DOI: 10.1002/ente.

201300009

Gasification of Low-Grade Coal in a Dual Fluidized-Bed

Steam Gasifier
Stefan Kern,* Christoph Pfeifer, and Hermann Hofbauer[a]
The gasification of a bituminous coal was performed in
a dual fluidized-bed (DFB) steam gasifier at a fuel power of
90 kWth. The main aim of these tests was to prove the suitability of the DFB system for cheap low-grade coals that are
often delivered with a wide range of particle sizes and ash
loads. The fine fraction in particular can become entrained in
the gas stream and thus be responsible for changes in the

system performance and gas quality. The selected gasifier

bed material was olivine, with an applied particle size of
375 mm, the steam-to-carbon ratio was 1.3 kgH2O kgC1, and
the gasification temperature was 850 8C. In addition to standard online analysis of the main components of the product
gas, impurities that included NH3, H2S, and tar were also examined.

Introduction
In addition to renewable fuels, such as biomass, and their
thermal utilization,[1] coal will continue to play a major role
in the global primary energy mix to satisfy increasing energy
demands; in contrast, the contribution of oil will decrease
after peak oil is reached. Huge amounts of coal are currently
available; the reserves that can be mined at low cost were
calculated in 2007 to be sufficient to last for at least another
148 years.[2] Although coal-based gasification processes for
power generation have not been proven to have an economic
advantage in comparison to combustion power plants that
use coal or other fossil fuels, the investment costs for integrated gasification and combined cycle (IGCC) power plants
are much higher, and power generation by coal gasification
retains certain advantages. For instance, the electrical efficiency is greater[3] and if the process is combined with carbon
capture and storage (CCS) the costs are lower in terms of
both initial investment and operation.[2] For the gasification
of coal, commercially available reactor designs include entrained-flow, moving-bed, and fluidized-bed gasifiers. In contrast to biomass gasification, for which fluidized-bed reactors
are used in most industrial-sized plants, for coal gasification,
the most commonly employed reactor design is currently the
entrained-flow reactor.[4] This type of reactor offers the benefits of a gas that is free of condensable hydrocarbons (tars)
as a result of its operation at very high temperatures (1200
1600 8C) and it is also able to operate with liquid fuels. In addition, as a result of the high temperatures and fine fuel particles, the carbon conversion to gas is nearly complete in
a single stage. The most significant disadvantages of these reactors are that the fuel has to be ready to be ground to
a small particle size (which is not possible for some fuel
types) and that pure O2 is required to drive the process autothermally, which means that the heat for gasification is provided by partial oxidation in the gasifier. To maintain a nitrogen-free product gas, steam or CO2 can be used as a gasification agent. The advantage of using steam instead of CO2 is
Energy Technol. 2013, 1, 253 264

that the reactivity of steam is on average approximately four

times higher than that of CO2,[5] therefore, residence times of
the char in the gasification section are shorter and the gasification efficiency is higher. As the use of steam or CO2 as
a gasification agent results in an allothermal process, the
heat required for endothermic gasification reactions has to
be provided externally. As a solution to the problem of of introducing such heat externally on an industrial scale, dual
fluidized-bed (DFB) gasification technologies can be utilized,
which separate the combustion zone (which provides the
energy for gasification) from the gasification zone, and pure
steam is used as the gasification agent. By circulating the bed
material between these two reactors, the heat from the combustion reactor is carried to the gasification reactor. As with
single-stage fluidized-bed reactors, this two-stage process
needs to be operated at temperatures below the ash-softening temperature of the fuels. As a result, the highest temperature that can be reached by fluidized-bed gasification is approximately 1000 8C. DFB steam gasifiers usually operate at
gasification temperatures in the range of 800900 8C. The
lower gasification temperatures employed during fluidizedbed gasification with respect to entrained-flow gasification
lead to lower carbon conversions[6] and residual char is often
left behind in a single-stage reactor. As a consequence,
highly reactive coal with a comparably high content of volatile components, such as lignite, is favored.[4] Through the use
of a separate combustion reactor, the residual char can be
used to provide the heat for gasification as it is applied in
the DFB gasifier.
[a] S. Kern, Dr. C. Pfeifer, Prof. Dr. H. Hofbauer
Vienna University of Technology
Institute of Chemical Engineering
Getreidemarkt 9/166, 1060 Vienna (Austria)
Fax: (+ 43) 1 58801 16699
E-mail: stefan.kern@tuwien.ac.at
st.kern@aon.at

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253

S. Kern et al.
Another approach to coal gasification is the production of
valuable products (e.g., FischerTropsch fuels, syngas, methanol) from cheap, low-quality coal. Coals with very high ash
contents are usually considered undesirable as an increase in
fuel ash leads to a decrease in gasification and combustion
efficiency because as the heat in the ash cannot be fully recovered. Furthermore, a high ash content can lead to fouling
and increase the amount of waste for disposal.[4] Nevertheless, if the ash content is not high enough to cause the abovementioned problems, ash can actually be beneficial for the
process if it contains catalytically active matter. Although alkaline metals often cause problems with ash melting, they
are also suitable to catalyze gasification and reforming reactions. In this regard, the following order of activity has been
determined:
K2CO3 >
Na2CO3 > trona
[Na3(CO3)(HCO3)2 H2O] > borax (Na2B4O710 H2O).[7] Calcium has
been identified to play a major role in the promotion of
watergas-shift reactions if present as CaO. Clemens et al.
found that for gasification with steam, the Ca content of coal
ash both promotes the watergas-shift equilibrium and influences the composition of the product gas.[8] This effect is produced if the gasification products remain in the vicinity of
the char surface, which indicates that improved gaschar contact promotes the catalytic activity. In their comparison of
CaO and MgO for the steam reforming of biomass tars, Delgado et al. determined an activity series in which dolomite
was the most active material followed by magnesite and calcite.[9] CaO is, in addition to MgO, one of the major components of dolomite, a cheap and disposable catalyst commonly
used as an in-bed, catalytically active additive that contains
SiO2, Fe2O3, and Al2O3 as trace minerals.[10] Low-quality
coals are also often characterized by high sulfur contents,
which is significant given that sulfur compounds must be removed from the product gas in the majority of cases. The primary form of sulfur in the product gas is H2S,[11] although
minor concentrations of COS are also found. CS2 is generally
a product of secondary reactions of COS and H2S, but only
to a negligible extent as these reactions occur above 850 8C.
As a result, CS2 formation is only a matter of interest in entrained-flow gasification, in which these high temperatures
are observed, and not in fluidized-bed gasification.[12]
To examine the potential for the DFB gasification of highash coals, a coal with an ash content of 31 wt %db was used
for gasification with steam at a fuel power of 90 kWth. In addition to its chemical properties, the fuel particle size has
a significant influence on the process performance, in particular the emission of char and dust in the product gas as well
as the formation of tar and the watergas-shift equilibrium.
This is significant as the particle size of low-quality coals
often varies considerably on delivery, and a high coal-dust
content can lead to the entrainment of particles in the gas
produced by a fluidized-bed gasifier. To assess the influence
of fine particles, two gasification tests were performed under
the same process conditions but with different particle size
distributions.

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Gasification of solid feedstock with steam

For the gasification of a solid carbonaceous feedstock with
pure steam, the influence of the amount of steam present in
the reactor is essential for system performance and product
gas quality.[13] Therefore, it is mandatory to maintain the
same amount of steam for the gasification of solid carbon for
all operating points. For gasification with pure steam, the
overall gasification reaction can be expressed as:

y
Cx Hy xH2 O ! xCO x H2
2

DH R, 850 > 0
Equation (1) reveals that for each mole of carbon in the
feedstock, one mole of water is required for stoichiometric
fuel conversion. However in reality, the main elements of
a feedstock include carbon, hydrogen, and oxygen. Inclusion
of this in the overall steam gasification reaction results in
Equation (2):


y
Cx Hy Oz x  zH2 O ! xCO x  z H2
2

for x > z; DH R, 850 > 0

Based on Equation (2), theoretically, the stoichiometric
demand of steam is equal to xz if complete conversion of
the solid fuel (CxHyOz) is assumed. By using the equations
above, it can be estimated that a different amount of steam
present in the system can push the reaction towards the
products or reactants. Therefore, the amount of steam introduced into the gasification reactor is referred to as the introduced amount of fuel or the introduced amount of carbon by
the solid fuel. These ratios are the steam-to-fuel ratio (fSF)
[Eq. (3)] and the steam-to-carbon ratio (fSC) [Eq. (4)].
fSF;wt

fSC;wt

_ steam vH2 O m
_ fuel
m


_ fuel
1  vH2 O  vash m
_ steam vH2 O m
_ fuel
m
_ fuel
vC m

Equation (4) can be employed to determine the minimum

amount of steam that has to be present during the process
for a known fuel composition. Equation (5) can then be used
to calculate the stoichiometric steam demand fH2O :
H2 O x  z

In the tests performed here, the feedstock can be expressed as the system CxHyOz, which is free of sulfur and nitrogen. From the fuel analysis (Table 1), the molarities of C,
H, and O were determined as CH0.73O0.12 and fH2O as
60.04 molH2O kgdaf, N, S, Cl-free1 (1.08 kgH2O kgdaf, N, S, Cl-free1).
In most cases of gasifier operation, the actual amount of
steam in the system differs from that which is stoichiometrically required. To quantify the ratio of steam present to that

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Gasification of Coal in a Dual Fluidized-Bed Steam Gasifier

Results and Discussion

Table 1. Proximate and ultimate analysis of the feedstock.

Content
Component

Dry basis

As used

Water content [wt %]

Ash content [wt %]
C [wt %]
H [wt %]
N [wt %]
O [wt %]
S [wt %]
Cl [wt %]
Volatile matter [wt %]
Fixed carbon [wt %]
LHV [MJ kg1]

31.09
55.13
3.39
1.39
8.18
0.78
0.04
27.16
72.84
21.00

3.6
29.97
53.15
3.27
1.34
7.88
0.75
0.04
26.18
70.22
20.15

Overview
Coal gasification was performed at two operating points
(OP1, OP2), the general parameters of which are summarized in Table 2. OP1 and OP2 differed only in the fuel particle size distribution, and the other process parameters, such

Table 2. Key parameters of the gasification tests.

Value
Fuel size [mm] (coal)

which is theoretically needed, an equivalent ratio for steam

can be defined as that used for air combustion systems
(lH2O).
lH2 O

_ H2 O;actual
m
_ H2 O;stoich:
m

As an estimate of the potential of a fuel to form the main

product-gas components, the dependence of the calculated[14]
equilibrium compositions on temperature is shown in
Figure 1. This graph illustrates a system CxHyOz+fH2O H2O,
in which, according to fuel analysis, the molarities of the
feedstock (C, H, and O) are used as reactants together with
the stoichiometric amount of water required for the conversion to gas. The thermodynamic equilibrium composition is
calculated by minimization of the Gibbs free energy.[15]
By comparing the stoichiometric equilibrium values
(Figure 1) at 850 8C with the measured values presented later
(Figure 3), it can be estimated that a thermodynamic equilibrium will likely not be reached in the gasification reactor as
the residence time is too low at the relatively low temperatures used for coal gasification. Therefore, the product-gas
composition in entrained-flow gasifiers is closer to the thermodynamic equilibrium.

Gasification temperature [8C] (bubbling bed)

Mean temperature combustion reactor [8C]
Fuel power [kW] (coal)
Fuel mass flow [kg h1] (coal)
fSC [kgH2O kgcarbon1]
fSF [kgH2O kgfuel, daf1]
Initial bed material inventory [kg]

OP1: 0.38
OP2: 1.58
848  2
897  2
90
16.2
1.30
1.05
100

as gasification temperature, bed material particle size, and

fSC, were kept constant. To provide the required heat for
gasification at approximately 850 8C, the combustion reactor
was operated at a temperature slightly below 900 8C in both
cases. For OP1 the gasifier was operated with the fuel as delivered (only pieces larger than 10 mm were sieved out to
avoid loop-seal blockage), whereas for OP2 the fine fraction
was reduced by sieving. The two tests were performed separately, which means that both OPs had to go through the
start-up period of the system until the operating conditions
were reached. These steady-state operating conditions were
kept constant for at least 6 h to collect sufficient data for
mass and energy balances as well as to accomplish the discontinuous sampling methods. For both OP1 and OP2, the
fuel was introduced into the gasifier by using hopper 1, with
the coal introduced directly into the bubbling bed at medium
height by using a screw conveyor. The particle size distributions of the two coal size fractions are listed in Table 3. An
impression of the behavior of coal gasification by using the
DFB system can be achieved by highlighting the temperatures in the gasifier at the different operating points as well
as the fluidization conditions in the system. An overview of
the fluidization regime is presented in Table 4. The velocities
Umf, Ut, and their ratios to the actual superficial velocity in
the gasification and combustion reactors were used to characterize the fluidized-bed system. The process conditions
presented in Table 4 and the fuel particle size distribution

Table 3. Coal particle size distribution.

Figure 1. Calculated equilibrium product gas composition of the system

CxHyOz+fH2O H2O for the used coal (corresponding to fuel analysis in
Table 1).

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Value

OP1

OP2

dp10 [mm]
dp50 [mm]
dp90 [mm]

280
2600
7700

1400
4990
7860

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S. Kern et al.

Table 4. Fluidization conditions in the DFB system.

Value

OP1

OP2

Umf [m s1]
Ut [m s1]
Ug [m s1]
Ug/Umf
Ug/Ut
Uc [m s1]
Uc/Umf
Uc/Ut

0.07
3.36
0.40
5.51
0.12
9.42
130.79
2.80

0.07
3.36
0.41
5.64
0.12
9.23
128.19
2.74

produced where the superheated steam for fluidization is introduced into the bubbling bed because the steam temperature, which is approximately 300 8C, is significantly lower
than that of the bed material. However, as a result of the effective intermixing of the steam, bed material, and fuel particles as well as the high heat capacity of the bed material, the
temperature loss is limited. The set point for the gasification
temperature (850 8C) was chosen at the height of the middle
of the bubbling bed, which is where the fuel was also fed. In
the middle and upper sections of the freeboard, the temperature decreases steadily because of heat losses and energyconsuming reactions as well as the pyrolysis and gasification
of any entrained fine fuel particles in the freeboard. By comparing the two OPs, we can see that the temperature profile
exhibits a greater decrease if finer particles are present in
the freeboard. At the gasifier outlet situated at the end of
the freeboard, the temperature difference between the two
OPs is approximately 10 8C. This discrepancy is caused by
the higher amount of fine coal particles in the freeboard for
OP1 that are heated, release their volatile components, and
are partly gasified. A closer analysis of Figure 2 reveals that
the major difference in temperature between the two OPs
occurs in the splash zone and the lower freeboard section;
therefore, we can assume that the fast pyrolysis reactions
take place here, whereas the relatively slow char gasification
takes place above. Such behavior has already been documented in this field.[16] There is a demand for additional fuel
for the combustion reactor. For OP1, with fine particles in
the fuel, the demand for additional fuel for the combustion
reactor is higher than that for OP2. Consequently, the temperature of the recycled bed material differs slightly and
causes a deviation in the reference point of the bubbling bed
by 4 8C.

listed in Table 3 illustrate the problem caused by the presence of fine particles in a fluidized-bed reactor. The gasification of the fuel particles should take place in the bubbling
olivine bed, but to maintain the fluidization regime for a bubbling bed, a minimum fluidization velocity is required. In the
case presented here, coal gasification was accompanied by
a superficial velocity in the gasifier Ug of approximately
0.4 m s1.
At this fluidization velocity, the terminal velocity Ut of the
olivine particles is far from a value that results in their elutriation into the product gas, even for smaller particle sizes
(dp10). For the fuel particles, however, the situation is different, as the density of the coal is lower and the particle size is
widely distributed. This is particularly true of the fuel used in
OP1, in which some of these particles are entrained in the
product gas flow. The critical size for coal in the applied
gasification atmosphere is approximately 160 mm, and coal
particles that are smaller than this are elutriated immediately
after feeding into the gasifier. For the coal size distribution
used in OP1, for which the fine particles were not sieved out,
approximately 6.8 wt % of the fuel particles were smaller
than 160 mm. In the case of OP2, for which most of the fine
fraction was removed, only 2.0 wt % of the initial mass left
Product gas composition
the bubbling bed to enter the gas phase immediately. How
these particles, which are generally neither completely devoThe DFB gasification process yields two separate gas
latilized nor gasified, affect the temperature profile and gas
streams, a product-gas stream (gasification reactor) and
quality will be discussed below.
The temperature profile in the
gasification reactor is presented
in Figure 2. This diagram illustrates that the temperature
varies with the height of the reactor (relative to the surface of
the bubbling bed) and between
the two OPs as a result of several factors. The hot bed material, which transports the heat
from the combustion reactor to
the gasification reactor, is recycled back to the gasification reactor through the lower freeboard section. This produces
a local hot spot at which the
highest temperature in the reactor is recorded. A cold spot is Figure 2. Temperature profiles during gasification in the gasification reactor.

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Gasification of Coal in a Dual Fluidized-Bed Steam Gasifier

a conventional flue-gas stream (combustion reactor). The
product gas primarily consists of H2, CO, CO2, CH4, C2H4,
C2H6, and unconverted H2O. The remaining gas components
are made up by the following components or impurities:
*

*
*

A N2 content of < 1.5 vol %db is typically present in the

product gas as N2 is used as an inert gas in the fuel-feeding system.
Gaseous C2C5 hydrocarbons that are not detected by the
measurement devices employed.
H2S derived from sulfur in the fuel.
NH3 derived from nitrogen in the fuel.

The main gas components of the product gas are displayed

in Figure 3. The H2 content varied very little between the
two tests: 54.2 vol %db for OP1 and 53.2 vol %db for OP2. The
CO content was 17.9 vol %db for the test that included more
fine particles (OP1) and 19.3 vol %db for OP2. The CO2 content was not affected by particle size, with concentrations of
approximately 15.5 vol %db measured in both cases. An increased amount of fine particles resulted in slightly higher
CH4 and C2H4 levels (OP1).

Figure 3. Product gas composition of the performed tests.

Product-gas pollutants in the form of entrained dust and

char were also detected (Figure 4). The dust comprised a mixture of fuel ash and dust produced by the attrition of the bed
material. As coal particles smaller than 160 mm were entrained to the product gas straight after fuel feeding, the concentration of particulate matter was significantly higher for
OP1 than OP2. Considering the high fuel-ash content found
during the initial fuel analysis (Table 1), it is not surprising
that such an amount of inorganic dust should also be present
in the entrained coal particles. The amount of dust (inorganic
particulate matter) was nearly three times that of char (organic particulate matter) because levels of char were reduced
in the freeboard as a result of partial gasification and
carbon-consuming reactions, such as watergas reactions, the
Boudouard reaction, and methanation. The effect of solidcarbon reduction in the freeboard of a bubbling fluidizedbed gasifier has been described for wood gasification by
Miccio et al.[17]
Energy Technol. 2013, 1, 253 264

Figure 4. Entrained dust and char in the product gas.

The levels of H2S and NH3 were measured for OP1. The
mean value found for H2S was 5130 ppmv, whereas NH3 was
detected in an amount of 7514 ppmv in the product gas.
These impurities are derived from the sulfur and nitrogen
content of the coal. In the reducing atmosphere of a gasification reactor, the majority of nitrogen introduced in the fuel
is released in the product gas as NH3, whereas only a minor
amount is converted to HCN.[18] In a DFB steam gasifier, nitrogen is released predominantly in the gasification reactor
into the product gas, whereas the flue gas is nearly free of
any fuel-bound nitrogen components.[19, 20] Khan[21] determined that about 31 % of sulfur in coal is transferred in the
gaseous products (H2S + COS) after coal pyrolysis, and 19 %
of the total gas H2S content has to be accounted for COS
compounds in the gas.[21] In previous investigations on DFB
gasifiers, the release of H2S in the product gas has been calculated to be between 50 and 90 % of the introduced amount
of sulfur, with the remainder leaving the system as SO2 in
the combustion reactor or captured in the ash.[19, 20] As the
fuel composition did not differ in the present study between
the two OPs, and the release of H2S and NH3 in the product
gas is mostly defined by the fuel sulfur and nitrogen content,
it can be assumed that similar values of both impurities
would be found for OP2.
The detection of condensable hydrocarbons (tar) is
a matter of particular interest in fluidized-bed gasification.
Tar was sampled several times for each OP, and the mean
values of gravimetrically- and GCMS-detectable tar found
are displayed in Figure 5. This reveals the influence on tar
productionof the coal and char particle content of the atmosphere inside the gasifier. Although the gasification of coal
with a low content of fine particles (OP2) resulted in only
2.4 g Nm3db1 of gravimetrically detectable tar and
4.5 g Nm3db1 of GCMS-detectable tar components, the inclusion of the fines fraction (OP1) increased these values to
6.3 g Nm3db1 of gravimetrically detectable tar and
8.1 g Nm3db1 of GCMS-detectable tar. This finding matches
the results of other investigations that have examined biomass. In their analysis of the steam gasification of a mixture
of sawdust and pellets, Wilk and Hofbauer found approximately twice as much GCMS- and gravimetrically detectable tar than that in the gasification of 100 % pellets.[22] The

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S. Kern et al.

Table 5. Relative contribution of tar components to GCMS tar.

Figure 5. Amounts of detected tar in the product gas.

authors argued that the main reason for this difference was
that approximately 9 % of the mixed fuel, mainly sawdust,
was transported immediately out of the fluidized bed with
the fluidization steam. As a result, pyrolysis and gasification
took place in the freeboard section of the gasifier, in which
the interaction of the pyrolysis products with the hot, catalytically active bed material was absent. This process ultimately
led to a significant reduction in tar decomposition. Another
common interpretation of the higher tar content of fine particles is that they provide less resistance for the devolatilizing
gases; in larger particles the pyrolysis gas has to pass a layer
of char, and thus secondary catalytic tar cracking reactions
can take place.[23] Table 5 summarizes the relative contribution of each tar compound in the GCMS-detectable tar. As
the origin of the feedstock used in both OP scenarios was
the same, the actual composition of the GCMS-detectable
tar did not differ much when small fuel particles were entrained in the freeboard. Nevertheless, a tendency towards
classes of tar produced by devolatilization can be imagined
for OP1, as evidenced by the lower contribution of naphthalene, a tar component that is mostly a product of secondary
and tertiary tar reactions.
The high ash content of the coal makes it necessary to consider its effect on the system. The applied (wet) fuel feeding
rate of 16.2 kg h1 corresponds to the introduction of
4.86 kg h1 of ash into the gasifier. According to the measurements of dust concentration in the product gas (Figure 4),
the product gas stream, and the total ash in the product gas
and flue gas streams, the balance of the ash is closed. Figures 6 and 7 show the mass flow [kg h1] for inorganic matter
that enters and leaves the gasification reactor, respectively.
The most important issue to consider is that the entrained
particles also include a large amount of inorganic matter. As
larger coal particles also likely contain larger (sand/gravel)
ash particles, it is not surprising that a total of 3.8 kg h1 of
ash left the DFB system through the product and flue-gas
streams for OP1, whereas for OP2 only 1.52 kg h1 of ash
was observed. In addition, as the mean ash particle size increased after fuel sieving, the terminal velocity Ut of most of
the ash particles was increased above the superficial gas velocity Ug in the gasification reactor. Only the fraction that
was sufficiently small was able to escape the system. Hence,

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Component

OP1

OP2

Naphthalene [wt %]
Acenaphthylene [wt %]
Indene [wt %]
Anthracene [wt %]
Fluoranthene [wt %]
Fluorene [wt %]
Phenanthrene [wt %]
Dibenzofuran [wt %]
Pyrene [wt %]
4,5-Methylphenanthrene [wt %]
Carbazole [wt %]
2-Methylnaphthalene [wt %]
Benzo[a]anthracene [wt %]
1-Benzothiophene [wt %]
Chrysen [wt %]
Quinoline [wt %]
Biphenyl [wt %]
Styrene [wt %]
Diethyl phthalate [wt %]
1-Methylnapthalene [wt %]
Benzo[a]pyrene [wt %]
Benzo[b]flouranthene [wt %]
Benzo[k]flouranthene [wt %]
Isoquinoline [wt %]
Phenol [wt %]
Phenylacetylene [wt %]
Benzofuran [wt %]
Acenaphthene [wt %]
Benzo[g, h, i]perylene [wt %]
Indole [wt %]
Others [wt %]

29.62
13.07
7.77
8.58
6.46
4.30
3.92
3.84
3.35
1.94
1.68
1.54
1.49
1.47
1.40
1.46
1.00
0.91
0.89
0.79
0.75
0.71
0.55
0.49
0.45
0.39
0.33
0.31
0.29
0.27
0.0

31.35
13.22
7.04
8.59
5.90
3.78
3.38
3.91
2.87
1.63
1.71
1.49
1.39
1.36
1.37
1.30
1.19
0.82
0.94
0.66
0.76
0.85
0.70
0.51
0.65
0.35
0.32
0.34
0.73
0.28
0.6

Figure 6. Ash balance for OP1 [kg h1].

Figure 7. Ash balance for OP2 [kg h1].

for OP1 only 1.25 kg h1 of ash accumulated in the system,

whereas for OP2 3.53 kg h1 was unable to leave the fluidized
bed as no ash-removal device was available at the pilot

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Gasification of Coal in a Dual Fluidized-Bed Steam Gasifier

plant. However, the operation of the DFB pilot plant was
not jeopardized by accumulating ash as the system was in operation for less than 8 h with coal as a feedstock. Nevertheless, a slight pressure increase in the bubbling bed was recorded for OP2, which demonstrates the increased amount
of inorganic matter in the system. For operations on an industrial scale, an ash-removal system would be required as
the large amount of fuel ash can easily lead to bed-material
agglomeration if species that lower the ash-melting temperature exceed a critical concentration level. Therefore the compositions of the fuel ash and the ash collected from the gas
streams that exit the reactor were detected by X-ray fluorescence (XRF) analysis. A benefit of fuel ash is its potential
for catalytic activity. The main components in the fuel ash
were Si, Al, and Fe with minor amounts of Ca, K, P, Ti, and
Mg (Table 6). Although fuel ash can play a significant role in
increasing the catalytic activity, no enhancement was observed in this study in terms of tar reduction. This suggests
that the large quantities of Si and Al measured here were
not highly catalytically active. In contrast, the minor components of K, Mg, and Ca are known to be active catalysts, although the extent of this activity depends on their compounds. In this study, it is probable that most of these alkali
metals were present as silicates and thus not very active. The
mass flow rates of the measured elements into and out of the
reactor in the fuel and as particles in gas are summarized in
Table 7. The higher output of Mg compared to its input
likely reflects attrition of the bed material.

Table 6. XRF analysis of coal and fly ash.

Component

Coal

Fly ash

SiO2 [wt %]
Al2O3 [wt %]
Fe2O3 [wt %]
K2O [wt %]
CaO [wt %]
MgO [wt %]
TiO2 [wt %]
V2O5 [wt %]
Cr2O3 [wt %]
MnO [wt %]
Na2O [wt %]
NiO [wt %]
ZnO [wt %]
Others [wt %]

55.617
21.392
10.977
3.086
3.402
1.111
1.330
0.153
0.159
0.158
0.375
0.122
0.147
1.971

51.908
22.066
13.368
2.930
2.270
3.948
1.126
0.136
0.170
0.133
0.253
0.224
0.186
1.283

Table 7. Mass flow rates of ash components.

Component
1

SiO2 [g h ]
Al2O3 [g h1]
Fe2O3 [g h1]
K2O [g h1]
CaO [g h1]
MgO [g h1]
TiO2 [g h1]
V2O5 [g h1]
Cr2O3 [g h1]
MnO [g h1]
Na2O [g h1]
NiO [g h1]
ZnO [g h1]
Others [g h1]
Sum [kg h1]

Product gas yield and conversion performance

This section focuses on the conversion of the reactants required for the gasification process, carbon and water, as well
as system performance. Table 8
summarizes the key data from
the gasification tests. The prodTable 8. Key data for the tests performed.
uct-gas yield was greater in the
Value
test without fine coal particles
Total
product gas yield [Nm3 h1]
(OP2) than that in OP1, which
O
content
of product gas [vol %]
H
2
likely reflects the longer mean
Product gas yield [Nm3db h1]
residence time of the fuel fracSpecific product gas yield [Nm3db kgfuel, daf1]
tion in the gasifier and would
Lower heating value [Mn Nm3db1]
Syngas
powerexcl. tar [kW]
lead to an increased carbon
[%]
h
CPP
conversion in the gasification
hC;IP [%]
reactor. The operation of
Water conversion, XH O, rel [kgH O kgfuel, daf1]
a DFB gasifier is characterized
Water conversion, XH O, rel [kgH O kgfuel, daf, N, S, Cl-free1]
Stoichiometric steam demand [kgH O kgfuel, daf, N, S, Cl-free1]
by the carbon conversion that
Stoichiometric
steam demand [molH O kgfuel, daf, N, S, Cl-free1]
takes place only in the gasificalH O [kgH O kgH O1]
tion reactor itself and the
Carbon conversion in the gasification reactor, XC, G [%]
carbon conversion that occurs
Overall carbon conversion of the DFB system, XC, DFB [%]
Specific tar content, GCMS [g kgfuel, daf1]
in the whole system (gasificaSpecific tar content, gravimetric [g kgfuel, daf1]
tion reactor and combustion reSpecific tar content, GCMS [g kgcarbon1]
actor together) through to the
Specific tar content, gravimetric [g kgcarbon1]
formation of product gas and
Tar intensity per kWh of syngas, GCMS [g kWhproduct gas1]
Tar intensity per kWh of syngas, gravimetric [g kWhproduct gas1]
flue gas. In the gasification retF [s]
actor, the carbon conversion
tC [s]
can be defined as the ratio of
2

Energy Technol. 2013, 1, 253 264

 2013 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Input feedstock

Output

2808.66
1080.28
554.34
155.83
171.82
56.11
67.17
7.71
8.03
7.99
18.96
6.15
7.40
99.55
5.05

789.00
335.40
203.19
44.53
34.50
60.00
17.12
2.07
2.58
2.02
3.85
3.40
2.83
19.50
1.52

OP1

OP2

27.34
57.03
12.82
1.19
11.59
41.28
44.00
51.80
0.45
0.47
1.10
61.16
0.42
36.41
93.13
9.66
7.50
12.07
9.38
2.51
1.95
4.1
0.8

28.80
51.39
14.47
1.34
11.78
47.34
50.72
59.77
0.50
0.51
1.10
61.16
0.47
41.28
96.04
5.99
3.18
7.49
3.98
1.37
0.73
4.1
0.8

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259

S. Kern et al.
carbon in the product gas stream that exits the gasification
reactor to the amount of carbon introduced in the solid fuel
[Eq. (7)]. In contrast, the carbon conversion that occurs in
the whole system includes the ratio of carbon that exits the
DFB system in both the product (gasification reactor) and
flue-gas streams (combustion reactor) to that introduced in
the solid fuel [Eq. (8)].
XC;G

_ C;PG
m
_ fuel
vC m

XC;DFB

_ C;PG m
_ C;FG
m
_ fuel
vC m

transported with the bed material from the gasification reactor to the combustion reactor. Nevertheless, there was a significant difference in the additional fuel demand for the combustion reactor observed for the two OPs. As shown in
Figure 8, there was more fuel required for OP1 to provide
the heat for the gasification reactor. This was already estimated by the temperature trend shown in Figure 2, which indicated that the temperature of the bed material was lower if
it moved from the gasification reactor to the combustion reactor during OP1.

The higher water content of the product gas in OP1 than

that of OP2 is another indicator that the gasification agent,
steam, did not react as effectively with carbon particles in
OP1. The amount of introduced water consumed or converted during the gasification and steam-reforming reactions can
be considered as an indicator for the whole process. Relative
water conversion is thus defined as the amount of water consumed per mass unit of converted fuel [Eq. (9)].
XH2 O;rel

_ H2 O;conv:
m


_ fuel
1  vH2 O  vash m

9
Figure 8. Additional fuel required for the combustion reactor.

According to this equation, the relative water conversion

of OP2 was greater than that of OP1 (Table 8), which suggests that the residence time of the fine particles present in
the freeboard at OP1 (tF) was too short for them to react
sufficiently with the steam. However, the values for the relative water conversion are relatively high in both cases compared to the gasification of biomass, in which relative water
conversions of approximately 0.15 kgH2O kgfuel, db1 are usually
reached[24] and for which the DFB system was originally designed. The source of these significantly increased values for
coal can be explained by two main reasons. In general, the
stoichiometric water demand of the coal used in this study is
approximately four times higher than that of wood pellets,
which makes it clear that gasification reactions that consume
steam dominate over the devolatilization process. The
second reason is that the amount of consumed water corresponds to the dry and ash-free fuel. As the input mass flow
rates for coal are lower than those of wood at the correct
fuel power and the ash content here was very high, the total
amount of dry and ash-free fuel was significantly lower. The
effect on the water conversion rate by the addition of coal to
a wood-gasification process in the same system has been
documented in detail for the cogasification of wood with
coal.[25]
The temperature of the gasification reactor during standard gasification operation is usually controlled by the
amount of additional fuel added to the combustion reactor.
Compared to the gasification of biomass, which contains less
fixed carbon than the fuel used here, the demand for additional fuel for OP1 and OP2 is relatively low. This is because
of the high amount of char in the bed that is consequently

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An evaluation of the efficiency of the gasification system

was performed by determining the cold gas efficiency. The
calculation of this value takes into account that pilot plants
usually do not reach the low ratio of heat losses seen in industrial plants. In the case of the present DFB pilot plant,
heat losses amounted to nearly 20 % of the fuel input.
Stidl[26] calculated the heat losses that occur through radiation for the main components of the 10 MWth DFB gasification plant in Oberwart, Austria.[27] Based on this data, the radiation heat loss for a typical industrial plant can be assumed
to be 2 % of the input fuel power. The cold gas efficiency
data can be effectively used to calculate the parameters for
an industrial-scale plant [Eq. (10)]. In contrast to this, the
cold gas efficiency for the pilot plant can be expressed as
shown in Equation (11), which neglects heat losses.
hC;IP

v_ PG LHVPG


_ PP Q
_ IP  3600
Pfuel;G Pfuel;C  Q

10

hC;PP

v_ PG LHVPG


Pfuel;G Pfuel;C  3600

11

Conclusion
DFB gasification is a fuel-flexible technology capable of the
conversion of carbonaceous feedstock into high-quality product gas. Even low-grade coal fuel can be successfully used as
a feedstock, despite both its low reaction rate at typically applied gasification temperatures (800900 8C) and its difficulty
of handling because of its very high ash content and wide

 2013 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Energy Technol. 2013, 1, 253 264

Gasification of Coal in a Dual Fluidized-Bed Steam Gasifier

particle size distribution. Reasonable product-gas quality and
energetic performance parameters were obtained. In reality,
the main obstacle encountered in using this fuel was not its
ash content, and the reduced process performance was instead caused by the low activity of the coal with the gasification agent, which led to less-efficient carbon and water conversion. In addition, if a large amount of fine particles are
present in the fuel, a high level of dust and entrained char is
produced as the fine particles are entrained in the gas phase
immediately after the fuel is fed into the gasifier. In this
study, the inclusion of fine fuel particles reduced the carbon
conversion rate further because of the production of ungasified carbon.
In its current configuration, the system is limited with
regard to large fractions of fine material in the feedstock.
However, a new design has been proposed[28, 29] that will
enable the conversion of fine material in contact with the
hot, catalytically active bed material. The tests presented
here have generally shown that the DFB-gasification process
is suitable even for materials with a low conversion rate and
high ash content.

Experimental Section

Figure 10. Scheme of the DFB gasification pilot plant at VUT.

The DFB pilot plant at the Vienna University of Technology

and, after particle separation from the flue gas at the exit of the
combustion reactor, it flows back to the gasifier through the
upper loop seal.

For experiments performed on a pilot scale, the Vienna University of Technology operates a 100 kW DFB-gasification reactor.
The basic principle of the DFB-gasification process is shown in
Figure 9, and a schematic drawing of the pilot rig is shown in
Figure 10. The system physically separates gasification and combustion, with two fluidized-bed reactors connected by loop seals.
The fuel, typically biomass but coal in this study, enters the
gasification reactor, a bubbling bed fluidized with steam, in
which drying, pyrolysis, and heterogeneous char gasification take
place. The residual char leaves at the base of the gasification reactor together with the bed material, which circulates between
the two reactors through the lower loop seal and into the combustion reactor. This reactor is implemented as a fast bed fluidized with air to maintain combustion of the residual char and additional fuel, if required. By burning char and additional fuel (if
required) in the combustion reactor, the bed material is heated

The pilot plant is equipped with three different hoppers to

enable fuel feeding at different positions into the gasification reactor and to enable the possibility of cogasification of two or
more pure substances at any mixing ratio. During the experiments performed in this study, only hopper 1 was used to introduce the fuel into the bubbling bed. A more detailed description
of the pilot plant, including the geometrical data, can be found
in Refs. [13, 15, 24]. For safety reasons, the hopper system is
flushed with N2. For standard gasification operation with a single
hopper used to feed the fuel, a volumetric flow rate of 0.1 m3 h1
of N2 was used.

Analyses
Product gas measurement
The compositions of product and flue gases were measured after
their exit from the reactors, of which the main gas components
CH4, H2, CO, CO2, and O2 were analyzed by using a Rosemount
NGA 2000 multicomponent gas analyzer, and N2, C2H4, and
C2H6 were analyzed by using an online GC (PerkinElmer Clarus
500). The detailed arrangement of the measurement system is explained in Ref. [16].

Tar, H2O, and entrained particulate matter measurement

Figure 9. Basic principle of the DFB gasification process.

Energy Technol. 2013, 1, 253 264

Tar was sampled isokinetically by using impinger bottles and analyzed gravimetrically by using GCMS. Tar sampling was applied discontinuously by condensing and dissolving the tar components. The measurement method was based on the tar protocol
according to CEN/TS 15439,[30] which concerns tars that originate
from biomass gasification. The method applied differed in that

 2013 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

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261

S. Kern et al.
toluene was employed as a solvent, whereas CEN/TS 15439 suggested the use of isopropanol (IPA). The use of toluene allowed
the simultaneous detection of the product-gas water content,
which could be measured as a separate phase in the impinger
bottles. However, this meant that tar components with a boiling
point lower than that of toluene, such as benzene, toluene, and
xylene (BTX), could not be detected, although the separation
performance for tar components larger than BTX is higher for
toluene than using IPA. A schematic of the arrangement of the
tar-sampling line is shown in Figure 11.

Analysis of inorganic components

The detection of the bed-material and fuel-inorganic-matter
(ash) compositions was performed by XRF analysis by using
a PANalytical Axios Advanced analyzer. This method is based
on the emission of characteristic fluorescent X-rays from a material excited by bombardment with high-energy X-rays or gamma
rays. Samples to be analyzed were melted at 1050 8C by using
a Merck Spectromelt and dumped at 400 8C on a stainless-steel
plate. Analysis was performed under vacuum by using a Rh
anode, an excitation voltage of
50 kV, and a tube current of
50 mA. The components were
calculated as oxides.

Bed material
Olivine is a naturally occurring
mineral composed of silicate tetrahedra that also contains Fe and
Mg in the form (Mg1xFex)SiO2,
although the content of these two
Figure 11. Sampling line for tar, water, and entrained particulate matter (char and dust).
elements varies with mining location. The catalytic-tar-reduction
effect caused by the use of olivine as a bed material has been
The gas entered the heated sampling line, which consisted of cyreported by Koppatz et al.,[13] and precalcination of the olivine
clone-filled and glass-wool-stuffed filter cartridges, in which dust
can considerably improve the catalytic activity.[31, 32] In this study,
and condensed tar components were deposited. Afterwards, the
the olivine used in the tests was provided by Magnolithe GmbH.
gas was led through six impinger bottles, five of which were
The results of the XRF analysis as well as the mechanical properfilled with toluene. The impinger bottles were located in a cooling
ties of the olivine bed material are shown in Table 9. As a result
bath maintained at 8 8C by using a cryostat and the tars and
of its hardness, high heat capacity, and high catalytic activity for
steam condensed there. The liquid phases in the impinger bottles
steam reforming, olivine is considered ideal for fluidized-bed apwere unified, and the aqueous phase was separated from the tolplications. A material particle size of dp50 = 375 mm was selected,
uene phase. The amount of water in the impinge bottle was dewhich corresponds to particle group B according to Geldart.[33] A
termined to calculate the water content in the gas stream. The
graph of the bed material size distribution is shown in Figure 12.
amount of toluene was also noted, and a sample was withdrawn
for GCMS analysis. The main part of the toluene was evaporated from the sample in a petri dish. To analyze the oil in the filter
Feedstock
cartridge, it was necessary to perform a Soxhlet extraction with
IPA. Again a sample of the IPA phase was withdrawn for GC
The coal used in the gasification tests was mined in Puertollano,
MS analysis. The IPA phase was handled in the same way as the
Spain. As a result of its characteristically high ash content, the
toluene phase. The toluene phase and the IPA phase were combined, which gave the amount of gravimetric tar in the product
gas. The filter cartridge was reduced to ashes by oxidizing the orTable 9. Chemical composition and mechanical properties of the used oliganic matter in a furnace. By weighing the cartridge before and
vine.
after the muffle-furnace treatment, the amount of entrained char
and dust was calculated. Finally, the GCMS samples were anaComposition and properties
lyzed to determine the tar composition. This measurement
0.43
Na2O [wt %]
method gave the gravimetric tar content, GCMS tar content,
MgO [wt %]
46.76
GCMS tar composition, water content, char load, and dust load
0.40
Al2O3 [wt %]
(inorganic matter).
39.84
SiO2 [wt %]

NH3 and H2S measurement

To measure the amounts of NH3 and H2S, the gas was sampled in
a similar way to that described above for tar, that is, by using impinger bottles, although in this case the solvents employed were
dilute H2SO4 for NH3 and an aqueous KOH solution for H2S.
The sampling lines (impinger bottles) were operated at 2 8C in
a glycol/ethanol mixture cooled by using a cryostatic temperature
regulator.

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P2O5 [wt %]
SO3 [wt %]
K2O [wt %]
CaO [wt %]
Cr2O3 [wt %]
MnO [wt %]
Fe2O3 [wt %]
NiO [wt %]
Cl [wt %]
Others [wt %]
Hardness [Mohs]
Particle density [kg m3]

 2013 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

0.03
0.06
0.32
0.90
0.28
0.15
10.32
0.31
0.10
0.11
67
2850

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Gasification of Coal in a Dual Fluidized-Bed Steam Gasifier

V_ PG [NM3db h1]

Volumetric flow rate of product gas

(dry)
XH2 O;rel [kgH2O kgfuel, daf1] Water conversion in the gasifier, related to the fuel input
XC,G [%]
Carbon conversion in the gasification reactor
XC,DFB [%]
Overall carbon conversion of the
DFB system
x [mol kgC, H, O1]
Molarity of carbon in the fuel (dry,
ash-, N-, Cl-, and S-free basis)
y [mol kgC, H, O1]
Molarity of hydrogen in the fuel
(dry, ash-, N-, Cl-, and S-free basis)
z [mol kgC, H, O1]
Molarity of oxygen in the fuel (dry,
ash-, N-, Cl-, and S-free basis)

Figure 12. Size distribution of the olivine bed material.

calorific value of the coal was low. The results of proximate and
ultimate analysis of the coal are summarized in Table 1.

Symbols
dp10 [mm]
dp50 [mm]
dp90 [mm]
DHR, 850 [kJ mol1]
LHVPG [MJ Nm3db1]
_ H2 0;actual [kg h1]
m
_ H2 0;stoich: [kg h1]
m
_ steam [kg h1]
m
_ fuel [kg h1]
m
_ H2 0;con: [kg h1]
m
_ C;PG [kg h1]
m
_ C;FG [kg h1]
m
Pfuel;G [kW]
Pfuel;C [kW]
_ PP [kW]
Q
_ IP [kW]
Q
T [8C or K]
Umf [m s1]
Ut [m s1]
Ug, Uc [m s1]

Particle size with mass fraction

< 10 %
Mean particle size
Particle size with mass fraction
> 90 %
Heat of reaction at 850 8C
Lower heating value of the product
gas (dry)
Actual mass flux of steam in the
gasification reactor
Actual mass flux of steam in the
gasification reactor
Mass flux of steam in the gasification reactor
Mass flux of solid fuel into the
gasification reactor
Amount of water that is converted
to product gas
Carbon flux in product gas stream
Carbon flux in flue gas stream
Input fuel power of solid fuel into
gasification reactor
Input fuel power of fuel for combustion reactor
Heat loss of the pilot plant
Heat loss of an industrial size plant
Temperature
Minimum fluidization velocity
Terminal velocity for a single particle
Superficial gas velocity in gasification reactor (g) and combustion reactor (c)

Energy Technol. 2013, 1, 253 264

Greek letters
H2 O [molH2O kgdaf, N,S,Cl-free1 or kgH2O kgdaf, N, S, Cl-free1]
Stoichiometric H2O demand
hC;IP
Cold gas efficiency calculated for an industrial plant
with the same fuel power as the pilot plant
hCPP
Cold gas efficiency of the pilot plant
fSF;wt [kgH2O kgfuel, daf1]
Steam-to-fuel ratio
fSC;wt [kgH2O kgC1]
Steam-to-carbon ratio
lH2 O [mol mol1], [kg kg1]
Stoichiometric H2O ratio
Product gas residence time in the bubbling bed
tB [s]
tF [s]
Product gas residence time in the freeboard of the
gasification reactor
tC [s]
Gas residence time in the combustion reactor
vi
Mass fraction in the fuel
Ash mass fraction in the fuel
vash
Carbon mass fraction in the fuel
vC
Water mass fraction in the fuel
vH2 O

Abbreviations and subscripts

BTX
c
daf
db
DFB
g
IP
IPA
OP
PAH
PP
PG
VUT

Benzene, toluene, xylene

Cold gas (efficiency), combustion reactor
Dry and ash free basis
Dry basis
Dual fluidized bed
Gasification reactor
Industrial plant
Isopropanol
Operating point
Polycyclic aromatic hydrocarbons
Pilot plant
Product gas
Vienna University of Technology

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263

S. Kern et al.

Acknowledgements
The authors gratefully acknowledge the financial support provided by the European Commission as this study was performed within the framework of the Fecundus project, funded
by the Research Fund for Coal and Steel of the European
Union (Contract No. RFCR-CT-2010-00009).
Keywords: ash industrial chemistry carbon combustion
energy conversion
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Received: January 17, 2013
Revised: February 18, 2013
Published online on April 5, 2013

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