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Article history: In the present study, we attempted to promote the steam gasication of coal char at low temperatures
Received 25 June 2012 (below 1173 K). A novel circulating uidized bed gasication reactor was developed. This reactor consisted
Received in revised form 19 September 2012 of three units: a pyrolyzer, a gasier, and a combustor. The main feature of the reactor was that the pyrolyzer
Accepted 20 September 2012
was physically isolated from the gasier. Such physical isolation of the pyrolysis zone (pyrolyzer) from the
Available online 11 October 2012
char gasication zone (gasier) in the reactor can prevent char gasication from being inhibited by contact
Keywords:
of the char with hydrogen gas or the tar vapor formed by pyrolysis. Therefore, char gasication was certainly
Coal promoted by the physical isolation of the pyrolyzer from the gasier in comparison with the conventional
Gasication gasication reactor, in which pyrolysis and subsequent char gasication proceed in one unit.
Fluidized bed 2012 Elsevier B.V. All rights reserved.
Inhibition
1. Introduction prevent the direct contact of the char in the gasier with volatiles
including the hydrogen gas formed by pyrolysis. However, so far, no
There have been many types of coal gasication systems using attempt to isolate the pyrolyzer from the gasier using a continuous
entrained bed, xed bed, uidized bed, and so on. The dual-bed gasi- reactor has been reported. In the present study, we developed a
cation system based on uidized bed technology has lately attracted novel continuous gasication reactor in which the inhibition of char
attention [15]. The dual-bed system essentially consists of two units: gasication by volatiles including hydrogen gas is minimized, and
an endothermic gasication reactor (gasier) and an exothermic veried the promotion of char gasication by the novel reactor.
combustion reactor (combustor). Because of this conguration, the
direct production of middle-calorie gas by the introduction of steam 2. Experimental
into the gasier is plausible, and this could provide a great advantage
over other gasication techniques. On the other hand, there are some 2.1. Sample
issues for the realization of the dual-bed system. A smaller amount of
char should be combusted in the combustor in order to increase the Indonesian low-rank coal, Adaro coal, was used as the coal sample.
efciency of the dual-bed system while maintaining the heat balance The sample properties are listed in Table 1. The size of the raw coal
between the gasier and combustor. In other words, the promotion was in the range 0.51.0 mm. The sample was dried at 353 K under
of char gasication at lower temperatures is essential; otherwise, vacuum for 8 h prior to use.
the gasier would need to be huge to extend the residence time of
the char. It is well known that the steam gasication of coal char is 2.2. Procedure
quite slow. Therefore, the promotion of char gasication is a critical
point in the design of the dual-bed system. One reason for the slow Fig. 2 shows a schematic diagram of the circulating uidized bed
gasication is the inhibition of char gasication by volatiles, including gasication reactor developed here. The three bubbling uidized
the hydrogen gas formed by pyrolysis and/or the gasication of char beds (pyrolyzer, gasier, and combustor) were interconnected. The
itself [6,7]. These reports [6,7] suggest that coal gasication can be raw coal was fed into the pyrolyzer at a rate of 0.8 g/min to evacuate
promoted by minimizing the inhibition of char gasication. Fig. 1 volatiles including hydrogen gas, and the char was circulated with the
shows the concept of the coal gasication system for promoting bed material to be gasied with steam in the gasier. The partial pres-
char gasication. The isolation of the pyrolysis zone (pyrolyzer) sure of steam in the gasier was about 20 kPa. Then, the resulting
from the gasication zone (gasier) in the gasication process can char was circulated with the bed material to the combustor to be
combusted. Non-porous silica sand or porous -alumina particles of
Corresponding author. Tel.: +81 29 861 8019; fax: +81 29 861 8209. 75150 m in diameter were used as the bed material. The pore vol-
E-mail address: koichi-matsuoka@aist.go.jp (K. Matsuoka). ume and BrunauerEmmettTeller (BET) specic surface area of the
0378-3820/$ see front matter 2012 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.fuproc.2012.09.036
44 K. Matsuoka et al. / Fuel Processing Technology 109 (2013) 4348
gas a 100
H2 yield
40
20
riser
gas
0
950 1000 1050 1100 1150 1200
Pyrolyzer temperature [K]
Coal(Isolated case) b
combustor Coal gas 20
air Coal
(Non-isolated case)
Coal 10
N2
downer 5
gasifier
0
950 1000 1050 1100 1150 1200
Pyrolyzer temperature [K]
steam
Fig. 3. (a) Yields of carbon-containing gas and H2 gas volatilized from pyrolyzer at
Fig. 2. Schematic diagram of pyrolyzergasier isolated circulating uidized bed gasi- different temperatures and (b) decrease in partial pressure of H2 in the gasier by
cation system. the evacuation of H2 from the pyrolyzer.
char and/or coke gasication by the isolation of the pyrolyzer from the important point in this gure is that in the isolated case, a higher
gasier was not effectively minimized at a low gasier temperature yield of combustible gases (apart from CO2) can be achieved than in
(973 K). On the contrary, at higher gasier temperatures (Fig. 5b the non-isolated case.
and c), the difference in the total product gas yield between the
non-isolated and isolated cases was substantial. For example, at the 3.2. Effect of bed material on gas yield
temperature of gasier/pyrolyzer of 1073 K, the gas yield from
the pyrolyzer was almost the same as that from the gasier in the Fig. 7 represents the product gas yields during pyrolysis or gasi-
non-isolated case. This suggests that the extra-gasication of the cation under different gasier temperatures using different bed mate-
char and/or coke would proceed in the pyrolyzer, which is likely in- rials. The product gas yields in the non-isolated case are shown in this
duced by the steam generated from the pyrolysis of the coal fed. gure to determine the role of the bed material on gas formation in
Furthermore, char and/or coke gasication proceeded through sup-
pression of the contact of char and/or coke with volatiles including 100
Carbon yield into product gas
hydrogen gas in the gasier. Because of the above two effects, gasi- Isolated
cation of char and/or coke would be promoted as observed in
[mol/100mol-C in coal]
80 Non-isolated
Fig. 5b and c.
Fig. 6 shows the product gas distribution in the non-isolated and
isolated cases at gasier temperatures of 973 K (a) and 1073 K (b) 60
under different pyrolysis temperatures. As shown in Fig. 6a, when
the pyrolyzer temperature was higher than that of the gasier, the
40
total product gas yield (especially H2 and CO gas yields) was in-
creased by the isolation. Char and/or coke gasication was not pro-
moted by this isolation when the pyrolyzer temperature was higher 20
than that of the gasier (Fig. 5a), so the increase in the amounts of
these gases (H2 and CO) resulted mainly from the enhancement of
0
pyrolysis at higher temperatures [14]. On the other hand, in Fig. 6b, 950 1000 1050 1100 1150 1200
the difference in the total product gas yield between the isolated
Gasifier temperature [K]
and non-isolated cases was mainly due to H2, CO, and CO2. This sug-
gests that char and/or coke gasication and the subsequent water Fig. 4. Total yield of product gas from pyrolyzer and gasier in non-isolated or isolated
gas shift reaction were enhanced in the isolated case. Another case at different gasier temperatures.
46 K. Matsuoka et al. / Fuel Processing Technology 109 (2013) 4348
a 100
by the alumina to form coke. The residence time of the coke in the
gasier was similar to that of the char particles. The coke can be gas-
Gas yield [mol/100mol-C in coal]
Gasifier temp. ied with steam in addition to the char; this is the main reason for the
80 difference in gas yield when silica sand or alumina is used as the bed
material.
Next, the effect of the isolation of the pyrolyzer from the gasier
60 on the product gas yield was examined with the different bed mate-
rials. The char conversion in the silica sand case is plotted against gas-
40 ier temperature in Fig. 8a, while the conversion of char + coke in the
Non-isolated Gasification alumina case is shown in Fig. 8b. The conversion of char and coke in
the alumina case was higher than in the silica sand case. If the coke
20 reactivity is the same as that of char, conversion of char + coke in
the isolated case (Fig. 8b) would be same as that of char (Fig. 8a).
Pyrolysis
Comparing Fig. 8a and b, conversion of char + coke was higher than
0
900 950 1000 1050 1100 1150 1200 that of char only. This result suggests that the reactivity of coke was
higher than that of char. In our previous study [15], the steam gasi-
Pyrolyzer temperature [K]
cation of char and coke on the alumina prepared by pyrolysis of
woody biomass sawdust was examined kinetically. Those results
b showed that the reactivity of biomass coke was higher than that of
100
char, because the structure of the coke on the alumina was not devel-
oped. The results observed in Fig. 8 are consistent with our previous
Gas yield [mol/100mol-C in coal]
80 Gasifier temp. reports [15], which suggests that the structure of Adaro coke is not
developed in comparison with that of char. The extent of the promo-
60
tion of char/coke gasication by isolation (difference in conversion
between isolated and non-isolated cases) in the alumina case was
Non-isolated somewhat higher than that in the silica sand case. Though not
40 shown in Fig. 3b, the decrease in H2 partial pressure in the gasier
in the isolated case with the alumina bed material was similar to
Gasification that in the silica sand case. As stated above, the alumina can capture
20
the tar rapidly. This rapid capture means that the concentration of
Pyrolysis
tar in the bed can be decreased, and gasication inhibition by the
0 tar can be suppressed by the alumina. Although the details have
900 950 1000 1050 1100 1150 1200 not yet been claried quantitatively, as Bayarsaikhan et al. [7] and
Pyrolyzer temperature [K] Kajitani et al. [17] suggested, tar is also a critical factor in the inhibi-
tion of the gasication of char and/or coke.
c 100
3.3. Kinetic analysis
Gas yield [mol/100mol-C in coal]
CO2
CO
CH4
C2H4
a b H2
CH4
1123 C2H4 1123
H2
Isolated
Isolated
1023 1073
973 973
Non-isolated Non-isolated
0 20 40 60 80 100 120 140 0 20 40 60 80 100 120 140
Yield [mol/100mol-C in coal] Yield [mol/100mol-C in coal]
Fig. 6. Product gas distribution in non-isolated case or isolated case at gasier temperatures of 973 K (a) and 1073 K (b) under different pyrolyzer temperatures. In non-isolated
case, gasier temperature was the same as that of pyrolyzer.
addition to that of hydrogen gas, it can be said that the extent of the pro-
motion of char gasication observed in Fig. 8a was appropriate. Detailed 50
kinetic analyses of coke as well as char under different temperatures on
the basis of the LH mechanism will be presented for a quantitative dis- 40
cussion of the isolation effect in another paper.
We have experimentally demonstrated the concept of isolation of 30
pyrolyzer from gasier in the present system. However, cracking of
the tar evolved from the pyrolyzer is still an important issue that 20
needs to be further investigated. Recently, Matsuhara et al. [18]
reported that the tar can be completely cracked by the coal char. In
10
the present system, the char can be used as a tar cracker by optimiz-
ing the operating conditions. If the extent of the char combustion is
0
controlled, the char can be recycled to the pyrolyzer from the com- 950 1000 1050 1100 1150 1200
bustor, where it can be used to crack the tar. Possibility of the tar Gasifier temperature [K]
b
Conversion [mol/100 mol-C in char+coke]
100
60
Pyrolysis(Al2O3)
Gasification(Al2O3)
Carbon yield in product gas
80 Pyrolysis(SiO2) 50
[mol/100mol-C in coal]
Gasification(SiO2)
40
60
30
40
20
20
10
0 0
1050 1100 1150 1200 950 1000 1050 1100 1150 1200
Gasifier temperature [K] Gasifier temperature [K]
Fig. 7. Effect of bed material on carbon yield in product gas under different gasication/ Fig. 8. Conversion of char (a) or char + coke (b) in isolated and non-isolated cases at
pyrolysis temperatures. different gasier temperatures. Bed material: (a) silica sand, (b) -alumina.
48 K. Matsuoka et al. / Fuel Processing Technology 109 (2013) 4348
100
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