Fuel xxx (2012) xxxxxx

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Fuel
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Dual bed pyrolysis gasication of coal: Process analysis and pilot test
Yuming Zhang a,b, Yin Wang a,, Lianguo Cai a,b, Changbin Yao a, Shiqiu Gao a, Chun-Zhu Li c,
Guangwen Xu a,
a
State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
b
Graduate University of Chinese Academy of Sciences, Beijing 100049, China
c
Fuels and Energy Technology Institute, Curtin University of Technology, GPO Box U1987, Perth, WA 6845, Australia

a r t i c l e i n f o a b s t r a c t

Article history: Via isolating the fuel pyrolysis and char gasication, the so-called dual bed pyrolysis gasication (DBPG)
Received 26 October 2011 was proposed to realize the co-production of pyrolysis products and gasication gas. The process simula-
Received in revised form 14 January 2012 tion with Aspen Plus shows that the DBPG process can run autothermally using air as the gasication
Accepted 16 January 2012
reagent, but the complete conversion of char in the gasier requires relatively high O/C ratio due to the
Available online 21 February 2012
absence of steam in the reactor. This would make the higher heating value (HHV) of the produced
gasication gas below 1000 kcal/Nm3. Adding steam to the char gasier can realize full char conversion
Keywords:
at lower O/C ratio to improve the gasication gas quality. The effect of air preheating on the gasication
Dual bed
Pyrolysis gasication
performance was further analyzed to optimize the operating conditions of DBPG. A pilot scale plant
Coal (100 kg-coal/h) of DBPG was established and tested by using air as the gasication reagent plant to verify
Decoupled conversion the technology feasibility. At the steady operating temperatures of 600 C for pyrolyzer and 850 C for gas-
Cogeneration ier, the produced pyrolysis gas was rich in hydrocarbons and the tar yield reached 8.4 wt% and was rich in
phenols and its derivatives, but the HHV of the gasication gas was only 510 kcal/Nm3, much lower than
the simulated value. A laboratory test on charair gasication in a uidized bed reactor further showed
that the short residence time of char inside the gasier and thus the low carbon conversion and the burn-
ing of the produced gas in the reactor was the cause for this lower heating value of the gasication gas.
2012 Elsevier Ltd. All rights reserved.

1. Introduction
The coal rich in volatiles, including lignite, subbituminite and
bituminite contains high-value chemical structures like aromatic
rings. These chemical structures are completely converted into
simple molecules of H2O, CO2, CO, H2, and hydrocarbons (C1C3)
in combustion and gasication. It is attractive and promising to ex-
tract these valuable chemicals prior to gasication or combustion
to produce ne chemicals and fuel oils. For this purpose, the so-
called coal topping concept was previously proposed in China
[1,2]. The coal topping process can be realized in a dual uidized
bed system with its riser of transport bed as the combustor and an-
other bed as the fuel pyrolyzer (see Fig. 1a). Between the two reac-
tors, the heat carrier particles (HCPs), which are usually coal ash
blended with char, are circulated to carry heat from the riser com-
bustor of char to the coal pyrolyzer to supply the pyrolysis-needed
endothermic heat.
For the dual bed coal topping process, the moving bed [3,4],
downer [5,6] and uidized bed [79] have been tested as the coal
pyrolyzer. Liang et al. [3] investigated tar yield in a lab-scale moving
Corresponding authors. Tel./fax: +86 10 8254 4886.
E-mail addresses: wangyin@home.ipe.ac.cn (Y. Wang), gwxu@home.ipe.ac.cn
(G. Xu).
bed pyrolyzer integrated into a circulating uidized bed (CFB) com-
bustor system, nding that the maximal tar yield was up to
11.0 wt% for Shenmu bituminite in dry coal basis using quartz sand
as the HCPs at 850 C. Then a pilot poly-generation plant was built
from retrotting a 75 steam-t/h CFB boiler through combining a
moving bed coal pyrolyzer with its combustor, and the test of this
plant realized a tar yield of 6.0 wt% (dry coal base) at 600 C for
the same Shenmu coal [4]. Wang et al. [5] conducted coal pyrolysis
in a downer reactor coupled with a riser combustor (coal treatment
capacity was 8 kg/h) and found that the optimal pyrolysis temper-
ature was 660 C and a tar yield of up to 14.5 wt% was obtained for a
kind of pulverized subbituminous coal below 280 lm. Zhu et al. [6]
investigated the effect of coal particle size on pyrolysis and char
reactivity in the downer reactor, showing that increasing the parti-
cle size raised the char yield but decreased char reactivity. A down-
er coal pyrolysis process coupled to a 75 steam-t/h CFB boiler was
also built in Hebei province of China, and a preliminary test showed
a satisfactory process performance and the further optimization for
the performance is still under way. For developing the dual bed
coal topping process with a uidized bed pyrolyzer, Zhang et al.
[7] investigated the pyrolysis of a Chinese subbituminous coal in
46 mm in a laboratory uidized bed reactor and found that the
maximal pyrolysis oil yield occurred at 600 C and the required res-
idence time of coal particles in the bed should be over 3 min. The

0016-2361/$ - see front matter 2012 Elsevier Ltd. All rights reserved.
doi:10.1016/j.fuel.2012.01.038

Please cite this article in press as: Zhang Y et al. Dual bed pyrolysis gasication of coal: Process analysis and pilot test. Fuel (2012), doi:10.1016/
j.fuel.2012.01.038
2 Y. Zhang et al. / Fuel xxx (2012) xxxxxx
Flue gas Tar +
Pyrolysis gas
Hot HCPs
Combustor
Pyrolyzer
Fuel
Char+HCPs
Air Fluidized gas Air / steam
a b
Fig. 1. Conceptual diagrams of technical processes of (a) coal topping (or dual bed pyrolysis combustion), (b) dual bed pyrolysis gasication (DBPG) and (c) dual uidized bed
gasication (DFBG).
study of Xiong et al. [8] in the same reactor further found that the
highest tar yield appeared at 550700 C for coals from lignite to
bituminite. They for the rst time demonstrated that the use of coal
ash as the bed material decreased evidently the yields of tar and
gas, but adopting the gas simulating the coal pyrolysis gas compo-
sition as the reaction atmosphere facilitated conversely the tarry
liquid production. Fang et al. [9] studied the pyrolysis of Huainan
bituminous coal in a uidized bed pyrolyzer integrated with a
75 steam-t/h CFB combustor and found that the polygeneration
system could run continuously and steadily with tar yield of
11 wt% at about 540 C of pyrolysis and the usual combustion tem-
peratures in the char combustor.
The preceding coal topping has so far referred to the process
illustrated in Fig. 1a exclusively, which is based on the integration
of the isolated coal pyrolysis with char combustion. It can thus be
called the dual bed pyrolysis combustion (DBPC). From the applica-
tion aspect, this implicates the retrot of CFB boilers so that the
coal chemical structures can be extracted to produce high-value
chemical products before the complete combustion of the coal.
Extending this reaction decoupling principle to the gasication
process in CFB-type reactors [10], we have proposed the dual bed
pyrolysis gasication (DBPG) process characterized with the inte-
gration of the isolated coal pyrolysis with char gasication [8], as
illustrated in Fig. 1b. This newly devised DBPG process intends to
extract the coal-inherent liquid and gas components in volatiles
before the through gasication of coal into CO, CO2 and H2.
As a coal pyrolysis process, the performance of the DBPG should
be similar to that of the DBPC highlighted in the second paragraph
shown above. As a coal gasication process, the DBPG should be
compared to the well-documented dual uidized bed gasication
(DFBG) illustrated in Fig. 1c. According to Zhang et al. [10], the
DFBG is featured with the isolation of the char combustion reaction
that generates the endothermic heat required by the reactions of
fuel pyrolysis and gasication occurring in another integrated reac-
tor (see Fig. 1c). The fundamentals and process characteristics of
DFBG have been extensively investigated in the community to
show its merit of producing middle caloric fuel gas without re-
course to the use of O2-rich gasication reagent and its particular
suitability for highly reactive fuels like biomass and lignite [11
15]. Against the DFBG, the newly proposed DBPG conceptualized
in Fig. 1b may take rather more attractive advantages as following:
(1) The DBPG allows the co-production of pyrolysis liquid and
gasication gas to realize value-added hierarchical utiliza-
tion of coal. This realizes actually the similar co-production
effect as Lurgi gasier but for powder coal and also easier
to recover the tar product as claried below.
Please cite this article in press as: Zhang Y et al. Dual bed pyrolysis gasication of coal: Process analysis and pilot test. Fuel (2012), doi:10.1016/
j.fuel.2012.01.038
Fuel gas Tar + Flue gas Fuel gas
Pyrolysis gas
Hot HCPs Hot HCPs
Combustor
Pyrolyzer
Gasifier
Gasifier
Fuel Fuel
Char+HCPs Char+HCPs
Fluidized gas Air Steam / Air
c
(2) The tarry matters present only in the gaseous pyrolysis
product, which greatly facilitates the tar recovery operation
and reduces the load of gas cleaning. For the processes like
Lurgi gasier and DFBG, the tarry matters present in the
large-volume gasication gas, raising thus the load of gas
cleaning.
(3) The DFBG may require ue gas cleaning system such as
desulphurization and denitration in addition to the gasica-
tion gas cleaning. For DBPG, however, the gas cleaning is
only for the gasication gas that may be mixed with the
pyrolysis gas after its recovery of liquid tar.
(4) The oxygen consumption for DBPG should be lower than in
DFBG because the efuent temperatures of the pyrolysis
product are lower than that of the gasication gas in the
DFBG.
(5) In DBPG the isolation of coal pyrolysis and char gasication
creates the circumstance of gasication without the pres-
ence of pyrolysis gas around the char particle, to facilitate
thus the char gasication [16,17].
With the foregoing technical advantages, the DBPG would ap-
pear to be a promising new gasication technology that may have
great potential applications for the production of fuel gas as the
Lurgi-type or CFB-based gasiers. With the intention of demon-
strating the feasibility of this newly proposed technology, this
study performed rst a process simulation using Aspen Plus to
clarify the heat and mass ow features and the performance char-
acteristics of the technology. In turn, a pilot test at the capacity
treating about 100 kg/h coal was conducted to further show the
technology feasibility and process characteristics. Thus, it hopes
to not only verify the rationality of the new DBPG technology but
display also the conception of hierarchical conversion and value-
added utilization of coal in gasication processes.
2. Experimental section
2.1. Process simulation
The Aspen Plus model used to simulate the dual bed pyrolysis
gasication (DBPG) process is shown in Fig. 2, which consisted
mainly of the modules for coal pyrolysis and char gasication.
The supplementary parts around such two modules included the
elements decomposer for fuel, gassolid separator (cyclones), heat
exchanger, gasliquid splitter and mixer. Coal was rst broken into
its elements (H, C, O, N, S), ash and water as its moisture in the
decomposer and then was heated up to 600 C by mixing with
 Y. Zhang et al. / Fuel xxx (2012) xxxxxx
Fig. 2. A conceptual diagram of the Aspen Plus simulation model for the DBPG process.
HCPs from the gasier. The enthalpy needed for breaking the
chemical bonds in coal pyrolysis was assumed to be 108 kJ/kg
[18]. The decomposed elements were conveyed to pyrolyzer (the
RYIED block). Because there is no coal pyrolysis model in Aspen
Plus, the laboratory experimental data from pyrolyzing Fugu bit-
uminite were used to represent the performance of the pyrolysis
module. The properties of the tested bituminite were shown in Ta-
ble 1, and the pyrolysis experiment was conducted in a laboratory
uidized bed reactor [19] of silica sand at 600 C and using nitro-
gen as the uidizing gas. The pyrolysis product yields for tar, gas,
char and pyrolysis water were found to be 11.74 wt%, 8.10 wt%,
72.93 wt% and 7.23 wt% (water was calculated by difference),
respectively. In the pyrolysis module the formed product was split
into two streams, the char to the gasier and the volatiles to the
splitter for getting the tar and pyrolysis gas products. In the gasi-
cation module the char from the pyrolysis reacted with the air pre-
heated by the hot product gas from the gasier. In this char
gasication module, not only fuel gas is produced but the HCPs
are also heated up to provide the endothermic heat required by
fuel pyrolysis. The hot HCPs were separated from the fuel gas
through the cyclone (SSplit module) and returned to the pyrolyzer.
Table 2 lists the considered reactions for char gasication in the
simulation (pyrolysis was based on experimental data). One can
see that the reactions related to S and N were not considered and
this would not much affect the mass and heat ows of the simula-
tion which are related mainly to C, H and O. The char gasier em-
ployed the RGibbs [20,21] and Rstoic modules to simulate the char
gasication reactions. Char reacted with the gasication reagents
heterogeneously to lead to the reactions R1R3 with O2, CO2 and
steam, respectively. The homogeneous reactions among the gener-
ated gas species and gasication reagents in turn took place, of
which the water gas shift (WGS) reaction was supposed to be at
the chemical equilibrium to adjust the composition of the product
gas [22]. Table 2 shows also that char reacted with oxygen via two
successive steps, rst being oxidized to form CO and in turn the CO
Table 1
Proximate and ultimate analyses of the tested Fugu bituminite.
Ultimate analysis (dafa wt%)
C H N S
82.92 4.66 1.26 0.22
a
daf: Ash free basis.
b
ad: Air dried basis.
c
VM: volatile matters.
d
FC: xed carbon.
Please cite this article in press as: Zhang Y et al. Dual bed pyrolysis gasication of coal: Process analysis and pilot test. Fuel (2012), doi:10.1016/
j.fuel.2012.01.038
3
is further oxidized to CO2. The ash in coal was supposed to transfer
completely into char in pyrolysis, but after char gasication the hot
ash fully remained in the system as the HCPs. Meanwhile, sand was
blended with the ash to balance the energy between pyrolysis and
gasication.
2.2. Pilot experiment
A pilot plant of coal DBPG was established and Fig. 3 shows its
schematic diagram. The plant had a coal treatment capacity of
about 100 kg/h, and consisted mainly of a pneumatic gasier and
a uidized bed pyrolyzer. A loop seal connected the pyrolyzer
and the bottom of the gasier, while a cyclone on the top of the ri-
ser served to separate the HCPs from the gasication gas. The gas-
ier had two stages with different inner diameters (I.D.) and
heights (H), 370 mm (I.D.)  1800 mm (H) for the lower stage
and 200 mm (I.D.)  7300 mm (H) for the upper stage. In between
there was a transition of 300 mm high. The pyrolyzer was rectan-
gular with its inner size of 730 mm (L)  340 mm (W). The dipleg
of the cyclone was about 160 mm below the outlet of the overow
pipe of the pyrolyzer to form the particle circulation but prevent
the gas ow into the leg from the pyrolyzer. A roots blower was
employed to provide the air for the gasier and pyrolyzer, and an-
other for the loop seal. Liquid nitrogen vaporized by an aerotran
was used as the uidized gas of the uidized bed pyrolyzer, while
air was used in startup and ending the test. Nitrogen was the tracer
gas for determining the volume of the pyrolysis and gasication
gas.
At the downstream of the pyrolyzer, two electrically-warmed
high-efciency cyclones were installed to separate ne solid parti-
cles from tar-rich pyrolysis gas, and the gas was in turn cooled by
the water scrubber. A heat exchanger (condenser) and an electric
tar precipitator (ETP) were installed in the downstream of the
scrubber to collect tar. The connection tubes between cyclone
and ETP were all washed with acetone after each experiment for
Proximate analysis (adb wt%) HHV
O Moisture Ash VMc FCd (MJ/kg)
10.94 4.57 4.44 33.75 57.24 31.90
4 Y. Zhang et al. / Fuel xxx (2012) xxxxxx

Table 2
Considered gasication reactions of char in Aspen Plus simulation.

Reactions Enthalpy variationa

Heterogeneous reactions

C 0:5O2 ! CO Carbon gasification R1 111 kJ/mol

C CO2 ! 2CO Boudouard reaction R2 +172 kJ/mol

C H2 O ! CO H2 Carbon steam gasification R3 +131 kJ/mol

Homogeneous reactions

CO 0:5O2 ! CO2 CO combustion R4 283 kJ/mol

H2 0:5O2 ! H2 O H2 combustion R5 242 kJ/mol

CO H2 O ! CO2 H2 Water gas shift R6 41 kJ/mol

CO 3H2 ! CH4 H2 O Methanation R7 206 kJ/mol

a
The positive sign indicates the endothermic reactions and the negative sign indicates the exothermic reaction.

Fig. 3. A schematic diagram of the 100 kg/h dual bed pyrolysis gasication pilot plant.

tar recovery and the removal of possible tube blockage. Tar was
mainly collected from the tar-rich oating liquid in the scrubbing
water, and about 10% was also from the liquid of the condenser
and ETP and the tube-washing acetone. All these tarry liquids were
mixed together and a small part of the liquid mixture was taken to
determine the tar yield by recovering its containing tar through in
succession, ltration, dewatering (using H2Ofree MgSO4) and ace-
tone evaporation. The tar yield was the mass ratio of the tar to dry-
base coal treated. For analyzing the produced gas composition, two
gas ports were set behind the cyclones of the gasier and pyrolyzer

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 Y. Zhang et al. / Fuel xxx (2012) xxxxxx
to sample the gasication and pyrolysis gases, respectively. The
temperatures in the pyrolyzer and gasier were measured with
K-type thermocouples and recorded in a computer equipped with
data acquisition software.
The test was started by loading a reasonable amount of silica
sand (about 150 kg), the HCPs, into the system (mainly in gasier).
Then an oil burner (diesel) was turned on to generate hot ue gas
to heat up the HCPs and the gasier. When the desired tempera-
ture (ignition temperature of coal, about 500 C) was reached in
the bed, coal was continuously fed into the gasier from a hopper
to replace oil burner. After the temperature in the particle bed in
the gasier reached 700 C, the particle circulation was started to
heat the whole system including pyrolyzer, loop seal and connec-
tion pipes. When the temperature in the pyrolyzer reached the de-
sired temperature of about 400 C, coal feeding was switched to
the screw feeder connected to the pyrolyzer. When the pyrolyzer
temperature became steady the uidizing gas to the pyrolyzer
was changed into nitrogen from air to convert the reaction gradu-
ally into pyrolysis.
A gas chromatograph (Agilent GC 3000) was used to measure
the molar compositions of pyrolysis and gasication gases. The
pyrolysis tar was collected from the scrubber as well as the ETP
and was further extracted (removing dust and water) according
to the method detailed in Refs. [8,19]. A GCMS (Agilent 6890GC/
5792MS) was further adopted to analyze the composition features
of the tar.
A kind of Fugu bituminite coal was used for both the pilot test
and process simulation, and Table 1 shows the results of its prox-
imate and ultimate analysis. The coal had low ash and sulfur con-
tents but high volatiles, indicating its high suitability for pyrolysis
to make tar. The coal size adopted for the pilot test was below
8.0 mm, and the used HCPs were silica sand with a Sauter mean
diameter of 500 lm.
3. Results and discussion
3.1. Simulation using only air as gasication reagent
With the model in Fig. 2 and using the experimental pyrolysis
data as the input for the pyrolyzer, the simulation was conducted
rst by using air as the reagent for the char gasication in the riser
and then steam was introduced into the reactor to optimize the
gasication performance. The considered heat loss for the DBPG
system was supposed to be constantly 2% of the energy of the char
into the gasier. In the simulation, the pyrolysis temperature was
kept at 600 C, while the O2/C molar ratio for the gasier was var-
ied to determine the required solid circulation rate shown with the
mass ratio Rc calculated by
Gskg  m2  s1  Am2
Rc ; 1
F f kg  s1
whereas Gs, A and Ff refer to the particle circulation rate, cross-sec-
tional area of the gasier and the coal feeding rate, respectively.
Fig. 4a shows the gasier temperature Tg (pyrolyzer was xed at
600 C) and mass ratio Rc varying with O2/C in the gasier for the
case with only air as the gasication reagent. As anticipated,
increasing the air fed into the gasier raised the temperature in
the gasier and decreased the mass ratio Rc. The higher gasier
temperature implied a higher temperature for the HCPs into the
pyrolyzer. For maintaining the pyrolyzer constantly at 600 C the
lower particle circulation rate Gs was thus needed, which de-
creased in turn the ratio Rc of the circulated HCPs to the fed fuel
Ff. At O2/C = 0.35, the gasier temperature was 860 C and its cor-
responding Rc was 3.5, a particle circulation rate easily achievable
for CFB.
Please cite this article in press as: Zhang Y et al. Dual bed pyrolysis gasication of coal: Process analysis and pilot test. Fuel (2012), doi:10.1016/
j.fuel.2012.01.038
5
Fig. 4b shows the composition of the produced gas from the gas-
ier corresponding to Fig. 4a. The volumetric fractions of H2 and
CO2 slightly decreased with raising the O2/C ratio, whereas that
of CO increased. The decrease in the H2 fraction was mainly caused
by H2 combustion (R5) at the increased O2/C ratio, while the en-
hanced Boudouard reaction (R2) at the elevated gasier tempera-
ture was responsible for the increase in CO concentration. For
char gasication without the presence of steam, the production
of H2 should be limited to have low H2 fraction and constrained
methanation reaction (R7). The HHV of the produced gasication
gas decreased from about 1030 to 965 kcal/Nm3 with increasing
the O2/C ratio from 0.25 to 0.50. This means that the dilution effect
of N2 from increasing the air supply was more pronounced than
that caused by the formed CO at the higher O2/C. The data in
Fig. 4b shows that for air gasication of char the critical O2/C
should be below 0.35 for ensuring the produced gas to have an
HHV of 1000 kcal/Nm3.
Fig. 4c shows correspondingly that the higher O2/C ratio led to
the higher cold gas efciency (CGE) and carbon conversion (vC) de-
ned against the fuel char into the riser gasier. Here, the CGE re-
fers to the HHV ratio of the gasication gas to the char, and the
element conversion (i.e. C and H) shows the percentage of the ele-
ment transferred to the gasication gas from the char. Char gasi-
cation was promoted with more air fed into the gasier to have
thus the gradually higher vC. At O2/C = 0.50, the vC was over 90%
but the CGE was only 57%. The gas composition in Table 3 claries
that the major combustible gas was CO and H2 fraction was as low
as 5 vol%. This gas composition feature complied well with the fact
that the dominant reactions for char air-gasication were the reac-
tions R1 and R2.
In summary of Fig. 4, one can see that the DBPG was indeed
technically feasible, even if using only air as the gasication re-
agent for the char into the riser. Nonetheless, in the case with air
reagent it was hard to achieve the complete conversion of char.
For char gasication there was limited steam gasication reaction
R3 and water gas shift (WGS) reaction R6. Thus, the formed CO2
was also limited so that the reaction R2 cannot fully consume
the C left by the reaction R1. This caused thus the realized C con-
version vC at O2/C = 0.50 to be below 93% and the HHV of the pro-
duced gas to be low as 965 kcal/Nm3. Consequently, the use of
steam is expected to have an important role for the char gasica-
tion in DBPG.
3.2. Simulation with the presence of steam
For the simulation shown herein the O2/C ratio was kept con-
stantly at 0.50 and the calculation was made against varied ratios
of steam to carbon, i.e. the steam/C ratio estimated on the basis of
the char into the gasier. Fig. 5 shows the results obtained. From
Fig. 5a one can see that the gasier temperature decreased from
984 C to about 750 C with raising the steam/C ratio from 0 to
0.25 (O2/C was xed). Meanwhile, the Rc was almost tripled to be-
come close to 7 at steam/C = 0.25. For char gasication in the gas-
ier, the expected lowest reaction temperature should be about
900 C, showing that the allowed highest steam feed was limited
to the steam/C ratio of about 0.1. Otherwise, the gasier tempera-
ture should be too low. Of course, this is the case corresponding to
our adopted pyrolysis input, and the allowed steam feed would
vary with the pyrolysis extent. Considering the required Rc, we
can believe that it is quite easy to satisfy the entailed particle cir-
culation conditions because the CFB-based systems allow often the
mass ratios over 10 of circulated HCPs over the fed coal.
With the presence of steam, the char gasication reactions dee-
ply involved with the production and conversion of H2 (R3), (R5),
(R6), and (R7). This obviously increased the concentration of H2
in the gasication gas, as shown in Fig. 5b where the H2 fraction
6 Y. Zhang et al. / Fuel xxx (2012) xxxxxx

Fig. 4. Variations of performance parameters with O2/C for the gasier, (a) gasier temperature and mass ratio of solid circulation rate over fed coal, (b) gasication-produced
gas composition and its HHV and (c) carbon conversion and cold gas efciency (CGE) of char gasication.

Table 3
Compositions of the pyrolysis gas from laboratory experiment and gasication gas H elements in gasification gas mol  H elements in char mol
vH :
from process simulation. H elements in steam mol
Composition of pyrolysis gas (vol%) 2
H2 CH4 CO CO2 CnHm HHV (kcal/Nm3)
26.17 41.71 15.50 7.22 9.19 6773 The result indicates that thermodynamically most of the ele-
ment H in the steam could be converted into gaseous products
Composition of gasication gas (vol%)
H2 CH4 CO CO2 CGE (%) HHV (kcal/Nm3) for the simulated conditions. Also, comparing to the C conversion
Case a 5.18 0.07 26.69 4.46 56.76 965 only with air as gasication reagent in Fig. 4c, it reveals that the
Case b 7.91 0.65 27.41 4.24 67.19 1076 addition of steam into the char gasier greatly facilitated the car-
Case a: using only air as the gasication reagent at O2/C = 0.50. bon conversion via the steam gasication reaction R3 shown in Ta-
Case b: using air + steam as the gasication reagent at O2/C = 0.50, steam/C = 0.10. ble 2. A steam/C molar ratio of about 0.1 was theoretically
sufcient to realize the full C conversion at the tested O2/C ratio
of 0.5 for the coal and the simulated pyrolysis conditions. The con-
version vH was highest at steam/C = 0.15 (94%) and then slightly
raised to 10 vol% from 5 vol% corresponding to the increase of the decreased because no carbon was left for further steam gasica-
steam/C ratio from 0 to 0.25. The slight decrease of the CO fraction tion. The cold gas efciency (CGE) increased with raising the
and increase of the H2 and CO2 concentrations were also associated steam/C ratio. Considering the practically possible gasication
with the water gas shift reaction (R6) which was promoted in the temperature of higher than 900 C, the viable CGE would vary be-
steam-containing atmosphere. Table 3 shows also the detailed gas tween 57% and 67% corresponding to steam/C < 0.10 at O2/C = 0.5.
composition (case b) to verify these changes. The HHV of the gas- This CGE is relatively low and the O2/C ratio is relatively high com-
ication gas increased correspondingly, especially under the paring to usual direct coal gasication because the gasier of DBPG
steam/C ratios of 0.1 whereat the HHV was 1076 kcal/Nm3, indicat- supplied also the endothermic heat for the coal pyrolyzer.
ing an increase of about 12% comparing to the case at O2/C = 0.5 In summary of the above analysis for Figs. 4 and 5 we can see
without steam reagent. that the DBPG is technically feasible to allow co-production of
Fig. 5c reveals that the carbon of char was fully converted at the pyrolysis products (tar and pyrolysis gas) and the gasication
steam/C molar ratios higher than 0.10 and the H conversion vH de- gas. The latter is either fuel gas when the reagent for the char gas-
ned below was about 90% for all the simulated conditions. ier is air or its mixture with steam (the simulated case) or syngas

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 Y. Zhang et al. / Fuel xxx (2012) xxxxxx 7

Fig. 5. Variations of performance parameters with steam/C at constant O2/C = 0.50 for the gasier, (a) gasier temperature and mass ratio of solid circulation rate to fed coal,
(b) gasication-produced gas composition and its HHV and (c) carbon and hydrogen conversion and cold gas efciency (CGE) of char gasication.

if the reagent is pure O2 blended with steam or CO2. The DBPG in-
volves hot char (without inherent moisture) gasication in the gas-
ier and the complete conversion of the char requires relatively
higher O2/C ratio because there is no H2O from the fuel to facilitate
the gasication reaction, lowering thus the heating value of the
produced gas. For air + steam gasication reagent there are prac-
tically suitable operating conditions. For example, in Figs. 4 and 5
the major parameters for the char gasier should be the O2/C molar
ratio of about 0.5, steam/C molar ratio of about 0.1 and the circu-
lation mass ratio Rc of 3.0 (HCPs against fed coal). The correspond-
ing performances were the char gasier temperature of about
900 C, coal pyrolysis temperature of 600 C, theoretically full C
conversion which led to the CGE of up to 67% dened against the
char energy inputted into the gasier, and the gasication gas
HHV of 1076 kcal/Nm3. These conditions and performance vary
surely with the coal type and mass/energy distribution in
pyrolysis.
3.3. Energy distribution and utilization analysis
Fig. 6 exemplies how the inputted coal energy was allocated
through the conversion in DBPG by taking the cases of (a)
O2/C = 0.50, steam/C = 0 and (b) O2/C = 0.50, steam/C = 0.10, and
their pyrolysis and gasication temperatures were 600 C and
850 C, respectively. The inputted energy with 100 kg/h coal
(3190 MJ) was split into four streams in the pyrolyzer, which, were
with the pyrolysis gas, water, tar and char, respectively. Gasifying
the char split further its containing energy (sensible heat and chem-
ical energy) into a few other streams of which the chemical energy
in the gasication gas was shown as the cold gas efciency (CGE). It
is noteworthy that the percentage numbers in Fig. 6 were against
the energy of coal for the pyrolysis but against the energy of char
for the gasication. Nonetheless, the data for pyrolysis were based
on a xed experimental input, having thus no variation for the two
cases. The heat loss was accounted only for the gasier and was
specied to be 2.0% of the char energy. In the case (b), the energy
input via steam was not considered in calculating such percentages.
Through pyrolysis, 74.05% of the coal energy entered the char
and 7.90% was with the pyrolysis gas. For the case (a) the CGE
and the sensible heat of the gasication gas were 56.78% and
17.58% of the energy with the char, respectively. The energy
needed to supply for the coal pyrolysis was 3.78%, including two
parts, the energy preheating coal to the desired pyrolysis temper-
ature and that needed to break down the chemical bonds of large
molecules. Without steam into the gasier the unreacted char for
the calculated case was 6.40% of the energy of the char. In the case

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j.fuel.2012.01.038
8 Y. Zhang et al. / Fuel xxx (2012) xxxxxx
a (otherwise, the CGE might not increase). In the simulation preheat-
b the gasication reagent was conducted and the total steady-state
Fig. 6. Examples of estimated energy distribution in the dual bed pyrolysis
gasication (DBPG) process for the cases of (a) O2/C = 0.50, steam/C = 0 and (b)
O2/C = 0.50, steam/C = 0.10 under temperature of 600 C for pyrolysis.
(b), there was no unreacted carbon (fully converted) and the CGE
increased by 10% to reach about 67.19%. Its sensible heat of the
gasication gas was slightly lower than in the case (a) because
of the lowered gas temperature (about 900 C against about
1000 C).
For both the cases (a) and (b) the consumed energy inside the
gasier, including preheating gas reagent and particles and provid-
ing the endothermic heat of char gasication reactions, was shown
with others in Fig. 6 because it was hard to accurately specify
this percentage without considering the inputted energy via steam
in the case (b). In general, this internally consumed energy should
be higher for the case (b) but a part of the consumed energy was
from the steam itself including its latent and sensible heat.
Fig. 6 shows that it was valuable to use the sensible heat of the
gasication gas. Thus, Fig. 7 shows how preheating the gasication
reagent (air + steam) affected the gasication performance. The
simulated conditions were the same as for that in Fig. 5 (i.e.
O2/C = 0.5 and varying the steam/C ratio) but the gasication re-
agent was preheated to 400 C with the sensible heat of the pro-
duced gasication gas in lowering its temperature to Tm from Tg.
As shown in Fig. 7, the Tm was above 500 C for the simulated
steam/C molar ratios of up to 0.25, and with raising the steam/C ra-
tio the difference between Tg and Tm slightly increased from 250 to
260 C in correspondence with the more steam in the reagent gas.
Comparing to Fig. 5, the preheating in Fig. 7 raised the gasica-
tion temperature by about 110 C and the desired gasier temper-
ature of 900 C was maintained at the steam/C ratio of 0.15 (<0.10
in Fig. 5). This means that preheating the gasication reagent with
the sensible heat of the product gas expanded the viable operation
range of the char gasication. For the specied steam/C molar ratio
the CGE in Fig. 7c was about 1.0% higher than that in Fig. 5c so that
the CGE was about 72% at steam/C = 0.15, the allowable highest
steam/C ratio for keeping the gasication temperature of 900 C.
Because the C conversion reached theoretically 100% at steam/
C > 0.10 (see Fig. 7c), the further increase in CGE with raising the
steam/C ratio referred to a result from the increased H amount
converted from the fed steam (vH was a constant but the steam
amount was more at the higher steam/C ratio). Nonetheless, in this
Please cite this article in press as: Zhang Y et al. Dual bed pyrolysis gasication of coal: Process analysis and pilot test. Fuel (2012), doi:10.1016/
j.fuel.2012.01.038
calculated CGE the energy with the steam was not considered
ing the gasication reagent did not vary much the composition and
HHV of the gasication gas, although a very slight increment in its
H2 fraction and HHV could be identied due to the corresponding
variation in the thermodynamic equilibrium constant of the water
gas shift reaction. However, this refers to the result of thermody-
namic simulation without considering the kinetic limits.
3.4. Pilot demonstration with air gasication
With the pilot plant shown in Fig. 3, the pilot test using air as
operation time was up to 200 h. Fig. 8 shows the typical tempera-
tures in the pyrolyzer (a) and gasier (b) in one of the tests. The
height in Fig. 8 indicated the distance between gas distributor
and the position of the thermocouples. There was no particle circu-
lation during heating the gasier with diesel burner, and the pyro-
lyzer was rst operated with air to raise its temperature and in
turn with N2 to switch the reaction in the bed into coal pyrolysis.
Because the evaporated liquid N2 had much lower temperature
than air, the switch of air to N2 at about 320 min induced a sharp
decrease (200 C) in the pyrolyzer temperatures, which led to a
slight decrease in the riser temperatures as well due to the circula-
tion of the temperature-lowered particles from the pyrolyzer to the
riser.
The steady operation was lasted for 500 min to maintain the
typical temperatures in the pyrolyzer and gasier at 600 C and
850 C, respectively. For the gasier (Fig. 8b), the rapid decrease
of the windbox temperature indicated the stop of the diesel burner
and the start of the coal burning inside the gasier. Then, we can
see that the temperatures in the gasier were almost vertically
uniform at about 850 C, complying well with the operation fea-
tures of the riser reactor. The pyrolyzer temperatures had a rapid
increase at the beginning, indicating the effective circulation of
sand particles (i.e. the HCPs) into the pyrolyzer from the riser.
Then, we can see that the temperature in the lower part of the
pyrolyzer was slightly lower than the upper part of the bed. This
was attributed to the cooling effect of the low-temperature uidiz-
ing gas, which was air rst and then the evaporated liquid N2, at its
entrance into the particle bed of the pyrolyzer. The steady temper-
ature for the pyrolyzer was thus about 600 C and vertically uni-
form above certain bed height, for example, 500 mm from the
gas distributor.
Table 4 shows that the volatiles left in the char sample taken
from the above pilot test was about 17 wt%, much lower than
33 wt% in the original coal. The tar yield for the test was about
8.4 ad-wt% (air dried basis coal), which was lower than the tar
yield in the laboratory (11.7 ad-wt%). Here, the tar product in-
cluded the parts recovered from cooling scrubber, condenser, ETP
and the connection tubes. The difference in the tar yield between
the pilot and laboratory tests would reect the inuence of particle
circulation (tar adsorbed onto HCPs) as well as the possible short
reaction time of pyrolysis. The laboratory test was in a uidized
bed without particle circulation and reaction time limit (batch
test). Fig. 9 shows the chemical species in the tar identied with
GCMS, and all species with concentrations higher than 1.0 wt%
were numbered and their corresponding substance names were
listed in the gure. The main chemicals were phenol (6) and its
derivatives, naphthalene derivatives (8) and phenanthrene (11)
derivatives. A literature work testing the similar bituminous coal
in a moving bed coal pyrolyzer integrated with a 75 t-steam/h
CFB boiler reported a tar yield of 6.0 db-wt% at 600 C and about
20 wt% of the produced tar was light oil and phenol [4]. Thus, the
use of uidized bed as the pyrolyzer would lead to compatible per-
formance in terms of tar production.
 Y. Zhang et al. / Fuel xxx (2012) xxxxxx 9

Fig. 7. Variations of performance parameters with steam/C at constant O2/C = 0.50 for the gasier when the gasication reagent was preheated to 400 C by the sensible heat
of the produced gas, (a) gasier temperature and mass ratio of solid circulation rate over fed coal, (b) gasication-produced gas composition and its HHV and (c) carbon
conversion and cold gas efciency (CGE) of char gasication.

The DBPG process generates both pyrolysis gas and gasica-
tion gas, but in our test the pyrolysis gas was mixed with N2
due to the use of N2 as the uidizing gas of the pyrolyzer.
Fig. 10 shows the typical composition characteristics of the pyro-
lysis gas free of N2 (a) and gasication gas (b) and their corre-
sponding HHVs. The pyrolysis gas was rich in CH4 (31.4 vol%),
CnHm (14.9 vol%) and H2 (24.5 vol%). Especially, the hydrocarbon
(CH4 and CnHm) contents reached 46.3 vol%, having thus the
HHV of 6200 kcal/Nm3 (N2 free). This infers that the pyrolysis in-
volved considerable break and hydrogenation of methyl chains
like CxHy (<600 C) and the cross link of the coal macromolecules
(600800 C) [23].
Fig. 10b shows that the gasication gas was with relatively high
CO fraction but low CH4 and CnHm concentrations, indicating just
the feature of air gasication of char. It was found also that the pro-
duced gasication gas from the gasier was almost free of tarry
matters to allow the direct cooling of the gas in a heat exchanger
downstream the gasier. Nonetheless, the HHV of the gas was only
510 kcal/Nm3, much lower than the value of 1009 kcal/Nm3 shown
in the preceding simulation at O2/C = 0.35 and 860 C (no steam).
The relatively low gasication temperature and short reaction time
in the gasier of air with char (only 1.5 s), which led to low C con-
version, would be the major cause. In fact, the estimated C
conversion on the basis of the composition and volume of the pro-
duced gas was only 43%, verifying thus the anticipation.
To verify the points, the char of the same coal in sizes of 0.5
1.0 mm made in a N2 atmosphere at 600 C was gasied continu-
ously in a laboratory uidized bed reactor that allowed the
unreacted char to ow out continuously. The reactor provided only
1.02.0 s for the supplied air to react with the char uidized in the
reactor, although the char particles could stay in the dense bed for
30 min. It was found that the steadily generated gas at O2/C = 0.35
had a heating value of about 600 kcal/Nm3. Considering that the
laboratory setup was electric-heated while the energy for pilot test
was self-sustained, this result thus veried well that the short
reaction time of air with char in the pilot gasier was responsible
for the lower heating value of its produced gas. The potential solu-
tions to this problem are to enhance the char gasication reaction
by, for example, elevating the reaction temperature, prolonging the
reaction time of air with char, using rather ne char particles or
highly reactive char and increasing the char density inside the
reactor [24]. In commercial transport bed (riser) reactors, all of
these means can be realized to a certain degree to facilitate greatly
the airchar reaction and consequently to make the gasication
close to the theoretical simulation results shown in Section
3.13.3.

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10 Y. Zhang et al. / Fuel xxx (2012) xxxxxx

a a
750 Air N2 40 6000

Gas composition [V%]

32 5000

HHV [kcal/Nm ]
Temperature [ oC]

600

3
4000
450 24
3000
16
300 330mm 2000
700mm
900mm 8 1000
150

0
0
b
1000
b 12 500

Gas composition [V%]

HHV [kcal/Nm ]
3
400
9
Temperature [ C]

800
o

300
600 6
Windbox 200
1900mm
400
6000mm 3
100
8700mm
200
0 0
H2 CH 4 CO CO2 CnHm HHV
0
0 100 200 300 400 500 600 700 Fig. 10. Composition and HHV of the (a) pyrolysis gas (N2 free) and (b) gasication
Time [min] gas products from the pilot test corresponding to Fig. 8.

Fig. 8. Variation of temperature with operating time in the (a) pyrolyzer and (b)
gasier in a typical pilot test for a Fugu bituminite.
in the practical gasication plants which allow higher reaction
temperatures (to about 1000 C), longer reaction time for air with
char (up to 5 s) and higher char density inside the gasier.
Considering all the above results and analysis, we can then con-
clude that the pilot test of this article well proved the technology
feasibility of the DBPG process analyzed in last three sections. 4. Conclusions
Although the experimental heating value of the gasication gas
was low in this article, as a result of the short reaction time of A dual bed pyrolysis gasication (DBPG) process combining a
air with char and the relatively low gasication temperature in uidized bed coal pyrolyzer and a pneumatic char gasier was pro-
the pilot gasier (850 C), it is expected to overcome this problem posed to realize a hierarchical conversion of coal by co-producing

Table 4
Proximate and ultimate analyses of typical char samples from laboratory and pilot tests.

Char samples Ultimate analysis (daf.wt%) Proximate analysis (ad.wt%)

C H N S O Moisture Ash V.M. F.C.
Lab. test 89.63 2.34 1.08 0.23 6.72 1.38 6.38 17.70 74.54
Pilot test 89.92 2.53 1.14 0.21 6.20 3.38 12.05 17.04 67.53

1: Oxirane,3-ethyl-2,2-dimethyl- 2: 1H-Indene, 1-methylene-

1
3: Naphthalene, 2-methyl- 4: Naphthalene, 2-methyl-
20
5: Biphenyl 6: Phenol 7: Phenol, 3-methyl-
8: Naphthalene, 1,6,7-trimethyl- 9: Dibenzofuran
Abundance [10 ]
9

10: Fluorene 11: Phenanthrene

15 11
12: Phenanthrene, 1-methyl- 15: Fluoranthene
13: 1H-Cyclopropa phenanthrene,1a,9b-dihyd 6
10
14: 5,16[1',2']:8,13[1'',2'']-Dibenzenodiben
8
34 7 9 10 13
2 12 14
5 15
5

0
10 20 30 40 50
Time [min]

Fig. 9. Composition analysis of pyrolysis tar product from the pilot test corresponding to Fig. 8 for a Fugu bituminite using GCMS chromatogram.

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 Y. Zhang et al. / Fuel xxx (2012) xxxxxx
pyrolysis oil and gasication gas which can be either fuel gas or
syngas. Different from other traditional gasication processes,
the DBPG provides a way to extract the aromatic chemicals as well
as volatile gases containing inherently in coal before the full
destruction of the coal molecules into small ones like CO, CO2, H2
and H2O. This article presented rst a process simulation for DBPG
using Aspen Plus to clarify its mass and heat balance characteris-
tics and also to reveal its thermodynamic performances of gasica-
tion under varied operating conditions. The results show that the
DBPG is technically feasible to realize co-production, but the cold
gas efciency dened for the char gasier (against its inputted en-
ergy) is relatively lower than the direct coal gasier because of its
providence of the endothermic heat for the integrated pyrolyzer.
For the DBPG process it is relatively hard to realize the full carbon
conversion in the char gasier (no steam in the fuel), if no steam
was fed into the gasier as a part of the gasication reagent. The
added steam, for example, according to the steam-to-carbon (of
char) molar ratio of 0.1, would allow more than 90% of the steam
to be converted into product gas. For maintaining the coal pyro-
lyzer temperature of about 600 C and char gasier temperature
over 900 C, the viable steam/C molar ratio can be up to 0.1 and
O2/C ratio was about 0.5. By using the sensible heat of the gas-
ier-generated product gas to preheat the reagent air + steam,
the viable operating conditions were further expanded to allow
the steam/C ratio of up to 0.15. Under optimized operating condi-
tions it is possible to have the full C conversion in the gasier and
the corresponding cold gas efciency can be up to 72%.
A pilot plant built according to the principle of DBPG and treat-
ing about 100 kg-coal/h has realized its successful steady operation
with a kind of subbituminite and using air as the gasication re-
agent at the pyrolysis temperature of about 600 C and gasication
temperature of about 850 C. The produced pyrolysis tar (about
8.4 db-wt% coal) were rich in phenols and its derivatives (analyzed
with GCMS). Thus, the pilot test well demonstrated the technol-
ogy feasibility of the newly proposed DBPG. Because of the rela-
tively low gasier temperature (850 C) and short reaction time
(1.5 s) of the air reagent with char, the produced gasication
gas had low heating value, but the problem can be overcome
through elevating the gasication temperature and prolonging
the reaction time of air with char.
Acknowledgments
The study was nancially supported by National Basic Research
Program of China (973 Program, 2011CB201304), National Natural
Science Foundation of China (21076217), National Key Technology
Development Programs of China (2009BAC64B05, 2010BAC66B01),
and Chinese Academy of Sciences. The authors are also grateful to
Doctor Xi Zeng and Qi Zhou, Master Shisheng Wu and Yang Song
for their helps in performing the pilot tests.
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j.fuel.2012.01.038
11
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