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h i g h l i g h t s
Spouted bed reactor is an interesting technology for biomass steam gasication.
Temperature improves gas and hydrogen yields and carbon conversion efciency.
Steam/biomass ratio has a positive effect on gas composition and conversion.
Biomass particle size has shown a limited effect on gasication performance.
High tar yields are obtained and consequently cracking catalysts should be used.
a r t i c l e
i n f o
Article history:
Received 6 June 2013
Received in revised form 23 September 2013
Accepted 8 October 2013
Available online 17 October 2013
Keywords:
Steam gasication
Spouted bed
Biomass
Hydrogen
a b s t r a c t
Pinewood sawdust has been gasied by using steam as gasifying agent in a conical spouted bed reactor
operating in continuous regime. A study has been made of the effect of temperature (in the 800900 C
range), steam/biomass ratio (between 0 and 2) and sawdust particle size (0.31, 12 and 24 mm ranges)
on the distribution of products (gas, tar and char) and their composition has been studied. Temperature
has a positive effect on the gas composition by increasing H2 content and reducing that of CO. Furthermore, the tar and char yields are reduced as gasication temperature is higher. An increase in steam/biomass ratio from 0 to 1 has a positive effect on hydrogen concentration, char gasication and tar
reforming, and a further increase in this parameter from 1 to 2 gives way to only a limited improvement
in the results. Sawdust particle diameter plays a minor role in the gasication process in the temperature
range studied, which must be attributed to the high heat transfer rate in the bed. Thus, this technology
allows operating with coarse sawdust particles without reducing the syngas yield. However, the reduced
gas residence time gives way to a high tar yield.
2013 Elsevier B.V. All rights reserved.
1. Introduction
Biomass is regarded as the most promising alternative to fossil
fuels, given that when it is properly exploited it does not contribute to a net rise in the level of CO2 in the atmosphere. Furthermore,
it is the only renewable source of xed carbon that can be used for
generating both heat and power and converted into liquid, solid,
and gaseous fuels and chemicals [1,2].
Gasication is considered to be one of the most effective methods for the upgrading of biomass because the gas produced can be
used directly as fuel or as renewable raw material for the large
scale production of valuable chemical products and fuels.
The main advantage of using steam as gasifying agent lies in the
production of gas with a high hydrogen concentration, and the
Corresponding author. Tel.: +34 946012527; fax: +34 946 013 500.
E-mail address: martin.olazar@ehu.es (M. Olazar).
1385-8947/$ - see front matter 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.cej.2013.10.018
260
Table 1
Raw biomass characterization.
Ultimate analysis (wt%)
Carbon
Hydrogen
Nitrogen
Oxygen
49.33
6.06
0.04
44.57
73.4
16.7
0.5
9.4
19.8
261
oxygenates char
131:3 kJ mol
90:1 kJ mol
3
1
5
1
41:2 kJ mol
206:3 kJ mol
1
262
Fig. 3. Effect of gasication temperature on the tar content in the gaseous product
stream (on a dry basis) (Fig. 3a), char yield (Fig. 3b) and carbon conversion
efciency (Fig. 3c). Steam/biomass = 1, particle size 12 mm.
the gaseous stream is rather high. The maximum tar content is obtained at 800 C (364 g Nm3, on a dry basis) and this value decreases to 142 g Nm3 operating at 900 C due to the positive
effect of temperature on tar cracking and reforming reactions
(Eq. (5)) [46].
The tar yield is highly dependent on gasication conditions,
such as residence time, temperature and S/B ratio. Therefore, very
different results are obtained depending on the technology used.
Thus, Wei et al. [39] have studied the steam gasication (S/
B = 0.6) of pinewood sawdust in a free fall reactor and have observed a signicant decrease in tar content in the gaseous product
stream with temperature from 46 g Nm3 at 750 C to 6 g Nm3 at
850 C. Rapagna et al. [7] have used a uid bed of sand for the
steam gasication (S/B = 1) of almond shells at 770 C, obtaining
a tar content of 43 g Nm3. Gil et al. [5] have studied the gasication (S/B = 0.9) of pinewood at 780 C also in a uid bed made up of
sand, with the tar yields being in the 3080 g Nm3 range. Michel
et al. [9] have obtained high tar yields in the steam gasication of
miscanthus giganteus in a uidised bed reactor using olivine as primary catalyst, at the highest temperature studied of 880 C, i.e.,
46 g of tar (gbiomass+water)1 for a S/B ratio of 1.1. The tar values obtained by Umeki et al. [47] using an updraft gasier are between 50
and 100 g Nm3, although it should be noted that the S/B ratios
used in this study are very high because superheated steam is used
in this reactor to provide energy for the gasication process.
In order to reduce the tar content in the gaseous product stream
obtained in the steam gasication of biomass (usually lower when
air or steam/O2 mixtures are used as gasication agent) [5,46],
different options have been studied in the literature, such as the
use of catalysts and on-line cracking/reforming [48]. Koppatz
et al. [14] have obtained low tar concentrations (19 g Nm3) in the
steam gasication of wood pellets in a dual uidised bed at 850 C
using sand as inert bed material, and they managed to reduce this
concentration by 3560% (depending on tar nature) by using
olivine as catalyst. Carpenter et al. [49] have studied a two-step
process, that is, gasication in a uidised bed followed by thermal
cracking in-line at 875 C, obtaining a tar concentration of
49 g Nm3. Eka et al. [50] have also studied a two-step process
involving pyrolysis (500 C) in a screw kiln and subsequent
cracking or catalytic reforming at 760 C. Their runs with sand in
the second reactor give way to a high tar yield, 33 wt%, but this
value is reduced to 25% when using a reforming Ni/SiO2 catalyst.
As observed in Fig. 3b, char gasication is enhanced by temperature due to the highly endothermic nature of steam (Eqs. (2) and
(3)) and dry char (Eq. (4)) gasication reactions. The char yield at
800 C is 8.9% and decreases to 4.5% at 900 C. It should be noted
that this result depends on char residence time in the reactor. Thus,
char gasication reaction kinetics is slow even above 800 C and,
consequently, char yield depends on its residence time. In this
study, each continuous run lasted for around 20 min, with the char
remaining in the reactor for this period of time.
The char yields obtained in the literature by other authors differ
considerably due to the wide variety of technologies used and the
different kinds of biomasses studied. Thus, several studies have
been carried out in dual uidised beds in which the char is burned
to provide energy for the endothermic gasication process. Other
studies pay attention to the effect of operating conditions on gas
composition, but the char yields are not determined. The reduction
in char yield with temperature has been mentioned by other
authors [9,39]. Thus, the char yields obtained by both Uemiki
et al. [47] in an updraft gasier and Rapagna et al. [7] in a uid
bed are higher than those in this paper, with values being over
10%. Michel et al. [9] have used a uid bed and observed a minimum char yield of 6.7% at the maximum temperature studied of
880 C. Wei et al. [39] achieved efcient char gasication in a free
fall reactor at 850 C, with char yield being as low as 2%.
As observed in Fig. 3c, carbon conversion efciency increases
with temperature, from 50% at 800 C to 70% at 900 C, by tar
cracking and char gasication reactions to yield gases. This result
may be improved by increasing the char residence time in the reactor. The spouted bed reactor is able to operate without deuidization problems with high amounts of char in the bed and,
consequently, with high residence times for the char. In addition,
the char can be burned to provide energy for the process, which
will not cause loss of efciency in the gasication process.
However, tar formation leads to a loss of efciency in the conversion of biomass to gases, given that tar condensation gives
way to the formation of aerosols in the process equipment, engines, turbines and so on. Consequently, the main challenge to increase carbon conversion efciency lies in the cracking of the tar to
obtain higher gas yields. Tar reduction can be achieved by primary
measures (inside the gasier) or secondary ones (downstream of
the gasier). Thus, successful results are reported in a previous
study dealing with the steam gasication of waste plastics, in
which two different cracking catalysts (olivine and c-Al2O3) have
been used to reduce the tar content in the syngas produced [38].
263
Table 2
Variables studied and their levels.
Temperature (C)
S/B ratio
800
850
900
0 (0.11)a
1 (1.22)
2 (2.33)
0.31
12
24
a
The values in brackets correspond to the S/B ratio calculated considering the
biomass moisture content.
264
Table 3
Detailed composition (wt%) of the tar fraction obtained at different temperatures.
Compound
800 C
850 C
900 C
Toluene
Phenol
2-Ethyl phenol
3-Methyl phenol
Naphtalene
2,3-Dihydrobenzofuran
1-Methyl naphtalene
2-Methyl naphtalene
Biphenylene
1,7-Dimethyl naphtalene
2-Ethenyl naphtalene
1,2-Dimethyl naphtalene
2,3-Dimethyl naphtalene
Acenaphthene
Biphenylene
4-Methyl-1,10 -biphenyle
2-Methyl-1,10 -biphenyle
1-Naphtalenol
Dibenzofurane
3-Methyl-1,10 -biphenile
1-(2-Propenyl)-naphtalene
9-Methanol uoreno
1H-Phenalene
Fluorene
1-Methyl-9H-uorene
4-Methyl dibenzofurane
[1,10 -Biphenyl]-3-ol
p-Hydroxyphenile
9H-Fluoren-9-one
2-Dibenzofuranol
Anthracene
Phenanthrene
9-Methyl anthracene
2-Methyl anthracene
1-Methyl anthracene
4H-Cyclopentaphenanthrene
1-Methyl phenanthrene
2-Phenyl naphtanele
9-Ethenyl anthracene
1-Phenyl naphtalene
Pyrene
4,5-Dihydropyrene
Fluoranthene
1-Methyl pyrene
2,3-Benzouorene
Benzo[c] phenanthrene
Benzanthrene
Benzo [e] acefenantrilene
Perylene
Benzo [j] uoranthene
Unidentied
3.5
2.1
0.1
7.8
4.2
0.6
1.0
0.6
0.8
0.3
0.4
0.3
0.1
0.8
2.3
0.4
1.1
1.2
2.7
0.9
0.2
0.4
0.3
1.6
0.7
0.4
0.6
0.5
0.4
1.5
5.1
1.7
0.9
0.8
0.6
1.9
0.9
1.4
0.2
0.4
2.4
0.6
4.1
0.3
0.2
0.6
0.4
0.1
0.3
0.2
39.0
4.0
2.0
0.1
5.6
7.0
0.2
1.2
0.0
1.0
0.5
0.0
0.2
0.1
0.6
3.0
0.3
0.3
3.3
0.5
1.7
0.2
0.2
0.2
3.5
0.5
0.6
0.3
0.6
0.5
0.5
9.6
3.2
1.0
1.1
0.5
2.7
1.0
1.9
0.1
0.3
4.3
0.1
0.5
0.5
0.2
0.8
0.5
0.0
0.1
0.2
32.7
5.2
2.5
0.0
4.1
13.3
0.0
1.4
0.0
1.6
0.0
0.7
0.2
0.1
0.6
3.3
0.3
0.0
5.3
0.1
3.0
0.1
0.1
0.1
6.1
0.6
0.3
0.1
0.7
0.3
0.0
14.6
3.5
0.8
0.9
0.2
1.5
0.8
1.7
0.0
0.0
4.5
0.0
4.3
0.1
0.1
0.0
0.0
0.0
0.0
0.0
16.8
Fig. 5. Effect of steam/biomass ratio on the gaseous fraction composition (on a dry
basis). 900 C, particle size 12 mm.
Fig. 6. Effect of steam/biomass ratio on the tar content in the gaseous product
stream (on a dry basis) (Fig. 6a), char yield (Fig. 6b) and carbon conversion
efciency (Fig. 6c). 900 C, particle size 12 mm.
trends depending on the range of S/B ratios used. Thus, Umeki et al.
[47] and Luo et al. [40] have observed the same trend as in this
study, up to S/B ratios of 3 and 2.1, respectively, but they have reported a decrease in the concentration of both hydrogen and carbon dioxide for higher S/B values.
The maximum hydrogen content of 41% has been obtained
operating with an S/B ratio of 2, with an H2/CO ratio being of
around 1.4 under these conditions. Subsequent catalytic reforming
of the gaseous product would increase the content of hydrogen
and, therefore, the H2/CO ratio. Thus, Orio et al. [53] have reported
that the tars obtained by steam gasication are more suitable for
subsequent elimination than those obtained using other gasifying
agents.
Fig. 6 shows the effect of the S/B ratio on tar content in the gaseous product stream (Fig. 6a), char yield (Fig. 6b) and carbon conversion efciency (Fig. 6c). As observed in Fig. 6a, the tar content
has been reduced from 154 g Nm3 with a S/B ratio of 0 to 142
g Nm3 with an S/B = 1, given that an increase in the S/B ratio promotes tar cracking and reforming reactions (Eq. (5)). However, a
further increase in the S/B ratio from 1 to 2 only slightly reduces
the tar content of the gaseous product. Similarly, the increase in
the gas yield is also rather low when the S/B ratio is increased from
1 to 2. Thus, the gas yield reaches 83.8 g/100 g biomass when
operating with an S/B ratio of 2, whereas the yields are 81.6 and
66.5 g/100 g of biomass with an S/B ratio of 1 and 0, respectively.
An additional positive effect of operating with high S/B ratios is
the enhancement of char gasication (Eqs. (2) and (3)). Thus, a
signicant reduction in char yield is observed, from 10.7% using
an S/B = 0 to 3.6% with the maximum ratio used being S/B = 2.
The enhancement of char gasication and the slight reduction
in the tar content give way to an increase in carbon conversion
265
Fig. 8. Effect of sawdust particle size on the gaseous fraction composition (on a dry
basis). 850 C, Steam/biomass = 1.
Fig. 9. Effect of sawdust particle size on the tar content in the gaseous product
stream (on a dry basis) (Fig. 9a), char yield (Fig. 9b) and carbon conversion
efciency (Fig. 9c). 850 C, Steam/biomass = 1.
Fig. 7. Effect of steam/biomass ratio on the tar fraction composition. 900 C, particle
size 12 mm.
266
Acknowledgements
This work was carried out with nancial support from the
Ministry of Science and Education of the Spanish Government
(Project CTQ2010-16133), from the Basque Government (Project
IT748-13 ) and from the University of the Basque Country (UFI
11/39). Maider Amutio thanks the University of the Basque
Country for her postgraduate Grant (UPV/EHU2011).
Fig. 10. Effect of sawdust particle size on the tar fraction composition. 850 C,
Steam/biomass = 1.
The consequence of increasing both tar and char yields by operating with larger sawdust particles is a decrease in carbon conversion
efciency (Fig. 9c).
The effect of particle size is almost negligible in the range studied, and coarse particles (24 mm) may therefore be used without
signicant operational problems, with the performance being
similar to that observed with ne biomass particles. This result is
especially interesting for the economy of the process, given that
the cost of reducing biomass particle size is of around 10% of the
output energy obtained in the gasication process [54,56,57].
However, as particle size is increased the steam gasication rate
decreases [58] and the residence times required for gasication
are also higher, so the reactor volume must be higher for obtaining
the same output [54,59].
Fig. 10 shows the tar composition obtained with different
sawdust particle sizes. As observed, the composition of the tar is
almost independent of biomass particle size. Therefore, particle
size has no inuence on subsequent tar cracking processes.
4. Conclusions
The conical spouted bed reactor is an interesting technology for
the continuous steam gasication of biomass given its capacity for
operating in isothermal regime, versatility in the steam/biomass
ratio and absence of deuidization problems. An increase in gasication temperature improves process efciency in terms of conversion to gases, with the maximum carbon conversion efciency
being 70% at 900 C. Furthermore, an increase in temperature also
has a positive effect on the hydrogen content in the gases, with a
value of 38% at 900 C.
An increase in the steam/biomass ratio has a positive effect on
the gas fraction composition by increasing the hydrogen content
and the hydrogen/carbon monoxide ratio, which is interesting for
the applications of the syngas produced. In addition, higher steam
concentrations in the reaction environment enhance both tar
cracking and char gasication, and so increase carbon conversion
efciency.
Biomass particle size has a limited effect on both gas composition and tar and char yields, even when particles are coarse
(24 mm), which is explained by the high heat and mass transfer
rates in the conical spouted bed reactor. This is an encouraging
result because biomass grinding requires a signicant amount of
energy.
A rather high tar yield is obtained in the steam gasication of
biomass, given that under the optimum conditions (900 C,
steam/biomass = 2) the tar content in the gas is 168 g Nm3. The
use of catalysts for cracking/reforming will be addressed in future
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