Fuel 86 (2007) 194–202

www.fuelfirst.com

Experimental investigation of role of steam in entrained

flow coal gasification
Nenad Crnomarkovic, Branislav Repic, Rastko Mladenovic *,
Olivera Neskovic, Miomir Veljkovic
Institute of Nuclear Sciences – Vinca, Laboratory for Thermal Engineering and Energy, P.O. Box 522, 11001 Belgrade, Serbia and Montenegro

Received 13 January 2006; received in revised form 16 June 2006; accepted 21 June 2006
Available online 26 July 2006

Abstract

Experimental investigations of the influence of excess oxygen coefficient, H2O/coal mass ratio using high-temperature steam, mean
mass diameter of pulverized coal and coal size fraction on basic characteristics of coal gasification were performed. Experiments were
carried out on a laboratory scale (0.09 m i.d. · 1.5 m high) coal gasification apparatus with lignite type of coal. Influence of steam
was realized through comparison of results obtained from experiments with (H2O/coal = 0.287 kg kg1) and without steam addition
(H2O/coal = 0.024 kg kg1). High values of carbon conversion, obtained both for finely ground and for coarse pulverized coal points
to the easiness of lignite gasification, i.e. to its high suitability for gasification.
 2006 Elsevier Ltd. All rights reserved.

Keywords: Coal gasification; Entrained flow; Steam

1. Introduction of CO2. Ash particles emission is lower as well, and thermal

Gasification is a coal conversion process by which com-
bustible gas from coal is produced. Gas obtained by coal
gasification can be used in many ways: for electricity pro-
duction (which is probably the most important use), in
chemical industry for petrol, methanol and ammonia syn-
thesis, for ore reduction, as an industrial fuel, as a town
gas for domestic uses, for residential heating etc. According
to predictions made by Longwell et al. [1], systems of elec-
tricity production which use coal gasification will become
competitive with other technologies of electricity produc-
tion after 2006. The main advantage of these systems, so-
called integrated gasification combined cycle systems, when
compared to conventional plants with pulverized coal (PC)
combustion, is easier and more efficient removal of sulfur
and nitrogen oxides precursors, as well as easier removal
*
Corresponding author. Tel.: +381 11 2458 222x217/+381 64 2471665
(mobile); fax: +381 11 2453 670.
E-mail address: rastkom@vin.bg.ac.yu (R. Mladenovic).
efficiency is higher by about 5–10%.
Coal gasification processes are known, well studied and
described in literature [2–4]. There are three basic reactor
types which are employed in the gasifier design: fixed
bed, fluidized bed and the entrained flow. In the investi-
gations described in this study, entrained flow coal gasifica-
tion has been chosen as a promising way of gas production,
due to its high coal throughput, insensitivity to coal type
and its simplicity in design and technology [5].
Entrained flow coal gasification process has been widely
investigated experimentally in small-scale gasifiers, and
with different types of coals [5–8]. Small-scale entrained
flow coal gasifiers are suitable for establishing a relation-
ship between laboratory and commercial gasifiers. Lee
et al. [8] show that it is difficult to generalize the gasification
characteristics for coals of different properties because var-
ious reactions take place in coal gasification. On the other
hand, some investigations state [5–7] that carbon conver-
sion is essentially independent of coal type. One of the
main reasons for this study is to examine the performance

0016-2361/$ - see front matter  2006 Elsevier Ltd. All rights reserved.
doi:10.1016/j.fuel.2006.06.015
 N. Crnomarkovic et al. / Fuel 86 (2007) 194–202
of Serbian lignites under entrained flow gasification condi-
tions. These fuels have high moisture and ash contents,
which will affect their performance. The data obtained
can be used to validate models of entrained flow gasifiers
using lignite.
The main goals of the investigations in this study were
experimental assessment of the gasification of indigenous
lignite in an entrained flow gasifier, and determination of
the influence of main parameters. The following investiga-
tions were performed: the influence of excess oxygen coef-
ficient (k); the influence of mean mass diameter of PC; the
influence of H2O/coal mass ratio using high-temperature
steam, and the influence of coal size fraction on basic char-
acteristics of PC gasification.
2. Basic reactions of coal gasification
Coal gasification essentially comprises of two successive
processes: pyrolysis (between 573 and 773 K) and char gas-
ification [4,9]. Basic reactions of coal gasification processes
can be divided into two groups: exothermic and endother-
mic reactions. Main exothermic reactions are reactions of
oxygen with carbon and hydrogen from coal, and the water
gas shift reaction. Main endothermic reactions are reac-
tions of CO2 reduction (Boudouard’s reaction) and the
water gas reaction.
Reactions of oxygen with carbon and hydrogen from
coal supply heat which is necessary for endothermic reac-
tions [2]:
C þ O2 ¼ CO2 DH 0298 ¼ 393:51 kJ mol1
1
2H2 þ O2 ¼ 2H2 O DH 0298 ¼ 285:84 kJ mol
These reactions proceed to complete consumption of
oxygen. Water gas shift reaction is a slightly exothermic
reaction:
H2 O þ CO ¼ H2 þ CO2 DH 0298 ¼ 41:17 kJ mol1
Reaction of CO2 with carbon is an endothermic
reaction:
C þ CO2 ¼ 2CO DH 0298 ¼ 172:5 kJ mol1
The most intensive change of concentrations occurs in
the temperature range from 700 to 1200 K. Above the tem-
perature of 1200 K, the concentration of CO2 is almost 0%
(vol%), and the concentration of CO is almost 100%
(vol%). Water gas reaction is an endothermic reaction:
C þ H2 O ¼ H2 þ CO DH 0298 ¼ 131:3 kJ mol1
The most intensive decomposition of steam occurs in the
temperature range from 600 to 1100 K. Above the temper-
ature of 1100 K, the concentration of steam is almost 0%
(vol%), while hydrogen and CO concentrations are equal
and approach 50% (vol%).
Sebastian [10] studied the influence of steam temperature
on entrained coal gasification products. The results were
obtained by translation of operating results from experi-
195
mental to adiabatic conditions and assuming exit gas tem-
perature of 1255 K. The H2O/coal mass ratio was varied
from 0 to 2.5 kg kg1 of dry, ash-free coal. It was reported
that the steam injected must be superheated to minimum
temperature of about 1255 K to act as a heat-transfer med-
ium. Any increase in H2O/coal ratio below that temperature
would decrease the percentage of carbon gasified and thus
the yield of synthesis gas, and increase the oxygen require-
ment. Azuhata et al. [5] performed experiments on
entrained coal gasification, in which two H2O/coal ratios
were used: 0.03 and 0.32 kg kg1. Partial coal combustion
was achieved in premixed flame. Although steam was pre-
heated up to 590 K, the production of hydrogen was hardly
affected by steam injection, but lower H2O/coal ratio
yielded higher levels of CO and lower levels of CO2.
3. Apparatus, coal properties and experimental procedure
3.1. Experimental facility
Experiments were carried out on a laboratory scale
(0.09 m i.d. · 1.5 m high) down-fired coal gasification
apparatus (Fig. 1). This reactor was built for the purposes
of a project (research programme) started in agreement
with the Electric Power Industry of Serbia, with the aim
to determine the gasification properties of Serbian lignites.
In the later phase, the project was supported by the Minis-
try of Science of Serbia. After the research programme was
completed, all research on this reactor terminated.
The burner (3), through which oxygen, air, propane–
ð1Þ
butane (PB) and PC are introduced, is placed on top of
ð2Þ the reactor [11]. Pulverized coal enters the reactor along
the axis together with the carrying air. The oxygen for com-
pletion of PB combustion is introduced together with the
air in the primary stream that surrounds the PC stream.
The pressure in the reactor was atmospheric. Using a screw
ð3Þ type coal feeder with a capacity of 3–6 kg/h, coal was intro-
duced into the reactor along the reactor axis. The oxygen
needed for partial coal combustion and complete hydrogen
combustion was injected through the primary stream.
ð4Þ Hydrogen was injected through the secondary stream, sur-
rounding the primary stream. Partial coal combustion and
complete hydrogen combustion were performed in diffu-
sion flame.
The combustion products are cooled in the scrubber
with water. Solid products were collected by filtering of
the scrubber water, and the gaseous products were col-
lected in glass sampling vessels (8). The concentrations of
ð5Þ
major gas species in dry product gas, i.e. CO, CO2, H2,
NH3, H2S, O2 and N2, were measured with mass spectrom-
eter, which could not differentiate CO from N2, due to a
small difference of molecular masses.
3.2. Coal sample
Coal used in experiments was domestic lignite Kolubara
pit D. Coal was ground in a laboratory mill as fine and
196 N. Crnomarkovic et al. / Fuel 86 (2007) 194–202

Fig. 1. Scheme of the apparatus. The main parts: (1) reactor, (2) pulverized coal feeder, (3) burner, (4) probe, (5) gas cooling vessel, (6) condensate removal
vessel, (7) filter, (8) gas ampoula, (9) rotameter, (10) gas sampling pump, (11) flue gas fan, (12) data acquisition unit, (13) particle collector, (14) scrubber,
(15) valve, (PB) propane–butane mixture.

coarse PC. The results of the PC sieve analyses are pre- of fine and coarse PC, and some size fractions of fine PC,
sented in Table 1. The proximate and ultimate analyses are presented in Table 2.

3.3. Experimental procedure

Table 1
Particle size distributions of fine and coarse pulverized coal At the beginning of the experiment, the reactor was
Sieve Diameter Coarse PC Fine PC heated by means of PB (50–50% mixture) combustion in
range (lm) Wt (%) Cum. wt (%) Wt (%) Cum. wt (%)
air. When the temperature of the outside surface of ceram-
ics reached 500 C, the heating of the reactor ceased, and
R500 >500 0.00 0.00 0.00 0.00
R315/500 315–500 23.81 23.81 0.00 0.00
PC combustion began. After the completion of reactor
R125/315 125–315 39.12 62.93 7.89 7.89 heating, oxygen was injected around the coal–air mixture
R90/125 90–125 14.09 77.02 18.26 26.15 introduction pipe, in amounts necessary for PB combus-
R71/90 71–90 11.32 88.34 28.22 54.37 tion, and also air, in amounts necessary for PC combus-
R50/71 50–71 4.74 93.08 22.46 76.83 tion. Around the O2/air introduction pipe, PB was
R0/50 0–50 6.92 100.00 23.17 100.00
injected in order to maintain a reducing atmosphere in
Mass mean diameter 211.95 79.08 the furnace. In the end, pulverized coal feeding into the
(lm)
reactor was turned on. Oxygen, PB and coal–air mixture

Table 2
Proximate and ultimate analyses of fine and coarse PC and some size fractions of fine PC
R90  26%a R90  77%a R0/50b R50/90b R90b
Proximate analysis (wt% ar)
Moisture (%) 2.3 5.0 4.8 7.3 2.9
Volatile matter (%) 50.6 49.2 43.6 45.5 50.5
Ash (%) 6.4 6.3 14.0 10.6 5.8
Fixed carbon (%) 40.7 39.5 37.6 36.6 40.8
Low heating value (kJ kg1) 26,205 26,205 23,245 23,444 26,203
Ultimate analysis (wt% db)
C (%) 54.6 53.0 48.6 49.1 54.6
H (%) 5.3 5.1 4.7 4.8 5.3
Scomb (%) 0.61 0.60 0.54 0.55 0.61
N (%) 0.72 0.70 0.64 0.65 0.72
O (%) (by difference) 30.0 29.3 26.7 27.0 30.0
a
Remainder on the 90 lm sieve.
b
Size fraction in the range 0–50 lm, 50–90 lm and >90 lm.
 N. Crnomarkovic et al. / Fuel 86 (2007) 194–202 197

were introduced just after the burner throat. After that, the
combustion began, and gas products sampling was done
after achieving a steady-state process.
3.4. The choice of experimental parameters
The mass flows of coal and oxygen were chosen in order
to establish the value of average specific volume heat
release in the reactor (qv) and excess oxygen coefficient
(k) to be similar to those obtained in other experiments
of coal gasification (Table 3). The value of qv is calculated
as qv = (Gpc * Hl)/Vr (kW/m3), where Gpc (kg/s) is the mass
flow of PC, Hl (kJ/kg) – coal lower heating value and Vr
(m3) – reactor volume. The mass flow of oxygen MO2 is cal-
culated as MO2 = MPC * k * Omin (kg/s), where MPC (kg/s)
is the mass flow of pulverized coal and Omin (kg/kg) stands
for the minimum amount of oxygen needed for complete
combustion. The volume flow of hydrogen is established
by adopting the H2O/coal mass ratio to be 0.32 (kg/kg),
which is usually used in some practical experiments [5].
The chosen value of qv for this reactor was 4000 (kW/
m3), as the mean value of similar experiments. The values
of some operating parameters are presented in Table 4.
Five groups of experiments were performed (Table 5):
(1) experiments with fine PC, and with introduction of
steam; (2) experiments with fine PC and without introduc-
tion of steam; (3) experiments with coarsest PC and with
introduction of steam; (4) and (5) experiments with a size
fraction of fine PC and with introduction of steam. In
experiments without steam addition only coal and oxygen
were injected. In experiments with steam addition hydro-
gen was injected together with coal and oxygen to produce
high-temperature steam. The H2O/coal mass ratio is
defined as the ratio of sum of the whole steam mass flows
(steam was obtained from hydrogen combustion and from
coal moisture), and mass flow of dry coal. The excess oxy-
gen coefficient k is defined as the ratio of mass flow rate of
injected oxygen to the mass flow rate of oxygen needed for
the complete combustion of coal.
The third group of experiments was repeated twice in
order to estimate the accuracy of measurement. The accu-
racy of coal feed rate (standard deviation) was within
±0.35%. The ash content in the coal gasified was accurate
to within ±6.2%. The accuracies of gas species were ±7.6%
for H2, ±3.82% for CO with N2, ±3.8% for CO2, ±2.8%
for NH3, ±3.6% for H2S and ±9.8% for HCN.

4. Results and discussion

Table 3
The values of average specific volume heat release in the reactor and excess
oxygen coefficient Continuous measurement of four temperatures along
the reactor axis (distances of 354, 708, 1062 and 1416 mm
Reference Excess oxygen Average specific
coefficient k (–) volume heat release form the burner) was carried out with the HP3852S acqui-
in the reactor (kW/m3) sition system. Measured gas temperatures are shown in
[5] 0.35–0.61 3352–4460 Fig. 2. Higher temperatures prevailed in experiments with
[6] 0.35–0.61 2979–3492 steam addition, because of additional heat released by the
[10] 0.3–0.448 5063 steam formation reaction.
[12] 0.31–0.459 5063 The most important characteristic of gasified coal
[13] 0.329 5063
particles was the mass fraction of dry, ash-free gasified
[14] 0.416 2580–3789
coal (GC). The level of GC is a result of complex processes:
coal devolatilization, volatile combustion, char combustion
Table 4 and char reactions with H2O and CO2. This level increased
The values of some operating parameters
with an increase in k, because of the increased concentra-
Pulverized coal Volume flow of Mass flow of Volume flow tion of oxygen available for combustion reactions. The
or size fraction oxygen for coal pulverized of hydrogen
combustion (m3/h) coal (kg/h) (m3/h)
mass fraction of gasified coal GC, expressed in %, was
determined by the modified ash balance method [13], with
R90  26% 2.5–4.0 5.0 1.77
R90  77% 2.5–4.0 5.0 1.56
ash contents (in %) used for calculations instead of weight
R0/50 (fine PC) 2.53–4.0 5.63 1.77 fractions:
R50/90 (fine PC) 2.54–4.0 5.58 1.55
R90 (fine PC) 2.52–4.0 5.0 1.77 GC ¼ ðAgc  Arc Þ  104 =ðAgc  ð100  Arc ÞÞ ð6Þ

Table 5
The values of some operating parameters for all groups of experiments
Mean mass diameter Mass flow H2O/coal Excess Group of Steam
of PC or size of pulverized mass ratio oxygen experiments
fraction (lm) coal (kg/h) (kg/kg) coefficient, k (–)
79.08 5.10 0.287 0.43; 0.56; 0.73 (1) Yes
79.08 5.10 0.024 0.41; 0.54 (2) No
211.95 4.01 0.397 0.35; 0.46; 0.60 (3) Yes
R50/90 4.30 0.407 0.47; 0.61; 0.80 (4) Yes
R90 3.37 0.430 0.40; 0.53; 0.69 (5) Yes
198 N. Crnomarkovic et al. / Fuel 86 (2007) 194–202

1500 90

1400 T H O =2022.40 K

Carbon conversion (%)

2

85
1300

T H O =2249.34 K
Temperature (K)

1200 80 2

1100
75 T H O =2456.28 K
1000 2

900
70
800 2.0

700

Residence time (s)

1.5
200 400 600 800 1000 1200 1400 1600
Distance from the burner (mm)
1.0
Fig. 2. Measured temperatures along the reactor axis for the first group of
T H O =2249.34 K
experiments, H2O/coal = 0.287 kg kg1, (j) k = 0.43, (.) k = 0.56, (m) 2

k = 0.73. T H O =2456.28 K
0.5 2

T H O =2022.40 K
2

where Agc is the ash content of GC (dry basis), and Arc is

0.0
the ash content of raw coal (dry basis). Carbon conversion,
defined as the ratio of mass flow rate of carbon in the gas 50

phase and mass flow rate of carbon fed by coal, was deter- T H O =2456.28 K
45 2
T H O =2249.34 K
mined on the basis of the level of GC and evolution of ele- 2
CO + N2 (vol %)

ments from coal during the whole process. 40

Gasification efficiency is defined as the ratio of chemi-
35
cally bound energy in produced gases from 1 kg of fuel
and chemically bound energy in 1 kg of fuel. In this study 30 T H O=2022.40 K
gasification efficiency is calculated as the ratio of chemi- 2

25
cally bound energy of CO and H2 in the produced gases,
and chemically bound energy of gasified amounts of car- 20
bon and H2 due to incomplete transformation of coal com-
50
bustible fraction into the gaseous phase. Compounds NH3
45
and H2S, although being combustible, are not included in T H O =2022.40 K
2
the balance, since they should be removed from the pro- 40
CO2 (vol %)

duced gases before utilization. 35

Carbon-monoxide (CO), although interfered by N2 in 30

mass spectrometry, was determined by calculation, based 25
on the mass balance of all coal elements during gasification 20 T H O =2456.28 K
T H O =2249.34 K
2

and on measured concentrations of all components of the 2

15
dry product gas [11].
10
25
4.1. Influence of excess oxygen coefficient k
20 TH O=2456.28 K TH O=2249.34 K TH O=2022.40 K
2 2
Experimental results of carbon conversion and composi- 2

tion of dry product gas are shown in Figs. 3–6. The carbon
H2 (vol %)

15
conversion (Fig. 3) in all experiments increased with an
increase of k. With increasing k, oxygen volumetric flow 10
rate increased, which allowed more fuel to be consumed
by combustion. High values of carbon conversion, which 5

are characteristic of coal gasification in premixed flame,

0
can be explained only by high reactivity of lignite Kolu- 0.35 0.40 0.45 0.50 0.55 0.60 0.65 0.70 0.75 0.80 0.85
bara. The PC particles residence time in the reactor λ (-)
decreased with increasing k (Fig. 3). With increasing k,
the mass flow rate and the temperature of the gaseous Fig. 3. Influence of excess oxygen coefficient k and H2O/coal mass ratio:
phase increased, which resulted in shorter PC particles res- (m) dav = 79.08 mm, H2O/coal = 0.287 kg kg1; (j) dav = 79.08 mm,
H2O/coal = 0.024 kg kg1.
idence time in the reactor.
 N. Crnomarkovic et al. / Fuel 86 (2007) 194–202 199

15 100

90

Carbon conversion (%)

80

T H O =2249.34 K 70
NH3 (vol %)

10 2

60
T H O =2456.28 K T H O =2022.40 K 50
2 2

40

5 30

20

4 2.0

1.5

Residence time (s)

3
HCN (vol %)

T H O=2249.34 K
2
1.0
2 T =2456.28 K
HO 2

T H O =2022.40 K
2
0.5
1

0.0
0
50
5
45
40
4
CO + N2 (vol %)

35
H2S (vol %)

3 30
25
2 T H O =2456.28 K 20
2

T H O =2022.40 K 15
2

1 T H O =2249.34 K 10
2
5
0
55
50
50
45 T H O =2249.34 K
T H O =2456.28 K 45
2 2
CO2 (vol %)

40 40
ηgas (%)

35 35

30
30
T H O =2022.40 K 25
2
25 20

20
0.35 0.40 0.45 0.50 0.55 0.60 0.65 0.70 0.75 0.80 0.85
20
λ (-)

Fig. 4. Influence of excess oxygen coefficient k and H2O/coal mass ratio

15
H2 (vol %)

(the marks are the same as in Fig. 3).

The product gas contents are a consequence of simulta-

10
neous occurrence of many reactions described earlier. In
PC gasification processes, the reactor space can be divided
into combustion and reduction zones [14]. In the oxidation 5
zone, reactions of coal and semi-char particles with oxygen 0.35 0.40 0.45 0.50 0.55 0.60 0.65 0.70 0.75 0.80 0.85

occur, while reactions of semi-char particles with gases pro- λ (-)

duced in the oxidation zone, and containing very little or Fig. 5. Influence of excess oxygen coefficient k and mean mass diameter of
no oxygen, occur in the reduction zone. pulverized coal and size fraction: (·) dav = 79.08 mm, H2O/coal =
With increasing k, heat released by coal combustion 0.287 kg kg1; (m) R50/90, H2O/coal = 0.407 kg kg1; (.) R90, H2O/
increased, and therefore measured temperatures of the coal = 0.430 kg kg1; (j) dav = 211.95 mm, H2O/coal = 0.397 kg kg1.
200 N. Crnomarkovic et al. / Fuel 86 (2007) 194–202

conditions for occurrence of endothermic reactions of

18
carbon.
In all performed experiments with steam addition, CO
16
concentration decreased (Fig. 3c and 5c) and CO2 concen-
NH3 (vol %)

tration increased (Figs. 3 and 5) with an increase of k.

14
Increase of CO2 concentration in the product gas is a result
12
of the water gas shift reaction and the carbon conversion
dependence of k. The concentration of H2 in dry product
10
gas (Figs. 3 and 5) increased with an increase of k in the
experiments with steam addition, but it decreased without
steam addition. The concentration of NH3 (Figs. 4 and 6)
6.0 was not dependent of k except in the third and fourth
5.5
5.0
group of experiments, in which NH3 concentration
4.5 decreased with increasing k. High NH3 content influenced
the content of other components in the product gas, espe-
HCN (vol %)

4.0
3.5 cially H2, because one atom of nitrogen binds three atoms
3.0 of hydrogen which would, in opposite, constitute hydrogen
2.5
2.0
or steam molecules.
1.5 Concentration of NH3 in dry product gas was somewhat
1.0 higher than expected as a result of NH3 produced by coal
0.5 nitrogen transformation. This could have come, to an
extent, as a result of NH3 interference in mass spectrometry
6.0 with OH radicals (not converted to H2O), but transforma-
5.5
5.0
tions of coal and air nitrogen most probably have a greater
4.5 influence. Theoretically, if all coal nitrogen was converted
4.0 to NH3, its concentration would be 1.5% (by volume),
H2S (vol %)

3.5 but the measured NH3 concentration was 10–15% (by vol-
3.0 ume). High NH3 concentrations in the product gas sug-
2.5
gested that NH3 originated both from coal and air
2.0
1.5 nitrogen. Most probably, high concentration of NH3 is a
1.0 result of transformation of air nitrogen to NOx in the com-
0.5 bustion zone, and subsequent reduction of NOx to NH3 in
the reduction zone. The mass balance calculations have
45 shown that this high value of NH3 concentration is possi-
40 ble. As assessed by the mass balance, a significant portion
of air nitrogen, while passing through hydrogen flame (with
35
temperature of up to 2000 C), transforms to NO in the
ηgas (%)

30 combustion zone. Further on along the reactor, in the

25
20
15
10
0.35 0.40 0.45 0.50 0.55 0.60 0.65 0.70 0.75 0.80 0.85
λ (-)
Fig. 6. Influence of excess oxygen coefficient k and mean mass diameter of
pulverized coal and size fraction (the marks are the same as in Fig. 5).
gaseous phase increased. This produced suitable conditions
for the formation of H2 and CO, by endothermic reactions
of semi-char carbon with CO2 and steam. On the other
hand, with increasing k the amount of carbon in semi-char
particles decreased due to higher carbon conversion, since
there was less and less carbon available for reactions with
CO2 and steam. Similarly, with increasing k, coal particles
residence time in the reactor decreased, which worsened the
reduction zone, formed NO transforms to NH3, and also
to another nitrogen compound – HCN. The content of
HCN in dry product gas was between 0.62% and 5.73%
(Figs. 4 and 6).
The sulfur compounds in the product gas originate as a
result of coal sulfur transformations. Only H2S was
detected in the product gas. Measured H2S concentrations
(Figs. 4 and 6) were higher than those that should arise by
coal sulfur transformation, except in R50/90 size fraction
experiments. In those experiments, the lowest value of
H2S concentration in product gas was measured. This fact
may be a consequence of sulfur oxides reaction with Ca
and Mg oxides in coal ash. In this coal sample, highest val-
ues of mentioned oxides contents were detected, when com-
pared to the value of combustible sulfur caused by higher
ash content. Concentration of H2S in dry product gas
decreased with k increase, except in the third and fifth
group of experiments. Gasification efficiencies (Figs. 4
and 6) decreased with k increase, which can be explained
 N. Crnomarkovic et al. / Fuel 86 (2007) 194–202
by product gas composition, i.e. the method of calculation
for this coefficient, which was described earlier.
4.2. Influence of mass ratio H2O/coal using high-temperature
steam
The influence of H2O/coal mass ratio was investigated
using data obtained in the experiments with fine PC –
groups (1) (with introduction of steam) and (2) (without
steam introduction). Increase of H2O/coal mass ratio in
experiments occurs by introduction of hydrogen into the
reactor and its combustion in pure oxygen stream. The
introduction of hydrogen increases the vapor content in
the beginning of the process, and also the quantity of inlet
heat in process. The basic reactions of vapor are with car-
bon and CO. Reaction of vapor with carbon is endother-
mic, and with increased temperature, contents of H2 and
CO in the product gas also increase. Reaction of vapor
with CO is exothermic, and with increased temperature,
H2 and CO2 contents in the product gas decrease. In the
experiment without introduction of hydrogen, water vapor
is in the gaseous phase, since it has been introduced with
coal, and due to combustion of a portion of coal hydrogen.
The carbon conversion (Fig. 3) decreased with an
increase of H2O/coal mass ratio. Quite the opposite was
anticipated since with introduction of steam, the conversion
of carbon would increase due to the steam reaction with car-
bon from coal. The obtained results may be explained by
the following: since steam was obtained by hydrogen com-
bustion, introduction of steam (i.e. higher steam mass flow
rate), both the temperature and the mass flow rate of the
product gas increased. This caused the gas velocity to rise,
which resulted in lower particle residence time in the reactor
(reduction of approximately 0.3 s at k = 0.53, Fig. 3). This
reduced residence time presumably had a greater influence
on burn-out degree (level) than the rise of steam content.
Increase of H2O/coal mass ratio influenced the following:
rise of H2 (Fig. 3), CO (Fig. 3) and HCN content (Fig. 4) and
decrease of CO2 (Fig. 3), NH3 (Fig. 4) and H2S content
(Fig. 4) in dry product gas. Increase of H2 and CO contents
in the produced gas are probably influenced by steam reac-
tion with carbon (H2O + C ! H2 + CO), but there was
not a carbon conversion increase to confirm this statement.
The increase of H2 content could have come as a result of
steam reaction with CO (H2O + CO ! H2 + CO2), but then
the CO content should have decreased and CO2 content
should have increased, which was not the case. This sug-
gested that the increase of CO was probably a result of
CO2 reactions with carbon (CO2 + C ! 2CO). With
increasing H2O/coal mass ratio gasification efficiency
(Fig. 4) increased.
4.3. Influence of mean mass diameter of pulverized
coal and size fraction
The influence of mean mass diameter of PC is investi-
gated in order to compare the first and the third groups
201
of experiments. The influence of coal size fraction on char-
acteristics of gasification is investigated in order to com-
pare the fourth and the fifth groups of experiments.
In experiments with different mean mass diameters of
PC and coal size fractions, the influence of coal particles
outer surface area was investigated. Separated coal size
fractions also include the influence of changed ash content.
In comparison with the mean coal sample (Table 2), the
size fraction R0/50 has almost double, the size fraction
R50/90 almost 75% higher, and the size fraction R90 slightly
smaller ash content. The obtained results almost confirm
earlier performed investigations of the influence of increase
of PC mean mass diameter.
The carbon conversion (Fig. 5) decreased with increas-
ing the mean mass diameter of PC. The obtained values
of carbon conversion are relatively high in comparison
with values received previously [13], for much lower
changes of PC mean mass diameter. With increasing of
the mean mass diameter, the coal particle residence time
in the reactor increased (Fig. 5).
With increasing of PC mean mass diameter, H2 (Fig. 5)
and CO contents (Fig. 5) decreased, and CO2 (Fig. 5), NH3
(Fig. 6), HCN (Fig. 6) and H2S (Fig. 6) contents in dry
product gas increased. Also, the vapor content in wet prod-
uct gas increased. This means that contents of all incom-
bustible components of the product gas increased,
including NH3 and H2S products, which are necessarily
removed from the product gas before its commercial use.
Also, with increasing of PC mean mass diameter gasifica-
tion efficiency (Fig. 6) decreased.
Influence of PC size fractions is the same as the influence
of increase of PC mean mass diameter. Contents of CO,
HCN and H2S in dry product gas were higher for R90 size
fraction (Figs. 5 and 6), but the contents of CO2, H2 and
NH3 were higher for R50/90 size fraction (Figs. 5 and 6).
This resulted in slightly higher gasification efficiency for
the R50/90 size fraction (Fig. 6).
5. Conclusions
Experimental investigation of the role of steam in
entrained flow coal gasification was performed with a lignite
type of coal. In experiments with steam addition, H2 and
CO2 concentrations increased while CO concentration
decreased with excess oxygen coefficient k increase. In exper-
iments without steam addition, H2 and CO2 concentrations
decreased while CO concentration increased with k increase.
Carbon conversion increased with k increase in both groups
of experiments. The concentrations of H2 and CO increased
with an increase of H2O/coal ratio due to introduction of
high-temperature steam in the process, while CO2 concen-
tration and carbon conversion decreased. Product gas of
PC with larger mass diameter dav = 211.95 lm had lower
contents of H2 and CO, and larger contents of CO2, when
compared to the product gas of PC with smaller mass diam-
eter dav = 79.08 lm. Product gas obtained in the experiment
with R50/90 coal size fraction had larger contents of H2 and
202 N. Crnomarkovic et al. / Fuel 86 (2007) 194–202
lower contents of CO and CO2, when compared to the prod-
uct gas obtained in the R90 PC size fraction experiment.
Acknowledgements
This work was supported by the Ministry of Science and
Environmental Protection of the Republic of Serbia and
Electric Power Industry of Serbia.
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