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Prog.EnergyCombust.Sci., 1984,Vol.10,pp. 319 339. 0360-1285/8450.

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LAMINAR DIFFUSION FLAMELET MODELS


IN N O N - P R E M I X E D T U R B U L E N T C O M B U S T I O N
N . PETERS
lnstitutJh'r Allgemeine Mechanik, R W T H Aachen, F.R.G.

Abstract The laminar flamelet concept views a turbulent diffusion flame as an ensemble of laminar
diffusion flamelets. Work relevant to the flamelet concept is spread over various fields in the literature:
laminar flame studies, asymptotic analysis, theory of turbulence and percolation theory. This review tries to
gather and integrate this material in order to derive a self-consistent formulation. Under the assumption of
equal diffusivities a coordinate-free formulation of the flamelet structure is given. This assumption is relaxed
and flow dependent effects are considered. It is shown that the steady laminar counterflow diffusion flame
exhibits a very similar scalar structure as unsteady distorted mixing layers in a turbulent flow field.
Therefore the counterflow geometry is proposed to be the most representative steady flow field to study
chemistry models and molecular transport effects in laminar flamelets. The conserved scalar model is
interpreted as the most basic flamelet structure. Non-equilibrium calculations are reviewed.
The coupling between non-equilibrium chemistry and turbulence is achieved by the statistical description
of two parameters: the mixture fraction and the instantaneous scalar dissipation rate. The hypothesis of
statistical independence of these two parameters is discussed. Calculation methods for the marginal
distributions are reviewed. It is shown how local quenching of diffusion flamelets leads to a reduction of
burnable flamelets. However, there are burnable ftamelets in a turbulent flame which are not reached by an
ignition source. This phenomenon is described by percolation theory. Complementary approaches related
to local quenching effects and connectedness are combined to derive criteria for the stabilization of lifted
flames and to blow out. Further applications of the flamelet concept are reviewed and work to be done is
discussed.

NOMENCLATURE u component of local flame velocity vector


Uo nozzle exit velocity
a normalized temperature difference of the two feeds u: component of flow velocity vector
aij number of atoms of element j in a molecule of laminar flame velocity at stoichiometric mixture
species i vr
wl chemical production rate of species i
aq stagnation point velocity gradient at quenching x~ coordinate
as stagnation point velocity gradient y~ mass fraction of species i
B frequency factor Z~ mass fraction of element j
C Chapman-Rubesinparameter(pp)/(pp)o ~ Z z , Z 3 transformed coordinates
cp mean specific heat at constant pressure
small expansion coefficient
cvl specific heat of species i g
turbulent dissipation
D diffusion coefficient, defined by (2.3)
similarity coordinate
D~k multicomponent diffusion coefficient r/
2 thermal conductivity
d nozzle diameter dynamic viscosity
E activation energy v~,v~' stoichiometric coefficients
f non-dimensional stream function
_pv/(p~p~a~)l~2 P density
ff variance of the lognormal distribution
f' non-dimensional tangentialvelocity u/(asx )
variance of the velocity distribution
H stabilization height a~
transformed time coordinate
h enthalpy
instantaneous scalar dissipation rate
hi enthalpy of species i Z
Ji non-dimensionaldiffusion f l u x j i / ( p ~ u ~ a y / 2 Subscripts
j,~ diffusion flux of species i
C carbon element
k" kinetic energy of turbulence
F fuel, flame
Le Lewisnumber 2/(p%D)
H hydrogen element
Mi molecular weight of species i max at maximum temperature
)~ mean molecular weight O oxygen element
n number of species
02 oxygen
P probability density function q at quenching
Pb fraction of burnable flamelets ref reference value
Pc probability ofconnectedness st at stoichiometric mixture
p, probability that the local flame velocity exceeds the
local flow velocity
Pr Prandtl number/.t%/2 1. INTRODUCTION
qR radiative heat flux
T temperature C h e m i c a l l y reacting flows m a y p r o f i t a b l y be discussed
t time in t e r m s o f the c h a r a c t e r i s t i c time scales r e q u i r e d for

319
320 N. PETEl~S

convection, diffusion and reaction. Non-premixed developed by Janicka and Kollmann6 to calculate NO
combustion is generally associated with diffusion formation 7 and OH-profiles 8 in hydrogen-air dif-
flames which owe their name to the rate-controlling fusion flames. Their formulation uses a three-body
step of these three processes--to diffusion. The con- recombination reaction as the only kinetic step and is
vective and diffusive time scales are in general of the restricted to close-to-equilibrium Hz-flames. This
same order of magnitude but the chemical time scale is formulation has been extended by Bilger9 who uses a
very much smaller. Therefore the assumption of fast large Damk6hler-number perturbation and expands
chemistry (local chemical equilibrium) appears to be the mass fractions around their equilibrium value.
self-explanatory. It is an assumption which introduces Exact equations are then derived for the perturba-
an important simplification, since it eliminates many tions. The averaged forms of these equations contain
parameters, those associated with chemical kinetics, unknown terms that must in general be calculated on
from the analysis. the basis of a joint pdf. Bilger has shown how this
This global comparison of time scales, however, approach is simplified in the case of phototechnical
may not be sufficient in turbulent flows where local smog reactions and for hydrogen air flames? °
diffusion time scales vary considerably. The fast Recently Bilger and Sterner developed a two-variable
chemistry assumption is then locally not valid and formulation11 and a three-variable formulation 12 for
non-equilibrium effects must be taken into account. If hydrocarbon combustion to predict CO-burnout.
the average diffusion time scale approaches the order Large Damk6hler number perturbation techniques
of magnitude of the chemical time scale, local are restricted to close-to-equilibrium combustion.
quenching will occur. A further reduction of diffusion They cannot include far-from-equilibrium effects such
time scales then leads to lift-off and even blow-off of as flame extinction. However, extinction phenomena
the entire turbulent flame. But already in globally are typical for all flames and a chemical mechanism
stable flames the variation of diffusion time scales may that does not predict them is clearly incomplete. For a
interact selectively with the different chemical pro- global one-step reaction it is known that extinction is
cesses occurring in the system. Their chemical time due to a large activation energy of the combustion
scales may be quite different. For instance, the time reaction. It has been demonstrated by Borghi 13 that
required for combustion and generation of heat is the closure of the chemical source term by moment
much smaller than the time required for the formation methods becomes intractable if the activation energy
of pollutants such as NO x and soot. Technical flames is large. A presumed joint pdf for the conserved scalar
are usually operated such that the combustion and the temperature as progress variable was used 1~
reactions are brought to completion with a minimum to derive a closed form expression for the mean
of pollutants being formed. One may therefore say turbulent reaction rate in the limit of large activation
that the art of technical combustion consist in con- energies. Effects far-from-equilibriumwere included in
trolling the time scales within the non-equilibrium this study showing how quenching would reduce the
range to meet the opposing requirements of fuel turbulent reaction rate.
burnout, stability and low pollutant emission. As a different approach, Spalding's ESCIMO
model ~s (Engulfment, Stretching, Coherence, Interdif-
fusion, Moving-Observer) falls into the category of
1.1. Non-Equilibrium Effects in Diffusion Flames
non-equilibrium models. The model appears more
Treated by other than Flamelet Models
speculative than well-founded but it has some inter-
Over many years the fast chemistry assumption has esting features that will be treated in a rigorous way in
been used in non-premixed combustion to predict the laminar flamelet formulation. It contains two
global properties of turbulent flames on the basis of parts, the "biographic" part describing the chemistry
semi-empirical turbulence models. The essential aspects associated with "folds" and the "demo-
feature of the calculation is the introduction of a graphic" part describing the fold distribution. The
chemistry-independent "conserved scalar" variable biographic part may best be understood by relating
called the mixture fraction. All scalars such as tem- the folds to the flamelets described in this review: they
perature, concentrations and density are uniquely consist of an unsteady one-dimensional structure in
related to the mixture fraction on the basis of the fast terms of a normalized space coordinate. For non-
chemistry assumption. The conserved scalar approach premixed combustion, only the steady-state flame
has been reviewed by Bilger, ~'2 Williams and Libby; 3 sheet approximation which excludes non-equilibrium
and its computational implications by Jones 4 and chemistry, has been used so far,16 but chemical kinetic
Jones and Whitelaw. 5 However, the fast chemistry effects can in principle be incorporated. This was
assumption fails whenever non-equilibriumeffects are demonstrated for premixed flames by Tam? 7
important. In semi-empirical turbulence models, "Stretching rate" and "age" appear as external
balance equations for the moments of the fluctuating parameters in the equations. The demographic part
quantities are derived with unknown terms modelled remains obscure, since it is difficult to see how the
on the basis of experimental data. Non-equilibrium formulation is related to basic balance equations in
effects need at least one additional "progress" variable chemical hydrodynamics. It closely resembles a pdf
to be included and the equations for its moments to be transport equation formulation for the characteristic
modelled. A two variable formulation has been time scales of the folds. It will be shown below how the
Laminar diffusionflamelet models 321

effects of "stretching" and "aging" can be incorporated on quenching conditions as the last term in (2.2),
within a single parameter, the instantaneous scalar which describes heat loss due to radiation. The effect
dissipation rate, in the laminar flamelet formulation, of pressure changes and the analogy between pressure
and how straight-forward statistics relate its distribu- decrease and volumetric heat loss has been analysed
tion to the properties of the turbulent flow field. for premixed flames in Ref. 18.
Transport properties are often simplified by
neglecting the Dufour and Soret effect and by
1.2. Outline
replacing multicomponent diffusion by Fick's law
The objective of this review is to show how the with a single diffusion coefficient
conserved scalar formulation can be extended to
0Yi ,~
include non-equilibrium effects. In Section 2 it will be ji~ = - p D - - , pD - --, i.e. Le = 1. (2.3)
demonstrated that a general coordinate transforma- 0.'¢ ~ cv
tion, using the mixture fraction as independent vari- Such an approximation is unappealing on principle
able, leads to a one-dimensional quasi-steady struc- grounds and may lead to considerable errors.
ture of all scalar profiles in terms of the mixture Systematic investigations of transport properties have
fraction. The essential non-equilibrium parameter is been performed for premixed flame calculations19 and
the instantaneous scalar dissipation rate at stoichio- for diffusion flames, z° In the asymptotic theory of
metric conditions, Zst. The physical significance of this premixed flames, using the limit of large activation
quantity will be demonstrated. In Section 3 fast- energies, it is shown that even small deviations from
chemistry models and some modifications reported in the assumption of equal diffusivities leads to a qualita-
the literature will be interpreted as flamelet represen- tively different description of stretch effects and
tations in the limit X~t-* 0. The construction of non- stability.21
equilibrium models either from numerical calcula- In non-premixed combustion, however, (2.3) leads
tions or asymptotic analysis will be discussed. to even greater analytical simplifications than in pre-
Particular emphasis will be placed on conditions that mixed combustion since it permits the introduction of
lead to local quenching events. The statistics of the a single conserved scalar variable to which all element
two parameters that appear in the flamelet formula- mass fractions are linearly related. A further
tion, the mixture fraction and the instantaneous scalar assumption that is needed for the conserved scalar
dissipation rate, are discussed in Section 4. Existing formulation is that the flow consists of two feeds, the
theoretical predictions and experimental data are fuel and the oxidizer, and that no-flux conditions
collected and the underlying assumptions are apply on all other bounding surfaces? The two-feed
discussed. The fraction of burnable flamelets is assumption has been relaxed by Lockwood and
derived. Percolation theory is introduced to describe Salooja, 22 who consider three feeds, the fuel feed and
situations where flamelets that are not reached by an two oxidizer feeds with different oxygen-to-inert
ignition source remain unignited although they could ratios.
burn. In Section 5 first applications of flamelet models
are presented. Finally, an outlook on work to be done
is given in Section 6. 2.1. The Mixture Fraction
While reacting species are consumed or produced,
chemical elements are conserved during chemical
2. THE LAMINAR FLAMELET F O R M U L A T I O N reactions. Therefore the mass fraction of the chemical
element j
The balance equations for species and enthalpy may
be written as aum j
Zj = i=1
L ~ Yi (2.4)
oY, or, oj,~
p ~t +PV~ +-- : I~ i (2.1) obeys a conservation equation which is obtained by
0x~ 0x~
summation over (2.1) according to (2.4). Introducing
0h 0 0h] the operator L this is
p ~ + p v ~ Ox~ c~x~\c e Ox~/

L ( Z j ) = - p ~ - + p v ~ Ox~ (
¢?x~ pD Ox~/
- c~x~i=,hi~p~X~ +ji~ + c t + q a "
a " a i j M j f DSYi .
(2.2) - ox , l M, +;ff t25t
In (2.2) the viscous dissipation term and spatial
pressure gradients have been neglected on the basis of where the chemical source terms cancel identically. It
the low Mach number approximation. In open is seen that the r.h.s, of (2.5) and the first term on the
diffusion flames the term t3p/c~t may be omitted as well. r.h.s, of (2.2) vanish if (2.3) is introduced.
In Diesel engine or stratified charge engine com- Extending the notation of Zj to linear combinations
bustion, which are both non-premixed systems with of element mass fractions, one may introduce fuel and
changing bulk pressure, it can have a similar influence oxidizer element mass fractions. For fuels containing
322 N. PETERS

only carbon, hydrogen and oxygen as elements one oxidizer x2I


defines

Z r = ZC, F -[-ZH,F -~-Zo, F


(2.6)
Zo = Zc, o +ZH,o + Z o , o fuel
where Zj, F is the mass fraction o f e l e m e n t j in the
mixture originating from the fuel and Zj,o is the mass
fraction of element j in the mixture originating from Z=Zst
the oxidizer. Ze and Zo are defined such that they are FIG. 1. Schematic representation of the coordinate trans-
equal to the fuel and oxygen mass fractions in the formation.
corresponding non-reacting mixture. The general
definition of the conserved scalar ~ for a two-feed sufficiently high, a condition to be discussed below.
system (index 1 denoting the fuel stream and index 2 We will call this thin layer and the surrounding inert
the oxidizer stream) is mixing region a laminar diffusion flamelet. The
concept of laminar diffusion flamelets in a turbulent
ZF -- YF,2 Z o -- Yo,2
diffusion flame has been introduced by Williams. 24
YF, 1 - - YF,2 YO,1 -- Yo,2 Let us introduce a coordinate system attached to the
This definition includes the possibility that the fuel surface of stoichiometric mixture. We replace the
and oxidizer streams are partially premixed. To coordinate x 1 by the mixture fraction Z and define the
differentiate from this case we will use the notation Z original coordinate system such that the coordinate x 1
for the mixture fraction in unpremixed systems with does not lie within this surface (cf. Fig. 1). This is a
YF,2 = 0 , YO,1 = 0 coordinate transformation of the Crocco-type, who
expressed the temperature as a function of another
ZF Zo dependent variable, the velocity, in a fiat plate
Z- YF,1 - 1 - Yo,~" (2.7)
boundary layer. Here the scalars T and Y~ will be
In terms of Z the stoichiometric mixture is obtained as expressed as functions of the mixture fraction Z. By
definition, the new coordinate Z is locally normal to
YFlV,oMo.]_ 1 the surface of stoichiometric mixture. Using Z z = Xz,
Zst = 1 Y%,zV'FMF; (2.8) Z 3 = x 3, r = t as the other independent variables, we
obtain with the transformation rules
Assuming (2.3), it is seen that the mixture fraction
obeys the equation 0 8 8Z 8 8 8Z 8
L(Z) = 0. (2.9) 8t-0r I-0t 8 Z ' S x x 8x 1 8 Z

Also, using the definition of the enthalpy 8 0 OZ 0


8x k ~Z~k+~X~xkSZ , (k = 2,3) (2.13)

h= ~ hiYi, dh=cpdT+ ~ h, dYi (2.10) formally from (2.1) and (2.11) with (2.3) and (2.9) the
i=1 i-1
equations
the temperature equation can be derived from (2.1)-
8Y~ / S Z \ 2 82Y~ .
(2.3) as p ~ = pDkff~x~) ~ - + w , - R ( Y ~ ) (2.14)

i = 1 Cp Cp
= pD _ _\8x~,~] - - i E,7 --
e p w,'.

+ ¢pi 8Yi 8T 2 8% 8T
i/'=1 -Cp
- p D - -8Xa
--q 8Xo~ cp2 8x~ Sx~ "
+-- +qR
ep
(2.11)
where the operator R is defined as
For approximate solutions the last two terms in (2.11)
are in general neglected as being small compared to ( ~7-
0 ~ 8- - ) ~(pD) 8 8(pD) 8
R=p
the source term. /)2 v ~ 2 -1-/)3 t ~ 3 8X 2 8 Z 2 8x 3 8 Z 3
3 (SZ 02 02 )
2.2. Transformation into a Coordinate-Free System + ~-~2 • (2.16)
- - P D k E2= 2 8Xk OZOZ k 8Z k
We follow Ref. 23 and assume the mixture fraction
Equations (2.14) and (2.15) describe the flamelet
Z to be given in the flow field as a function of space
structure. In the thin inner reaction zone all terms
and time by solution of (2.9). Then the surface of
involving derivatives with respect to Z 2 and Z 3 are of
stoichiometric mixture can be determined from
lower order compared to the first term on the r.h.s, of
Z(xo~, t) = Zst. (2.12) (2.14) and (2.15). It can formally be shown by intro-
ducing a stretched coordinate
Combustion takes place in a thin layer in the vicinity
of this surface if the local mixture fraction gradient is ( = ( Z - Zst)/g (2.17)
Laminar diffusionflameletmodels 323

reoction
ioerf oufer zone zone iner~ outer zono

Zsf
Z~

FIG. 2. Schematicrepresentation of the flamelet structure.

into (2.14)-(2.16), where e is the inverse of the non- the outer zones will depend on the amplitude of the
dimensional activation energy, that the operator R is disturbances from the inner zone.
of higher order in e.23 For a one-step reaction with a Saitoh and Otsuka 25 have analysed, both
large activation energy the frozen flow structure of the numerically and experimentally, the frequency
outer layers is to a leading order equal to the response of counterflow diffusion flames to small
equilibrium structure, which depends on Z only. amplitude velocity oscillations. They observed a
The flamelet formulation leads therefore to a one- frequency response of flame-zone oscillations that
dimensional structure normal to the surface of compares well with a theory based on the flame sheet
stoichiometric mixture. Applying the same arguments approximation (cf. Section 3). In this case the scalar
to the unsteady terms in Eqs (2.14) and (2.15) shows profiles depend on Z only and the entire flamelet
that these terms can be neglected in the inner reaction structure is quasi-steady. The observed decrease of the
zone as well. Exceptions to this quasi-steady burning response of the amplitude with increasing frequencies
state may occur only close to quenching or if the is therefore, essentially that of the mixture field to
unsteady disturbances introduced by the turbulent velocity fluctuations, independent of chemistry. The
flow field occur on a very short time scale of order flame oscillates then with the mixture field with a
O(re2). "flapping flame''26 behaviour. However, when the
The influence of the flow field is introduced into the flame was highly diluted, it was extinguished by low-
Eqs (2.14) and (2.15) by the instantaneous scalar frequency flow field oscillations, indicating a large
dissipation rate defined by amplitude interaction of external disturbances with
non-equilibriumeffects. We conclude that except close
X=
2 ( zi2=2 ( zl2+( zl 2 ( zl2l to extinction, the unsteady terms in (2.14) and (2.15)
may be neglected in the entire structure, if the flamelet
(2.18) is burning.
This leads to five different states of the flamelet:
It has the dimension one per sec and may be interpreted
as the inverse of a characteristic diffusion time. Due 1. The steady unreacted initial mixture.
to the transformation it incorporates implicitly the 2. The unsteady transition after ignition.
influence of convection and diffusion normal to the 3. The quasi-steady burning state.
surface of stoichiometric mixture. A schematic solution 4. The unsteady transition after quenching.
for the temperature profile is shown in Fig. 2. The 5. The unsteady transition after re-ignition.
flamelet structure consists essentially of a thin inner
reaction zone embedded between two chemically inert The possibility that quenched flamelets will not be
outer zones. Since unsteady terms are of lower order re-ignited with the consequence of unburnt fuel
in the thin reaction zone, disturbances which act via Z emission is also contained in point 4.
on the flame structure, are transmitted immediately to The unreacted structure is simply given by (2.7) for
the outer zones which are described by a balance of ZF, Zo in terms of Z. Equations for the quasi-steady
the diffusion term and the unsteady term in Eqs (2.14) burning state have been derived by Bilger, 27'28 on the
and (2.15). Whether unsteady effects are important in basis of the a priori assumption, Yi= Yi(Z). The
324 N. PETERS

unsteady transitions require the specification of initial


conditions and depend therefore on a larger number of t
parameters. This makes their statistical treatment in Tmox
an Eulerian frame of reference more difficult. As they
can be expected to occur less frequently than the
steady states in turbulent diffusion flames, their con-
tribution will be omitted.
By characterizing the flamelet structure by the in-
stantaneous value of z(Z, t) the analysis focuses on the
low frequency part of the ;(-spectrum. For high fre-
quencies the time average value of ;((Z, t) would be -1 -1
more representative, but differences would only be Xq tog Xst~
important if high-frequency oscillations of ;( were
FIG.4. The S-shaped curve showing quenching (Q) and
accompanied by large amplitudes. Another auto-ignition (1).
restriction, mentioned before, concerns the magnitude
of local mixture gradients and therefore the magni-
tude of Z. If ;( is too small, the neglection of higher
order terms in (2.14)-(2.15) is no longer justified. shown in Fig. 4. Here the maximum temperature is
When this happens, however, the equilibrium limit is plotted over the inverse of ;(st for given chemical
approached, where again the flamelet structure kinetics. Burning of the flamelet corresponds to the
depends on Z only. upper branch of the curve. If ;(st is increased the curve
In summary, the proposed flamelet structure con- is traversed to the left until ;(q is reached, beyond
sists of two quasi-steady states, the unreacted initial which only the lower, extinguished steady state exists.
mixture and the burning state, both as a function of The transition from the point Q to the lower state
the mixture fraction as independent variable. This corresponds to the unsteady transition described by
distinguishes it from previous formulations, in state 4. Auto-ignition, which would correspond to an
particular the biographic part of ESCIMO, where an unsteady transition from the point I to the upper
unsteady fold structure in the one-dimensional curve, is unlikely to occur in diffusion flames, since the
physical space is considered. required very large residence times (very small values
of ;(st) are not reached. Ignition of the initial mixture
or re-ignition of quenched flamelets will therefore
2.3. Physical Significance of the Instantaneous Scalar require an ignition source (cf. Section 4).
Dissipation Rate The parameter ;(q can be interpreted as a global
If we assume the flamelet to be burning and increase kinetic quantity describing non-equilibrium effects in
;( (characterized by ;(st = ;((Zst)) with time, heat con- diffusion flames. It is the critical value where finite rate
duction from the reaction zone to both sides will kinetics just balance diffusion. In this sense it is
increase. Temperature profiles for different values of equivalent to the flame velocity in premixed flames
;(~t are schematically shown in Fig. 3. There is a shift of which also represents a global kinetic quantity. Both
the reaction zone to larger values of Z if Z~t is small. If quantities are in principle interrelated but care must
;(~t is increased beyond the critical value ;(q heat con- be taken to use the equivalent chemistry model for
duction to both sides can no longer be balanced by both, premixed and diffusion flames. Numerical
heat production due to chemical reaction and the values of ;(q will be given in Section 3.
flamelet is quenched. This behaviour is illustrated by To obtain a physical idea about the instantaneous
the well-known S-shaped curve for the steady states scalar dissipation rate let us consider a one-dimen-
sional laminar mixing layer governed by the equation
~z ,~ / ~z\
p ~ 7 = ~xLPD~x) (2.19)

with the initial and boundary conditions


t=O:Z=lforx<O, Z=Oforx>O
t > O : Z = 1 for x---~-oo, Z=Ofor x---++m.
(2.20)
With the assumption
p2D = (p2D)rer (2.21)

st we obtain in terms of tile similarity coordinate


Z~
FIG. 3. Schematic representation of the temperature as a r/ = ~ (Dreft)- 1/2 P~ dx (2.22)
function ol Z and Zst. Pref
Laminar diffusionftameletmodels 325

the solution important influence on the quenching condition. This


effect is in principle flow dependent but the variation
1
Z = ~erfc(q). (2.23) between different flows is less important than the effect
itself. The second point above becomes important due
The instantaneous scalar dissipation rate is to the shift of the reaction zone demonstrated in Fig. 2.
This shift may be considerable if Zst is small. For
1 hydrocarbon air flames Zst is typically around 0.05
z(Z, t) = 27t exp ( - 2r/2(Z)). (2.24)
and the reaction zone shifts to about two to three
For small values of Z (large values of q) the comple- times this value close to extinction if a one-step
reaction is considered. This case is analysed in Ref. 30.
mentary error function erfc may be replaced by
n - '/2r/- 1exp -r/2 such that Z can be expressed as However, the effect may be less important for real
kinetics.
= 2Z 2[erfc- ~(2Z)]2/t (2.25) The use of laminar ftamelets in turbulent flows
requires a parametric representation of the g profile,
where erfc- ~ is the inverse (not the reciprocal) of the
complementary error function. With Z fixed, the preferably by a single parameter. The value
Zst = x(Z~t) has been proposed in Ref. 23. This choice
scalar dissipation rate is therefore inversely propor-
tional to time. This is equivalent to the "aging" was motivated by asymptotic analysis for large activa-
process in Ref. 15. tion energies where the change ofx is considered to be
a higher order effect. It can also be justified by the fact
We may likewise consider a mixing layer that has
that Z~t is a known constant for any fuel-air mixture.
been distorted such that the surface at Z = 0.5 is given
by x 1 = xs (x2, x3, t). We postulate that the profile can However, ~(stis not representative for the actual scalar
dissipation rate in the reaction zone. Liew et al. 31
now be described by Eq. (2.19) in terms of the
coordinate x relative to the distorted surface recently suggested that the value of Zm~x at the
maximum temperature would be a better choice. We
X = X 1 --XS(X2,x3, t ). will use both values in the following.
If flow dependent effects are important, one could
Then Z is calculated as
think of several laminar flow models to be representa-
1 2 ~X S 2 OX s 2 tive for flamelets in turbulent flows. If the properties of
all these different models were analysed, a weighted
average on the basis of their statistical representation
(2.26)
in turbulent flames could be calculated. This pro-
The last term in brackets describes the area increase of cedure, however, may not provide any better results
the mixing layer with respect to the undisturbed case. than the choice of a single laminar flow model, whose
Compared with the model developed in Ref. 15 this properties are more representative than others. If one
term can be interpreted as '"stretch". It should be assumes that flamelets of the mixing layer type are
noted, however, that contrary to "ESCIMO" the predominant in turbulent diffusion flames, it seems
present ftamelet formulation treats both effects by a appropriate to choose a laminar flow configuration
single variable and therefore needs a statistical that fulfils the following requirements:
description for this variable only.
1. it is a steady-state configuration that can be
investigated experimentally;
2.4. Flow-Dependent Effects 2. the Z dependence of the x-profile follows closely
that of unsteady mixing layers.
An essential objective of the flamelet formulation is
to uncouple chemical kinetics from turbulence. It Such a configuratio~ is the counter-flow geometry
should therefore be possible to evaluate the scalar or stagnation-point flow. It has the additional advan-
profiles from a laminar flow configuration and to use tage that in recent years counter-flow diffusion flames
them in a turbulent flow. This requires that: have been studied theoretically and experimentally
more often than any other diffusion flame configura-
1. the assumption (2.3), required by the definition
tion, since the governing equations reduce via a
of the mixture fraction, leads to sufficiently good
similarity transformation to one-dimensional
approximations;
equations. In Ref. 23 it is shown that under certain
2. the Z-dependence of z(Z, t) agrees sufficiently
simplifying assumptions the z-profile is for small Z
well for the laminar and turbulent flows con-
sidered. Z = 4a~Z2[erfc 1(2Z)] 2 (2.27)
With respect to the first point, a recent study of Law where as is the stagnation-point velocity gradient.
and Chung 29 is of interest. These authors have Comparison with (2.25) shows the same Z-depen-
analysed the influence of fuel and oxidizer Lewis- dence as the unsteady mixing layer. We therefore
numbers different from unity, for three different flow propose to use the counter-flow configuration as the
configurations using the limit of large activation representative laminar flow model with arbitrarily
energies. They find a change of the maximum flame complicated transport properties and chemistry. The
temperature proportional to ( L e - 1) and therefore an steady, one-dimensional equations may be written in
326 N. PETERS

terms of the similarity coordinate The origin of the non-dimensional stream function is
fixed by
(2.28)
q \(PP)~) pdy
f = f~ f'd~/. (2.37)
as

The only fluid mechanical parameter in these


0 /'c0f'~ f0f' p~ f,2
~t ~)+ ~+7- = 0 (2.29) equations is the stagnation-point velocity gradient as.
Once these equations have been solved, there appears
~Ji ~Yi " the problem of how to define the mixture fraction Z
I-f~-q+W~ = 0 ( i = 1,2 ..... n)
@ and how to calculate z(Z). Bilger28 has faced this
problem when he analysed experimental data. He
(2.30)
noticed important differences of the normalized

c~Tt,,~qqJ+f~-&li=aL
( J' + Pr
4
& l J = O.
element mass fractions in the flame front due to
differential diffusion and proposed to use the element
mass fraction of carbon Zc, to represent Z. Other
(2.31) definitions, such as the average value of all element
The diffusion flux may be expressed either by a binary mass fractions could also be appropriate. The scalar
diffusion law dissipation rate, z(Z), is then to be evaluated with
D = , ~ / C p p =- D(T, Yi) calculated as a function of Z.
J~ = - C pD~ ~Y~ C - Pp (2.32) The temperature dependence of D may not be as
@ ' (p~)~
critical as it first appears. For time-dependent one-
or by a multicomponent diffusion law dimensional flows, or plane two-dimensional steady
boundary-layer flows, a density transformation of the
pDik 3 _ form of (2.22) or (2.28) and the use of the assumption
Ji = ~ L C ~ - ~ (MY,) (2.33)
k=l (2.21) or C -= I leads to the same governing equations
as in the constant density case. This implies that a
where thermo-diffusion effects as well as Dufour decrease of density due to combustion decreases the
effects have been neglected. The non-dimensional scalar gradient by a factor P/Pr~f which for a constant
reaction rate is Prandtl number cancels with the increase of D in
X ~ D~2Z/c~Y 2. The variation of Z with Z is therefore
W~= #~ (2.34) not expected to differ very much from (2.27) for small
Pa,
values of Z. The values Z~t and Zmax can then be
and the boundary conditions are calculated. Again an approximate relation between
tl= - o o : f" = ( p j p _ ~ ) a / 2 , y~= Y ~ _ ~ , h = h _ ~ ~(max and ;(st is given by (2.27) if the shift from Zst to
Zmax is known. It may also be noted that the form
(2.35)
rl = + oo : f' = l, Y~= Y~oo,h = h ~. (2.36) X = ~ e x p { - 2 [ e r f c - 1(2Z)] 2} (2.38)

I
T 2000 I
['el I .... chemico[ equilibrium
, \ I
I -- non equilibrium
// ", tI --,-- experimentol doto
1500 I
Lsco[e spill

1000

500

0
f'
0 0.0~, ] 0.68
stoich
0.'12 0.'16 0.2 o'.4 o'.6 o', 12o
Z~

FIG. 5, Temperature profiles over Z for the counter flow diffusion flame in Ref. 35.
Laminar diffusion flamelet models 327

0.2 I 1.0
. . . . equilibrium I /
-- non equilibrium I sca[e split / /
0.16 --.-- experimental data , ~ 0.8

012 / 0.6

008

0.04

-J, , , 1 .-"--'-~:-~--7
- - - ~ •

004 0.08 0.12 0.16 0.2 0.4 0.6 0.B


stoich Z
Fla. 6. Fuel and oxygen profiles over Z for the flame in Ref. 35.

I
. . . . chemical equilibrium I ~',
r/ ~,
0.2
..__ H20 /", "
0.16-
%%\\\ ii I "sk

0.12- ;k"
H xlO//' \~ \ "~
0~)8- Ii x I ~-" ~ x \

// --
LU2 ,/ .--'" \ r s c o l e Spilt ', ",, \.

0.04- / ." ,,9 "


i /,/ I ~, - ~ . --%~ x x,,x

,,/ " ""


_.;;;/ I ........ "- "-J-'--

o641 I
008 0112 0116 0.2 0 ./,.. 0.6 08 I
stoich Z
FIG. 7. Chemical equilibrium product profiles over Z for the flame in Ref. 35.

I
I 0.2 J
Yi non equilibrium I

1 :
calculation i
0.16 i scnte split

I
H20 I
0.12 I

I
0.08

0.04
y
o.641 068 o12 o'16 02 ok 0'6 o18 i
stoich Z
FIG. 8. Non-equilibrium product profiles over Z for the flame in Ref. 35.

Jpzcs I0:3-C
328 N. PETERS

I
r
[
0.2
Experimental data I
I

I
0.16 I
~scnle split
I
/ i
0.12

0.08

0.0t~

0 .
0.64[ t 008 0'12 0'16 0.2 016 018 i
stoich Z - -

FIG. 9. Experimental product profiles and the modified flame sheet model over Z for the flame in Ref. 35.

should be used instead of (2.27) for C = 1 if Z is not 3.1.1. The flame-sheet model
small. This form is to be compared with Eq. (2.24). The oldest conserved scalar model is the flame-
sheet model by Burke and Schumann. 38 It is based on
the assumption of a one-step irreversible reaction with
3. C H E M I S T R Y MODELS fast chemistry and complete combustion. It has been
The coordinate-free formulation of diffusion used by Becker, 39 Lockwood and Naguib 4° and many
flamelets allows the use of arbitrarily complicated others. It also incorporates an essential feature found
chemistry including pollutant formation like N O x and in non-equilibrium flames: the fact that the fuel
soot. The turbulent flow field acts upon the flamelet diffuses nearly unreacted to the surface of stoichio-
structure only through Xst. Since fairly accurate metric mixture. It has the disadvantage that inter-
kinetic data are available today for hydrogen and mediate products such as CO and H 2 are not
hydrocarbon flames 32'33 and non-intrusive measure- predicted. A modification based on the equation
ment techniques such as Raman scattering are suf-
v~ F + vb2 0 2~ VCO C O -1- V~l 2 H 2 + V~o: C O 2
ficiently reliable for steady laminar flames, it is only a
matter of choice and of available resources to deter- + v~i2oH 2 0 + radicals (3.1)
mine the flamelet structure. Tsuji 34 has recently
reviewed experimental data of counter-flow diffusion would yield such intermediates but requires the speci-
flames in this journal. One of the most complete set of fication of the stoichiometric coefficients of the
profiles is probably still Tsuji and Yamaoka's data products. F r o m an examination of the water-gas
from the 13th Symposium on Combustion. 35 A flow partial equilibrium in diffusion flames (cf. Refs 28 and
field calculation for these data based on the flame 41), follows the ratio
sheet approximation has been performed by
Takeno. 36 A numerical analysis for the same K -
v~o "V~2o 3. (3.2)
conditions has been performed, 37 comparing a full v~o2 " vi~2
equilibrium and a non-equilibrium calculation with Likewise, the ratio
the experimental profiles. The results have been re-
plotted in mixture fraction space in Figs 5-9. These v'fi~
K 1 = - - ~
0.2 (3.3)
figures shall serve as a guideline for the discussion of v'fi~o
the different models to follow. can be deduced from the experimental data in Fig. 9. A
further inspection shows that the elemental C/H ratio
is reduced to about 1/3 due to H-atoms contained in
3.1. Conserved Scalar Models
radicals and a faster differential diffusion of atomic
In the past these models have been widely used, and molecular hydrogen out of the reaction zone. This
mainly for two reasons: (1) they describe the flamelet leads to the stoichiometric coefficients, v~o = 3/8,
structure as a function of a single variable, the mixture v'fi2 = 1/4, v~o2 = 5/8 and v'fi~o= 5/4, and with v'd2 =
fraction Z, and require therefore statistics of this 23/16 to a flame surface located at ZF = 0.075 instead
variable only; (2) application has not focused on of Z~t = 0.055. The resulting linear product profiles are
flames where non-equilibrium effects were important. included in Fig. 9.
Laminar diffusionflameletmodels 329

3.1.2. The chemical equilibrium model with experimental data. This comparison revealed
An alternative to the flame-sheet model is the systematic differences between predicted and experi-
assumption of full chemical equilibrium which corre- mental data, that require further investigation.
sponds to the exact limit Zst~ 0. The local equilibrium
as a function of the mixture fraction may be calculated 3.1.4. Conserved scalar models, based on experimental
with the aid of an equilibrium program. 42 This has data
been done successfully by Kent and Bilger43 for Several laminar diffusion flame experiments have
hydrogen flames. Difficulties arise, when the equi- been plotted over the mixture fraction as independent
librium model is applied to hydrocarbon flames. Jones variables by Bilger, 28 in order to determine reaction
and McGuirk 44 and Jones and Priddin 45 tried to rates. The first to use experimental data in the context
predict the combustion in gas-turbine combustion ofa flamelet model were Liew, Bray and Moss 52 using
chambers. They find an overprediction of CO and H 2 data by Mitchell et al. ~a They showed an improve-
levels resulting from the equilibrium values which are ment compared to full equilibrium calculations for an
too large in the fuel-rich mixture. This becomes open turbulent methane-air flame by Hassan et al. 54
evident from the comparison of the profiles in Figs The analysis uses the mixture fraction as the only
7 9. It is seen that the equilibrium profiles of H 2 and variable and assumes implicitly that the instantaneous
CO have very strong peaks in the fuel-rich region scalar dissipation rate in the laminar experiment is
around Z = 0.2-0.3, which are not present in the non- such that its variations in the turbulent flame are
equilibrium calculation or the experimental data. To unimportant. Other experimental data that could be
this peak corresponds the consumption of CH 4 in the used are those from counter-flow diffusion flames of
entire region Z < 0.2 seen in Fig. 6 which also is Tsuji and Yamaoka. 35 For the same configuration
unrealistic. It seems unlikely that local diffusion time there also exist profiles for CH4, 02, CO 2, CO, H20,
scales in turbulent flames will ever be large enough to N 2 and temperature in methane flames by Langkau.55
allow for local chemical equilibrium to be reached. The velocity gradient in his experiments was
as = 40 sec. In these experiments the effect of pre-
3.1.3. Partial equilibrium models heating of air to 245°C was also investigated, but no
An evident alternative to the equilibrium model is dramatic change was observed.
the assumption of partial equilibrium for some species
and non-equilibrium for others. It may be noted that
3.2. Non-Equilibrium Models
this is implicitly done in equilibrium calculations by
excluding species like NO, NO 2 and solid carbon. Non-equilibrium models need to take into account,
Partial equilibrium for other than flamelet models was in addition to the mixture fraction, a non-equilibrium
considered in Refs 11 and 12. parameter, preferably Xst. They can be constructed
A partial equilibrium model of the flamelet type was from numerical non-equilibrium calculations based
developed by Eickhoff and Grethe. 46 This model uses on experimental data or, if the general structure is of
the early idea of Libby and Economos 47 of an equi- interest, more rigorously by asymptotic methods.
librium flame zone in the centre part of a laminar Each of these methods has its advantages and disad-
diffusion flame, which is embedded within frozen flow vantages. The numerical method has the advantage of
zones on both sides. The picture of freezing of the being able to include realistic chemistry, but the com-
chemical reaction and the transition from chemical putational effort can be high. It suffers from remaining
equilibrium to frozen flow had been shown to be a inaccuracies in elementary kinetic schemes and kinetic
large activation energy phenomenon where the transi- parameters, in particular with respect to pyrolysis
tion zones have the structure of premixed flames. 48''.9 reactions in the fuel-rich region. The asymptotic
Eickhoff and Grethe 46 arbitrarily truncate the full method is restricted to a relatively small number of
equilibrium at a mixture fraction of about Z = 0.13 reactions but it provides, in general, closed form solu-
and obtain discontinuous profiles at this value. The tions which allow one to check various effects analyti-
first-order discontinuity in the profiles is clearly un- cally.
realistic and unnecessary in view of Refs 47-49.
Nevertheless, in contrast to the full equilibrium model, 3.2.1. Numerical calculations with elementary kinetics
the model is found to predict CO and H z in the fuel- Non-equilibrium calculations of laminar diffusion
rich part of a turbulent jet flame quite well. flames with a large number of elementary reactions
Conserved scalar models that assume the com- have first been performed in Ref. 37 and for the
bustion reactions in chemical equilibrium, but treat counter-flow flame in Ref. 35. A total number of 36
the NO formation as a finite rate process, may also be elementary reactions was used. These calculations are
considered as partial equilibrium models. Models of replotted in Figs 5, 6 and 8 showing a good agreement
this type have been developed. ~°'~1 The NO forma- with the experiment for the temperature, CH4, 0 2,
tion was based on the Zeldovich mechanism exploit- CO 2 and H 2 0 but too low values for H 2 and CO. This
ing the fact that it has a very large activation energy. A is probably due to the inaccuracy of the kinetic data
closed-form expression was derived in Ref. 50 for the and to the neglect of pyrolysis reactions. More recent
mean NO formation rate in turbulent diffusion flames. kinetic calculations were performed by Mitchell, 56
It was applied 51 to turbulent jet flames and compared Hahn et al. 57 and Hahn and Wendt. 5s In the context
330 N. PETERS

of laminar flamelet models for turbulent diffusion adjacent surfaces of stoichiometric mixture may
flames there are non-equilibrium calculations in the change sufficiently to separate the flame zones in
thesis by Grethe 59 and in the recent thesis by L[ew.6° physical space, but will not necessarily reach 0 or 1.
Both use the same one-dimensional time-dependent For instance, we may assume the flame zones to be
equations that Spalding 15 has proposed for the separated by a rich mixture and separate the flamelets
"biographic" part of his ESCIMO-model. Grethe 59 at the maximum value of Z. Then boundary condi-
considers methane-air diffusion flames and partially tions are to be applied at this value of Z. For a one-
premixed diffusion flames with Le = 1 using 29 step irreversible reaction this situation has been
elementary reactions. Some results are given by Eick- analysed in detail in Ref. 76. It is shown that the
hoffand Grethe 61 and in a recent review by Eickhoff. 62 diffusion flamelets are disconnected, if the variation of
Unfortunately the conserved scalar profiles are not the mixture fraction is large enough such that the
given so that the actual value of)~t cannot be deduced. corresponding flame temperature is lower than a
Liew 6° uses binary diffusion coefficients with characteristic freezing temperature. The flamelets may
respect to the mixture, uses 38 reactions and calculates then be treated as partially premixed diffusion
Zmax. He compares his calculations for constant and flamelets. It is interesting to note that they are more
decreasing fold thickness with the methane flame by sensitive to flame stretch than non-premixed diffusion
Mitchell, Clomburg and Sarofim. 53 These results are flamelets and that extinction occurs at a lower value of
reported in Ref. 31. He observed the shift of maximum the scalar dissipation rate.
temperature towards larger values of Z with in-
creasing Xmax. This is consistent with the schematic
3.3. The Influence of the Instantaneous Scalar
representation in Fig. 3 and the results obtained by
Dissipation Rate on Flamelet Profiles
activation energy asymptotics.l 4,63
The qualitative influence of the scalar dissipation
3.2.2. Asymptotic flamelet models rate has already been discussed in paragraph 2.3.
Lifi/m 64 was the first to use the method of matched Figure 4 shows schematically, that the temperature of
asymptotic expansions to describe the interaction of the burning state is relatively insensitive to changes of
diffusion and finite rate kinetics for a one-step irrever- the actual value of Xst. In evaluating the experimental
sible reaction in the inner zone of a laminar diffusion data of Abdel-Khalik,v7 Bilger 2s finds the mass
flame. He, and later Fendell6s used the limit of large fractions of the fuel C7H16 , 0 2 and CO2 to be
Damk6hler numbers where the activation energy is insensitive to changes of X by three orders of magni-
assumed to be an order-one quantity. Clarke, 66"67 tude. He finds certain influences on intermediates such
Clarke and Moss 68 and Allison and Clarke 69 have as CH 4 and C z H 4 and notes that radicals such as OH,
considered this limit for more realistic multiple O, H may show a much greater variation.
reaction kinetics, to model hydrogen/oxygen diffusion The last argument is certainly also valid for the
flames. An analysis for a two-step chain reaction was formation of NO. The temperature-sensitivity of the
performed by Bush and Fendell.7° Extinction con- NO formation reactions based on the Zeldovich-
ditions, however, cannot be derived in this limit since mechanism is well known (cf. Refs 49 and 50). Small
the plot of the temperature over the characteristic changes in the maximum flame temperature will
Damk6hler number does not exhibit a turning point therefore lead to large changes in the NO formation
as shown in Fig. 4. Lifi~n63 showed that activation rate. One of the future objectives of non-equilibrium
energy asymptotics is a suitable tool to study models will be to determine the influence of X on the
extinction phenomena in steady state diffusion flames. NO formation rate. Another important future field of
Lifi~m and Crespo TM studied the unsteady transition research is related to soot formation in diffusion
from auto-ignition, premixed burning to a diffusion flames. 78 It is easily observed that a laminar (or
flame structure in a non-premixed system. Allison and turbulent) diffusion flame changes colour from yellow
Clarke v2 used activation energy asymptotics for a to blue if the flow velocity is increased, indicating that
kinetic scheme of six elementary reactions for the local residence time is too small to permit the
hydrogen-oxygen flames. Sohrab et al. 7 3 investigated formation of radiating soot particles. Since the
the effect of radiant heat loss on extinction. Lifi/tn TM increase of flow velocity corresponds to an increase of
also analysed the effect of a Lewis number different )~, the colour of a diffusion flamelet is a measure of the
from unity for counter-flow diffusion flames within the local scalar dissipation rate.
framework of the "premixed flame regime". A comple- Soot formation in turbulent acetylene diffusion
mentary analysis was performed by Law and Chung 29 flames has recently been investigated by Kent and
within the framework of Lifi/m's "diffusion flame Bastin. 79 They find that soot volume profiles scale
regime". The interaction of reverse reactions with the with the flame time d/u. (For dimensional reasons, the
main reaction is studied in Ref. 75. flame time is inversely proportional to the mean scalar
Asymptotic analysis can also clarify a question dissipation rate.) Soot formation and oxidation rates
related to boundary conditions. In Section 2 flamelets are mixing-controlled at low flow rates and kinetically
were assumed to be extended in mixture fraction space controlled at high flow rates, as is to be expected from
from Z = 0 to Z = 1. In turbulent flames this is un- the arguments given above. A more detailed analysis
likely to be the case. The mixture fraction between two by Kent and Wagner 8° of sooting laminar flames shows
Laminar diffusion flamelet models 331

400
t 14 I
×q
Oq

ool 12

10
200 - oo 97// 97
100

016 0.18 020


X02

FIG. 10. Evaluation ofxg for nitrogen-diluted methane flames from data. s2

a very great sensitivity on the local soot temperature. counter-flow diffusion flames of Ishizuka and Tsuji s2
A temperature drop by radiation freezes the soot have been interpolated s3 to derive values of Zq for
burnout at about 1300K. The same phenomena is methane air flames diluted with nitrogen. These
observed in turbulent flames. 79 curves are shown in Fig. 10 as a function of the mole
fraction of oxygen in the oxidizer stream. They were
constructed for constant values of Z~t, implying that
3.4. Local Quenching of DifJusion Flamelets
both, the fuel and the oxidizer streams were diluted.
Another phenomenon related to the scalar dissipa- The value OfZq = 7.8/sec is to be compared with the
tion rate is the local quenching of diffusion flamelets. numerical calculation of Liew et al. 62 who estimate a
This has also been discussed in paragraph 2.3 value of ~q,max 50sec, where Zq,max is evaluated at
~

following Fig. 4. If quenching occurs, all reactions the maximum temperature. The shift of thc reaction
including pollutant formation reactions cease zone may account for part of the difference between Zq
abruptly. It is therefore very important to have and Zq. . . . but not for this discrepancy. The
quantitative data on diffusion flame quenching in explanation lies probably in the unsteady numerical
terms of Zst. In Ref. 23 a closed form expression has approach used in Ref. 62. Bilger deduced a value Zq =
been derived for Zq for a one-step irreversible reaction 8/sec for methane based on a perturbation analysis
in the limit of a large activation energy. for a simplified reaction scheme. 12 F r o m his Z-profile
and the approximation of D 28 and the original space
4Z2t(X-Zst)2vb2Bpst e x p - ( a + T~t). coordinate, 34 a value of Z~t = 3.0/sec can be deduced
Zq = f12(1 +a(1 - Z ~ t ) ) M r for the stable methane flame with a s = 100/sec. Since
(3.5) quenching occurs at aq = 320/sec and a shift away
from Zst is to be observed, 34 this agrees with the
This expression shows the influence of characteristic estimate of Zq ~ 8/sec.
parameters, for instance a dependence on Z~t, but it
does not allow one to calculate Zq, since the frequency
factor, B, and the activation energy, E, are not known. 4. STATISTICSOF DIFFUSION FLAMELETSIN
TURBULENT FLOWS
Also, the effects of radiation, 73 differential diffusion 29
and reverse reactions 75 would change the asymptotic If the approximations discussed in Sections 2 and 3
result by factors of order one. Therefore another are acceptable, the flamelet depends only on two
approach to determine Zq was proposed. 23 It consists parameters: Z and Zst- In a turbulent flow field these
of analysing experimental data of counter flow dif- parameters are statistically distributed. To predict
fusion flames. Such an analysis based on Tsuji and non-equilibrium effects in turbulent diffusion flames,
Yamaoka's data 81 yields a value of Zq = 7.8/sec for it is therefore necessary to predict the joint distribu-
methane using the approximate formula (2.38). Simi- tion function of Z and Zst. In this chapter we will
larly, a value of Z0 ~ 9.7/sec can be derived for present some known properties of the joint proba-
p r o p a n e - a i r flames. Recent data on extinction of bility density function (pdf) of Z and Zst and propose
332 N. PETERS

methods to predict it. We will also discuss conse- between Z and ;(. The dissipation rate is found to be
quences of the statistical description related to flame approximately lognormal with a Z-dependence of the
lift-off and blow-off based on percolation theory. mean value that can be derived on the basis of Eqs
(2.24) and (2.26). The mixing layer ensemble can be
expected to represent the early part of a jet, where )~
4.1. Joint Statistics of the Conserved Scalar and Scalar
and Z would be statistically dependent. This is con-
Dissipation
sistent with the results of Ref. 85.
Using Bayes' theorem the joint pdf of Z and Z can
be written 4.1.1. Conserved scalar pdf models
Since prediction methods for turbulent flows are
Pzx(Z,z) = Pz(Z)Pz(zlZ). (4.1)
generally based on moments rather than on the pdf
Here Pz (Z) is the marginal distribution itself, a convenient method to determine the pdf is to
assume an n-parameter function and to relate the first
Pz (Z) = f o pzz (Z, Z) d?z (4.2) n moments to these parameters. As Z is bounded
between 0 and 1, the choice is reduced to a small
while P~(zIZ) is the conditioned pdf of Z for a fixed number of physically realistic functions. Richardson et
value of Z. Since it is more convenient to use Favre- al. 8v were the first to use a beta-function distribution,
averaged statistics than conventional time-averages Spalding88 used a sinusoidal pdf, Lockwood and
in turbulent combustion,1 we specify the pdf's by a Naguib 89 a "clipped Gauss" distribution and Rhodes
tilde as Favre-probability-density functions. We will and Harsha 9° a triangular pdf. The beta-function
denote the conditioned pdf at Z = Z~t by distribution has been most widely used in recent
years. 6'91'92 It has the advantage that its two
Px(Zst) = P,(zlZ = zst). (4.3) parameters can be related algebraically to the first two
If z and g were statistically independent, (4.1) would moments. It has the disadvantage that it cannot
reduce to approximate bimodal pdfs which are frequently ob-
served in intermittent free shear flows. Pope 93 has
/3zz (Z, Z) = Pz (Z)Px (Z) (4.4) determined the statistically-most-likely pdf and con-
where cludes that at least three moments are needed to
represent a number of experimentally observed scalar
Cl
pdfs.
Pz (z) = J0 Pz~ (z, z) dZ (4.5)
A characteristic feature of the scalar pdf is the
is the marginal distribution. Then the joint pdf can be appearance of an intermittency spike in the outer part
predicted by using the properties of Pz (Z) and Px O0 of free shear flows. The bimodal structure of the pdf in
to be discussed below, this region is therefore essentially due to contributions
The assumption of statistical independence, how- from the fully turbulent part of the flow and from the
ever, remains questionable. Bilger2 has argued in intermittent outer flow. These two are separated by a
favour of such an assumption. Meyers and O'Briena4 transition layer that has been called the viscous super-
studied the evolution of the joint pdf of Z and Z. They layer by Corrsin and Kistler. 94 In the early part of the
found that the turbulent transport term introduces jet flame most of the combustion is expected to take
weak statistical dependence between Z and g at place within this superlayer. Recently, a composite
moderate turbulent Reynolds numbers. In Ref. 85 a model has been developed that takes the three parts
pdf transport equation for Pz (Z) has been used to separately into account. 95 An evaluation of the scalar
calculate the conditioned mean pdf data by La Rue and Libby96 shows an un-
expectedly large contribution from the superlayer,
indicating that an important part of the scalar field is
;z = f 0 Z/3z(xIZ)dz (4.6) contained in regions with large local gradients. This is
consistent with Kolmogorov's third hypothesis, 97'98
on the basis of an a priori assumption about Pz(Z) in which states that the small-scale structures of turbul-
a round turbulent methane jet. It was found that the ence become less and less space filling as the scale size
result was insensitive to the choice of Pz(Z). The decreases. A simple dynamical model called the
comparison between the conditioned mean at fl-model, that gives a plausible description of the
2 = Zst = 0.055 and the unconditioned mean shows theory, was developed by Frisch et al. 99
fairly large differences at x/d = 10 and 20 but good
agreement further downstream. 4.1.2. Unconditioned scalar dissipation pdf models
However, all these evaluations rely on statistical Kolmogorov's third hypothesis can be extended to
assumptions about other quantities. A more direct scalar fields and provides a first guess about the shape
calculation of a turbulent mixing layer developing in of the scalar dissipation pdf. It then states that Z is
time was recently performed by Ashurst et al. 86 using lognormally distributed. Lognormality of a scalar was
the discrete vortex method combined with a very tested by Massiello 1°° on the center line of a round jet
accurate finite difference calculation of the scalar field. at x / d = 50 (cf. Gibson and Masiellol°l), and by
Their results show a strong statistical dependence Sreenivasan et al. 1°2 and Antonia and Sreenivasanm3
Laminar diffusionflameletmodels 333

in the inner part of a turbulent boundary layer. It was convenient to choose Z~t and ~q which are fixed con-
found that the distribution of g is close to lognormal stants rather than Zmaxand Zq,max which vary with Z.
even at relatively small Reynolds numbers. Recent
numerical calculations by Kerstein and Ashurst ~°4
4.3. Introduction of Percolation Theory
also confirm the lognormality assumption of the
scalar and show that it is insensitive to certain The probability Pb measures the ability of flamelets
assumptions about the flow field. One may therefore to burn, if an ignition source is available. This is not
write evident in an inhomogeneous turbulent flow field. If,
for instance, a flamelet has been quenched locally by a
P(Z) = Z a ~ exp - (ln Z-/~)2 (4.7) temporary value Zst > Zq and it is carried away from
the turbulent flame brush, it will not re-ignite when
the instantaneous scalar dissipation rate decreases
where the parameters ~ and a are related to the first
below Zq again. Also there may be flamelets that were
and second moment of Z by
not yet reached by an ignition source and stay
)~ = exp (# +½a2) unignited. Even within the turbulent flame brush there
(4.8)
= ~2 (exp a z - 1). may be burnable yet unignited clusters of flamelets
that are not connected to the burning flamelets. A
Therefore the pdf of g is known if Z and a are calcu-
theory that is able to account for such a situation is
lated. In principle, two-equation models of turbulence percolation theory. It has been introduced 23 into
provide the mean, either by relating it to the scalar
combustion theory and has in the following been
fluctuations and the turbulent time scale, g/F, by the applied by Kerstein and Law1°8 to spray combustion.
modelling assumption ~ Kerstein 1°9 has also derived a complementary
~ criterion for burning to that proposed in Ref. 23. We
; = c, e~ (4.7)
will discuss both criteria below.
Percolation theory describes the conduction in ran-
where the common estimate is cz = 2.0, or by deriving domly distributed networks (cf. Kirkpatrick 11°). For
a modelled equation for Z (Borghi and Dutoya, 1°5 example, if two opposite planes are connected by a
Elgobashi and Launder1°6). The variance a can be three-dimensional electric network and an increasing
deduced from Refs 100 and 102. Both find for com- number of connections between adjacent net points is
pletely different flows, for the component of Z in the successively and randomly interrupted, a threshold is
flow direction a value ofa~ ~ 4.0, while in Ref. 102 the finally reached, beyond which no current flows
sum of three components yields ~r2 = 2.0. This value through the network in the statistical average. This
certainly presents only a first guess which may be "percolation" threshold lies around a critical prob-
expected to he valid in the fully turbulent part of shear ability of Pc = Pcrit = 0.25 for the number of con-
flows. In the intermittent parts of free shear flows ducting bonds. If the network is two-dimensional, the
substantial changes of a and of Z from (4.7) may be probability Pcrit is around 0.5. The first criterion to be
expected. The influence of large coherent structures, discussed is related to local quenching of diffusion
which are not predicted by two-equation models of flamelets. We may view the surface of stoichiometric
turbulence, may also affect the scalar field consider- mixture in a turbulent diffusion flame as a two-dimen-
ably? °7 sional system. Local quenching events due to Zst > gq
correspond to holes, that have been punched ran-
domly into the surface. Such a system has been studied
experimentally by Last and Thouless 111 using con-
4.2. The Fraction of Burnable Flamelets
ducting graphite paper. They find conduction to drop
From the discussion in Section 3 we know that to zero if the fraction of the remaining surface reaches
laminar flamelets are extinguished, if the instan- Pcrit= 0.62. More recent theoretical work ~12 shows
taneous scalar dissipation rate exceeds the quenching that Pcrit should be around 0.718. By analogy it follows
value, Zq- We may therefore calculate the fraction of that flame propagation along the surface of stoichio-
burnable flamelets as the probability that Zst < AVq metric mixture will only be possible if the fraction of
burnable flamelets Pb exceeds Pcrit- However, percola-
Pb = t~ q Pz (Zst) dZst tion theory considers in general, homogeneous
systems at rest. In a turbulent flow field where the
mean flow velocity may be directed in an opposite
l lerf(!nzq/;~t+½as2t.~ (4.8)
, / direction to flame propagation, this corresponds to
the limit of an infinite propagation velocity. Since this
If statistical independence was assumed, the choice of is apparently not the case in diffusion flames, propaga-
Zq,max (evaluated at Z m a x rather than Zst as proposed tion against the mean flow direction, say xa, takes
in Ref. 31 would influence the result. However, the place only if the local velocity va does not exceed the
numerical results of Ref. 86 indicate a comparable x~-component ul of the local flame velocity vector,
shift of the mean value Zz as Z increases, as the shift of directed opposite to v1. At the surface of stoichio-
Zmax. Also for mathematical reasons it seems more metric mixture such events would have the same effect
334 N. PETERS

as local quenching events: those parts of the surface flame in Fig. 11. The general behaviour of Pb, Pu and Pc
which are advected downstream at too large a velocity can be estimated from the mean values in the jet. On
may be interpreted as interruptions of the network. To the centreline the mean scalar dissipation rate in-
account for this effect, a conditioned joint probability creases after the potential core, to a maximum around
density of Z, va and u 1 has been discussed in Ref. 23. x/d ~ 10 and decays proportionally to (x/d) 4 in the
Shortly, the analogy between flame propagation in similarity region. 85 Therefore Pb increases to one
non-premixed systems and percolation theory leads, according to (4.8) as Z and similarly .~st decreases. As
under certain rough assumptions, to the condition the mean velocity vl also decreases, but proportion-
that the critical value must be less than the product of ally to (x/d) 1, the probability pu is expected to show a
Pb and Pu similar behaviour. The mean value of the mixture
fraction stays constant in the potential core of the jet
Pb, =- PbPu< Pcrit,2D 0.718 = (4.9) and decays as (x/d)-~ in the similarity region. There-
where pu describes the probability that the local flame fore Pc is close to one in the fuel-rich region of the
velocity exceeds the local propagation velocity jet and decays to zero as it passes across the surface
of mean stoichiometric mixture. The condition,
1 1 ~{VF--fl~
P, = ~ + ~ e r l l - - / - (4.10) pb,(X, r ) = 0.718, yields then the dashed line in Fig. 11
\ c% / while the conditions, Pc = 0.25 and Pc = 0.75, lead to
The other criterion, derived by Kerstein a°9 con- the solid lines. The burning region of the flame is given
siders the degree of connectedness of the surface of by the intersection of the three curves. It is seen that
stoichiometric mixture. Here the system is considered the stabilization height, H, is essentially determined
as an ensemble of three-dimensional subsystems. If a by the criterion related to local quenching of diffusion
randomly-defined subsystem is internally connected it flamelets while most of the remaining flame envelope
is said to "percolate". All percolating subsystems are is determined by the criterion related to connected-
called the "medium", all non-percolating subsystems ness. The theoretical flame length, Lst, is defined by
the "void". It is shown that the surface of stoichio- the point on the axis where Z = Z~t.
metric mixture is the boundary of the medium and Within the burning region, Pb, and Pc are not equal
also the boundary of the void. If either the medium or to one and we therefore expect clusters of burnable
the void are disconnected, then their mutual but unignited flamelets to remain in this region. This
boundary, the surface of stoichiometric mixture, is effect is enhanced when the flow velocity is increased
disconnected. It follows from Ref. 109 that the prob- and the stabilization height shifts downstream. The
ability of connectedness Pc can be defined as the lowering of the mean temperature in the burning
volume fraction of the region where Z < Z~t region acts upon the density and mixture fraction
field, leading to a lower theoretical flame length. Thus,
j
Pc "= .z~,
o P(Z) dZ. (4.11) the burning region shifts upstream. Blow-off of the
entire flame will occur, if the remaining burning region
The system percolates if becomes the size of a large coherent structure that
carries it downstream. This blow-off mechanism has
Pc > Pcrit,3D = 0.25 (4.12) been postulated in Ref. 113. Other influences may be
and, due to symmetry between medium and void, if due to the finite size of the percolating region com-
also pared to the finite size of the "holes".

1 -Pc > Pcrit,3D,Pc < 0.75. (4.13)


5. APPLICATIONOF NON-EQUILIBRIUMFLAMELET
The first condition would hold for mixtures which are MODELSTO TURBULENTDIFFUSIONFLAMES
fuel lean in the average, while the second condition
would hold for fuel-rich mixtures. The present definition of non-equilibrium diffusion
Equations (4.9), (4.12) and (4.13) can be used to flamelets implies the use of the mixture fraction and
construct the envelope of the burning part of a the instantaneous scalar dissipation rate to describe
diffusion flame. This is schematically shown for a jet the flamelet structure. This formulation is very recent
and the author knows only two attempts to apply it:
H Lst L one is the work by Liew 6° who uses numerically
calculated non-equilibrium flamelets and the other is
a series of works on lift-off characteristics of diffusion
°'<-....~
• \
flames.a 13,85,83

5.1. Liew's Work


In Section 7 of his thesis, Liew 6° uses the two steady
states of a diffusion flamelet discussed in paragraph
/ " ~ Z = ~ Burning 2.2 to split the Favre average of a scalar q5defined by
region
FIG. 11. The burning region of a liftedjet flame constructed ~= ff fo~PZ,(Z,z)dzdZ (5.1)
with conditions from percolation theory.
Laminar diffusionflameletmodels 335

into a burning phase F and a non-burning phase I by turbulent diffusion flame as if it occurred in a tur-
assuming that ~bis independent of Z within each phase. bulent premixed flame. A characteristic of premixed
With ~bv(Z) and ~bl(Z) given, it follows by integration flames is the existence of a flame velocity at which the
of (5.1) over Z from 0 to ~(qand from Xqto ~ that flame propagates with respect to the unburnt mixture.
In the diffusion flame, mixing is considered to occur
= Pb~)F + (1 --Pb)~' (5.2)
prior to the onset of combustion, and the base of the
where diffusion flame is assumed to be stabilized by propa-
gation ofa premixed flame into the mixture.
~F = f £ C~FP(Z)dZ Recent experimental investigations by Hall et al. 119
and Gfinther et al. 12° follow this concept and deter-
and (5.3) mine the turbulent flame velocity as a function of the
local turbulent Reynolds number. They find the same
~, = f~ q~FP(Z)dZ. linear dependence on the turbulent Reynolds number
as Andrews et al., t2' but a proportionality coefficient
Similar definitions are derived for the second that is only half the one found in premixed flames.
moment of q~. He uses Zmax instead of Zst in the This seems to indicate that mixing has not occurred
definition of Pb and the assumption of statistical inde- down to the molecular level. In Ref. 113 the time
pendence between Z and Z. He also reviews experi- required for the turbulent mixing of a fluid element to
mental data on •, calculates it with (4.7) on the basis of approach local uniformity was estimated. It was con-
a ~'-gmodel and estimates a 2 = 1.15 from Ref. 101. He cluded that a sufficient amount of premixing at the
shows that the results are not sensitive to the value of molecular scale seems unlikely to justify the use of the
a z. He uses a beta-function model for the conserved premixed-flame concept.
scalar pdf and varies Zq.... between 20/sec and 60/sec. The question whether premixed flame propagation
Solving the turbulent flow field equations numeri- or diffusion flamelet quenching is the correct physical
cally he compares mean velocity and scalar calcula- description of the stabilization mechanism has again
tions (the latter based on (5.2)) with recent experi- been investigated.76 It was found that the answer
mental work by Hassan et al., 54 E1 Banhawy et al., x ~ depends on the variance of the mixture field around
Lockwood and Moneib 115 and Lenze and Zst as well as on the scalar dissipation rate. An
Gtinther.116 He finds fair agreement for velocity, CH4, essential concept in the analysis is the freezing of the
CO and temperature profiles and a weak sensitivity of reaction at sufficiently low adiabatic flame tempera-
these results on Z0,max" However, the challenging tures. The relation between freezing and premixed
feature in the experiments in Refs 54 and 116 is the burning has been established# 9
occurrence of 02 on the axis of the flame. Lenze and Assume the instantaneous mixture fraction field to
Giinther had stabilized their flame with oxygen from be given locally. Two traverses through the flow field
an annulus surrounding the fuel jet while Hassan, and the corresponding adiabatic temperature profiles
Lockwood and Moneib used hydrogen as stabilizer. are shown schematically in Fig. 12. In both cases the
In both cases the flame would have lifted if it had not same Favre mean value of ~ Z - ~ and there~fore the
been stabilized. This indicates that the scalar dissi- same mean ~st is assumed, but the variance, Zs{2, of the
pation rate around x/d = 10-20 was large enough to mixture fraction around stoichiometric is different.
provide local quenching events which would allow O z For large excursions from Zst the corresponding
to traverse the surface of stoichiometric mixture and adiabatic flame temperature drops below the rich
reach the axis. Liew 6° predicts a strong oxygen peak and/or the lean freezing temperature, such that the
with a maximum of around 3 ~o on the axis between reaction zones are separated and individual diffusion
x/d = 10-20 where Pb is small. The predicted peak is flamelets may exist. On the other hand, this is less
stronger than in the experiment and does not extend
down to x/d ~ 80 as the experiment does. Liew 6°
attributes the difference to unsteady post-extinction
effects and discusses the necessity and numerical
implications of a Lagrangian approach. Another and
still Eulerian approach would be the use of percola-
tion theory.

5.2. Prediction and Experiments on Stabilization


ZsIt~-
Heights of Lifted Turbulent Jet Flames
The theory of local quenching of diffusion flamelets
was used in Ref. 113 and subsequently in Ref. 85, to
predict stabilization heights of lifted jet flames. The
approach is an alternative concept to the popular view
(cf. Vanquickenborne and van Tiggelen,~17 Brzustow- FIG. 12. Schematic representation of mixture fraction pro-
ski la 8) which treats the stabilization mechanism in a files and the corresponding adiabatic flame temperature.
JPECS I0:3-C*
336 N. PETERS

~
z,,2 comparison, three different methods were employed
,min=T c for taking into account the radial position at which X
is to be evaluated. The differences between the
resulting curves illustrates the uncertainty involved in
seporofed defining the average scalar dissipation rate appropri-
diffusion flome[efs
ately.
A more precise calculation of the average scalar
dissipation rate was performed in Ref. 85 using a pdf
transport equation (cf. paragraph 4.1). A ~-g model
was used to calculate 7~,t without the assumption of
floraepropogofion statistical independence. The comparison between
measured stabilization heights for natural gas by
log Xsf ~ )(q Horch ~23 showed good agreement for small lift-off
heights but discrepancies for values H i d > 15. The
FIG. 13. Schematic representation of regions of premixed reason for these discrepancies was sought in the in-
flame propagation and separated diffusionflamelets.
homogeneity of the turbulent flow. It was argued that
instantaneous peaks of the scalar dissipation rate that
likely to occur for the small variance case in the right arise during the merging process of large coherent
hand part of Fig. 12. The reaction zone is connected structures could influence local quenching events in a
and a premixed flame may travel through the slightly way that cannot be represented by an average scalar
inhomogeneous mixture. If the mixture fraction dissipation rate.
gradient is larger than the assumed value, ;~t increases To investigate the discrepancies between theory
and the Damk6hler number decreases resulting in and experiments further, measurements of stabil-
higher freezing temperatures. Then freezing would ization heights in round methane-air jet flames
occar even at smaller variances. Finally, when )~t is of diluted with nitrogen were performed, s3 Flow condi-
the order of the quenching value of diffusion flamelets, tions were varied using nozzle diameters between 2
Zq, a small but finite variance Z ~ exists for which and 10 mm and exit velocities ranging up to 140 m/sec.
freezing events become unlikely. This is schematically It was shown that some of the differences found s5
shown in Fig. 13 where the curve, Tad,mi~ = T~, which were simply due to the fact that the natural gas used
equates the minimum adiabatic temperatures and the by Horch ~23 contained about 15% nitrogen which
corresponding freezing temperatures of Fig. 12, reduces the residence time d/u o at quenching by a
separates the regions of premixed flame propagation factor of about 2. In Fig. 14 theoretical and experi-
and diffusion flamelets. With respect to the contro- mental values of the non-dimensionaldissipation rate,
versy about lift-off in turbulent jet diffusion flames, it Z * = zd/uo, are plotted over the non-dimensional
is important to realize that both, Z~t and ~77, are large stabilization height H/d. The measured stabilization
at about x / d = 10 and decrease subsequently. There- heights are, however, still larger than predicted by the
fore the diffusion flamelet description seems to be theory. The more recent theory v6 has shown that
valid for an initially unpremixed jet into air. The more partial premixing makes the flamelet more sensitive to
detailed analysis shows that the R.M.S. fluctuation of flame stretch. The remaining discrepancies can there-
the mixture fraction around stoichiometric, needs to fore also be explained by premixing.
be less than about 10% for premixed flame propaga- The main aim in Ref. 83 was, however, to check the
tion. Otherwise local quenching occurs in the diffusion
t 7
flame regime.
Equation (4.8) has been used in the limit of ~i"
Zst=O0.5B
Z* x°2
~r----~0 ~13,85 to obtain the simplified stabilization con- -I • o2~o
- o 0 205
dition 5 ~L • o 200
~1 • o79s
)~st = Zq (5.4) 9, o ~ ,o
&

which is independent of Pcrit. It can be shown that the • ° 0 175

error induced by this approximation is small for 3 _ v o 17o

~\ + 0 210 V a n q u ; c k e n b o r n e /
cr < 0.5. Since Kolmogorov's third hypothesis predicts
2
a decrease of czwith increasing size of the volume over
• Ii+
which the average is taken, a volume average of Z~t 1
was used in Ref. 85 instead of the local value.
The order of magnitude of the average scalar dissi- 0
10 20 30 z,o 50
pation rate was calculated ~3 on the basis of a Hid
similarity solution for a turbulent round jet with
variable density. S~ The influence of intermittency was FIG. 14. Non-dimensional stabilization heights H/d as a
estimated on the basis of Wygnanski and Fiedler's ~22 function of the non-dimensional dissipation rate--~* =
zd/u o theoretical curve assuming statistical independence;
experimental data and statistical independence dashed area: statistical independence, both from Ref. 85;
between Z and Z was assumed. For the purpose of data points: Y.* Zqd/u measured in Ref. 83.
=
Laminar diffusion flamelet models
337

basic property of the laminar flamelet concept: the use flamelets. This was treated by introducing percolation
of laminar non-equilibrium data in turbulent diffusion theory. This area clearly needs further investigation. It
flames. Experimental residence times in the turbulent is likely that some aspects of percolation theory, which
flames were scaled with Zq-values derived from are already known to specialists, could improve our
laminar counterflow experiments 52 (cf. paragraph understanding of cluster burning in diffusion flames.
3.4). This made the curves for different dilution and In summary, the author believes that the laminar
different residence times collapse into one curve with, flamelet concept is a promising tool in studying non-
however, considerable experimental scatter. The equilibrium effects in turbulent diffusion flames.
scaling was performed for two values of Zst, 0.0548
and 0.0697, in order to compare with previous data by
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