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Large Eddy Simulation of turbulent nonpremixed sooting flames:

Presumed subfilter PDF model for finite-rate oxidation of soot

Citation for published version:

Colmán, HM, Attili, A & Mueller, ME 2023, 'Large Eddy Simulation of turbulent nonpremixed sooting flames:
Presumed subfilter PDF model for finite-rate oxidation of soot', Combustion and Flame.
https://doi.org/10.1016/j.combustflame.2022.112602

Digital Object Identifier (DOI):

10.1016/j.combustflame.2022.112602

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Combustion and Flame

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Download date: 01. sept. 2023

Manuscript Click here to view linked References

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9 Large Eddy Simulation of turbulent nonpremixed
10
11 sooting flames: Presumed subfilter PDF model for
12
13 finite-rate oxidation of soot
14
15
16 Hernando Maldonado Colmána,⇤, Antonio Attilib , Michael E. Muellera
17
a
18 Department of Mechanical and Aerospace Engineering, Princeton University, Princeton,
19 NJ 08544, USA
b
20 Institute for Multiscale Thermofluids, School of Engineering, University of Edinburgh,
21 Edinburgh, EH9 3FD, United Kingdom
22
23
24
25
26 Abstract
27
28
29 Modeling soot evolution in turbulent reacting flows using Large Eddy
30
31 Simulation (LES) is challenging due to the complex subfilter soot-turbulence-
32
33
chemistry interactions. Soot particles form at fuel-rich mixtures and are
34 subsequently oxidized as they are transported toward fuel-lean mixtures. In
35
36 previous work, this phenomenology was explicitly encoded into a presumed
37
38 subfilter PDF model for soot by confining soot strictly to mixtures where
39
40 growth rates exceed oxidation rates. However, this model implicitly assumed
41
42 that oxidation is infinitely fast. In this work, a new presumed subfilter PDF
43
44 model for soot is proposed to account for finite-rate soot oxidation. The
45
46 distribution of soot with respect to the flame structure (mixture fraction) is
47
48 modeled by comparing the local relative motion of di↵usionless soot particles
49
50 with respect to mixture fraction iso-contours with the local oxidation rate.
51
52 When the oxidation rate is suppressed or the transport rate is very fast, soot
53
54 ⇤
55 Corresponding author.
56 Email address: hm2524@princeton.edu (Hernando Maldonado Colmán)
57
58
59 Preprint submitted to Combustion and Flame December 22, 2022
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9 is allowed to penetrate further into fuel-lean mixtures. This model can allow
10
11 for soot leakage across the flame, a critical phenomenon in smoking flames.
12
13 The new model is validated a priori against Direct Numerical Simulation
14
15 (DNS) databases of turbulent nonpremixed jet flames and then a posteriori
16
17 against experimental measurements in a laboratory-scale turbulent jet flame.
18
19 A priori results show remarkably good agreement with filtered DNS data
20
21 and are shown to correctly allow for soot leakage at low Damköhler number.
22
23 Finally, LES results of the turbulent sooting jet flame show an improvement
24
25
of soot prediction using the new soot subfilter model compared to previous
26
works. In this flame, as in experiments, evidence of soot leakage is found near
27
28 the beginning of the sooting region, and this soot leakage cannot be predicted
29
30 with previous subfilter models that presume infinitely fast oxidation.
31
32 Keywords:
33
34 Soot; Soot-turbulence-chemistry interactions; Soot oxidation; Large Eddy
35
36 Simulation (LES); Presumed subfilter PDF
37
38
39 1. Introduction
40
41
42 Among the various computational modeling challenges of turbulent soot-
43
44 ing flames, small-scale soot-turbulence-chemistry interactions is one of the
45
46 most difficult. Soot particles are characterized by very small to null di↵usion
47
48 in the turbulent reacting flow and very slow chemical pathways in their for-
49
50 mation [1], leading to ligament-like soot particle-laden structures stretched
51
52 by the turbulent vortices [2, 3]. This results in significant soot intermittency,
53
54 both temporally and spatially, at unresolved scales [4]. Therefore, consider-
55
56
able modeling e↵orts are needed to provide closure for Large Eddy Simulation
57
58
59 2
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9 (LES).
10
11 A few attempts have been made to reproduce the high intermittency of
12
13 soot at unresolved LES subfilter scales, where the subfilter intermittency is
14
15 defined by Mueller and Pitsch [4] as the probability of not finding soot within
16
17 the filter volume. In that work [4], to capture this subfilter intermittency,
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19 a presumed subfilter PDF model for LES, which represents the statistical
20
21 distribution of scalar moments of the soot number density function and ac-
22
23 counts for turbulence-soot-chemistry interactions, was first introduced. In
24
25
the model, the subfilter PDF was divided into a non-sooting mode and a
26
sooting mode, each represented by delta functions, weighted by the subfilter
27
28 intermittency. In this first model, the probability of finding soot was uncor-
29
30 related with the thermochemical state since soot phenomena were explicitly
31
32 presumed to be slower than the gas-phase chemistry [4]. This soot subfilter
33
34 PDF model was applied in several turbulent combustion configurations [5–9].
35
36 The soot subfilter PDF model of Mueller and Pitsch [4] has been im-
37
38 proved in two ways. Berger et al. [10] reformulated the sooting mode to be
39
40 a lognormal distribution and, in an a priori analysis, found an improvement
41
42 of the prediction of the filtered coagulation source term. On the other hand,
43
44 Yang et al. [11] focused on formulating a correlation with the flame structure
45
46 (mixture fraction) and argued that soot phenomena occur at a wide range of
47
48
timescales. Specifically, soot oxidation can take place at similar timescales
49 as the combustion processes. Therefore, Yang et al. [11] developed a condi-
50
51 tional soot subfilter PDF confining soot to fuel-rich regions where soot surface
52
53 growth is faster than soot oxidation. This conditional PDF model was shown
54
55 to dramatically improve predictions of soot oxidation (by eliminating “spu-
56
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59 3
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9 rious” oxidation). However, due to its form, this conditional soot subfilter
10
11 PDF model implicitly assumes that oxidation is infinitely fast compared to
12
13 turbulent transport of soot.
14
15 The assumption of infinitely fast oxidation is not universally true. Soot
16
17 can leak into lean mixtures unoxidized in what are generally referred to
18
19 as smoking flames. The most common mechanism of smoking flames is the
20
21 suppression of oxidation rates due to a reduction in temperature by radiation
22
23 heat losses in flames with long residence times and large Damköhler numbers
24
25
(see, e.g., Ref. [12]). A second mechanism was proposed from computational
26
observations by Attili et al. [13, 14] in a three-dimensional DNS of an n-
27
28 heptane/nitrogen fueled non-premixed flame in the small Damköhler number
29
30 regime, when local extinction arises so soot oxidation is suppressed. A model
31
32 that assumes infinitely fast oxidation would not be able to capture these
33
34 finite-rate oxidation phenomena.
35
36 In this work, a new presumed subfilter PDF model to capture finite-rate
37
38 oxidation of soot particles in a turbulent reacting flow is proposed and is
39
40 implemented in an LES framework based on state-of-the-art combustion and
41
42 soot models [15, 16]. The new model accounts for the local relative motion of
43
44 di↵usionless soot particles relative to the mixture fraction iso-contour, given
45
46 by the mixture fraction displacement speed, which scales with the local mix-
47
48
ture fraction dissipation rate, and compares it against the local oxidation
49 rate, determining a new soot distribution with respect to the mixture frac-
50
51 tion. The finite-rate oxidation model is assessed a priori using the DNS data
52
53 from Attili et al. [14] at di↵erent Damköhler numbers and then evaluated a
54
55 posteriori in a turbulent nonpremixed jet flame [17].
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9 This paper is structured as follows. The fundamentals of LES model-
10
11 ing for turbulent combustion including soot evolution are introduced in Sec-
12
13 tion 2. Subfilter models to capture soot-turbulence-chemistry interactions
14
15 are presented in Section 3, including the considerations of the new presumed
16
17 soot subfilter PDF models as well as previous works. In Section 4, the new
18
19 soot subfilter PDF model is validated a priori using DNS data and compared
20
21 against previous models. Finally, an extensive a posteriori validation is made
22
23 in Section 5, by comparing computational results using the new and previous
24
25
models to experimental data in a laboratory-scale turbulent sooting flame.
26
27
28 2. LES modeling framework
29
30
31 The purpose of this section is to present the governing equations and
32
33 models involved in the LES framework for soot evolution in turbulent reacting
34
35 flows.
36
37
38
2.1. Soot model
39
40 A Number Density Function (NDF) statistically represents the soot parti-
41
42 cles classified by size, and the Population Balance Equation (PBE) describes
43
44
the evolution of the NDF in time, space, and internal (size) variables. In this
45
work, a bivariate NDF is considered, with internal variables soot particle
46
47 volume V and soot particle surface area S [18]. The PBE is computationally
48
49 expensive to solve, especially using multivariate NDFs. Instead, the method
50
51 of moments is used in which the evolution of the NDF is described by trans-
52
53 porting instead a few statistical moments Mx,y . For the bivariate NDF, the
54
55
56
57
58
59 5
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7
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9 soot statistical moment is defined as
10
11 1
X
12 Mx,y = V⌘x S⌘y N⌘ , (1)
13 ⌘=1
14
15
16
where N⌘ is the particle number density in the two-dimensional state space
17
element ⌘, corresponding to the particle “class” of volume V⌘ and surface
18
19 area S⌘ . The subscripts x and y indicate the order of the moment regarding
20
21 the soot size parameters V and S, respectively. The moments M0,0 , M1,0 , and
22
23 M0,1 have a physical meaning corresponding to the soot number density, the
24
25 soot volume fraction, and the total soot surface, respectively. The moment
26
27 transport equations require closure for the moment source terms Ṁx,y since
28
29 they are not directly evaluated using the moments Mx,y . The Hybrid Method
30
31 of Moments (HMOM) provide closures for these source terms describing dif-
32
33 ferent soot phenomena, such as nucleation, coagulation, condensation, sur-
34
35 face growth, oxidation, and oxidation-induced fragmentation. HMOM has
36
37 been extensively validated in numerous laminar flames [15, 18, 19]. HMOM
38
39
accounts for the bimodality of the NDF by transporting a supplementary
40 weighted delta function that mimics the number density of nascent soot par-
41
42 ticles N0 .
43
44 The soot moments Mx,y and the incipient particles N0 are denoted by the
45
46 soot scalar Mj and are governed by the transport equation:
47
48 @Mj @u⇤i Mj
49 + = Ṁj , (2)
50 @t @xi
51
52 where u⇤i stands for the total velocity of soot particles (flow and thermophore-
53
54 sis) and Ṁj are the soot scalar source terms. The latter is decomposed in
55
56 the di↵erent soot phenomena described above.
57
58
59 6
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9 2.2. Combustion model
10
11 In this work, combustion is modeled using the Radiation Flamelet/Progress
12
13 Variable (RFPV) model for non-adiabatic nonpremixed combustion [16, 20],
14
15 where the computations of the flow field and the detailed flame structure are
16
17 decoupled. A set of parameters–composed of mixture fraction Z, progress
18
19 variable C, and heat loss parameter H–describes the flame structure and
20
21 establishes a thermochemical database accessible by the LES solver.
22
23 The governing equations for Z, C, and H are written as follows:
24 ✓ ◆
25 @⇢Z @⇢ui Z @ @Z
26 + = ⇢DZ + ṁZ , (3)
27 @t @xi @xi @xi
28
29
30 ✓ ◆
31 @⇢C @⇢ui C @ @C
32 + = ⇢DC + ṁC , (4)
33
@t @xi @xi @xi
34
35
36 ✓ ◆
37 @⇢H @⇢ui H @ @H
38 + = ⇢DH + ⇢H
˙ + q̇RAD . (5)
@t @xi @xi @xi
39
40
41 The mixture fraction Z requires a source term ṁZ to account for the con-
42
43 sumption of PAH species to produce soot; the progress variable C has a source
44
45
term ṁC that is rescaled from for the change in the e↵ective stoichiometry
46 because of the large C/H ratio of PAH species removed from the gas mixture;
47
48 and the heat loss parameter H is zero-valued for adiabatic conditions [16].
49
50 q̇RAD indicates the radiative source term and considers the gas-phase opti-
51
52 cally thin gray model from Barlow et al. [21], which accounts for the species
53
54 CO2 , H2 O, CO, and CH4 , and the soot radiation model is from Hubbard and
55
56 Tien [22].
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59 7
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9 PAH chemistry has a much slower characteristic time scale compared to
10
11 the major combustion products. To incorporate this feature, special attention
12
13 is taken to the flow history dependence [23] so slow adjustment to fluctuating
14
15 scalar dissipation rates [24] that characterize PAH evolution, so an explicit
16
17 transport equation is written as [16]
18 ✓ ◆
19 @⇢YPAH @⇢ui YPAH @ @YPAH
+ = ⇢DPAH + ṁPAH , (6)
20 @t @xi @xi @xi
21
22 where ṁPAH is the summation of PAH species source terms. The PAH source
23
24 term is formulated following the work of Mueller and Pitsch [16]. For species
25
26 with slow chemistry (e.g., PAHs) confined in zones of small scalar dissipation
27
28 rates, a strain-sensitive transport approach (SSTA) is utilized [25]. Molecu-
29
30
lar Lewis numbers are considered for the species where molecular transport
31 dominates. However, fast chemistry species hold the unity Lewis number
32
33 assumption [24].
34
35
36 2.3. LES governing equations
37
38 The LES filtered scalar transport equations are obtained after a filtering
39
40 operation is applied to Eqs. 2-6 and gives the following system:
41 !
42 @⇢Ze @⇢e ui Ze @ ⇣ ⌘ @ @ e
Z
43 + = ui Ze ⇢ug
⇢e iZ +
eZ
⇢D + ṁZ , (7)
@t @xi @xi @xi @xi
44
45
46 !
47 @⇢Ce @⇢e e
ui C @ ⇣ e
⌘ @ e
eC @C
48 + = ⇢e
ui C ⇢ug
iC + ⇢D + ṁC , (8)
@t @xi @xi @xi @xi
49
50
51
52 @⇢He @⇢e e
ui H @ ⇣ e g
⌘
53
+ = ⇢e
ui H ⇢u i H
@t @xi @xi
54 ! (9)
55 @ @ e
H
+ eH
⇢D + ⇢H
˙ + q̇ RAD ,
56 @xi @xi
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59 8
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9
10
11 @⇢YePAH @⇢e ui YePAH @ ⇣ e ⌘
12 + = ui YPAH ⇢ug
⇢e Y
i PAH
13 @t @xi @xi
! (10)
14 e
15
@ e PAH @ YPAH + ṁPAH ,
+ ⇢D
16 @xi @xi
17
18
19
20 @M j @ uei ⇤ M j @
21 + = e⇤ M j
u u⇤i Mj + Ṁ j , (11)
@t @xi @xi i
22
23
24 e indicates the filtering and density-weighted filtering operations
where ' and '
25
26
applied to a variable ', respectively. In the right-hand side of every equa-
27 tion, the first term is the subfilter scalar flux and describes the unresolved
28
29 turbulent transport; the second term, except for the soot scalars because of
30
31 the negligible soot di↵usion assumption, is the filtered molecular di↵usion
32
33 flux; and the final terms are the filtered source terms. The unresolved terms
34
35 comprise the small-scale unresolved soot-turbulence-chemistry interactions,
36
37 and closure models are presented in the following section. The closure for
38
39 the filtered PAH source term developed by Mueller and Pitsch [16] is utilized
40
41 in this work.
42
43
44 3. Subfilter modeling for turbulence-chemistry-soot interactions
45
46
47 Small-scale unresolved soot-turbulence-chemistry interactions can be mod-
48
49 eled in LES by closing the filtered source terms Q̇ through a convolution
50
51 against a density-weighted joint subfilter PDF Pe(⇠k , Mj ), which depends on
52
53 the thermochemical variables ⇠k and soot scalars Mj :
54
55 x 1
56 Q̇(⇠k , Mj ) = ⇢ Q̇(⇠k , Mj )Pe(⇠k , Mj )d⇠k dMj , (12)
⇢
57
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59 9
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7
8
9 where the subfilter PDF Pe(⇠k , Mj ) needs to be modeled. By Bayes’ theorem,
10
11 the subfilter PDF can be written as
12
13
14 Pe(⇠k , Mj ) = Pe(⇠k )Pe(Mj | ⇠k ), (13)
15
16
17 where Pe(⇠k ) is modeled as a beta distribution for the mixture fraction Pe(Z) =
18
19
e j ), Zv (xj )) [20, 26], where Z(x
(Z, Z(x f2 (xj )
e j ) and Zv (xj ) = Z Ze2 (xj ) are
20
21 the local filtered and subfilter variance of the mixture fraction, respectively.
22 f2 [16], in addition
23 Another transport equation is therefore solved for filtered Z
24
25
to Eqs. 7–11, in order to compute the subfilter mixture fraction variance Zv ,
26
which is also included in the RFPV database, for the computation of such
27
28 presumed subfilter PDFs of Eqs. 12–13. The conditional soot subfilter PDF
29
30 Pe(Mj | ⇠k ) is discussed in the following subsection.
31
32
33 3.1. Previous models
34
35 Mueller and Pitsch [4] modeled a presumed subfilter PDF for soot-turbulence
36
37 interactions as a highly intermittent (at the subfilter level) bimodal PDF with
38
39 two states corresponding to sooting PeS and non-sooting PeN S modes, written
40
41 as
42
43
44 Pe(Mj | ⇠k ) = ! PeN S + (1 !)PeS , (14)
45
46
47 where ! is the soot subfilter intermittency and represents the probability of
48
49 not finding soot at the subfilter scale. Mueller and Pitsch [4] argued that
50
51 the characteristic time scales of soot were slower than the heat releasing
52
53 combustion chemistry so the subfilter PDF model could be considered as
54
55
independent of the thermochemical variables Pe(Mj | ⇠k ) = Pe(Mj ). Further-
56 more, since soot is highly intermittent, delta functions were considered to
57
58
59 10
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9 construct the bimodal distribution, where the non-sooting mode is
10
11
12 PeN S = (Mj ) (15)
13
14
15 and the sooting mode is
16
17
18 PeS = (Mj Mj⇤ ). (16)
19
20
21 This model is referred to as the marginal (Marg) model. The subfilter inter-
22
23 mittency depends on a second-order moment. For the marginal model, the
24
25 subfilter intermittency is written as [4]
26
2
27 Mj
28 !=1 . (17)
29 Mj2
30
31 The best quantity to model the subfilter intermittency is M0,0 (total number
32
33 density), and a transport equation must then be solved for the second-order
34
35 2
moment M0,0 [4]. Mj⇤ are chosen such that M j are obtained upon convolution
36
37 against Pe(⇠k , Mj ) as follows:
38
39 x
40 Mj = Mj P (Mj | ⇠k ) Pe (⇠k ) d⇠k dMj
41 Z
42 = (1 !)Mj ⇤
Pe (Z) dZ
43 (18)
44 2
45
M 0,0
= Mj⇤ .
46 2
M0,0
47
48 Therefore, Mj⇤ in terms of the filtered soot scalars is
49
50
51 Mj
52 Mj⇤ = (19)
1 !
53
54
55
To determine the filtered source terms, first note that the soot scalar
56 source terms for oxidation (ox) and surface growth (sg) can be written as
57
58
59 11
60
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6
7
8
9 the product of the oxidation or growth rate coefficients and a function of the
10
11 moments:
12
13
ox/sg
14 Ṁj = kox/sg (⇠k )f (Mj ). (20)
15
16
17 Then, the filtered source terms for oxidation and surface growth are obtained
18
19 from convolution against the joint subfilter PDF:
20
21 ox/sg x
22 Ṁ j = kox/sg (⇠k ) f (Mj ) P (Mj | ⇠k ) Pe (⇠k ) d⇠k dMj . (21)
23
24
25 Evaluating Eq. 21 with the Marg model gives
26 " 2 #
27 ox/sg M 0,0
28 Ṁ j =e
kox/sg f Mj⇤ , (22)
2
29 M0,0
30
31 where e
kox/sg is the density-weighted filtered rate coefficient.
32
33 Later, Yang et al. [11] attempted to model the conditional soot subfil-
34
35 ter PDF. The authors considered that soot is confined to subfilter mixtures
36
37 where growth rates exceed oxidation rates, and, at the same time, compet-
38
39 itive with gas-phase chemistry time scales but very fast compared to other
40
41 soot processes. Therefore, they considered a presumed subfilter PDF for the
42
43 sooting mode that depends on the mixture fraction Z as
44
45
46 PeS = Mj Mj⇤ (Z, st ) , (23)
47
48
49 where Mj⇤ (Z, st ) = Mj⇤⇤ H(Z, st ) and Mj⇤⇤ are chosen such that M j is re-
50
51 covered upon convolution against Pe(⇠k ). H(Z, st ) = H(Z Zsoot ( st )) is
52
53 the Heaviside function, and Zsoot is the mixture fraction value at which the
54
55
soot surface growth is equal to the rate of soot oxidation. This Zsoot varies
56 with the mixture fraction dissipation rate (reference at stoichiometric mixture
57
58
59 12
60
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2
3
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5
6
7
8
9 fraction) st . With the Heaviside function, this model actually implicitly as-
10
11 sumes that soot oxidation is infinitely fast. Hereafter, this model from Yang
12
13 et al. [11] will be referred to as the Infinitely Fast Oxidation (IFO) model.
14
15 The IFO model requires a modification of the subfilter intermittency in
16
17 Eq. 17 to recover the filtered soot scalars upon convolution:
18 2
19 1 M 0,0
20 !=1 R · , (24)
21 H(Z Zsoot )Pe(Z)dZ 2
M0,0
22
23 where Pe(Z) is the beta distribution as stated before. Then, analogously to
24
25 Eqs. 18-19, the expression for Mj⇤⇤ (Z) after some algebraic manipulation is
26
27 written as
28
29 Mj
Mj⇤⇤ = R . (25)
30 (1 !) H(Z Zsoot )Pe(Z)dZ
31
32 Yang et al. [11] showed that the filtered source terms for oxidation and
33
34 surface growth for the IFO model can be expressed as
35 " 2 #
36 ox/sg M 0,0 ⇤⇤
37 Ṁ j = ǩox/sg f Mj , (26)
2
38 M0,0
39
40 where ǩox/sg is the rate coefficient convoluted against the thermochemical
41
42 PDF weighted by the Heaviside function:
43 "R #
44 kox/sg (⇠k ) H (Z Zsoot ) Pe (⇠k ) d⇠k
45 ǩox/sg = R . (27)
46 H (Z Zsoot ) Pe (⇠k ) d⇠k
47
48 All quantities in Eqs. 22,26-27 are functions of Z and st (via Zsoot ) and
49
50 can be precomputed and stored in a precomputed database [11].
51
52
53
3.2. Soot subfilter PDF for finite-rate oxidation
54
55
While the assumption of infinitely fast oxidation is valid under some con-
56 ditions, the assumption is not valid under all conditions. The IFO model
57
58
59 13
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5
6
7
8
9 is inconsistent with situations when soot escapes to very lean mixtures un-
10
11 oxidized as in smoking flames. Soot could escape unoxidized either due to
12
13 a suppressed oxidation rate or due to extremely fast transport. Even if not
14
15 escaping unoxidized, soot may penetrate into leaner mixtures than Zsoot due
16
17 to finite-rate oxidation. The transport of soot in Z-space is quantified using
18
19 the mixture fraction displacement speed vZ , defined as the relative motion
20
21 between a di↵usionless particle and a mixture fraction iso-surface, and ex-
22
23 pressed as [27]
24
25 r · (⇢DrZ)
vZ = . (28)
26 ⇢|rZ|
27
28 The velocity associated with this speed follows the opposite direction of the
29
30 vector normal to the Z iso-surface. The D corresponds to the mixture frac-
31
32 tion di↵usivity with unity Lewis number.
33
34 To determine how far soot is transported in Z-space before being com-
35
36 pletely oxidized, the mixture fraction distance Z is introduced and written
37
38 as
39
40 vZ |rZ|
Z = . (29)
41 kox
42
43 Equation 29 measures the displacement of soot in Z-space in an interval of
44
45 time equal to the characteristic time scale of oxidation (given by 1/kox ) and
46
47 is evaluated at Z = Zsoot . A fast kox and slow vZ will narrow Z, so soot is
48
49 oxidized rapidly, leading eventually to IFO. Conversely, a slow kox and fast vZ
50
51 will widen Z, so soot oxidizes slowly and can penetrate further toward and
52
53 potentially into fuel-lean mixtures. Since vZ scales with the scalar dissipation
54
55
rate, turbulent flames with high st (or low local Damköhler number) could
56 feature soot leakage into fuel-lean regions of the flame, which theoretically
57
58
59 14
60
61
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 1
2
3
4
5
6
7
8
9 could not be captured using IFO. Likewise, turbulent flames with locally
10
11 suppressed oxidation (due either to heat losses or local extinction with high
12
13 st ) could also feature soot leakage into fuel-lean regions of the flame, which
14
15 also could not be captured using IFO.
16
17 The new presumed subfilter PDF for finite-rate oxidation of soot, here-
18
19 after referred as FRO, is related to a function depending also on Z and st ,
20
21 with the following sooting mode PeS :
22
23
24
PeS = Mj Mj? (Z, st ) , (30)
25
26 where Mj? (Z, st ) = Mj?? G(Z, st ) and Mj?? are chosen such that the convolu-
27
28 tion of Mj? (Z, st ) against the joint subfilter PDF gives M j . Unlike the IFO
29
30 model, the activation of the sooting mode is given with a smoother transition
31
32 that begins just before Zsoot , which is described by a function G(Z, st ) here
33
34 proposed as
35 ✓ ◆
36 1 1 Z (Zsoot + Z /2)
37 G(Z, st ) = + tanh . (31)
2 2 Z /2
38
39 Compared to the IFO model, the function G is continuous at Zsoot with a
40
41 non-zero value. Like Zsoot , the mixture fraction distance can be deter-
Z
42
43 mined solely from information in mixture fraction space (so computed from
44
45 the combustion model). This requires rewriting the displacement speed in
46
47 mixture fraction space, which is given by
48 
49 1 1 @(⇢D) @(⇢ )
50 vZ |rZ| = r · (⇢DrZ) = + , (32)
51
⇢ 4⇢ D @Z @Z
52
53 where the mixture fraction dissipation rate is analytically related to st
54
55
based on a presumed profile in mixture fraction space [28]. Only positive
56 values of vZ are considered in the model, and negative values (drifting toward
57
58
59 15
60
61
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2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23
24
25 Figure 1: Sooting mode P̃S of the soot subfilter PDF models (Marg, IFO, and FRO) along
26 with the rate coefficients of oxidation kox and surface growth ksg , for a n-heptane non-
27
1
28 premixed flame at st = 10 s and similar conditions to the DNS presented in Section 4.
29
30
31 rich mixtures) are clipped to zero (i.e., IFO). When the particles drift toward
32
33 rich mixtures, they would not be oxidized, so this clipping has no influence
34
35 on the ultimate results. Figure 1 shows an example of the sooting mode
36
37 distribution P̃S in mixture fraction space using Marg, IFO, and FRO soot
38
39 subfilter models in an n-heptane/air counterflow di↵usion flame at st =
40 1
41 10 s at similar conditions to the DNS presented in Section 4. The crossing
42
43
of the oxidation and surface growth rates coefficients determine the mixture
44
fraction crossing at Z = Zsoot and characterizes the activation of IFO and
45
46 FRO models, where the latter is clearly admitting soot presence at leaner
47
48 mixtures as indicated by the non-zero PDF value at mixture fractions less
49
50 than Zsoot .
51
52
53
54
55
56
57
58
59 16
60
61
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 1
2
3
4
5
6
7
8
9 The filtered soot scalars can be expressed as a function of Mj?? as
10
11 x
12 Mj = Mj P (Mj | ⇠k ) Pe (⇠k ) d⇠k dMj
13 Z
14
15
= (1 !)Mj ??
G (Z, st ) Pe (Z) dZ
(33)
16 2
17 M 0,0
18 = Mj?? ,
2
19 M0,0
20
21 and, analogous to the IFO case, Mj?? can be rewritten as a function of the sub-
22
23 filter intermittency !, the filtered soot scalars, and the integral of G(Z, st )
24
25 against the thermochemical PDF Pe (Z), which is similar to what is obtained
26
27 for IFO in Eq. 25:
28
29 Mj
30 Mj?? = R . (34)
(1 !) G(Z, e
st )P (Z)dZ
31
32
33 The subfilter intermittency with the FRO model is given by
34
2
35 1 M 0,0
36 !=1 R · , (35)
37 G(Z, e
st )P (Z)dZ
2
M0,0
38
39 where the integral in the denominator can be calculated a priori for di↵erent
40
41 st as for the combustion model.
42
43 To determine the filtered source terms, the soot scalar source terms for
44
45 oxidation (ox) and surface growth (sg) are written as in Eq. 20. Then, the
46
47 filtered source terms for oxidation and surface growth are also obtained from
48
49
50
51
52
53
54
55
56
57
58
59 17
60
61
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 1
2
3
4
5
6
7
8
9 convolution against the joint subfilter PDF:
10
11 ox/sg x
12 Ṁ j = kox/sg (⇠k ) f (Mj ) P (Mj | ⇠k ) Pe (⇠k ) d⇠k dMj
13 Z
14 ⇥ ⇤
= kox/sg (⇠k ) G (Z, st ) P
e (⇠k ) d⇠k
(1 !)f Mj??
15
16 "R #" 2 #
17 kox/sg (⇠k ) G (Z, st ) Pe (⇠k ) d⇠k M 0,0 (36)
18 = R f Mj??
e
G (Z, st ) P (⇠k ) d⇠k 2
M0,0
19
20 " 2 #
21
M 0,0
= k̂ox/sg f Mj?? ,
22 2
M0,0
23
24
25 which is very similar to what is obtained for the marginal and IFO models in
26
the previous subsection. Here, k̂ox/sg is the rate coefficient convoluted against
27
28 the thermochemical PDF weighted by the G-function of Eq. 31:
29
30 "R #
31 kox/sg (⇠k ) G (Z, st ) Pe (⇠k ) d⇠k
32 k̂ox/sg = R . (37)
33
G (Z, st ) Pe (⇠k ) d⇠k
34
35 All quantities in Eq. 37 are functions of Z and st , so k̂ox/sg can be pre-
36
37 computed and stored in the thermochemical database, as was done for the
38
39 marginal and IFO models [11] as stated in the previous subsection.
40
41
42 4. A priori validation against DNS data
43
44
45 In this Section, the new subfilter PDF model for finite-rate oxidation
46
47 (FRO) of soot is assessed using a three-dimensional DNS database of tur-
48
49 bulent nonpremixed temporally evolving planar jet flames at atmospheric
50
51 pressure and two Damköhler numbers, from Attili et al. [13, 14]. A pri-
52
53 ori analyses are performed for the validation of the new model, including
54
55 comparison to results from the previous Marg [4] and IFO [11] models.
56
57
58
59 18
60
61
62
63
64
65
 1
2
3
4
5
6
7
8
9 4.1. DNS configuration
10
11 The DNS configurations consist of a nitrogen diluted n-heptane central
12
13 stream (85% N2 by volume) at 400 K and a coflowing stream of air at 800 K.
14
15 The stoichiometric mixture fraction is Zst = 0.147. The initial velocity distri-
16
17 bution in the fuel slab comes from an instantaneous realization of a turbulent
18
19 channel flow at Re⌧ = 390. Three cases were computed in Refs. [13, 14] by
20
21 varying the Damköhler number and maintaining the jet Reynolds number
22
23 Re = 2Uc H/⌫ ⇡ 15000, where Uc is the central jet velocity and H is the
24
25 jet width. The initial thermochemical properties in all cases are the same.
26
27 The velocities and lengths are rescaled to vary the Damköhler number. To
28
29 evaluate the FRO model, only two cases are considered, corresponding to the
30
31
medium and low Damköhler numbers (DaM = 2DaL ).
32
The combustion kinetics of n-heptane consist of a reduced mechanism
33
34 with 47 species and 290 reactions, that cover PAHs formation up to naph-
35
36 thalene [1]. Soot phenomena are modeled as in the previous section.
37
38 In the DNS, a discretized domain with Nx ⇥ Ny ⇥ Nz = 1024 ⇥ 1024 ⇥
39
40 512 grid points was utilized. For additional information about the DNS
41
42 configuration, the reader is referred to Ref. [14]. The strategy to analyze the
43
44 DNS data is similar to Yang et al. [11], where a layer of Nx ⇥ Ny ⇥ ( /h + 1)
45
46 points is extracted from the full grid, centered at z0 /h = 256, where and h
47
48 are respectively the filter and DNS grid spacing. This spanwise slice is located
49
50 in the homogeneous mesh region where the element size is hM = 64.4 µm
51
52 and hL = 45.5 µm for the DaM and DaL cases, respectively. The DNS
53
54
data extracted for the analyses correspond to the same non-dimensional time
55 ⌧ = t/tjet in both cases [14], where tjet = H/(2Ux ) is the jet time scale,
56
57
58
59 19
60
61
62
63
64
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 1
2
3
4
5
6
7
8
9 corresponding to t = 2.5 ms and t = 5 ms for DaL and DaM , respectively.
10
11 LES model validation requires the application of a low-pass filter to the se-
12
13 lected DNS snapshots. A three-dimensional, clipped and renormalized Gaus-
14
15 sian filter kernel is utilized, following the work of Yang et al. [11]:
16 " #
17 6 d 2
+ d 2
+ d 2
x y z
18 F (dx , dy , dz ) = 3 exp 2
, (38)
19
20
21 where is the filter width, di are distances from a point of study in the
22
23 Cartesian directions, and  is a renormalization constant that guarantees
24
25 the filter satisfies the following relationship:
26
27 /2h /2h /2h
28 X X X
29 F (ih, jh, kh) = 1, (39)
30 i= /2h j= /2h k= /2h
31
32 where the filter kernel is active over a cube of ( /h + 1)3 grid points. This
33
34 process is done by applying the Gaussian filter to groups of ( /h + 1)3 grid
35
36 points.
37
38
39 4.2. Results: Oxidation and surface growth
40 ox sg
41 The oxidation and surface growth filtered source terms, Ṁ 1,0 and Ṁ 1,0 ,
42
43 are evaluated using the new FRO subfilter model, using Eq. 36, and compared
44
45 against the Marg and IFO models. Building upon the strategy in the work
46
47 of Yang et al. [11], rather than relying on a combustion model to obtain
48
49 the oxidation and surface growth rate coefficients, these are obtained from
50
51 the DNS database. In this work, these rate coefficients are obtained with a
52
53 conditional average with respect to Z and st :
54
55
56 kox/sg (Z, st ) ⇡ h kox/sg (xj ) | Z(xj ), st (xj )i, (40)
57
58
59 20
60
61
62
63
64
65
 1
2
3
4
5
6
7
8
9 where h · | ⇠k i symbolizes the density-weighted conditional averaging opera-
10
11 tor. It should be noted that Yang et al. [11] considered only single conditional
12
13 averaging on Z. For the largest dissipation rates, Zsoot is undefined (i.e., sur-
14
15 face growth is never faster than oxidation), and, for these conditions, Zsoot
16
max
17 then defaults to Zsg , that is, the mixture fraction corresponding to the
18
19 maximum of the surface growth rate coefficient.
20
21 Soot oxidation and surface growth source terms depend on the total sur-
22
23 face area moment M0,1 , which is included in the computations. Moreover,
24
25
Yang et al. [11] showed that the subfilter -PDF of mixture fraction Pe(Z)
26
is sufficiently accurate to perform the analyses.
27
28 The filtered source terms for oxidation and surface growth using the Marg
29
30 model [4] are written as
31
32 Z 1
ox/sg
33 Ṁ 1,0 (xj ) = kox/sg (Z, e
st )P (Z)dZ · M 0,1 (xj ) . (41)
34 0
35
36 From the equation above, the filtered source terms using the IFO model
37
38 are
39
R1
40 ox/sg
0
kox/sg (Z, st )H(Z, st )Pe(Z)dZ
41 Ṁ 1,0 (xj ) = R1 · M 0,1 (xj ), (42)
42 H(Z, st ) e(Z)dZ
P
0
43
44 where the convolution is “weighted” by the Heaviside function. Then, using
45
46 the new FRO model the filtered source terms are calculated as:
47
48
R1
ox/sg kox/sg (Z, st )G(Z, st )Pe(Z)dZ
49 Ṁ 1,0 (xj ) = 0 R1 · M 0,1 (xj ), (43)
50 G(Z, st ) e(Z)dZ
P
0
51
52 where the “weighting” is now carried out by the function G from Eq. 31.
53
54 In order to make a fair comparison against the DNS data, the filtered
55
56 source terms of oxidation and surface growth are computed without using
57
58
59 21
60
61
62
63
64
65
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2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23 Figure 2: Comparison between the filtered DNS and the soot subfilter PDF models for
24 the filtered oxidation source term. The standard deviation is indicated for each model.
25
26
27
28 any subfilter PDF but with the conditionally averaged rate coefficients:
29
ox/sg
30
31
Ṁ 1,0 (xj ) = kox/sg (Z(xj ), st (xj )) · M0,1 (xj ), (44)
32
33
which is from now on referred as the filtered “DNS” case and kox/sg is the
34
35 one from the model (Eq. 40).
36 ox
37 Figure 2 shows parity plots of the filtered oxidation source terms Ṁ 1,0
38
39 at medium (left) and low (right) Damköhler numbers for the soot subfilter
40
41 PDF models compared to the filtered DNS. The normalized filter width is
42
43 /h = 32. Sample standard deviations are calculated and indicated in
44
45 the plots. Marg is visibly overestimating the oxidation compared to the
46
47 other models due to spurious oxidation [11], and the error is about 30
48
49 times greater than FRO (see zoomed out subfigure). Similar behavior was
50
51 encountered in Ref. [11] compared to the IFO model. IFO and FRO seems
52
53 to have a similar accuracy in the scatterplot, but, comparing the values,
54
55
FRO is more than two times as accurate. Overall, the FRO model tends
56 to reduce the slight overprediction of the magnitude of the oxidation source
57
58
59 22
60
61
62
63
64
65
 1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23 Figure 3: Comparison between the filtered DNS and the soot subfilter PDF models for the
24 filtered surface growth source term. The standard deviation is indicated for each model.
25
26
27
28 term compared to the IFO model.
29
30
Likewise, Fig. 3 shows parity plots of the filtered surface growth source
sg
31 terms Ṁ 1,0 at medium (left) and low (right) Damköhler numbers for the soot
32
33 subfilter PDF models compared to the filtered DNS. FRO is more accurate
34
35 than IFO, with a of about three in DaM and four in DaL times smaller. It
36
37 is interesting to note that the accuracy of the IFO model is actually worse
38
39 than the Marg model, which contradicts the previous work of Yang et al. [11].
40
41 This di↵erence is due to the double conditioning of the DNS data. Clearly,
42
43 the Heaviside function in the IFO model can degrade the accuracy of the
44
45 filtered surface growth source term. The FRO model, unlike the IFO model,
46
47 improves prediction of oxidation compared to the Marg model without de-
48
49 grading predictions of surface growth. Indeed, as shown in Fig. 1, there is
50
51 significant impact from an inclusion (respectively exclusion) of a portion of
52
53
surface growth e↵ects for mixtures with Z < Zsoot (respectively Z > Zsoot )
54 in the convolution operation of Eq. 37.
55
56
57
58
59 23
60
61
62
63
64
65
 1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23
24 Figure 4: Influence of the relative filter width at medium (solid lines) and low (dashed
25 lines) Damköhler number. Standard deviation of oxidation (left) and surface growth
26
27 (right) source terms of the di↵erent soot subfilter PDF models against the DNS filtered
28
data are compared.
29
30
31
32 4.3. Results: Influence of the filter width
33
34 The performance of the soot subfilter PDF models with varying the filter
35
36 width for both DaM and DaL cases are shown in Fig. 4 along with the evo-
37
38 lution of the error with the normalized filter width /h ranging from 2 to
39
40 128 for the oxidation (left) and surface growth (right) filtered source terms.
41
42 In the medium Damköhler number case (continuous lines), predicting the
43 ox
44
filtered oxidation source term Ṁ 1,0 using Marg maintains a large error of
45
up to two orders of magnitude compared to FRO. In general, FRO is much
46
47 better than IFO and Marg as discussed in the previous subsection. For small
48
49 relative filter widths ( /h < 8), Marg decreases the discrepancies until it has
50
51 similar performance to IFO and FRO. In other words, the subfilter model
52
53 is paramount except for near-DNS resolution, where the accuracy becomes
54
55 comparable.
56
57
58
59 24
60
61
62
63
64
65
 1
2
3
4
5
6
7
8
9 For the low Damköhler number case (dashed lines in Fig. 4), the per-
10
11 formances of the soot subfilter models on the oxidation source terms evolve
12
13 with a similar fashion as in the medium Damköhler number case but with
14
15 values lowered by a factor of 3 in average. Also, close to DNS resolution,
16
17 IFO and Marg have the same accuracy and FRO double the performance.
18
19 Regarding the surface growth filtered source term in Fig. 4 (right), the sam-
20
21 ple standard deviation evolution follows a similar trend as in the medium
22
23 Da case. Moreover, similar to the oxidation case, the accuracy in all models
24
25
is improved by a factor of 3 on average with the FRO model.
26
27
28
4.4. Analysis: Soot leakage at low Damköhler number
29
30 One of the motivations for developing the new subfilter model for finite-
31
32
rate oxidation (FRO) is the ability to predict the existence of soot at leaner
33
mixtures, which is theoretically disallowed in the IFO model. Attili et al. [14]
34
35 found in their DNS data that soot leaks to fuel-lean mixtures in the low
36
37 Damköhler number DaL case at t = 3.75 ms, which was attributed to local
38
39 weakening and flame quenching (so suppression of oxidation). In this sub-
40
41 section, an analysis is conducted to demonstrate the capability of the new
42
43 FRO model in capturing soot leakage. The dataset for this analysis consists
44
45 of a single plane from the DNS database, and only the FRO and IFO models
46
47 are considered.
48
49 Figure 5 (left) shows a scatter plot of soot volume fraction fv against the
50
51 mixture fraction Z in black squares. The red circles indicate the points where
52
53 G(Z, st ) > 0 using the FRO model and relative filter size /h = 4. The blue
54
55
triangles indicate the points where H(Z, st ) > 0 using the IFO model. The
56 limits of Zsoot ( min max
st ) are also indicated, Zsoot = 0.18 and Zsoot = 0.3 [11]. The
57
58
59 25
60
61
62
63
64
65
 1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23 Figure 5: Left: Scatter of the soot volume fraction in the mixture fraction space in the DaL
24
25 case. Filtered data ( /h = 4) using the FRO (red circles) and IFO (blue triangles) soot
26
27 subfilter PDF models are also included. Vertical lines indicate the stoichiometric mixture
28 fraction Zst = 0.147 and the limits of Zsoot ( st ):
min
Zsoot max
= 0.18 and Zsoot = 0.3. The
29
30 horizontal line indicates the minimum soot volume fraction considered in the analyses,
31 which is consistent to Attili et al. [14]. Right: Sooting mode distributions PeS in the
32
33 mixture fraction space for two points x1 (cyan star) and x2 (yellow star) extracted from
34
the filtered data, using the IFO and FRO models, in the left subfigure.
35
36
37 min
38 FRO model can predict soot phenomena for Z < Zsoot , which correspond to
39 max
40 about 9.3% of the events in Z < Zsoot . FRO can capture soot leakage across
41
42 the flame front and even into fuel-lean regions (Z  Zst = 0.147), which
43 max
44
represents the 5% of the events in Z < Zsoot . Only a few points with volume
45 fractions greater than 0.1 ppb occur where G = 0 and could not be captured
46
47 by the FRO model, and these exclusively occur where the volume fraction is
48
49 less than 0.3 ppb and for the leanest mixtures (i.e., very likely representing
50
51 soot that is just about finally burned out).
52
53 To characterize the sooting mode distributions in the lean and rich re-
54
55 gions, two data points with the same soot volume fraction fv = 0.36 ppb
56
57
58
59 26
60
61
62
63
64
65
 1
2
3
4
5
6
7
8
9 are extracted and labeled as x1 (cyan star) and x2 (yellow star), shown in
10
11 Fig. 5 (left), where ⇠(x1 ) = {Z = 0.125, st = 500 s 1 } and ⇠(x2 ) = {Z =
12
13 0.275, st = 100 s 1 } . The plot of Fig. 5 (right) shows the sooting mode
14
15 distributions H(Z, st ) (IFO) and G(Z, st ) (FRO). At x1 , the FRO model
16
17 shows a wide transition in the sooting mode and correctly allows for some
18
19 soot at this very lean mixture. Conversely, using the IFO, the sharp transi-
20
21 tion at Zsoot does not capture the leakage e↵ects to lean mixture fractions. At
22
23 x2 , the FRO model exhibits a much narrower width in mixture fraction space
24
25
and is almost the same as the IFO model since the soot at this rich mixture
26
fraction will not penetrate to leaner mixtures. Therefore, as demonstrated,
27
28 the FRO model, unlike the IFO model, is capable of correctly predicting the
29
30 leakage of soot to leaner mixture fractions, consistent with the DNS data of
31
32 Attili et al. [14].
33
34 To assess the potential of the new soot subfilter model in the soot leakage
35 ox
36 region, the filtered soot oxidation source terms Ṁ 1,0 are compared between
37
38 the FRO and IFO models. The analysis is made in the fuel-lean part of the
39
40 soot leakage region where Z < 0.1 and soot volume fraction fv 0.1 ppb,
41
42 in order to be at the same range as in Ref. [14], and restricted to points
43
44 where the thermochemical PDF (beta distribution) is greater than 1% over
45
46 this mixture fraction range. Parity plots are shown in Fig. 6, using di↵erent
47
48
relative filter widths /h = 2, 4, 8, and 16. The discrepancies of the models
49 against the DNS are quantified using the standard deviation as in previous
50
51 subsections and are indicated in the upper-left corner of each subfigure. The
52
53 prediction of the oxidation source terms using the FRO model agrees very
54
55 well with the filtered DNS data. As the size of the relative filter width
56
57
58
59 27
60
61
62
63
64
65
 1
2
3
4
5
6
7
8
9 increases, the FRO model performance decreases slightly but is still superior
10
11 to the IFO. At /h = 16, the FRO model declines in performance and later,
12
13 at /h = 32 and on, it degenerates into a similar shape and error value as
14
15 IFO (not shown). Additionally, it should be noted that a few points with
16
17 the FRO model incorrectly predict zero source term, which occurs due to an
18
19 underprediction of the width of the FRO model in mixture fraction space.
20
21 The soot particles are driven to the fuel-lean regions by transport e↵ects
22
23 induced by the locally fast strain rates. As a final note, since the Heaviside
24
25
function of IFO is zero in this fuel-lean region so no soot present, the filtered
26
oxidation source includes contributions only from richer mixtures where the
27
28 beta distribution of mixture fraction is non-zero.
29
30
31
32 5. A posteriori validation: LES of the Sandia flame
33
34 In this section, additional a posteriori LES evaluation of the soot subfilter
35
36 PDF models is conducted. The flame configuration selected is the Sandia
37
38 turbulent nonpremixed jet flame, introduced by Zhang et al. [17]. LES
39
40 results obtained with the three subfilter PDF models are compared with
41
42 experimental measurements.
43
44
45 5.1. Experimental setup
46
47 The Sandia flame from Ref. [17] consists of a turbulent nonpremixed
48
49 piloted jet flame at atmospheric pressure. Pure ethylene is injected at the
50
51 central jet with Re = 20, 000, where the bulk velocity is 54.7 m/s and the
52
53 jet inner diameter is D = 3.2 mm. The pilot flame, with outer diameter of
54
55
19.1 mm, is obtained from an ethylene-air premixture at = 0.9, in order to
56 acquire a thermal power equivalent to 2% of the main jet. A surrounding air
57
58
59 28
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2
3
4
5
6
7
8
9 coflow is injected at 0.6 m/s to isolate the flame from external perturbations.
10
11 More characteristics about the burner can be found in Zhang et al. [17]. The
12
13 experimental database used for the comparisons in this work includes mean
14
15 and RMS temperature profiles [29], mean and RMS soot volume fraction
16
17 profiles [30, 31], resolved soot intermittency and soot temperature profiles
18
19 [30], and chemical species profiles such as OH [17, 30].
20
21
22 5.2. Computational framework
23
24 Computational simulations are carried out in NGA, a finite di↵erence
25
26 code for grid-filtered LES of low-Mach number turbulent reacting flows [32,
27
28 33]. The computational domain of the Sandia burner consists of a struc-
29
30 tured cylindrical mesh of 192 ⇥ 96 ⇥ 32 points in the streamwise, radial, and
31
32
circumferential directions, respectively. The dimensions of the domain are
33
300D ⇥ 70D in the streamwise and radial direction, respectively. The grid
34
35 is taken from Yang et al. [11], which stretches the cells in both radial and
36
37 streamwise directions. The central jet unsteady velocity inflow profile was
38
39 generated using a simulation of flow through a periodic pipe.
40
41 The thermochemical database consists of solutions to the nonpremixed
42
43 flamelet equations with radiative heat losses (RFPV) computed with FlameMas-
44
45 ter [34]. As discussed in subsection 2.2, the RFPV database is parameterized
46
47 e Zv , C,
by Z, e and H
e with a resolution of 100 divisions per parameter. The
48
49 combustion chemistry (158 species and 1804 reactions.) used to generate
50
51 the RFPV database is from Blanquart et al. [35], which covers gas-phase
52
53 kinetics for ethylene up to 4-rings PAHs (C18 H10 ), and Narayanaswamy et
54
55
al. [36], which extends the previous kinetics to account for high-temperature
56 oxidation of substituted aromatic species.
57
58
59 29
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3
4
5
6
7
8
9 5.3. Results: Temperature and soot volume fraction
10
11 Figure 7 shows the radial profiles of mean (top) and RMS (bottom) tem-
12
13 perature at two di↵erent locations downstream the burner exit: x/D = 134
14
15 (left) and x/D = 175 (right). A comparison is made between computational
16
17 results using the Marg, IFO, and FRO soot subfilter models and experimental
18
19 measurements [29].
20
21 At both positions, the mean temperature predicted by Marg is higher
22
23 than the other models and the experimental measurements, which is accen-
24
25 tuated at x/D = 175 with about 300 K of disagreement at the centerline.
26
27 This is because the Marg model underpredicts soot, as shown below, so soot
28
29 radiation [11]. However, using IFO and FRO, the computational results
30
31
compare favorably with the experimental measurements, albeit with a slight
32
underprediction.
33
34 The RMS temperature plots in Fig. 7 (bottom) show more significant
35
36 di↵erences between computational results and experimental measurements
37
38 at both axial positions. The computational results only include the resolved
39
40 contribution to the RMS, and, on this coarse grid, the unresolved subfilter
41
42 temperature variance is not an insignificant contribution. However, the re-
43
44 sults indicate good agreement with the experimental measurements nonethe-
45
46 less.
47
48 To better see the influence of the soot subfilter model on the temperature
49
50 evolution, the temperature profile along the centerline is shown in Fig. 8.
51
52 Results show that the Marg model overpredicts the temperature for x/D >
53
54
100 with a maximum di↵erence of about 700 K at x/D ⇡ 240. The lack
55 of soot using the Marg model (see Fig. 10) makes it unable to predict the
56
57
58
59 30
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7
8
9 correct amount of radiative losses in the flame. However, IFO and FRO show
10
11 almost identical temperature profiles and agree well with the experimental
12
13 data, which suggest the amount of soot produced in both models is about
14
15 the same.
16
17 Mean (top) and normalized RMS (bottom) soot volume fraction profiles
18
19 are plotted in Fig. 9 at di↵erent axial positions: x/D = 70.3, x/D = 132.8,
20
21 and x/D = 195.3. Computational results using the three soot subfilter PDF
22
23 models and experimental measurements [31] are compared.
24
25
Mean profiles show that FRO model captures better the soot volume
26
fraction fv in the upstream portion of the sooting region of the flame (x/D =
27
28 70.3). Then, at about the middle of the sooting region (x/D = 132.8),
29
30 the IFO and FRO models overpredict experimental measurements at the
31
32 centerline by about a factor of three. Further downstream at x/D = 195.3,
33
34 soot is overpredicted by a factor of two using the IFO and FRO models. In
35
36 all cases the Marg model overpredicts oxidation, so the mean fv is almost
37
38 zero in the entire flame, as discussed by Yang et al. [11]. A more detailed
39
40 analysis at x/D = 70.3, in Fig. 9 (left), where FRO indicates a significant
41
42 improvement over IFO, will be presented in a later section.
43
44 The soot volume fraction fluctuations are scaled by the mean since the
45
46 mean values shown above di↵er with the experiments. The normalized RMS
47
48
profiles of soot volume fraction, obtained by dividing the RMS values by the
49 mean values, are plotted in Fig. 9 (bottom) and show that soot fluctuations
50
51 levels are better captured using the FRO and IFO models (except for the
52
53 IFO model in the upstream region). In general, these two models capture
54
55 very well the fluctuations in the sooting region (r/D  10) and beyond that,
56
57
58
59 31
60
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2
3
4
5
6
7
8
9 since soot predicted is negligible, the relative fluctuations grow abruptly.
10
11 Since the Marg model incorrectly predicts the mean soot volume fraction,
12
13 the fluctuations are quite inaccurate, being extremely underpredicted in the
14
15 far upstream region to overpredicted in the downstream region.
16
17 The mean soot volume fraction profile along the centerline is plotted in
18
19 Fig. 10 and compares the computational results obtained with the three soot
20
21 subfilter models and experimental measurements [17]. The Marg model un-
22
23 derpredicts the maximum soot volume fraction value by a factor of more than
24
25
20 compared to experimental measurements. The IFO and FRO model pre-
26
dict the same maximum value of soot volume fraction and the peak position
27
28 slightly shifted downstream the burner by a distance of about 15D com-
29
30 pared to the experimental measurements. However, the new FRO subfilter
31
32 model can capture better the inception zone starting at x/D = 40 through
33
34 x/D = 80, where relatively high strain rate has been observed in experiments
35
36 [30]. This is consistent with the a priori analysis of Section 4 at the low
37
38 Damköhler number case, in which better performance of the FRO model is
39
40 obtained. Moving downstream, st decreases, and the regime becomes more
41
42 similar to the medium Damköhler number case, where soot surface growth is
43
44 less accurate and therefore overpredicted with the IFO model. Since the IFO
45
46 model overpredicts the surface growth more than FRO, the mean soot vol-
47
48
ume fraction with IFO increases much more rapidly even though reaching the
49 same maximum value (due to a comparable overprediction of both surface
50
51 growth and oxidation). Further downstream, IFO overestimates oxidation
52
53 compared to FRO, so fv decreases more rapidly (x/D = 200) and FRO pre-
54
55 dicts soot for a longer extent consistent with the experimental measurements.
56
57
58
59 32
60
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2
3
4
5
6
7
8
9 Overall, since the IFO model overpredicts both surface growth and oxidation,
10
11 the increase and decrease of soot is faster than the FRO model (and the ex-
12
13 perimental measurements), and soot is confined to a streamwise region that
14
15 is more compact than the FRO model (and the experimental measurements)
16
17 even though reaching the same maximum soot volume fraction.
18
19
20 5.4. Results: Soot intermittency and soot temperature
21
22 The resolved soot intermittency in the Sandia flame was studied exper-
23
24 imentally by Shaddix et al. [30] and indicates the probability of not en-
25
26 countering soot in space and time contingent on a threshold value of soot
27
28 volume fraction experimentally established. This value was set to fv = 0.03
29
30 ppm [30]. A probability of one indicates that no soot was detected over the
31
32
experimental threshold. To further validate the soot subfilter models and
33
understand the discrepancies in the previous section, computational results
34
35 using IFO and FRO soot subfilter models are compared against experimental
36
37 measurements from Ref. [30].
38
39 Figure 11 shows the resolved intermittency profile along the centerline.
40
41 The computational results indicate a correspondence to the mean soot volume
42
43 fraction profile in Fig. 10, where the FRO model is in better agreement
44
45 than IFO to experimental results at the beginning and at the end of the
46
47 sooting region. Both models overestimate the soot presence in the growth
48
49 region, but this is not unexpected with the overprediction of the mean soot
50
51 volume fraction. Briefly, the LES results predict more and consistent soot
52
53 so are overpredicting the mean soot volume fraction but underpredicting the
54
55
intermittency and normalized RMS near the maximum of the mean soot
56 volume fraction compared to the experimental measurements. The source
57
58
59 33
60
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2
3
4
5
6
7
8
9 of this more consistent and less intermittent nature of soot predicted by the
10
11 LES model requires further investigation.
12
13 Experimental measurements of the soot temperature are also available
14
15 [17]. This is determined by averaging the temperature where soot is present
16
17 (i.e., when the resolved intermittency is zero) in the turbulent flame and is
18
19 linked to the location of soot in the mixture fraction space. Figure 12 il-
20
21 lustrates the centerline profiles of the soot temperature Tsoot using IFO and
22
23 FRO subfilter models and the experimental data. Tsoot is well predicted by
24
25
both models between x/D = 75 and x/D = 200. In the upstream and down-
26
stream portions of the sooting region, the soot temperature is underpredicted
27
28 by FRO (no soot present in IFO model). The explanation for this discrep-
29
30 ancy could be attributed to two possible e↵ects. In the upstream region, this
31
32 could indicate that soot forms at mixture fractions richer than the exper-
33
34 imental measurements, and, in the downstream region, this could indicate
35
36 excessive soot radiation. However, there are no experimental measurements
37
38 to confirm these possibilities.
39
40
41 5.5. Results: Soot source terms
42
43 The variation of soot volume fraction predictions obtained in Fig. 10 could
44
45 be attributed to the e↵ects of the soot subfilter PDF models on the mixing
46
47 and flow field, or on the soot source terms [11]. Therefore, both causes will
48
49 be examined in the Sandia flame.
50
51 Figure 13 shows the mean mixture fraction along the centerline using
52
53 the three soot subfilter models. All of the subfilter models predict similar
54
55
values of Z, so all models have no e↵ect on the mixing and flow field. Similar
56 conclusions were obtained for a di↵erent flame by Yang et al. [11]. Therefore,
57
58
59 34
60
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2
3
4
5
6
7
8
9 the di↵erences between results obtained with di↵erent soot subfilter PDF
10
11 models come from the impact of the soot subfilter PDF models on the soot
12
13 source terms.
14
15 In the a priori analysis, the soot subfilter models were shown to funda-
16
17 mentally exert influence on the oxidation and surface growth source terms.
18
19 To analyze these source terms from the LES results, the source terms are
20
21 normalized because they depend on the predicted amount soot. As observed
22
23 in Figs. 10 and 11, the new FRO model is superior to the IFO model at
24
25
the beginning and at the end of the sooting region, and the analysis will be
26
focused on those regions. Figure 14 show the conditional normalized source
27
28 terms of oxidation (top) and surface growth (bottom) in mixture fraction at
29
30 two axial positions x/D = 100 and x/D = 205. The interval of Z is selected
31
32 such that the conditional soot volume fraction is greater than zero.
33
34 The normalized oxidation source term using the Marg model is greater
35
36 than the other two models in both locations, with di↵erences up to two
37
38 orders of magnitude. These results agrees to what it was observed in the a
39
40 priori analysis in Section 4. The gap between the IFO and FRO models is
41
42 smaller. At x/D = 100, the maximum di↵erence takes place at Z = 0.11
43
44 where IFO predicts a source term with double the value obtained using FRO.
45
46 At x/D = 205 this di↵erence is reduced, with a 40% di↵erence near the
47
48
stoichiometric value of mixture fraction (Zst = 0.0635).
49 The normalized surface growth source terms in Fig. 14 (bottom) exhibits
50
51 a di↵erent trend, where in general they are at the same order of magnitude.
52
53 Similar to the oxidation case, the Marg model overestimates surface growth
54
55 at both axial positions compared to FRO, with maximum di↵erences of a
56
57
58
59 35
60
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2
3
4
5
6
7
8
9 factor of about three at x/D = 100 and up to eight at x/D = 205. However,
10
11 since oxidation is extremely overpredicted, soot cannot grow using the Marg
12
13 model. The di↵erence between IFO and FRO are in the same proportion
14
15 as in the oxidation case. At x/D = 100, the ratio between IFO and FRO
16
17 predictions at Z = 0.11 is about 1.75, and at x/D = 205 the ratio near the
18
19 stoichiometric mixture is about two.
20
21 Nonetheless, these results verify the discussion at the end of subsec-
22
23 tion 5.3. At x/D = 100, the more dominant surface growth term is larger
24
25
for IFO compared to FRO, which results in sharper growth around this loca-
26
tion (see Fig. 10). Conversely, at x/D = 205, the dominant oxidation term
27
28 is larger for IFO than FRO, which results in a more rapid decrease of soot
29
30 (see Figs. 10 and 11). As shown in Fig. 5, compared to the experimental
31
32 measurements, the qualitative behavior of the FRO model is correct.
33
34
35 5.6. Further analysis: Soot leakage in the Sandia flame
36
37 As discussed before, at high or low local Damköhler numbers soot
st
38
39 might overcome oxidation and escape to fuel-lean regions. In the Sandia
40
41 flame, Shaddix et al. [30] experimentally observed soot leakage by superim-
42
43 posing OH PLIF imaging with LII soot observations, at a distance relatively
44
45 close to the burner exit (x/D ⇡ 70) where the flow still exhibits high strain
46
47 rate (high st ) but soot starts to grow. The measurements indicated some-
48
49 times an overlap of soot from the LII image with (weak) OH from the PLIF
50
51 image. In order to further validate the new soot subfilter model and con-
52
53 firm what discussed in subsection 4.4, a further comparison of computational
54
55
results of soot and OH using the IFO and FRO soot subfilter PDF models
56 against experimental measurements is conducted.
57
58
59 36
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2
3
4
5
6
7
8
9 Rather than qualitative comparisons of two images, the presence of soot
10
11 leakage in the computational results is assessed through conditional statis-
12
13 tics. Figure 15 (left) illustrates the conditional soot volume fraction hfv | Zi
14
15 at the axial position x/D = 70.3 in mixture fraction and shows that soot
16
17 leakage is indeed predicted by the new FRO model (vertical line indicates
18
19 the stoichiometric mixture Zst ), while the conditional volume fraction pre-
20
21 dicted by the IFO model is negligibly small for fuel-lean mixtures (i.e., no
22
23 leakage). The conditional OH mass fraction hYOH | Zi is also included and
24
25
confirms that soot leakage is occurring into regions where OH is (at least
26
sometimes) present.
27
28 Figure 15 (right) shows the radial profiles of soot volume fraction (ex-
29
30 tracted from Fig. 9) and normalized OH mass fraction at x/D = 70.3. For
31
32 the latter, the normalized OH presence is obtained computationally by divid-
33
34 max
ing the mean OH mass fraction profile by its maximum value YOH /YOH and
35
36 experimentally by dividing the OH PLIF signal [17, 30] by its maximum value
37
38 [OH · PLIF]/[OH · PLIF]max . The vertical line indicates the spatial position
39
40 of the mean stoichiometric mixture fraction. With the FRO model, both
41
42 profiles are quantitatively consistent with the experimental measurements
43
44 (albeit soot slightly overpredicted).
45
46 These results validate the capability of the FRO model to capture soot
47
48
leakage into fuel-lean regions. However, further studies are needed in tur-
49 bulent smoking flames to extensively validate the new soot subfilter model,
50
51 which is left for future work.
52
53
54
55
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5
6
7
8
9 6. Conclusions
10
11
12 In this work, a new presumed filter PDF model is proposed to capture
13
14 finite-rate oxidation (FRO) of soot particles in turbulent reacting flows. This
15
16 new model corrects the inconsistencies of previous models. The model not
17
18 only eliminates spurious oxidation but also allow for the capturing of soot
19
20 leakage into fuel-lean mixtures either when the oxidation rate is slow or when
21
22
the turbulent transport is fast, for instance, in turbulent smoking flames.
23 A priori analyses and validation of the FRO model have been conducted
24
25 using DNS data of turbulent nonpremixed flames with medium (DaM ) and
26
27 low (DaL ) Damköhler numbers. Results indicate a significant improvement in
28
29 the prediction of oxidation source term compared to previous models, which
30
31 achieve an accuracy increase of two (respectively three) times to an order
32
33 of magnitude in the DaM (respectively DaL ) case. Overall, results indicate
34
35 that the new FRO model improves oxidation predictions without degrading
36
37 the predictions of surface growth as opposed to previous models. Finally, the
38
39 potential to capture soot leakage using the FRO model was assessed, showing
40
41 very good agreement with the filtered DNS data.
42
43
A substantial a posteriori validation was carried out in a turbulent non-
44
premixed sooting jet flame. The new soot subfilter PDF model was imple-
45
46 mented within an LES framework and results where compared to previous
47
48 models, the Marginal (Marg) and Infinitely Fast Oxidation (IFO) models,
49
50 and experimental measurements. Temperature results using the FRO model
51
52 show similar agreement compared with the IFO model, while the Marg model
53
54 tends to overpredict it because of the incorrect prediction of soot so under-
55
56 prediction of radiative heat losses. Computational results of soot volume
57
58
59 38
60
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 1
2
3
4
5
6
7
8
9 fraction show an extreme underprediction using the Marg model compared
10
11 to experiments, while good predictions are found using FRO and IFO. The
12
13 FRO model however is able to capture better the initial and final stages
14
15 of the sooting region across the flame. The soot source terms of oxidation
16
17 and surface growth were later studied at the initial and final portion of the
18
19 sooting region, which explains the mechanism of soot evolution using the
20
21 three models and also why previous models overpredict oxidation or surface
22
23 growth, confirming what was observed in the soot volume fraction discussion.
24
25
Finally, to consolidate the capability of the FRO model to capture the soot
26
leakage in fuel-lean regions, an analysis of the computational results using
27
28 FRO and IFO models shows that the FRO model indeed agrees with experi-
29
30 mental measurements (while IFO fails), where the sooting region begins and
31
32 the strain rate is still relatively high, and confirms the observations of the
33
34 a priori analyses. Nevertheless, additional investigation might be needed to
35
36 extensively validate the new FRO model in other situations, for instance, in
37
38 turbulent smoking flames (such as the JP-8 Sandia flame [17], where much
39
40 more soot leakage was experimentally observed) and turbulent pressurized
41
42 flames, which will be addressed in the future.
43
44
45 Acknowledgments
46
47
48 The authors gratefully acknowledge funding from NASA under grant
49
50 NNX16AP90A and NSF under grant CBET-2028318. The authors also ac-
51
52 knowledge valuable support in the form of computational time on the Tiger
53
54 high performance computer center at Princeton University, which is jointly
55
56 supported by the Princeton Institute for Computational Science and Engi-
57
58
59 39
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6
7
8
9 neering (PICSciE) and the Princeton University Office of Information Tech-
10
11 nology’s Research Computing department.
12
13
14
15 References
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44 Figure 6: Parity plots of filtered soot oxidation source term using IFO and FRO soot
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46 subfilter models versus the DNS filtered case. The analyzed data correspond to grid
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points belonging to the lean soot leakage region (Z < 0.1) and using di↵erent relative
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49 filter width /h. The standard deviation is indicated for each model.
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42 Figure 7: Mean (top) and RMS (bottom) temperature radial profiles at two di↵erent po-
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sitions above the Sandia burner: x/D = 134 (left) and x/D = 175 (right). Comparison
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45 of computational results using the three soot subfilter models and experimental measure-
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47 ments from Ref. [29].
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39 Figure 8: Mean temperature profiles along the centerline in the Sandia burner. Compar-
40 ison of computational results using the three soot subfilter PDF models and two experi-
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43 Figure 9: Mean (top) and normalized RMS (bottom) soot volume fraction radial profiles
44 at three di↵erent positions above the Sandia burner: x/D = 70.3 (left), x/D = 132.8
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46 (middle) and x/D = 195.3 (right). Comparison of computational results using the three
47 soot subfilter PDF models and experimental measurements from Ref. [31].
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26 Figure 10: Mean soot volume fraction profiles along the centerline in the Sandia burner.
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28 Comparison of computational results using the three soot subfilter PDF models and ex-
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30 perimental measurements from Ref. [30].
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51 Figure 11: Soot resolved intermittency along the centerline in the Sandia burner. Com-
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parison of computational results using the IFO and FRO soot subfilter PDF models and
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27 Figure 12: Soot temperature along the centerline in the Sandia burner. Comparison of
28 computational results using the IFO and FRO soot subfilter PDF models and experimental
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30 measurements [17].
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52 Figure 13: Mean mixture fraction along the centerline in the Sandia burner: soot subfilter
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54 PDF models do not a↵ect the mixture processes.
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41 Figure 14: Profiles of normalized conditional mean soot volume fraction source terms
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43 hdfv /dt | Zi/hfv | Zi in mixture fraction Z, for oxidation (magnitude, top) and surface
44 growth (bottom), and at two di↵erent positions above the Sandia burner: x/D = 100
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46 (left) and x/D = 205. Comparison of computational results using the three soot subfilter
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PDF models.
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35 Figure 15: Left: conditional mean OH mass fraction hYOH | Zi and soot volume fraction
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37 hfv |Zi profiles in mixture fraction Z. The stoichiometric mixture is also indicated (vertical
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line). Right: Radial profiles of normalized OH mass fraction and mean soot volume
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40 fraction fv . Comparison of computational results using the IFO and FRO soot subfilter
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42 PDF models and experimental measurements [17, 30] at x/D = 70.3. The vertical line
43 indicates the spatial position where hZi = Zst .
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