Combustion and Flame 159 (2012) 2789–2798

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Combustion and Flame

j o u r n a l h o m e p a g e : w w w . e l s e v i e r . c o m / l o c a t e / c o m b u s t fl a m e

Numerical investigation of soot formation mechanisms in partially-premixed

ethylene–air co-flow flames
Victor Chernov a, Qingan Zhang a,1, Murray John Thomson a,⇑, Seth Benjamin Dworkin b
a
Mechanical and Industrial Engineering, University of Toronto, 5 King’s College Circle, Toronto, Ontario, Canada M5S 2G8
b
Mechanical and Industrial Engineering, Ryerson University, 350 Victoria Street, Toronto, Ontario, Canada M5B 2K3

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

Article history: Recently, an improved chemical mechanism of PAH growth was developed and tested in soot computa-
Received 31 October 2011 tions for a laminar co-flow non-premixed ethylene–air diffusion flame [Dworkin et al., Combust. Flame
Received in revised form 22 February 2012 158(9) (2011) 1682–1695]. With the intention of testing the robustness of the solution methodology
Accepted 23 February 2012
on partially-premixed systems, this work used the same algorithm as that in the study of Dworkin
Available online 1 May 2012
et al. for computations of two sets of sooting partially-premixed co-flow laminar ethylene–air flames.
The results show very good qualitative and good quantitative agreement with the experimental results
Keywords:
for soot volume fractions and soot precursors, without any changes to the parameters of the model.
Soot
Laminar flame
The soot yield was found to initially increase with decreasing primary equivalence ratios, and then to
Diffusion flame decrease for U < 24, reaching levels lower than the non-premixed case for U < 10. On the flame center-
Partially-premixed flame line, both PAH and acetylene-related processes were found to be important for soot growth. The initial
Computational combustion increase in the soot yield was linked to higher inception rates. On the wings of the flame the dominant
soot growth process was found to be HACA growth. The initial increase in the soot yield was mostly due
to higher acetylene yield leading to faster surface growth. The primary air was also found to influence the
soot oxidation process by increasing OH radicals in both the centerline and the wings region.
Ó 2012 Published by Elsevier Inc. on behalf of The Combustion Institute.

1. Introduction The laminar co-flow diffusion flame is a common configuration

Reducing the environmental impact of combustion is one of the
major goals in the design of energy systems. One of the most impor-
tant combustion-generated pollutants is soot. Soot consists of small,
sub-micron particles that contain mostly carbon. The size of the par-
ticles vary according to the flame conditions. Soot poses various
risks and influences many areas; it is a health hazard, it plays a role
in climate change, it reduces the lifetime of energy producing com-
ponents, and it is an esthetic nuisance. Understanding the mecha-
nisms behind the formation and behavior of these particles can
help create less polluting- and more effective combustion systems.
Soot inception, growth, and oxidation are influenced both by
the chemistry and fluid dynamics of the system [1]. Many practical
systems feature complex geometries and the combustion is usually
non-premixed and turbulent. Unfortunately, a detailed soot emis-
sion model of such systems is not feasible, both due to the high
computational cost involved, and due to the lack of a complete
understanding of the processes behind soot behavior.
⇑ Corresponding author. Fax: +1 416 978 7753.
E-mail addresses: victor@mie.utoronto.ca (V. Chernov), aqzhang@alumni.
utoronto.ca (Q. Zhang), thomson@mie.utoronto.ca (M.J. Thomson), seth.dworkin@
ryerson.ca (S.B. Dworkin).
1
Has moved to Canadian Natural Resources Limited, 855-2nd St. SW Calgary, AB,
Canada T2P 4J8.
that is used to study soot behavior. The most popular configuration
for investigation of laminar co-flow flames is the annular burner
[2]. This burner allows for the studying of convection–diffusion ef-
fects on the soot behavior without the additional complexities that
are introduced when the flame is turbulent. Many experimental
and computational studies have been conducted using the Santoro
burner by various groups [3–11].
The partially-premixed flame is an additional step towards a
more complete understanding of combustion processes. In this
case, the co-flow configuration is used, but the central tube sup-
plies a rich mixture of fuel and air. Partial premixing is important
for several reasons. Firstly, many practical combustion applica-
tions, such as gas-turbine combustors and domestic appliances
are partially-premixed. In most cases, the aforementioned flames
are turbulent, but understanding the laminar case is an important
step towards understanding those flames. Secondly, in turbulent
flames, different degrees of mixing are present. Data gathered from
partially-premixed laminar flames has the potential of providing
insights for turbulent flame analysis. Thirdly, the additional com-
plexity of the partially-premixed configuration allows for better
validation of the computational methods and approaches.
Unfortunately, the amount of works that have examined soot
formation in the partially-premixed configuration is limited.
Works that include soot measurement either contain a spatial

0010-2180/$ - see front matter Ó 2012 Published by Elsevier Inc. on behalf of The Combustion Institute.
doi:10.1016/j.combustflame.2012.02.023
2790 V. Chernov et al. / Combustion and Flame 159 (2012) 2789–2798
measurement of a soot volume fraction without species measure-
ments [12–14], or soot volume fraction, temperature and species
concentration on the centerline only [15].
The number of works that included computational analysis of
the soot formation in partially-premixed laminar flames is even
smaller. Domenico et al. [16] calculated the soot volume fraction
in the partially-premixed Santoro configuration. The authors used
the sectional approach for PAH growth and a two-equation soot
model. The results were compared with several experimental
works, including that of McEnally and Pfefferle [15]. Only one pre-
mixing ratio was shown, though the authors say that all the other
ratios measured by McEnally and Pfefferle [15] were tested. The re-
sults showed good agreement with the experiments, but their use
of a two-equation soot model prevents detailed soot analysis. Katta
et al. [14] used a different burner for a partially-premixed flame.
They too used a two-equation soot model. For the non-premixed
case, the soot volume fractions that were calculated were higher
than measured values, and for low premixing the computations
showed agreements with the measurements. Increasing premixing
caused a major disparity between the predicted and measured pro-
files of soot volume fraction.
The common approximation that the simple two-equation soot
model uses is that of soot as monodispersed carbon spheres. This is
far from physical reality [16]. Soot particles are complex aggre-
gates of carbon spheres. When performing a fundamental analysis,
this point should be taken into account. A common approach is to
use the sectional representation [17,18]. Earlier works have
adopted a sectional representation for the mass of a soot spherical
particle only [3–5,19]. A more robust approach is to use the sec-
tional model for both the sizes of the spherical particles, and for
the number of the primary particles per aggregates [9–11]. The lat-
ter approach is used in the present work.
One of the main challenges in soot modeling is describing soot
inception. Most detailed computational studies model the nucle-
ation of a soot particle as a result of a collision of two pyrene mol-
ecules [20]. Therefore it is vital to have a reliable pathway to
pyrene creation. The under-prediction by most aforementioned
works of the soot volume fraction on the centerline of the flame,
where the dominant process is inception, underlines this problem.
The most common mechanism for pyrene creation is the
hydrogen-abstraction-acetylene-addition (HACA) pathway [20,21].
However, this pathway was deemed to be incomplete, and re-
cently, a new mechanism that includes additional pyrene path-
ways was suggested [22]. Dworkin et al. [23] implemented an
updated reaction scheme from [22] for a laminar ethylene diffusion
flame, and obtained a significant improvement of the soot volume
fractions compared to the HACA-dominated mechanisms.
Our main interest in this work is to examine whether this im-
proved chemical mechanism of PAH growth, coupled with the sec-
tional representation, can predict the main trends of a set of
partially-premixed flames. Therefore, we continue the work of
Dworkin et al. [23], and implement the mechanism that was sug-
gested by Slavinskaya and Frank [22] in partially-premixed flames
of ethylene and air. The computational setup is shown in Section 2.
Experimental works of Arana et al. [13], called ‘‘Dataset 1’’, and of
McEnally and Pfefferle [15], called ‘‘Dataset 2’’, were used for mod-
el validation. The computed results for soot volume fractions, and
species, for both flames, are shown in Section 3, and a discussion is
held in Section 4.
2. Computational model and setup
The computational approach is summarized here, however, for a
more detailed description, the reader is directed to [9,10,23]. The
axial symmetry of the burner permits use of a two-dimensional (z
and r) coordinate system. For the gaseous phase, fully-coupled
elliptical conservation equations for mass, energy, and species mass
fraction are solved. Soot particle dynamics are described using a
sectional model. Soot particle mass ranges are divided logarithmi-
cally into 35 discrete sections. Soot aggregates that are composed
of primary particles of equal size with a constant fractal dimension
of 1.8, are divided similarly to 35 sections for the number of primary
particles per aggregate. Conservation equations of soot aggregate
number densities and primary particle number densities are solved.
The nucleation of a soot particle is modeled as the collision of
two pyrene molecules [20]. Soot surface growth is implemented
using the HACA mechanism and PAH condensation. The empirical
correction parameter a, which reconciles the inaccuracies in treat-
ing sites on the soot surface as corresponding sites on gaseous PAH
molecules, is chosen to be a = 0.078, the same value as that used by
Dworkin et al. [23]. Radiative heat transfer by soot, H2O, CO2, and
CO is calculated using the discrete-ordinates method, and a statis-
tical narrow-band correlated-k-based model [24].
Two experimental datasets are modeled. The first dataset, la-
beled ‘‘Dataset 1’’ in this work, is modeled after the experiments
of Arana et al. [13]. The second dataset, labeled ‘‘Dataset 2’’ in this
work, is modeled after the experiments of McEnally and Pfefferle
[15]. Both are based on a Santoro laminar coaxial annular burner
[2]. For both datasets, a fuel–air mixture flows from a 0.55 cm-in-
ner-radius tube, and the secondary air flows from a 5.41 cm-radius
outer tube. The computational domain extends to 12.29 cm (192
control volumes) in the axial direction, and to 5.41 cm (92 control
volumes) in the radial direction. A non-uniform mesh with fine res-
olution in the flame region is used. The inlet velocities are assumed
to be uniform. The inlet temperature of the fuel mixture is set to
400 K and the temperature of the secondary air is set to 300 K.
The fuel temperature inlet conditions are based on the experimen-
tal data of Dataset 2 [15]. Dataset 1 [13] does not provide temper-
ature measurements at the inlet and since the experimental
conditions were similar, it was decided to use the same inlet tem-
peratures for both flames. Symmetry, no-slip (a chimney encloses
the flame), and zero-gradient conditions are enforced at the center-
line, the outer radial boundary, and the outflow boundary condi-
tions, respectively. The flame is solved using distributed-memory
parallel processing, with the computational domain divided uni-
formly into 192 subdomains, with the boundaries of each subdo-
main perpendicular to the z-axis.
The inlet velocities and the composition of the fuel mixtures
were different for the two datasets. The fuel mixture in Dataset 1
[13] consisted of a mixture of ethylene and air. Five flames (with
different primary equivalence ratios U) are investigated. U is de-
fined as the ratio of the primary air flowrate that is required for
complete combustion, to the actual primary flow rate. The inlet
velocity and the composition of the fuel–air mix for different val-
ues of U are given in Table 1. The composition is given in mole frac-
tions. The secondary air velocity is ua = 8.905 cm/s. Spatial soot
volume fractions were measured. No species concentrations were
reported in [13].
The fuel mixture of Dataset 2 [15] consists of ethylene, air,
nitrogen, and argon. Six flames are investigated. The inlet velocity
and the composition of the fuel–air mix for different values of U
Table 1
The inlet velocity and the composition of the fuel–air mix for different values of U for
Dataset 1 [13].
U uf (cm/s) X C2 H4 X O2 X N2
1 7.072 1 0 0
24 11.29 0.62647 0.07807 0.29546
20 12.13 0.58292 0.08717 0.32991
10 17.19 0.4114 0.123 0.4656
5 27.32 0.2589 0.1549 0.5862
 V. Chernov et al. / Combustion and Flame 159 (2012) 2789–2798 2791

Table 2
The inlet velocity and the composition of the fuel–air mix for different values of U for
Dataset 2 [15].

U uf (cm/s) X C2 H4 X O2 X N2 X Ar

1 16.7 0.3025 0 0.6875 0.01

24 19.69 0.25662 0.03169 0.70317 0.00852
12 22.67 0.22283 0.05504 0.71474 0.00739
6 28.87 0.17498 0.0881 0.73111 0.00581
4 26.13 0.14499 0.10882 0.74138 0.00481
3 30.78 0.12309 0.12395 0.74887 0.00409

are given in Table 2. The composition is given in mole fractions.

The secondary air inlet is partially obstructed by a copper ring that
extends from a radius of 2.75 cm, to the outer chimney (i.e. at z = 0,
r P 2.75 cm, uair = 0). This led to the secondary air velocity at the
inlet being ua = 32.63 cm/s. Centerline soot volume fractions and
species concentrations were reported. The results are reported as
a function of normalized axial distance, where the normalizing fac-
tor is the height, HT at which the maximum temperature is
observed.

3. Comparisons of the computed results with the experimental

data

3.1. Centerline soot volume fraction

Figure 1 shows the soot volume fractions along the centerline

for Dataset 1 [13]. The authors in [13] do not report the experimen-
tal uncertainty, but judging from the scatter of the experimental
results on Fig. 1 alone, an uncertainty of 30% is a reasonable esti-
mate; the actual total uncertainty might be higher due to a lack
of reliable estimates of the optical parameters of soot. It can be
seen that the predictions have the correct order of magnitude
and follow the same general trend as the experimental data. The
plots in Fig. 1 also indicate a systematic under-prediction by a fac-
tor of two to three.
Figure 2 shows the soot volume fractions along the centerline
for Dataset 2 [15]. The fuel mixture in Dataset 2 is diluted with
N2 and Ar and the flame temperature is about 150 degrees lower
than the flame temperature in Dataset 1 [13]. It can be seen that
excellent qualitative agreement was obtained – the results capture
well the slight increase in soot when U is decreased from infinity
(non-premixed) to 24, and the subsequent decrease in soot con-
centration as U is further decreased. The overall shape and loca-
tion, relative to the flame height, of the region in which the soot
is present, is also captured well. Quantity-wise, the soot volume
fraction is under-predicted by a factor of six, which is in line with
centerline predictions made by Dworkin et al. [23]. The under-pre-
diction factor is similar for all primary equivalence ratios.
Neither Dataset 1 [13] nor Dataset 2 [15] show centerline soot
volume fractions varying significantly with U in the U > 10 range.

3.2. Radial soot volume fractions

Figure 3 shows experimental (left side) and numerical (right

side) comparisons for radial profiles of soot volume fraction, at var-
ious axial heights for Dataset 1 [13]. Here, the comparisons are
made lower in the flame at (a) z = 2 cm, (b) z = 3 cm, and (c)
z = 4 cm. Similarly, Fig. 4 shows the same comparisons higher up
in the flame at (a) z = 5 cm and (b) z = 6 cm. Unfortunately, no ra-
dial measurements were reported for Dataset 2 [15]. The model
predicts well the trends for U = 5, U = 10, and U = 20, with the soot
on the wings (in the r = 2 cm and r = 4 cm ranges) decreasing with
increased flowrates of primary air. One discrepancy is that in the
experimental data, the largest soot concentrations are seen at
Fig. 1. Centerline soot volume fractions of Dataset 1 for various primary equiva-
lence ratios: (a) U = 1, (b) U = 24, (c) U = 20, (d) U = 10, (e) U = 5. The line solid is
the model predictions, the symbols are the experimental results from Arana et al.
[13].
U = 24, whereas in the computed data, the largest soot concentra-
tions are at U = 1. The model does not predict the slight soot vol-
ume fraction increase for U = 24 over that of U = 1 seen on the
wings in Figs. 3 and 4. However, quantitatively, the predictions fall
2792 V. Chernov et al. / Combustion and Flame 159 (2012) 2789–2798

Fig. 2. Centerline soot volume fractions of Dataset 2 for different primary equivalence ratios (a) computed and (b) measured [15].

Fig. 3. Radial soot volume fractions for the lower part of Dataset 1 (a) z = 2 cm, (b) z = 3 cm, (c) z = 4 cm. The left hand side figures show experimental results [13], the right
hand side figures show computed results.
 V. Chernov et al. / Combustion and Flame 159 (2012) 2789–2798 2793

within experimental errors for all primary equivalence ratios ex-
cept U = 5. The predicted flame is slightly higher than the mea-
sured one, and therefore does not predict as well soot volume
fractions for z = 6 cm (Fig. 4b). At this height soot has essentially
burned out, but the model still predicts the existence of a signifi-
cant amount of soot. It is important to mention that the qualitative
agreement was obtained using the non-premixed modeling param-
eters of Dworkin et al. [23], without any modifications, thereby
demonstrating model robustness.
3.3. Centerline species
Species measurements were reported for Dataset 2 [15] only. The
measurements were taken along the centerline. Figures 5–7 show
the concentrations of acetylene, benzene and naphthalene, respec-
tively. In each of the Figs. 5–7, the computed concentration profiles
are plotted on the left, and the measured values appear on the right.
The trends of initial increase and subsequent decrease of the species
is captured by the computations for each of these three species. The
quality of the comparisons differ among the species. Acetylene
(Fig. 5) is predicted very well for the non-premixed case, but the var-
iation in its peak concentration with increased primary air flow is
much smaller than that which was observed experimentally. Ben-
zene (Fig. 6) computations are remarkably accurate in the concen-
trations and in the shape of the profile. Naphthalene (Fig. 7) is
under-predicted by a factor of two for all primary equivalence ratios.
Despite significant experimental uncertainty in the measured
values, the data suggests that the reason for the under-prediction

Fig. 4. Radial soot volume fractions for the higher part of Dataset 1 (a) z = 5 cm and (b) z = 6 cm. The left hand side figures show experimental results [13], the right hand side
figures show computed results.

Fig. 5. Centerline acetylene concentrations of Dataset 2 for different primary equivalence ratios (a) computed and (b) measured [15].
2794 V. Chernov et al. / Combustion and Flame 159 (2012) 2789–2798

Fig. 6. Centerline benzene concentrations of Dataset 2 for different primary equivalence ratios (a) computed and (b) measured [15].

Fig. 7. Centerline naphthalene concentrations of Dataset 2 for different primary equivalence ratios (a) computed and (b) measured [15].

of the soot volume fractions for Dataset 2 [15] is the gas-phase
reaction mechanism that under-predicts the growth of PAHs. For
each level of premixing (U), the growth to benzene (the first aro-
matic ring) is very well predicted (Fig. 6). However, the growth
of the second ring to naphthalene is consistently under-predicted
by about a factor of two (Fig. 7). This suggests that despite signif-
icant development, the pathways to PAH growth in the chemical
mechanism [22,23] may still be incomplete. This fact is further
supported by the under-prediction of soot in the inception-
dominated flame centerline (Figs. 1 and 2) by a factor of two to
eight, which has been shown to be closely correlated to pyrene
(the fourth aromatic ring) [23]. As the size of the PAHs increases,
so too does the under-prediction factor. This remains an open area
of investigation in chemical mechanism development.
It should be noted that the PAH measurements in Figs. 6 and 7
have a large uncertainty. McEnally and Pfefferle [15] report an
uncertainty of 30% for the benzene measurements and a factor of
three for the naphthalene measurements. As a result, the only con-
crete conclusion that can be said about the computational results is
that they are consistent with the measurements. This difficulty
highlights a general challenge that flame and soot modeling is
facing – the lack of accurate PAH species measurements in flames
for model validation.
4. Discussion
One of the most interesting results that is observed in partially-
premixed flames is that the soot does not monotonically decrease
with decreasing primary equivalence ratio. Figure 2 illustrates this
behavior by showing that the soot volume fraction for U = 24 is
slightly higher than for the non-premixed case, and otherwise
the soot volume fraction decreases with decreasing U. However,
since soot volume fraction is influenced not only by the combus-
tion processes, but also by the initial fuel concentration, it is best
to look at the local soot yields (i.e. the fraction of the fuel carbon
converted to soot), in order to assess the nature of the soot behav-
ior in the partially-premixed flames. Figure 8a shows the com-
puted centerline local soot yield normalized by the maximum
centerline local soot yield, for the non-premixed case of Dataset
2 [15]. Figure 8b shows the computed local soot yield on the max-
imum soot path through the wings of the flame, normalized by the
 V. Chernov et al. / Combustion and Flame 159 (2012) 2789–2798 2795

Fig. 8. The computed normalized soot yield (a) on the centerline in Dataset 2 [15] and (b) on the path of maximum soot in Dataset 1 [13].

maximum local soot yield for the non-premixed case of Dataset 1

[13]. The path of maximum soot is an axial collection of points,
where their radial location is determined according to the maxi-
mum soot point at that particular height. The maximum soot path
is often referred to as ‘‘wings’’, since in most parts of the flame that
region is located somewhat off the burner centerline. Wings are
usually characterized by fast soot growth and most of the soot
can be found in this region. It is located just inside of the flamefront
in the non-premixed case.
We see that in both flame regions, the centerline and the wings,
there is a trend of initially rising local soot yield peaking at U = 24
and subsequently, declining with decreasing U. However, we can
also see that a wide range of primary equivalence ratios exhibit lo-
cal soot yields higher than in the non-premixed case (U = 12, 24 on Fig. 9. The computed relative mass contribution for the centerline of Dataset 2 [15].
the centerline and U = 10, 20, 24 on the maximum soot path). The
local soot yields start to fall to levels below the non-premixed case
only for low values of primary equivalence ratio (U 6 6 for the cen-
terline of Dataset 2 [15] and U < 10 for the wings of Dataset 1 [13]).
The next sections explain this phenomenon by identifying the
dominant soot processes in both flame regions, and by finding their
relation to the presence of the primary air.

4.1. Centerline soot behavior

Soot growth is influenced by three main processes: inception,

acetylene HACA surface growth, and PAH condensation. In this
work, we choose to divide these processes into two parts for the
analysis; PAH related processes, and acetylene related processes.
In practice it means that inception and PAH condensation are
examined together, and the HACA surface growth is examined sep-
arately. The reason for this treatment is that currently the incep-
tion model of a collision of two pyrene molecules [20] is not a
comprehensive way to couple the PAH gas-phase mechanism with
the soot growth mechanism, and the PAH condensation model
when considering incipient soot particles is akin to an inception
process.
Figure 9 shows the relative contribution to the soot mass of
growth species, as a function of the primary equivalence ratio U,
on the centerline of flames, in Dataset 2 [15]. It can be seen that
with increased primary air flow, the contribution of acetylene
along the centerline is increased, while the contribution of PAHs
is decreased. It can be seen that both processes contribute signifi-
cantly, and both are important as far as the soot mass is concerned.
Figure 9 does not tell the whole story. In our group’s previous
work [23], it was found that for the ethylene diffusion flame, the
correct prediction of centerline soot volume fraction is dominated
Fig. 10. Computed relative values of the inception rate and local soot yield on the
centerline of Dataset 2 [15].
by inception – changing the values of a had a negligible influence
on the soot volume fraction, but a mechanism that predicted pyr-
ene concentration more accurately on the centerline played a vital
role in obtaining accurate soot volume fractions. The present work
shows that inception, even though it is modeled in a representative
manner, plays a very important role in explaining the higher cen-
terline local soot yield profiles for U > 6 that are seen in Fig. 8a. Fig-
ure 10 shows the values of the maximum inception rate and local
soot yield normalized by the non-premixed flame values for Data-
set 2 [15]. It can be seen that inception correlates closely with the
local soot yield, suggesting that indeed inception is an important
mechanism converting carbon to soot on the centerline, and that
the current inception model is able to describe qualitatively the
physics of the particle nucleation. Therefore, the explanation for
2796 V. Chernov et al. / Combustion and Flame 159 (2012) 2789–2798

Fig. 11. Computed centerline soot volume fraction of Dataset 2 [15] for (a) U = 24 and (b) U = 3 for three different oxidation modes.

Fig. 12. Computed mole fractions along the centerline of Dataset 2 [15] (a) O2 and (b) OH.

the soot yield behavior seen in Fig. 8a lies in the gas phase PAH
chemistry that is responsible for the changes in inception rates
with changing primary equivalence ratios.
Let us examine the soot oxidation processes. Soot oxidation is
modeled using two species, O2 and OH. To better understand their
respective roles in partially-premixed flames, Fig. 11 shows the
computed centerline soot volume fraction for Dataset 2 [15], with
three different oxidative models; the first model considers both O2
and OH to be participating in soot surface oxidation, the second
model is with OH participating only, and the third model is with
O2 oxidation only. It can be seen from Fig. 11a that O2 oxidation
does not affect peak soot levels. However for the case of little pre-
mixing (U = 24) when O2 oxidation is removed, the soot is not
completely oxidized at the end of the computational domain and
shows characteristics of a smoking flame. When OH oxidation is re-
moved (O2 oxidation only), the centerline soot volume fraction in-
creases slightly and the effect of OH oxidation on peak soot levels
increases with further decreasing primary equivalence ratio. From
Fig. 10b, it can be seen that in the case of heavy premixing (U = 3),
when oxidation by OH is removed, the soot volume fraction center-
line profile increases by a factor of two, whereas removing O2
oxidation has a negligible effect. Here it can be concluded that in
the flame region, the dominant oxidative species is OH. As premix-
ing is increased, OH oxidation of soot increases and lowers peak
levels. O2 oxidation is only important in the post-flame region of
the less-premixed flames.
The oxidative species can originate from two sources; from the
primary or the secondary air. Figure 12a shows the concentration
of O2 along the centerline of Dataset 2 [15]. It can be seen that
O2 from the primary air is consumed before z/HT = 0.5, for all values
of U. In the context of Fig. 11a, from which it is noted that O2 oxi-
dation only becomes significant after z/HT = 0.8 for U = 24, it can be
concluded that in the cases where O2 participates in the soot oxi-
dation, it comes from the secondary air. Figure 12b shows that
the concentration of OH increases with decreasing U, and that its
concentration starts to rise approximately at z/HT = 0.6. Figure
11b shows that the soot oxidation for U = 3 starts at around the
same height. According to our calculations, the differences in OH
fractions cannot be explained by temperature differences only.
Therefore we can conclude that the OH that participates in soot
oxidation on the centerline originates from the reactions of the pri-
mary air with the fuel.
 V. Chernov et al. / Combustion and Flame 159 (2012) 2789–2798
4.2. Soot behavior on the path of maximum soot (wings)
It is common to assume that HACA growth is the main contrib-
utor to soot mass on the wings of the flame [23]. Figure 13 shows
the relative contribution to the soot mass of growth species as a
function of the primary equivalence ratio U on the wings of flames
in Dataset 1 [13], at the point of maximum soot. It can be seen that
HACA growth is the dominant process of soot growth for the full
range of U.
Examining the behavior of acetylene on the wings can explain
the reason for the initial increase in the soot yield with decreasing
U. Figure 14 shows the local yields of acetylene on the wings. It can
be seen that the local yield of acetylene (i.e., the relative amount of
fuel converted to acetylene) increases monotonically with decreas-
ing primary equivalence ratio.
The total mass gain is also a function of the oxidation, which
inhibits the growth of the soot particles. Figure 15 shows the mole
fraction of OH along the maximum soot path of Dataset 1 [13], for
each of the primary equivalence ratios. O2 is not shown since in the
growth region it is negligible. It can be seen that the concentration
of OH increased by a factor of seven between the non-premixed
case and U = 5, which leads to faster soot oxidation. Therefore it
can be concluded that the partial premixing influences the soot
on the wings in two competing ways; firstly, it provides relative in-
creases in acetylene concentration, which contributes to the fast
soot growth on the wings, and tends to increase soot formation
as partial premixing is increased, and secondly, it provides more
OH to the wings, which increases the soot oxidation, and tends
to decrease soot formation as partial premixing is increased. For
a wide range of primary equivalence ratios (24 6 U 6 10), soot
yields are slightly higher than in the non-premixed case, and do
not vary significantly between the different values of U, suggesting
that the effects of the increases in OH are balanced by the increases
Fig. 13. The computed relative mass contribution for the wings of Dataset 1 [13].
Fig. 14. Computed local yields of acetylene along the maximum soot path of
Dataset 1 [13].
2797
Fig. 15. Calculated OH mole fractions along the maximum soot path of Dataset 1
[13].
in acetylene and pyrene. At high premixing (U 6 5), soot yields are
decreased, suggesting that the effects of increased OH dominate
over the increases in acetylene and pyrene.
5. Conclusions
A detailed soot model including PAH growth, soot inception,
and aerosol dynamics, was applied for the first time to a set of
partially-premixed laminar flames of ethylene and air. The goals
were to see whether the computations are able to track the trends
of soot formation, to assess the accuracy of the model, and to draw
conclusions about main effects on soot processes caused by partial
premixing. The computed results were tested against two experi-
mental sets of data. Several main conclusions can be drawn.
All of the computed results were within reasonable accuracy of
soot prediction, and some results exhibited excellent quantitative
agreement with the experiments. Major trends were also predicted
well in most cases. All this was done without changing any param-
eter in the soot model proposed by Dworkin et al. [23] for non-
premixed flames, which demonstrates the model’s robustness.
It was found that the soot yield initially increases with the
introduction of the primary air. When the flowrate of the primary
air is further increased, the soot yield decreases and only falls be-
low the soot yield of the non-premixed flame for U < 10. The rea-
son for this lies mainly in the gas phase chemistry, but specifics
differ according to the flame region.
The centerline soot growth was found to be related to soot
inception rates. The non-monotonic increase in soot yield from
U = 1 to U = 24, followed by subsequently decreasing soot yields
for successively lowering values of U, was found to be attributable
to the gas phase PAH chemistry that controls soot inception. Both
the acetylene addition through the HACA mechanism, and the PAH
induced growth through inception and condensation were found to
be important factors in the soot mass accumulation. On the wings,
the soot mass yield was dominated by acetylene addition. The non-
monotonic increase in soot yield from U = 1 to U = 24, the plateau
for 24 6 U 6 10, and the eventual decrease for U = 5 was found to
be attributable to competing factors; increasing OH for soot oxida-
tion, and increasing acetylene for growth with decreasing U. The
initial increase in acetylene caused higher soot yields for U = 24.
For lower primary equivalence ratios, these increases were bal-
anced by the increases in OH, which eventually became dominant
at U = 5.
The soot oxidation was found to be OH dominated, both on the
centerline and on the wings. The OH effect increased with lower
primary equivalence ratios (higher levels of premixing). For both
datasets, increases in the flowrate of the primary air led to a rapid
and full consumption of the O2 in the fuel stream, and to increased
supply of OH radicals, both to the centerline and in the wings
region.
2798 V. Chernov et al. / Combustion and Flame 159 (2012) 2789–2798
Acknowledgments
The authors acknowledge Dr. Nadezhda A. Slavinskaya, Prof. Pe-
ter Frank, and Prof. Uwe Riedel of the German Aerospace Centre
(DLR) for providing the DLR reaction mechanism. The authors
acknowledge Mr. Lyon Sachs of Montreal, Canada for financial sup-
port. The authors acknowledge the Natural Sciences and Engineer-
ing Research Council of Canada and the Ontario Ministry of
Research and Innovation for financial support. Computations were
performed on the GPC supercomputer at the SciNet HPC Consor-
tium. SciNet is funded by: the Canada Foundation for Innovation
under the auspices of Compute Canada; the Government of Ontar-
io; Ontario Research Fund – Research Excellence; and the Univer-
sity of Toronto.
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