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Towards a predictive evaporation model for multi-component hydrocarbon

droplets at all pressure conditions

Article  in  International Journal of Heat and Mass Transfer · July 2011

DOI: 10.1016/j.ijheatmasstransfer.2011.03.031

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 Towards a predictive evaporation model for multi-component

hydrocarbon droplets at all pressure conditions

V. Ebrahimian a and C. Habchi a1

a
IFP, Engine CFD and Simulation Department, Rueil-Malmaison, FRANCE

Abstract

In this paper, a new evaporation model for multi-component hydrocarbon droplets is

proposed. Compared to previously published models, it has two new features. First, an

expression of the Stephan velocity is proposed which ensures gas mass conservation. In

addition, the evaporation rate of each species is obtained by the integration of the exact

equation of species mass fraction. Second, the heat flux due to species diffusion is taken into

account in addition to the classical conduction heat flux between the gas and the liquid

droplets. The comprehensive multi-component droplets vaporization model including the

above two features is presented for high and low pressure conditions, for which a real and a

perfect fluid equation of state (EOS) has been used, respectively. Free convection is also taken

into account using the Grashof number in the Kulmala-Vesala correlations [1] for the

Sherwood and Nusselt numbers. The model is compared with very accurate experimental data

which were recently obtained by Chauveau et al. [2] at atmospheric pressure and temperature

ranges of 473-973K for n-heptane and 548-623K for n-decane droplets of 400 µm initial size.

A very good agreement with the experimental data including micro-gravity conditions has

been obtained. Indeed, the results have confirmed that the free convection process plays a

significant role in the evaporation rate of liquid droplets under earth gravity and quiescent

conditions. This shows the relevance of the new features of the model. The numerical results

1
Corresponding author: e-mail Chawki.HABCHI@ifp.fr, Tel: +33147526151, Fax : +33147527068
have also shown that real fluid EOS is not necessary at atmospheric pressure for the

temperature range given above. In addition, the numerical results of the new model are also

compared with the experimental data of Birouk [3] for two-component droplets of n-heptane

and n-decane with different compositions of the liquid mixture. Finally, the non-ideality of the

mixture is shown to become significant at high ambient pressures and especially at low

ambient temperature conditions where a real-gas EOS is needed.

Keywords: Droplets evaporation; Multi-component model; Stephan velocity; free convection;

complex diffusion.

1 Introduction

Droplet vaporization has intensively been investigated experimentally and numerically

during the past decades. Indeed, this phenomenon is of interest to many fields of engineering

applications. The detailed evaporation of multi-component droplets during the combustion of

fuel sprays in automotive engines or gas turbines is a prominent example. The influence of the

volatility between the numerous components of practical fuels on pollutant emissions still

needs to be understood. Although numerical simulation of the mentioned phenomena has

received a considerable attention in the past, few experimental accurate data are available for

the validation of droplet evaporation models even at atmospheric pressure. Most isolated

droplet evaporation experiments have been conducted with the drop suspended on a support

fiber to avoid the experimental difficulties for free-falling droplets [4-7]. The support fiber

which has a relatively large diameter (more or less 150µm) increases the drop evaporation rate

due to the heat transfer through the fiber to the drop even at low ambient temperatures. Yang

& Wong [8] have studied the effects of heat conduction into the droplets through the fiber and

the liquid-phase absorption of the radiation from the furnace wall on the evaporation rate of

droplets at micro-gravity condition. They found that without considering these effects, there is
a large discrepancy between their theoretical results and the experimental data of Nomura et

al. [4]. More recently, Chauveau et al. [2] studied the effects of fiber diameter and gas

temperature on droplet vaporization. In their experiments, a cross micro-fiber with small

diameter of 14µm is used to reduce the effect of heat conduction on the droplets evaporation

rate. To consider the effect of free convection, Chauveau et al. [2] applied both normal and

micro-gravity conditions to the droplets vaporization.

Droplets vaporization models from the literature such as [9, 10] have compared their

numerical results mainly on the experiments with large sizes of fibers [4-7]. Consequently,

these models have overestimated usually the vaporization rate in order to be close to the

measurements. Moreover, most previous models neglect the heat flux between the gas and the

droplet due to the enthalpy transport by species diffusion during the evaporation process. In

addition, the mass conservation is not rigorously respected when Fick's law is used to model

the diffusion velocity in the mass conservation equation of the gas mixture. Thus, a new

model that could have a better estimation of droplets vaporization is needed. Furthermore, a

real gas equation of state (EOS) have to be used in order to take into account non-ideality

effects for pressure and/or temperature supercritical conditions [11, 12]. In addition, the case

of droplets vaporization under quiescent conditions (i.e. without forced convective velocity)

will be considered. Indeed, the effect of natural convection on the evaporation rate may

become significant in quiescent regions of complex configurations. Noteworthy studies on

natural convection, normal and micro-gravity effects have been performed by some authors

[4, 13-16]. The natural convection effect can be presented in term of the Grashof number. In

fact, the Grashof number plays the same role in natural convection that the Reynolds number

plays in forced convection [17]. To consider the effect of natural convection, Ranz and

Marshall [18] introduced the Grashof number in the definition of Sherwood and Nusselt

numbers. In the present study, the most recent correlation of Kulmala & Vesala [1] is used for
the evaluation of Sherwood and Nusselt numbers with consideration of natural convection

effect.

This paper is organized as follows. In Section 2, a general multi-component droplet

evaporation model is proposed which takes into account a modified Stephan velocity and

enthalpy diffusion of gaseous species to compute the evaporation rate. In Section 3, the

numerical results of a single-component isolated drop are compared with the experimental

data of Chauveau et al. [2] and Yuen and Chen [19]. Results for the vaporization of droplets

in normal and micro-gravity environments at various temperatures are expressed as a function

of droplets diameter. The effects of high pressure and fluid ideality on vaporization are also

investigated in Section 3.2 using the real and ideal gas EOS. The experimental data of

Nomura et al. [4] at high pressure conditions have not been used in this paper because of the

uncertainty of the experiments mentioned above. To our knowledge, few experimental data

exist for the evaporation of multi-component droplets. In section 3.3, the numerical results are

compared with the experimental data of Birouk [3] in the case of a two-component droplets

vaporization.

2 Multi-component Droplet Evaporation Model

The droplet evaporation models are generally based on the conservation equations of

mass, momentum and energy. In the basic conservation equation of species ( see Equation

(2.1)), the total convective velocity includes a first component u, usually called Stefan

velocity and a second component Vi, called the diffusion velocity of species i. This last may

result from the pressure gradients (i.e. pressure diffusion), the temperature gradients (i.e. Soret

effect), the external force fields (i.e. forced diffusion) and the concentration gradients (i.e.

ordinary diffusion). The mass conservation equation of gas mixture is conserved by diffusive

mass flux which is commonly approximated by Fick's law. In this case, the effects of pressure

diffusion and Soret effects are usually assumed to be small [20-22], although, sometimes the
effects of Soret may be significant [11, 23]. A general expression for the determination of the

diffusion velocity is proposed by Williams [24] which is very complex and costly, especially

for multi-species gas. A simplified expression for the diffusion velocity in multi-species gas

has been already presented by Hirschfelder et al. [25] which neglects the pressure gradients

and volume forces. Using Hirschfelder's law reduces the complexity of the exact resolution of

Vi; but, it does not recover the mass conservation equation of the gas mixture. To overcome

this problem, an additional term is suggested by some authors [20, 26] to ensure gas mass

conservation equation. Similarly, a modified Stephan velocity which ensures the mass

conservation of gas mixture is derived below for the droplets vaporization modeling

considering Hirschfelder's law. The model uses spherical droplet hypothesis with no

interaction between droplets. The effects of radiation, Soret and Dufour are neglected and

there is no chemical reaction in the gaseous environment. The one-third rule is used for the

properties of the gaseous mixture in the film region around the droplet [27]. Gas phase quasi-

steadiness and isobaric assumptions are applied to the model. The discrete fluid method is

used for multi-component droplet which resolves the continuity equation for all droplet

components. The droplet temperature is assumed to be uniform during all the process of

evaporation (i.e. the infinite thermal conductivity assumption is invoked). The last hypothesis

gives an average temperature in the droplet which is different from the real surface

temperature. Some methods have been presented to evaluate the temperature profile in

droplets [22, 28]. Nevertheless, temperature uniformity is a reasonable assumption, at least for

small droplets for which the heating period is short. Liquid species mass fraction in liquid

phase is time dependent; but there is no species diffusion in the liquid phase. The components

mass fraction in the liquid phase assumed to be constant in all parts of the droplet (i.e. there is

no liquid component mass fraction profile inside the droplet). However, there are some
valuable works which consider the species diffusion in the liquid phase [29, 30] and

consequently the profile of liquid components mass fraction inside the liquid phase.

The resulting governing equations for the model consist of the two phase flow equations

for the gas and liquid phases along with the thermodynamic equilibrium condition at the

liquid-gas interface.

2.1 Gas phase governing equations

Mass conservation equation of the species is expressed as

∂ρ g Yi
+ ∇. ( ρ g Yi ( u + Vi ) ) = 0 (2.1)
∂t

where u and g are the velocity and density of the gas mixture and Yi and Vi are the mass

fraction and diffusion velocity of species i respectively. Summation of Equation (2.1) over all

gas species N gives the mass conservation equation:

∂ρ g
+ ∇. ( ρ g u ) = 0 (2.2)
∂t

The internal energy conservation equation for the gas phase is:

∂ρ g I
+ ∇. ( ρ g uI ) = −∇.J + σ : ∇u − P∇.u (2.3)
∂t

where σ : ∇u represents the heat production due to the shear stress, σ , and P∇.u is the

compressibility effect. These two terms are neglected in the present study. J represents the

heat flux vector. It includes the contributions due to heat conduction and enthalpy diffusion

and may be written as follows:

J = −λg ∇T + ρ g hi (YV
i i) (2.4)
i

where g is the thermal conduction coefficient of the gas mixture in the film region (Figure 1),

T the gas temperature and hi the specific enthalpy of species i .

2.2 Liquid phase balance equation

As discussed above, droplet surface temperature is assumed to be equal to the mean

temperature of the droplet (Ts=Td). The energy conservation equation for the two phase

system consisting of the droplet and the surrounding gas mixture gives the change of liquid

droplet energy as:

dTd
md C pf = Ql (2.5)
dt

where md is the droplet mass, Cpf is the specific heat of liquid at constant pressure, Td is the

temperature of the droplet and Ql is the heat penetrating into the liquid phase. According to

Figure 1, the energy balance at the liquid surface could be written as:

Ql = Qg − mLv , g (2.6)

where Qg is the heat flux from the gas to the liquid (Qg = J.A), and A is the droplet surface

area. m and Lv , g are the total evaporation mass flow rate and latent heat of the evaporated

species mixture, respectively. Since the real gas EOS is applied to gas mixture, Lv , g is a

function of (P,T). However, Lv , g is only a function of temperature in case of ideal gas EOS

assumption.

2.3 Vapor-Liquid Equilibrium

The evaporation of droplet consists of resolving two phase flow equations as well as

satisfying the thermodynamic equilibrium condition at the liquid-gas interface. This

equilibrium is based on the assumption that at the liquid-gas interface, the chemical potential

for liquid and gas phases are equal for each species i. At low pressure conditions, ideal gas

hypothesis with the ideal gas EOS seems to be a good assumption. In this condition, the ideal

solution could be said to follow the Raoult's law [31]. However, at high pressure conditions

and particularly in supercritical conditions, the gaseous species do not follow the ideal gas

behavior and the effects on some parameters like transport and physical properties variation,
gas solubility increase into the liquid phase and thermodynamics’ non-ideality should be

taken into account for the liquid-vapor equilibrium.

In this study, both ideal and real gases EOS are evaluated. They are used especially to

determine the mass fraction of gas species at droplets surface as well as latent heat of

vaporization. The complete procedure is presented in Appendix B for a well-known cubic

Peng-Robinson (PR) EOS [32].

2.4 Mass flow rate

Based on the previous works, some authors [9, 10] have considered the gaseous

boundary layer around the droplet to evaluate heat and mass fluxes. These models give the

instantaneous droplet vaporization rate from the integration of the quasi-steady species

balance around the droplet. By definition [26], the diffusion velocity in Equation (2.1) has to

obey to the following constraint:

i i =0
YV (2.7)
i =1

Furthermore, the sum of mass fractions must be unity:

N
Yi = 1 (2.8)
i =1

Considering Equations (2.1) and (2.8), there are N unknowns (Yi) with N+1 equations. Thus,

the system is over determined. However, if all species of Equation (2.1) are added and the

identity of Equation (2.7) is used, the mass conservation equation (Equation (2.2)) is

recovered:

∂ρ g N
+ ∇. ( ρ g u ) = −∇. ρ g i i =0
YV (2.9)
∂t i =1

Solving the above equation with the general diffusion velocity is too complex and most codes

use Hirschfelder's law [25, 33] in the following form:

Vi X i = − Dig ∇ ( X i ) (2.10)
where X is the mole fraction of species i and Dig the diffusion coefficient of species i into the

gas mixture. In the present study, the above Hirschfelder's law will be used in the form of

mass fraction to be compatible with the model. Using the following relation between the mole

fraction and mass fraction of species i :

W
X i = Yi (2.11)
Wi

one obtains the Hirschfelder's law in the form of mass fraction of species i as:

N
Xk
ViYi = − Dig 1 − X i + Yi ∇ ( Yi ) (2.12)
k =1 Yk
k ≠i

Using the Hirschfelder's law, the summation of Equation (2.1) over the N gaseous species

gives the global mass conservation equation as:

∂ρ g N N
Xk
+ ∇. ( ρ g u ) = ∇ ρ g Dig 1 − X i + Yi ∇ ( Yi ) (2.13)
∂t i =1 k =1 Yk
k ≠i

where the right hand side of the above equation is not zero, unless the diffusion coefficients

Dig are assumed to have the same value for all the species (this is the case of the KIVA code

[34] for instance). Thus, the global mass conservation may not be ensured. One method to

implement Hirschfelder's law with different diffusion coefficients while maintaining global

mass conservation is to add a correction velocity uc [26] to the absolute velocity in the species

Equation (2.1):

∂ρ g Yi
( ) Xk
N
+ ∇. ρ g Yi ( u + u c ) = ∇ ρ g Dig 1 − X i + Yi ∇ (Yi ) (2.14)
∂t k =1 Yk
k ≠i

If all species equations are summed, the mass conservation equation must be recovered:
∂ρ g N N
Xk
+ ∇. ( ρ g u ) = ∇ ρ g Dig 1 − X i + Yi ∇ (Yi ) − ρ g u c = 0 (2.15)
∂t i =1 k =1 Yk
k ≠i

Thus,

N N
Xk
uc = Dig 1 − X i + Yi ∇ (Yi ) (2.16)
i =1 k =1 Yk
k ≠i

Assuming quasi-steady evaporation and integrating Equation (2.15) for liquid species leads to

the mean droplet vaporization rate:

Nl
m= mi = 4π rd2 ρ g u (2.17)
i =1

where rd is the droplet radius. Integrating Equation (2.14) for liquid species between the

droplet surface at rd and infinity where:

∂Yi
Yi = Yi ∞ , u∞ = u∞c = 0 , =0 (2.18)
∂r r =∞

gives the following relation for the mass evaporation rate:

Dig N
X ks ∂Yi
mi = 4π rd2 ρ g Yi s u + u c − 1 − X is + Yi s (2.19)
Yi s k =1 Yks ∂r
k ≠i
r = rs

Substituting Equations (2.16) and (2.17) into Equation (2.19) gives:

mi = mYi s + 2π rd ρ g ×

N
X ks Nl N
X as (2.20)
i( i i ) Shk (Yks − Yk∞ )
∞
Dig 1 − X is + Yi s s
Sh Y s
− Y − Yi
s
Dkg 1 − X s
k + Yk
s
s
k =1 Yk k =1 a =1 Ya
k ≠i a≠k

In the above equation, Nl is the total number of liquid components, Yis and Yi are the mass

fraction of component i at the droplet surface and at infinity respectively. The dimensionless

Sherwood number is defined as the mass fraction gradient at the droplet surface over the

average mass fraction gradient:

 ∂Yi
2rd
∂r r = rd
Shi = − ∞
(2.21)
Yi − Y
s
i

To consider the effect of natural convection due to volume forces such as gravity, the

following relation is used for the Sherwood number:

( ( ))
1/ 2
Shi = 2.0009 + 0.514 max Rei , max ( Gri , 0 )
1/2
Sci1/3 (2.22)

with

ρig rd2Vrel µig 8 g 0 rd (T − Td ) 3 ∞

Rei = , Sci = , Gri = (2.23)

µig ρig Dig (ν i∞ ) T ∞
2

where, Vrel is the relative velocity between the gas and droplet, ig, ig and Dig are the dynamic

viscosity, partial density and binary diffusion coefficient of species i in the gas mixture of the

film region, g0 is the gravity acceleration; T and ν i∞ are the gas mixture temperature,

kinematic viscosity of species i at infinity; Td is the droplet temperature and Gri, Rei and Sci

are the Grashof, Reynolds and Schmidt numbers of species i respectively. Hence, the

Sherwood number has different value for different components. The physical parameters in

the film region (with index g) are evaluated at the reference temperature [27]:

Tref = Td + Ar (T ∞ − Td ) (2.24)

where Ar is the averaging parameter. For the one-third rule: Ar=1/3. Equation (2.22) is the

Kulmala-Vesala correlation [1] where the Grashof number is introduced. Summation of

Equation (2.20) over all liquid components, gives the total mass evaporation rate:

Nl Nl Nl
N
X ks N
X as
2π rd ρ g Dig 1 − X is + Yi s Shi (Yi s − Yi ∞ ) − Yi s . Dkg 1 − X ks + Yks Shk (Yks − Yk∞ )
i =1 k =1 Yks i =1 k =1 a =1 Yas
k ≠i a ≠k (2.25)
m= Nl
1− Yi s
i =1

Consequently, from the above Equation (2.25) and Equation (2.17), the Stephan velocity is

given as:
 Nl Nl Nl
N
X ks N
X as
Dig 1 − X is + Yi s Shi (Yi s − Yi ∞ ) − Yi s . Dkg 1 − X ks + Yks Shk (Yks − Yk∞ )
i =1 k =1 Yks i =1 k =1 a =1 Yas
u=
k ≠i a≠k
(2.26)
Nl
2rd 1 − Yi s
i =1

The total mass evaporation rate could also be obtained from the combination of internal

energy conservation equation of gas mixture (Equation (2.3)) with Equation (2.17). This

approach needs an implicit method that is more difficult and costly.

2.5 Gaseous heat flux

During the evaporation process of a drop, the internal energy of the surrounding gas

changes simultaneously to its composition. The heat flux in the gas phase comprises three

contributions. The first one is the thermal conduction flux usually modeled by a Fourier law;

the second contribution is associated with compositional changes resulting from species

diffusion; and the third contribution is the Dufour effect which is related to concentration

gradients [35, 36]. Although the Dufour effect [11, 37] and enthalpy diffusion [21] have been

shown to be significant, most of the droplet vaporization models in the literature [9, 10]

assumed the heat flux only due to the first contribution thermal conduction. Droplet

evaporation models which do not have an appropriate estimation for the heat flux, can lead to

anomalous temperature gradients and to an over/under-estimation in the drop evaporation

rate. It is shown that Navier-Stokes solvers which incorporate enthalpy diffusion can provide

much more accurate results than without considering this term [20]. Similarly, the Dufour

effect has been neglected in this study. In this case, the heat flux from the gas to the drop is

then assumed to be the sum of the two first contributions where the (YiVi) term in Equation

(2.4) is given by Equation (2.12). Hence, the Equation (2.4) could be rewritten as follows:

Nl N
X ks
Qg = Qconduction − Qenthalpy = 2π rd λg Nu (T ∞ − Td ) − ρ g Dig 1 − X is + Yi s hi Shi (Yi s − Yi ∞ ) (2.27)
i =1 k =1 Yks
k ≠i

where Nu is the dimensionless Nusselt number defined as:

 ∂T
2rd
∂r r = rd
Nu = − ∞
(2.28)
Td − T

Similarly to the Sherwood number, the following correlation is used for the Nusselt

number[1]:

( ( ))
1/ 2
Nu = 2.0009 + 0.514 max Re, max ( Gr , 0 )
1/ 2
Pr1/ 3 (2.29)

where Pr is the Prandtl number defined as:

C pg µ g
Pr = (2.30)
λg

where, Cpg is the specific heat of the gas mixture in the film region at constant pressure.

An iterative method is needed for the implicit procedure of calculating the mass flow

rate, droplet temperature and composition of the liquid and gas mixtures at the liquid-gas

interface and also in the liquid phase. In this work, a Newton iterative method has been used.

A typical iteration is described as follows: From the thermodynamic equilibrium condition

(Equation (5.5) for real gas model and Equation (5.16) for ideal gas model) and with the

initial temperature and composition of the mixture, one can determine the species mass

fraction in the liquid and gas phases. The physical and transport properties of the liquid and

the gas can be obtained from the estimation techniques and mixing rule as recommended by

Reid et al. [31] (see appendix A). From Equations (2.25) and (2.27) one can obtain the total

evaporation mass flow rate and the heat flux from the gas phase to the droplet. The energy

balance at the liquid-gas interface (Equation (2.6)) gives the new droplet temperature. The

variation of droplet radius is evaluated using the droplet mass mdn . The new droplet radius

(exponent n+1) is obtained by mass conservation:

1/ 3

mdn − m.∆t
rdn +1 = (2.31)
4
πρl
3
where t is the time step and l is the droplet density which is assumed to be constant in each

time step. However, the density change of the drop with the temperature is taken into account

using the Rackett correlation [31].

2.6 Single-component isolated droplet evaporation model

In the case of a single-component isolated droplet, the expression for the mass flow rate

(Equation (2.25)) reduces to the following simplified form:

N
X ks
m = 2π rd ρ g Dvg 1 − X vs + Yvs Sh (Yvs − Yv∞ ) (2.32)
k =1 Yks

In addition, in case of binary mixture (for instance: n-heptane (1) and Nitrogen (2)) one has:

N
Xk X X W X
Dvg 1 − X v + Yv = D1g 1 − X 1 + Y1 2 = 2 2 D12 1 − X 1 2 = D12 (2.33)
k =1 Yk Y2 X2 W Y2

which leads to:

m = 2π rd ρ g D12 Sh (Y1s − Y1∞ ) (2.34)

From Equation (2.27), the following expression for the heat flux can be obtained:

Qg = 2π rd λg Nu (T ∞ − Td ) − mhg (2.35)

where hg is the specific enthalpy of the vapor at Tref.

3 Results and discussion

The multi-component droplet evaporation model presented above has been implemented in

IFP-C3D code [38] already including the Abramzon and Sirignano droplet evaporation model

[9] (referred to subsequently as AS-1989).

3.1 Single-component isolated droplet

While there are some works that take into account the convective flow around the droplet

[39-42], we apply this model to a single-component isolated droplet to be able to compare its

results with the most realistic vaporization experiment of an isolated single droplet obtained
recently by Chauveau et al. [2]. The results of the new model are also compared with the

numerical results of the model of Abramzon and Sirignano [9].

An isolated single-component droplet with an initial diameter of 400 m is placed at the

center of a large cube with the dimension of 1.5×1.5×1.5 m3 in order to avoid numerical

border effects. A uniform mesh of 3×3×3 cells is used. There is no air flow in the cube and

the calculation is performed at atmospheric pressure with several ambient temperatures. Table

1 presents different cases studied in this work.

The droplet vaporization phenomenon consists of two main periods; the heating-up

period when heat transfer increases the droplet temperature, and the vaporization period,

when the heat transfer from the gas to the droplet is dedicated to vaporize the droplet. In the

experiment of Chauveau et al. [2], the droplet was initially at room temperature. However, the

droplet surface regression is recorded while it is already heated during the placement of the

droplet inside the heating chamber (i.e furnace). Thus, the exact initial temperature of the

droplet T0 is unknown at the beginning of the measurement procedure. Figure 2 illustrates the

variations of squared dimensionless droplet diameters with time for several initial droplet

temperatures. According to this figure, it is shown that T0 is proportional to the ambient gas

temperature T . As shown in Table 1, at low temperature T = 473 K, T0 seems to be

unaffected by the heater. However, T0 reaches a temperature up to 340 K when the ambient

temperature is 973 K. Furthermore, it is important to notice that the evaporation rate is

identical for all curves depicted in Figure 2 with the different T0, and is very close to the

experimental results. These numerical results may also indicate that the temperature

uniformity inside the droplet may be considered as an acceptable assumption especially for

high T0 values.

The results of the single-component droplet evaporation are presented in Figure 3 for

n-heptane and in Figure 4 for n-decane droplet for the different gas temperatures given in
Table 1 at normal gravity condition. As discussed in the Introduction, the differences between

the experimental data of Nomura et al. [4] and Chauveau et al. [2] (Figure 3(a) and (b)) are

due to the heat transfer through the fiber to the droplet in the experiments of Nomura et al.

[4]. According to Figure 3 and Figure 4, results of the new model are much more closer to the

experimental results of Chauveau et al. [2] than the results of the AS-1989 model (Abramzon

and Sirignano [9]). In fact, the new Stephan velocity (Equation (2.26)) and the enthalpy

diffusion in Equation (2.4) seem to be two crucial features for the evaporation rate and heat

flux from the gas to the liquid. Also, the results show that at atmospheric pressure and

regardless of the evaporation models, both ideal and real gas assumptions present a similar

behavior. Indeed, the temperature variation (as can be seen in Figure 3 for n-heptane and in

Figure 4 for n-decane droplets) leads to a similar behavior for both real and ideal gas models.

Because of the low computational time of the ideal gas model compared to the real gas model,

it is a good approximation for the thermodynamic equilibrium condition at low pressures for

the range of gas temperature used in this work. However, the deviation from the ideality may

be important for very cold conditions.

At the micro-gravity condition, the natural convection effects are eliminated. Figure 5

shows the vaporization rate constant K, which is introduced as ∂ (d 2 ) / ∂t , as a function of gas

ambient temperature for micro-gravity condition. As can be seen in this Figure, the

vaporization rate K has a quasi-linear evolution with gas temperature. In addition, the new

model has closer numerical results to the experiments than the AS-1989 model. The numerical

results of the calculation for both the normal and micro-gravity conditions are compared in

Figure 6 for two different gas temperatures. At the normal gravity condition, the droplet is

deformed during its lifetime due to the buoyancy force and non-spherical evaporation. The

buoyancy force increases the evaporation rate for both ambient temperatures. The differences
between the two conditions are more obvious in the vaporization period rather than the

droplet heating-up period as shown in Figure 6.

Temperature evolution for n-heptane and n-decane droplets is illustrated in Figure 7.

This temperature represents the average temperature of the droplet which increases from the

initial value up to a constant. Indeed, as for the surface drop regression curves, two different

periods could be distinguished: the heating period, when the temperature of the droplet

increases, and the evaporation period, when the droplet temperature has a constant value

defined as the wet-bulb temperature. According to Figure 7, the droplet temperature is always

less than the saturation temperature of the liquid even at super-critical conditions (Figure 7

(a)). The wet-bulb temperatures obtained at different gas temperatures and at atmospheric

pressure are shown in Figure 8 for n-heptane droplet. These numerical results are compared

with the experimental data of Yuen and Chen [19] for normal gravity condition. They have a

similar behavior as the wet-bulb temperatures obtained from the new model are very close to

the experimental data. Indeed, the maximum deviation from the experimental results is less

than 2%.

Figure 9(a) shows the ratio of conduction heat flux to the enthalpy diffusion heat flux

for n-heptane droplet in the temperature range of 473 K to 973 K. In this Figure, the enthalpy

diffusion heat flux represents 55 to 75% of the conduction heat flux for the mentioned

temperatures. One can obviously conclude that the contribution of the enthalpy heat flux on

the total gas heat flux could not be neglected in a droplet evaporation model.

Figure 9(b) and (c) shows the heat fluxes in the gas and liquid phases. The heat fluxes

due to conduction and enthalpy diffusion of species have not the same behavior in the

heating-up period. Indeed, the heat flux due to conduction reduces as the droplet temperature

increases; whilst, the enthalpy diffusion of species increases as the surface mass fraction of

liquid increases. Since the temperature of the droplet reaches a constant value (at the
beginning of the vaporization period), there is no more heat flux inside the droplet. In this

situation, the heat flux from the gas to the liquid, which is dedicated to vaporize the droplet,

begins to reduce gradually due to the reduction of both conduction heat flux and heat flux due

to the enthalpy diffusion of species. According to Figure 9(b) and (c), in the vaporization

period, the conduction, the enthalpy diffusion and consequently the total gas heat flux

decrease due to the decrease in droplet surface area.

The instantaneous vaporization rate for n-heptane and n-decane droplets at different

ambient temperatures and at atmospheric pressure is illustrated in Figure 10. The vaporization

rate first increases during the heating-up period, when the temperature of the droplet (Figure

7) as well as the mass fraction of liquid at the droplet surface (Figure 9 (b) and (c)) increase,

and then decreases (since the mass fraction and temperature gradients are constant) due to the

decrease in droplet surface area.

Finally, a sensitivity study on the effect of the averaging parameter Ar in Equation (2.24)

on the evaporation rate has been conducted. Two values of Ar (Ar=1/2 and Ar=1/3) have been

tested using n-heptane droplets. The numerical results are shown in Figure 11 (a) and (b) in

terms of evaporation rates and in Figure 11 (c) and (d) in terms of droplet temperatures. For

the high gas temperature case, the best evaporation rate is obtained when the one-third rule

Ar=1/3 is used for determination of properties of gaseous mixture in the film region around

the droplet. On the other hand, at low ambient temperature, the difference between the

numerical results obtained using Ar=1/2 and Ar=1/3 is small.

3.2 Numerical study of the pressure effects on droplet vaporization

Ambient pressure is an important parameter which determines the degree of mixture

ideality. The effects of ambient pressure on n-heptane droplet vaporization are investigated at

sub/super-critical conditions using both ideal and real gas models. The results are presented in

Figure 12 for two ambient temperatures of 473 K and 973 K and for different pressures. It
appears that the ideal gas model is more sensitive to the pressure variations than the real gas

model especially at very high ambient pressures. Comparison of Figure 12 (a) and (b) shows

that the real gas model tends to vaporize the droplet more rapidly. In addition, one can

observe that at super-critical pressure conditions (more than 5 MPa), there is a large

difference between the real and ideal gas models prediction. In this situation the non-ideality

of the fluid becomes significant. At low or sub-critical pressure conditions (e.g., 2 MPa), the

deviation from ideality remains small.

An investigation of the effect of ambient pressure on the droplet temperature is shown

in Figure 12 (c) and (d) for sub and super-critical ambient temperatures respectively. To

satisfy the equilibrium conditions in the deal gas model, the droplet temperature at

supercritical ambient pressures tend to be higher than in the real gas model. This behavior has

also been discussed by Givler and Abraham [43]. As shown in Figure 12 (d), at super-critical

pressures, the temperature of the droplet reaches the critical temperature of the liquid in the

ideal gas model. In fact, this limitation is applied to the model to avoid the temperature of the

droplet to be higher than the critical temperature of the liquid. The temperature limitation

approach is different for the real gas model. As illustrated in Figure 13, liquid temperature for

the real gas model is limited by the dew point line in the phase envelope diagram. The phase

envelope diagram depends on the composition of the mixture which changes at each time

step. In other words, there is not a unique phase envelope diagram for the entire droplet life

time. In Figure 13, phase envelope diagrams have been drawn for four different cases (cases

in Table 2). The mole fractions of each component and the wet-bulb temperatures (given in

Table 2) are obtained at the end of droplet life time. According to Figure 13, the dew point

and consequently the wet-bulb temperature of the droplet increases as the pressure increases

(from 2 to 10 MPa). Still, increasing the pressure from 10 to 15 MPa causes a reduction in the

dew point and subsequently the wet-bulb temperature at 15MPa. This phenomenon is in
accordance with the droplet temperature curves presented in Figure 12 (d). This numerical

study leads to the conclusion that the pressure and the temperature are the parameters that

affect the ideality of the fluid. At high pressure and/or low temperature conditions, different

behaviors of the droplet vaporization are observed with real and ideal gas models.

3.3 Two-component isolated droplet

The model is also compared with the experimental data of Birouk [3] obtained by

evaporating a two-component drop made up of a mixture of n-heptane and n-decane in

nitrogen at a temperature of 293 K and a pressure of 0.1 MPa. In the experiment of Birouk

[3], the droplet is suspended on a vertical quartz fiber with 0.2 mm diameter and the

temperature of the drop is initially of 293 K. The numerical results obtained for the stagnant

condition are presented in Figure 14. A classical distillation is obtained. In the numerical

results, the most volatile component (n-heptane) is first completely depleted followed then by

n-decane. Indeed, in Figure 14 the numerical results show that the evaporation of n-decane

starts later than in the experiment. To explain this behavior, we have introduced a virtual

diameter dn-decane which is proportional to the initial volume fraction of n-decane αn-decane in

the droplet. In Figure 14(a), the value of αn-decane = 0.3 leads to a virtual diameter for n-decane

dn-decane=0.669d0 and (dn-decane/d0)2 0.45. Hence, n-decane should evaporate alone as a

single-component, at least when (d/d0)2 reaches the value of 0.45. Actually, n-decane begins

to evaporate in the same time as n-heptane (at the beginning of the evaporation process) with

less evaporation rate which causes a reduction of the virtual diameter dn-decane. Thus, the

evaporation of n-decane should begin at (d/d0)2<0.45. This behavior is well represented in

Figure 14(a) as well as in Figure 14(b) for the numerical model. This reasoning leads to the

conclusion that the initial volume fraction of n-decane in droplets was probably overestimated

by Birouk [3] in their experiments. A probable scenario may be that a certain fraction of n-

heptane was already evaporated before the beginning of the measurement procedure of Birouk
[3]. Reconsidering Figure 14(a) with a new initial composition of liquid mixture (65% n-

heptane) in the numerical calculation shows closer behavior between the numerical results

and experimental data. In this case, the results of Birouk [3] shows faster evaporation of the

first component (n-heptane) which is due to the effects of heat conduction through the fiber.

As can be seen in Figure 14(c), droplet temperature decreases at the beginning of evaporation

process and then increases to the ambient temperature. In the first part of the temperature

curve (Part 1: which mostly corresponds to the evaporation of n-heptane), the differences

between the droplet temperature and ambient temperature cause the heat flux through the fiber

to be important. Since the second component (n-decane) starts to evaporate, there is not a

considerable temperature difference between the droplet and the ambient gas. Thus, the effect

of conduction heat flux through the fiber is negligible in part 2 (Figure 14(c)). That is why the

slope of the experimental and numerical curves in Figure 14(a) are identical.

4 Conclusion

A new multi-component droplet evaporation model has been suggested. It is based on a

new Stephan velocity which recovers the mass conservation equation when Hirschfelder's law

is used for the diffusion velocity. In addition, the heat flux is assumed to be the summation of

heat conduction and enthalpy diffusion of species. Enthalpy diffusion accounts for energy

changes associated with compositional changes resulting from species diffusion. The

following conclusion are made:

• The numerical results of the new model are in very good agreement with the

experimental results of Chauveau et al. [2] at atmospheric pressure.

• The numerical results have shown that the heat flux due to the enthalpy diffusion of

species could not be neglected in comparison to the conduction heat flux.

• Infinite thermal conductivity assumption inside the droplet which has been invoked in

this study gives acceptable results compared to the experimental results of Chauveau et al. [2].
• The results show that the gravity and consequently, natural convection affects the

droplet evaporation rate for quiescent conditions.

• A sensitivity study on the choice of the averaging parameter has shown that more

satisfying results are obtained with the one-third rule (Ar = 1/3) at sub and super-critical

ambient temperatures.

• At low pressure conditions, the ideal gas model could be a good assumption for the

droplet vaporization in the range of gas temperatures used in this study. However, at high

pressure and/or low temperature conditions, there is a large difference between the real and

ideal gas models. This leads to the conclusion that at high pressure conditions, a real gas

model that could better represents the thermodynamic equilibrium condition is needed.

• The multi-component droplet vaporization model has been applied to a two-

component droplet (n-heptane/n-decane) test case. The numerical results are compared with

the experimental results of Birouk [3]. It is shown that in both numerical model and

experiments, the n-decane (the less volatile component) evaporates with the same evaporation

rate. However, this could not be observed in the evaporation of n-heptane (the most volatile)

component. It may be due to the over-estimation of experimental initial volume fraction of the

most volatile component in the droplet and due to the heat flux through the fiber.

Acknowledgment

The authors wish to acknowledge the experimental data provided by C. Chauveau and co-

workers from ICARE-CNRS and LME, Polytech’Orléans, France. The discussion with Dr B.

Cuenot from CERFACS Toulouse and Prof. T. Poinsot from IMFT Toulouse and their advices

are greatly acknowledged.

5 Appendix A: physical properties of the gas mixture

Some properties like g, g, Dg, hi and g are calculated at the reference temperature Tref

(Equation (2.24)) while others like and are obtained at T . Density of the gas mixture is

calculated from the ideal/real gas equation of state with the appropriate temperature. For the

binary diffusion coefficient Dg in the gas mixture, the correlation of Wilke and Lee [31] has

been used. Then, the diffusion coefficient of each species into the gas mixture is obtained

from the following relation:

N
1 − Yi X αWα
Dig = = α ≠i
(5.1)
N Xα N Xα
α ≠i
W α ≠i
Dα i Dα i

where Dai=Dg for component i.

Dynamic viscosity and thermal conduction coefficients ( g (W.m-1s-1) and g (Kg.m-1s-1)) are

obtained at Tref:

32 32
AT A1 = 252 × 10−5 AT A1 = 1457 × 10−9
λg = 1 ref
with , µg =
1 ref
with (5.2)
Tref + A2 A2 = 200 K Tref + A2 A2 = 110 K

is obtained from Equation (5.2) at the ambient temperature T . Specific heat of liquid at

constant pressure Cpf is calculated from the enthalpy gradient at the reference temperature Tref.

Specific enthalpy hi for each component is obtained from the tabulated thermodynamic data

like Burcat [44].

6 Appendix B: Vapor-Liquid Equilibrium (using Real and Ideal gas EOS)

At the liquid-gas interface, for every component i in the mixture, the condition of

thermodynamic equilibrium is given by [31]:

f i v = fi l (5.3)
where f is the fugacity. The v and l exponents stand for vapor and liquid phases respectively.

The fugacity of a component in a mixture depends on the temperature, pressure and

composition of that mixture. Reid et al. [31] introduced the fugacity coefficient φi as follows:

fi
φi = (5.4)
XiP

where Xi is the mole fraction of component i and P is the total pressure. Assuming a non-ideal

solution, the surface mole fraction of the droplet can be determined using the thermodynamic

equilibrium condition for the partial vaporization at the given temperature and pressure as

[45]:

X i , gφi , g = X i ,lφis,l (5.5)

where the fugacity coefficients are evaluated from an equation of state. The two-parameter

cubic equation of state is often used for hydrocarbon mixtures. It can be expressed by

RT am
P= − 2 . (5.6)
V − bm V + kbmV + k ′bm2

An equivalent form of Equation (5.6) is:

Z 3 − (1 + B∗ − kB∗ ) Z 2 + ( A∗ + k ′B∗2 − kB∗ − kB∗2 ) Z − A∗ B∗ − k ′B∗2 − k ′B∗3 = 0 (5.7)

Where

am P bm P
A∗ = , B∗ = (5.8)
R 2T 2 RT

In Equation (5.7), Z is the compressibility factor which represents the deviation from the ideal

gas model. One of the well-known cubic equations is the Peng-Robinson (PR) equation [32].

For this equation, k and k' take on the integer values of 2 and -1 respectively. The two

parameters of am and bm are obtained from the mixing rules:

X i , g X j , g ( ai a j ) (1 − k ) ,
1/ 2
am = ij bm = X i , g bi (5.9)
i j i

Where for pure components:

 2
1/ 2
0.45724 R 2Tc2,i T 0.07780 RTc ,i
ai = 1 + f ωi 1 − , bi = (5.10)
Pc ,i Tc ,i Pc ,i

f ωi = 0.37464 + 1.54226ωi − 0.26992ωi2 (5.11)

In the above Equations, R is the universal gas constant, i, Tc,i and Pc,i are the acentric factor,

critical temperature and pressure of component i and kij is the binary interaction parameter

which is assumed to be zero for hydrocarbon mixtures [31]. From the Peng-Robinson

equation of state, the fugacity coefficients will be:

bi
ln φi = ( Z − 1) − ln ( Z − B∗ ) +
A ∗
b i
− δ i ln
2 Z + B∗ k + k 2 − 4k ′ ( ) (5.12)
bm b
B k − 4k ′ m
∗ 2
2 Z + B ∗ k − k 2 − 4k ′ ( )
where

bi Tc ,i / Pc ,i 2ai1/ 2
= , δi = X j ,l a1/j 2 (1 − kij ) (5.13)
bm X j , g Tc , j / Pc , j am j
j

The mole fraction of each component is obtained from Equation (5.5) and Equation (5.12)

with an iterative method. The latent heat of vaporization for each component, Lv,i(Td), can be

calculated from the fugacity at constant pressure and composition of mixture, by:

RT 2 ∂
Lv ,i = −
Wi ∂T
( ln φi, g − ln φi ,l ) (5.14)
P ,n i

where Wi is the molar weight of component i. The latent heat of vaporization, Lv,g used in

Equation (2.6), is determined from the following mixing rule:

N
X i , g Lv ,i
Lv , g = i =1
N
(5.15)
X i,g
i =1

In the case of an ideal fluid mixture, the thermodynamic equilibrium condition at the liquid-

gas interface is expressed by:

X i , g P = X i ,l Pv ,i (5.16)

where Pv,i(Td) is the vapor pressure of species i at the droplet temperature. The mass fraction

of each component is obtained from the mole fraction by:

N
X iWi
W
Yi = X i i , W= i =1
N
(5.17)
W
Xi
i =1

where W is the mean molecular weight.

Figure 1: The schematic of droplet with the gaseous film region around it.
 (a) Gas temperature = 473 K (b) Gas temperature = 973 K
Figure 2: Temporal variation of the normalized droplet projected surface area for n-heptane
 (a) T ∞ = 473K (data of Nomura at Tgas = 471 K) (b) T ∞ = 623K (data of Nomura at Tgas = 648 K)

(c) T ∞ = 823K (d) T ∞ = 973K

Figure 3: Comparison of n-heptane droplet vaporization with the experiment of Chauveau et al. [2] and Nomura
et al. [4] and the model of Abramzon & Sirignano (AS-1989) [9] ( P ∞ = 0.1MPa , normal gravity).
 (a) T ∞ = 548 K (b) T ∞ = 623K
Figure 4: Comparison of n-decane droplet vaporization with the experiment of Chauveau et al. [2] and the
model of Abramzon & Sirignano (AS-1989) [9] ( P ∞ = 0.1MPa , normal gravity).
Figure 5: Comparison of the vaporization rate of n-heptane droplet with the experiment of Chauveau et al. [2]
and the model of Abramzon & Sirignano (AS-1989) [9] ( P ∞ = 0.1MPa , micro-gravity, g = 10−2 g 0 ).
 (a) T ∞ = 473K (b) T ∞ = 973K
Figure 6: Comparison of n-heptane droplet vaporization with real gas EOS for normal and micro-gravity
( g = 10−2 g 0 ) conditions ( P ∞ = 0.1MPa ).
 (a) n-heptane (b) n-decane
Figure 7: Droplet Temperature for different gas temperatures at the normal gravity condition and
( P ∞ = 0.1MPa ). The droplet initial diameter is 400 µm.
Figure 8: Wet-Bulb Temperatures as a function of gas temperatures for n-heptane droplet, ( P ∞ = 0.1MPa ).
(a) Comparison of enthalpy diffusion and conduction
(b) T ∞ = 473K
heat fluxes

(c) T ∞ = 973K
Figure 9: Heat flux in gas and liquid phases along with the surface mass fraction of n-heptane droplet with real
gas EOS at normal gravity condition, ( P ∞ = 0.1MPa ).
 (a) n-heptane (b) n-decane
Figure 10: Vaporization rate versus time for different gas temperatures at the normal gravity condition and
( P ∞ = 0.1MPa ). The droplet initial diameter is 400 µm.
 (a) T ∞ = 473K (b) T ∞ = 973K

(c) T ∞ = 473K (d) T ∞ = 973K

Figure 11: Effect of averaging parameter (Ar) on evaporation of n-heptane droplet at normal gravity
( P ∞ = 0.1MPa ).
 (a) T ∞ = 473K (b) T ∞ = 973K

(c) T ∞ = 473K (d) T ∞ = 973K

Figure 12: High-pressure vaporization at normal gravity; ideality and non-ideality comparisons
Figure 13: Phase envelope diagram for N-heptane/Nitrogen mixture
 (a) 70% n-heptane, 30% n-decane, Fitted: 65% n-
(b) 30% n-heptane, 70% n-decane
heptane, 35% n-decane

(c) New model : 70% n-heptane, 30% n-decane, Fitted: 65% n-heptane, 35% n-decane
Figure 14: Comparison of vaporization rate of droplet with real gas EOS and normal gravity condition with the
experiment of Birouk [3] and the model of Abramzon & Sirignano (AS-1989) [9] ( P ∞ = 0.1MPa ). Part 1:
Transient temperature during the mixture evaporation, Part 2: Quasi-steady temperature during n-decane
evaporation
 Table 1: Droplet vaporization case studies

Liquid Droplet Ambient Temperature T (K) Initial Droplet Temperature T0 (K)

473 300

623 310
n-Heptane
823 320

973 340

548 300
n-Decane
623 310
Table 2: High gas pressures numerical studies. Effects of the pressure on the wet-bulb temperature at T = 973K

(real gas model).

Mole fraction in liquid Mole fraction in gas Wet-bulbs

Cases Component P (MPa)
phase phase Temperature (K)

n-heptane 0.95 0.46

case 1 2 459
Nitrogen 0.05 0.54

n-heptane 0.885 0.4

case 2 5 489
Nitrogen 0.115 0.6

n-heptane 0.716 0.365

case 3 10 501
Nitrogen 0.284 0.635

n-heptane 0.6 0.323

case 4 15 493
Nitrogen 0.4 0.677
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