Fuel 86 (2007) 656–668

www.fuelfirst.com

Flame and radiation characteristics of gas-fired O2/CO2 combustion

Klas Andersson *, Filip Johnsson
Department of Energy and Environment, Energy Technology, Chalmers University of Technology, SE – 412 96 Göteborg, Sweden

Received 27 June 2006; accepted 9 August 2006

Available online 11 September 2006

Abstract

This paper presents an experimental study on the flame properties of O2/CO2 combustion (oxy-fuel combustion) with focus on the
radiation characteristics and the burn-out behaviour. The experiments were carried out in a 100 kWth test unit which facilitates
O2/CO2 combustion with real flue gas recycle. The tests comprise a reference test in air and two O2/CO2 test cases with different recycled
feed gas mixture concentrations of O2 (OF 21 @ 21 vol.% O2, 79 vol.% CO2 and OF 27 @ 27 vol.% O2, 73 vol.% CO2). In-furnace gas
concentration, temperature and total radiation (uni-directional) profiles are presented and discussed. The results show that the fuel burn-
out is delayed for the OF 21 case compared to air-fired conditions as a consequence of reduced temperature levels. Instead, the OF 27
case results in more similar combustion behaviour compared to the reference conditions in terms of in-flame temperature and gas con-
centration levels, but with significantly increased flame radiation intensity. The information obtained from the radiation and temperature
profiles show that the flame emissivity for the OF 21 and OF 27 cases both differ from air-fired conditions. The total emissivity and the
gas emissivity of the OF 27 and the air-fired environment are discussed by means of an available model. The gas emissivity model shows
that the increase in radiation intensity (up to 30%) of the OF 27 flame compared to the air flame can partly, but not solely, be explained
by an increased gas emissivity. Hence, the results show that the OF 27 flame yields a higher radiative contribution from in-flame soot
compared to the air-fired flame in addition to the known contribution from the elevated CO2 partial pressure.
 2006 Elsevier Ltd. All rights reserved.

Keywords: O2/CO2 combustion; Oxy-fuel; Flame characteristics

1. Introduction ing which energy production from non-fossil energy

Most scientists agree that there is a strong connection
between climate change and the anthropogenic emissions
of greenhouse gases of which CO2 is by far the most impor-
tant one in terms of amount emitted. Drastic measures are
required to reduce the CO2 emissions. Capture of CO2
from large point sources such as power plants with subse-
quent geological storage offers the possibility of a signifi-
cant and relatively quick response to climate change at a
reasonable cost. Successful commercialization of such tech-
nology could therefore provide a transition to a future dur-
*
Corresponding author. Tel.: +46 31 772 5242; fax: +46 772 3592.
E-mail addresses: klas.andersson@me.chalmers.se, klon@entek.chal-
mers.se (K. Andersson).
sources can grow over time. At present there are no power
plants with CO2 capture available on a commercial scale,
but long time aquifer storage is currently applied and eval-
uated in the North Sea and show promising results [1]. The
CO2 could also be stored in connection to enhanced oil
recovery (EOR). Such storage has been closely monitored
in the Weyburn project in Canada, see e.g. [2]. The highest
cost is however on the capture side and to reduce the spe-
cific costs for capture different concepts are discussed. The
O2/CO2 combustion process is one method which seems to
have the potential to give a competitive CO2 capture cost
[3]. In O2/CO2 combustion the fuel is burnt in a mixture
consisting of oxygen and recycled flue gas with the oxygen
produced in a cryogenic Air Separation Unit (ASU), yield-
ing a high concentration of CO2 in the product flue gas and
thereby lowering the capture cost. The cost for the capture

0016-2361/$ - see front matter  2006 Elsevier Ltd. All rights reserved.
doi:10.1016/j.fuel.2006.08.013
 K. Andersson, F. Johnsson / Fuel 86 (2007) 656–668 657

Nomenclature

a, b, c correlation parameters TBR measured furnace wall temperature RHS of the

cji correlation constants probe ports (C)
Hi heating value, inferior (MJ/kg) Tg gas temperature (C)
L path length (cm) Tgmin minimum gas temperature (C)
M reduction factor Tgmax maximum gas temperature (C)
p pressure (bar) Tmr mean radiation temperature (C)
pa partial pressure (bar) Ts furnace wall temperature (C)
PE equivalent pressure (bar)
(paL)m correlation parameter Greek symbols
pCO2 CO2 partial pressure (bar) a absorptivity
pH2 O H2O partial pressure (bar) aCO2 CO2 absorptivity
q radiation intensity (W/m2 sr) aH2 O H2O absorptivity
q1 radiation intensity from combustion gases and ag total gas absorptivity
furnace wall (W/m2 sr) eb furnace wall emissivity
q2 radiation intensity from combustion gases (W/ em mean emissivity
m2 sr) eg total gas emissivity
q3 radiation intensity from furnace wall (W/m2 sr) es soot emissivity
Q+ emitted heat flux (W/m2) ek spectral emissivity
Q incident heat flux (W/m2) e0 zero partial pressure emissivity
RkT gives, for a temperature T (K) and a wavelength f partial pressure ratio: pH2O/(pCO2 þ pH2 O Þ
interval k to k + dk, the black-body radiation r Bolzmann constant (W/m2 K4)
RkTdk k stoichiometric ratio
TBL measured furnace wall temperature LHS of the
probe ports (C)

is instead mainly due to the energy penalty in the ASU. To
design, optimize and scale up furnaces in power plants with
O2/CO2 combustion, models must be validated with exper-
iments under well defined conditions.
Experimental studies on coal-fired O2/CO2 combustion
have been performed in laboratory and semi-industrial
scale test facilities of different size e.g. in [4–7] and more
recently in [8–10]. The experimental work performed has
to a large extent focused on the emission characteristics
for different coal types with an emphasis put on the mech-
anisms of NOx formation during flue gas recycling condi-
tions (e.g. [8,9,11]). The study given in [10] also combines
experimental work with CFD modelling in order to evalu-
ate different burner and combustor designs. Detailed stud-
ies on the in-furnace combustion characteristics have been
performed on semi-industrial scale under natural-gas-fired
conditions [12] as well as under coal-fired conditions [13].
Little fundamental data is available on the radiative prop-
erties of different O2/CO2 mixtures and fuels, but the tests
performed in [12] included measurements of the axial
hemispheric heat flux distribution, from which it was con-
cluded that a feed gas concentration of 28 vol.% O2 during
O2/CO2 combustion produced similar heat flux character-
istics compared to air-fired conditions. Profile measure-
ments of the hemispheric radiative heat flux are also
reported in [13], but for coal-fired conditions using an
ellipsoidal radiation probe. In general, the dominating
contribution to the local incident radiative flux originates
from the surrounding walls in refractory lined furnaces
such as the one used in the present study as well as in
the studies given in [12,13]. The wall dominance on hemi-
spheric radiation measurements is obviously further accen-
tuated for moderate and non-sooty flames with low
emissivity of the flame envelope. In order to reduce the
influence of the hot furnace walls on the radiation data,
uni-directional measurements of the radiation intensity
have been carried out in this study, which hence improve
the possibility for interpretation of the difference between
the three test environments investigated. In addition,
detailed profiles on temperatures and gas concentrations
have been measured to characterize the properties of the
different flames to facilitate a discussion of the flame emis-
sivities in relation to the radiation profiles. The industrial
application of O2/CO2 combustion is most likely to be
based on pulverized coal plant technology, whereas
instead this study presents results performed under gas-
fired conditions. By avoiding solids to take part in the
combustion the complexity is reduced in terms of e.g.
the combustion reaction schemes as well as the radiative
heat transfer mechanisms. Hence, this improves the possi-
bility to better isolate the differences between air and O2/
CO2-fired conditions and to determine the influence of
the CO2 on the gas emissivity versus the total emissivity
with the subsequent effect on the radiative heat transfer
in a moderately sooty flame without the dominance of coal
particles and ash.
658 K. Andersson, F. Johnsson / Fuel 86 (2007) 656–668

In the literature there is a lack of fundamental work on 2. Experiments

the difference in flame radiation characteristics between
mixtures of O2/CO2 and air for well defined conditions in
terms of temperature and gas concentration fields. Such
data is required in order to assess the difference in radiative
properties in terms of emissivity between air and O2/CO2
combustion for different types of fuels and mixtures of
O2/CO2 with the overall aim of describing the implications
for combustion and radiation models presently used in
commercial CFD codes. The aim of this paper is thus to
determine and compare the difference in total radiation
intensity between three well defined combustion conditions
consisting of two O2/CO2 test cases and one air-fired refer-
ence case for a gaseous fuel. The mean emissivity is then
determined based on the experimental data and as a com-
parison the gas emissivity is calculated by an existing gas
emissivity model [14]. Another important part of the work
presented is to describe the difference in combustion perfor-
mance between the three test environments. The differences
are discussed in relation to the measured gas composition
and temperature distributions of the flames tested. Below
is a description of the experimental equipment used for
the measurements and the theory used for evaluating and
analysing the radiative properties of the three combustion
environments investigated, followed by a description of
the results from the study.
The Chalmers test unit, shown in Fig. 1, is designed to
study O2/CO2 combustion under real flue gas recycling
conditions. In this work, gas-fired tests were carried out
with a fuel input of about 80 kW. The test conditions
and fuel properties (propane) are specified in Tables 2
and 3, respectively. The cylindrical refractory lined reactor
is down-fired with an inner diameter of 0.8 m and an inner
height of 2.4 m. The tests can be run under O2/CO2 condi-
tions (with different mixing ratios between O2 and CO2/
H2O), with air or with oxygen enriched combustion, with
the latter condition by means of direct oxygen injection
in the burner. Tests with direct oxygen injection are, how-
ever, not part of the work given in this paper. The flue gas
recycle loop includes one separate temperature controlled
cooler and one condenser enabling both wet and dry flue
gas recycling (Fig. 1). The dotted line indicates the flue
gas path in the recycle loop for the tests performed in this
work, in which dry flue gas recycling conditions are
applied. The flue gas temperature after the condenser is
reduced to about 25–30 C corresponding to 2–2.5 vol.%
water content in the recycled flue gas, and thus similar to
non-preheated air-fired conditions. The ratio of the volu-
metric flow between the recycle stream and the stack gas
is set by two frequency controlled ID-fans.

Direct O2 injection

Primary/secondary
register

FI TI
Pilot burner air/O2/CO2 fan mixing point
O2/flue gas
Air inlet
pre-heater
SC

Wet flue gas Dry flue gas

FI

FI

recycle recycle
FI

FI

Cylindrical
Measurement
furnace
ports R1, R2...R7

SC
2400 mm

Cooling tube 1/4

TI PIC FI

Flue gas Flue gas

800 mm Stack gas
cooler condenser TI
TC TC
C3H8
O2

Cooling water

Fig. 1. The CHALMERS 100 kW O2/CO2 combustion test unit.

 K. Andersson, F. Johnsson / Fuel 86 (2007) 656–668 659

For the experiments given in this paper, the oxygen is
mixed into the recycled flue gas up-stream the ID-fan in
the recycle loop. To improve the mixing of the oxygen
and the recycled flue gas, the oxygen/flue gas mixture (feed
gas) then has to pass plates that protrude perpendicular
into the tube of the gas recycle tube. After passing through
the recycle fan the feed gas is divided into a primary and a
secondary stream which enters the two burner registers.
Approximately 40% of the total flow enters the primary
register. The ratio between the primary and secondary
stream is adjusted by individual valve settings and the vol-
umetric flows are continuously measured by turbine flow
meters. Both oxygen and propane is supplied from bundles
of gas tubes. The oxygen and propane flows are measured
and controlled by mass flow meters.
In order to reduce the time for the combustor to reach
thermal steady state conditions, cooling tubes with variable
length and an outer diameter of 50 mm are inserted from
the top of the combustion chamber at four positions close
to the wall, equally distanced from the flame. The temper-
ature and flow rate of the incoming and outgoing cooling
water is continuously measured for heat balance and mod-
elling purposes. Wall temperature conditions are moni-
tored by means of thermocouples (type K) measuring the
temperature 20 mm from the inner wall surface at 2 · 7
positions at each side of the probe ports R1–R7 (Table
1). The ports along the side of the furnace are used for
in-furnace measurements, by means of water-cooled
probes. A number of ports are available down stream of
the reactor exit and at various positions in the flue gas
recycle pass, which allow for gas composition measure-
ments of the flue gas as well as the recycled feed gas. This
Table 1
Measurement positions on the Chalmers 100 kW O2/CO2 unit
Port number Distance from burner (mm)
R1 46
R2 215
R3 384
R4 553
R5 800
R6 998
R7 1400
enables the detection of possible sources to air infiltration
during flue gas recycle operation.
The gas-fired burner consists of two separate lances for
fuel and direct oxygen injection (as mentioned, the oxygen
register is not used in these tests). The primary and second-
ary swirl registers are replaceable in order to facilitate a
change of the swirl number settings and the corresponding
mixing conditions of the flame. Table 2 lists the settings
used in the present work together with the overall test con-
ditions of the measurements.
All tests were performed at a stoichiometric ratio of
1.15 resulting in a target O2 excess of 3.0 vol.% for the
air and OF 21 cases and 3.8 vol.% for the OF 27 case.
The higher O2 excess in the latter case is due to that the
volumetric flow of recycled flue gas is about 20% lower
than in the OF 21 case. For the OF 27 case the residence
time is increased by the reduction in volumetric flue gas
flow and to some extent also by the change in temperature
distribution from air to oxy-fuel fired conditions. From
initial experiences it was found that the in-flame tempera-
ture distributions of the OF 27 and the reference case are
rather similar, i.e. the difference in temperature will only
moderately influence the relative change in residence time
from the air to the OF 27 case, whereas this change will be
more pronounced under the OF 21 conditions. All in-
furnace measurements have been repeated twice in order
to ensure satisfactory repeatability for each test con-
dition.
Gas composition data consisting of O2, CO, CO2 and
total hydrocarbon (HC) concentrations were measured
by a gas suction probe in the probe ports, at the furnace
exit and in the recycle loop. The total hydrocarbon con-
centration is measured as methane equivalents by means
of an FID (flame ionization detector) based instrument.
The analysis of O2, CO and CO2 were each performed
by two different instruments with different measurement
ranges, adapted for reference and O2/CO2 conditions,
respectively. The measurement principles of both O2
instruments are of paramagnetic type, CO is analyzed
based on NDIR (non-dispersive infrared absorption) and
CO2 is measured by means of NDIR and TC (thermal
conductivity). The suction probe consists of a heated inner
tube with controlled temperature to prevent condensation
inside the probe and a protecting water-cooled jacket. The
gas is dried and filtered before it is fed into the on-line gas

Table 2
Test conditions for the gas-fired tests
Heat input 80 kWth Fuel C3H8 Stoich ratio 1.15
Primary register Fin angle 45 Swirl No 0.79 Secondary register Fin angle 15 Swirl No 0.21
Test case Combustion media Temp feed gas [C] Feed gas composition (vol.%) Theoretic CO2 conc.
O2 N2 CO2 @ stack (vol.%)

Air Air 25–30 21 79 – 12

OF21 O2/CO2 dry recycle 25–30 21 – 79 97
OF27 O2/CO2 dry recycle 25–30 27 – 73 96
660 K. Andersson, F. Johnsson / Fuel 86 (2007) 656–668
analyser train. In order to avoid air-infiltration during the
measurements, the furnace was maintained at an excess
pressure of 20–50 Pa depending on the test condition.
The O2 excess in the stack gas was monitored throughout
the suction measurements in order to control the test
conditions.
The in-furnace temperature measurements were per-
formed with a water-cooled suction pyrometer with a full
length of 1900 mm. The tip of the probe consists of a
200 mm long ceramic tube with an inner diameter of
10 mm in which a Pt–PtRh 30% thermocouple (ANSI Type
B) is placed. The gas is sucked through a 6 mm hole on the
side of the ceramic tube and the design enables measure-
ments of temperatures up to 1700 C.
The radiation intensity measurements were carried out
using a narrow angle radiometer of IFRF-type (Fig. 2).
The probe consists of a straight tube, termed collimating
tube, with a 10 mm inner diameter and a length of about
2 m, which is covered by a protecting water-cooled jacket.
A temperature controlled receiver unit is located at the
rear end of the collimating tube. The radiation beam
passes through the collimating tube in which a number
of parallel baffles are mounted to limit the bundle of rays
and to restrict the viewing angle of the radiometer. The
beam reaches a high broadband reflectance mirror at
the receiver end of the probe, which focuses the beam
onto a thermopile. A known purge gas flow is applied
during both calibration and measurements to prohibit
radiating species and other contaminants to enter the
probe. The sensitivity of the signal to different purge gas
flow rates was evaluated both during calibration and mea-
surements in order to find the minimum flow applicable
to minimize the influence from the purging on the
in situ measurement conditions. In the present probe setup
Argon was used as purge gas at a flow rate of 10 ln/min.
The calibration of the narrow angle probe was performed
in a black-body furnace before and after each mea-
surement series to check the zero drift of the thermal
detector.
High broadband
reflectance mirror
Cooling
water
PT-100 Thermopile
Fig. 2. Schematic illustration of the narrow angle radiometer (IFRF type) used for the radiation intensity measurements.
3. Theory
3.1. Interpretation of radiation data
The following describes the interpretation of the radia-
tion data obtained with the above described narrow angle
radiometer probe and the method to characterize the flame
in terms of flame emissivity together with the gas emissivity
model applied [14]. For the interpretation, measurements
with the narrow angle probe were carried out both with
the hot refractory lined furnace wall and a cold non-reflect-
ing black body as backgrounds. The radiation intensity at
any given distance d from the hot furnace wall to the probe
opening represents the sum of:
(i) radiation from the flame and combustion gases
received along the viewing path of the probe,
(ii) background radiation from the hot refractory furnace
wall, partly absorbed by the gas layer along the view-
ing path d of the probe, and
(iii) in the background reflected radiation from the flame
and combustion gases (i) partly absorbed within the
interval d.
Thus, the total radiation intensity that reaches the probe
can be expressed as
Z 1 Z 1
q1 ¼ ek RkT g dk þ eb ð1  ek ÞRkT s dk
0 0
Z 1
þ ð1  eb Þ ek ð1  ek ÞRkT g dk ð1Þ
0
where q1 is the sum of contributions (i)–(iii) and the emis-
sivity of the flame and combustion gases at a certain wave-
length ek is treated as a general function of wavelength k
whereas the background wall emissivity eb is assumed con-
stant. The function RkT gives, for a temperature T (K) and
a wavelength interval k to k + dk, the black-body radiation
RkTdk. The temperatures Tg and Ts are the gas and back-
ground wall temperatures, respectively.
Electronic
shutter
Collimating tube
Cooling
water
 K. Andersson, F. Johnsson / Fuel 86 (2007) 656–668
For the measurement conditions employed (operational
conditions and measurement levels in the furnace), the fur-
nace wall temperature typically varies ±50 C (around an
average of 600 C) in all three cases. This results in an emis-
sivity of about 0.9 of the refractory lining material.
However, with the low conductivity and considerable
thickness of the furnace walls the conduction losses
through the lining are negligible at thermal steady state
conditions. Furthermore, on the wall surface, the convec-
tive term is small compared with the dominating radiative
term. Thus, since the heat exchange is in principle only due
to radiation the energy balance in Eqs. (2)–(6) gives that
the effective emissivity eb is equal to unity. With Ts being
the temperature and Qthe total incident heat flux of the
wall surface in the energy balance the total outgoing heat
flux Q+ can be written:
Qþ ¼ eb rT 4s þ ð1  eb ÞQ ð2Þ
According to the assumption above, all heat is exchanged
by means of radiation and hence the rate of emission must
equal the rate of absorption, from which follows:
eb rT 4s ¼ eb Q ð3Þ

Q ¼ rT 4s ð4Þ
þ þ
Q ¼ eb rT 4s þ ð1  eb ÞQ ð5Þ
Qþ ¼ rT 4s ð6Þ
Thus, it is clear that the effective emissivity eb is 1 regardless
of the actual emissivity of the material of the wall surface.
Therefore, the radiation from background reflection (iii)
can be disregarded, and Eq. (1) can instead be written as
Z 1 Z 1
q1 ¼ ek RkT g dk þ ð1  ek ÞRkT s dk ð7Þ
0 0
Eqs. (1) and (7) consider the wavelength dependence of the
emissivity of the flame/gas layer over which the total radia-
tion measurement is carried out. However, the measure-
ment data do not give information on the spectral
resolution of the radiation. Therefore a simplified treatment
of the data is required in order to evaluate the difference in
total emissivity between the air and the O2/CO2-environ-
ment, the latter being represented by the OF 27 case, due
to restricted measurement data for the OF 21 case. Hence,
for the air and the OF 27 case a method originally proposed
by Schmidt, as discussed in [15], is used to determine a total
mean emissivity of the gas layer, based on three separate
measurements of the radiation intensity. Different versions
of the method have been suggested, such as the two-path
method as described in [16], as well as for the calculation
of in-flame soot volume fraction in highly soot laden flames
[17]. The latter based on the fact that the method is always
exact monochromatically. In this work, however, the
method is used in its original form. The general basis of
the method is that the flame or gas layer is considered grey,
so that the emissivity becomes independent of wavelength
and equal to the absorptivity, independent of the relation
between the gas and the background temperature. The
661
scattering is neglected due to the small size of the soot par-
ticles and hence the emissivity is assumed equal to the
absorption. These assumptions result in a flame emissivity
independent of wavelength and, integrated over the spec-
trum, Eq. (7) can be written:
q1 ¼ rem T 4mr þ rð1  em ÞT 4s ð8Þ
where em represents the mean emissivity and Tmr the aver-
age radiation temperature of the gas layer concerned, i.e.
along the viewing path of the probe. In order to determine
em and Tmr, separate measurements of the radiation from
the gas layer rem T 4mr and the background furnace wall
rT 4s in Eq. (8) are required in addition to measurements
of q1, a procedure which is followed in the present work.
Hence, q2 is represented by the first term in Eq. (8). To-
gether with the net contribution of the background wall,
q3, the mean emissivity and the mean radiation tempera-
ture of the gas layer can be calculated according to
q  q2
em ¼ 1  1 ð9Þ
q
rffiffiffiffiffiffiffiffi 3
q
T mr ¼ 4 2 ð10Þ
em r
Obviously, with Tmr and em from Eqs. (9) and (10) simpli-
fications are introduced compared to real conditions for
which there is a wavelength dependant emissivity, ek, and
non-uniform concentration and temperature profiles within
the measurement volume. The grey approximation is also
less accurate in the case of a gas-fired flame compared to
e.g. a highly luminous oil flame. This since the gas band
radiation will have a stronger impact on the total emissivity
in a moderately sooty flame and cannot be neglected in
comparison to the continuous radiation due to soot and
especially so for O2/CO2 conditions. This implication on
the results will be further discussed in the results section.
3.1.1. Determination of total gas emissivity
As discussed above em will include emission from both
gas and soot. Therefore em can be expressed as
em ¼ eg þ es  Meg es ð11Þ
where eg and es are the gas and soot emissivities across the
gas layer and the product eges represents the band overlap
of soot and gas. A reduction factor M should be intro-
duced, which depends mainly on the gas temperature and
to less extent on the soot volume fraction. This is because
the emission bands of CO2 and H2O are not randomly
located in the spectrum and due to that the monochromatic
soot emissivity increases with decreasing wavelength. A
possible change in band overlap between soot and gas will
however not be treated in this work, due to its small effect
on the overall emissivity. There are no experimental data
available on the soot volume fraction from the flames
investigated in this work. Instead, in order to reveal if the
difference in mean emissivity between the two combustion
environments corresponds to the difference in gas emissiv-
ity, including H2O and CO2, the gas emissivity is deter-
662 K. Andersson, F. Johnsson / Fuel 86 (2007) 656–668

mined using the model by Leckner [14] running a Fortran and, finally, the total absorptivity of the gas mixture can be
routine provided in [18]. This model was chosen since it calculated from:
accommodates a high degree of generality for which it  
Ts Ts
has been recognised (cf. e.g. [19]). This, since the CO2 ag ¼ aCO2 þ aH2 O  De pH2 O L ; pCO2 L ð18Þ
and H2O emissivities are treated separately after which Tg Tg
the total emissivity of the mixture is determined by taking
a total band overlap correction term into consideration.
Hence, any arbitrary partial pressures of CO2 and H2O 3.2. Results and discussion
can be applied in the model. The polynomial correlations
of the model produce a maximum error of 5% for water va- Satisfactory experimental conditions were typically
pour and 10% for CO2 emissivities at temperatures above reached after some four to five hours with a CO2 concen-
400 K, compared to the spectral integration data upon tration level in the stack gas between 94 and 95 vol.%.
which the model is based [14]. The total emissivity for a Any discrepancy between the theoretical CO2 concentra-
mixture of CO2 and H2O is obtained from: tion level (96–97 vol.%) and the ones measured is due to
that N2 is still left in the recycling media and, to some
eg ¼ eCO2 þ eH2 O  DeðCO2 þH2 OÞ ð12Þ
extent also due to limitations in the instrument precision
In the model a zero partial pressure emissivity is given by of the CO2 analyzer which has a maximum error of ±2%
the correlation: of the full measurement range (0–100%).
"  j  i # Radial temperature profiles are plotted in Fig. 3 for the
X M X N
Tg pa L
e0 ðpa L;p ¼ 1 bar;T g Þ ¼ exp cji log10 three different cases: air, OF 21 and OF 27 (the radiation
i¼0 j¼0
T0 ðpa LÞ0 intensity profiles shown in the same figure will be discussed
later on). It has been well established experimentally that
ð13Þ
O2/CO2 conditions with a similar volumetric feed gas con-
where Tg is the gas temperature, T0 = 1000 K, p is the total centration of O2 as for air (i.e. 21 vol.%), yields signifi-
pressure, pa is the partial pressure and L is the path length cantly lower peak as well as overall combustion
of the gas, either CO2 or H2O, (paL)0 = 1 bar cm and Cji temperature levels compared to air-fired conditions (see
are correlation constants as given in [18]. The emissivity e.g. [8,12]). This is also the general impression obtained
for higher partial pressures, i.e. if pa > 0, can then be calcu- from a comparison of the OF 21 case and the air case of
lated according to: this work (cf. Fig. 3). For example, the highest measured
combustion temperatures for the OF 21 and the air-fired
eðpa L; p; T g Þ ða  1Þð1  P E Þ
¼1 case in port R2 (Fig. 3a) are approximately 1370 C and
e0 ðpa L; p ¼ 1 bar; T g Þ a þ b  1 þ PE 1550 C, respectively. The lower temperature in the OF
 2 ! 21 case is mainly a result from that CO2 has a higher spe-
ðpa LÞm
 exp c log10 ð14Þ cific heat capacity than N2 and to a certain extent that there
pa L
is an increase in radiation losses caused by the CO2 which
where a, b, c and (paL)m are correlation parameters and PE increases the gas emissivity. The significance of the latter
is an equivalent pressure, all given in [18]. For calculation effect obviously depends on the radiative properties of the
of the total gas emissivity the last term in Eq. (12) needs flame considered, i.e. to what extent other components
to be considered, which is due to the band overlap of the such as moisture, soot and particles contribute to the radi-
two gases. This correction term is written ative heat transfer. The emissivities of the O2/CO2 and the
  air-fired environments are further discussed below, and
f 10:4 related to the radiation intensity profiles.
DeðCO2 þH2 OÞ ¼  0; 0089f
10:7 þ 101f A reduction of the recycled flue gas is an obvious way to
 2:76
ðpCO2 þ pH2 O ÞL increase reactor temperature levels in order to improve the
 log10 ð15Þ combustion intensity, in this case from the OF 21 to the OF
ðpa LÞ0
27 case. As a result (Fig. 3) the temperature levels of the
with the partial pressure ratio f defined as OF 27 case approach those of the air case in contrast to
p H2 O the OF 21 case which yields significantly lower tempera-
f¼ ð16Þ tures compared to air firing. Both the air and the OF 27
pH2 O þ pCO2
cases exhibit a strong negative gradient in temperature
The absorptivity is determined by multiplying a factor between 50 and 100 mm from the furnace centreline, which
(Tg/Ts)0.5 to the emissivity evaluated at the external surface represents the location of the flame front. In the OF 21 case
temperature Ts and a temperature scaled pressure path the temperature starts to decrease already between the
length according to: centreline and 50 mm away from the centreline (0 mm),
 0:5   and no parabolic shape of the temperature profile can be
Tg Ts seen close to the centreline (the distributions are assumed
aðpa L; p; T g ; T s Þ ¼ e pa L ; p; T s ð17Þ
Ts Tg axi-symmetric). Although a weak trend of such a parabolic
 K. Andersson, F. Johnsson / Fuel 86 (2007) 656–668 663

45 1600 45 1600
Measurement port: R2 Measurement port: R3
1500 1500
40 40
Radiation intensity q [kW/m sr]

Radiation intensity q [kW/m2sr]

1400 1400
2

35 35

Gas temperature Tg [oC]

Gas temperature Tg [oC]

1300 1300

30 1200 30 1200

1100 1100
25 25
1000 1000

20 900 20 900

800 800
15 15
700 700
10 10
600 600

5 500 5 500
0 100 200 300 400 0 100 200 300 400
Distance from centreline [mm] Distance from centreline [mm]
Air: q1
OF 21: q1
OF 27: q1
Air: Tg
OF 21: Tg
OF 27: Tg

Fig. 3. Mean values of the measured radial radiation intensity profiles with hot refractory furnace wall as background (q1). The grey dotted profiles show
the corresponding gas temperatures.

temperature distribution may exist close to the centreline, tions, have been reported by Kimura et al. [6] and Liu
the tendencies in ports R2 and R3 clearly show a shift in et al. [8]. It should be noted that the gas concentration
position of the flame front (Fig. 3a and b). In addition, and temperature data from intrusive measurement instru-
as seen from the measurements in Port R2 (Fig. 3a), ments such as the ones used in this work rather represent
already between 50 and 100 mm the temperature of the average values over a certain measurement volume than a
OF 21 case decreases down to a level of about 700 C, value at an exact position. This applies to the gas suction
which corresponds to the gas temperature near the wall probes and suction pyrometers used here, especially the lat-
(400 mm) of both the OF 27 and the air-fired case. This ter probe due to the rather high suction velocity employed.
shows that for the OF 21 case, the physical volume of This is especially important to keep in mind for regions
the high temperature zone is smaller compared to the two with sharp gradients. For example, this is the case when
other cases. As will be discussed in the following section, comparing the HC profiles in Fig. 4a and the temperature
this influences the burn-out behaviour of the OF 21 case. profiles in Fig. 3a. The high concentration of unburned fuel
Radial gas concentration profiles (O2, CO, CO2 and at 50 mm from the centreline can be explained by the fact
HC) for ports 2 and 3 are given in Fig. 4, since these two that it corresponds to temperatures represented within a
ports represent the most intense combustion zone with distance from 50 to 100 mm from the centreline, i.e. some-
the highest measured temperatures for all cases. In Fig. 4 where in the range between 700 and 1200 C, rather than
it is seen that the gas composition of the flame envelope the exact same position as the temperature measurement
of the OF 21 case is clearly different from the two other at 50 mm. Compared to the OF 21 case the fuel burn-out
cases. The amount of unburned hydrocarbons is signifi- of the OF 27 case is favoured by the increased temperature
cantly higher for the OF 21 case and, as a consequence, level and improved mixing conditions between fuel and O2,
O2 is still present in the flame core as shown in Fig. 4a due to the reduced amount of recycled flue gas. The hydro-
and b. The suppressed development of the OF 21 flame is carbon levels are low and the oxygen profile at the centre-
further seen from the CO profiles (Fig. 4c and d) which give line exhibit a similar distinct zero-level as for air-fired
significantly lower concentration levels compared to the air conditions.
and OF 27 cases. The decline in combustion intensity of the The total intensity signal in Fig. 3 corresponds to q1 in
OF 21 case can to a large extent be attributed to the Eq. (8) with the furnace wall emissivity equal to unity.
reduced temperature levels compared to the other two The q1-profiles shown in Fig. 3 are a result from the probe
cases, as shown previously in Fig. 3. Similar results with being traversed through the combustion chamber and
poor combustion intensity and ignition stability in tests directed towards the opposite hot refractory lined furnace
with OF 21 feed gas mixtures, but under coal-fired condi- wall (not shown in the figure). Fig. 3a shows that the max-
664 K. Andersson, F. Johnsson / Fuel 86 (2007) 656–668

a 14 10
b 7 3
Meas. port: R2
Air: O2 9
12 6
OF 21: O2 2.5
8
OF 27: O2
O2 concentration [vol %]

O2 concentration [vol %]
10 Air: HC 5

HC concentration [vol %]
7
OF 21: HC

HC concentration [vol%]
2
OF 27: HC
8 6 4

5 1.5
6 3
Meas. port: R3
4 Air: O2
2 OF 21: O2 1
4 3
OF 27: O2
Air: HC
2 1
2 OF 21: HC 0.5
OF 27: HC
1
0
0
0 0
0 100 200 300 400 0 100 200 300 400
Distance from centreline [mm] Distance from centreline [mm]
c d 8
14 95 95
7

12 Meas. port: R2 Meas. port: R3

CO2 concentration [vol %]

Air: CO 90 6
CO concentration [vol %]

Air: CO 90
CO concentration [vol%]

CO2 concentration [vol %]

OF 21: CO OF 21: CO
10
OF 27: CO 5 OF 27: CO
Air: CO2 Air: CO2
85 85
8 OF 21: CO2 OF 21: CO2
4
OF 27: CO2 OF 27: CO2

6 3
10 10

4 2

5 1 5
2

0
0
0 0
0 100 200 300 400 0 100 200 300 400
Distance from centreline [mm] Distance from centreline [mm]

Fig. 4. Measured radial O2 and HC (a and b) and CO and CO2(c and d) mean concentration profiles at positions R2 and R3, respectively.

imum measured radiation intensity 100 mm from the centr- increase in CO2 partial pressure (approximately eight times
eline is recorded close to the flame boundary as indicated the pressure level of normal air-fired conditions), from
by the temperature profiles. Moving towards the probe which an increase in gas band radiation is anticipated.
wall to the right the intensity drops, as the absorption The difference in total emissivity and in gas emissivity is
becomes higher than the emission. therefore compared between the O2/CO2 and air cases in
The information from the temperature distributions order to evaluate if the increase in overall emissivity can
shown previously together with the radial profiles of radia- be attributed to an increase in CO2 band radiation only.
tion shows that the emissivities of both O2/CO2 environ- The O2/CO2 environment is represented by the OF 27 case;
ments differ from those of reference conditions in air. As since the experimental radiation data is restricted for the
seen the radiation intensity is higher in the OF 27 case than OF 21 case (i.e. no measurement data is available on q2).
in the air case despite the fact that the radial temperature It should be noted that significant differences in emissivity
levels are generally lower or similar to those of air. Further- may exist also between OF 21 and OF 27 conditions since
more, it can also be seen that in spite of the overall lower the soot volume fraction may change from one O2/CO2
temperature levels of the OF 21 case compared to the air atmosphere to another. In fact, by comparing the shape
case, the OF 21 radiation intensity profiles approaches of the radiation intensity profiles in Fig. 3a it is seen that
those of the air case. The obvious physical difference the peak intensity 100 mm from the centreline is clearly
between the air case and the O2/CO2 conditions is the accentuated for the OF 27 condition, which is not the case
 K. Andersson, F. Johnsson / Fuel 86 (2007) 656–668 665

a 650 900

850
625
Wall temperature [oC]

Gas temperature [oC]

800
600

750
575

700
Air, TBR
550
Air, TBL Air, Tgmin
650
OF 21, TBR Air, Tgmax
OF 21, T OF 27, Tgmin
525 BL
OF 27, Tgmax
OF 27, TBR 600
OF 21, Tgmin
OF 27, TBL OF 21, Tgmax
500 550
0 200 400 600 800 1000 1200 1400 0 200 400 600 800 1000 1200 1400
Axial distance from burner inlet [mm] Axial distance from burner inlet [mm]
Fig. 5. (a) Axial distribution of the furnace wall temperature, 20 mm from the inner wall surface at the right (TBR) and the left (TBL) hand side of the
measurement ports. (b) Axial distribution of the minimum (Tgmin) and maximum (Tgmax) gas temperatures at the inner surface of the furnace wall.

in the two other test environments. This may indicate local suction pyrometer. The furnace wall temperatures are mea-
differences in emissivity between the tests conditions, which sured at the right (TBR) and left hand side (TBL) of the
could be caused by changes in soot volume fraction. probe ports on the same axial distances from the burner
In order to determine the total mean emissivity, the as shown in Table 1. As seen, the distribution of gas and
background wall temperature needs to be determined. wall temperatures correlate well for all three cases with
Fig. 5 shows the furnace wall temperatures for the three the highest gas and wall temperatures obtained in the OF
cases, measured with thermocouples at a distance 20 mm 27 case at a distance of 800 mm from the burner, where
from the inner furnace wall surface (a) together with the the temperature drops faster than for both air and OF 21.
measured minimum and maximum gas temperature (b), Fig. 6a shows a comparison of radiation intensity pro-
measured close to the inner furnace wall surface with the files for air and OF 27 conditions in port R3, measured

OF 27 conditions - Ts [oC]
a b 660 670 680 690 700

45 0.7 1050
Meas Port: R3 Measurement port: R3
Air - q1 Air: ε m
40 Mean radiation temperature, Tmr = f(Ts)
OF 27 - q1 OF 27: ε m
Radiation intensity q [kW/m2sr]

Air - q2 OF 27:Tmr 1000

ε m = f(Ts)

35 OF 27 - q2 0.6 Air:Tmr

30
950
Mean emissivity

25 0.5

900
20

15 0.4
850
10

5 0.3 800
0 100 200 300 400 630 640 650 660 670 680
Distance from centreline [mm] Air conditions - Ts [oC]

Fig. 6. (a) Comparison of radiation intensity profiles, air and OF 27 conditions, measured against both cold black-body target (q2) and hot refractory
furnace wall (q1) in port R3. (b) Tmr and em based on the measurements given in Fig. 6a and calculated as a function of different furnace wall temperatures
(Air: 655 ± 20 C and OF 27: 680 ± 20 C).
666 K. Andersson, F. Johnsson / Fuel 86 (2007) 656–668
against both a cold black-body target, which represents the
term q2 in Eq. (9), and the hot refractory lined furnace wall,
i.e. q1 in Eq. (9). These data together with the radiation
intensity reading of the background wall alone, q3 in Eq.
(9), is used to determine the mean flame emissivity, em,
and an average flame radiation temperature, Tmr, for the
OF 27 and air-fired conditions, respectively. The results
are presented in Fig. 6b, where em and Tmr are plotted as
a function of the background furnace wall temperature.
For the calculation the radiation intensities at 400 mm
from the centreline are used, since the furnace cross sec-
tional emissivity is of interest. As can be seen, the accuracy
of the surface wall temperature prediction is critical. With
the predicted wall surface temperatures, i.e. 655 C for the
air case and 680 C for the OF 27 case, the total emissivity
becomes 0.41 and the mean radiation temperature becomes
about 930 C for the air-fired case, and for the OF 27 case
the total emissivity becomes 0.52 and the mean radiation
temperature becomes approximately 950 C.
There was a difficulty to obtain a stable radiation
intensity signal from the furnace wall alone (i.e. q3) since
the water-cooling of the probe cool down the wall as soon
as the probe is positioned close to the wall. Therefore, the
measurements of wall radiation intensity was repeated
twice for the air-fired test condition in port R3 with a
measured intensity of 13.4 ± 0.4 kW/m2 sr which together
with eb = 1 corresponds to an inner wall surface tempera-
ture of 655 C with an error margin of about ±10 C.
This repetition was however not carried out for the OF
27 condition, but instead the same DT over the 20 mm
of refractory lining has been assumed as for air-fired con-
ditions, based on the temperature measurements shown in
Fig. 5. The measured furnace wall temperatures, 20 mm
from the inner wall surface, are shown in Fig. 5a. As seen,
the temperature level corresponding to probe port R3, in
principle constant in time, is approximately 25 C higher
for OF 27 conditions compared to those of air from
which the inner wall surface temperature Ts has been esti-
mated to 680 ± 10 C for the OF 27 condition. Including
the thermocouple measurement error this results in a total
error margin of about ±20 C for the assumed wall
temperatures.
Eqs. (12)–(18) are applied to determine the gas emissiv-
ity with the input parameters listed in Table 4, where the
partial pressures of the two respective gases are assumed
constant within the measurement volume. Compared to
measurement data this assumption does not introduce
any significant error as seen in Fig. 4d, where the radial
CO2 profile (on dry basis) shows relatively small changes
in the total concentration level. As previously described,
the gas concentration measurements were performed on
dry basis, and so the water vapour concentration is
obtained from stoichiometric calculations with conditions
as specified in Table 2 and fuel properties according to
Table 3. The background surface temperatures are the
same as the ones used in Fig. 6b although the error margin
has been disregarded, since in this case it has a negligible
Table 3
Fuel composition and oxygen quality
Fuel analysis (average mole content)
Methane 0 mol%
Ethane < 0.1 mol%
Propane 98.3 mol%
Butanes 1.1 mol%
Pentanes and higher <0.1 mol%
Total unsaturated HC <0.1 mol%
Sulphur <1 mg/kg
Hi 46.4 MJ/kg
Oxygen
Quality (industrial std) 2.5 –
Oxygen content 99.5 vol.%
influence on the results. The path length of the gases is
the same as the inner diameter of the furnace.
The results from the gas emissivity model using Eqs.
(12)–(18) are given in Fig. 7, where eg is shown as a func-
tion of average gas temperature for the furnace cross sec-
tion (cf. the average flame radiation temperature Tmr in
Fig. 6b). The emissivity of the water vapour is significant
in both environments although dry flue gas recycling is
applied, with air and OF 27 conditions given in Fig. 7a
and b, respectively. In fact, at lower gas temperatures
eH2 O is still dominating over eCO2 also in the OF 27 case
(Fig. 7b) although the temperature dependence of eH2 O
reduces its importance at higher radiation temperatures
such as in the near flame region. The measured gas temper-
atures in port R3 (Fig. 3b) show a close resemblance for the
two cases as does the calculation of the mean radiation
temperature in Fig. 6b.
For a similar mean gas temperature as the air case the
OF 27 total gas emissivity is increased with about 20–
30% for the gas temperature interval given in Fig. 7, where
the difference is accentuated at higher temperatures due to
the stronger temperature dependence of eH2 O compared
eCO2 for the conditions specified in Table 4. For example,
with the mean radiation temperatures given in Fig. 6b,
i.e. in the range between 930 and 950 C, eg becomes
0.23 in the air-fired case and 0.29 in the OF 27 case. When
comparing the absolute values of the change in em (Fig. 6b)
and eg (Fig. 7) it is seen that for similar gas temperatures
(Fig. 3b), the difference between the two combustion envi-
ronments in terms of increased radiation intensity of the
OF 27 case (Figs. 3 and 6a) can only partly be explained
by the high CO2 content in the combustion gas. Errors
introduced in the calculation of em, mainly due to the wall
temperature prediction, as shown in Fig. 6b, and the grey
gas approximation, as will be discussed below, should not
be neglected when comparing em and eg. Yet, the conclu-
sion that the total emissivity of the OF 27 flame increases
more than that suggested by an increased emissivity due
to CO2, is consistent with the measured radiation intensi-
ties for the OF 27 environment compared to air. For the
OF 27 case the peak intensity increases with more than
30% and the net incident wall intensity (q2 in Fig. 6a)
 K. Andersson, F. Johnsson / Fuel 86 (2007) 656–668 667

a 0.36
Test case: Air
b 0.36
Test case: OF 27
ε CO2 ε CO2
0.32 0.32
ε H 2O ε H 2O
εg εg
Gas emissivity ε=f(Tg)

Gas emissivity ε=f(Tg)

0.28 0.28

0.24 0.24

0.2 0.2

0.16 0.16

0.12 0.12

0.08 0.08
700 800 900 1000 1100 1200 1300 700 800 900 1000 1100 1200 1300

Average gas temperature Tg [oC] Average gas temperature Tg [oC]

c 0.42
Test case: Air
d 0.42
Test case: OF 27
Total gas emissivity and absorptivity εg /α g

0.4
εg Total gas emissivity and absorptivity ε /α 0.4 εg
0.38 0.38 α g hot BBT
α g hot BBT
0.36 0.36 α g cold BBT
α g cold BBT
0.34 0.34

0.32 0.32

0.3 0.3

0.28 0.28

0.26 0.26

0.24 0.24

0.22 0.22

0.2 0.2

0.18 0.18

0.16 0.16
700 800 900 1000 1100 1200 1300 700 800 900 1000 1100 1200 1300

Average gas temperature Tg [oC] Average gas temperature Tg [oC]

Fig. 7. The gas emissivity given as a function of average gas temperature of the furnace cross section for (a) air-fired conditions and (b) OF 27 conditions
with the hot furnace wall as background. The gas emissivity and absorptivity as a function of average gas temperature for (c) air-fired conditions and (d)
OF 27 conditions with both hot and cold black-body targets (BBT) as backgrounds.

Table 4
Input parameters, partial pressure (pa), background surface radiation
temperature (Ts) and path length (L) to the gas emissivity model
Test case pCO2
Air 0.10
OF 27 0.78
increases with approximately 20% in port R3 (Fig. 3b)
compared to the air case despite similar temperature
profiles.
Fig. 7c shows that the maximum difference between the
total gas emissivity and absorptivity for the reference con-
dition in air is approximately 10% when the gas tempera-
ture varies between 700 C and 1300 C with two different
background temperatures, i.e. the background temperature
equal to the furnace wall temperature or to that of a cold
black-body target. The difference increases for the OF 27
pH2O Ts (K) L (m) case with a maximum difference of about 25% between
0.14 928 0.80 emissivity and absorptivity for the corresponding gas and
0.18 953 0.80 background temperatures, which to some extent affects
the calculation accuracy of the total mean emissivity, since
the combusting flow is not a prefect grey gas as assumed.
Yet, for the mean radiation temperatures and total mean
emissivities calculated (cf. Fig. 6b) the relative error is sig-
nificantly reduced and the results obtained from Eqs. (9)
and (10) show good agreement with the measurement data
shown in Figs. 3 and 6. Hence, a comparison of the mean
emissivity as obtained from Eqs. (9) and (10), in relation to
the total gas emissivities determined according to Eqs.
(12)–(18) shows that the significant increase in radiation
668 K. Andersson, F. Johnsson / Fuel 86 (2007) 656–668
intensity of the OF 27 case compared to the air case is due
to an increased in-flame soot volume-fraction in addition
to the increased band radiation from the CO2.
4. Conclusions
This paper presents measurement data for three different
test cases: reference tests in air and two O2/CO2 test cases
with different recycled feed gas concentrations of O2 (21
and 27 vol.%) and CO2 (79 and 73 vol.%). The measure-
ments show that the temperature levels of the OF 21 flame
are significantly lower than in the reference conditions in
air due to cooling by the recycled CO2, which results in a
suppressed development of the OF 21 flame. Compared
to the OF 21 case the fuel burn-out of the OF 27 case is
favoured by the increased temperature level and improved
mixing conditions between fuel and O2. The OF 27 case
therefore exhibits similar overall combustion behaviour
as the air-fired reference case in terms of gas concentration
and temperature profiles. The analysis of the temperature
and radiation profiles suggests significant changes in emis-
sivities for the O2/CO2 environments compared to refer-
ence conditions in air. For example, the flame radiation
intensity increases with up to 30% for the OF 27 case com-
pared to air-fired conditions despite the fact that the radial
temperature levels are generally lower or similar to those of
air. The difference in total mean emissivity compared to the
difference in gas emissivity for the air and the OF 27 case
shows that the higher radiation intensity in the OF 27 case
cannot solely be explained by an increased gas emissivity.
Hence, the combined experimental and modelling results
show that the in-flame soot volume fraction increases from
the air-fired flame to the OF 27 flame. Changes in soot vol-
ume fraction should therefore be taken into consideration
when modelling the radiative heat transfer of gas-fired
O2/CO2 flames in addition to changes in CO2 and H2O
concentration levels.
Acknowledgement
This work was financed by the Swedish Energy Agency,
the ENCAP project (SES6-CT-2004-502666) within the EU
6th Frame Work Programme and AGA Gas AB.
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