
respectively, and as feeding height the ports on 4.6 and 2.5 m
were examined. These parameters are also listed in Table 2.
To find the reasons for the influences discovered during the
screening tests, for some selected operating conditions axial
profiles of the gas composition were measured. Especially
the conditions inside the riser near the distributor and around
the fuel feeding port were examined. It was of great interest
whether the fuel fed at higher positions reached the bottom
zone or was carried away by the gas flow, in particular at high
gas velocities. Answers were also expected with regard to the
extension of the combustion region in air gasification. Up to
which height is oxygen detectable?
In contrast to the screening test experiments where more
than one condition can be tested during one experimental day,
for the axial profile measurements the plant was operated at
one chosen set of operating parameters for the whole day.
This is also some kind of long-term feasibility test for the
Table 2
Low and high value for screening tests
Factor λ T utop hfeed
Level − + − + − + − +
Value 0.3 0.6 750 ◦ C 850 ◦ C 3.5 m/s 5 m/s 2.5 m
721
operation of the gasifier at the chosen condition. Because
sewage sludge has a high ash content and the ash tends to
bake in the course of time and to form agglomerates which
lead to defluidization, the higher temperatures where omitted
and the axial profile measurements were carried out at 1023 K
only.
An axial profile of gas concentration was also measured
using only N2 as fluidizing gas. Therefore only the pyrolysis
gas composition was measured, although some homogeneous
gas phase reactions will also occur. The pyrolysis experiment
is interesting especially with regard to the carbon oxides. Is
carbon monoxide the only product of devolatilization or will
carbon dioxide be released as well to a certain extent?
In order to examine the CO2 -reforming reactions in gasi-
fication, axial profile measurements were carried out with a
fluidizing agent mixed from N2 and CO2 . Both of them were
supplied from separate gas cylinders containing 100% of car-
bon dioxide and nitrogen, respectively. They were mixed
directly below the distributor plate. The amount of carbon
dioxide in the mixture was desired to be the same as the oxy-
gen in air, so that a switch from air gasification conditions to
the CO2 /N2 -mixture was just a replacement of the oxygen in
the gasifying agent by carbon dioxide.
At first, it was intended to measure additionally the gas
composition with a H2 O/N2 -mixture as gasifying agent, but
as the heat of evaporation must also be supplied by the elec-
trical heating, this idea has been dropped. This is not too
bad because there was no great difference expected between
fluidizing with nitrogen and with a CO2 /N2 - or H2 O/N2 -
mixture, respectively, since Kersten [12] has shown that in
a conventional non-catalytic atmospheric CFB gasifier, op-
erated below 1000 ◦ C, carbon dioxide gasification and steam
reforming reactions do not proceed to a significant extent.
Therefore the measurement of the axial profile of gas com-
position in gasification with a CO2 /N2 -mixture is just an ex-
periment to verify that Kersten’s statement is also true for
sewage sludge gasification.
3. Modeling
It was intended to develop a mathematical model for the
simulation of the gasifier. As it was intended not only to in-
clude the fluid dynamics of the circulating fluidized-bed sys-
tem but also to model the reaction network for gasification,
the main gasification reactions have to be considered. Addi-
tionally a choice had to be made whether these reactions can
be modeled by equilibrium consideration or with a kinetic
approach. It was decided to include kinetic rate expressions
in the simulation program; nevertheless, an equilibrium cal-
culation of gasification was also performed. Kinetic rate ex-
pressions for the gasification reactions included in the model
were chosen from the literature. With the axially measured
gas composition, it should be possible to adjust the kinetic
rate constants measured for coal or biomass to sewage sludge
4.6 m
behavior.
722 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736
The reaction network chosen for the modeling part con-
sists of the devolatilization reaction and the homogeneous
and heterogeneous oxidation and gasification reactions. The
drying process was assumed to occur in parallel with the
devolatilization. For modeling purposes it is important to
know the mass fraction of the initial fuel, which is py-
rolyzed. It is assumed that the total yield of volatiles equals
the volatile content of the parent fuel determined by the
proximate analysis. Subsequently the composition of the
volatiles becomes interesting. For the sake of simplifica-
tion it was assumed that the char consists of pure car-
bon. The released volatiles could be assumed to decom-
pose according to the following stoichiometrically consistent
equation:
Cvc Hvh Ovo Svs Nvn
→ vs H2 S + 2 v n N2
1
+ ξCO vo CO + 2 (1 − ξCO )vo CO2
1
+[(1 − 2ξC2 H4 − 6ξtar )vc − 21 (ξCO + 1)vo ]CH4
+ [ 21 vh − 2(1 − ξC2 H4 − 4.5ξtar )vc + (ξCO + 1)vo
− vs ]H2 + ξC2 H4 vc C2 H4 + ξtar vc C6 H6
In Eq. (1) vi is the mole fraction of component i (i = C, H,
O, S, N) in the volatiles. Eq. (1) assumes that
• All nitrogen is released as N2 . Additionally NH3 could be
taken into account as primary product of devolatilization,
as van der Drift et al. [13] and Kurkela [14] found that
about 60% of the fuel-bound nitrogen is converted to NH3 ,
but for simplicity reasons the component NH3 is neglected
here.
• All sulfur is released as H2 S, because in gasification oxy-
gen is scarce and sulfur will be released as H2 S and not as
SO2 .
• The oxygen might be released as CO only, or as a mixture
of CO and CO2 .
• The rest of the carbon in the volatiles results in the
products CH4 , C2 H4 and an additional tar component
(C6 H6 ).
• The hydrogen not consumed by H2 S and hydrocarbons
will decompose as H2 .
Thus, one has to introduce three splitting factors:
• one parameter for the part of the oxygen reacting to CO
(␰CO );
• one parameter for the fraction of carbon reacting to tar
(␰tar );
• finally, one parameter for the fraction of carbon reacting
to C2 H4 (ξC2 H4 ).
The total flux of volatiles in mol/s depends on the fuel feed
rate ṁfuel and the composition only:
ṁvol ṁfuel xvol,raw
ṅvol = =
Mvol v c M C + v h M H + v o M O + v s MS + v n M N
(2)
The release flux of the gaseous species H2 S, N2 , CO, CH4
and H2 (and CO2 , C2 H4 , C6 H6 ) are only fractions of the total
mole flux.
The heterogeneous reactions occurring during gasification
are char reacting with oxygen, water vapor or carbon dioxide,
respectively. The two reactions with oxygen can be expressed
in one equation, as can the two possible reactions with water
vapor:
␣C + O2 → 2(␣ − 1)CO + (2 − ␣)CO2 , where
1 ≤ ␣ ≤2 (1’)
C + ␤H2 O → (2 − ␤)CO + (␤ − 1)CO2 + ␤H2 , where
1 ≤ ␣ ≤2 (2’)
C + CO2 → 2CO (3’)
The splitting factor α in the combustion reaction
(1) determines the ratio of produced carbon monoxide to car-
bon dioxide. There are empirical correlations available for the
prediction of α. The correlation given by Linjewile and Agar-
wal [15] was used in the present model giving, e.g. α = 1.3
for T = 1023 K and α = 1.2 at T = 1123 K.
In the steam gasification or so-called heterogeneous wa-
ter gas shift reaction (reaction (2 )), the splitting factor β as
introduced by Matsui et al. [16] will be adopted in the model
with the value β = 1.2.
As long as oxygen is present combustion of the gaseous
species CH4 , H2 and CO will take place:
CH4 + 21 O2 → CO + 2H2 (4’)
H2 + 21 O2 → H2 O (5’)
CO + 21 O2 → CO2 (6’)
If all oxygen is consumed, carbon monoxide and hydrogen
could take part in the well-known water-gas shift reaction:
CO + H2 O ↔ CO2 + H2 (7’)
The water-gas shift reaction is an equilibrium reaction.
Depending on temperature, the equilibrium is on the side of
the products or the educts. So the reaction can be driven in
both directions. As reaction (7 ) is a reaction with constant
volume, pressure will not influence the equilibrium.
A very pressure sensitive reaction is the reaction of water
vapor with methane (steam reforming):
CH4 + H2 O ↔ CO + 3H2 (8’)
Also a CO2 -gasification of methane (CO2 reforming) could
be considered. As product gases only CO and H2 are taken
into account:
CH4 + CO2 ↔ 2CO + 2H2 (9’)
 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736
In this study of gasification reactions it was not intended
to model the complete reaction scheme of nitrogen and sulfur
compounds especially as biomass fuels do not contain as
much sulfur as coal does. Therefore the nitrogen and sulfur
contained in the fuel was modeled to be released as volatile
N2 and H2 S, respectively (Eq. (1)).
3.1. Equilibrium calculation
To solve simultaneously the equilibrium of the nine reac-
tion equations, two possible strategies can be pursued. One is
the calculation of the equilibrium composition by minimiz-
ing the Gibbs free energy (or Gibbs free enthalpy) [17]. The
second possibility is to solve the reaction scheme with the
so called relaxation method [18,19]. The relaxation method
was chosen to calculate the equilibrium composition in the
present paper. In this method it is assumed that each reaction
takes place in a separate reactor and reacts to equilibrium.
This equilibrium composition enters the next reactor, and the
next reaction can reach equilibrium. Leaving the last reactor,
the composition enters again the first reactor and the chain of
equilibrium calculation starts a second time. So the equilib-
rium composition for all reactions is found iteratively. The
procedure can be stopped when the molar amount of each
component does not change any more before and after a re-
actor cascade.
All reaction equations defined above were considered. The
Gibbs free enthalpy of reaction and the equilibrium constant
was calculated according to Eqs. (3) and (4), respectively.

the bottom zone the two-phase theory of fluidization [24]
gR0
= vi gf,i
0
(3)
 
gR0
K = exp − (4)
RT
The data for the Gibbs free energy of formation for each
component was taken from the JANAF thermochemical ta-
bles [20]. The data is given for several temperatures in steps
of 100 K. The temperature range from 800 to 1300 K was
chosen, and the calculated equilibrium constants were fitted
to a function of the Arrhenius type to find the equilibrium
constant for each temperature in-between the given temper-
ature steps.
3.2. Kinetic rate expressions
For all kinetic rate expressions r in the model, the unit
used is mol/(m3 s). The gas concentrations are all given in
mol of the model compound and are based on m3 reaction
volume. When in the literature different units were used, the
expressions were modified to fit this unit.
dci
r=
dt
The amount of the reaction rate is related to the reaction
equations formulated above. In order to determine the con-
723
sumption of the components, the reaction rate has to be mul-
tiplied by the stoichiometric coefficient νij of that component
i given in the reaction equation j. The reaction rates used in
the present paper are simplified overall-reaction rates and ac-
count for all mechanisms. This is of course a simplification,
but the gasification process is controlled by the chemical re-
action [21], and the particle size as well as the initial char
mass has no significant effect. As the reactions rates are in
mol/(m3 s), for the solids the reaction rates have to be multi-
plied with the molar mass of the solid species for the balance
equations.
3.3. Model equations
As the facility used for the experiments is very tall, and
horizontal mixing was complete, the first model presented
in the present paper is a 1.5-dimensional or “pseudo two-
dimensional” model. Although concentration changes were
only considered in the axial direction, the model somewhat
describes two dimensions, because the riser was divided hor-
izontally into different phases. The model is unsteady-state
and semi-empirical. Conservation equations for solids and
gas are based on the semi-empirical model by Kruse et al.
[22].
To model the circulating fluidized-bed gasifier, the riser
was cut axially into three zones, the bottom zone, upper dilute
zone and exit zone. As done in Kruse and Werther [23], the
fluid-dynamic behavior of the bottom zone is considered to
be similar to that of a bubbling fluidized bed. Therefore, in
was used. In the upper dilute zone a core-annulus model was
applied. The exit zone was modeled as continuous stirred tank
reactor for gas and solids.
The solid material in the fluidized bed is composed of
inert bed material and fuel. The fuel consists of volatiles, wa-
ter, carbon and ash. To be able to describe the drying, the
devolatilization, and the carbon gasification separately, the
components of the fuel were treated as independent “pseudo
solids”. So four different solid species were considered: car-
bon, ash (or inerts), volatiles, and the solid-bound water. Nine
components in the gas were chosen to represent the gasifi-
cation gas, namely oxygen (O2 ), carbon dioxide (CO2 ), car-
bon monoxide (CO), methane (CH4 ), hydrogen (H2 ), water
(H2 O), nitrogen (N2 ), hydrogen sulphide (H2 S), and a hydro-
carbon representing the tar (C6 H6 ). Benzene was chosen as
the model compound for the tar because it was determined
earlier as the major single component in the producer gas
representing 60–80% of the total tar [25].
In the bottom zone the bubble phase was believed to be
particle free. The suspension contains particles and gas and
was believed to be in minimum fluidization state. Gas flows
in plug flow in both the bubble and suspension phase. The
(5) solids are evenly distributed and are transported by dispersion
only. Gas–solid reactions occur in the suspension phase only.
Homogeneous gas reactions take place in the bubble and in
the suspension phase. Because of the reaction the change in
724 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736

volume of gas results in a higher velocity. The suspension for the solids in the suspension phase of the bottom zone
phase gas stays at minimum fluidization, only the bubble 
∂xsbz,i 
phase gas velocity is increased. Thus, there is a net flow ac- =0 (11)
cording to Yan et al. [26] that considers the production or ∂z z=0
reduction of gaseous volume by reaction. This net flow is

directed from the suspension phase to the bubble phase. In ∂xsbz,i 
−cv,bz Ds,ax ρs
∂z z=Hbz
addition, there is exchange of gas between these two phases.
The conservation equation for the gaseous component i in

the bubble phase in the bottom zone reads as follows: −fd cvd vd ρs (xsd,i − xsbz,i )
= (12)
−(1 − fd )cvl vl ρs (xsl,i − xsbz,i )
∂cgb,i ∂(ub cgb,i )
εb +
∂t ∂z The feeding of gas and solids (feed and return) was de-

scribed by an ousting model instead of absolute mass flow
= −Kbs (cgb,i − cgs,i ) + εb vi,j rb,j + ∆bz ṅ
net flow,i rates. Doing this, it is taken into consideration that for ex-
j(g–g)
ample during feeding the solid volume concentration can in-
(6)
crease or decrease in case the solids present are ousted by
solids with lower volume concentration. The distribution is
In the suspension phase the gas is transported by disper- approximated with the Gaussian error-function (ferf ).
sion and convection with minimum fluidization velocity. The  
conservation equation reads: xsbz,i
ṁReturn,i = 1 − Gs ferf (13)
xReturn,i
∂cgs,i ∂2 cgs,i
(1 − εb )εmf − (1 − εb )εmf Dg,ax  
∂t ∂z2 xsbz,i
ṁ = 1 − ṁ Feed ferf (14)
∂cgs,i
Feed,i
xFeed,i
+ (1 − εb )umf
∂z In the upper dilute zone a core-annulus model with height-


= Kbs (cgb,i − cgs,i ) + (1 − εb )εmf vi,j rsusp,j depending core radius is used. The gas flow across the bound-
j(g–g) ary between the core and the annulus is described by an ex-

change flow, and the change in volume again is modeled by
+ cv,bz vi,j rsusp,j − ∆bz ṅ
net flow,i (7) a net flow. The change in solids across the boundary is due to
j(g–s) convective compensation because of the enlarging or short-
ening of the core and the annulus region. Additionally, be-
The solids in the bottom zone were calculated with trans- cause there will be entrainment of downfalling particles by
port by dispersion only. So the mass balance equation for the the gas stream at the boundary from core to annulus phase,
component i of the fuel particle is the following. an exchange flow for the solid phase was defined. The frac-
tion of the dense phase, i.e. the annulus region, of the total
∂xsbz,i ∂2 xsbz,i
cv,bz ρs − cv,bz Ds,ax ρs cross-sectional area is described by the variable fd . The solids
∂t ∂z2 volume concentration in the two regions is contained in cv


= ṁ
Feed,i + ṁReturn,i + cv,bz Mi vi,j rsusp,j (8) with the index l or d for lean and dense phase, respectively.
j(g–s) For the velocity of gas the variable u and for the velocity
of solids v is used. As in the dense phase the flow is down-
Because the reaction rate is in mol/(m3 s) it has to be mul- ward, the velocities are defined negative. It follows for the
tiplied by the molar mass of the solid component i here, since balance for gas in the dense phase of the upper dilute zone
the balance for the solids is in kg/m3 . for component i:
The boundary conditions for the mass balance equations
∂[fd cgd,i ] ∂[fd cgd,i ]
in the bottom zone are the following. (1 − cvd ) + (1 − cvd )ud
For gas in the bubble phase it holds ∂t ∂z
∂fd
cgb,i |h=0 = cgb,i,IN (9) = (1 − cv,d )ud cgl,i − Kdl,g (cgd,i − cgl,i )
∂z
for gas in the suspension phase 


∂cgs,i  + fd (1 − cvd ) vi,j rdense,j
−(1 − εb )εmf Dg,ax
∂z z=0 j(g–g)
 
∂cgs,i 

= +(1 − εb )umf (cgs,i,IN − cgs,i ), =0 + cvd vi,j rdense,j  − ∆ud ṅ
∂z z=Hbz net flow,i (15)
(10) j(g–s)
 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736 725

the balance for gas in the lean phase for component i: ∂cgez,i
(1 − cv,ez ) Hez
∂[(1 − fd )(1 − cvl )cgl,i ] ∂[(1 − fd )(1 − cvl )ul cgl,i ] ∂t
+ = (−uez + fd (1 − cvd )ud )cgez,i + (1 − fd )(1 − cvl )ul cgl,i
∂t ∂z
 
∂fd


= −(1 − cvd )ud cgl,i + Kdl,g (cgd,i − cgl,i ) + (1 − fd )
∂z + (1 − cv,ez ) vi,j rez,j + cv,ez vi,j rez,j  Hez
  j(g–g) j(g–s)


(23)
× (1 − cvl ) vi,j rlean,j + cvl vi,j rlean,j 
j(g–g) j(g–s) the balance for solids in the exit zone for component i:
+ ∆ud ṅ (16) ∂xsez,i
net flow,i cv,ez ρs Hez
∂t
the balance for solids in the dense phase of the upper dilute = −Gs,i + fd ccv vd ρs xsez,i + (1 − fd )cvl vl ρs xsl,i
zone for component i:

  +cv,ez Mi vi,j rez,j Hez (24)
∂ fd xsd,i ∂ fd xsd,i j(g–s)
cvd ρs + cvd vd ρs
∂t ∂z The variables, which are not yet known, are defined ac-
∂fd
cording to the following closure laws. In the mass balances
= cvd vd ρs xsl,i + fd cvd Mi vi,j rdense,j (17) above the gas and solids velocities (umf , ub , ud , ul , uez , vd , vl )
∂z
j(g–s) have yet to be determined, as well as the void fractions (εmf ,
the balance for solids in the lean phase for component i: εb ) and solid volume concentrations (cv,bz , cvl , cvd , cv,ez )
  and the fraction of the dense zone from the cross sec-
∂ (1 − fd )cvl xsl,i ∂ (1 − fd )cvl vl xsl,i tional area (fd ). The solid density is assumed to be constant
ρs + ρs
∂t ∂z ρs = 2600 kg/m3 . The solids circulation rate Gs as well as the
∂fd
solid volume concentration in the bottom zone and in the exit
= −cvd vd ρs xsl,i + (1 − fd )cvl Mi vi,j rlean,j zone, respectively, are input parameters for the model and are
∂z
j(g–s) taken from measurements.
(18) The minimum fluidization void fraction εmf and velocity
umf have to be determined for the bed material and are input
The boundary conditions for these four equations for the
parameters of the model. The velocity of gas in the dense
gas in the dense phase:
phase is assumed to be constant and was set to −0.75 m/s
at z = Hap − Hez : cgd,i = cgez,i (19) according to optical probe measurements by Schoenfelder
[28]. The solids volume concentration in the dense phase cvd
for the gas in the lean phase: was assumed to be constant over the riser height. cvd was set
to 0.25 according to the findings of Schoenfelder.
at z = Hbz : In the bottom zone it holds
(1 − fd )(1 − cvl )ul cgl,i = −fd (1 − cvd )ud cgl,i + ub cgb,i cv,bz = (1 − εb )(1 − εmf ) (25)
+(1 − εb )umf cgs,i (20)
This relationship defines the solids volume concentration
for the solids in the dense phase: in the bottom zone, which is the fraction not occupied by
the gas phase. The solids volume concentration in the bottom
at z = Hap − Hez : xsd,i = xsez,i (21) zone was assumed to be constant and was set to cv,bz = 0.3.
Thus Eq. (25) allows us to determine εb .
for the solids in the lean phase: The gas velocity in the dense phase can be determined
using the following equation used by Schoenfelder [28]:
at z = Hbz :
 
(1 − fd )cvl vl xsl,i = −fd cvd vd xsd,i + (fd cvd vd umf 1 − cvd nRZ −1
ud − vd = (26)
1 − εmf 1 − εmf
+(1 − fd )cvl vl )xsbz,i (22)
For the remaining unknowns the same amount of linear
The exchange coefficient Kdl,g is dependent on the fraction independent equations is necessary.
of the dense phase of the total cross sectional area fd , as In this model as in the great majority of gasification models
described by Schoenfelder et al. [27]. in fluidized beds [29], an empirical correlation to describe the
The exit zone was modeled as a continuous stirred tank fluid dynamics inside the reactor is used. Thus the need to
reactor. The balance for gaseous component i in the exit zone solve the momentum equations is avoided. The mean solids
is obtained as volume concentration for each height of the riser contains the
726 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736

two parts of solids volume concentration in the dense and in At the bottom (z = 0) the incoming gas flow V̇IN is dis-
the lean phase: tributed on the two phases,
c̄v = (1 − fd )cvl + fd cvd (27) z = 0 : V̇IN = (ub + (1 − εb )umf )At (35)
This mean solids volume concentration can be determined In the upper dilute zone the homogeneous and heteroge-
from axial pressure measurements and can be fitted to the neous reactions in both core and annulus regions contribute
following empirical exponential equation according to Kunii to the velocity in the lean phase, because the velocity of gas
and Levenspiel [30]: in the dense phase is assumed to be constant. The axial profile
c̄v = cv,ez + (cv,bz − cv,ez ) exp(−αcv (z − Hbz )) (28) of the gas velocity in the lean phase can be expressed by
∂ul
The solids circulation rate Gs results from the upwards (1 − fd )(1 − cvl )
flowing solids in the lean phase and the downwards flowing ∂z
  
solids in the dense phase (remember vd to be negative!).


RT  
= (1 − fd )(1 − cvl ) vi,j rlean,j 
Gs = fd cvd vd ρs xsd + (1 − fd )cvl vl ρs xsl (29) P
i j(g–g)
The solids velocity in the lean phase vl is contained in  
an approach given by Martin [31] for the settling velocity of


+ (1 − fd )cvl  vi,j rlean,j 
single particles.
i j(g–s)
 2  
1√


Re = 18 1 + Ar − 1 (30) 
9 + fd (1 − cvd ) vi,j rdense,j 
i j(g–g)
This equation is valid for 0 < Re < 105 , with the Reynolds  
and the Archimedes number defined by


+ fd cvd  vi,j rdense,j  (36)
dp (ul − vl ) i j(g–s)
Rep = (31)
vG
With the condition at the boundary to the bottom zone:
gdp3 ρs
Arp = 2 (32) ub + (1 − εb )umf |z=Hbz
vG ρ g
= fd (1 − cvd )ud + (1 − fd )(1 − cvd )ul (37)
From Eq. (30) it follows
 2
vG 1√ The gas velocity in the exit zone is
vl = ul − 18 1+ Ar − 1 (33)
dp 9
uez = fd (1 − cvd )ud + (1 − fd )(1 − cvd )ul
The axial velocity profile in the riser is determined by the   
homogeneous and heterogeneous gasification reactions. In RT 


+ cv,ez  vi,j rez,j 
the bottom zone heterogeneous reactions occur only in the P
i j(g–s)
suspension phase. Solids are consumed and gas is produced.  
As it is assumed that the suspension phase stays in minimum


fluidization state, the surplus gas contributes to the velocity + (1 − cv,ez )  vi,j rez,j  Hez (38)
in the bubbles only. Thus, we get the following differential i j(g–g)
equation for the velocity profile in the bubble phase of the
bottom zone: Not only the velocity but also the concentration of each
    component i in the gas changes because of reaction. Yan et
∂ub RT  


= εb vi,j rb,j  al. [26] pointed out the significance of a ‘net flow’. So their
∂z P calculation of the net flow is adopted in this model. The total
i j(g–g)
   net flow in the bottom zone is



+ (1 − εb )εmf   vi,j rsusp,j 


∆bz ṅ
net flow =
(1 − εb )εmf vi,j rsusp,j
i j(g–g)
   i j(g–g)



+ cv,bz   vi,j rsusp,j  (34)

i
+ cv,bz vi,j rsusp,j  (39)
j(g–s)
j(g–s)
 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736 727

And the net flow of each component i in the bottom zone can It is obvious that the parameter with the highest influence
be calculated from is the air ratio λ. This is not surprising and in agreement with
 previous literature [13,32,33]; and the chosen higher value of
c

λ = 0.6 is the upper limit for an operation condition which can
∆bz ṅ
net flow,i = 
gs,i (1 − εb )εmf vi,j rsusp,j
i cgs,i i j(g–g)
be called gasification. Vriesmann et al. [34] even stated that
 the lower heating value of gas produced at air ratios higher

than 0.45 is not very useful for combustion purposes.
+ cv,bz vi,j rsusp,j  (40) The parameter temperature shows the trend that with
j(g–s) higher temperature the heating value of the gas increases.
This can certainly be understood looking at the tar cracking
The corresponding equation for the upper dilute zone for and the other endothermal gasification reactions, which will
the total net flow is perform better at higher temperatures.
 For the feeding height, if one looks at the lower heat-




∆ud ṅnet flow = fd (1 − cvd ) vi,j rdense,j ing value of the gas, no clear trend is obvious. For high
i j(g–g)
velocity and low air ratio the heating value becomes better
 the lower down the fuel is fed into the riser. The parame-

ter gas velocity has the least influence on the product gas
+ fd cvd vi,j rdense,j  (41) composition. Therefore, neither a final statement about the
j(g–s) best feeding height nor about the optimal gas velocity can be
made.
and for the gas species i in the upper dilute zone it holds
In general, it should be stated here that the feasibility



of sewage sludge gasification in a circulating fluidized bed
c
∆ud ṅ
net flow,i = 
gs,i fd (1 − cvd ) vi,j rdense,j has been proven with these experimental findings. The lower
i cgs,i i j(g–g) heating value obtained in the experiments, and also the over-
 all efficiency of the process, fits well with the range known

for gasification of for instance wood, as these were reported
+ fd cvd vi,j rdense,j  (42) in the literature. An efficiency for the gasification process,
j(g–s)
V̇g LHVg (J/m3 )
ηeff = (43)
4. Results and discussion ṁs LHVs (J/kg)
of 58% for λ = 0.3 and 35% for λ = 0.6 was obtained. The
4.1. Screening experiments
efficiency given in the literature ranges from 46% to 63%
With screening experiments the influence of the air ratio, for biomass like barley, grass and miscanthus [35] to about
gas velocity, temperature, and the feeding height on the prod- 68–87% for wood [12,36–38].
uct gas composition and lower heating value was examined. The produced gas from the sewage sludge gasification per-
The higher and lower levels chosen for these parameters were formed in this work had on average a lower heating value of
given in Table 2. 4.7 MJ/m3 from the experiments at λ = 0.3 and 1.9 MJ/m3
In Fig. 4 all the measured results are shown. The con- for λ = 0.6. This compares well with the lower heating value
centration of the combustible components H2 , CO, CH4 and given by Kersten [12] who measured 3–5.8 MJ/m3 STP in air
C2 H4 are given as well as the concentration of carbon diox- gasification of wood (λ = 0.4–0.2).
ide and the lower heating value of the synthesis gas. All the The carbon conversion in the present study was calcu-
values refer to dry gas at standard temperature and pressure lated from the carbon detected in the gas (without tar) and
(STP). The two left columns of diagrams in Fig. 4 refer to was about 96% for the λ = 0.6 experiments, and at λ = 0.3 it
the experiments at the lower velocity (3.5 m/s), the two right was 85% on average. In the literature, a carbon conversion of
columns of diagrams show the results for the higher veloc- 97% [35,38] or even complete carbon conversion [39] is often
ity (5 m/s). For each of the velocities there is one column of given for wood and other biomass fuels. But, if the amount of
diagrams for the measurements with the higher feeding port carbon in the tar is excluded from the balance given by Ker-
(4.6 m, left column of the two), and one for the lower feeding sten [12], a conversion of 87% at λ = 0.3 is obtained, which
port (2.5 m, right column of the two). In all diagrams on the agrees with the calculated value in this work.
abscissa the temperature (750 and 850 ◦ C) is shown, and in
all diagrams the results for the two air ratios (λ = 0.3, λ = 0.6) 4.2. Axial profile measurements
are given.
On the ordinate the gas concentration and the lower heat- Axial profile measurements of the gas composition have
ing value in weight percent and kJ/m3 on a water-free basis been performed to better understand the results of the screen-
are given, respectively. ing tests. Especially the influence of the feeding height, which
728 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736

Fig. 4. Results of screening tests: influence of λ, T, utop and hfeed .

Fig. 5. Axial profile of gas composition measured at λ = 0.6, utop = 5 m/s, and hfeed = 2.5 m (H2 O calculated from O-mass balance).
 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736 729

Fig. 6. Axial profile of gas composition measured at λ = 0.6, utop = 5 m/s, and hfeed = 4.6 m (H2 O calculated from O-mass balance).

showed no uniform trend for different gas velocities, needed
more explanation.
To further examine the influence of the feeding height, in
Figs. 5 and 6 the results from axial profile measurements at
λ = 0.6 with a gas velocity at the top of 5 m/s and a feed-
ing height of 2.5 m and 4.6 m, respectively, are shown. As
measurements at λ = 0.3 were restricted to the temperature of
750 ◦ C because of ash agglomeration problems, the follow-
ing diagrams all refer to this latter temperature. The height
of the measurement position above the distributor is given on
the abscissa, and the gas concentration is on the ordinate. For
convenience an arrow points at the feeding location. In case
there were repeated measurements at one measurement port,
as for example at the position after the cyclone in Fig. 5, the
single symbols were shifted to the sides so that the repeata-
bility of the measurement is visible.
The concentrations given are all based on the raw gas state.
All gases but the water content were measured as dry gas and
were then calculated to the raw gas condition by the water
content. Because in some cases the water content had not been
measured, the H2 O-concentration used is calculated from the
oxygen mass-balance. This method was used earlier in case
a water measurement has not been carried out [40], and a
comparison to the measured values showed good agreement
in the present work.
Obviously, in the experiments with the high superficial
gas velocity, the particles entering at the upper feeding loca-
tion did not reach the bottom zone to react there. Pyrolysis
products such as hydrogen, methane and ethylene were only
measured above the feeding point (cf. Fig. 6). Narvaéz et al.
[33] found already that for a bubbling fluidized bed feeding
near the bottom is recommended for gas of good quality. Be-
cause the gas quality from the experiments with λ = 0.6 is
poor, the same axial profiles were intended to be measured
at λ = 0.3. But operation of the plant at λ = 0.3 was not easy
with the higher feeding port. With the higher velocity steady
state operation could not be held long enough for axial pro-
file measurement, because possibly many unreacted particles
were entrained from the riser and reacted further in the down-
comer, which lead to blocking. Therefore, it can be stated that
a feeding port in the upper section, even though possible, is
not advisable.
To examine the influence of the velocity, axial profiles
were measured with a superficial gas velocity of 3.5 and 5 m/s,
respectively, at λ = 0.3 with feeding at the 2.5 m position. The
results are shown in Figs. 7 and 8.
Comparing the results from the experiments with the same
feeding height but different gas velocities, it is obvious that at
the higher gas velocity the hydrogen concentration is higher
while the CO concentration remains roughly constant, and

Fig. 7. Axial profile of gas composition measured at λ = 0.3, utop = 3.5 m/s, and hfeed = 2.5 m.
730 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736

Fig. 8. Axial profile of gas composition measured at λ = 0.3, utop = 5 m/s, and hfeed = 2.5 m (H2 O calculated from O-mass balance).

therefore not only a lower feeding height but also a higher
velocity is recommended.
4.3. Pyrolysis and CO2 -gasification experiment
The measurements of the gas composition from pyroly-
sis and with a CO2 /N2 -mixture, respectively, have been con-
ducted to get information on the direct pyrolysis components,
and also to test the kinetic rate expressions taken from litera-
ture. Using the 1.5-dimensional model of the CFB, the kinetic
constants from different authors were applied and adjusted
if necessary to simulate the axial profiles measured during
the experiments. In Table 3 the average exit gas composition
from the two experiments are given, respectively.
Looking first at the results from pyrolysis, it is obvious
that carbon dioxide is a primary product of the decomposition
reaction. Because no oxygen is added to the reaction chamber,
the oxygen in the CO2 can only result from the fuel particles.
Therefore the splitting factor ξ CO is not equal to one.
What else can be seen from Table 3 is that the addition
of CO2 to the nitrogen in the fluidizing gas does not lead
to increased carbon conversion. The water gas shift reaction
is influenced, however, resulting in slightly lower hydrogen
content and increase in the water concentration, whereas a
change in the amount of carbon monoxide could not be de-
tected. The reason will certainly be the low temperature in the
experiments. At these temperatures the Boudouard reaction
does not proceed to a significant extent, as already reported
by Kersten [12]. Also the CO2 -reforming of methane does not
seem to proceed because although the methane concentration
is decreasing, the hydrogen and carbon monoxide values do
not increase. The results might be compared with the pyroly-
sis gas composition given by Schuller and Brat [41] (Table 4).
The concentrations given by the authors are on a nitrogen-free
basis, but qualitative agreement is good: The carbon dioxide
and carbon monoxide concentration detected in the gas are
nearly equal and the hydrogen content is approximately twice
that of the carbon monoxide. Only the methane concentration
obtained by Schuller and Brat is lower.
4.4. Results from the equilibrium calculation
The calculations were carried out for the composition of
the dried sewage sludge used in the experiments. The de-
volatilization products were calculated as presented above
and were taken as input concentrations. The chosen air ra-
tio for the equilibrium calculation was λ = 0.3. The resulting
equilibrium compositions were computed. In Fig. 9 the con-
centration for the main components are shown. They are given
Table 4
Pyrolysis gas composition according to Schuller and Brat [41] in volume
percent
Component vol%N-free
H2 21.8–40.9
CO 15.55–44.05
CO2 18.4–41.0
CH4 5.9–14.5

Table 3
Exit gas composition from pyrolysis and CO2 -gasification experiments
vol% raw CO2 CO H2 CH4 C2 H 4 H2 O
Pyrolysis 4.0 4.8 8.1 4.7 1.8 4.7
Fig. 9. Results from equilibrium calculations. Main components, composi-
CO2 -gasification (ψCO2 = 0.2) 16.6 4.8 6.1 3.6 1.5 5
tion in vol% at different temperatures.
 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736 731

Table 5
Kinetic rate constants valid for sewage sludge gasification
Reaction Kinetic rate expression, (mol/m3 s) kinetic constants Reference
(1 ) αC + O2 → 2(α − 1)CO + (2 − α)CO2 r(1) = k(1) cO2 f(1) [45]
f(1) = 0.05
 
k(1) = 5.957 × 102 (m/s K)Tp exp − 149,440 (J/mol) 6
 RTp dp
−3
α = 1+2f
1+fr with fr = 4.72 × 10
r
exp 37,737RT(J/mol)
p
[15]
k(2) cH2 O
(2 ) C + βH2 O → (2 − β)CO + (β − 1)CO2 + βH2 r(2) = (2) (2) (2) f(2) [16]
1+Kk H O cH2 O +Kk H cH2 +Kk CO cCO
2 2
f(2) = 2
 
(J/mol) ρchar
k(2) = 2.39 × 102 (m3 /s mol) exp − 129,000
RT MC (1 − X)
 
(2) −2 30,100 (J/mol)
Kk H2 O = 3.16 × 10 (m /mol) exp −
3
RT
 
Kk H2 O = 5.36 × 10−3 (m3 /mol) exp − 59,800RT(J/mol)
(2)
 
Kk CO = 8.25 × 10−5 (m3 /mol) exp − 96,100RT(J/mol) β = 1.2
(2)

X = 0.5
k(3) cCO2
(3 ) C + CO2 → 2CO r(3) = (3) (3) f(3) [46,47]
1+Kk CO cCO2 +Kk CO cCO
2
f(3) = 1
 
ρchar
k(3) = 4.89 × 107 (m3 /s mol) exp − 268,000
RT
(J/mol)
MC (1 − X)
= 6.60 × 10−2 (m3 /mol)
(3)
Kk CO
 
= 1.2 × 10−1 (m3 /mol) exp − 25,500RT(J/mol)
(3)
Kk CO
X = 0.35
(4 ) CH4 + 21 O2 → CO + 2H2 r(4) = k(4) cCH c f(4)
0.7 0.8
4 O2
[48]
f(4) = 100
 
0.75
k(4) = 1.58 × 1010 ((m3 ) /s mol0.75 ) exp − 202,641
RT
(J/mol)

(5 ) H2 + 21 O2 → H2 O r(5) = k(5) cO2 cH2 f(5)

f(5) = 0.001 [49]
 
k(5) = 1.08 × 1010 (m3 /mol s) exp − 125,525
RT
(J/mol)

(6 ) CO + 21 O2 → CO2 r(6) = k(6) cCO cH c f(6)

0.5 0.25
2 O O2
[48]
f(6) = 1
 
0.75
k(6) = 1.78 × 1010 ((m3 ) /s mol0.75 ) exp − 180,032
RT
(J/mol)
 
cCO cH
(7 ) CO + H2 O ↔ CO2 + H2 r(7) = k(7) cCO cH2 O − K 2 2 f(7) [50]
(7)eq

f(7) = 0.1
 
k(7) = 2.778 (m3 /mol s) exp − 12,560RT(J/mol)
 4 (J/mol)

K(7)eq = 0.022 exp 3.473×10RT
 
cCO cH
3
(8 ) CH4 + H2 O ↔ CO + 3H2 r(8) = k(8) cH2 O cCH4 − K 2 cS f(8) [51]
(8)eq

f(8) = 0.1
 
k(8) = 4.916 × 10−10 T 2 (kg m4 /s mol2 K2 ) exp − 36,150RT(J/mol) 1
MC ρchar dp
 5 (J/mol)

2
K(8)eq = 3.106 × 1014 (mol/m3 ) exp − 2.088×10 RT
(9 ) CH4 + CO2 ↔ 2CO + 2H2 Neglected (does not proceed, too slow)
(10 ) C2 H4 + O2 → 2CO + 2H2 r(10) = k(10) cC0.92 H4 cO
1.18
2
f(10) [52]
f(10) = 1
 
1.08
k(12) = 3.71 × 1012 ((m3 ) /s mol1.08 ) exp − 209,205
RT
(J/mol)

(11 ) C6 H6 + 3O2 → 6CO + 3H2 r(11) = k(11) ctar cO2

 
k(11) = 1.58 × 1012 (m3 /s mol) exp − 202,641
RT
(J/mol)
732 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736
in vol% based on the raw gas for temperatures in the range
from 800 to 1300 K.
There is a big change in composition from 800 to 900 K. At
temperatures above 1000 K the composition does not change
significantly. The main products are H2 and CO in nearly
the same amount; the H2 :CO ratio is around one. This ra-
tio stays the same for all temperatures, but from 800 to
1000 K the H2 - and CO-concentration doubles, respectively.
The CH4 - and CO2 -content at higher temperatures is aston-
ishingly low (nearly zero). The equilibrium concentration of
water is nearly unaffected by a change in the temperature
(around four volume per cent). Looking at the experimen-
tally determined composition of a gasification gas given in
the literature or measured in this work, it can be stated that
there must be strong kinetic influence that affects the com-
position because during gasification with air there are con-
siderable amounts of carbon dioxide present, and it has not
Fig. 10. Axial profiles of measured gas composition in (a) pyrolysis, (b) CO2 -gasification, and (c) air-gasification experiments and modeling results from
pseudo two-dimensional model.
been reported that the hydrogen and carbon monoxide con-
centrations calculated above were ever measured in air gasi-
fication. The same deviation between measured synthesis gas
composition and the concentrations predicted by equilibrium
calculation has been detected by Li et al. [17] and Kersten
[12].
Therefore the kinetic approach was chosen to model the re-
action network in the program. The pseudo two-dimensional
model was used to check the kinetic rate expressions taken
from the literature, whether they are also valid for sewage
sludge gasification, and whether they are applicable for gasi-
fication in circulating fluidized beds, too. To adjust the ki-
netics for some reactions of the complete reaction network
separately from the others, the measurements of the gas com-
position along the riser height during pyrolysis and CO2 /N2 -
gasification were taken, respectively. The best fit for the
splitting factor for the distribution of the oxygen-content in
 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736
the fuel to CO and CO2 was obtained for ξ CO = 0.3. With
nitrogen as the only fluidizing gas in the pyrolysis experi-
ments, the heterogeneous gasification reactions can perform
only with the steam released during drying and with the car-
bon dioxide from the devolatilization. These take part in the
water-gas shift reaction, too; and gasification reactions of the
hydrocarbons (reaction (8 ) and (9 )) might also play a role.
But especially the CO2 -gasification experiments showed that
a higher amount of carbon dioxide present in the gasifier
did not significantly alter the gas composition in comparison
to the pyrolysis experiment. This has also been detected by
Garcı̀a et al. [42] who achieved only higher conversion and
higher CO-concentration in their experiments with pine saw-
dust in a fluidized-bed gasifier at 700 ◦ C with higher amounts
of catalyst in the reactor.
As the amount of carbon dioxide strongly influences the
equilibrium of the water-gas shift reaction, it can be stated
that the water-gas shift reaction is nearly unaffected and
must therefore be far from equilibrium. Chamberland and
Labrecque [40] also found that the final composition of the
synthesis gas is not that expected from the equilibrium con-
stants but depends far more on the pyrolysis reactions. So
the assumption often made in gasification modeling that the
water-gas shift reaction reaches equilibrium is obviously
wrong. Hamel [43] also reported that equilibrium of the
water-gas-shift reaction in fluidized bed is seldom attained.
This is why, although the kinetic rate expression is formulated
as a rate equation for reversible reactions according to Franks
[44] with the equilibrium constant, the kinetic constant for the
reaction is smaller than one. A kinetic rate constant smaller
than one signifies that the attainment of the equilibrium is
slowed down.
The reactions, which have already been presented above,
are listed again in Table 5. They are given together with the
kinetic rate expressions, which are valid for sewage sludge
gasification.
As has been discussed already, the carbon dioxide reform-
ing reaction does not proceed to a significant extent and was
therefore omitted. For the partial combustion of the tar com-
pound (e.g. benzene) a rate expression of second order with
a kinetic rate constant similar to the one for the methane-
oxidation was used (see reaction (11 ) in Table 5).
In Table 5 the reactions (10 ) and (11 ) are the partial com-
bustion of ethylene and tar, respectively.
C2 H4 + O2 → 2CO + 2H2 (10’)
C6 H6 + 3O2 → 6CO + 3H2 (11’)
For the adjustment of the oxidation reaction kinetics, dif-
ferent measurements of axial gas composition profiles were
available. In Fig. 10 the measured axial profiles from the
pyrolysis, CO2 -gasification and one of the air-gasification
experiments are shown, together with the modeling results.
For the air-gasification experiment simulation, the measure-
ment at λ = 0.3 with a superficial gas velocity at the top of
utop = 3.5 m/s at the temperature of T = 750 ◦ C was chosen,
733
where the feed was supplied at hfeed = 2.5 m above the dis-
tributor plate. Agreement of the measured gas composition
with the calculation results from the pseudo two-dimensional
model is good. The best fit was obtained for the splitting fac-
tor for the amount of ethylene with ξC2 H4 = 0.1, and for the
one for the tar amount with ξ tar = 0.005. With this tar coeffi-
cient a benzene concentration of 1460 mg/m3 was calculated
for the λ = 0.3 case.
5. Conclusions
Combustion, pyrolysis and gasification of sewage sludge
in the circulating fluidized bed were examined by both, ex-
perimental and modeling studies.
In order to obtain information about the optimal operation
parameters, several gasification experiments were performed
with dried sewage sludge (>90% dry matter) in a pilot-scale
circulating fluidized bed. The experimental program was sub-
divided into screening tests, axial gas composition measure-
ments, and additional pyrolysis as well as CO2 -gasification
experiments. The program for the screening tests was de-
veloped based on statistical methods and was conducted to
determine the influence of the temperature, air ratio, feeding
height, and superficial gas velocity. Axial profile measure-
ments were performed to better understand the processes in-
side the riser; different gasification gases than air were used
to learn about the devolatilization and reforming reactions
and kinetics.
From the experimental part, the following conclusions can
be drawn:
• The excess air ratio has the most significant influence on
the produced gas composition. A value of λ = 0.3 is a good
choice for the operation of a gasifier for sewage sludge.
• Temperature has the second most important influence. At
higher temperatures a more valuable gas is produced. But
the choice of temperature in sewage sludge gasification
is limited due to the risk of melting, agglomeration and
sintering of the sewage sludge ash.
• Although no clear trend is obvious for the optimal feed-
ing height, for good gas quality a feeding port close to the
bottom of the riser is recommended, because mixing of
the fuel particles is better there. Feeding at higher loca-
tions leads to particle entrainment and incomplete carbon
conversion.
• With near-bottom feeding, high velocities are attainable
and therefore a high fuel throughput can be achieved.
• The extension of the combustion zone at the bottom of the
riser is small.
• In pyrolysis, in spite of the lack of oxygen in the surround-
ing gas, not only carbon monoxide is produced, but also
carbon dioxide is a primary product of the devolatilization
reaction.
• CO2 -gasification reactions do not proceed to a significant
extent at the low temperatures necessary to prevent ash
sintering.
734 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736

• The water-gas shift reaction does not reach equilibrium. k reaction rate constant (m3 /(kg s))
Considering the diameter of 0.1 m and its height of 15 m kcvl parameter for the calculation of the cv -profile
the reactor can be described as one-dimensional. A 1.5- (kcvl = 0.65)
dimensional model was developed, which contains the fluid- Kbs mass transfer coefficient between bubble and sus-
dynamic characteristics of the circulating fluidized bed with pension phase in the bottom zone (1/s)
gas and solids upflow in the center and downflow at the wall. Kdl mass transfer coefficient between dense and lean
A complete reaction network for pyrolysis, combustion and phase in the upper dilute zone (1/s)
gasification was formulated. Most kinetic rate expressions Kk adsorption constant according to Reed (1981)
were taken from the literature. Three open parameters are re- (1/atm)
lated to the devolatilization process, namely the splitting fac- K, Kp , Keq equilibrium constant ((various units))
tor ξ CO which describes the part of the oxygen in the volatile LHV lower heating value (J/m3 , J/kg)
matter which is released in the form of CO, the splitting fac- ṁ mass flow (kg/s)
tor ξC2 H4 for the fraction of carbon in the volatiles which is ṁ mass flow based on an area (kg/(m2 s))
released as C2 H4 and the splitting factor ξ tar for the carbon ṁ mass flow based on a volume (kg/(m3 s))
fraction which is released as tar (and which is balanced as M molar mass (kg/mol)
C6 H6 ), respectively. Since the composition of pyrolysis gas n molar amount (mol)
is strongly dependent on the heating rate of the fuel particles n local cell number in the pseudo two-dimensional
these latter parameters must be determined under fluidized- model
bed conditions. Numerical values of ξ CO , ξC2 H4 and ξ tar were ṅ molar flow (mol/s)
therefore obtained by fitting the model calculations to three nRZ Richardson–Zaki exponent (nRZ = 3)
sets of measured axial profiles of the species O2 , CO2 , CO, ṅ molar net flow (convection because of reaction)
H2 , CH4 , C2 H4 and H2 O which were taken under conditions (mol/(m3 s))
of pyrolysis, CO2 -gasification and air-gasification, respec- P system pressure (Pa)
tively. The model is seen to give a good description of the Pe Peclet number
reactor behavior under any of these conditions. In particular, r reaction rate (mol/(m3 s))
under air gasification conditions the model is seen to give a R ideal gas constant (J/(mol K))
good description of the combustion zone near the bottom of Re Reynolds number
the riser. The thus determined reaction kinetics can be used t time (s)
for simulation calculations of fluidized-bed gasifiers with dif- T temperature (K)
ferent geometries [53]. ub volumetric gas flow in the bubble phase divided by
the cross-sectional area of the reactor
ud interstitial gas velocity in dense phase (upper dilute
Appendix A. Nomenclature zone) (m/s)
uez superficial gas velocity in the exit zone (m/s)
ul interstitial gas velocity in lean phase (upper dilute
Ar Archimedes number zone) (m/s)
At cross-sectional area of reactor (m2 ) umf minimum fluidizing velocity (superficial) (m/s)
c concentration (mol/m3 , kg/m3 ) v velocity of solids (m/s)
cS char or carbon concentration in kinetic rate expres- vi mole fraction of component i in volatiles) (i = C, H,
sion (kg/m3 ) O, S, N) (mol/mol)
cv solids volume concentration V̇ volume flow (m3 /s)
c̄v average solids volume concentration w water (kg, mol)
dp particle diameter (m, mm, ␮m) x mass fraction (kg/kg)
D dispersion coefficient (m2 /s) x3,50 particle diameter of fifty percent mass fraction (mm,
fd volume fraction of the dense phase ␮m)
ferf Gaussian error function X carbon conversion
f(No.) fitting factor for the reaction specified z coordinate in axial direction (m)
gf,i0 standard Gibbs free energy of formation for compo-
nent i (J/mol) Greek letters
G Gibbs free enthalpy (J/mol) α splitting factor for the reaction of carbon and O2
Gs solids circulation rate (kg/(m2 s)) αcv coefficient for the fitting of the c̄v (m−1 )
h height in one zone (m) β splitting factor for the reaction of carbon and H2 O
h0R heat of reaction (J/mol) ε void fraction
H height of one zone (m) η dynamic viscosity (Pas)
HHV higher heating value (J/m3 , J/kg) ηeff efficiency
i, j counting variables λ air ratio
 I. Petersen, J. Werther / Chemical Engineering and Processing 44 (2005) 717–736 735

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