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Article history:
Received 21 January 2011
Received in revised form 18 October 2011
Accepted 25 October 2011
Available online 8 November 2011
Keywords:
Biomass
High temperature
Steam addition
Soot
Entrained ow gasication
a b s t r a c t
Biomass (wood and straw) gasication has been studied in a laboratory scale atmospheric pressure
entrained ow reactor. Effects of reaction temperature, steam/carbon molar ratio, excess air ratio, and
biomass type on the solid, liquid and gas products were investigated. The biomass was completely converted at all investigated operating conditions and the syngas contained nearly no tar but some soot at
the highest applied reaction temperature of 1350 C. With a rise of reaction temperature from 1000 C
to 1350 C, the yield of producer gas (dened as the sum of H2, CO, CO2 and hydrocarbons up to C3 species) increased dramatically by 72%. The H2/CO molar ratio in syngas was close to 1 at reaction temperature above 1200 C with steam addition. Higher temperature was benecial to lower the amount of tar
while the soot yield showed a peak of 56.7 g/kg fuel at 1200 C. With steam addition, the producer gas
yield and in particular the H2 yield increased gradually, while the CO yield decreased slowly. The molar
ratio of H2/CO was equal to 1 with the largest supplied amount of steam addition (H2O/C = 1). Steam addition gave an obvious reduction in the soot yield, but it was not possible to completely avoid soot. Increasing excess air ratio from 0.25 to 0.50 gave no signicant change in the producer gas yield, but the yields of
H2, CO, and soot decreased, the CO2 yield increased, and the molar ratio of H2/CO decreased. Moreover,
wood and straw gasication provided similar product compositions. At 1350 C and with steam addition,
the syngas composition is close to equilibrium as veried by calculation.
2011 Elsevier Ltd. All rights reserved.
1. Introduction
Biofuels play an important role in helping to address some global challenges, such as energy supply security, and environment
and climate protection [16]. Governments, particularly those in
the OECD (Organization for Economic Cooperation and Development) are striving to become less dependent on imported oil and
are seeking diversied sources of energy supply. Biofuels can contribute to a more secure and diverse energy supply [5,6]. Furthermore, biofuels are CO2 neutral because the growth of new plants
will absorb CO2 through photosynthesis even though the production and consumption of biofuels emit CO2 as well. Therefore, utilization of biofuels can reduce dependence on imported oil, reduce
CO2 emission, and provide a growing market for the farming
community.
Gasication is a thermochemical process currently available for
biofuel production, and converts solid carbonaceous materials to a
synthesis gas, a mixture rich in H2, CO, CO2, and CH4, by partial
oxidation at elevated temperature [7,8]. The syngas produced by
gasication can be used to synthesize liquid fuels and chemicals or
to produce power in a combined cycle plant. However, some
challenges of the gasication technology still exist, such as the
Corresponding author. Tel.: +45 45 25 28 41; fax: +45 45 88 22 58.
E-mail address: aj@kt.dtu.dk (A.D. Jensen).
0016-2361/$ - see front matter 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.fuel.2011.10.063
590
Table 1
Ultimate and proximate analysis of wood and straw (on a delivered basis).
Wood
Straw
Proximate analysis
Moisture (wt%)
Ash (wt%)
Volatile (wt%)
Fixed carbon (by diff.) (wt%)
Lower heating value (MJ/kg)
9.04
0.61
76.70
13.65
16.44
8.65
4.76
69.87
16.72
15.76
Ultimate analysis
Carbon (wt%)
Hydrogen (wt%)
Oxygen (by diff.) (wt%)
Nitrogen (wt%)
Sulfur (wt%)
45.05
5.76
39.41
0.13
0.01
42.88
5.65
37.51
0.49
0.06
100
80
60
wood
straw
20
0
0
200
400
600
800
Based on the measured data of soot, gas, and hydrocarbons, carbon mass balances were calculated for all applied experiments
listed in Table 2, and the results are shown in Fig. 3. In the gure,
the contents of lighter hydrocarbons (CxHy including CH4, C2H4,
and C3H8), CO2, CO and soot were calculated by the measured products, while the tar and larger hydrocarbons contents were estimated by the gap of the carbon mass balance. In operating
591
Fuel feeder
Feeding gas
Main gas
Steam generator
Water
Preheater
Protective gas
air
Reactor
N2
Heat exchanger
Flue gas outlet
Metal filter
Cyclone
Pump
Gas analyzer
and Micro GC
Pump
Table 2
Experimental conditions applied in wood and straw gasication.
No. T
(C)
H2O/C k
(mol/ ()
mol)
O2
t
(vol%) (s)
x y
Nitrogen Water
Air
Fuel
ow
ow
feeding ow
(Nl/min) (Nl/min) (g/min)
rate
(g/min)
1
2
3
4
Wood 5
6
7
8
9
10
11
1000
1200
1200
1350
1350
1350
1350
1350
1350
1350
1350
0.5
0.0
0.5
0.0
0.0
0.0
0.5
0.5
0.5
1.0
1.0
0.25 5
0.25 5
0.25 5
0.25 5
0.35 7
0.50 10
0.25 5
0.35 7
0.50 10
0.25 5
0.35 7
2.98
2.49
2.51
2.21
2.21
2.24
2.15
2.17
2.23
2.20
2.17
9.1
9.2
9.2
9.5
9.1
9.1
9.5
9.1
9.1
9.5
9.1
10
10
10
10
13
19
10
13
19
10
13
30
30
30
30
26
21
30
26
21
30
26
3.3
0
3.3
0
0
0
3.3
3.3
3.3
6.7
6.7
12
Straw 13
14
15
1350
1350
1350
1350
0.0
0.0
1.0
1.0
0.25
0.35
0.25
0.35
2.19
2.18
2.13
2.17
9.5
9.5
9.5
9.5
10
14
10
14
30
27
30
27
0
0
6.7
6.7
5
7
5
7
condition 1 (at 1000 C), the carbon mass balance had a large deviation (22 wt%) due to the high content of tar and larger hydrocarbons in the syngas. At higher temperatures (at 1200 C and
1350 C), the carbon mass balance closure was better, typically
within 9%. The hydrogen and oxygen mass balance could not be
closed since water yields were not determined, so they are not
shown in this paper.
Carbonout/Carbonin (%)
Fuel
Csoot/Cin
CCO /Cin
2
CCO/Cin
100
80
60
40
20
0
1
10 11 12 13 14 15
Operating conditions
Fig. 3. Carbon balances for all applied experiments: the carbon contents in soot,
CxHy, CO2 and CO are calculated based on the experimental measurement, while the
carbon content in tar and larger CxHy is determined by the gap of the carbon mass
balance.
592
and the remaining small amount probably was mixed with soot.
Fig. 4 shows the effect of reaction temperature on the soot yield
for wood gasication at k = 0.25. A sharp increase from 8.5 g/kg fuel
to 58.7 g/kg fuel in the soot yield was observed when the reaction
temperature was increased from 1000 C to 1200 C at H2O/C = 0.5.
Then it declined to 35.3 g/kg fuel as the reaction temperature further
increased to 1350 C. It is widely observed that soot is produced in
high temperature processes (10002500 C), such as pyrolysis and
gasication [2530]. Thus increasing the reaction temperature favors soot formation. However, at higher temperature, soot or its precursors probably have higher gasication reactivity. As a result of
the competition between soot formation and destruction [3033],
its yield starts to drop down after reaching a peak value at
1200 C. As shown in Fig. 4, the same trend was observed for the
experiments without steam addition (H2O/C = 0) at higher temperature (12001350 C).
Comparing Fig. 4 to Fig. 3, it is found that the soot yield was
lowest at 1000 C, whereas the amount of tar in the syngas was
highest. However, at 1350 C, a signicant yield of soot was produced, while there was nearly no tar in the gas due to cracking
and the reaction with steam of the heavy hydrocarbon chains to
form H2, CO and CO2 [34]. This shows that there is a trade off
60
50
40
30
20
H2O/C=0.5
10
H2O/C=0
0
1000
1100
1200
1300
1400
T (C)
Fig. 4. Effect of reaction temperature on the soot yield in wood gasication at
k = 0.25.
char was left, while soot often was observed. Very low amounts of
ash were collected in the cyclone, because the ash mainly melted
and deposited on the wall of the reactor due to the high temperature
1000
0.75
1200
1300
1400
1000
1100
1200
1300
1400
0.75
H2O/C=0.5
H2O/C=0
0.60
1100
0.60
0.45
0.45
0.30
0.30
0.15
0.15
0.00
0.30
H2
CO
CO2
CxHy
0.00
0.08
0.25
0.06
0.20
0.15
0.04
0.10
0.02
0.05
0.00
0.00
1000
1100
1200
1300
1400
1000
1100
1200
1300
1400
T (C)
0.06
H2O/C=0.5 H2O/C=0
CH4
0.06
0.05
C2H4
0.05
0.04
C3H8
0.04
0.03
0.03
0.02
0.02
0.01
0.01
0.00
0.00
1000
1100
1200
1300
1400
1000
1100
1200
1300
1400
T (C)
593
1.5
1.0
1.2
0.8
H2/CO
0.9
0.6
0.4
0.6
H2O/C=0.5
0.3
H2O/C=0.5
0.2
H2O/C=0
H2O/C=0
0.0
0.0
1000
1100
1200
1300
1400
1000
1100
1200
1300
1400
T (C)
T (C)
50
40
30
20
=0.25
10
=0.35
0
0.00
0.25
0.50
0.75
1.00
H2O/C (mol/mol)
Fig. 7. Effect of steam/carbon molar ratio on the soot yield in wood gasication at
1350 C.
between soot and tar formation, which may result from soot formation by tar and hydrocarbon polymerization competing with
soot gasication by CO2 and H2O at high temperature.
594
0.00
0.25
0.50
0.75
1.00
0.00
0.25
0.50
0.75
1.00
0.75
0.75
0.60
0.60
0.45
0.45
0.30
0.30
=0.25
=0.35
0.15
0.15
H2
0.00
0.35
CO
0.00
0.015
CO2 CxHy
0.30
0.012
0.25
0.009
0.20
0.15
0.006
0.10
0.003
0.05
0.00
0.000
0.00
0.25
0.50
0.75
1.00
0.00
0.25
0.50
0.75
1.00
H2O/C (mol/mol)
1.8
1.0
1.5
0.8
1.2
H2/CO
Fig. 8. Effect of steam/carbon molar ratio on the gas yield in wood gasication at 1350 C.
0.9
0.6
0.4
0.6
=0.25
0.3
=0.25
0.2
=0.35
=0.35
0.0
0.0
0.00
0.25
0.50
0.75
1.00
0.00
0.25
0.50
0.75
1.00
H2O/C (mol/mol)
H2O/C (mol/mol)
Fig. 9. Effect of steam/carbon molar ratio on the indicators in wood gasication at 1350 C.
50
40
30
20
H2O/C=0.5
10
H2O/C=0
0
0.25
0.30
0.35
0.40
0.45
0.50
Fig. 10. Effect of excess air ratio on the soot yield in wood gasication at 1350 C.
595
0.25
0.30
0.35
0.40
0.45
0.50
0.25
0.30
0.35
0.40
0.45
0.50
0.75
0.75
0.60
0.60
0.45
0.45
0.30
0.30
H2O/C=0.5
0.15
0.15
H2O/C=0
0.00
0.50
H2
CO
CO2
CxHy
0.00
0.012
0.40
0.009
0.30
0.006
0.20
0.003
0.10
0.000
0.00
0.25
0.30
0.35
0.40
0.45
0.50
0.25
0.30
0.35
0.40
0.45
0.50
Fig. 11. Effect of excess air ratio on the gas yield in wood gasication at 1350 C.
1.0
1.4
0.8
1.2
1.0
H2/CO
1.6
0.8
0.6
0.4
0.6
0.4
H2O/C=0.5
0.2
H2O/C=0.5
0.2
H2O/C=0
H2O/C=0
0.0
0.0
0.25
0.30
0.35
0.40
0.45
0.50
0.25
0.30
0.35
0.40
0.45
Fig. 12. Effect of excess air ratio on the indicators in wood gasication at 1350 C.
Fig. 13. SEM images of soot produced in wood and straw gasication.
0.50
50
45
=0.25; H2O/C=0
=0.25; H2O/C=1
=0.35; H2O/C=0
=0.35; H2O/C=1
596
40
35
30
25
20
15
10
5
2.0
=0.25; H2O/C=0
=0.25; H2O/C=1
1.8
=0.35; H2O/C=0
=0.35; H2O/C=1
1.6
1.4
1.2
1.0
0.8
0.6
0.4
0.2
0.0
0
wood
wood
straw
straw
Biomass type
Biomass type
Fig. 14. Effect of biomass type on the soot yield in wood and straw gasication at
1350 C.
1.2
wood
0.90
H2
0.75
=0.25; H2O/C=1
=0.35; H2O/C=0
=0.35; H2O/C=1
1.0
0.8
H2/CO
might be caused by the cracking and reforming of larger hydrocarbons and tar. Similar trends were observed at k = 0.35.
The variation of the producer gas yield with the steam/carbon
molar ratio in wood gasication at 1350 C is shown in Fig. 9a.
With addition of steam, the producer gas yield increased about
0.110.18 Nm3/kg fuel, most likely due to the promotion of steam
gasication of soot and the increase of steam cracking and reforming of larger hydrocarbons and tar. According to Figs. 8 and 9a, it
can be concluded that even a high amount of steam injection
(H2O/C = 1) only makes small changes of the gas yields.
The effect of steam/carbon molar ratio on the molar ratio of H2/
CO in wood gasication at 1350 C is shown in Fig. 9b. This ratio
increased from 0.7 to 1 with the increased steam/carbon molar ratio from 0 to 0.5 at k = 0.25, and was then nearly constant at steam/
carbon molar ratio larger than 0.5. At k = 0.35, the molar ratio of
H2/CO kept increasing continually with the steam/carbon molar
ratio in the range of 01, and its maximum value was also 1. The
molar ratio of H2/CO is equal to 1 with the largest supplied amount
of steam addition (H2O/C = 1).
=0.25; H2O/C=0
0.6
0.4
0.2
0.0
wood
straw
Biomass type
straw
wood
=0.25; H2O/C=0
=0.25; H2O/C=1
=0.35; H2O/C=0
=0.35; H2O/C=1
straw
CO
0.90
0.75
0.60
0.60
0.45
0.45
0.30
0.30
0.15
0.15
0.00
0.30
0.00
CO2
CxHy
0.012
0.25
0.009
0.20
0.15
0.006
0.10
0.003
0.05
0.00
wood
straw
wood
straw
Biomass type
Fig. 15. Effect of biomass type on the gas yield in wood and straw gasication at 1350 C.
0.000
597
Csoot/Cin
x y
CC H /Cin
CCO /Cin
x y
CCO/Cin
Carbonout/Carbonin (%)
100
80
60
40
20
13e
13c
14e
14c
13e
13c
14e
14c
15e
15c
15e
15c
12e
12c
12e
12c
11e
11c
10e
10c
9e
9c
8e
8c
7e
7c
6e
6c
5e
5c
4e
4c
3e
3c
2e
2c
1e
1c
Operating conditions
HH O/Hin
HC H /Hin
HH /Hin
x y
Hydrogenout/Hydrogenin (%)
100
80
60
40
20
11e
11c
10e
10c
8e
8c
9e
9c
7e
7c
6e
6c
5e
5c
4e
4c
3e
3c
2e
2c
1e
1c
Operating conditions
CO2 yield increased from 0.19 Nm3/kg fuel to 0.40 Nm3/kg fuel.
This is due to the oxidation of soot, H2, CO and other gaseous species [13,16,19,40]. There was no large drop in the CO yield when
the excess air ratio increased from 0.25 to 0.35, probably because
the partial combustion of hydrocarbons and soot could produce a
certain amount of CO and then a part of them might be further oxidized to CO2, which nearly keeps the CO yield constant. However,
when the excess air ratio was increased to 0.5, the CO yield decreased. With and without steam addition, the gas yield had the
same variation tendency as the excess air ratio increased.
The producer gas yield shown in Fig. 12a is obtained at different
excess air ratios in the range of 0.250.5 in wood gasication at
1350 C. The amount of producer gas nearly kept constant with
an increase of excess air ratio especially between 0.25 and 0.35.
The soot oxidation forms gas while the H2 combustion consumes
gas, so based on an overall consideration of formation and consumption, the increased excess air ratio does not inuence the producer gas yield a lot.
598
Csoot/Cin
CC H /Cin
CCO /Cin
CCO/Cin
Carbonout/Carbonin (%)
x y
100
80
60
4e
4c
4a
12e
12c
12a
Operating conditions
Fig. 18. Comparison among experimental, equilibrium calculation and recalculated
experimental results at 1350 C with H2O/C = 0 and k = 0.25: e means experimental
results, c means equilibrium calculation results and a means recalculated and
normalized experimental results assuming soot and hydrocarbons are gasied by CO2.
100
CH4
H2O
H2
CO2
CO
80
60
40
20
0
100
CH4
H2O
CO2
CO
H2
80
60
40
20
0
600
800
1000
1200
1400
600
800
1000
T (C)
T (C)
(a) H2O/C=0
(b) H2O/C=1
1200
1400
Fig. 19. Effects of reaction temperature and steam/carbon molar ratio on the product distribution with k = 0.25 at equilibrium conditions.
4. Conclusions
Gasication of two types of biomass, wood and straw, has been
investigated in a laboratory scale atmospheric pressure entrained
ow reactor at low oxygen concentration to ensure isothermal
conditions. In all experiments, the char was completely converted.
At 1200 C and 1350 C, all calculated carbon mass balance closures were reasonable, typically within 9%, but at 1000 C, the
carbon mass balance has a large deviation (22 wt%) due to the high
content of unmeasured tar and larger hydrocarbons in the syngas.
The yields of producer gas (dened as the sum of H2, CO, CO2 and
hydrocarbons up to C3 species) increased by 72% when the reaction
temperature was increased from 1000 C to 1350 C because of
steam reforming of tar and heavier hydrocarbons. The H2/CO molar
ratio in syngas was close to 1 at higher temperatures (>1200 C)
with steam addition. At 1350 C, a signicant yield of soot was produced, while there was nearly no tar formation. Conversely, at
1000 C, the soot yield was lowest, whereas the amount of tar
was highest. Thus, there is a trade off between soot and tar formation. When steam was introduced, the yields of producer gas and
H2 increased slightly while the CO yield decreased a little. The molar ratio of H2/CO was equal to 1 with the largest addition amount
of steam (H2O/C = 1). The soot yield can be reduced approximately
by 2050% with H2O/C = 1. The amount of producer gas nearly kept
constant with an increase of excess air ratio from 0.25 to 0.5 especially in the range of 0.250.35. Increasing excess air ratio from
0.25 to 0.5 decreased the yields of H2 and CO by about 25% and
12% respectively, increased the yield of CO2 by 89111%, and decreased the H2/CO molar ratio. Increasing excess air ratio also led
to a sharp drop of the soot yield by about 75%. The applied biomass
type has little inuence on the product compositions. At 1350 C
and with steam addition, the experimental results are close to
the gas composition obtained by equilibrium calculation.
From an energy efciency point of view, a relatively low reactor
temperature and a minimum of oxygen and water should be employed. However from a viewpoint of utilizing the syngas as a fuel,
the highest temperature (T = 1350 C), the largest amount of steam
addition (H2O/C = 1), and a suitable excess air ratio (k = 0.35) are
desirable providing high yields of H2 and CO with low yield of soot
599
and almost without tar, and a suitable molar ratio of H2/CO (close
to 1) for synthesis of higher alcohols.
Acknowledgements
This work was carried out as a part of the Combustion and
Harmful Emission Control (CHEC) research centre at the Department of Chemical and Biochemical Engineering, Technical University of Denmark. The Danish Research Council for Technology and
Production under project 09-064201/FTP and the Danish Energy
Agency are acknowledged for sponsoring the project.
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