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Lu Ding, Kunio Yoshikawa, Minoru Fukuhara, Yuto Kowata, Shunsuke Nakamura, Dai Xin, Li Muhan
Lu Ding, Kunio Yoshikawa, Minoru Fukuhara, Yuto Kowata, Shunsuke Nakamura, Dai Xin, Li Muhan
Fuel
journal homepage: www.elsevier.com/locate/fuel
A R T I C L E I N F O A B S T R A C T
Keywords: Ultra-small biomass gasification and power generation systems are a promising technology for disaster areas in
Carbonized pellets developed countries and non-electrified rural areas of developing countries. The gasification characteristics of
Carbonized briquettes carbonized wood pellets and carbonized wood briquettes without or with 1 wt% sea salt were tested in a pilot-
Updraft fixed bed gasifiers scale updraft fixed-bed gasifier. The results showed that the carbon balance during gasification was easily
Tar removal
achieved, and most of the chlorine in the carbonized briquettes with sea salt remained in the residual char and
Gas engine
fly ash after gasification. Inorganic chlorine in the solid fuel was transformed into organic chlorine combined
with carbon matrix after heat treatment in the gasifier. Syngas with a low heating value higher than 4 MJ·m−3
could be continuously obtained when the system reached a stable condition, which enabled power generation
using a gas engine. A combination of several secondary tar removal processes was adopted for the syngas
purification. The tar content in the syngas after the gas cleaning for 425 °C-carbonized pellet, 425 °C-carbonized
briquette, 475 °C-carbonized briquette, and 475 °C-carbonized briquette with sea salt was 0.98, 0.26, 1.4, and
0.2 g·Nm−3, respectively. During the stable stage, 425 °C-carbonized pellet showed the highest cold gas effi-
ciency (CGE) of 45.6% and carbon conversion efficiency (CCE) of 57.8%, respectively, with an equivalence ratio
(ER) of 0.24. A lower carbonization temperature showed a higher CGE and CCE. The residual char and fly ash
after gasification could be considered for reuse as feedstock to further improve the overall process efficiency. The
maximum output power was 23 kW at an air flow rate of 40 Nm3/h during the gasification of carbonized pellets,
and the corresponding overall power generation efficiency of the engine using the syngas was about 27.8%. For
475 °C carbonized briquette, the maximum output power was 18 kW at an air flow rate of 40 Nm3/h, and the
corresponding overall power generation efficiency of the engine using the syngas was about 25.5%.
⁎
Corresponding author.
E-mail address: dinglu101@163.com (L. Ding).
https://doi.org/10.1016/j.fuel.2018.01.080
Received 20 October 2017; Received in revised form 18 January 2018; Accepted 22 January 2018
0016-2361/ © 2018 Elsevier Ltd. All rights reserved.
L. Ding et al. Fuel 220 (2018) 210–219
Fig. 1. The photo and schematic diagram for different reaction zones in the updraft gasifier.
Raw biomass always contains a high water content (20–60 wt%) [25]. The one-batch capacity of the carbonization system was about
and will produce syngas with high tar concentrations when directly 80–100 kg of dry wood, and the size of wood block used was usually
applied in gasification. It is reported that the tar content in syngas about 15 cm × 8 cm × 5 cm. It was noted that most of the wood block
should be lower than 0.1 g·Nm−3 for the safe operation of internal remained uncarbonized over the torrefaction temperature range. The
combustion engines [11,12]. Using fresh biomass as gasification feed- uncarbonized wood and half-carbonized wood char were very difficult
stock increases the load on a syngas purification system. In order to to crush when the carbonization temperature was lower than 400 °C;
overcome unfavorable factors caused by water and tar issues, some therefore, the wood block was carbonized within 400–500 °C to enable
researchers have explored the gasification application using torrefied or crushing and densification.
carbonized biomass [13–16]. Kuo et al. simulated the gasification As the carbonized wood char was in a low energy density and loose
performances of raw and torrefied bamboo in a downdraft fixed-bed state, unfavorable situations such as hot-points or channeling occurred
gasifier. The effects of the equivalence ratio (ER) and steam supply ratio easily when fresh char was fed directly into the gasifier as bed material.
on the syngas yield and quality, CGE, and CCE were evaluated, and the Therefore, high-strength carbonized pellets or carbonized briquettes
optimal feed conditions for gasification were predicted [13]. Deng et al. were prepared as gasification feedstock using a pelletizer or briquetter
torrefied rice straw and rape stalks for their co-gasification of coal. They so as to ensure stable operation of the gasifier. An updraft fixed-bed
mention that the properties of the torrefied agricultural residues are gasifier may be the most appropriate fixed-bed type to realize the de-
closer to those of coal, so torrefaction is a promising method for co- sired portability and distributed character. This is because the tem-
gasification [14]. Actually, the hydrophobicity and uniform characters perature of syngas from the outlet of an updraft fixed-bed gasifier is
of the biomass can also be significantly improved after the torrefaction much lower than that of the downdraft type [26], which could sig-
or carbonization pretreatments [17–19]. These two processes reduce nificantly reduce the size of the cooling system. Also, the operation of
the O/C ratio and improve the energy density of the biomass, which is an updraft fixed-bed gasifier is much easier than other types of gasifiers.
favorable for the thermal application of the solid fuels [20]. Compared So far, most small-scale and distributed biomass gasification power
with carbonization at temperatures higher than 400 °C, biomass torre- generation systems are based on the utilization of raw biomass or
faction always finishes within the lower temperature range of charcoal [27–32]. To the best of our knowledge, there are no published
200–350 °C [21,22]. Therefore, more volatile matter remained in the papers on pilot-scale gasification based on carbonized biomass pellets/
torrefaction char than in the carbonization char. This led to a higher briquettes. In our study, biomass was first carbonized and then densi-
syngas production rate by using the torrefaction char as gasification fied into carbonized pellets/briquettes for the corresponding gasifica-
feedstock, whereas the corresponding tar content in the syngas would tion process. In certain areas of Japan, waste wood resources are
also increase by using torrefaction char produced at a lower thermal sometimes soaked in seawater after a tsunami, so it is necessary to
treatment temperature. explore the effects of the salt from seawater on biomass gasification
So far, most of the devices for torrefaction or carbonization are performance. Moreover, the release characteristic of chlorine is also a
mainly based on electrical heating [23,24,19]. In a commercial che- key point, considering the associated erosion issues during gasification.
mical plant, there is a great amount of hot exhaust gas, which can be Therefore, besides carbonized pellets/briquettes, carbonized briquettes
utilized to reduce the energy consumed in torrefaction or carbonization. mixed with 1 wt% sea salt were also investigated for gasification. The
However, electrical heating or the utilization of waste heat from a big cold gas efficiency, carbon conversion and balance, and residual char
factory is very difficult to achieve in a power-starved disaster zone or characteristics were evaluated. Also, the tar removal efficiency using
remote area. In our system, the carbonization furnace was based on several physical separation devices was also discussed considering the
non-electric heating, wherein the entire system was heated using the requirements of the gas engine. Finally, the performance of the gas
combustion heat from volatile matter in the waste wood, which might engine was reported.
be the most appropriate way to achieve portability in the open field
211
L. Ding et al. Fuel 220 (2018) 210–219
The chlorine content in solid and tar samples was measured using an
Table 2
The characteristic data of cedar wood and the corresponding carbonized pellet/briquette.
Sample Proximate analysis/d, wt.% Ultimate analysis/d, wt.% LHV/MJ·kg−1 Chemical formula
VM FC Ash C H N O
Cedar wood 72.95 26.83 0.21 36.02 4.41 0.10 59.18 18.8 CH1.469O1.232N0.002
425 °C-Carbonized pellet 36.68 62.93 0.39 79.05 3.70 0.27 16.59 32.7 CH0.562O0.157N0.003
425 °C-Carbonized briquette 34.03 65.54 0.43 79.06 3.61 0.30 16.60 30.6 CH0.548O0.157N0.003
475 °C-Carbonized briquette 27.13 70.37 2.50 82.81 2.74 0.35 11.51 34.3 CH0.397O0.104N0.004
475 °C-carbonized briquette with salt 23.38 73.05 3.56 85.56 2.88 0.30 7.61 29.0 CH0.404O0.067N0.003
Note: VM-volatile matter; FC-fixed carbon; d-dry basis; LHV denotes the low heating value of wood.
212
L. Ding et al. Fuel 220 (2018) 210–219
Table 3
The summarization of gasification data of carbonized pellets/briquettes.
Material balance 425 °C-carbonized briquette 475 °C-carbonized briquette 475 °C-carbonized briquette with sea salt 425 °C-Carbonized pellet
Note: The consumed carbon = Total carbon in the feedstock-the residual carbon remained in the residual char and fly ash after gasification.
observed
curved-fitted
2p3/2
XPS intensity
2p1/2 2p3/2
2p1/2 2p3/2
Peak Bingding energy/eV Compounds Mole fraction/% Peak Bingding energy/eV Compounds Mole fraction/%
C l 2p 198.6 NaCl,KCl 74.74 Cl 2p 198.5 NaCl,KCl 69.28
C l 2p 200.8 C-Cl 25.26 Cl 2p 200 C-Cl 30.72
observed
curved-fitted
Bottom residual char observed
XPS intensity
of salt-briquette curved-fitted
2p3/2
XPS intensity
2p1/2
2p3/2
2p3/2
2p1/2 2p1/2
213
L. Ding et al. Fuel 220 (2018) 210–219
70 5.5
Gas compositions/vol.%
50 5.0
H2
O2
40 N2
CH4
CO 4.5
30
CO2
20
4.0
10
3.57
0
3.5
1.0 1.5 2.0 2.5 3.0 3.5 1.0 1.5 2.0 2.5 3.0 3.5
Reaction time/h Reaction time/h
o
(a) 425 C-carbonized pellet
3
Low heating value of syngas/MJ/m
70 5.5
60
H2 5.04
Gas compositions/vol.%
O2 5.0 4.90
50 N2
CH4 4.69
40 CO 4.54 4.54
CO2 4.54
4.5
30 4.25 4.50
20 3.97
4.0
3.77
10
0 3.5
0 1 2 3 4 5 0 1 2 3 4 5
Reaction time/h Reaction time/h
70 5.5
5.21
3
Low heating value of syngas/MJ/m
4.95 4.94
60 5.0
H2
Gas compositions/vol.%
O2
50 4.5 4.30
N2
CH4 4.19 4.33 4.02
40 4.0 3.84
CO
CO2
30 3.5
20 3.0 3.02
10 2.5 2.31
2.06
0 2.0
1 2 3 4 5 6 7 1 2 3 4 5 6 7
Reaction time/h Reaction time/h
o
(c) 475 C- carbonized briquette
70 5.5
3
Low heating value of syngas/MJ/m
60 5.0
H2
Gas compositions/vol.%
20 3.0
10 2.5
2.21
0 2.0
1 2 3 4 5 6 1 2 3 4 5 6
Reaction time/h Reaction time/h
(d) 475oC- carbonized briquette with sea salt
Fig. 3. Variation of compositions and low heating value of syngas with time.
Therefore, the total amount of carbon consumed in the carbonized was well demonstrated.
pellets/briquettes should have been close to the total carbon in the For the gasification of carbonized briquettes with sea salt, the
syngas. Table 3 indicates that the carbon balance during the three tests chlorine balance was also analyzed. Table 4 indicates that after
214
L. Ding et al. Fuel 220 (2018) 210–219
Table 5 gasification, most of Cl still remained in the solid residual char and fly
Typical gas composition data from commercial wood and charcoal gasification in fixed ash. Some researchers found that inorganic Cl in the carbonaceous
bed gasifiers (moisture content: wood 20%, charcoal 7%) [36].
materials would change to organic Cl, which was bonded to carbon
Component H2 (%) N2 (%) CH4 (%) CO (%) CO2 (%) Heating value matrix during the heat treatment [33,35]. In order to further analyze
(MJ·m−3) the distributed forms of Cl in the solid samples, an XPS method was
adopted to evaluate the inorganic and organic Cl content; the resulting
Wood gas 12–20 50–54 2–3 17–22 9–15 5–5.9
XPS spectra are shown in Fig. 2. It was found that the mass percentages
Charcoal gas 4–10 55–65 0–2 28–32 1–3 4.5–5.6
of organic Cl in the residual char from the bottom and top layers of the
gasifier were 25.26% and 30.72%, respectively, which were much
higher than those in the carbonized briquette with sea salt (7.23%). The
inorganic chlorine released from the high-temperature combustion
215
L. Ding et al. Fuel 220 (2018) 210–219
Table 6 production during gasification and syngas with a higher heating value
The characteristics data of Nisshin salad oil. at the very beginning stage. The hydrogen content of the carbonized
materials was significantly lower when compared with that of raw
Material Viscosity (20 °C) Specific gravity Water content
biomass during gasification owing to the low volatile matter content
Nisshin salad oil 63 mpa 0.919 g·cm−3 0.02 wt% remaining in the carbonized pellets/briquettes. In any case, the low
heating value of the syngas was higher than 4 MJ·m−3 after operating
for several hours and could be continuously obtained, which enabled
60
rd
power generation using the gas engine. Compared with carbonized
nd
2 test 3 test briquettes, carbonized pellets presented a stable and high-quality
st
1 test syngas composition at an earlier stage.
50
Tar remove efficiency of oil-scrubber/%
Secondary tar removal systems were adopted in our study for syngas
th
5 test purification. The detailed methods for tar collection and analysis are
40 reported in a previous study [37]. Fig. 4(a)–(c) shows that the tar
content in the syngas from both carbonized pellets/briquettes was
much lower than the conventional value (10–150 g·Nm−3) from an
30
updraft fixed-bed gasifier. The corresponding tar removal efficiency of
475 °C-carbonized briquette was 46.2%. As the tar content in the syngas
20 after purification (1.4 g·Nm−3) of 475 °C-carbonized briquette was still
much higher than the upper limit (< 0.1 g·Nm−3) for the stable op-
th eration of internal combustion engines [37], Nisshin salad oil (a vege-
10
4 test table oil made in Japan) was supplied to the oil scrubber of the tar
cleaning system during the gasification of other feedstock. The detailed
characteristics of this oil are shown in Table 6. The corresponding tar
0 removal efficiencies of 425 °C-carbonized briquette and carbonized
4 8 12 16 20 24
pellet were 94.0% and 78.6%, respectively. It was noted that the tar
Continuous operation time/h
removal efficiency decreased significantly from 425 °C-carbonized bri-
Fig. 5. Tar remove efficiency of the oil scrubber with reaction time. quette to carbonized pellet. Actually, the tar removal efficiency of the
purification system decreased with an increase in the operating time of
zones might have been absorbed by the relatively low-temperature the gasification tests, if the secondary tar removal system was not re-
carbon matrix in the upper layer of the gasifier and changed to organic generated after a one-batch gasification test. The tar removal efficiency
chlorine bonded with carbon matrix (C-Cl). It was noted that the con- of the oil scrubber as a function of operating time after several gasifi-
tent of the organic Cl in the fly ash collected by a cyclone separator was cation tests is shown in Fig. 5. For the first three gasification tests, the
not significantly increased (8.44%). The reason might be that most of tar removal efficiency of the oil scrubber stayed at about 50%, which
the fly ash was formed as carbonized briquettes were continuously means that the oil scrubber reached the saturation point (the point at
supplied to the gasifier during the gasification process. A fine powder of which the tar removal efficiency changes little with time) after four
sea salt mixed into the briquettes or produced by briquette breakage hours of operation. For the fourth test, the oil scrubber was stopped
during the crash and carbon conversion was rapidly carried out of the when we measured the outlet tar content. This was because of a high-
gasifier by the syngas and collected by the subsequent cyclone se- pressure loss in the whole system, which led to syngas leakage from the
parator. The fly ash did not stay a significant time in the moderate- gasifier; therefore, the tar removal efficiency was much lower. For the
temperature zone of the gasifier, which led to lower conversion of in- fifth gasification test, the tar removal efficiency decreased to about
organic Cl to organic Cl. In general, the Cl content of the syngas was 40%, which meant that degradation had occurred in the performance of
very low, only 0.145 g·Nm−3, which means that even with seawater- the oil scrubber. The breakpoint (the point at which deterioration of the
soaked waste wood from a disaster area, the erosion issues on the de- oil starts and new oil or regeneration of oil is required) may have oc-
vice caused by volatilization, and the deposition of Cl might not be curred after 20 h of operation. Therefore, part of the used oil must be
significant. replaced by new oil or regenerated periodically for continuous gasifi-
cation operation [38].
We failed to analyze the tar content in the syngas after the cyclone
3.2. Syngas quality and tar removal efficiency analysis separator because the syngas sampling pipe was blocked during the
gasification of briquettes with sea salt. However, it was noted that the
Fig. 3 shows the compositions and corresponding low heating values tar concentrations in the syngas from briquettes with sea salt before the
of the syngas during the three tests. It was found that the concentrations oil scrubber and after the char bed were really much lower than those
of CO and H2 were kept almost constant after the system reached a from carbonized briquettes without sea salt: only 0.4 g·Nm−3 and
stable state, and the syngas compositions and low heating values of the 0.2 g·Nm−3, respectively. The reason for this might be that sea salt in
carbonized pellets/briquettes were similar to the results from charcoal the briquette contributed to the catalytic cracking of tar inside the
gasification, as shown in Table 5 [36]. Compared with 475 °C-carbo- gasifier. In a recent study, Umeki et al. found that alkali metal salts
nized briquette, 425 °C-carbonized briquette presents a higher H2
Table 7
Variations of ER, CCE, and CGE with different solid fuels.
Material balance 425 °C-carbonized briquette 475 °C-carbonized briquette 475 °C-carbonized briquette with sea 425 °C-Carbonized pellet
salt
216
L. Ding et al. Fuel 220 (2018) 210–219
1.0 1.0
o Residual char of
475 C-carbonized briquette o
o 475 C-carbonized briquette
475 C-carbonized briquette
0.8 0.8 Residual char of
with sea salt o
475 C-carbonized
briquette with sea salt
0.6 0.6
Conversion X
Conversion X
0.4 0.4
0.2 0.2
0.0 0.0
0 2 4 6 8 0 2 4 6 8
Time (min) Time (min)
1.0
o
Fly ash of 475 C-carbonized
briquette
o
0.8 Fly ash of 475 C-carbonized
briquette with sea salt
Conversion X
0.6
0.4
0.2
0.0
0 2 4 6 8
Time (min)
Fig. 6. The reactivity of char and gasification residues from carbonized briquette.
Cgas
contribute to tar reduction during biomass gasification [39]. CCE = × 100%
Cfuel (3)
−3
3.3. CCE and CGE analysis Note: LHVgas-The average low heating value of syngas, (MJ·Nm );
Qgas-The average flow rate of syngas, (Nm3·h−1); LHVfuel-The average
Usually, the ER is the key operating parameter for air gasification low heating value of solid fuel, (MJ·kg−1); Qfuel-The average feed rate
Table 9
The proximate and ultimate analysis of residual char and fly ash after gasification.
VM FC Ash C H N O
Residual char of 475 °C-carbonized briquette 20.21 78.60 1.21 85.34 3.33 0.21 9.89
Residual char of 475 °C-carbonized briquette with sea salt 12.18 86.07 1.75 88.19 1.94 0.40 7.66
Fly ash of 475 °C-carbonized briquette 16.26 74.43 9.31 79.65 1.00 0.42 9.42
Fly ash of 475 °C-carbonized briquette with sea salt 16.62 78.68 4.70 85.20 1.03 0.53 8.33
217
L. Ding et al. Fuel 220 (2018) 210–219
9
o
Fly ash of Fly ash of 475 C-carbonized
o 6 briquette with sea salt
475 C-carbonized briquette
3
2
0 0
1 10 100 1000 1 10 100 1000
Fig. 7. The particle size distribution of fly ash from carbonized briquette with or without sea salt.
of solid fuel, (kg·h−1); Cgas-Total carbon amount in the syngas, (kg); fly ash was lower than 10%, which would not significantly decrease the
Cfuel-Total carbon amount in solid fuel, (kg). gasification efficiency when they were reused as fuels. It was noted that
Although there were some differences in the volatile matter and the pelletizing/briquetting processes would be optimized by adding a
carbon contents for the three gasification feedstocks, Table 7 indicates certain amount of fly ash into the new char for densification. This was
that the CGE had a positive correlation with the CCE. It is interesting to because the particles of fly ash were in the small size range, as shown in
find that the carbonized briquettes produced at a lower temperature Fig. 7 (analyzed using a Hydro 2000-MU particle size analyzer);
displayed a higher CCE and CGE. Also, carbonized pellets displayed a therefore, the contact area of char particles from fly ash was large,
higher CCE and CGE compared with carbonized briquettes owing to the which was favorable for homogenous mixing with binders and bio-oil.
high reactivity of carbonized pellets. The cylindrical pellets had the
diameter of 3 mm and length of 1–2 cm, and the spheroidal briquette 3.5. Analysis of power generation
had an equatorial radius of 1.5 cm and polar radius of 1 cm. Therefore,
the carbonized pellets would have experienced a much lower diffusion The overall efficiency of the gas engine during the stable operation
effect during the gasification process. However, the CGE and CCE in our stage was evaluated according to the following equations:
study were lower than those in the gasification of raw wood. Gunar-
Qgas
athne et al. found that the CGE at ER = 0.2 was 75.9% during wood SGC =
pellet gasification in a pilot-scale updraft gasifier [41]. Pedroso et al. (Vout ) × I (5)
also obtained a relatively high CGE (67%) during wood chip gasifica-
3.6
tion in a bottom-feed updraft gasifier [42]. The relatively low CGE in ηE = ⎛ ⎜
⎞·100[%] ⎟
this study was due to the utilization of carbonized pellets/briquettes ⎝ (LHVG ) × SGC ⎠ (6)
with a much lower volatile content. Moreover, a proper increase of ER
Note: Vout-output voltage of electric generator (V); I-output current
was favorable for increasing the CGE and CCE on the premise that the
of electric generator (A); Qgas-gas average flow (Nm3 h−1); LHVG-
syngas quality was not affected and the operating temperature was
heating value of the producer gas (MJ Nm−3); SGC- specific gas con-
lower than the upper limit value of the gasifier. Therefore, we will
sumption (Nm3·kW−1·h−1); ηE -Overall efficiency of engine.
continuously operate the whole system at different ER values in the
After calculation, the average low heating value of the syngas
future to determine the best conditions for improving the utilization
during the stable power generation stage was 5.32 MJ/m3. In addition,
efficiency of carbonized pellets/briquettes. In addition, the discharged
the maximum output power was 23 kW at an air flow rate of 40Nm3/h
residual char and fly ash could be reused as gasification feedstock (char
during the gasification of carbonized pellets, and the corresponding
recycling) so as to further improve the overall process efficiency.
overall efficiency of the gas engine using the syngas was about 27.8%.
For 475 °C-carbonized briquette, the average low heating value of the
3.4. Characteristics of residual char and fly ash syngas during the stable stage was 4.33 MJ/m3, the maximum output
power was 18 kW at an air flow rate of 40 Nm3/h, and the corre-
The reactivity of char and gasification residues from carbonized sponding overall efficiency of the gas engine using the syngas was about
briquettes with and without sea salt were compared to consider the 25.5%. Therefore, carbonized pellets presented a higher overall effi-
reuse of residual char and fly ash. The reactivity index [43] of solid fuel ciency of the gas engine than carbonized briquettes owing to the higher
was taken as the quantitative index system of the reactivity. average low heating value of the syngas obtained from the gasification
process.
R 0.5 = 0.5/ t0.5 (4)
where R0.5 is the reactivity index of residual coke (min−1), t0.5 is the 4. Conclusion
time required to reach a fixed carbon conversion of 50 wt% (min).
Fig. 6 and Table 8 indicate that the reactivity of carbonized bri- The gasification characteristics of carbonized pellets/briquettes
quette with sea salt was somewhat higher than that of carbonized bri- were studied using a pilot-scale updraft fixed-bed gasifier. The gasifi-
quette without salt due to the latent catalytic effects of NaCl. Mean- cation system reached a stable state after several hours of operation,
while, the reactivities of the residual char or fly ash of carbonized and almost constant CO and H2 contents could be supplied in the syngas
briquette with and without sea salt were very similar and still high. for power generation. Meanwhile, the tar concentration in the syngas
Moreover, Table 9 shows that the ash content of the residual char and was lower than 5 g·Nm−3 at the outlet of the gasifier. Several
218
L. Ding et al. Fuel 220 (2018) 210–219
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