Applied Energy 87 (2010) 3162–3170

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Applied Energy
journal homepage: www.elsevier.com/locate/apenergy

Predictions of the impurities in the CO2 stream of an oxy-coal combustion plant

Hao Liu *, Yingjuan Shao
Department of Architecture and Built Environment, Faculty of Engineering, University of Nottingham, University Park, Nottingham NG7 2RD, UK

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

Article history: Whilst all three main carbon capture technologies (post-combustion, pre-combustion and oxy-fuel com-
Received 13 October 2009 bustion) can produce a CO2 dominant stream, other impurities are expected to be present in the CO2
Received in revised form 19 April 2010 stream. The impurities in the CO2 stream can adversely affect other processes of the carbon capture
Accepted 21 April 2010
and storage (CCS) chain including the purification, compression, transportation and storage of the CO2
Available online 26 May 2010
stream. Both the nature and the concentrations of potential impurities expected to be present in the
CO2 stream of a CCS-integrated power plant depend on not only the type of the power plant but also
Keywords:
the carbon capture method used. The present paper focuses on the predictions of impurities expected
Oxy-coal combustion
Carbon capture
to be present in the CO2 stream of an oxy-coal combustion plant. The main gaseous impurities of the
CCS impurities CO2 stream of oxy-coal combustion are N2/Ar, O2 and H2O. Even the air ingress to the boiler and its aux-
Nitrogen oxides iliaries is small enough to be neglected, the N2/Ar concentration of the CO2 stream can vary between ca.
Sulphur dioxides 1% and 6%, mainly depending on the O2 purity of the air separation unit, and the O2 concentration can
Flue gas composition vary between ca. 3% and 5%, mainly depending on the combustion stoichiometry of the boiler. The
H2O concentration of the CO2 stream can vary from ca. 10% to over 40%, mainly depending on the fuel
moisture and the partitioning of recycling flue gas (RFG) between wet-RFG and dry-RFG. NOx and SO2
are the two main polluting impurities of the CO2 stream of an oxy-coal combustion plant and their con-
centrations are expected to be well above those found in the flue gas of an air-coal combustion plant. The
concentration of NOx in the flue gas of an oxy-coal combustion plant can be up to ca. two times to that of
an equivalent air-coal combustion plant. The amount of NOx emitted by the oxy-coal combustion plant,
however, is expected to be much smaller than that of the air-coal combustion plant. The reductions of the
recirculated NOx within the combustion furnace by the reburning mechanism and the char-NO reactions
are the main reason for a smaller amount of NOx emitted by the oxy-coal combustion plant. The concen-
tration of SO2 in the flue gas of an oxy-coal combustion plant can be up to six times to that of an equiv-
alent air-coal combustion plant if the recycling flue gas is not desulphurized. The flue gas volume flow
rate of an oxy-coal combustion plant is much smaller (<20%) than that of an equivalent air-coal combus-
tion plant, which is a significant advantage for the purification of the flue gas.
Ó 2010 Elsevier Ltd. All rights reserved.

1. Introduction
Carbon capture and storage (CCS) is regarded as one of the fu-
ture carbon abatement methods to stabilise CO2 concentrations
in the atmosphere [1]. It involves the separation and capture of
CO2 from major CO2 emitters such as large-scale power plants,
transportation and storage of the capture CO2 at a storage location
for long-term isolation from the atmosphere. CCS is not a new
technology and CO2 has been captured, transported and stored
from naturally occurring CO2 sources since 1970s for enhanced
oil recovery (EOR) in oil fields [2]. However there is little experi-
ence of fully integrated CCS systems with anthropogenic CO2
sources and therefore further pilot studies and demonstrations
* Corresponding author. Tel.: +44 115 8467674; fax: +44 115 9513159.
E-mail address: liu.hao@nottingham.ac.uk (H. Liu).
have to be performed before a CCS system can be installed and uti-
lized with a large-scale power plant.
At the present time, there are three main capture methods of
CO2 applicable to large-scale power plants: post-combustion,
pre-combustion and oxy-fuel combustion [3–5]. With these CO2
capture methods, a highly concentrated CO2 stream could be
obtained from the power plant processes. However, the impurities
found in the flue gases of large-scale power plants have the poten-
tial to pass through each step of the CCS process and could interact
adversely with the carbon capture process, the compression equip-
ment, the phase properties of the CO2 stream, the purification pro-
cess, the transportation pipelines and the geological storage site
[6–10]. Both the nature and the concentrations of potential impu-
rities expected to be present in the CO2 stream of a CCS-integrated
power plant depend on not only the type of the power plant but
also the carbon capture method used. In particular, the concentra-
tions of potential impurities in the CO2 stream of an oxy-coal

0306-2619/$ - see front matter Ó 2010 Elsevier Ltd. All rights reserved.
doi:10.1016/j.apenergy.2010.04.014
 H. Liu, Y. Shao / Applied Energy 87 (2010) 3162–3170
combustion plant can vary greatly depending on the operating
conditions of the oxy-coal combustion plant.
Oxy-fuel capture of CO2 involves the combustion of a fuel in
oxygen rather than air, producing a lower volume of flue gas with
a much higher concentration of CO2. The flue gas consists mainly of
water vapour, high concentrations of CO2 and excess O2 which is
needed to ensure complete combustion of the fuel. This flue gas
composition makes the separation of CO2 from the gas stream eas-
ier and less energy demanding than post-combustion capture as
water vapour can be easily removed by cooling and condensing
the gas stream, leaving a high concentration of CO2-rich gas [3–
5,11–13]. To ensure the combustion temperature and heat transfer
inside the oxy-fuel combustion boiler comparable to that of coal-
air combustion, the O2 needed for combustion and supplied by
air separation units (ASU) is diluted with the recirculated flue
gas (RFG) which is mainly of CO2, with the O2 concentration in
the oxidizer kept at about 30–35% [14–16]. An additional benefit
of recycling the CO2 back into the boiler before undergoing purifi-
cation and compression, is that the size of the combustion plants
can be reduced by approximately 20% when compared to conven-
tional, air-combustion systems [3]. After the flue gas stream is
dried, compressed and purified if necessary, the gas stream com-
posed of mainly CO2 is ready for transportation and storage.
Oxy-fuel combustion technologies have been used in metallur-
gical and glass industries but are yet to be fully demonstrated or
commercialized for CCS purposes with fossil fuel-fired power
plants [3,5,13]. However, in recent years, oxy-coal combustion
for CCS purposes has advanced rapidly from laboratory studies
(e.g. [14–17]) to pilot-scale demonstrations (e.g. [18,19]). The
30 MW pilot-scale CCS demonstration plant of Vattenfall [18]
which was designed as an oxy-coal combustion plant started its
operation from September 2008. In July 2009, Doosan Babcock
started the demonstration of the world’s largest OxyCoal™ Clean
Combustion system on a full-size 40 MWth burner in Scotland,
UK [19].
Although the flue gas of an oxy-coal combustion plant is mainly
of CO2, it also contains various impurities, such as H2O, N2, NOx, SOx
and O2. In addition, the flue gas recirculation of oxy-coal combus-
tion could result in ‘accumulation’ of impurities in the furnace if
the impurities in the flue gas are not removed prior to the recircu-
lation. This means that the concentrations of some impurities such
as SO2 and NOx in the flue gas of an oxy-coal combustion plant can
be significantly higher than those in the flue gas of an air-coal com-
bustion plant. The concentrations of various impurities present in
the flue gas of an oxy-coal combustion plant depend on many fac-
tors such as the purity of oxygen generated from the air separation
Wet-RFG
Flue gas
heater
2nd Ox
Boiler
1st Ox Coal prep
Fig. 1. A block diagram of an oxy-coal combustion plant.
3163
unit and the operating conditions of the plant (fuel properties, stoi-
chiometry of combustion, flue recirculation arrangement etc.).
Although some studies have listed the expected concentrations of
various impurities [3,10,20], few have predicted the concentrations
of impurities in the CO2 stream of an oxy-coal combustion plant
under different operating conditions. The results of such predic-
tions could provide realistic data on the concentrations of impuri-
ties likely to be present in the CO2 stream to those researchers who
are investigating the impacts of impurities on the thermodynamic
properties, compression, transportation and storage of the CO2
stream.
The main objective of the present study is to predict the concen-
trations of CO2 and its main impurities namely, H2O, N2/Ar, O2, SO2
and NOx in the flue gas of an oxy-coal combustion plant under var-
ious conditions.
2.Predictions of the impurities in the CO2 stream of an oxy-coal
combustion plant
A block diagram for an oxy-coal combustion plant to be mod-
elled is presented in Fig. 1, which is the similar to that of EPRI
[20]. The flue gas desulphurisation (FGD) unit of the diagram pre-
sented by EPRI [20] was omitted in this study. According to EPRI
[20], if the SO2 concentration in the flue gas is higher than
3000 ppmv, the recirculated flue gas (RFG) should first pass
through an FGD unit which follows the particulate removal device,
such as an ESP or a baghouse. High concentrations of SO2 can cause
serious corrosion problems to the flue gas recirculation fans and
ducts as well as the combustion furnace. Exclusion of the FGD unit
in the modelling plant provides the opportunity to predict how
high the concentration of SO2 can be in the CO2 stream of the
oxy-coal combustion plant. Particulates are separated by ESP or
bag-filters before recycling, to limit their accumulation in the fur-
nace and erosion [21]. Although wet-RFG, which denotes that the
recirculated flue gas includes water vapour, is thermodynamically
favourable compared to dry-RFG, which denotes that the water va-
pour in the recirculated flue gas is removed, dry-RFG would be re-
quired if the level of water vapour or SO2 in the RFG is restricted
[21]. For example, when RFG is used for coal drying and transpor-
tation duties, dry-RFG is likely to be used, as shown in Fig. 1. The
majority of oxygen needed for combustion is supplied by ASU
but RFG also provides some oxygen for combustion as RFG contains
excess oxygen which is needed to ensure complete combustion. As
the oxygen purity of a typical ASU is in the order of 95–99%, the
oxygen from ASU also brings small amounts of nitrogen (N2) and
Dry-RFG
ESP or Cooler
baghouse condenser
To CO 2
purification,
Water compression
O2/N2 from ASU
Coal
3164 H. Liu, Y. Shao / Applied Energy 87 (2010) 3162–3170

argon (Ar). The oxygen from ASU mixes with RFG before entering
the combustion furnace as two streams of the oxidizer (1st Ox
and 2nd Ox in Fig. 1) which are lumped together in the modelling.
2.1. Methodology of modelling
The oxy-coal plant shown in Fig. 1 is modelled as a black box by
applying principles of mass conservations, stoichiometry and com-
bustion reactions which are detailed in the Appendix. The adopted
assumptions together with their justifications are described below:
(1) Complete combustion has been achieved within the furnace:
most modern air-coal combustion power plant boilers achieve
combustion efficiency better than 99% and therefore correctly
designed oxy-coal combustion power plant boilers are expected
to achieve near 100% combustion efficiency.
(2) NOx is modelled and expressed as NO2 only and SOx as SO2
only: This assumption is usually adopted with any stoichiometric
combustion calculations.
(3) NOx is assumed to be formed from coal-N only, whereas the
percentage of coal-N converted to NOx is given by an input param-
eter: Although thermal-NOx and prompt-NOx contribute to NOx
formations, NOx formed from coal-N is expected to be the domi-
nant part of NOx formed from coal combustion. The percentage
of coal-N converted to NOx depends on not only the boiler/burner
design but also the coal properties and other factors. However, its
prediction is beyond the scope of this study and therefore is desig-
nated as an input parameter.
(4) Recirculated NOx can be reduced in the furnace, with the
percentage of reduction being used as an input parameter: The
reduction of the recirculated NOx depends on the boiler burner
flame conditions, the recycling flue gas inlet position on the boiler,
the coal/char properties and many other factors [15,16,22]. How-
ever, its prediction is beyond the scope of this study and therefore
is designated as an input parameter.
(5) Coal-S is assumed to be converted to SO2 only: During pul-
verised coal combustion, majority of coal-S is oxidised to SO2 in
the furnace.
(6) SO2 formed from the conversion of coal-S can be retained by
the coal ash, with the percentage of retention being used as an
input parameter: The retention of the SO2 formed from the oxida-
tion of coal-S by the coal ash depends on not only the coal ash con-
tent and properties but also the burner and furnace designs such as
air-staging [23]. However, its prediction is beyond the scope of this
study and therefore is designated as an input parameter.
(7) Impurities (N2, Ar and others) of ASU are lumped together as
N2/Ar, with the purity of O2 from ASU being used as an input
parameter: Considering that Argon is only a small fraction of N2
in air, Argon is lumped together with N2 as N2/Ar in this study.
However, it should be noted that the proportions of N2 and Ar in
the lumped impurity N2/Ar depend on not only the O2 purity of
ASU but also the air separation technology used. To simply the
modelling, N2 and Ar (and other minor components in air) are
lumped together as N2/Ar without specifically specifying the pro-
portions of N2 and Ar in the lumped impurity of N2/Ar.
(8) Air ingress to the boiler and its auxiliaries is not included in
the modelling: Some levels of air ingress are inevitable with any
power plant boilers. However, they are dependent on the construc-
tions of the individual boiler and its auxiliaries and can occur any-
where within the boiler/auxiliary system. In order to simplify the
modelling, air ingress is not included in the modelling.
The modelling of the air-coal combustion plant having the same
capacity as the oxy-coal combustion plant has also been carried
out by using the same assumptions of oxy-coal combustion, e.g.
regarding the conversion of fuel-N to NOx and the retention of
SO2 by coal ash, unless otherwise stated. For air-coal combustion,
it is assumed that there is little flue gas recirculation as this is
the likely case with many air-coal combustion power plant boilers.
Table 1 lists the input parameters of the model, including the de-
fault values and the ranges that have been modelled. Table 2 lists
the main output parameters of the model.
All the flow rates of the plant are normalized to the coal flow
rate. The modelling is performed by an excel worksheet and in-
cludes five iterations involving the concentration ratios of N2/Ar
and CO2, SO2 and CO2, H2O and CO2, NOx and CO2 in the flue gas
and the concentration ratio of O2 and CO2 in the oxidizer. The max-
imum relative error of iterations was set as 105. Three coals have
been modelled: a UK bituminous coal which had been experimen-
tally investigated by the author and his colleagues with a 20 kW
oxy-coal combustor [14,15], Pittsburgh #8 and a US sub-bitumi-
nous coal which had been used as the main CCS candidate coals
of EPRI report [20]. Table 3 shows the analyses of the three coals.
2.2. Modelling results and discussion
The standard modelling conditions are those defined by the de-
fault values of the input parameters shown in Table 1. The default
Table 2
List of main output parameters.
Device/description Output parameters
ASU Flow rate (litre@STP/kg coal)a
RFG Total RFG flow rate (litre@STP/kg coal)
Oxidizer Total oxidizer flow rate (litre@STP/kg coal), dry
composition (O2, CO2, N2/Ar, NOx, SO2) and H2O content
Flue gas emitted by Dry and wet flue flow rates (litre@STP/kg coal, as % of
oxy-coal air-coal combustion), dry composition (O2, CO2, N2/Ar,
NOx, SO2) and wet composition (O2, CO2, N2/Ar, NOx,
SO2, H2O)
NOx emitted by Amount (g/GJ), as % of coal-air combustion
oxy-coal
a
STP – 273 K, 1 atm.

Table 1
Input parameters including their default values and ranges to be modelled.

Input parameters Defaulta Ranges

Coal elemental analysis and gross calorific value (on as a received basis) UK Bit. coal UK Bit., Pittsburgh #8, US Sub-Bit.
O2 concentration in the oxidizer (dry basis, %) 30 30, 32.5, 35
O2 purity of ASU (%) 97 95, 97, 99
Overall stoichiometry of the boiler 1.20 1.10, 1.15, 1.20
% of SO2 formed from the oxidation of fuel-S retained by coal ash 5 5, 10, 20
% of conversion of fuel-S to SO2 100 100
% of conversion of fuel-N to NOx 20 10, 20, 30, 40
% of recycled NOx reduced in the furnace 70 50, 60, 70, 80
wt.% of RFG as wet-RFG (on a dry basis) 40 0, 20, 40, 60, 100
a
Default values are those of likely typical values in reality or chosen for the standard modelling case.
 H. Liu, Y. Shao / Applied Energy 87 (2010) 3162–3170 3165

Table 3
Analyses of coals.

Coal Elemental analysis (wt.%, as received) GCV (MJ/kg)

C H N S O Ash M
UK bituminous 70.57 4.62 1.62 2.06 7.07 11.42 2.64 30.35
Pittsburgh #8 73.78 4.88 1.42 2.13 5.41 7.33 5.05 31.05
US Sub-bituminous 48.18 3.31 0.7 0.37 11.88 5.32 30.24 19.14

Table 4
Main modelling results with the three selected coals.

Coal/parameter UK bituminous Pittsburgh #8 Sub-bituminous

Flue gas composition of oxy-coal (db – dry basis, wb – wet basis) CO2 (%, db) 90.27 90.27 91.19
O2 (%, db) 5.19 5.20 5.14
N2/Ar (%, db) 3.48 3.51 3.34
SO2 (ppmv, db) 9388 9284 2495
NOx (ppmv, db) 1112 928 732
H2O (%, wb) 11.58 12.13 21.28
SO2 and NOx of air-coal SO2 (ppmv, db) 1570 1544 432
NOx (ppmv, db) 587 489 389
Volume flow and emissions of oxy-coal as % of air-coal Dry flue gas 16.73 16.63 17.33
Wet flue gas 17.80 17.74 19.46
NOx emitted 31.68 31.51 32.61

values are those of likely typical values in reality (e.g. O2 concen-
tration in the oxidizer 30%, 20% of fuel-N converted to NOx) or
chosen for the standard modelling case (e.g., UK Bituminous Coal).
The effect of a specific input parameter on the output parameters
listed in Table 2 has been studied by varying the value of the spe-
cific input parameter while other input parameters are kept con-
stant at their default values.
2.2.1. Modelling results with the three selected coals
Table 4 summarizes the main modelling results with the three
selected coals under the standard modelling conditions. As ex-
pected, the dominant component of the flue gas of oxy-coal com-
bustion is CO2 but there are also significant amounts of H2O, O2
and N2/Ar in the flue gas. For the three coals modelled, under
otherwise the standard modelling conditions, the dry flue gas con-
tains about 90.3–91.2% of CO2, 5.1–5.2% of O2 and 3.3–3.5% of N2/
Ar. On a wet basis, the flue gas contains about 11–12% of water va-
pour for the coals with low moisture contents (UK bituminous and
Pittsburgh #8) and over 21% of water vapour for the coal with a
high moisture content (the US sub-bituminous coal). As will be
shown later, the concentrations of the main components in the flue
gas will be greatly affected by the O2 purity of ASU, the stoichiom-
etry of the combustion, the partitioning of RFG between wet-RFG
and dry-RFG, and the O2 concentration of the oxidizer.
The concentrations of NOx and SO2 in the flue gas of an oxy-coal
combustion plant are much higher than those of air-coal combus-
tion plant as shown in Table 4. The concentration of NOx in the flue
gas of oxy-coal combustion is almost doubled, whereas the con-
centration of SO2 is about six times of that of air-combustion. How-
ever, the amount of NOx by oxy-coal combustion is much smaller
than that of air-combustion. Under the standard modelling condi-
tions, oxy-coal combustion emits about a third of NOx. The reduc-
tion in the amount of NOx emitted with oxy-coal combustion is
mainly due to the reductions of the recirculated NOx in the furnace
by hydrocarbon radicals (i.e. the reburn mechanism [24]) and the
char-NO reactions [22]. The actual level of the recirculated NOx
reduction depends on the boiler burner flame conditions, the recir-
culating flue gas inlet position on the boiler and coal/char reactiv-
ity [15,16,22] and therefore is expected to be quite variable for
boilers with different designs and/or burning different coals. The
effect of the assumed level of the recirculated NOx reduction on
the NOx emissions of oxy-coal combustion will be shown later.
These modelling results are in qualitative agreement with the
experimental findings of Wall et al. [16] who had performed pi-
lot-scale oxy-coal combustion with real flue gas recirculations
and found that oxy-coal combustion emitted about a third of NOx
produced by air-combustion.
For the UK bituminous coal and Pittsburgh #8 which have about
2.1 wt.% of fuel-S, the predicted SO2 concentrations in the flue gas
of oxy-coal combustion are about 9000 ppmv, well above the limit
of 3000 ppmv suggested by EPRI [20] when FGD is needed before
the flue gas is recirculated to the boiler. On the other hand, for
the sub-bituminous coal which has low fuel-S (0.37 wt.%), the pre-
dicted SO2 concentration in the flue gas of oxy-coal combustion is
about 2500 ppmv which is below the 3000 ppmv limit.
The flue gas composition of an oxy-coal combustion plant is af-
fected by many factors as will be shown in the following sections.
Nevertheless, the flue gas compositions shown in Table 4 which
were obtained under the standard modelling conditions for three
different coals can be used as representative compositions to
investigate the impact of impurities on other parts of an oxy-coal
based CCS system including CO2 purification, compression, trans-
portation and storage.
Table 4 also shows that oxy-coal combustion emits much lower
volume flue gases than air-coal combustion. The volume flow rate
of the flue gas of oxy-coal combustion is <20% of air-coal combus-
tion and this can be a significant advantage when the flue gas of
the oxy-coal combustion plant needs to be purified. For example,
if a Selective Catalytic Reduction (SCR) is needed to reduce the
NOx concentration in the flue gas, a much smaller SCR than that
of the air-coal combustion plant can be used for the oxy-coal com-
bustion plant. Recirculation of flue gases containing high concen-
trations of NOx will not cause serious corrosion problems to the
boiler, the recirculation ducts and fans and therefore, for oxy-coal
combustion plants, SCR, if needed, can be installed after the flue
recirculation point. This is contrasting to FGD which, if needed,
should be installed before the flue recirculation point [20].
2.2.2. Effect of oxygen purity of ASU on the flue gas composition and
the flow rates of ASU, RFG and flue gas
Typical oxygen purity of ASU is likely to be within the range of
95–99%. Impurities (mainly N2/Ar) within the oxygen stream of
3166 H. Liu, Y. Shao / Applied Energy 87 (2010) 3162–3170

Exhaust N2 /Ar concentration (dry basis), %

95 10
Exhaust CO2 concentration (dry basis), %

95 10

CO2 concentration (dry basis), %

O2 concentration (dry basis), %

CO2 O2
CO2 N2 /Ar
93 8
SR =1.20 (O2 = 5.20%)
93 8

91 6
91 6

89 4
89 4

87 2
87 2

85 0
85 0 1.10 1.15 1.20
94 96 98 100
Stoichiometric ratio
O2 Purity, %
Fig. 4. Effect of stoichiometry on the exhaust CO2 and O2 concentrations.
Fig. 2. Effect of O2 purity on exhaust CO2 and N2/Ar concentrations.

remains at ca. 3.5% which corresponds to the O2 purity of 97%, irre-

ASU will be found in the flue gas of the oxy-coal combustion plant. spective of the stoichiometry. As would be expected, higher stoi-
Fig. 2 clearly shows that increasing the O2 purity from 95% to 99% chiometry would also mean higher flow rates of ASU, RFG as well
will result in an increase in the CO2 concentration of the flue gas as the flue gas to be exhausted as shown in Fig. 5. However, it
from 88.0% to 92.6% (on a dry basis) and a decrease in the N2/Ar should be pointed out that the increase in the flow rate of RFG is
concentration of the flue gas from 5.8% to 1.2% (on a dry basis). more than 10 times of the increase in the flow rate of ASU or the
The presence of a large quantity of N2/Ar in the flue gas will in- flue gas emitted when the combustion stoichiometry is increased
crease the energy consumption of compression and transportation. from 1.1 to 1.2. Under the modelling conditions of Fig. 5, the flow
The O2 purity of the ASU also affects the flow rates of ASU and rate of RFG is only about 2.6–3.0 times of that of ASU or flue gas
RFG as well as the flue gas which is to be purified, compressed, emitted. Higher stoichiometry requires more O2 flow supplied to
transported and stored as shown in Fig. 3. With a higher O2 purity, the boiler and to keep the O2 concentration in the oxidizer constant
a lower flow rate of ASU is needed but to keep the O2 concentration at the fixed value (30%) more RFG is needed. The O2 flow comes
in the oxidizer at the fixed level (30%, dry basis), a higher flow rate from both ASU and RFG. The higher the combustion stoichiometry,
of RFG is needed. As the flow rate of the flue gas mainly depends on the higher the O2 concentration in the flue gas and hence more O2
the flow rate of ASU, therefore, the flow rate of the flue gas also flow is provided by RFG. Therefore, the required increase in the
decreases with the increase in the O2 purity of ASU. flow rate of ASU would be smaller than that was indicated by the
ratio of the flow rates between ASU and RFG. As the flow rate of
the flue gas emitted mainly depends on the flow rate of ASU, its in-
2.2.3. Effect of stoichiometry on the flue gas composition and the flow
crease resulted from the increase in stoichiometry from 1.1 to 1.2
rates of ASU, RFG and flue gas
is more or less the same as the increase in the flow rate of ASU.
To ensure complete combustion, the overall stoichiometry of a
conventional air-coal combustion boiler of a power plant is always
maintained above 1.0 and most likely within the range of 1.1 and 2.2.4. Effect of the partitioning of RFG between dry-RFG and wet-RFG
1.2. Similar stoichiometery is expected to be used with an oxy-coal on the flue gas composition
combustion boiler. Fig. 4 shows that reducing stoichiometry from The partitioning of RFG between dry-RFG and wet-RFG depends
1.20 to 1.1 would result in a decrease in the flue gas O2 concentra- on several factors such as the power plant coal preparation system
tion from 5.2% to 2.8% and an increase in the flue gas CO2 concen- and the coal properties. It mainly affects the water vapour content
tration from 90.3% to 92.6%. The flue gas N2/Ar concentration Flow from ASU and flue gas emitted, litre/kg coal
Flue gas emitted, Flow from ASU, litre/kg coal

5000 2000 5000 1700

Flue gas recirculated, litre/kg coal

Total RFG (wet), litre/kg coal

4800 1800 4800 1680

4600 1600 4600 1660

4400 1400 4400 1640

Flue gas emitted (wet)
Flow from ASU Flue gas emitted (wet)
4200 1200 4200 1620
- - Total RFG (wet) Flow from ASU
- - Total RFG (wet)
4000 1000 4000 1600
94 96 98 100 1.10 1.15 1.20
O2 purity, % Stoichiometry

Fig. 3. Effect of O2 purity on the flow rates of ASU, RFG and the flue gas. Fig. 5. Effect of stoichiometry on the flow rates of ASU, RFG and the flue gas.
 H. Liu, Y. Shao / Applied Energy 87 (2010) 3162–3170 3167

CO2 and H2O concentration in we flue gas, %
90
80
70
60
50
40
30
20
10
0 Over the past decades, considerable efforts have been made to
Fig. 6. Effect of the partitioning of RFG between dry-RFG and wet-RFG on CO2 and
H2O concentrations in the wet flue gas.
of the flue gas and the wet flue gas composition. For the two coals
with low moisture contents (UK Bituminous coal and Pittsburgh
#8), Fig. 6 shows that if all of the RFG is dry-RFG, the CO2 and
H2O concentrations of the wet flue gas would be about 82.4–
82.7% and 8.4–8.8%, respectively, but if all RFG is wet-RFG, they
would be about 64.5–65.6% and 27.4–28.5%, respectively. On the
other hand, for the sub-bituminous coal which has a high moisture
content (30.24 wt.%), the CO2 and H2O concentrations of the wet
flue gas would be about 76.7% and 15.9%, respectively, if all RFG
is dry-RFG, and 51.9% and 43.1%, respectively, if all RFG is wet-
RFG. High concentrations of H2O in RFG may have adverse impacts
such as corrosion problems on recirculation ducts and fans. But
wet-RFG can be carried out at higher temperatures than dry-RFG
and this can have a positive effect on the energy performance of
the combustion system [16,21]. However, in practice, both wet-
RFG and dry-RFG are likely to be used together in an oxy-coal com-
bustion plant.
2.2.5. Effect of the level of the recirculated NOx reduction on NOx
emissions
As pointed out above, the level of the recirculated NOx reduction
depends on not only the burner flame conditions but also the RFG
injection positions on the boiler as well as the coal/char activity.
NOx concentration in the flue gas (dry basis), ppmv
The 20 kW oxy-coal combustion tests of Liu et al. [15] found that
the reduction of the recirculated NOx was within the range of
70–90% if RFG was injected via the burner. But the reduction of
the recirculated NOx would drop to 30–50% if RFG was injected
above the burner as tertiary oxidizer. The effect of the assumed
reduction level of the recirculated NOx on the predicted NOx con-
UK Bitu
Pittsburgh centration in the flue gas is shown in Fig. 7. As expected, higher
Subbitu
Closed - CO2
percentages of reduction for the recirculated NOx result in lower
Open - H2O NOx concentrations in the flue gas of the oxy-coal combustion
plant and much less NOx being emitted by the oxy-coal combustion
plant compared with the air-coal combustion.
2.2.6. Effect of the conversion from coal-N to NOx on NOx emissions
0 20 40 60 80 100 reduce the conversion of coal-N to NOx with conventional air-coal
% of RFG as wet-RFG combustion plants. Several combustion modification measures
such as low-NOx burners and air-staging are commonly used with
most modern coal-fired power plants and have been very success-
ful in reducing NOx emissions. It is believed that these combustion
modification measures to reduce NOx emissions are likely to be
applicable to oxy-coal combustion [21] and this has been proved
by some previous laboratory tests (e.g. [14,15]).
Nevertheless, the conversion of fuel-N to NOx can be totally dif-
ferent from the default value (20%). Or in another scenario, the de-
sign of an oxy-coal combustion plant can focus on combustion,
rather than on NOx emissions, if an oxy-coal combustion based
CCS system can handle the expected NOx emissions [21]. With
higher levels of conversion from coal-N to NOx, higher concentra-
tions of NOx are expected in the flue gas of oxy-coal combustion
as shown in Fig. 8. For the UK bituminous coal, with 40% conver-
sion of coal-N to NOx, the NOx concentration in the flue gas of
oxy-coal combustion is expected to be over 2200 ppmv.
2.2.7. Effect of SO2 retention by coal ash on SO2 emissions
The retention of the SO2 formed from the oxidation of coal-S by
the coal ash depends on not only the coal ash content and proper-
ties but also the burner and furnace designs such as air-staging
[23]. Coals with high ash contents and rich in calcium oxides can
absorb more SO2 than other coals, especially under typical fluid-
ized bed combustion conditions where stable calcium sulphates
can be formed. For pulverised coal combustion with air, Li et al.
[23] showed that air-staged combustion can effectively reduce
SOx emissions by means of sulphur self-retention of coal ash when
the primary combustion zone of stoichiometry was within the
range of 0.85–0.95. Sulphur retention by coal ash was also experi-
mentally observed by Wall et al. [16] who reported that the fly ash

NOx concentration in the dry flue gas, ppmv

NOx emitted by Oxy-Coal as % of Air-Coal

NOx concentration 40
1500
% of NOx emitted as of air-coal
2400
2200
Oxy-coal
1400 37 2000 Air-coal
1800
1600
1300 34
1400
1200
1200 31 1000
800
600
1100 28
400
200
1000 25 0
50 55 60 65 70 75 80 0 10 20 30 40 50
% of the reduction of the recycled NOx in the furnace % of fuel-N converted to NOx

Fig. 7. The effect of the assumed reduction of the recycled NOx in the furnace on the Fig. 8. Effect of the conversion of coal-N to NOx on NOx emissions of oxy-coal
NOx concentration in the flue gas and the amount of NOx emitted. combustion and air-coal combustion.
3168 H. Liu, Y. Shao / Applied Energy 87 (2010) 3162–3170

10000 8400 1300

NOx concentration (wet basis), ppmv

SO2 concentration (wet basis), ppmv
SO2 concentration (dry basis), ppmv

SO2
8000 NOx
8300 1200

6000
Oxy-Coal Exhaust SO2 8200 1100
Air-Coal Exhaust SO2
4000
8100 1000
2000

8000 900
0 30 31 32 33 34 35
0 5 10 15 20 25 O2 concentration in the oxidizer (dry basis), %
% of SO2 retained by ash, %
Fig. 11. Effect of the O2 concentration in the oxidizer on the concentrations of NOx
Fig. 9. The effect of SO2 retention by coal ash on SO2 emissions. and SO2 in the flue gas.

produced during oxy-coal combustion contained slightly more sul-

Flow rates of flue gas and ASU, litre/kg coal

phur and the furnace deposits contained significantly more sul- 5000
1800
phur compared to air-coal combustion samples.
Fig. 9 shows the effect of the level of SO2 retention by coal ash

RFG (wet) litre/kg coal

on the SO2 emissions of oxy-coal combustion and air-coal combus-
1750 4500
tion. For the UK bituminous coal which has a fuel-S content of
2.06 wt.%, the SO2 concentration in the flue gas of oxy-coal com-
bustion remains high (7918–9388 ppmv), which is about 6 times
1700 4000
of that of air-coal combustion, within the likely range (5–20%) of
sulphur retention by the coal ash. Very high SO2 concentrations
can cause severe corrosion problems with the recycling fans and
1650 3500
ducts as well as the combustion furnace. EPRI [20] recommended Flue gas emitted (wet)
that the maximum SO2 concentration in RFG should be limited to Flow of ASU
Total RFG (wet)
3000 ppmv. When burning coals with high coal-S such as the UK
1600 3000
bituminous coal and the Pittsburgh #8, a FGD unit is therefore
30 32 34 36
needed to reduce SO2 concentration in the flue gas before the flue
gas is recirculated back to the oxy-coal combustion furnace. O2 concentration in the oxidize (dry basis), %

Fig. 12. Effect of the O2 concentration in the oxidizer on the flow rates of ASU, RFG
2.2.8. Effect of O2 concentration in the oxidizer and flue gas.
The O2 concentration in the oxidizer has a profound influence
on the flame temperature, in-furnace heat transfer and char-burn- Normann et al. [21] even proposed that the O2 concentration in
out of an oxy-coal combustion plant [4,14–16]. The O2 concentra- the oxidizer well above 35% could be used to achieve high combus-
tion in the oxidizer of an oxy-coal combustion plant is required to tion temperatures (2073–2273 K) which could reduce NOx emis-
be in the range of 30–35% so that the oxy-coal combustion plant sions of oxy-coal combustion.
can match the expected combustion temperature and heat transfer The O2 concentration in the oxidizer of oxy-coal combustion af-
of a conventional air-coal combustion plant [4,14–17]. Recently, fects the flue gas composition. Fig. 10 shows that the concentra-
tions of water vapour (H2O) and O2 increase with, whereas the
O2, N2/Ar and H2O concentrations (wet basis), %

concentration of CO2 decreases with the O2 concentration in the

oxidizer. The N2/Ar concentration of the flue gas is more or less
14 86
independent of the O2 concentration in the oxidizer within the
CO2 concentration (wet basis), %

range studied. Fig. 11 shows that the concentration of NOx in the

12 84
O2
flue gas increases, whereas the concentration of SO2 in the flue
N2/Ar gas decreases with the O2 concentration in the oxidizer. With a
10 82
H2O higher O2 concentration in the oxidizer, less flue gas needs to be
CO2 recirculated (Fig. 12). Therefore, less NOx is reduced by the reburn-
8 80 ing mechanism and the char-NO reactions, and less SO2 is accumu-
lated in the furnace, resulting in higher NOx emissions and lower
6 78 SO2 emissions, respectively. Fig. 12 also shows that with a higher
O2 concentration in the oxidizer, a slightly higher flow rate of
4 76 ASU is required and a slightly more flue gas is to be exhausted.

2 74
30 31 32 33 34 35 3. Conclusions
O2 concentration in the oxidizer (dry basis), %
The present study focused on the predictions of the impurities
Fig. 10. Effect of the O2 concentration in the oxidizer on the concentrations of CO2, within the CO2 stream of an oxy-coal combustion plant. The mod-
O2, H2O and N2/Ar in the flue gas. elling results show that:
 H. Liu, Y. Shao / Applied Energy 87 (2010) 3162–3170 3169

(1) The flue gas composition of oxy-coal combustion depends on FO2 ;Stoi ¼ 18:6667C þ 56H þ 16N þ 7ðSAOÞ ð1Þ
a number of factors, particularly the coal properties, the O2
where C, H, N, S and O are wt.% of carbon, hydrogen, nitrogen, sul-
purity of ASU, the stoichiometry of the boiler, the O2 concen-
phur and oxygen in the coal on an as received basis and are input
tration in the oxidizer and the partitioning of RFG between
parameters. Molecular weights of carbon, hydrogen, nitrogen, sul-
dry-RFG and wet-RFG. The flue gas compositions obtained
phur and oxygen elements are assumed to be 12, 1, 14, 32 and
under standard modelling conditions with three different
16, respectively.
coals, shown in Table 4, can be used as ‘representative flue
2. Actual O2 volume flow supplied for the combustion of 1 kg
gas compositions’ for the studies of the impacts of impurities
coal:
on oxy-coal CO2 purification, compression, transportation
and storage. FO2 ;Actual ¼ SR  FO2 ;Stoi ð2Þ
(2) The main gaseous impurities of the CO2 stream of oxy-coal
where SR is the stoichiometric ratio of the combustion and is an in-
combustion are N2/Ar, O2 and H2O. Ignoring the air ingress
put parameter.
to the boiler and its auxiliaries, the N2/Ar concentration
3. Actual O2 volume flow supplied for the combustion consists
can vary between ca. 1% and 6%, mainly depending on the
of two parts, one part supplied by the ASU (FO2 ;ASU ) and the other
O2 purity of ASU, and the O2 concentration can vary between
part brought in by the RFG (FO2 ;RFG ):
ca. 3% and 5%, mainly depending on the combustion stoichi-
ometry of the boiler. The H2O concentration can vary from FO2 ;Actual ¼ FO2 ;ASU þ FO2 ;RFG ð3Þ
ca. 10% to over 40%, mainly depending on the fuel moisture
4. The total volume flow from the ASU depends on the O2 purity
and the partitioning of RFG between dry-RFG and wet-RFG.
of the ASU and consists of two parts, one part being the O2 flow and
(3) NOx and SO2 are the two main polluting impurities of the
the other part being the N2/Ar flow:
CO2 stream of oxy-coal combustion and their concentrations
are expected to be well above those found in the flue gas of FASU ¼ FO2 ;ASU þ FN2 =Ar;ASU ð4Þ
an air-coal combustion plant. The concentration of NOx in FASU ¼ FO2 ;ASU =PurityASU ð5Þ
the flue gas of an oxy-coal combustion plant can be up to FN2 =Ar;ASU ¼ FASU  ð1  PurityASU Þ ð6Þ
ca. two times to that of an equivalent air-coal combustion
plant. The amount of NOx emitted by the oxy-coal combus- where PurityASU is the O2 purity of ASU and is an input parameter.
tion plant, however, is expected to be much smaller than 5. The volume flow of the total dry-RFG consists of volume
that of the air-coal combustion plant. The reductions of the flows of O2, CO2, N2/Ar, NOx and SO2,
recirculated NOx within the combustion furnace by the
FDry;RFG ¼ FO2 ;RFG þ FCO2 ;RFG þ FN2 =Ar;RFG þ FNOx ;RFG þ FSO2 ;RFG ð7Þ
reburning mechanism and the char-NO reactions are the
main reason for a smaller amount of NOx emitted by the 6. The volume flow of the total wet-RFG is the sum of the vol-
oxy-coal combustion plant. The concentration of SO2 in the ume flow of the total dry-RFG and H2O brought in by wet flue
flue gas of an oxy-coal combustion plant can be up to six gas recirculation:
times to that of an air-coal combustion plant. For coals with
FWet;RFG ¼ FDry;RFG þ FH2 O;RFG ð8Þ
coal-S in the order of 2%, if FGD units are not installed before
the flue gas recirculation point, the SO2 concentration the 7. FH2O,RFG depends on the volume flow of the total dry-RFG and
flue gas would be about 3 times of the limit value the percentage of RFG as wet flue gas recirculation, fWet-RFG, which
(3000 ppmv) recommended by EPRI [20] for RFG. The reten- is an input parameter:
tion of SO2 by coal ash can reduce the SO2 concentration in
FH2 O;RFG ¼ FDry;RFG  f Wet-RFG  H2 OWetFlue =ð1  H2 OWetFlue Þ ð9Þ
the flue gas of an oxy-coal combustion plant to some extent.
(4) The flue gas volume flow rate of an oxy-coal combustion where H2OWetFlue is the volume fraction of H2O in the wet flue gas.
plant is much smaller (<20%) than that of an equivalent 8. The total volume flow of the dry oxidizer is the sum of the
air-coal combustion plant, which is a significant advantage volume flow of ASU and that of the total dry-RFG:
for the purification of the flue gas.
FDry;Oxidizer ¼ FASU þ FDry;RFG ð10Þ

Acknowledgments 9. The volume fraction of O2 in the dry oxidizer is specified as an

input parameter (O2Oxidizer) and relates to FO2 ;Actual and FDry,Oxidizer as
The author would like to acknowledge the financial support to follows:
the multidisciplinary research project ‘Influence of Impurities on O2Oxidizer ¼ FO2 ;Actual =FDry;Oxidizer ð11Þ
CO2 Transport and Storage’ of the Bridging the Gaps fund of EPSRC
(EP/E018580/1) via University of Nottingham. The other investiga- 10. FO2 ;RFG , FN2 =Ar;RFG , FNOx ;RFG and FSO2 ;RFG depend on the volume
tors of the research project including J. Billingham, M. Clarke, T.C. flow of the total dry-RFG and the volume fractions of O2, CO2, N2/
Drage, R.S. Graham, E. Norris and Michel Whitehouse are acknowl- Ar, NOx and SO2 in the dry flue gas:
edged for their contributions to the discussions on the background FO2 ;RFG ¼ FDry;RFG  O2DryFlue ð12Þ
knowledge of the present paper. Deborah White is also acknowl-
FCO2 ;RFG ¼ FDry;RFG  CO2 DryFlue ð13Þ
edged for her contribution to the background literature survey.
FN2 =Ar;RFG ¼ FDry;RFG  N2 =ArDryFlue ð14Þ
FNOx ;RFG ¼ FDry;RFG  NOxDryFlue ð15Þ
Appendix A FSO2 ;RFG ¼ FDry;RFG  SO2DryFlue ð16Þ

The list of the main equations used with the modelling of oxy- 11. To work out the flue gas composition, the volume flows of
coal combustion. O2, H2O, CO2, N2/Ar, NOx and SO2 in the flue gas are calculated as
The unit of all volume flow rates is litre@273 K, 1 atm/kg coal follows:
(as received).
FO2 ;Flue ¼ ðSR  1ÞFO2 ;Stoi ð17Þ
1. Stoichiometric requirement of O2 volume flow for the com-
bustion of 1 kg coal:
FH2 O;Flue ¼ 112H þ 12:4444M þ FH2 O;RFG ð18Þ
3170 H. Liu, Y. Shao / Applied Energy 87 (2010) 3162–3170
where M is the moisture content of the coal on an as received basis
(wt.%) and is an input parameter.
FCO2 ;Flue ¼ 18:6667C þ FCO2 ;RFG
FN2 =Ar;Flue ¼ FN2 =Ar;ASU þ FN2 =Ar;RFG
FNOx ;Flue ¼ 0:16N  f NANO þ FNOx ;RFG  ð100  f NOred Þ=100
where fN–NO is the % of coal-N converted to NOx, fNOred is the % of the
recycled NOx reduced in the furnace and both are input parameters.
FSO2 ;Flue ¼ 0:07S  ð100  f SO2 ret Þ þ FSO2 ;RFG
where f SO2 ret is the % of SO2 formed from the oxidation of coal-S that
has been retained by coal ash and is an input parameter.
12. The flue gas composition can be worked out by using the
volume flows of O2, H2O, CO2, N2/Ar, NOx and SO2 in the flue gas:
FTotal;DryFlue ¼ FO2 ;Flue þ FCO2 ;Flue þ FN2 =Ar;Flue þ FNOx ;Flue þ FSO2 ;Flue
FTotal;WetFlue ¼ FTotal;DryFlue þ FH2 O;Flue
O2DryFlue ¼ FO2 ;Flue =FTotal;DryFlue
CO2DryFlue ¼ FCO2 ;Flue =FTotal;DryFlue
N2 =ArDryFlue ¼ FN2 =Ar;Flue =FTotal;DryFlue
NOxDryFlue ¼ FNOx ;Flue =FTotal;DryFlue
SO2 DryFlue ¼ FSO2 ;Flue =FTotal;DryFlue
H2OWetFlue ¼ FH2 O;Flue =FTotal;WetFlue
13. The volume flows of the flue gases emitted from the oxy-
coal combustion plant can be calculated as follows:
FDry;FlueEmit ¼ FTotal;DryFlue  FDry;RFG
FWet;FlueEmit ¼ FDry;FlueEmit =ð1  H2OWetFlue Þ
As described above, to solve above equations, five iterations
involving the concentration ratios of N2/Ar and CO2, SO2 and CO2,
H2O and CO2, NOx and CO2 in the flue gas and the concentration ra-
tio of O2 and CO2 in the oxidizer have been used.
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