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University of Seville, Chemical and Environmental Engineering Department, ETSI, Camino de los descubrimientos sn, Seville 41092, Spain
Chalmers University of Technology, Department of Energy and Environment, Gteborg S-412 96, Sweden
a r t i c l e i n f o
a b s t r a c t
Article history:
Received 5 June 2011
Accepted 13 December 2011
Available online 22 December 2011
Methods to increase the conversion of char and tar in uidized bed gasiers (FBG) are discussed, with the
focus on small to medium-size biomass/waste gasiers for power production (from 0.5 to 10 MWe).
Optimization of such systems aims at (i) maximizing energy utilization of the fuel (maximizing char
conversion), (ii) minimizing secondary treatment of the gas (by avoiding complex tar cleaning), and
(iii) application in small biomass-to-electricity gasication plants. The efciency of various measures to
increase tar and char conversion within a gasication reactor (primary methods) is discussed. The optimization of FBG by using in-bed catalysts, by addition of steam and enriched air as gasication agent, and
by secondary-air injection, although improving the process, is shown to be insufcient to attain the gas
purity required for burning the gas in an engine to produce electricity. Staged gasication is identied as
the only method capable of reaching the targets mentioned above with reasonable simplicity and cost, so it
is ideal for power production. A promising new stage gasication process is presented. It is based on three
stages: FB devolatilization, non-catalytic air/steam reforming of the gas coming from the devolatilizer, and
chemical ltering of the gas and gasication of the char in a moving bed supplied with the char generated
in the devolatilizer. Design considerations and comparison with one-stage FBG are discussed.
2011 Elsevier Ltd. All rights reserved.
Keywords:
Gasication
Fluidized bed
Char
Tar
Biomass
Optimization
1. Introduction
Gasication is a thermo-chemical route for conversion of solid
fuel into gas used in a variety of applications [1,2]. Gasication in
uidized bed (FB) has several advantages over that in xed/moving
bed or entrained-ow [3]. FB provides high mixing and reaction
rates, accommodates variation in fuel quality, and allows scaling-up
of the process, making it ideal for processing of biomass and waste.
Various concepts have been developed for gasication in FB.
Stand-alone, air-blown, bubbling FB gasication (FBG) is a simple,
directly heated design, but it delivers a gas diluted by nitrogen,
having low heating value (4e6 MJ/Nm3) and high tar content
(10e40 g/Nm3). Medium heating-value gas (10e15 MJ/Nm3) can be
produced by directly heated gasiers using mixtures of oxygen and
steam in one single reactor [4], or by indirectly heated gasiers
using air and steam in a dual FB reactor [5]. In all types of FBG the
tar concentration in the gas is high, since the process temperature is
kept relatively low to prevent agglomeration and sintering of bed
material [1e3]. The low temperature also results in incomplete
1454
Lower
Higher
Tar content
Lower
Lower
Char conversion
Sintering
Decreasing risk
700 C
800 C
Agro
fuels
Higher
Increasing risk
900 C
Refused Woody
derived biomass
fuel
1000 C
Coal
the unconverted char: the energy in the tar contained in a gas with
a concentration of 20 gtar/Nm3drygas (taking a heating value 35 MJ/
kgtar) represents less than 1% of the energy in the fuel. Therefore,
the energy in the unconverted char constitutes the most signicant
energy loss that can be recovered in an improved gasier. The
fraction of the char converted has been assumed constant in this
example, but, of course, this value depends on char reactivity,
gasication temperature and reaction time. The latter depends on
the entrainment and mixing of the char in the bed, both related to
gas velocity and char size. The interaction of all these variables is
discussed below.
The need for tar conversion depends on the use of the gas. For
distributed power production by gasication, the most convenient
option is to burn the gas in a gas engine, and this requires tar
reduction. The acceptable limit for tar is usually expressed on the
basis of species concentration, being in the range of 50e100 mg/Nm3.
However, it has been demonstrated that the dew point of the gas is
a more appropriate parameter for engine application: a dew point
below 30 C is recommended. Gas containing 100 mg/Nm3 tar with
a dew point above 70 C has been found to cause engine problems
[1]. Conversely, gas with a tar concentration above 5000 mg/Nm3
having a dew point of 20 C has been used in engines without
technical problems. This shows that the nature of the tar, and not
the tar concentration, is the key parameter for assessment of the
suitability of a gas for engine application.
Apart from tar, the gas from gasication of biomass and waste
contains other contaminants, such as alkaline metals, nitrogen,
chlorine and sulfur compounds, as well as dust. These compounds
can be removed by conventional equipment downstream of the
gasier if it is done before the gas condenses. Conversion of the tar
is preferred, since it increases the heating value of the gas.
2.2. Fundamentals of tar and char conversion in FBG
The fundamentals of char and tar conversion in a FBG have been
dealt with in detail elsewhere [3,13]. Here we only summarize the
main aspects to understand the methods to be described below.
The rate of devolatilization and the yields of primary char, tar, and
light gases vary mainly with the temperature and the heating rate at
which the fuel is transformed. General trends of devolatilization
have been published, where the yields of char, light gas, and tar as
a function of the temperature at various heating rates and particle
sizes are presented for a variety of biomass materials [14]. At the
lowest temperatures (<300 C) char is the main product. At middlerange temperatures (450e550 C) a maximum is observed for
liquids (condensable tar compounds). Further increase of temperature leads to higher production of gas at the expense of tar, while the
proportion of char remains roughly constant. Thermal decomposition of mm-sized particles in a FBG is referred to as primary pyrolysis, occurring in the lower range of temperature during the heating
up of a particle (300e500 C). Thereafter, at bed temperature in
a single-stage FBG (800e900 C), when most volatile matter has
been released, secondary conversion takes place, characterized by
the oxidation and reforming of gas and tar in the gasier. The
conversion of the char also takes place by gasication with CO2 and
steam, since O2 is rapidly consumed by the gas.
The conversion of char and tar is related to the effective time of
reaction with gas and catalysts, which in turn depends on the
residence time of fuel and char particles in the bed and on the local
mixing conditions [15]. Of particular importance is the contact
between char and tar with oxygen and steam and the position
where the fuel particle is devolatilized. Formation of bubbles,
bypassing of gas, entrainment of material and other factors inuence the reaction time [3,15]. The key operation parameter in a FB is
the supercial gas velocity and the properties of the fuel particle
1455
Fig. 2. Effect of temperature and char residence time on char conversion in a FBG.
Calculated by modeling based on data from Ref. [3].
1456
70%
65%
60%
55%
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
Steam / SBR
fuel ratio
Fig. 4. Optimization of an autothermal FBG by steam and enriched air as uidization
agent. Adapted from Ref. [20].
Fig. 5. (a) Conceptual diagram of staging of the gasication process by injection of secondary air. (b) Experimental temperature prole measured in a demonstration FBG with
secondary-air injection. Data taken from internal reports mentioned in Ref. [17].
compounds was achieved, but the total tar concentration was still
high (a few grams per Nm3), and the proportion of stable aromatic
tar compounds in the gas increased signicantly. Staging of the
gasication agent, oxygen and steam, despite being potentially
interesting, has not been reported. In any case, it seems that a more
distinct division of zones in the gasier is necessary to achieve the
tar reduction required. This makes it necessary to leave the
conventional design, as we will show in the new process introduced in Section 4.
3.4. Catalysts
An in-bed catalyst has a great inuence on the cracking and/or
reforming reactions [6,9e11]. Enhancement of local gas and solids
mixing is necessary for the efciency of the catalyst. Typical in-bed
catalysts are calcined limestone, dolomite, and olivine sand and,
less frequently, Ni-based or other metallic catalysts. The use of
cheap catalysts, such as natural mineral (dolomite, olivine, etc.)
reduces tar concentrations down to 0.5 g/Nm3. Fig. 6 shows the
dew point of the exit gas from a pilot FBG for 6 runs where two
types of catalyst were tested for different operating conditions
(equivalence ratios, ER). It is shown that the dew point is above
170 C, without signicant reduction between the tests. In spite of
this high dew point, the total tar concentration in the gas was
reduced by a factor of 5, from about 16 g/Nm3 down to 3 g/Nm3
[21]. This result points out that small amounts of heavy tar
contribute signicantly to the dew point of the gas, and this will
cause problems in applications where the gas has to be cooled to
the ambient temperature, so this method has to be complemented
by secondary treatment.
More effective catalysts, such as those based on nickel, improve
tar reduction in the bed, but their rapid degradation makes this
option less suitable. Ni-based catalysts are preferred in downstream vessels, but deactivation is still a problem to be solved [12].
Carbonaceous materials like activated carbon also have been found
to have catalytic activity for tar reduction [12,25e28]. Char generated in the process acts as a catalyst enhanced by the alkali and
alkaline earth-metals remaining in its structure, especially potassium in the form of carbonates, hydroxides or oxides, which affects
steam reforming of the nascent tar [26,27]. During the conversion
process, char undergoes signicant transformation, while it is
gasied by steam. Polymerization of PAH compounds in the char at
temperatures above 700 C [28] lowers the rate of char gasication
with steam, whereas below 600 C the char acts as a tar lter
reducing signicantly the tar concentration without being gasied.
To give a rough idea on the effectiveness of distinct catalysts,
experimental ndings [25] are illustrated in Fig. 7, taking
180
Alumina
175
170
0.2
Lime
0.25
0.3
0.35
Naphthalene
conversion (%)
185
1457
100
100
94.4
99.6
73.7
80
55
60
61
60.3
40
20
0
0.4
ER=fed O2 / stoichiometric O2
Fig. 6. The effect on the tar dew point of the gas of various catalysts used in-bed in
a FBG. Adapted from Ref. [21].
Fig. 7. Effect of various catalysts on naphthalene conversion at 900 C and 0.3 s residence time of the gas. Adapted from Abu El-Rub et al. [25].
1458
Biomass
Pyrolysis unit
Gasification unit
Heat
Pyrolysis gas,
tar and char
Steam+
Air
Char bed
HT Steam
Rapid devolatilization
at low T
High yield of tar
Gas seal
Solid
transport
Fuel
Char gasification
Catalytic tar reforming
Particle filtering
Gas quenching
Gas out
Air
Steam
Air
Steam
Solids out
Fig. 9. Basis for the conceptual development of the FLETGAS process with indication of
the essential steps occurring in various parts of the system.
1459
sd adb
sbed Ab Hr=F1 Yvol
where d is the initial equivalent diameter of a fuel particle and Yvol
the fraction of volatiles released from the particle, r is the bed
density, and a and b are empirical coefcients found in literature for
different fuels. (1 Yvol) is the solid, non-devolatilized part of the
fuel, i.e. the char, mainly made of ash and carbon. Specic data for
the fuel of reference (dried sewage sludge) can be found in Refs.
[42] and [43].
The bed height H is given by sd > nsbed, namely, the devolatilization time should be greater than a certain multiple n, to be
determined by experiments, of the average residence time of the
solid part of the fuel in the bed. Already here, we note a complication because the residual solid may be quite variable for different
fuels. For instance, sewage sludge, having a high content of ashes
(around 50% on dry basis), could be compared with wood, containing less than 1% of ash: the amount of solids, and hence, the
residence time, is smaller for sludge than for biomass. Another
consideration to be taken into account is the amount of inert
material for different fuels: whereas a high proportion of inert
material forms the bed during conversion of wood, minor amounts
are needed for dried sewage sludge, whose ash/char particles can
be properly uidized. The system is dimensioned for a reference
fuel, and it will have to be adjusted by changing process conditions
to some extent, corresponding to the properties of another fuel, to
perform in a satisfactory way.
1460
The fuel can be fed onto the beds surface. Devolatilizing fuel
particles are known to oat on the surface of the bed, and the bed is
not as well mixed as assumed for simplicity above. Since the
devolatilizing fuel particles move rapidly to the top of the bed in
any case, even if they are introduced at the bottom, it is an
advantage to design for fuel feed onto the surface of the bed,
removing potential problems involved in feeding against a counter
pressure (such as at the bottom of the bed). When the devolatilization is complete, the fuel particles (the char) are no longer lifted
by the released volatile gases but circulate in the entire bed. An
internal vertical division in the bed (not shown in Fig.10) establishes the required solids circulation pattern in the system.
4.4.2. The reformer
The gas ows out of the bed and enters the reformer located
downstream with a temperature of 700e750 C. As has been
pointed out before, the fresh tar compounds are reactive and the tar
is drastically reduced in the reformer, where a gas temperature of
up to 1200 C is created by partial combustion of air. The injection
of steam into the reformer avoids coking and polymerization of tar.
The steam temperature, about 450 C, is attained by heat exchange
with the hot outlet product gas, reproducing the behavior of an
industrial autothermal gasier. The optimum conditions to reform
different tars can be found by dedicated experiments, such as those
described in Ref. [44] and references therein. Conversion of the
various tar compounds under different operating conditions using
a variety of kinetic data of tar cracking and reforming has been
investigated also by modeling [3,45].
4.4.3. The moving bed: tar reforming and char gasication in the
third stage
The solids (char and ash) are transferred from the devolatilizer
to the moving, packed bed, composed of char and ashes, which
descend in the nal step of the equipment located in the shaft that
follows the gas reforming step. The reformer gas passes this bed
and transfers its heat to the bed. This bed acts as a catalytic lter,
promoting tar decomposition reactions with simultaneous steam
gasication, the latter cooling down gas and bed (chemical quench)
by the endothermic char gasication reaction with steam. Hence,
this bed is a combined heat and mass exchanger, whose number of
transfer units (length, at a given temperature difference) determines its performance [45]. The length of the moving bed is
determined by the maximum of the following two values: (i) that
enabling complete conversion of the tar, and (ii) that for complete
conversion of char. The kinetics used for the design of the pilot
plant are specied elsewhere [45]. The cross section is selected by
considering the share between excessive pressure drop in the xed
bed and to have proper distribution of gas and solid in the bed.
Finally, the ashes exit the bed containing very little carbon in the
case of a successful design, and likewise, the gas has a negligible
concentration of tar after passing the two reduction steps. The low
temperature of the gas and solids streams leaving the system
contributes to attain a product gas with higher chemical energy
and, therefore, increases the gasication efciency of the system.
VALVE
NONCATALYTIC
REFORMER
Fuel
DEVOLATILIZER
Steam +
Enriched Air
LOOP-SEAL
CHAR
CONVERTER
Fuel
gas
Ash
Steam +
Enriched Air
Steam +
Enriched Air
GAS
SOLID
Fig. 10. Diagram of the performance of the FLETGAS process with indication of solid
and gas ows (with arrows).
One stage
Produced
Gas
1461
Three stages
T max = 1200 C
Air
T = 750 C
T = 820 C
T = 660 C
Tin = 1120 C
Fuel
Fuel
Tout = 880 C
Air
Steam
Air
Produced
gas
Air
Solids out
Fig. 11. Comparison between a single-stage FBG and a three-stage FBG system (FLETGAS) for sewage sludge gasication (maximum temperature set at the bed 820 C).
5. Conclusions
Measures to optimize fuel conversion have been discussed in
order to achieve high tar and char conversion in FBG for biomass
and waste. Treatment of tarry gas downstream of the gasier is
complex and expensive for power production in small and
medium-size gasication plants, so methods to improve tar
conversion within the gasier (primary methods) are preferred for
such plants. The optimization of conventional FBG by primary
methods such as in-bed catalysts, addition of steam and enriched
air, and secondary-air injection, although improving the process, is
shown to be insufcient to attain the gas purity required for
burning the gas in an engine to produce electricity. Staged gasication creates zones in the gasier, which promote high conversion
of char and tar and, therefore, it is an effective way to conduct
gasication. Various developments for small-scale gasication have
been proposed over the last decade based on xed bed, but none of
them has still reached commercial status. A new three-stage
gasier (FLETGAS), based on a uidized bed design, has been
a
Ab
b
d
ECN
ER
F
FB
FBG
H
HPAH
LAH
LPAH
PAH
Yvol
r
sd
sbed
coefcient (e)
cross section of the bed (m2)
coefcient (e)
equivalent diameter of fuel particle (m)
Energy Research Centre of the Netherlands
equivalence ratio (e)
fuel feed rate (kg/s)
uidized bed
uidized bed gasier
height (m)
heavy PAH
light aromatic hydrocarbon
light PAH
polycyclic aromatic hydrocarbon
mass fraction of volatiles in the fuel (e)
density of bed (kg/m3)
devolatilization time (s)
mean residence time of fuel in the bed (s)
1462
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