Pulverized coal combustion and NO

x
emissions in high
temperature air from circulating fluidized bed
Qinggang Lu
a,

, Jianguo Zhu
b
, Tianyu Niu
b
, Guoliang Song
a
, Yongjie Na
a
a
Institute of Engineering Thermophysics, Chinese Academy of Sciences, Beijing 100190, PR China
b
Graduate School of the Chinese Academy of Sciences, Beijing 100190, PR China
A R T I C L E I N F O A B S T R A C T
Article history:
Received 14 December 2007
Received in revised form12 May 2008
Accepted 17 May 2008
A new technique of achieving high temperature air was adopted by combustion in high
excess air ratio in a circulating fluidized bed (CFB). Experiments on pulverized coal
combustion in high temperature air from the CFB were made in a down-fired combustor
with the diameter of 220 mm and the height of 3000 mm. High temperature air with lower
oxygen concentrations can be achieved steadily and continuously by combustion in the
circulating fluidized bed. Pulverized coal combustion in high temperature air shows a
uniform temperature profile along the axis of the down-fired combustor and the
combustion efficiency is 99.8%. The NO
x
emission is 390 mg/m
3
, 13% lower than the
regulation for thermal power plants in China. The HCN and NH
3
emissions, as well as N
2
O,
are about zero in the exhaust.
2008 Published by Elsevier B.V.
Keywords:
Pulverized coal combustion
High temperature air
Circulating fluidized bed
NO
x
1. Introduction
Technology of high temperature air combustion has been
successfully used to gaseous fuels with many advantages,
such as energy saving, good flame stability and low NO
x
emissions [13]. It is expected that this technology can also be
used to pulverized coal combustion.
In 2002, Suda et al. [4] studied pulverized coal combustion
behavior and NO
x
emissions in high temperature air proposed
by an electric heater and a heat exchanger. The experiments
revealed that the high temperature air combustion could
significantly reduce NO
x
emissions and improve burnout of
coal. Also, the results of numerical simulations had a good
agreement with those of experiments [5]. It becomes more and
more interesting and attracting to combust pulverized coal in
high temperature air, especially in China with coal as major
energy.
High temperature air can be achieved by a pair of
honeycomb heat exchangers with clean gas as fuel, alterna-
tively switched in a time period of about 25 s [68]. However, it
is difficult to combust pulverized coal directly in such
equipment because coal ash in flue gas plugs the heating
elements.
A new technique of achieving high temperature air was
adopted by combustion in high excess air ratio in a circulating
fluidized bed (CFB) [9]. CFB combustion has advantages of
combustion stability, fuel feasibility and low pollutant emis-
sions [1013].
A test rig was built and experiments were carried out. The
process of pulverized coal combustion and NO
x
emissions in
high temperature air were discussed in this paper.
2. Experiment
2.1. Test rig
A test rig diagram is shown in Fig. 1. It is composed of a down-
fired combustor (DFC), a circulating fluidized bed (CFB) and an
auxiliary system. A horizontal tube with 48 mm in diameter
and 300 mm in length is used to guide high temperature air
from the CFB to the DFC.
F U E L P R O C E S S I N G T E C H N O L O G Y 8 9 ( 2 0 0 8 ) 1 1 8 6 1 1 9 2
Corresponding author. Tel.: +86 10 82543119.
E-mail address: zhujianguo@mail.etp.ac.cn (Q. Lu).
0378-3820/$ see front matter 2008 Published by Elsevier B.V.
doi:10.1016/j.fuproc.2008.05.008
avai l abl e at www. sci encedi r ect . com
www. el sevi er. com/ l ocat e/ f upr oc
Total air flow supplied to the circulating fluidized bed with
the diameter of 100 mm and the height of 3000 mm, with coal
as fuel, is much higher than that for stoichiometric combus-
tion and O
2
concentration is about 8% with temperature about
1073 K at the outlet of the circulating fluidized bed. The gas
from the circulating fluidized bed can be named as high
temperature air with lower oxygen concentration. Similar to
ordinary flue gas, the composition of high temperature air
includes O
2
, N
2
, CO
2
, H
2
O and NO
x
etc. The function of the
circulating fluidized bed is to provide high temperature air for
pulverized coal combustion in the down-fired combustor with
the diameter of 220 mm and the height of 3000 mm.
Pulverized coal is supplied to the down-fired combustor by
a screwfeeder and pneumatically fed to a nozzle with primary
air flow of 2 m
3
/h. The primary air is at atmospheric
temperature. The nozzle is at the top center of the down-
fired combustor and 7 mm in diameter. The high temperature
air from the circulating fluidized bed can be named as
secondary air for pulverized coal combustion. In order to
decrease the NO
x
emissions for pulverized coal combustion in
high temperature air, tertiary air with oxygen concentration of
21% at atmospheric temperature is supplied to the down-fired
combustor at the position of 600 mm below the nozzle.
There are 9 thermocouples in the test rig, 3 NiCr/NiSi
thermocouples in the CFB and 6 Pt/PtRh thermocouples in the
DFC with their accuracy of 0.5% t. Temperatures are measured
and recorded in a computer at an interval of 6 s. There are six
sampling ports. One is at the outlet of the cyclone for sampling
high temperature air from the CFB, one is behind the bag filter
for sampling exhaust from the down-fired combustor and the
other four are at the down-fired combustor 100 mm, 300 mm,
800 mm and 1800 mm below the nozzle. Gas samples are
continuously drawn fromthe gas sampling ports witha water-
cooled treatment for quenching gas reactions. All the gas
samples are dried and filtered before they enter individual on-
line analysers. O
2
and CO
2
are measured by a portable analyser
(KM9106) with an accuracy of 0.1%. CO, N
2
O, NO, NO
2
, HCNand
NH
3
are measured by a Gasmet FTIR DX-400 analyser with an
accuracy of 1 ppm. Gas analysis data is also recorded at an
interval of 6 s.
Noticeably, the gas composition and temperature at the
position of 0 mm below the DFC nozzle are those of high
temperature air from CFB.
2.2. Coal characteristics
A bituminous coal was used in the experiments for both the
circulating fluidized bed and the down-fired combustor. Its
proximate and ultimate analyses are listed in Table 1.
Bituminous coal, smaller than 2 mm with d
50
cut size of
0.4 mm, was screwed into the riser at a port 240 mm above the
bottom, andthesizedistributionof coal particles isgiveninFig. 2.
Fig. 1 Schematic of the experimental apparatus.
Table 1 Analysis of the bituminous coal
Items Data
Proximate analysis w/% Moisture
a
11.00
Volatile matter
b
30.61
Fixed carbon
a
51.99
Ash
a
14.08
Low heating value
a
/(MJ/kg) 24.17
Ultimate analysis
b
w/% Carbon 83.54
Hydrogen 4.57
Nitrogen 0.85
Oxygen 9.52
Sulfur 1.53
Note:
a
As received;
b
Dry ash free basis.
Fig. 2 Size distribution of coal particles.
Fig. 3 Size distribution of quartz sand.
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Quartz sand smaller than 0.7 mm and in 2.5 kg was added
into the riser as circulating fluidized bed material, and the size
distribution is given in Fig. 3.
The size distribution of pulverized coal is given in Fig. 4,
smaller than 500 m with 50% cut size about 120 m.
2.3. Experimental conditions
Experimental conditions are listed in Table 2.

ER
is the air equivalence ratio in the reducing zone of the
down-fired combustor at the range of 0600 mm below the
nozzle.

ER
is defined as:
Oxygenflowinprimaryair Oxygenflowinsecondaryair
Oxygenflowinprimaryair Oxygenflowinsecondaryair
Oxygenflowintertiaryair=Excess air ratio
In the experiments,
ER
is set to 0.7, about 70%of theoretical
air flow supplied to the down-fired combustor at the range of
0600 mm below the nozzle. The furnace temperature is
controlled at about 1373 K for protecting the furnace material
from damage. The pulverized coal feed rate is 2.0 kg/h and the
excess air ratio is 1.2.
3. Results and discussion
3.1. Combustion characteristics
Three thermocouples were used to measure the gas tempera-
ture intheCFB. One is at theoutlet of theCFBfor measuringhigh
temperature air, the other twoare at the positionof 100 mmand
2950 mm above the air distribution plate, respectively.
The temperatures variation with time at the CFB is shown
in Fig. 5. It is obvious that high temperature air with oxygen
concentration of 8% and temperature of 1073 K can be
achieved steadily and continuously by coal combustion in
high excess air ratio in the CFB.
The temperature profile along the axis of the down-fired
combustor, shown in Fig. 6, is uniform, the maximum tempera-
turedifferenceisabout 297K, whichis far belowthoseof ordinary
combustion of pulverized coal [14], the maximum flame
temperatureis 1373Kat thepositionof 300mmbelowthenozzle.
At the position of 100 mm below the nozzle, the furnace
temperature is about 1291 K and the residence time of
pulverized coal is about 0.1 s. So, the pulverized coal fueled
into the combustor has a fast heating rate of 10,180 K/s, a
positive effect to reduce the ignition time and to increase the
release rate of volatile matter.
According to the investigation of Yu et al. [15], heating
conditions play an important role during devolatilization by
affecting the yield of volatile species, thermoplastic properties,
swelling andchar structure. Anincreasedheating rate increases
swelling and porosity, as well as the yield of tars and volatile
matter. The higher heating rateof pulverizedcoal is beneficial to
accelerate the combustion process and to stabilize the flame.
CO
2
concentration profile along the axis of the down-fired
combustor is shown in Fig. 7. It is evident that the average
concentration of CO
2
is higher than that of ordinary pulverized
coal combustion, which cannot only decrease the maximum
flame temperature but also reduce the formation of nitrogen
oxides [1618].
CO concentrations along the axis of the down-fired
combustor are shown in Fig. 8. CO concentrations at the
range of 0600 mm below the nozzle are higher than those of
600 mm behind the nozzle, which is due to 70% theoretical air
flow supplied to the range of 0600 mm below the nozzle.
Fig. 4 Size distribution of pulverized coal.
Table 2 Experimental conditions for pulverized coal
combustion
Parameter Data
Primary air temperature /K 293
O
2
concentration in primary air /% 21
Secondary air temperature /K 1073
O
2
concentration in secondary air /% 8
Tertiary air temperature /K 293
O
2
concentration in tertiary air /% 21
Pulverized coal feed rate /kg/h 2.0
Furnace temperature / K 1373

ER
in the reducing zone 0.7
Excess air ratio 1.2
Fig. 5 Temperature variations with time at the CFB.
Fig. 6 Temperature profile along the axis of DFC.
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In the experiment, ash was sampled at the position of
300 mm, 1800 mm and 3000 mm below the nozzle, respec-
tively. The volatile remaining rate, shown in Fig. 9, is the ratio
of the volatile content in sampled ash to the volatile content in
the raw coal from DFC. It can be calculated by the ash balance
and the calculation formula is:
R
V;ii

V
SA;ii
A
RC
V
RC
A
SA;ii
1
Where:
R
V,i i
Remaining rate of volatile matter in i i section, %
V
SA,i i
Volatile content of sampled ash in i i section, %
A
RC
Ash content in row coal, %
V
RC
Volatile content in raw coal, %
A
SA,i i
Ash content of sampled ash in i i section, %
The volatile remaining rate is about 7.6% at the position of
300 mm below the nozzle, lower than Suda et al.'s [4] results.
The volatile has a fast release rate at the range of 0300 mm
below the nozzle than that of 300 mm behind the nozzle.
The fixed carbon remaining rates along the axis of the
down-fired combustor are shown in Fig. 10. The calculatin
method of fixed carbon remaining rate is similar to that of
volatile remaining rate, and it can be calculated as:
R
FC;ii

FC
SA;ii
A
RC
FC
RC
A
SA;ii
2
Where:
R
FC,i i
Remaining rate of fixed carbon in i i section, %
FC
SA,i i
Fixed carbon content of sampled ash in i i section, %
FC
RC
Fixed carbon content in raw coal, %
At the position of 300 mm below the nozzle, the fixed
carbon remaining rate is about 21.3%, and it is close to zero at
the position of 1800 mm below the nozzle.
In the experiments, the air flow supplied to the range of 0
300 mm below the nozzle is accounted for 70% of theoretical
air flow for pulverized coal combustion. So, the fixed carbon
is difficult to convert into other species totally at the range of
0300 mm below the nozzle.
The combustion rate of fixed carbon is mainly dependent
on temperatures, sizes and oxygen concentrations. It can be
described as:
dm
p
dt
pkq
P
d
2
PX
O2
: : :
3
Where k is the reaction rate constant, d the mean size,
P
the particle density, P the pressure and X
O
2
the oxygen
concentration. k can be described as [19]:
k
1
1=k
c
1=k
d
4
Where, k
c
is the chemical rate coefficient, and can be
described as:
k
c
4:016e 08 exp
29790
RT
p

5
k
d
is the diffusion rate coefficient, and can be described as:
k
d

2D
d
6
R is the universal gas constant, D the mass diffusion
coefficient, d the mean diameter of pulverized coal and T
p
the
particle surface temperature.
In the conditions of pulverized coal combustion in high
temperature air from the CFB, the calculation value of k
c
/k
d
is
about 1.08. So, the combustion rate of fixed carbon is
Fig. 7 CO
2
concentration along the axis of DFC.
Fig. 8 CO concentration along the axis of DFC.
Fig. 9 Volatile remaining rate along the axis of DFC.
Fig. 10 0 Fixed carbon remaining rate along the axis of DFC.
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controlled by both the chemical reaction rate and the diffusion
rate.
The combustion efficiency can be defined as:
CombustionEfficiencyg
f Coal Heating Values Heating Values of Unburnedcarbon;
HydrogenandCOgases generationg= Coal Heating Values
The mass fraction of combustible substance is 1.8% in the
fly ash fromthe bottomof the water cooler, and COis 100 ppm
at the outlet of the down-fired combustor. So, the combustion
efficiency is 99.8%.
3.2. Distribution of gaseous nitrogen species
The remaining rates of fuel-nitrogen, shown in Fig. 11, can be
calculated as:
R
N;ii

N
SA;ii
A
RC
N
RC
A
SA;ii
7
Where:
R
N,i i
Remaining rate of fuel-N in i i section, %
N
SA,i i
N content of sampled ash in i i section, %
N
RC
N content in raw coal, %
At the position of 300 mm below the nozzle, N remaining
rate is about 21.8%. About 95% of the volatile matter has
released at the range of 0300 mm below the nozzle, fuel-
nitrogen is mainly in char at the range of 300 mm below the
nozzle. Fuel-nitrogen can be divided into volatile-nitrogen and
char-nitrogen[2022]. However, it is difficult to give the ratio of
volatile-nitrogen and char-nitrogen.
The probability of char-nitrogen to NO
x
increases as the
tertiary air supplied to the down-fired combustor at the
position of 600 mm below the nozzle.
HCN concentrations along the axis of the down-fired
combustor are shown in Fig. 12.
The maximumconcentrationof HCNis about 10 ppmat the
position of 100 mm below the nozzle, mainly from the release
of volatile-nitrogen. It is sure that the volatile matter has
started its release at an early time at the range of 0100 mm
below the nozzle. The HCN concentration is about zero at the
range of 300 mm below the nozzle.
HCN, an instable species, can be further converted into
other species [23].
Generally, in oxidizing atmosphere, the reaction of HCN is
as follows:
HCN
7
4
O
2
X NOCO
2

1
2
H
2
O R:1
However, in reducing atmosphere, the reaction of HCNis as
follows:
HCN
5
4
O
2
X
1
2
N
2
CO
2

1
2
H
2
O R:2
R.2 may be the major reaction route of HCN in the
experimental conditions.
The injection of NH
3
to the flue gas, widely used in power
plants, is an effective method to reduct nitrogen oxides [24,25].
NH
3
concentrations along the axis of the down-fired
combustor are shown in Fig. 13. NH
3
has an initial concentra-
tion of about 20 ppmin the high temperature air fromthe CFB,
decreasing continuously along the axis of the down-fired
combustor.
Fig. 11 1 N remaining rate along the axis of DFC.
Fig. 12 2 HCN concentration along the axis of DFC.
Fig. 13 3 NH
3
concentration along the axis of DFC.
Fig. 14 4 N
2
O concentration along the axis of DFC.
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In the reducing zone at the range of 0600 mm below the
nozzle, NH
3
may take part in some reactions of NO reduction.
NO NH
i
N
2
R:3
The maximum concentration of N
2
O, shown in Fig. 14, is
about 50 ppmat the position of 100 mm belowthe nozzle, also
mainly from the release of volatile-nitrogen. The N
2
O emis-
sion is about zero in the exhaust.
As well known, N
2
O decreases with increasing furnace
temperatures. At the temperature of 1273 K, more than 90% of
N
2
O is decomposed. In the experiments, the average tempera-
ture of the down-fired combustor is about 1373 K and
therefore most of the N
2
O is thermally decomposed.
NO concentrations along the axis of the down-fired
combustor are shown in Fig. 15.
NO concentration in the high temperature air is 387 ppm,
which is quite high due to the low riser and the high excess air
ratio of the CFB. NO concentration decreases in the reducing
zone at the range of 0600 mm below the nozzle. NO in the
high temperature air could be reduced and decomposed by
homogeneous reactions and heterogeneous reaction.
Except for the reaction of R.3, main paths of homogeneous
reactions of NO reduction in reducing zone are [26]:
NO CH
i
HCN R:4
NO HCNN
2
R:5
NOCOX CO
2

1
2
N
2
R:6
In the down-fired combustor, especially in the reducing
zone, heterogeneous reactions may play an important role in
NO decomposition.
Main route for the heterogeneous NO reduction by chars is
as follows [26]:
NOC
f
X C O
1
2
N
2
R:7
NO concentration has a little increase at the position of
800 mm below the nozzle. There exists oxidizing atmosphere
in the lower part as the tertiary air supplied to the combustor
at the position of 600 mm below the nozzle. As a result, the
nitrogen-containing species, such as HCN, NH
3
and char-
nitrogen, may convert into NO at the range of 600 mm below
the nozzle.
NO
2
concentrations are below 1 ppm at the different axis
position of the down-fired combustor.
The NO
x
(NO
x
=NO+NO
2
) emission is 390 mg/m
3
(@ 6% O
2
),
13% lower than the regulation for thermal power plants in
China.
Conversion ratio of fuel-nitrogen of pulverized coal to NO
x
in the down-fired combustor is defined as:
(The absolute value of NO
x
in the exhaust from DFCThe
absolute value of NO
x
in the high temperature air from CFB)/
The calculated absolute value of NO
x
in the exhaust from DFC
with all fuel-N of pulverized coal changes to NO
x
.
The conversion ratio of fuel-N to NO
x
in the down-fired
combustor is 11.8%.
Total Fuel Nitrogen (TFN) concentrations, shown in Fig. 16,
are defined as the summation of NO, N
2
O, NO
2
, HCN and NH
3
.
The major part of TFN is NO. The concentration profile of TFN
is similar to that of NO shown in Fig. 15.
4. Conclusions
In this paper, a process of pulverized coal combustion in high
temperature air from a circulating fluidized bed and NO
x
emissions are described and analyzed. The following conclu-
sions can be obtained:
1 High temperature air with lower oxygen concentrations
can be achieved steadily and continuously by combustion
in a circulating fluidized bed.
2 Pulverized coal combustion in high temperature air from a
circulating fluidized bed shows a uniform temperature
profile along the axis of the down-fired combustor. The
combustion efficiency of pulverized coal is about 99.8%.
3 NO
x
emission is 390 mg/m
3
, 13% lower than the regulation
for thermal power plants in China. The conversion ratio of
fuel-nitrogen of pulverized coal to NO
x
is 11.8% in the
down-fired combustor.
4 The N
2
O emission, as well as HCN and NH
3
, is about zero in
the exhaust from the down-fired combustor.
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