A Parametric Study of N O z E m i s s i o n from Turbulent H a and

CH 4 Jet Diffusion F l a m e s
RUEY-HUNG CHEN*
Department of Mechanical, Materials and Aero.~paceEngineering, Unicersity of Central Florida. Orlando, Florida
32816-2450

Nitrogen dioxide (NO z) emission levels of fuel jets were experimentally studied for H z, H . . / H e mixtures, a
H z / H e / C H ~ mixture, and C H 4. The study was undertaken to understand the dependence of NO z emission
in turbulent diffusion flames on parameters other than the widely known effects of rapid mixing. These
parameters are fuel types (CH4 vs H2). the initial NO level, and the flame temperature. The fuel mixtures
were chosen such that these factors could be investigated independently. In all the flames studied, NO2/NO~
increases with dccreasing NO concentration in the flame and with decreasing adiabatic flame temperature.
"['he CH~ fuel demonstrates a qualitatively different influence on the NO2/NO, ratio than !-I2. Its effects
are most pronounced whcn the flame blowout limit is approached. Adding a small amount of CH 4 to the H,
flames also qualitatively affected the NO2/NO t ratio. © 1998by The Combustion Institute

INTRODUCTION sion flames, and to nearly 100% in C3H 8 flames

The present study was motivated by previous
studies of hot gas jets (not flames) that showed
that the N O 2 / N O x ratio was affected by cer-
tain system parameters. The hot gas might be
produced using combustion methods and with
a controlled amount of NO added, before it
exited the nozzle. The parameters affecting the
I~,T#"'k l ~ T f ~
1,,-'2/ ,,'-,x rati~ of the hot gas jets are the jet
fluid temperature, the NO level in the jet, and
the trace amount of fuel existing in the sur-
roundings. This paper seeks to study these
factors that may affect the N O z / N O x ratio in
turbulent jet diffusion flames. NO 2, which is
potentially more hazardous than NO and re-
sponsible for photochemical smog formation, is
more soluble than NO and may be removed by
scrubbing processes [1]. The ability to control
the N O z / N O x ratio in practical diffusion
flames is thus technologically relevant.
Some previous experimental observations of
significant N O , levels are shown in Table 1 for
diffusion flames in various combustion devices
and hot gas jets generated using premixed
flames of H 2 and C3H8 [2-11]. The N O , / N O x
ratio ranges from a few percent in simple H 2
jet flames to about 50% for coaxial jet diffu-
* Formerly with Department of Aerospace Engineering,
The University of Michigan-Ann Arbor, and Department
of Mechanical and Aerospace Engineering, Princeton Uni-
versity.
0010-2180/98/$19.00
PII S0010-2180(97)00111-9
under gas turbine conditions (i.e., coaxial air
with swirl) [3, 4, 9]. It is known from the
foregoing references that the mixing in turbu-
lent jet flames was increased by adding coaxial
air flows. Further mixing enhancement were
achieved by imparting swirling motion to the
coaxial air flow. The mixing enhancement was
seen as the flame lengths were significantly
reduced. One conclusion is that rapid mixing
promotes N O to NO2 conversion by generating
H O 2 radicals around the flame [12-14].
For hot gas jets containing NO, some other
factors besides mixing rates have been demon-
strated to influence the N O 2 / N O x ratio, The
following conclusions were made of various hot
gas jet studies. (1) The N O z / N O x ratio in-
creases with decreasing temperatures of the
hot gas jet [7]. (2) The N O z / N O x ratio de-
creases with the "initial" NO level [6]. (3) The
N O 2 / N O ~ ratio could reach 90% if the sur-
rounding air is "doped" with trace amounts of
hydrocarbon fuel species [14]. The degree of
promotion is related to the hydrocarbon fuel's
ability to generate HO2 in the mixing region
and the NO to N O , conversion increased with
the hydrocarbon fuel concentration added to
the surrounding air [14]. Similar effects of hy-
drocarbon were also observed in flow reactors
and laminar diffusion flames, where up to 100%
NO to NO~ conversion occurred [1, 15]. It is
noted that (1) and (2) were observed when the
surrounding air was not "doped" with hydro-
carbons.
COMBUSTION AND FLAME l ! 2: 188-198 (1998)
© 1998 by The Combustion Institute
Published by Elsevier Science Inc.
N O , EMISSION F R O M T U R B U L E N T D I F F U S I O N FLAMES 1891

TABLE I

Some Experimental Results of Emitted NO2/NO , Ratio of Various Flame Types

Reference Flame Type Fuel Reynolds Number NOz/NO,
7 Hot jet of lean prcmixed C3H ~ up to 81%
flame products ~
Hot jet of rich premixed C 3H s up to 90%
flame products"
6 Hot jet of lean premixed C3H ~ ( + NO) up to 70%
flame products (& = (l.37)"
2 Turbulent jet diffusion flames C3Hs I-6.0 × 104 49-58%
18 Premixed (~b = 0.45-11.625) C~Hs up to 100%
9 Gas turbine combustor Natural gas up to )011%
I0 Turbulent jet diffusion flames C 311,~ up to 811%
with weaklyswirled coaxial air
)) Turbulent jet diffusion flames C31-I~ = 50%
3 Turbulent co~txialjet diffusion tlamc H, 5,0110 2-14%
CI 1~ 5,(1011 2-23%
3. 8 Swirl-stabilized
turbulent H, 10,000-30,000 25-67%
diffusion flame
5 Turbulent jet diffusion flame 40r; CO/30r~ H 2/311c; N, 8,5011 --- 50%
Present Turbulent jet diffusion flame H, 5,0110-17,115 !.5-4.6%
study CI714 5,0(8)- ) 2,000 8-40%
H ,-He 5,001)- 12,001) 2.6-50%

Hot product jets arc generated using lean or rich premixed flames, product gases of which are then introduced into
surrounding air.

The effects of hydrocarbon presence, when N O J N O x ratio in turbulent jet diffusion

coupled with those of flame temperature and
initial NO concentration, were not clear from
previous diffusion flame studies [2-4]. They
have yet to be systematically studied. The fuel
effects are to be expected, especially when the
flame is near its blowout limits. The fuel may
leak through ~he lifted flame ba~e, through the
flame due to finite rate chemistry, or simply
through the locations of local quenching
("holes"). As the blowout limits are ap-
proached, the amount of leakage increases,
rendering the air surrounding and downstream
of the flame to be increasingly "doped" with
the fuel. This situation is similar to a hot gas
jet issued into air containing doped fuel
[12-14].
In diffusion flames, the highest temperatures
exist only at the flame location, where NO
forms. For the far field probe, a diffusion flame
acts as a high temperature source of gas con-
taining NO, as in hot gas jets. It is therefore
interesting to explore whether similar issues
(the observations (1) and (2) in the preceding
text) exist, as found in hot gas jet studies, and
how these system parameters affect the
flames.
As a first step, only H2 and C H 4 a r e chosen
as fuels: H2, He-diluted H2, CH4, and a mix-
ture of 59% H 2 , 36% He, and 5% C H 4. The
fuel mixtures are designed sG that the effects
of temperature, the NO level, and fuel types
can be independently studied. The aim is to
understand the effects of flame temperature,
NO level, and CH 4 level. No direct compari-
son can be drawn between a hot gas jet and a
turbulent je'~ diffusion flame. However, the
conclusion from hot gas jet studies helps iden-
tify parameters to be studied for the present
turbulent jet diffusion flames.
EXPERI1V~=ENT
The details and procedures of the experimen-
tal setup, the NOx measurement, and probe
effects are exactly the same as those described
in [:3, 4, 8] and are sketched in Fig. 1. The
b u r , er sketched in Fig. 1 was originally de-
signed to allow the use of coaxial air, as indi-
cated in the figure. For the present study, the
flame was that of a simple fuel jet and the
190 R.-H. C H E N

WATER-COOLED A chemiluminescence analyzer combined

with a stainless steel thermal converter and a
water-cooled stainless steel probe [3, 4, 8] was
used to differentiate N O and N O 2. Probe ef-
fects were shown to be negligible [3, 4, 8]. The
probe was always located at more than one
,~ THERMOCOUPLE flame length downstream o f the flame tip,
where the concentration of NO~ was nearly
uniform across the exit and thus allowed easy
conversion of the emission indices from con-
centration (ppm) levels. The wall t e m p e r a t u r e
during N O x sampling was monitored and was
in the range of 300-400°C. The day to day
repeatability o f these measurements was found
to be within 10% for NOx and N O and the
accuracy is 0.5 ppm. The test conditions are
given in Table 2, which also contains flame
lengths, conversion factors of emission index of
N O x from p p m levels, and the calculated adia-
~ HONEYCOMB
ANDSCREEN batic flame t e m p e r a t u r e s of the fuel mixtures
chosen. Adiabatic flame t e m p e r a t u r e calcula-
!
COl:LOW AIR L---- COAXIAL AIR tions, using the C E C code [16], led to the
WITH OR WITHOUT choice of 59% H 2 / 3 6 % H e / 5 % C H 4 and
FUEL SWIRL
60% H . , / 4 0 % He, because their adiabatic
Fig. 1. Experimental facility.
flame t e m p e r a t u r e s are close to that o f C H 4
flames. The molecular weight used for emis-
coaxial air tube was removed. A circular con- sion index is that of NO. Due to the effects o f
finement of 15 cm in d i a m e t e r and 91.5 cm in initial N O concentrations mentioned in the
length was placed concentrically with the Introduction, p p m levels a p p e a r to be more
burner. T h e coflowing air velocity was kept to relevant for the present study. The overall
be less than 1% of the fuel jet velocity and was equivalence ratio based on the fuel and
m e a n t to eliminate the wall effect of the con- coflowing air flow rates was kept equal to 0.5
finement; no visual difference was observed (i.e., 100% excess air) for all flames so that the
between confined and unconfined flames. comparison of initial N O levels is meaningful.

TABLE2
Experimental Conditions, Flame Length, Calculated Adiabatic Flame Temperature, and Emission Index
Conversion Factor
Adiabatic Flame EmissionIndex
Jet Diameter, Jet Reynolds Flame Length Temperature ConversionFactor
Fuel dr ( m m ) Number (Re)~ ( Lf/dt: ) (Tf, K)h (g/kg ppm- ~Y
CH4 1.6, 2.6, 3.7 5000-12,000 185 -194 2227 0.1)376
H2 1.6, 2.6, 3.7 5000-17,115 179 -192 2383 0.0789
80% H2/20% He 1.6, 2.6, 3.7 5000-12,000 140-155 2324 0.1005
60% H2/40% He 1.6, 2.6, 3.7 5000-10,000 94 -98 2227 I}.1365
40% H 2/60% He 1.6, 2.6, 3.7 5000-8,000 70 -76 2040 0.2086
59% H2/36% He/5% CH 4 2.6 5000-9,000 --- 110 2235 0.0451
a Based on fluid properties at 298 ~r. effective viscosities of fuel mixtures calculated according to Ref. 17.
b Calculated using CEC code [16].
c Based on the molecular weight of NO.
NO, EMISSION FROM T U R B U L E N T DIFFUSION FLAMES
It is noted that the number of NO, data was
limited for some flame conditions. This is pri-
marily due to the flame blowout limits. No
pilot flame or other mechanism was used to
extend the blowout limits. This is because local
extinction, flame liftoff, and near-blowout con-
ditions are the primary reasons for incomplete
combustion rendering surrotmding air to be
"doped" with fuel species and it is one of the
focuses of this study.
RESULTS AND DISCUSSION
NO~ measurements (Figs. 2-6) were donc un-
der increasing Reynolds number (Re) until the
flames blew off, except for thc pure H ~ flames
which remained attached throughout thc ex-
perimental conditions. For those flames that
blew out, flame liftoff preceded blowout.
Reynolds numbers were based on the jet fluid
properties at the exit and at 298 K. The effec-
tive viscosity of the jet fluid/fuel mixture was
calculated according to Ref. 17. Fig. 2 shows
the emission levels of oxides of nitrogen of
100% hydrogen jet diffusion flames with jet
diameters (d r) equal to 0.16, 0.26, and 0.37 cm.
The ppm levels of NO~ for these flames ap-
peared as emission indices in a previous article
[3]. It is noticed that NO, levels for larger jct
diameters are higher at all Reynolds numbers,
primarily due to longer residence time or larger
flame volumes/lengths for Zeldovich/thermal
NO to form [3, 4]. It decreases with Reynolds
number for a given jet diameter, primarily due
to a decrease in residence time [3]. The
N O 2 / N O , ratio increases only slightly or rc-
mains constant with the Reynolds number, as
can be seen in Fig. 2.
The qualitative trends of the NO_,/NO, ra-
tio of H 2 and CH4 flames are in sharp contrast
(see Figs. 2 and 3). In the case of CH~ jet
flames (Fig. 3), NO2/NO~ increases by a factor
of 3 - 4 from Re = 5000 to blowout with
Reynolds number for a given jet diameter,
while NO~ level remains nearly constant (24-26
ppm for both d e = 0.26 and 0.37 cm; flames
with d~-= 0.16 cm blew out beyond Re =
6000). The values of N O 2 / N O ~ of these flames
are about 10 times higher than those of pure
H 2 flames (20-30% vs 2 - 3 % ) within similar
Reynolds number ranges and jet diameters
191
(Fig. 2). Further results will be shown in the
following tcxt that H , and CH4 have signifi-
cantly diffcrent effects on the N O , / N O ~ ratio.
Effect of "Initial" NO Concentration and
Flame Temperature
To study the effects of the flame/product gas
temperature without the complication of fuel
effects, He was added to H~. Calculated adia-
batic flame temperatures for H 2. 811% H_,/20%
He, 6{1~ H2/40% He, and 40% H 2 / 6 0 % He
flamcs arc 2383, 2324, 2227, and 21}40 K, re-
spectively. The results of the NO_,/NO X ratio
and NO, of thcse 20% He- and 40% He-di-
luted flames are plotted in Figs. 4 and 5. It is
sccn that in these H , flames (including the
undiluted) that the N6,_/NO, ratio increases
with increasing degree of dilution for a given
jet diameter and, therefore, with decreasing
flame/product gas temperature, similar to
trends in hot gas jets. For example, as the
degree of He dilution increases from zero to
40% (Figs. 2 and 5), thc NO_,/NO~ ratio in-
creases from less than 3 to about 20-40% for
the three jet diameters. For 60% He dilution,
the ratio ranges from 40-50% (not shown be-
cause of limited data due to flame blowout and
the low NO level, which was well within experi-
mental uncertainty).
Considering the temperatures of these flames
and that NO 2 will be converted back to NO at
temperatures greater than about 1500 K (cf.
[18]), only NO can form and exist at the flame
zone. The NO, levels at the measuring loca-
tion can therefore be viewed as the "initial"
concentration of NO for the far-field sampling
probe. Therefore for the far-field probe, the
measured NO~ level is the "initial" NO level,
similar to those of hot gas jets. For all diluted
and undiluted H 2 flames (Figs. 2, 4, and 5),
initial NO decreases or remains nearly con-
stant with Re for a given jet diameter. Similar
observations and NO emission level analysis
can be found in Refs. 3 and 4.
Comparing flames having a given degree of
dilution and similar Reynolds numbers (i.e., a
given adiabatic flame temperature; Figs. 2, 4,
and 5) but different jet diameters, the
N O 2 / N O ~ ratio indeed increases with decreas-
192 R.-H. C ~ E N

80 5

¢ ~ (a) d F = 0 . 1 6 c m
4
60
3

2
40

20 i i i i i i 0
4000 6000 8000 10000 12000 14000 16000 18000

100

(b) dF = 0.26 cm
4
80

3 dz

~ 60 6
z
z

40 i ! ! i ~ , 1
4000 6000 8000 10000 12000 14000 16000 18000

160 5

(C) (:IF = 0.37 em

140

120
o o
o o o o ' ,o----I~

100 = i i = = = 1
4000 6000 8000 10000 12000 14000 16000 18000

R e y n o l d s N u m b e r (Re)
Fig. 2. NOt levels and NO2/NO ~ ratio as functions of the Reynolds number of turbulent I I,
jet diffusion flames. The ppm levels of NO, are equivalent to Chcn and Driscolrs emission
index [3].

ing initial N O level. In undiluted H~ flames
the N O level decreases approximately three-
fold from about 130 to 40 ppm, from dr: = 3.7
to 1.6 ram, and the N O 2 / N O ~ ratio increases
by about 50% (Fig. 2). In diluted flames (Figs.
4 and 5) similar trends can be seen; the
N O J N O x ratio is doubled o r tripled from
d e = 3.7 to 1.6 mm. These observatlJns are
true for diluted H ,_ flames near blowout. !t is
recalled that the diluted flames were o p e r a t e d
up to the Reynolds number for blowout in
Figs. 4 and 5.
F o r a given Reynolds number, a smaller jet
d i a m e t e r requires a higher jet exit velocity.
This leads to more rapid mixing and for this
reason the N O J N O x ratio should be higher,
NO_, EMISSION FROM T U R B U L E N T DIFFUSION FLAMES 193

50

(a) dF = 0.26 cm
28 40

26 30

24 20

22 10

2O 1 I | ! 0
40O0 6000 8000 10000 12000

50

(b) dF = 0,37 em
28 40

26 30

24 20

22 10

2O I t i i 0
4000 6000 8000 10000 12000

Reynolds Number (Re)

Fig. 3. N O t levels a n d N O 2 / N O ~ r a t i o as f u n c t i o n s o f the R e y n o l d s n u m b e r o f t u r b u l e n t C H 4
jet diffusion tlames.

as is well known [6, 7, 12, 13]. However, for a
given jet diameter and Reynolds number (i.e.,
same mixing rate), NO2/NOx increases with
the degree of dilution and, therefore, with de-
creasing "initial" NO level. This is seen in the
case of d r = 0.16 cm and Re = 6000, as shown
in Figs. 2, 4, and 5. The N O J N O x ratios are
about 3.5, 6.5, and 40% for pure, 20% He-, and
40% He-diluted H 2 flames, respectively. An-
other example is that of d~. = 0.37 cm and
Re = 10,000, where the N O J N O x ratios are
1.5, 3.0, and 23.0% for pure, 20% He-, and
40% He-diluted H 2 flames, respectively. This
trend can also be seen, both qualitatively and
quantitatively, for other Reynolds numbers and
d r = 0.26 cm.
However, it should be noted that both initial
NO level and flame temperature of these he-
lium-diluted H 2 flames decrease with increas-
ing degree of dilution. This is also consistent
with the fact that the thermal mechanism is
the only cause for NO formation. Therefore
the effects of initial NO level and temperature
cannot be separated. An attempt to fix initial
NO concentration but allow for different flame
temperature would require a comparison of
d r = 0.26 cm CH4 flame with Re = 8000 (Fig.
3a) and d~. = 0.16 cm 80% H i 2 0 % He with
Re = 10,000 (Fig. 4a). Both of these flames are
close to the blowout limit. Both of their initial
NO levels are equal to 26 ppm and the CH4
flame produces a five times higher N O 2 / N O x
ratio than the H 2 flame (40 vs 8%). A smaller
jet diameter and a higher Reynolds number of
the 20% He-diluted H 2 flames means more
rapid mixing in these flames. It is then noted
that factors other than mixing must play a role
in determining the NOE/NO x ratio. If one
follows the results of hot gas jets, the lower
adiabatic flame temperature of CH4 flames
m a y be responsible for the higher N O , / N O x
ratio.
194 R.-H. C H E N

35

30

25
~ (a) dF = 0 . 1 6 cm

20 i i i i

4000 6000 8000 10000 12000

lO
(b) dF = 0.26 crn
8
55

5o
3 4 ~
~ 4s
2
z

40 i i i i o
4000 6000 8000 10000 12000

(c) dF = 0.37 cm

_~ • •
o

o o

50 i i i i

4000 6000 8000 10000 12000

Reynolds Number (Re)

Fig. 4. NOt levels and NO~/NO, ratio as functions of the Reynolds number of 8(1%
Hj2U% tie turbulent 1-12 jet diffusion flames: (a) dr = 0.16 cm; (b) d~. = 0.26 cm; (c)
d~ = 0.37 cm.

For similar initial NO levels but different
flame t e m p e r a t u r e s consider pure H 2 flames
with d F = 0.16 cm and 20% He-diluted H 2
flames with dr = 0.26 cm (Figs. 2a and 4b).
For Re = 7000-12,000 these flames have N O
levels in the range of 4 0 - 5 0 ppm. A lower
adiabatic flame temperature (2324 K with 20%
He dilution vs 2383 K of pure H 2) results in
doubling tile N O z / N O x ratio (5 vs 2.5%), de-
spite the smaller jet diameter and higher jet
velocities of the pure H 2 flames implies smaller
turbulent mL~ng time scale for the same
Reynolds numbers. It can be concluded that
for diluted and undiluted H 2 flames, a lower
flame temperature leads to a higher N O 2 / N O x
ratio for similar given initial NO levels.
NO 2 E M I S S I O N F R O M T U R B U L E N T D I F F U S I O N F L A M E S 195

(a) dF = 0 . 1 6 em
40

3O

4 20

2 lO

o -- i i I i L n 0
40o0 5000 6000 7000 8000 9000 10000 11000

10 5O
(b) dF --- 0.26 cm
8 40

6 30 C~
z
4 20 0
z
2 10

0 i i i I i 0
4000 5000 6000 7000 8000 9000 1ooo0 11 o00

• (C) dF = 0.37 em
40
4--- ""
30

o o
f 20
o....---~ °
10

5 i i i i i i 0

4000 5000 6000 7000 8000 9000 10000 11000

Reynolds Number (Re)

Fig. 5. NO, levels and NO.,/NO, ratio as functions of the Reynolds number of 611c+
112/40"4 lie turbulent tt 2 jet diffusion flames: (a) tit = ().16 cm; (b) dr. = 0.26 crn: (c)
d F =(I.37 cm.

To further separate the effect of flame tem-
perature, 60% H 2 / 4 0 % He and c n 4 flames
(Figs. 3 and 5) should be c o m p a r e d since they
have essentially the same adiabatic flame tem-
perature, 2227 K. F o r d F = 0.26 and 0.37 cm,
C H 4 flames produce higher initial N O concen-
tration (by a factor of 2 - 3 ) and higher
N O J N O x ratios than those of 40% H e - d i -
luted H , flames by a factor of about 2 toward
the blowout limit, as can clearly be seen by
comparing the results of Figs. 3 and 5. Such an
observation, without considering the hydrocar-
bon fuel effects, is contrary to the results from
pure and diluted H , flames as well as hot gas
jet studies. Combining the preceding observa-
tions suggests that there are factors other than
196 R.-H. C H E N

25

z
o............4/ \
/ /

0 I I I i i 0

4000 5000 6000 7000 8000 9000 10000

Reynolds Number (Re)

Fig. 6. Comparison of NO~ levels and NO,/NO x ratio of 50% H2/36% He/5% CH 4, 60%
H2/4(l% He, and CH4 flames that have similar adiabatic flame temperatures (-= 2230 K). For
all flames d~. = 0.26 cm. Solid symbols, NO, level; empty symbols, NO,/NO,.

mixing, flame t e m p e r a t u r e , a n d initial N O con- d i f f e r e n t in H 2 a n d C H 4 flames. T h e

c e n t r a t i o n affecting N O to N O 2 c o n v e r s i o n
w h e n H z and C H 4 flames are c o m p a r e d .
Differences between H 2 and C H 4 F l a m e s
F r o m the p r e v i o u s observations, t h e qualitative
t r e n d s of the N O 2 / N O x ratio a r e t h e r e f o r e
N O 2 / N O x ratio o f C H 4 flames increases by a
factor o f 3 - 4 as the R e y n o l d s n u m b e r in-
creases f r o m 5000 t o w a r d b l o w o u t ( R e -'- 8000
a n d 12,000 for d r = 0.26 and 0.37 cm, respec-
tively, as shown in Fig. 2). Since t h e N O z / N O x
ratio o f H 2 flames increases at best only slightly
with R e e v e n n e a r t h e b l o w o u t limit, t h e dif-
NO,- EMISSION FROM T U R B U L E N T DIFFUSION FLAMES
ference between the NO_,/NO, ratios of CH~
and H~ flames is therefore most pronounced
near the blowout limit. Speeitic comparison
can be made bctwecn C H 4 and 6{1% H , / 4 0 %
He flames with dr: = 0.26 cm (Figs. 3a and 5b),
as discussed in the previous paragraph. These
flames have similar blowout Reynolds numbers
( = 8000). While the lower initial NO level may
favor 60% He/4(Jq~: H , flames in producing
NO_,, the N O , / N O , ratio of CH 4 flames near
blowout is more than double that of 6t)c~
H_,/40% Hc flamcs. Similar comparison leads
to exactly opposite results sufficiently removed
from blowout (Re = 50110), for which their
NO_,/NO x ratios arc comparablc and approxi-
mately equal to 22~. This can be due to the
following facts. First, as blowout is approached,
the fuel icakagc through the flamc and lifted
flame base into the air bccomcs morc pro-
nounced. Second, far from flamc blowout lim-
its, the lower initial NO levels of the 60q;
H 2 / 4 0 % He flame can more than compensate
for the less pronounced fuel leakage effects of
CH 4 flames. Then an effect similar to hydro-
carbon addition to the air surrounding the hot
gas jets containing NO might have occurred,
resulting in higher NO_,/NO~ [14]. It has bccn
experimentally shown that a heptane diffusion
flame produced higher N O , / N O , ratios as thc
surrounding air was doped with increasing
amounts of C 3 H s o r natural gas, while the
total NO,. level was not affected [15]; the ratio
could reach nearly 100% when there was ap-
proximately 1000 ppm of natural gas or 2110
ppm of C3H s in the surrounding air.
To further demonstrate the effcct of CH~, a
small amount of it was added to a H , / H e
mixture. The mole ratio was 59% H_,, 5%
CH4, and 36% He by volume for comparisons
with CH 4 flames. This ratio was chosen from
many trial runs and adiabatic flame tempera-
ture calculations because the initial NO con-
centration ( = 25 ppm at Re = 7000) and flame
temperature ( = 2235 K) are nominally equal
in both flames. The results, along with those of
60% H 2 / 4 0 % He flames (2227 K) are shown
in Fig. 6. All flames of Fig. 6 had dr.. = 0.26
cm.
It is noted that for the 59% H , / 3 6 % H e / 5 %
CH 4 flame, the N O 2 / N O ~ ratio increases by a
factor of 2 from Re = 5000 toward blowout
197
conditions (Re-~ 90~)). This is qualitatively
similar to CH 4 flamc:i (a factor of 4; cf, Fig. 3)
and different from H , flames, diluted or undi-
luted (Figs. 2, 4, and'5). This suggests that a
small amount of CH4 may indeed have a quali-
tative effect on the N O 2 / N O x ratio compared
to 611% H2/40% He and other H2 flames. As
noted earlier, the N O 2 / N O ~ ratio of these H 2
flames is insensitive to Reynolds number/mix-
ing, even toward the blowout limit.
For this 59% H 2 / 3 6 % H e / 5 % CH 4 flame
the N O 2 / N O ~ ratio is approximately less than
one-half of that of CH 4 flames in the similar
range of Reynolds numbers (except for Re =
50(~)), although their initial NO levels and
flame temperatures are comparable. Near the
blowout limits (Re = 8000 and 91100 for CH4
and 59% H.,/36% H e / 5 % C H . flames, re-
spectively) the 59% H_,/36% H e / 5 % CH4
flame produced a lower NO2/NO~ ratio al-
though its initial NO level is lower than that of
the CH~ flame. This again suggests the domi-
nant effects of the C H 4 fuel.
Compared to 60% H.,/40% He flames, the
59% H 2 / 3 6 % H e / 5 % CH 4 flames still yielded
lower NO2/NO,., suggesting that there may be
competing effects of low initial NO levels and
fuel type (recall that their flame temperatures
are nearly equal) when CH 4 concentration is
low (see Fig. 6). As shown in Fig. 6, the pure
CH 4 flames approaching blowout yield higher
values of N O 2 / N O , than 40% He-diluted H_,
flames, although the initial NO levels are
higher in the former than in the latter. In this
case. the effect of the predominant CH4 fuel
appears to outweigh the effect of the low ini-
tial NO of H ,- flames and it is most clear when
the flame approaches blowout.
CONCLUSION AND REMARKS
The dependence of NO, emission in turbulent
diffusion flames on parameters other than the
widely known effects of rapid mixing was ex-
perimentally demonstrated. In all the H 2 and
He-diluted H., flames studied, NO2/NO.~ in-
creases with decreasing NO concentration in
flames and with decreasing flame temperature.
The C H 4 fuel demonstrates qualitatively dif-
ferent influence on the NO_,/NO~ ratio than
H,. Its effects are most pronounced when the
198
flame blowout limit is a p p r o a c h e d . A d d i n g a
small a m o u n t of C H 4 to H , flames was also
shown to qualitatively affect the N O 2 / N O ,
ratio. T h e trends r e p o r t e d should f u r t h e r pro-
vide useful c o m p a r i s o n s for numerical simula-
tions of N O , emission from turbulent diffusion
flames.
It is difficult to c o m p a r e N O , emission from
jet flames and hot gas jets. H o w e v e r , the re-
sults of previous hot gas jets do p r o v i d e a basis
for choosing the p a r a m e t e r s studied in this
paper. W h e n the N O x p r o b e is placed in the
far field, the flame may be viewed as the source
of h i g h - t e m p e r a t u r e gas c o n t a i n i n g N O , m u c h
like hot gas jets. It would be interesting for
future studies to carry o u t field m e a s u r e m e n t s
of t e m p e r a t u r e , NOx, and u n b u r n e d hydrocar-
bon concentrations. These measurements
should address w h e t h e r and how fuel leakage
and i n c o m p l e t e c o m b u s t i o n d u e to finite-rate
kinetics and n e a r - b l o w o u t c o n d i t i o n s cause the
surroundings and postflame regions to be
d o p e d with fuel. C o n s e q u e n t l y , m o r e light will
be shed on the m e c h a n i s m of NO_, emission
f r o m diffusion flames.
The work was supported by The Gas Research
htstitute o f Chicago (Project Manager, J. A. Kez-
erie), while the attthor was with The Unh'ersity o f
Michigan. 7he author thanks E - K . Yu ]'or his
help with the figures presented in this article'.
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Receit'ed 30 Not'ember 1995; accepted 21 Febnmry 1997