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Phase change of multicomponent mixtures in

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Conference Paper · January 2001

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 Phase change of multicomponent mixtures
in annular ow
J.R. Barbosa, Jr., G.F. Hewitt and S.M. Richardson

Department of Chemical Engineering and Chemical Technology,

Imperial College of Science, Technology and Medicine,
Prince Consort Road, London, SW7 2BY, UK.

Abstract
A study is presented on the role of droplet interchange in the annular ow regime and on
its in uence on the mechanisms by which heat is transferred to or from the two-phase mixture
in convective boiling or condensation of multicomponent mixtures. A modelling framework
based on dierential conservation equations is applied to calculate the distributions of phase
concentration, interfacial and wall temperatures and heat transfer coecient for both evaporat-
ing and condensing systems under various conditions. Results are compared with those obtained
experimentally for boiling of hydrocarbon mixtures (Kandlbinder, 1997) and condensation of
R-407C (Cavallini et al., 1999).
Key words: Annular ow; boiling; condensation; multicomponent mixtures

1. Introduction
Droplet entrainment and deposition are vigorous mass exchange phenomena which dis-
rupt the hydrodynamic equilibrium of annular ow. Drops are created by the shearing
action of the gas ow at the crest of large amplitude waves which travel on a liquid lm
attached to the wall. The drops entrained from the lm move along the channel in the gas
core, some of the droplets being re-deposited as they pass along the channel. Amongst
many other eects, these phenomena are known to exert a high in uence on important
ow parameters like pressure drop (Fore and Dukler, 1995).
The objective of this study is to investigate the role of droplet interchange in the
annular ow regime and its in uence on the mechanisms by which heat is transferred
to and from the two-phase mixture in convective boiling and condensation. The signi-
cance of droplet interchange seems to have been overlooked in previous multicomponent
phase change studies and the correct prediction of this mechanism may hold the key to
understanding the behaviour of the heat transfer coecient at high qualities.
The heat transfer coecient for mixture systems is dened by the following equation,
 = T q,_w T ; (1)
w E
1
where q_w is the heat ux applied to the channel wall, Tw is the temperature of the inner
wall and TE is an equilibrium temperature calculated based on the system local pressure
and enthalpy. For mixtures undergoing condensation TE is the dew point temperature,
whereas for boiling or evaporation TE is the bubble point temperature.
Recent experiments carried out at HTFS Harwell and Imperial College (Kandlbinder,
1997) and elsewhere (Cavallini et al., 1999) demonstrated a deterioration and an im-
provement of  at high qualities for boiling and condensing ows, respectively. It is
believed that the departure from mechanical equilibrium caused by droplet entrainment
and deposition plays a vital role in determining the distributions of interfacial and of wall
temperature in such systems. These trends are not picked up by methods and correlations
that do not take into account droplet interchange.
A modelling framework based on dierential conservation equations is used to calcu-
late the distributions of phase concentrations, interfacial and wall temperatures and heat
transfer coecients for both evaporating and condensing systems at various conditions.
Rates of droplet entrainment and deposition are calculated using an extension to mul-
ticomponent systems (Barbosa and Hewitt, 2001a, 2001b). Interphase transfer of mass
and heat is dealt with using a Colburn-Drew methodology.
This paper is organised as follows. Section 2 gives a theoretical overview of the prob-
lem. The calculation methodology is presented in Section 3. Results are presented
in Section 4. These are compared with experimental data obtained for boiling of n-
pentane/n-hexane/iso-octane mixtures (Kandlbinder, 1997) and condensation of R-407C
(Cavallini et al., 1999). Finally, conclusions are drawn in Section 5.

2. Theoretical background
2.1. Boiling/Evaporation

In design calculations, the two-phase ow pattern is ignored and it is implicitly assumed

that the whole of the liquid ow is available for evaporation (Fig.1.a). Usually, a ash
calculation is used to determine the amount of liquid which has evaporated for a given wall
heat ux and the saturation (bubble point) temperature of the mixture. The preferential
evaporation of the more volatile component gives rise to axial gradients of saturation
temperature and of mean concentration in both phases.
In a real situation, however, where the annular ow pattern (Fig.1.b) is the dominant
conguration, not all of the liquid is present as a lm coating the inner wall of the pipe.
Rather, the core is a fairly homogeneous mixture of vapour and entrained droplets. Due
to the distribution of the liquid phase within the pipe, the temperature driving force
for liquid lm evaporation is much higher than that for droplet evaporation. Therefore,
in real annular ow, not all of the liquid phase will be available for evaporation at a
given distance along the pipe. This hydrodynamic eect breaks down the equilibrium
relationship existing between quality, X , and mixture saturation temperature, i.e., when
X = 0, Tsat = Tbub and when X = 1, Tsat = Tdew .
If we consider that the evaporation process is governed by forced convective heat
transfer and that the lm may be regarded as fully mixed, then the interface temperature
TI represents an equilibrium value between the vapour adjacent to the interface and a
liquid phase having a mean concentration corresponding to that of the liquid lm. Heat
transfer through the lm is governed by the dierence between the wall temperature, Tw ,
and TI . Even in the case where all the liquid is in the lm (Fig. 1.a), TI will dier,

2
for multicomponent evaporation, from TE due to mass transfer resistances in the vapour.
These resistances may be dealt with using classical methods (Colburn and Drew, 1937;
Webb, 1995). However, if the concentration of the respective component in the droplets
diers from that in the liquid lm (Fig. 1.b), then this eect can have a profound in uence
and vitiates the direct application of the classical methods.

Implicitly Actual
assumed in situation
design

(a) LOW HIGH (b)

Concentration of more volatile
component

Figure 1. Illustration of the problem of phase

change in annular ow.
In Fig. 1.b, the bottom end of the picture represents the onset of annular ow. If
droplet evaporation is ignored, then it is not illogical to assume that the droplets will
retain a concentration equal to that of the liquid lm at the point at which they were
created (entrained). As an axial gradient of concentration is established in the liquid lm
due to the preferential evaporation of the more volatile component, droplets generated
at distinct co-ordinates will have distinct concentrations. Thus, at a particular distance,
a spectrum of concentration is found in the population of depositing droplets. When
calculating the mean liquid lm concentration (and hence the interface temperature), it
is necessary to take account of both the fraction of the liquid phase which is present and
droplets and also of the mean concentration of these droplets. The fraction entrained
as droplets can be calculated using methodologies developed for single component uids
(see for instance Hawkes, 1996). Using these methods, it is, for instance, possible to
calculate the conditions under which all of the liquid is entrained as droplets and the lm
is dried out. However, to deal with the multicomponent case, there is a need to carry out
detailed tracking of the concentration of the respective component in the entraining and
depositing droplets so that the mean concentration of the components in the droplets can
be calculated at any given location.
Following the work of Shock (1976), one approach to solve the problem (Barbosa and
Hewitt, 1999) is to ignore mass transfer resistances in the vapour phase. Shock analysed
the evaporation of a water-ethanol mixture, with a boiling range of the order of 20 K. He
could not evaluate precisely the signicance of mixture eects as the dierences in wall
temperature due to such eects may be small compared with those due to limitations
3
of his model for determination of the temperature drop across the lm. The systems
studied here have boiling ranges at atmospheric pressure nearly 2.5 times greater than
those analysed by Shock and mass transfer eects are likely to be much more signicant.
In summary, the decrease in  observed in mixture systems is due to a denition of
the heat transfer coecient based on the temperature dierence Tw , TE . The interface
temperature, TI , can be higher than TE due to the eect not only of mass transfer but
also (and mainly) due to the dierences in concentration between the droplets and the
lm.

2.2. Condensation

It is intuitive to think that the eects described in Section 2.1 will work in an opposite
way for condensation, i.e., it will make the lm become locally richer in the more volatile
component than the droplets. This eect may then give rise to an enhancement of the heat
transfer coecient, Eq.(1), as the wall temperatures for the hydrodynamic equilibrium
case are higher than those for real annular ow.
However, the relative eect of droplet interchange on the condensation heat transfer
may be less than in evaporation due to two reasons. Firstly, typical boiling ranges
of mixtures used in condensing systems (and therefore experiments) are much lower
than some observed in boiling experiments (R-407C at 1.5 MPa has a boiling range
of the order of 5 K). This makes the saturation temperature imbalance between the
liquid lm and droplets much more subtle. Secondly, in evaporation, diusive mass
transfer resistance and droplet interchange work in the same way, i.e., towards a decrease
in the heat transfer coecient. In condensation, however, the heat transfer coecient
deterioration due to mass transfer resistance may be sucient to cancel out or overcome
any increase associated with droplet interchange.

3. Modelling
Mass conservation equations can be derived for the annular ow regime (Barbosa and
Hewitt, 2001a, 2001b). For a NOC -component mixture, these are given by,
0 1
X
d m_ = 4 @hDi , E , NOC
dz LF dT m_ I;j A ; (2)
j =1

X
d m_ = 4 NOC
dz GC
dT j=1 m_ I;j ; (3)

d m_ = 4 (E , hDi) ; (4)
dz LE dT
2 3
d x = 4 4(hDx i , hDix ) + NOCX
dz LF;i d m_ LF;i LF;i m_ I;j xLF;i , m_ I;i5 ; (5)
T LF j =1
0 1
d y = 4 @m_ , NOC X A
dz b;i dT m_ GC I;i j=1 m_ I;j yb;i : (6)

4
where m_ denotes a mass owrate per unit pipe cross-sectional area. The subscripts LF ,
LE , GC , I and b relate to the liquid lm, entrained liquid, gas core, interface and bulk.
D and E are the droplet entrainment and deposition rates. The cumulative operator hi
quanties the deposition of groups of droplets with distinct concentrations (Barbosa and
Hewitt, 2001). The interfacial mass uxes m_ I;i are positive for evaporation and negative
for condensation. An energy balance for the gas core gives,
d T = 4 [ (T , T ) + (E , hDi) c (T , T )] :
m_ C cpC dz (7)
C
d GC I C
T
pLE I C

The rst term in the RHS of Eq.(7) is the conductive contribution of the heat ux to
the vapour phase. The second term is the net energy released/absorbed by the entrained
liquid due to entrainment and deposition. m_ C , cpC and TC are the core mass ux,
specic heat capacity and temperature, respectively. These are calculated based on the
assumption of a homogeneous (no slip) ow in the vapour core.
Momentum balance equations are written in terms of pressure gradients (accelera-
tional, gravitational, frictional). These are as follows (Hawkes, 1996).
dp = dp + dp + dp ; (8)
dz dz a dz f dz g
" #
dp = , (u , u ) dm_ GC + 4 (E + hDi) , duC [m_ + hm_ i] ; (9)
C LF
dza dz d dz GC
T
LE

dp = ,2 I ; (10)
dz f rI
dp = , g; (11)
C
dz g
where C and uC are the homogeneous core density and velocity, respectively. rI is
the distance from the pipe centre line to the interface. I is the interfacial shear stress
calculated using the correlation by Whalley and Hewitt (1978).
At each integration step
z, an iterative procedure is carried out to determine the
interfacial mass uxes, compositions and temperature. The solution algorithm for the
interphase heat and mass transfer calculation is comprised by the following steps (Webb,
1995),
1. Known: xLF (= xLF ; fully mixed lm hypothesis), yb;i, TC ;
I ;i b;i

2. Calculate: yI;i, TI ! Bubble point temperature subroutine;

3. Guess: PNOC
j =1 m _ I;j ;
4. Calculate: P m_ I ;j
N OC
m_ ! Eq. (16);
j =1 I ;j

5. Calculate: q_GC ! Eq. (12);

6. Compare: If q_GC 6= q_w , q_ED , update PNOC
j =1 m
_ I;j and return to step 4.

5
 The set of equations used in the interfacial heat and mass balances iterative calculation
is summarised below. These are based on a Film (Colburn-Drew) Theory. For heat
transfer,
X
NOC
 e (T , T );
q_GC = m_ I;j
hv;j + GC I T
C (12)
j =1

 = GC T ;
GC (13)
e , 1 T

1 X
NOC
T =  m_ I;j cpGC;j : (14)
GC j =1

GC dT = 0:023Re0:8 Pr0:4 : (15)

GC GC GC

For mass transfer,

X
NOC X,1
NOC
m_ I;i = yI;i m_ I;j + GC 
BGC (yI;i , yb;i) ;
i;k
(16)
j =1 k=1
 ] = [B ] [] fexp [] , [I ]g,1 ;
[BGC (17)
GC

1 X
NOC
[] =  m_ I;j [BGC ],1: (18)
GC j =1

[BGC ] dT [
],1 = 0:023Re0GC

:8 [Sc ]0:4 ;
GC (19)
[ScGC ] = GC [
],1; (20)
GC
where [
] is the matrix of Fickian diusion coecients. For the multicomponent
mixtures, it is calculated using an Eective Diusivity Method in which only the main
diagonal elements of [
] are dierent than zero. These are given by,
ii = i3 , where
i = 1; 2. For the binary case, [
] is reduced to a scalar, 12 . ij is the ideal gas vapour
diusion coecient. In Eqs.(12)-(20), ,  and  are density, viscosity and thermal
conductivity. ReGC and PrGC are the vapour phase Reynolds and Prandtl numbers.
[BGC ] is the zero- ux matrix of mass transfer coecients. q_GC is the interfacial heat ux.
Thermodynamic and transport properties were calculated using the methods suggested
by Assael et al. (1996).
Finally, the wall temperature, Tw , is determined by applying a correlation for the heat
transfer coecient in the liquid lm. In the boiling case, the correlation by Chen (1963)
is used. The nucleate boiling component is corrected for mixture eects as suggested
by Palen and Small (1964). In the condensation case, only the macroconvective (forced
convection) term of the Chen correlation is used.
In boiling/evaporating ows, a signicant amount of liquid may be entrained as
droplets at the onset of annular ow (Hewitt and Hall-Taylor, 1970). Therefore, a value of
10% (close to the equilibrium value) was chosen as the initial condition. For condensation,
the initial entrained fraction is 0%.
6
4. Results
Comparisons are made with the experimental data obtained by Kandlbinder (1997) for
boiling and Cavallini et al. (1999) for condensation. Kandlbinder carried out forced con-
vective boiling experiments at various pressures for both binary and ternary mixtures of
n-pentane/n-hexane/iso-octane in a 8.68 m long, vertical 321 stainless steel, electrically
heated test section. The inner and outer diameters were 25.4 and 38.0 mm, respec-
tively. The overall values of mole fraction of the data sets investigated here are 0.7/0.3
(n-pentane/iso-octane) | Mixture 1 | and 0.31/0.22/0.47 (n-pentane/n-hexane/iso-
octane) | Mixture 3. Along the test section, bulk uid and wall temperatures were
measured. Bulk temperatures, the temperature of the uid at the centre line of the
tube, were measured at 12 equally spaced (750 mm) locations. Wall temperatures were
measured at 74 points along the test section.
Cavallini et al. conducted condensation experiments using R-407C (a non-azeotropic
ternary mixture of R-32, R-125 and R134a, respectively 23, 25 and 52 % by weight) at
pressures of the order of 17.0 bara in a 1 m long, horizontal stainless steel double pipe test
section. The inner diameter of the inner pipe was 8.0 mm and condensation of the test
uid was achieved by passing cold water through the outer annular gap. In the present
study, care was taken so that the conditions analysed fell on the annular/semi-annular
ow regime in the ow pattern map presented by Cavallini et al. In these cases, it is
expected that gravity eects (resulting on a variation of the thickness of the liquid lm
around the periphery of the pipe) are of a higher order. Refrigerant and wall temperatures
at the inlet and outlet of the test section were measured using thermocouples inserted at
both the centre line of the inner tube and at the tube wall. The average condensation
heat transfer coecient is given by the ratio between the wall heat ux (obtained from the
axial temperature gradient on the coolant side) and the logarithmic mean temperature
dierence between the two-phase mixture (dew point temperature) and the pipe wall.
Figures 2 and 3 illustrate typical variations of liquid phase (lm and droplets) mean
concentration for boiling and condensation, respectively. The eect of hydrodynamic
non-equilibrium can be observed in both cases. In the boiling example, as the quality
increases, the droplets become richer in the more volatile component than the liquid lm.
In condensation, the lm gets richer in the more volatile components (R-32 and R-125)
as the quality increases. As the changes in concentration are much more pronounced for
the hydrocarbon system, it is expected that the non-equilibrium eects will be greater
on this system than on the refrigerant mixture.
Temperature proles for a typical boiling case are shown in Fig. 4. The agreement
between experimental and predicted wall and core temperatures is very good. The mono-
tonic increase of the interface temperature with increasing distance (or quality) can be
clearly observed.
A typical local heat transfer coecient prediction of the boiling data is presented
in in Fig. 5. Predictions using other methods, such as the correlations by Kandlikar
(1998), Palen (1983) and Sardesai et al. (1982), are also shown. Of these, only the
equilibrium resistance method by Sardesai et al. (1982) picks up the decreasing heat
transfer coecient trend. However, it underestimates the data quite considerably.
Average heat transfer coecients for condensation are shown in Fig. 6. These were
calculated for three dierent total mass uxes, namely 200, 400 and 750 kg m,2 s,1 . The
agreement between experimental and predicted data is satisfactory, presenting deviations
always lower than 20%.

7
 C O N C E N T R A T IO N O F N -P E N T A N E (M A S S F R A C T IO N )
0.60

0.50
D ro p le ts

0.40
F ilm

0.30
4 .0 0 5 .0 0 6 .0 0 7 .0 0 8 .0 0 9 .0 0
D IS T A N C E [m ]

Figure 2. Liquid lm concentration in boiling. Mixture 1, p = 0:32MPa,

q_w = 49:3kWm,2, m_ T = 305kgm,2s,1.

0.30
LIQ U ID P H A S E C O N C E N T R A T IO N (M A S S F R A C T IO N )

R -125
F ilm
0.2 8
D ro p le ts

0 .11 0.26

R -32
F ilm
0 .10 D ro ple ts

0 .09
0 .40 0.80 1.20 1.60 2.00 2.40
D IS T A N C E [m ]

Figure 3. Liquid lm concentration in condensation. R-407C, p = 1:7MPa,

q_w = 33:7kWm,2, m_ T = 402kgm,2s,1.

8
 410

W a ll

T E M P E R A T U R E [K ]
400

In te rfa ce

390
C o re

380
4 .00 5 .0 0 6 .00 7 .0 0 8.0 0 9 .00
z [m ]

Figure 4. Temperature distributions in boiling. Mixture 3, p = 0:24MPa,

q_w = 40:5kWm,2, m_ T = 298kgm,2s,1.

5000

Kandlikar (1998)
HEAT TRANSFER COEFFICIENT [W/m2K]

4000
Palen (1983)

3000

Sardesai et al.
(1982)

Barbosa and Hewitt

2000 (2001)

Kandlbinder, 1997

1000
2.00 4.00 6.00 8.00 10.00
DISTANCE [m]

Figure 5. Heat transfer coecient predictions in boiling. Mixture 1, p = 0:23MPa,

q_w = 49:8kWm,2, m_ T = 293kgm,2s,1.

9
 8000

P R E D IC TE D H E A T T R A N S F E R C O E FF IC IE N T (W /m 2 K )
+20%
6000

-2 0 %
4000

C o n de nsatio n of R -40 7 C
2000 d ata o f C a vallini et a l. (19 99 )

2 00 kg/m 2s

4 00 kg/m 2s

7 50 kg/m 2s
0

0 2 0 00 4 0 00 6 00 0 8 00 0
M E A S U R E D H E A T TR A N S FE R C O E F FIC IE N T (W /m 2 K )

Figure 6. Prediction of condensation heat transfer coecients for R-407C.

5. Conclusions
This paper presented a modelling study on the in uence of droplet interchange on phase
change heat transfer to binary and ternary mixtures in annular ow. The main conclu-
sions arising from this work are as follows,
1. droplet entrainment and deposition eects cause dierences between lm and droplet
concentrations. Analysis of these eects suggests that the heat transfer coecient
decreases with increasing quality for boiling/evaporating ows, whereas it increases
with increasing quality for condensation;
2. the calculation methodology presented was successful at predicting both boiling
and condensation heat transfer data;
3. a more detailed set of experiments, aimed specically at investigating the in uence
of droplet interchange on condensation heat transfer of multicomponent mixtures,
would be very useful in order to consolidate the analysis.

Acknowledgements
The authors thank Dr. Luisa Rossetto (Universita di Padova, Italy) for kindly providing
the experimental data on condensation. JRB thanks the Brazilian National Research
Council (CNPq - Conselho Nacional de Desenvolvimento Cientco e Tecnologico) for
the award of a scholarship (Grant No. 200085/97-2).

10
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