You are on page 1of 6

1186 Energy & Fuels 2005, 19, 1186-1191

Effect of Superficial Velocity on Tar from Downdraft


Gasification of Biomass
Takashi Yamazaki,*,† Hirokazu Kozu,† Sadamu Yamagata,† Naoto Murao,†
Sachio Ohta,† Satoru Shiya,‡ and Tatsuo Ohba‡
Department of Environmental and Resource Engineering, Hokkaido University,
Kita-ku Kita-13 Nishi-8, Sapporo 060-8628, Japan

Received November 2, 2004. Revised Manuscript Received February 15, 2005

Changes in the amount and composition of tar according to superficial velocity (SV) were
investigated in a downdraft biomass gasifier. SV of the downdraft gasification with air was varied
in the range of 0.3-0.7 m/s, and tar was recovered at the gasifier outlet. The tar was classified
as gravimetric tar and gas-chromatography-detectable (GC-detectable) tar. The lowest gravimetric
tar yield (0.7%) was obtained at 0.4 m/s SV, and the highest was obtained at 0.7 m/s. GC-detectable
tar yield was highest (1.5%) at 0.7 m/s. One-ring aromatics and naphthalene accounted for more
than 80% of GC-detectable tar mass. Some constituents of GC-detectable tar showed specific
trends according to SV, although the main composition did not show extreme change. The effect
of SV on the production of gases and particles was also studied.

1. Introduction Kurkela and Ståhlberg observed that tar yield decreased


with an increase in the temperature of freeboard during
Tar in the producer gas from biomass gasification
the gasification of Finnish peat, sawdust, and German
often causes operational problems in internal combus-
brown coal in a pressurized fluidized bed with air and
tion (IC) engines. Downdraft gasifiers generally produce
steam.6 Kinoshita et al. performed sawdust gasification
less tar than updraft gasifiers or fluidized-bed gasifiers,
in an indirectly heated fluidized-bed gasifier and re-
so they are expected to be used for electrical generation
ported that tar yield decreased with increasing temper-
systems that incorporate IC engines.1 However, the tar
ature.7 Other studies showed that high temperature
concentrations generated in most downdraft gasifiers
reduced the tar yield.8-12 As for the effect of residence
still exceed the limit for IC engines, and further tar
time, Fagbemi et al. indicated that tar yield decreased
reduction is needed.1-3
with residence time in the range of 0.3-4 s,15 while
Tar removal technologies can be categorized into two
Kinoshita et al. reported that tar yield was not influ-
approaches: improvement of the gasification process
enced much by the change of residence time from 3.2 to
itself inside the gasifier (primary removal), and gas
4.8 s.7 It is well-known that tar conversion depends on
cleaning outside the gasifier (secondary removal).4
the time of residence in the presence of catalysts.16
Secondary removal is costly and often does not fulfill
Ekstrom et al. showed that char plays a role in tar
the requirements of gas quality for IC engines.5 Primary
cracking.17 In a downdraft gasifier where tar passes
methods have not been fully investigated.4 These meth-
through a char bed, increasing the residence time may
ods involve proper gasification design, use of a suitable
decrease the amount of tar.
catalyst during gasification, and the optimization of
For directly heated downdraft gasifiers that use air
operational parameters. Many studies, most of which
as a gasification agent, airflow rate is the most impor-
used indirectly heated gasifiers and fluidized bed gasifi-
tant operating parametersmuch more important than
ers, have been conducted on operational parameters
such as temperature, residence time, equivalence ratio, (8) Narváez, I.; Orı́o, A.; Aznar, M. P.; Corella, J. Ind. Eng. Chem.
Res. 1996, 35, 2110-2120.
oxygen partial pressure, and gasification medium.6-14 (9) Jensen, P. A.; Larsen, E.; Jørgensen, K. H. In Proceedings of the
9th European Bioenergy Conference, Copenhagen, Denmark, 1996;
* Corresponding author: Tel: +81-11-706-6836. Fax: +81-11-706- Pergamon: Oxford, 1996; pp 1371-1375.
6835. E-mail: zakky@eng.hokudai.ac.jp. (10) Yu, Q.; Brage, C.; Chen, G.; Sjöström, K. J. Anal. Appl. Pyrolysis
† Hokkaido University. 1997, 40-41, 481-489.
‡ Japan Wood Energy Co., Ltd. (11) Padban, N.; Wang, W.; Ye, Z.; Bjerle, I.; Odenbrand, I. Energy
(1) Beenackers, A. A. C. M. Renewable Energy 1999, 16, 1180-1186. Fuels 2000, 14, 603-611.
(2) Milne, T. A.; Abatzoglou, N.; Evans, R. J. Biomass gasifier (12) Morf, P.; Hasler, P.; Nussbaumer, T. Fuel 2002, 81, 843-853.
“Tars”: their nature, formation, and conversion; NREL/TP-570-25357; (13) Padban, N.; Odenbrand, I. Energy Fuels 1999, 13, 1067-1073.
Golden, CO, 1998. (14) Gil, J.; Corella, J.; Aznar, M. P.; Caballero, M. A. Biomass
(3) Knoef, H. A. M. Biomass Bioenergy 2000, 18, 39-54. Bioenergy 1999, 17, 389-403.
(4) Devi, L.; Ptasinski, K. J.; Janssen, F. J. J. G. Biomass Bioenergy (15) Fagbemi, L.; Khezami, L.; Capart, R. Appl. Energy 2001, 69,
2003, 24, 125-140. 293-306.
(5) Hasler, P.; Nussbaumer, T. Biomass Bioenergy 1999, 16, 385- (16) Corella, J.; Anzar, M. P.; Gil, J.; Caballero, A. Energy Fuels
395. 1999, 13, 1122-1127.
(6) Kurkela, E.; Ståhlberg, E. Fuel Process. Technol. 1992, 31, 1-21. (17) Ekström, C.; Lindman, N.; Pettersson, R. In Fundamentals of
(7) Kinoshita, C. M.; Wang, Y.; Zhou, J. J. Anal. Appl. Pyrolysis Thermochemical Biomass Conversion; Elsevier Applied Science: Lon-
1994, 29, 169-181. don and New York, 1985; pp 601-618.

10.1021/ef0497210 CCC: $30.25 © 2005 American Chemical Society


Published on Web 03/22/2005
Effect of SV on Tar from Downdraft Gasification Energy & Fuels, Vol. 19, No. 3, 2005 1187

Figure 1. Scheme of the laboratory-scale gasification plant with a downdraft gasifier.

temperature and residence time. Increasing the airflow


rate achieves a high burning rate, resulting in increased
temperature and decreased residence time. So optimiz-
ing the airflow rate is essential for proper operation.
However, optimized airflow rate is specific to the
individual gasifier; therefore, it cannot be generalized
to various gasifiers. Reed et al. suggested superficial
velocity (gas flow rate divided by the internal cross
section of the gasifier) as the most important measure
of gasifier performance, as it controls gas production
rate, fuel consumption rate, gas energy content, char
and tar production rate, and so on.18 Superficial velocity
(SV), which increases with airflow rate, is independent
of gasifier size and permits comparison of gasifiers of
different dimensions.18,19 Bui et al. used specific gasifi-
cation rate, the fuel consumption rate divided by the
internal cross section of the gasifier, as a parameter of
tar content from two directly heated gasifiers.20 SV
correlates linearly with specific gasification rate, ac-
cording to Tiangco et al.21 Few studies have examined
the effect of these parameters on tar characteristics. In
light of this, our investigation addressed the effect of
SV on the amount and composition of tar.
In this study, a laboratory-scale gasifier was operated
while SV was changed from 0.3 to 0.7 m/s. The yields
Figure 2. Downdraft gasifier.
and the constituents of the sampled tar, as well as those
of gases and particles, were measured and are reported. Table 1. Properties of Todo Fir Chips

2. Experimental Section moisture content [wt %, wet basis] 9-13


size [mm]
2.1. Gasification System and Operation. All experiments width 10-20
were carried out with a laboratory-scale gasifier coupled to a length 20-50
gas engine generator (Figure 1). The gasification plant consists thickness 5
of a downdraft gasifier, ash separator, gas cooler, gas filter, bulk density [kg/m3] 110-120
2.3-kVA IC engine (GM2600SSM, Denyo), and two blowers proximate analysis [wt %, db]
volatile matter 79.3
(0.04, 0.15 kW). Sampling units for gases, tar, and particles fixed carbon 20.4
are installed at the gasifier exit. An orifice to measure gas flow ash 0.3
rate is placed after the gas cooler. Manometers and K- ultimate analysis [wt %, db]
thermocouples are set up at the same place as the sampling C 51.0
units and the orifice. This system uses air as the gasification H 5.7
O 43.0
agent. The airflow rate can be adjusted by the valve at the N 0.0
inlet of the gasifier. The downdraft gasifier (Figure 2) is a ash 0.3
cylindrical chamber 1050 mm in height and 250 mm in high heating value [MJ/kg, db] 21.2
diameter. It has a 70-mm-diameter throat and four 12-mm-
diameter nozzles. The nozzles are 70 mm higher than the
(18) Reed, T. B.; Walt, R.; Ellis, S.; Das, A.; Deutch, S. In Proceedings throat. The K-thermocouple is installed at the same height as
of the 4th Biomass Conference of the Americas, Oakland, California,
1999; Elsevier Science, Ltd.: Oxford, 1999; Vol. 2, pp 1001-1007.
the four nozzles to measure temperature at this point as the
(19) Reed, T. B.; Gaur, S. A survey of biomass gasification 2001; reference temperature of the gasifier.
NERL and BEF, Inc.: Golden, CO, 2001. Woodchips (Todo fir) were used for fuel. Their properties
(20) Bui, T.; Loof, R.; Bhattacharya, S. C. Energy 1994, 19, 397-
404.
are shown in Table 1. The chips (4 kg) were supplied to the
(21) Tiangco, V. M.; Jenkins, B. M.; Goss, J. R. Biomass Bioenergy gasifier and ignited. After the ignition, air was supplied with
1996, 11, 51-62. a 0.04-kW blower. At the beginning of operation, gas from the
1188 Energy & Fuels, Vol. 19, No. 3, 2005 Yamazaki et al.

room temperature. The fifth (containing the same solvent) and


the sixth (containing no solvent) were cooled at -20 °C in a
cold bath. To avoid filter breakage by clogging, sampling trains
were replaced during a run with the sampling duration of 8
to 15 min.
After sampling, tar was extracted from sampling filter by
Soxhlet extraction with 2-propanol. The extracted tar was
added to the 2-propanol tar solution in the impingers, and 50
mL of the resultant solution (filter tar plus impinger tar
solution) was concentrated using a rotary evaporator (55-57
°C, 230 hPa). The tar residue was weighed for each sample.
After tar extraction, the filter was dried at 110 °C for 12 h to
obtain the particle weight.
Figure 3. Profiles of the reference temperature and the gas The organic constituents in the tar solution were identified
flow rate during gasification (Run D). using GC-MS (HP5890, Hewlett-Packard) and quantified using
GC-FID (HP5890, Hewlett-Packard). For both analyses, two
silica capillary columns were used: HP-1 (0.35 µm) for high-
volatility compounds, and HP-5 (0.25 µm) for low-volatility
compounds. In addition to the tar solution, the tar residue was
determined by GC-FID after redissolution into 2-propanol.
The particles on the filter after extraction were observed
by scanning electron microscopy (SEM: S-3200N, Hitachi).

3. Results and Discussion


3.1. Experimental Results. The results of each
experiment are summarized in Table 2. Each data point
represents the mean value obtained from each run.
Superficial velocity (SV) was calculated from gas flow
rate divided by the internal cross section of the gasifier,
i.e., the throat cross-sectional area (0.00385 m2). The
reference temperature of the gasifier became higher
with an increase in SV. As shown in Table 2, equivalent
Figure 4. Sampling system for tar and particles. ratios, the weight ratio of supplied oxygen to oxygen
needed for complete combustion of fuel, were 0.33-0.41
gasifier bypassed downstream units (from the ash separator and show no clear trends with respect to SV.
to the IC engine) to prevent pollutants from contaminating 3.2. Gases. The effect of SV on gas composition is
the units. This start-up operation was continued for 10 min, shown in Figure 5. Concentrations of CO and H2 showed
after which the gas flow rate to the downstream units was similar trends in SV from 0.3 to 0.7 m/s, increasing from
roughly constant (Figure 3). The airflow rate at the gasifier 15 to 21 vol % and from 8 to 11 vol %, respectively. In
inlet was kept between 3.0 and 6.7 m3/h, a rate that enables contrast, CO2 decreased from 17 to 13 vol % at the same
the IC engine to run. This steady-state operation was contin- condition. CH4 concentration did not change much.
ued for 20 to 50 min, depending on the airflow rate setting,
These trends may have resulted from the promotion of
which controls the fuel-consumption rate. At the end of the
experiment, N2 gas was introduced into the gasifier for water-gas reaction (C + H2O/H2 + CO), which is
extinguishment. Chip residue and char remaining in the promoted at temperatures higher than approximately
gasifier were recovered and weighed after each experiment. 700 °C.19 The change in gas composition was remarkable
2.2. Measurement of Products. 2.2.1. Gases. Gases (H2, for SV between 0.3 and 0.4 m/s, but gas composition was
CO, CO2, CH4, and N2) were sucked by air pump (AP115, constant at SVs exceeding 0.4 m/s. The low heating
Iwaki) and distributed into the sampling loop of GC-TCD (GC- value (LHV) of the gases was 3.5-4.7 MJ/m3 in the
14A, Shimazu, column: active carbon 30/60). The samples region of 0.3-0.7 m/s SV, and gas composition produced
were introduced into the GC by manual operation of the valve above 0.4 m/s SV was more suitable for the IC engine.
of the sampling loop every 5 min for analysis. An active carbon 3.3. Tar Amount. Tar was classified as gravimetric
column cannot separate N2 from O2, but the concentrations of tar and GC-detectable tar by determination method.
O2 at the gasifier outlet were less than 1%, which was
Gravimetric tar, heavy tar, refers to unidentified sub-
confirmed by occasional analysis of the sample gas using a
molecular sieve column (molecular sieve 5A). The flow rate of stances that GC-MS cannot qualify because of their high
gases was measured continuously using a digital manometer. molecular weight. It is measured as the residue from
Water content of gas was measured with an absorption tar solution of 2-propanol after the evaporation of the
bottle containing 10 g of calcium chloride. After filtering by alcohol, according to the “Tar Guideline: A standard
glass-fiber thimble, the gases were introduced into the bottle method for measurement of tars and particles in bio-
for 15 min during steady-state operation. mass producer gases”.22 GC-detectable tar, light tar,
2.2.2. Tar and Particles. Tar sampling was carried out represents the sum of the compounds in tar solution
using the sampling train shown in Figure 4, according to the quantified by GC-FID. Gravimetric tar in the present
“Tar Guideline: A standard method for measurement of tars
and particles in biomass producer gases”.22 Quasi-isokinetic (22) Neeft, J. P. A.; Paasen, S.; Knoef, H. A. M.; Buffinga, G. J.;
sampling was performed by adjusting the sampling flow rate Zielke, U.; Sjöström, K.; Brage, C.; Hasler, P.; Simell, P. A.; Suoma-
lainen, M.; Dorrington, M. A.; Thomas, L. In Proceedings of the 12th
manually every 3 min. The particle filter was a silica-fiber European Conference and Technology Exhibition on Biomass for
thimble (25 × 90 mm, Whatman), and six impingers were used. Energy, Industry and Climate Protection, Amsterdam, 2002; ETA-
The first four (containing 2-propanol as solvent) were kept at Renewable Energies; WIP-Munich: Firenze, 2002; pp 469-472.
Effect of SV on Tar from Downdraft Gasification Energy & Fuels, Vol. 19, No. 3, 2005 1189

Table 2. Summary of the Results of Each Experiment


run (ID)
A B C D E F G
flow rate [m3/h] 3 3.3 3.6 4.3 4.7 6 6.7
run time [min] 50 50 50 35 30 25 20
input [kg]
biomass 1.46 1.32 1.66 1.29 1.28 1.50 1.25
water 0.17 0.16 0.17 0.16 0.19 0.20 0.17
O2 0.69 0.75 0.83 0.69 0.65 0.68 0.61
N2 2.27 2.47 2.74 2.26 2.14 2.24 2.02
sum 4.59 4.70 5.40 4.40 4.26 4.63 4.05
output [kg]
dry gas 3.76 3.83 4.88 4.05 3.82 4.01 3.25
water 0.44 0.54 0.47 0.39 0.47 0.57 0.52
tar 0.02 0.03 0.01 0.02 0.02 0.03 0.05
char 0.08 0.05 0.06 0.02 0.02 0.03 0.02
particle, ash trace trace trace trace trace trace trace
sum 4.30 4.45 5.43 4.48 4.33 4.64 3.83
gas volume [m3N] 3.49 3.67 4.73 3.85 3.83 4.07 3.41
gas flow rate [m3N/h] 4.19 4.41 5.68 6.60 7.66 9.78 10.24
superficial velocity [m/s] 0.30 0.32 0.41 0.48 0.55 0.71 0.74
reference temperature [°C] 671 ((84) 672 ((80) 792 ((105) 938 ((96) no data 995 ((81) 970 ((76)
equivalent ratio [-] 0.34 0.41 0.36 0.39 0.37 0.33 0.36
mass balance [-] 0.94 0.95 1.01 1.02 1.02 1.00 0.95

tar yield (3.0%) at 0.7 m/s SV in the present study can


be attributed to short residence time.
Short residence time sometimes is accompanied by
channeling, which causes the flow of gas in the gasifier
to become nonuniform.23 Channeling appears at the
combustion zone and the reduction zone of the gasifier.
At the combustion zone, oxygen gas, which decreases
tar,9 is not distributed evenly in the gasifier, resulting
in increased tar yield. At the reduction zone, the gas
tends to flow at the reactor surface as a result of the
edge effect of channeling;23 therefore, tar bypasses the
char bed where tar is cracked,17 resulting in increased
Figure 5. Effect of superficial velocity on the composition of tar yield. The change in tar composition, which is shown
gases.
in the following section, supports the idea that channels
were present.
3.4. Tar Constituents. The effect of SV on GC-
detectable tar composition was examined. The yield of
each constituent in GC-detectable tar and their relative
ratios by weight are shown in Table 3 and Figure 7,
respectively. Benzene is not usually included in tar, but
it is shown in Table 3 as a reference. Toluene, phenol,
cresol, and naphthalene were primary constituents of
the GC-detectable tar, and 1-ring aromatics and naph-
thalene accounted for more than 80% of such tar mass.
Some groups of the GC-detectable tar have specific
trends according to SV, but the main composition does
Figure 6. Effect of superficial velocity on tar yields. not show extreme change.
GC-detectable tar can be classified by the structural
study was corrected by the subtraction of the amount formula of its constituent compounds. Evans and Milne
of GC-detectable tar remaining in gravimetric tar after proposed using molecular beam mass spectrometry
the evaporation of 2-propanol. (MBMS) to systematically classify pyrolysis products as
Figure 6 shows the effect of SV on the yields of primary, secondary, and tertiary tar.25 In addition to
gravimetric tar and GC-detectable tar. The lowest that classification, tertiary tar can be subdivided into
gravimetric tar yield (0.7%) and the highest (3.0%) were alkyl tertiary tar and condensed tertiary tar, with the
obtained at SV of 0.4 and 0.7 m/s, respectively. The former including alkyl derivatives of aromatics such as
highest GC-detectable tar yield (1.5%) was also obtained toluene and methylnaphthalene and the latter being
at 0.7 m/s. Reed et al. examined the effect of SV in the PAHs without substituents such as naphthalene,
region of 0.05-0.44 m/s on tar content, and reported acenaphthylene, and anthracene.2,24 Oxygenates (phe-
that the lowest tar concentration was obtained at 0.44 nol, cresols, and benzofuran) are known to form by the
m/s.18 This result was consistent with our results.
Higher SV leads to higher temperature, which has (23) Tarhan, S. Energy Sources 2003, 25, 1183-1191.
the positive effect of increasing the conversion of tar6-12 (24) Evans, R. J.; Milne, T. A. Energy Fuels 1987, 1, 123-137.
(25) Evans, R. J.; Milne, T. A. In Developments in Thermochemical
but the negative effect of reducing the conversion of tar Biomass Conversion; Blackie Academic and Professional: London,
by shortening the residence time.15,16 Hence, the high 1997; Vol. 2, pp 803-816.
1190 Energy & Fuels, Vol. 19, No. 3, 2005 Yamazaki et al.

Figure 7. Relative ratio by weight of each constituent of tar with respect to superficial velocity.

Table 3. Yields of Each Constituent of Tar with Respect


to Superficial Velocity
superficial velocity [m/ s]
compound [g/kg-dry biomass] 0.30 0.32 0.41 0.48 0.55 0.71 0.74
benzenea 3.21 3.65 5.80 3.35 6.07 5.35 7.18
toluene 1.17 1.41 1.84 0.98 1.84 1.63 2.24
ethyl benzene 0.21 0.21 0.15 0.10 0.20 0.16 0.29
p-xylene 0.31 0.37 0.39 0.22 0.41 0.35 0.51
styrene 0.50 0.56 0.74 0.39 0.74 0.69 1.01
o-xylene 0.05 0.13 0.11 0.06 0.10 0.10 0.16
phenol 1.13 2.11 1.14 0.88 1.72 1.58 2.87
benzofuran 0.28 0.48 0.32 0.14 0.36 0.36 0.48
o-cresol 0.37 0.57 0.27 0.28 0.46 0.39 0.65
indene 0.40 0.34 0.60 0.36 0.64 0.49 0.89
m- or p-cresol 0.84 1.38 0.70 0.67 1.25 1.13 1.77 Figure 8. Effect of superficial velocity on the yields of
naphthalene 0.77 1.02 1.27 0.85 1.60 1.16 1.74 oxygenates and condensed tertiary tar.
1-methyl naphthalene 0.20 0.27 0.21 0.14 0.28 0.20 0.34 Ståhlberg reported that the yields of naphthalene and
2-methyl naphthalene 0.13 0.10 0.13 0.08 0.17 0.12 0.21
biphenyl 0.04 0.06 0.06 0.04 0.08 0.08 0.11
phenanthrene, or condensed tertiary tar, decreased with
acenaphthylene 0.16 0.27 0.24 0.18 0.36 0.39 0.48 an increase in freeboard temperature of the fluidized
acenaphthene 0.04 0.06 0.04 0.04 0.06 0.07 0.09 bed, they also showed that naphthalene was stable at
fluorene 0.03 0.07 0.06 0.05 0.09 0.11 0.13 high temperature and phenol was subject to decomposi-
anthracene 0.05 0.09 0.09 0.08 0.15 0.17 0.20 tion.6 The trend of changes in yields of oxygenates and
phenanthrene 0.02 0.04 0.03 0.03 0.05 0.06 0.07
fluoranthene 0.03 0.04 0.04 0.04 0.06 0.07 0.10 tertiary condensed tar obtained in the present study can
pyrene 0.03 0.04 0.04 0.04 0.06 0.07 0.10 be explained as follows: at low SV (0.3 m/s), the
benzo[a]anthracene n.d. n.d. 0.01 n.d. n.d. 0.02 0.07 temperature of the gasifier is too low to promote the
chrysene n.d. n.d. 0.01 n.d. n.d. 0.02 0.07 conversion of oxygenates to condensed tertiary tar,
benzo[b]fluoranthene n.d. 0.03 n.d. n.d. n.d. n.d. 0.09
benzo[k]fluoranthene n.d. n.d. 0.02 n.d. n.d. 0.01 0.08
resulting in high yield of oxygenates and low yield of
benzo[a]pyrene n.d. n.d. 0.04 n.d. n.d. 0.02 0.12 condensed tertiary tar. The gasifier temperature in-
benzo[g,h,I]perylene n.d. n.d. n.d. n.d. n.d. n.d. 0.10 creases with an increase in SV, which accelerates the
a Benzene is not included in tar; however, it is tabulated as a conversion of oxygenates to condensed tertiary tar.
reference substance. Consequently, the yield of oxygenates decreases and
that of condensed tertiary tar increases between 0.4 and
cracking of lignin-derived materials and are classified 0.5 m/s SV. In the region of SV of 0.5-0.7 m/s, both
as secondary tar.25 oxygenates and condensed tertiary tar increase. This
The effect of SV on the change in the yields of result is inconsistent with the expected results. It was
oxygenates and condensed tertiary tar is shown in expected that there would be an inverse correlation
Figure 8. The yield of oxygenates had a minimum at between oxygenates and condensed tertiary tar. This
0.4-0.5 m/s SV, while that of condensed tertiary tar contradiction can be due to channeling, which increases
increased with increasing SV. According to the pyrolysis with SV.23 As mentioned above, channeling leads to
pathway suggested by Evans and Milne, oxygenates are increased amounts of tar that includes oxygenates at
converted to tertiary tar at high pyrolysis severity.25 the combustion zone. When channeling occurs, oxygen-
Brage et al. proposed that phenols are intermediates ates undergo one of two processes depending on their
in the formation of naphthalene.26 A study of tar passage through the reduction zone. One portion of the
distribution using MBMS showed that secondary tar oxygenates is converted to condensed tertiary tar by
and tertiary alkyl tar were maximum at the cracking passage through the char bed at high temperature. The
temperature of approximately 800 °C and 900 °C, other portion of the oxygenates is not substantially
respectively, and that condensed tertiary tar was the converted by bypass of the char bed. Therefore, con-
primary component at cracking temperatures exceeding densed tertiary tar increased with increases in oxygen-
900 °C.24 Results from other studies10,12 were consistent ates at high SV.
with the trend described above. Although Kurkela and Figure 9 shows the composition of condensed tertiary
tar at different SVs. The molar ratio of 2-ring aromatics
(26) Brage, C.; Yu, Q.; Sjöström, K. Fuel 1996, 75, 213-219. in condensed tertiary tar was the lowest (80%) at 0.7m/s
Effect of SV on Tar from Downdraft Gasification Energy & Fuels, Vol. 19, No. 3, 2005 1191

Figure 11. Effect of superficial velocity on particle yields.

The collected particles indicate the sum of soot, frag-


Figure 9. Molar ratios of 2-ring, 3-ring, and 4-ring aromatics ments of char, and ash particles.
in condensed tertiary tar at different superficial velocities. Figure 11 shows the effect of superficial velocity on
particle yield. The highest particle yield was obtained
at 0.74 m/s and the lowest at 0.3 m/s. This result is
explained in two ways. (1) Higher SV leads to greater
linear velocity, which causes more fragments of char to
be conveyed from the char bed, and which in turn causes
the particle yield to become higher. (2) Higher SV leads
to higher molar ratios of 3-ring and 4-ring aromatics
(Figure 9). The increase in the molecular weight of
PAHs leads to soot formation via surface growth and
agglomeration;31 therefore, higher SV leads to higher
soot yield. However each constituent’s contribution to
particle yield is unknown. To estimate yields of soot,
char, and ash in particles, further analysis of particles
must be done.

Figure 10. SEM images of the agglomerate of submicrometer 4. Conclusions


particles (left) and the coarse particles collected on the filter
(right). An experimental investigation was conducted on the
effect of superficial velocity (SV) on tar, particles, and
SV, although their yields increased with SV. Kinoshita gases. The results allow for the following conclusions:
et al. and Yu et al. showed that the proportions of 1-ring • The lowest gravimetric tar yield of 0.7% was
and 2-ring aromatics in tar decreased with increasing obtained at 0.4 m/s SV, and the highest was obtained
temperature, whereas those of 3-ring and 4-ring aro- at 0.7 m/s. High tar yields at high SV are attributed to
matics increased.7,10 Kinoshita el al. also showed that short residence time and channeling.
the yields of 1-ring and 2-ring aromatics decreased with • In the region of 0.4-0.6 m/s SV, which gave low tar
increasing residence time, while those of 3-ring and yield, the gas composition was suitable for operation of
4-ring aromatics increased.7 McGrath et al. also re- an IC engine.
ported that higher thermal cracking temperature and • Toluene, phenol, cresol, and naphthalene were
longer residence time favored the formation of 3-ring primary constituents of the GC-detectable tar. One-ring
and 4-ring aromatics.27 In the present study, the aromatics and naphthalene accounted for more than
changes in the composition of condensed tertiary tar can 80% of such tar. The main composition of the GC-
be explained by the influence of temperature: since at detectable tar did not show extreme change according
higher SV a portion of the tar passed through the to SV.
higher-temperature zone, which favors heavier PAH, • The yield of oxygenates was at the minimum
the molar ratios of 3-ring and 4-ring aromatics increased between 0.4 and 0.5 m/s SV and at the maximum at
with increases in SV. 0.7 m/s SV. The yield of condensed tertiary tar increased
3.5. Particles. Figure 10 shows SEM images of the with increasing SV.
filter after extraction. Agglomerate of submicrometer • Particle yield increased with increasing SV.
particles, which may be identified as soot, was observed.
Acknowledgment. We are grateful to Ms. Hiroko
In addition to the agglomerate, coarse particles with
Tsushima (Center for Instrumental Analysis, Hokkaido
diameters on the order of micrometers were observed,
University) for ultimate analysis of Todo fir chips.
and each particle seemed to be a fragment of char. It is
well-known that ash particles composed of inorganic EF0497210
compounds are produced from biomass gasification.28-30
(29) De Bari, I.; Barisano, D.; Cardinale, M.; Matera, D.; Nanna,
F.; Viggiano, D. Energy Fuels 2000, 14, 889-898.
(27) McGrath, T.; Sharma, R.; Hajaligol, M. Fuel 2001, 80, 1787- (30) Hindsgaul, C.; Schramm, J.; Gratz, L.; Henriksen, U.; Bentzen,
1797. J. D. Bioresour. Technol. 2000, 73, 147-155.
(28) Turn, S. Q.; Kinoshita, C. M.; Ishimura, D. M.; Zhou, J. Fuel (31) Amann, C. A.; Siegla, D. C. Aerosol Sci. Technol. 1982, 1, 73-
1998, 77, 135-146. 101.

You might also like