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Numerical Modeling of the Effects of

Fuel Dilution and Strain Rate on Reaction
Zone Structure and NOx Formation in
Flameless Combustion
a a b
Hamdi Mohamed , Hmaeid Bentîcha & Sassi Mohamed
a
Laboratoire d'Etudes des Systèmes Thermiques et Energétique
(LESTE), Ecole Nationale d'Ingénieurs de Monastir, Monastir, Tunisia
b
The Petroleum Institute, Abu Dhabi, UAE
Version of record first published: 10 Aug 2009.

To cite this article: Hamdi Mohamed , Hmaeid Bentîcha & Sassi Mohamed (2009): Numerical Modeling
of the Effects of Fuel Dilution and Strain Rate on Reaction Zone Structure and NOx Formation in
Flameless Combustion, Combustion Science and Technology, 181:8, 1078-1091

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 Combust. Sci. and Tech., 181: 1078–1091, 2009
Copyright # Taylor & Francis Group, LLC
ISSN: 0010-2202 print=1563-521X online
DOI: 10.1080/00102200903073909

NUMERICAL MODELING OF THE EFFECTS OF FUEL

DILUTION AND STRAIN RATE ON REACTION ZONE
STRUCTURE AND NOX FORMATION IN FLAMELESS
COMBUSTION

Hamdi Mohamed,1 Hmaeid Bentı̂cha,1 and Sassi Mohamed2

1
Laboratoire d’Etudes des Systèmes Thermiques et Energétique (LESTE),
Ecole Nationale d’Ingénieurs de Monastir, Monastir, Tunisia
2
The Petroleum Institute, Abu Dhabi, UAE
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High-temperature oxidation is one of the most promising technologies to reduce pollutants

in combustion systems. The optimization of high-temperature oxidation is very complex,
but has many advantages in the suppression of the thermal NO formation even at relatively
high temperatures. The present study is based on parametric simulations of non-premixed
counter-flow flames of methane with nitrogen dilution and highly preheated air. The objec-
tive of this study is to understand the effects of fuel dilution and strain rate on reaction zone
structure and NOx formation in flameless combustion. This study shows that NOx mass
fractions decrease with an increasing strain rate as well as increasing methane dilution with
nitrogen.

Keywords: Combustion; Flameless; Fuel dilution; NOx emissions; Strain rate

INTRODUCTION
Current research and development activity in the field of combustion
technology is focused on improved energy efficiency and control and reduction of
pollutant emissions from stationary industrial and transportation sources. High-
temperature air combustion (HiTAC; see Katsuki et al., 1998) technology is a
promising candidate for energy saving and low NOx emission in engineering and
industrial application. HiTAC, also referred to as flameless oxidation (FLOX)
(Wünning et al., 1997) and moderate and intense low oxygen dilution (MILD) com-
bustion (De Joannon et al., 2000), is a combustion technology that forms an invisible
flame with theoretically an evenly distributed temperature with very low noise. It is
reported that flameless combustion produces extremely low NOx emissions by utiliz-
ing high-temperature and low-oxygen content inlet air resulting from recirculating
high percentage of hot exhaust gas into the reaction zone.

Received 17 July 2008; revised 12 May 2009; accepted 28 May 2009.

Address correspondence to Hamdi Mohamed, Laboratoire d’Etudes des Systèmes Thermiques et
Energétique (LESTE), Ecole Nationale d’Ingénieurs de Monastir, 5000 Monastir, Tunisia. E-mail:
hamdimh@yahoo.fr

1078
 FLAME COMBUSTION AND NOX FORMATION 1079

Wünning et al. (1997) studied flameless oxidation (combustion) using

experimental and numerical techniques. The study revealed the ability of flameless
combustion to lower NOx emissions through lowered adiabatic flame temperatures.
Ju and Niioka (1997) studied NO formation in a non-premixed two-dimensional
laminar jet flame for the understanding of the effects of turbulence on combustion.
The study showed that the formation of prompt NO is observed in the flame reaction
zone, while the thermal NO mechanism is the predominant path for NO formation
on the high-temperature air side. The emission index of NO was shown to have a
high sensitivity to the oxidizer preheat temperature, increasing drastically with an
increasing preheat temperature.
Maruta et al. (2000) investigated the flameless combustion of methane with
nitrogen dilution and air in a laminar counter-flow geometry. The study revealed
that when the oxidizer temperature is high (1500 K) and the fuel is at a concen-
tration of 5%, flameless combustion can be observed. Fuse et al. (2002) investi-
gated experimentally and numerically the effects of air temperature and oxygen
content on NOx emission in a counter-flow diffusion flame. Hamdi et al. (2004)
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investigated the high-temperature air combustion of partially premixed methane=

air (lean or rich) flames in counter-flow geometry. The study illustrated that the
flame structure for the rich partially premixed flame is significantly affected by
the oxygen concentration in the air, and a significant reduction in NOx emission
is observed. Mungekar and Atreya (2007) presented an experimental and computa-
tional study of NO formation and flame structure in low-strain-rate partially pre-
mixed methane=air counter-flow flame with different dilution mixtures of the fuel
and oxidant streams.
Recently, Hamdi et al. (2008) studied the possibility of integration of the flame-
less combustion mode to an adiabatic combustor, typically used in gas turbine
engines by means of a specific zero-dimensional loop reactor model. The study illu-
strated clearly that the flameless oxidation appears as a promising technique for
industrial gas turbine combustor applications, as even at high operating tempera-
tures and pressures, NOx emissions could be reduced by flameless combustion to
very low levels.
The present study is based on parametric simulations of non-premixed
streams of methane with nitrogen dilution and preheated air. The objective of this
study is to understand the effects of fuel dilution and strain rate on flameless com-
bustion using numerical simulations of a counter-flow non-premixed nitrogen
diluted methane vs. preheated air streams. In particular, the study focuses on
the effects of preheated air temperature, fuel dilution, and strain rate on the flame
structure and NOx formation using an OPPDIF code, the GRI-3.0 mechanism.
This mechanism is widely used to model natural gas combustion, including the
formation of NOx.

NOX FORMATION AND MECHANISM

Glassman (1996) identifies three mechanisms for the formation of NO in com-
bustion devices: the oxidation of atmospheric N2 via thermal NO mechanism,
prompt NO mechanism, and the oxidation of nitrogen-containing compounds in
fossil fuels. In the present study, we are concerned with the first two mechanisms,
 1080 H. MOHAMED ET AL.

thermal and prompt NOx formations. The thermal NO mechanism is described by

the extended Zel’dovich mechanism:

O þ N2 $ NO þ N

N þ O2 $ NO þ O

N þ OH $ NO þ H

The prompt NO mechanism is relatively more complex and has lately been developed
with reasonable confidence (Miller & Bowman, 1989). Prompt NO is formed
when the nitrogen in the air reacts with flame radical to form CN compounds, which
subsequently can react and form NO.
The mechanisms that govern the formation of NOx has been well studied and
documented; however, total agreement on a concrete mechanism that fully governs
the production of all nitrous oxides has not been reached. The GRI-3.0 mechanism
is used to represent the individual elementary reactions involved in the gas phase
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combustion of natural gases (such as methane and propane) with air (Glassman,
1996).

EMISSION INDEX
The emission index for NO is a convenient way of describing the amount of NO
produced per unit mass of fuel. This quantity can be used to compare flames of differ-
ent fuel concentrations along with different strain rates and preheat air temperatures.
The relationship for the emission index of NO used in this study is given by
RL
WNO 0 xNO dx
EINO ¼
RL
WCH4 0 xCH4 dx

where W is the molecular weight of the species associated with the index, x is the net
production rate, and L corresponds to the length of the computational domain, and
refers physically to the separation distance between the fuel and oxidizer jet inlets.
The emission index has dimensions of [kgNO=kgfuel] and is reported in the figures of
this work in [gNO=kgfuel].

COMPUTATIONAL CONFIGURATION AND CONDITIONS

The configuration used in this study is a counter-flow of fuel and oxidizer (see
Figure 1). The separation distance between the two inlets is 5 cm. The flow
conditions adopted in this study are listed in the Table 1. Tow values of preheat
air temperature 1000 and 2000 K are used, while the fuel inlet temperature was kept
constant at 300 K. This study used an average strain rate given by:

Velocity u
strain rate ¼ 2 ¼2
Separation distance L
 FLAME COMBUSTION AND NOX FORMATION 1081
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Figure 1 Counter-flow of fuel and oxidizer.

Table 1 The inlet flow conditions

Fuel concentration (%) Velocity (cm=s) Strain rate (s
1)

15 60 24
13 50 20
11 40 16
9 30 12
7 20 8
5 (flameless) 10 4

The solution is computed using Sandia’s Oppdif code (Lutz et al., 1996) along with
the GRI-Mech 3.0 mechanism (Glassman, 1996) for methane and NOx chemistries.

RESULTS AND DISCUSSION

Effects of Fuel Concentration
Fuel concentration directly affects the strength of the reacting mixture. The
additional dilution of nitrogen on the fuel stream results in an important reduction
in flame temperature, which affects the dominant mechanisms for NOx formation,
especially the thermal NO production mechanism.
As fuel concentration is increased, it is evident that for given conditions, the
amount of fuel available for use in the elementary reactions involving CH4 is
 1082 H. MOHAMED ET AL.

increased. This would tend to increase the overall rate of chemistry as well as the
overall adiabatic flame temperature.
Figures 2 through 5 show the emission index of both thermal and prompt NO
mechanisms as function of fuel concentration at two air preheating temperatures
(2000 K and 1000 K) and for two strain rates (24 s
1 and 4 s
1). The results show that
both mechanisms follow similar trends of increasing with increasing fuel concen-
tration. This trend is consistent with that of increasing overall emission index with
increasing fuel concentration. However, at higher preheat temperatures, the highly
temperature-dependent thermal mechanism has a larger contribution than the
prompt mechanism, while at lower preheat temperatures, prompt NO becomes the
more dominant mechanism. As fuel concentration increases, the dominance of either
thermal (at high preheat temperatures) or prompt (at low preheat temperatures)
increases. It should be noticed here that the overall NO represents the emission index
for NO from all elementary reactions involving the production and consumption of
NO, while the emission index of thermal NO (or prompt NO) represents only the
contribution of thermal NO (or prompt NO) mechanisms. In addition, the integral
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given in the defining equation of the emission index is carried out by applying the
trapezoid rule to the data gathered by the Oppdif post-processor for the reaction
rates of each species. The relative contributions of thermal or prompt NO mechan-
isms are evaluated to identify possible shifts in the dominant NO chemistry as a
function of the computational parameters.
Figure 6 shows the effect of fuel concentration on the radicals O and OH along
with the peak temperature profile, which are all heavily involved in the mechanism
that produces thermal NO. All three increase with an increasing fuel concentration;

Figure 2 Emission index profiles for NOx vs. fuel concentration at air preheated temperature of 2000 K
and strain rate of 24 s
1.
 FLAME COMBUSTION AND NOX FORMATION 1083
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Figure 3 Emission index profiles for NOx vs. fuel concentration at air preheated temperature of 2000 K
and strain rate of 4 s
1.

Figure 4 Emission index profiles for NOx vs. fuel concentration at air preheated temperature of 1000 K
and strain rate of 24 s1.
 1084 H. MOHAMED ET AL.
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Figure 5 Emission index profiles for NOx vs. fuel concentration at air preheated temperature of 1000 K
and strain rate of 4 s
1.

Figure 6 Mass fractions profiles for O and OH vs. fuel concentration at air preheated temperature of
2000 K and strain rate of 24 s
1.
 FLAME COMBUSTION AND NOX FORMATION 1085

however, the OH radical increases five-fold while the O radical only doubles over the
considered fuel range. This seems to indicate that the sensitivity of thermal NO
production is as much related to the O radical pool as the peak temperature in
the reaction zone, but not as much on the OH radical concentration.

Effects of Strain Rate

In contrast with fuel concentration, strain rate affects the residence time of
species in the reaction zone and contributes to the further thinning of the flame
structure, thereby altering the balances of transport by convection and diffusion
within the flame. Changes in residence time will affect primarily relatively slow
reactions, such as the ones associated with the thermal NO production mechanism.
Therefore, while the residence time is lessened as strain rate is increased; the
transport of fuel and oxidizer into the flame is increased, providing more ‘‘food’’
for the flame. Residence time will have an increased effect on slower reaction
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mechanisms. NO and H2 differ in their relative reaction speeds. H2 is a fast reactant

in comparison with NO and will therefore have a lessened sensitivity to a decrease in
residence time, while NO would have a much greater sensitivity to this parameter.
As strain rate increases, the residence time in the reaction zone decreases.
Increased strain may result in local extinction of the flame due an important
reduction in the heat release rate and the rate of chemistry. In flameless combustion,
increased strain also results in tangible reductions in the rate of heat release and
chemistry. Figure 7, which shows profiles of NO and H2 mass fractions as functions

Figure 7 Mass fractions profiles for NO and H2 vs. strain rate at air preheated temperature of 2000 K and
fuel concentration of 15%.
 1086 H. MOHAMED ET AL.

of strain rate at a preheat temperature of 2000 K, depicts this decrease in profiles of

H2 and NO concentrations due to a decrease in residence time for 15% methane
dilution. It can be seen that NO and H2 follow similar trends. Both initially increase
with strain rate, but then decrease at higher strain rate values; this is due to the
initial increase in transport of both fuel and oxidizer to the flame (i.e., a higher sup-
ply of fuel and oxidizer is brought to the flame, resulting in higher peak temperature
and NO, while at even higher strain rates, residence time is decreased and the pro-
gress of the NO reaction is slowed due to its relatively slow reaction). Similarly, H2
follows the same trend; however, it is also important to note that the magnitude
of the profile of H2 mass fractions are of the same order, yet the net change
from the lowest strain rate to the highest is much smaller for the hydrogen molecule,
indicating that H2 is less sensitive to increases in strain rate than NO due to the
faster H2 mechanism.
Figure 7 is a good example of the balance between residence time and trans-
port. When strain rate is decreased, residence time is increased, while a lower supply
of fuel and oxidizer is brought into the flame. This results in an initial increase in
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both mass fractions, as more fuel and oxidizer are supplied to the flame, however,
as strain is lowered further, the flame begins to feel the effects of less fuel and oxidi-
zer transport and there is then a decrease in both NO and H2.
Figure 8 shows that the H2 dependence on strain rate is not the same for all
oxidizer preheat temperatures. When fuel dilution is held constant at 15% and air
preheat temperature is changed to 1000 K, H2 increases monotonically instead of
decreasing with strain rate. However, the difference between the maximum of the

Figure 8 Mass fractions profiles for NO and H2 vs. strain rate at air preheated temperature of 1000 K and
fuel concentration of 15%.
 FLAME COMBUSTION AND NOX FORMATION 1087

hydrogen peak values and the minimum is again very small, reinforcing the con-
clusion that the hydrogen molecule mass fraction is much less sensitive to strain rate
than NO. However, NO does follow the same trend as observed when the preheat
temperature is 2000 K.
In the flameless combustion case (i.e., fuel concentration of 5%), the data indi-
cates that H2 is much less sensitive to strain rate than NO. However, in Figure 9,
which shows the profiles of NO and H2 mass fractions for the flameless condition,
the trends for profiles of H2 mass fraction have reversed, from decreasing with strain
rate at a preheat temperature of 2000 K and increasing with strain rate at a preheat
temperature of 1000 K to the exact opposite.
The trend of increasing hydrogen has been reversed, as can be seen in Figure 10.
The changes, however, between the profiles of H2 mass fraction corresponding to the
highest and lowest strain rates is increased when the preheat temperature is lowered
to 1000 K. Figure 10 shows that the mass fraction of NO decreases and then slightly
increases again at higher strain rates. This is possibly due to the overall weak chemi-
cal reaction.
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Figures 11 through 14 depict the emission index of NO resulting from the indi-
vidual thermal and prompt NO mechanisms along with the overall emission index of
NO. An overall decrease can be seen in both indices as strain rate increases; however,
the balance between transport and residence time can be seen in the thermal NO
emission index, suggesting that the thermal mechanism is perhaps the slower pro-
gressing mechanism. It can again be seen that when preheat temperature is
decreased, the dominant NO production mechanism shifts from thermal to prompt

Figure 9 Mass fractions profiles for NO and H2 vs. strain rate at air preheated temperature of 2000 K and
fuel concentration of 5% (flameless combustion case).
 1088 H. MOHAMED ET AL.
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Figure 10 Mass fractions profiles for NO and H2 vs. strain rate at air preheated temperature of 1000 K and
fuel concentration of 5% (flameless combustion case).

due to the high dependence of the thermal mechanism on temperature. Strain rate is
seen to have no appreciable role in either the conventional flame or the flameless
cases in shifting the dominating contribution of thermal to prompt NO. The NO

Figure 11 Emission index profiles for NOx vs. strain rate at air preheated temperature of 2000 K and fuel
concentration 15%.
 FLAME COMBUSTION AND NOX FORMATION 1089
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Figure 12 Emission index profiles for NOx vs. strain rate at air preheated temperature of 1000 K and fuel
concentration 15%.

Figure 13 Emission index profiles for NOx vs. strain rate at air preheated temperature of 2000 K and fuel
concentration 5% (flameless combustion case).
 1090 H. MOHAMED ET AL.
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Figure 14 Emission index profiles for NOx vs. strain rate at air preheated temperature of 1100 K and fuel
concentration 5% (flameless combustion case).

emission index shows similar magnitude at higher preheat temperatures. This is due
to the normalization by the amount of fuel consumed. However, as preheat is low-
ered, the sensitivity of flameless combustion to oxidizer temperature and subse-
quently excess enthalpy is seen as the emission index drops drastically.

CONCLUSION
The present study is based on parametric simulations of non-premixed counter-
flow flames of methane with nitrogen dilution and highly preheated air to understand
the effects of fuel dilution and strain rate on reaction zone structure and NOx forma-
tion in flameless combustion.
Through this study, it can be seen that there is a general decrease in the
production of NO and H2 with a decrease in fuel concentration. This is due to the
reduced fuel supply to the flame zone. The emission index of NO was found to
decrease as fuel concentration is lowered due in part to the lower reaction rate as fuel
concentration is decreased. While there is a decrease in the overall NO emission
index as fuel concentration is decreased, there is also a decrease in the individual con-
tributions of thermal and prompt NO. Due to the high dependence on temperature
seen in the thermal NO mechanism, the thermal NO mechanism is dominant at
higher preheat temperatures, while the prompt is dominant at lower preheat
temperatures. In contrast with fuel concentration, strain rate has been seen to have
a large effect on the slower NO formation mechanisms, but not the fast ones due to a
balance between decreased residence times and higher mass transport to the reaction
zone and vice versa.
 FLAME COMBUSTION AND NOX FORMATION 1091

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