ZERO TEST EMISSIONS OF SULPHUR DIOXIDE FROM LARGE COAL

UNDER STAGED FLUIDIZED BED COMBUSTION

W. Z. KHAN and B. M. GIBBS

Department of Chemical Engineering, King Fahd University of Petroleum and Minerals, Dhahran,
Kingdom of Saudi Arabia

(Received 10 July, 1995; accepted 9 May, 1996)

Abstract. This paper reports the emissions of SO2 from large coal under staged combustion without

any additive. A stainless steel combustor, 2 m high and 0.3 0.3 m in cross section was used.
Fluidizing air was supplied through a multihole distributor. An adjustable secondary air injector was
used along the vertical axis of the combustor to introduce secondary air in the freeboard. From 040%
of total air was injected in the freeboard above the bed. The experiments were carried out at fluidizing
velocities of 12 m s 1 , bed temperatures of 11031153  K, 2040% excess air, and bed particle
sizes of 665 m. Bed temperature and level of air staging had the most significant effect on SO2
emissions.
Key words: fluidized bed, sulphur dioxide emissions, staged combustion

1. Introduction

Sulphur dioxide is one of the most widespread constituent of global pollution.

It is emitted during the combustion of most fuels. Emissions of SOx and NOx
have increased throughout the world due to increased burning of fossil fuels. The
air-staged combustion technique, if coupled with the addition of limestone, can
economically reduce sulphur dioxide (Khan, 1995).
The literature reports two possible methods for staged combustion, which are (a)
two beds in series with two distributors (used by Tomita, M. et al., 1980) and, (b) a
simple air staging technique. In the staged operation mode, the combustion air is
separated into a primary air stream which constitutes the fluidizing air supply to the
bed and a secondary air stream that is injected higher up in the bed or freeboard.
All the coal is injected into the primary stage so that the bed is maintained at
substoichiometric conditions. Combustion is completed following the introduction
of secondary air. However, overall excess air conditions are maintained in a similar
way as in conventional operation. Air-staging is a proven technique to reduce NOx
emissions, but at the same time, it causes increase in SO2 emissions. This increase is
due to the presence of secondary air in the freeboard that allows further combustion
(Bramer et al., 1988; Modrak et al., 1982; Nack et al., 1980; Tatebayashi et al.,
1980; Valk et al., 1987; Valk and Bramer, 1989; Zaunder et al., 1987).
The literature lack in providing enough data on sulphur dioxide emission under
staged combustion without a sorbent. Tatebayashi et al. (1980) have reported that in
two-stage combustion, primary air ratio, bed temperature, secondary air injection
height and fluidizing velocity have significant effects and that other parameters do

Water, Air, and Soil Pollution 96: 291300, 1997.

c 1997 Kluwer Academic Publishers. Printed in the Netherlands.

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292 W. Z. KHAN AND B. M. GIBBS

not. The objective of this study was to determine the effects of different ratios of
primary : secondary air on the generation of sulphur dioxide so that these data
could be used as a baseline for comparing efficiency of SO2 reduction if a sorbent
is added to the bed.
Sibtain (1989) reports a 4% increase in SO2 emission at 2 m s 1 fluidizing
velocity, 40% excess air and 65:35 staging. He attributes this increase to the lower
retention of SO2 by the calcareous component of ash due to less availability of
oxygen or due to regeneration of SO2 , captured by the calcareous part of ash;
whereas Barnes (1988) says that at high staging, this increase is due to the carryover
of unburnt fuel sulphur into the freeboard. Barnes (1988) found a significant effect
of bed temperature on SO2 emissions, which indicates that the rate of formation of
SO2 in the freeboard is affected by staging and changes in the temperature profile
of the freeboard.
In this study, the simple air staging technique was adopted where 60 to 85%
of the total air is injected through the distributor and the remainder is injected in
the freeboard of the fluidized combustor. The secondary air is injected at a height
of 100 cm above the distributor. This fixed height is used throughout the staged
combustion experiments. The 100 cm height was chosen on the basis of findings of
Barnes (1988) who used the same rig (0.3 m2 fluidized bed combustor), and found
that SO2 emissions decreased as the point of injection moved away from the bed
surface.

2. Experimental Procedure

The bed was preheated by a propane burner, fixed above the bed, and the fluidizing
air flow rate was set at the lowest level to minimize heating time. Coal feeding
was started when the bed temperature reached 823  K. The proximate and ultimate
analyses of the coal is given in Table I. When the bed temperature reached 1073  K,
the required coal feed rate was fixed, the propane burner was switched off and the
fluidizing air set at the required level. The secondary air was injected through a
secondary air injector, consisting of a stainless steel pipe with a 1.5 cm inside
diameter, containing twelve holes of 3.18 mm diameter. This injector was located
on the vertical axis of the combustor and its position above the bed or in the free-
board was adjustable. The bed temperature was maintained by using an adjustable
cooling coil. Values of O2 , CO, CO2 and SO2 were recorded continuously. Figure 1
demonstrates the features of the fluidized bed combustor.

3. Experimental Methods

The SO2 in the flue and the axial concentration profiles of SO2 and O2 through the
combustor were measured for a fluidizing velocity of 12 m s 1 ; the bed material

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 ZERO TEST EMISSIONS OF SULPHUR DIOXIDE 293
Table I
Typical analysis of coventry coal

Proximate analysis (dry basis) weight %

Ash 6.22
Volatile matter 33.00
Fixed carbon 60.78

Ultimate analysis (dry basis) weight %

Carbon 77.51
Hydrogen 4.8
Oxygen 8.5
Nitrogen 1.43
Sulfur 1.5
Moisture 5.0
Gross calorific value (MJ/kg) 31.185

Figure 1. Main features of fluidized bed combustor and ancillaries.

was sand, of 0.6650.700 mm size, staging level 040%, excess air 2040%, bed
temperature 11031153  K and Ca/S molar ratio of 3.

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294 W. Z. KHAN AND B. M. GIBBS

1
Figure 2. Effect of bed temperature on SO2 emissions F.V. = 1.0 m s .

4. Results and Discussion

4.1. EFFECT OF BED TEMPERATURE

Figure 2 illustrates the results for 1.0 m s 1 fluidizing velocity and two staging
levels of 70 : 30 and 60 : 40 and 20% excess air. At 40% excess air level, the SO2
emission increased when the amount of the secondary air was increased from 30
to 40%. The SO2 emissions are very sensitive to bed temperature. During 30%
secondary air, the rate of increase in SO2 emission was 0.02 ppm K 1 for the
temperature range of 11031123  K and 0.008 ppm K 1 for 11231153  K, and
in the case of 40% secondary air, this rate increased from 0.02 to 0.026 ppm
K 1 and 0.008 ppm K 1 to 0.022 ppm K 1 for the corresponding temperature
range. The SO2 emissions at different secondary air ratios appear to be affected
by combustion efficiency. Higher emissions at higher secondary air are due to
increased combustion of sulphur in the bed and freeboard. Figure 3 indicates a
similar trend obtained at a fluidizing velocity of 1.5 m s 1 and at both excess
air levels of 40 and 20%. The results demonstrate that the extent of SO2 emission
during staged combustion is strongly influenced by the amount of secondary air and
bed temperature. The higher emissions of SO2 for 20% excess air level, 1153  K
and for 30% secondary air (the expected deviation) are due to variations in the coal
feed rate during the run.
The effect of bed temperature for 2.0 m s 1 fluidizing velocity is shown in
Figure 4. The results obtained at 20% excess air for staging levels of 70 : 30 and
60 : 40 illustrate a similar trend i.e. higher emission at higher temperature. However,

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 ZERO TEST EMISSIONS OF SULPHUR DIOXIDE 295

1
Figure 3. Effect of bed temperature on SO2 emissions F.V. = 1.5 m s .

1
Figure 4. Effect of bed temperature on SO2 emissions F.V. = 2.0 m s , excess air 20%.

the rate of increase with temperature was lower compared to the emission at 1.0 and
1.5 m s 1 , the reason could be the lower residence time due to the high fluidizing
velocity. Valk et al. (1987) reports a 70% increase in SO2 emissions at a bed
temperature of 1153  K when it was increased from 1063  K. At 1153  K, oxygen
in the flue decreased from 10 to 6.7%, CO2 increased from 9.3 to 12.3% and CO
decreased from 0.45 to 0.1%.

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296 W. Z. KHAN AND B. M. GIBBS

Figure 5. Effect of PACR on SO2 emissions F.V. = 1.5 m s 1

, bed temperature 1123  K.

4.2. EFFECT OF EXCESS AIR

An increase in SO2 emissions as excess air is reduced was observed at both fluidiz-
ing velocities and all secondary air ratios. The SO2 emissions were increased by
10% when excess air was reduced from 40 to 20% at an overall fluidizing velocity
of 1.0 m s 1 and at primary to secondary air ratio of 60 : 40. At 70 : 30 staging,
only a 2% increase in SO2 was observed at equivalent conditions. The unexpected
trend at 40% secondary air for 1.5 m s 1 fluidizing was due to lower combustion
efficiency during this particular run.
At a particular air staging level, any change in excess air level causes a change
in primary air to coal ratio (PACR). This ratio is defined as the ratio of primary air
supplied to the stoichiometric air required, calculated from the coal composition. At
40% staging, an excess air level of 40% resulted in a PACR of 0.84, and 20% excess
air resulted in a PACR of 0.72. At a low PACR (<1 induction of substoichiometric
first stage), an increase in carry over of unburnt fuel sulphur species into the
freeboard where it subsequently oxidizes to SO2 could also increase SO2 emissions.
This indicates that oxidation of some of the sulphur bearing compounds to SO2
cannot be ignored in the second stage (above the bed). The effect of PACR on SO2
emissions can be seen in Figure 5.
Zaunder et al. (1987) report that air : fuel ratio in the primary stage has significant
influence on both 1) the rate of sulphur release from the coal and the ratio of H2 S
formed during fuel-rich combustion and, 2) the resulting primary and secondary
stage gas temperature. Valk and Bramer (1989) report that primary air factor and
coarseness of bed material has no significant effect on combustion efficiency, but

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 ZERO TEST EMISSIONS OF SULPHUR DIOXIDE 297

Figure 6. Effect of fluidizing velocity on SO2 emissions excess air 20%, bed temperature 1123  K.

SO2 increases with the decrease in PACR for both fine and coarse sand. Fine sand
produce a more reducing environment.

4.3. EFFECT OF FLUIDIZING VELOCITY

Figure 6 gives the effect of fluidizing velocity on SO2 emission at two staging
levels 70 : 30 and 60 : 40 and 20% excess air. An increase in SO2 emissions at high
fluidizing velocity can be attributed to reduced reaction time via a shorter residence
time in the oxidation zone and generation of SO2 from carried over unburnt particles
of coal. This effect of fluidizing velocity on SO2 emission is in agreement with the
previous findings of Tatebayashi et al. (1980).

4.4. AXIAL CONCENTRATION PROFILES OF SO2 AND OXYGEN

The axial concentration profile of SO2 and O2 at 40 and 20% excess air, 70 : 30 and
60 : 40 staging levels for 1.0 m s 1 fluidizing velocity and 1123  K bed temperature
is shown in Figure 7, and for 1.5 m s 1 fluidizing velocity in Figure 8. The SO2
concentration profile indicates the higher formation of SO2 in the bed and lower in
the freeboard compared to emissions from unstaged combustion (Khan et al., 1991).
The axial profile of SO2 needs to be linked with the oxygen profile. The oxygen
profile explains the trend of SO2 emission and supports the argument that, during
staged combustion, the bed stoichiometry change and higher amounts of oxygen
are consumed in the oxidation of coal near the coal injection point. For example,

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298 W. Z. KHAN AND B. M. GIBBS

1
Figure 7. Axial concentration profile of SO2 /O2 through the combustor F.V. = 1.0 m s , bed
temperature 1123  K.

1
Figure 8. Axial concentration profile of SO2 /O2 through the combustor F.V. = 1.5 m s , bed
temperature 1123  K.

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 ZERO TEST EMISSIONS OF SULPHUR DIOXIDE 299
during unstaged combustion at 1.0 m s 1 , 40% excess air, the SO2 emissions were
around 1000 ppm at 42 cm above the distributor and oxygen was 2.9%, whereas
during staged combustion (at 70 : 30) for similar operating conditions, the SO2
emissions at 42 cm were above 1300 ppm and oxygen was 1.55%. The oxygen
partial pressure measurements (PO2 <10 11 atm) in a 16 MW fluidized bed boiler
reported by Lyngfelt et al. (1988) indicate reducing conditions and even at an air
factor of 1.4 (40% excess air), 8090% of the time, the bed is under reducing
condition.

4.5. EMISSIONS OF CO AND COMBUSTION EFFICIENCY

During staged combustion, the CO level was consistently found to be higher com-
pared to that in an unstaged operation under similar operating conditions. The CO
level in the flue increased with an increase in staging levels and, at constant staging,
it increased as the excess air level was lowered. This increase could be due to a
higher inventory of unburnt hydrocarbon in the freeboard as compared to unstaged
combustion. The higher CO concentration in the flue during staged combustion is
in agreement with the previous findings of Tatebayashi et al. (1980) and Valk et al.
(1987) and is not surprising.
A decrease in combustion efficiency during staged combustion has been reported
by Tatebayashi et al. (1980), Valk et al. (1987) and Modrak (1982). The drop in
combustion efficiencies in the present investigation was in the range of 210%. The
combustion efficiencies were found to be in the range of 8590% for a coal size of 3
16 mm depending on the operating parameters. The lower combustion efficiencies
were observed at higher staging levels. The efficiency was further dropped when
the staged combustion was coupled with low excess air levels, which again is
not surprising. The decrease in combustion efficiency at higher staging is due to
insufficient secondary air residence time coupled with a low freeboard temperature.

5. Conclusion

The results indicate that SO2 emissions increase with a rise in bed temperature.
The extent of SO2 emission during staged combustion is strongly influenced by the
amount of secondary air and bed temperature. The rate of increase was between
0.008 and 0.02 ppm/ K for temperature range of 11031153  K. The rate of rise
was higher for 1.5 m s 1 fluidizing velocity than 1.0 m s 1 . For a given bed tem-
perature and excess air level, increasing the level of air staging or lowering the
PACR causes an increase in SO2 emissions. A lower combustion efficiency was
observed at higher staging levels, however, the drop was in the range of 210%.

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300 W. Z. KHAN AND B. M. GIBBS

References
Barnes, J. P.: 1988, Abatement of Nitric Oxide Emission from a Coal-Fixed Fluidized Bed Combus-
tor, Ph.D. Thesis, Department of Fuel and Energy, University of Leeds, Leeds, U.K.
Bramer, E. A. et al.: 1988, Sulphur Capture Under Reducing Conditions at Atmospheric Fluidized
Bed Combustion, Fourth International Fluidized Bed Combustion Conference, London, U.K.,
Vol. 1, p. I/11/1I/11/11.
Khan, W. Z. and Gibbs, B. M.: 1991, The Effects of Bed Temperature and Oxygen Stoichiometry
on Sulphur Dioxide Captured by Limestone in a Fluidized Bed Combustor, 11th International
Conference on Fluidized Bed Combustion. Montreal, Canada, ASME.
Khan, W. Z. and Gibbs, B. M.: 1995, Fuel, 74(6), p. 800805.
Lyngfelt, A. et al.: 1988, The Effect of Reducing Conditions on Sulphur Capture A Comparison
of Three Boilers, Fourth International Fluidized Bed Combustion Conference, London, U.K.,
Vol. II, p. II/10/1-II/10/11.
Modrak, T. M., Tang, J. T. and Auliso, C. J.: 1982, Sulphur Capture and NOx Reduction on the
6 60 AFBC Test Facility, Preprint ACS, Div. Fuel Chemistry, pp. 226242.

Nack, H. et al.: 1980, Control of SO2 and NOx Emissions by Bottles Multisolid Fluidized Bed
Combustion Process, Sixth International Conference on Fluidized Bed Combustion, Atlanta,
Georgia, USA, ASME, Vol. III, pp. 979985.
Sibtain, S. F.: 1989, The Control of Nitric Oxide Emission from a Coal-Fired Fluidized Bed Com-
bustor, Ph.D. Thesis, Department of Fuel and Energy, University of Leeds, Leeds, U.K.
Tomita, M., Hiramo, T. Adachi, T., Yamaguchi, H. and Horio, M.: 1980, Two-Staged Fluidized Bed
Combustion, Sixth International Conference on Fluidized Bed Combustion, Atlanta, Georgia,
USA, ASME, Vol. II, pp. 623631.
Tatebayashi, J. Okada, Y., Yano, K. and Ikeda, S: 1980, Simultaneous NOx and SOx Emissions
Reduction with Fluidized Bed Combustion, Sixth International Conference on Fluidized Bed
Combustion, Atlanta, Georgia, USA, ASME, Vol. III, pp. 986995.
Valk, M., Bramer, E. A. and Toissant, H. H. J.: 1987, Effect of Staged Combustion of Coal on
Emission Levels of NOx and SOx in a Fluidized Bed, 9th International Conference on Fluidized
Bed Combustion, Boston, USA, ASME, Vol. II, pp. 784794.
Valk, M. and Bramer, E.: 1989, Optimal Staged Combustion Conditions in a Fluidized Bed for
Simultaneous Low NOx and SO2 Emission Levels, Tenth International Conference on Fluidized
Bed Combustion, San Francisco, CA, USA, ASME, Vol. II, pp. 9951001.
Zaunder, B. et al.: 1987, SOx NOx Control in a Staged Cyclone Coal Combustor with Limestone
Injection, Preprint of Papers Presented at the 194th National Meeting at Louisiana, New Orleans,
32(4), pp. 375382.

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