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GeMer, D.. I d . Eng. Chem., Fundam., 10, 534 (1971). Shah, Y. T., Pearson, J. R. A.. Ind. Eng. Chem.

J. R. A.. Ind. Eng. Chem., Fundam.. 11, 150 (1972).


Kase, S..J. Appl. Polym. Sci., 18, 3279 (1974). Trouton, F. T.. Proc. Roy. SOC.Ser. A, 77, 426 (1906).
Matovich. M. A,, Pearson, J. R. A,. Ind. Eng. Chem., Fundam., 8, 512 (1969). Weinberger, C. B., Ph.D. Dissertation, University of Michigan, 1970
Miller, J. C., S.P.E. Trans., 3, 134 (1963). Weinberger, C. B., Goddard, J. D., Int. J. Multiphase Now, 1, 465 (1974).
Nickell, R . E., Tanner, R. I., Caswell. E., J. FIMMech., 65, 189 (1974).
Pearson. J. R. A,, Matovich. M. A,. Ind. Eng. Chem., Fundam., 8, 605 (1969). Received for reuiew January 20, 1975
Pearson, J. R. A,, Shah, Y. T., Trans. SOC.Rheol., 16, 519 (1972).
Pearson, J. R. A., Shah, Y. T.. Ind. Eng. Chem., Fundam., 13, 134 (1974). Accepted June 30,1975

A Model for Gas-Liquid Slug Flow in Horizontal and Near Horizontal


Tubes

Abraham E. Dukler’ and Martin G. Hubbard


Chemical Engineering Department, Universify of Houston, Houston, Texas 77004

A model is presented which permits the prediction in detail of the unsteady hydrodynamic behavior of gas-liquid
slug flow. The model is based on the observation that a fast moving slug overruns a slow moving liquid film ac-
celerating it to full slug velocity in a mixing eddy located at the front of the slug. A new film is shed behind the
slug which decelerates with time. Mixing in the slug takes place first due to the mixing eddy and then due to the
usual diffusion due to turbulence. The model predicts slug fluid velocity, velocity of propagation of the nose of
the slug, film velocity as a function of time and distance, length of the slug, film region behind the slug, and mix-
ing eddy and shape of the surface of the film region. Agreement with experimental data is good.

Introduction measured pressure drop and in some cases average holdup


Gas-liquid flow in conduits is a more complex phenome- under conditions where slug flow was observed to exist. A
non than single-phase flow primarily because the spacial careful study of these data and the experimental tech-
distribution of the two phases is unknown and difficult to niques reveal serious limitations in the results. In many in-
specify quantitatively. A variety of such distributions have stances a portion of the pressure measuring system was not
been qualitatively described by numerous investigators in fully developed slug flow. In some cases the slug length
(Hewitt and Hall Taylor, 1970; Hoogendoorn and Welling, (estimated by methods to be reported here) exceeded the
1965; Kosterin, 1949). Hubbard and Dukler (1966) suggest- distance between pressure taps. In most of these studies
ed that these many observed patterns really represented only air space existed between pressure taps at times. In all
the superposition of only three basic distributions: sepa- cases pressure drop was measured using highly damped
rated, intermittent or slug, and distributed flows. A still manometers to smooth out the fluctuations. Furthermore,
unresolved problem is the prediction of the particular com- these studies provide no information on the characteristics
bination to be expected given the flow rates, fluid proper- of slug flow such as frequencies, spacing, slug length veloci-
ties, conduit size, and inclination. A useful empirical corre- ties, etc.
lation has been proposed (Baker, 1954). The earliest attempt to study the details of slug flow
Intermittent or slug flow exists over a wide range of flow were by Kordyban (1961). He proposed a simple model
rates for moderate pipe sizes in a horizontal configuration. where slugs move at the velocity of the gas and “skate” or
Such a flow pattern is inherently unsteady with large time slide over the top of a substrate film without interaction or
variation of the mass flow rate, pressure, and velocity at mixing between the slug and film. Experimental data were
any cross section normal to the tube axis. This is so even taken in 6 ft long tubes of 0.315 and 0.420-in. i.d. with pres-
when the gas and liquid flow to the system is steady. As a sure taps separated by 1 ft. Thus the validity of the data is
result, processes of heat and mass transfer are also un- seriously in question. Based on their concept, the authors
steady with substantial fluctuations in temperature and develop an expression for pressure drop but this is in poor
concentration. This poses special and difficult problems for agreement with their data. In fact the classical Martinelli
the designer. I t is the purpose of this paper to present a correlation is shown to be a better predictor of the data
systematic model for the hydrodynamics of slug flow from than their own correlation. In 1963 Kordyban and Ranov
which the time varying behavior can be predicted. The (1963) reported new experimental data from a 10-ft long
model presented here is based partly on the work of Hub- pipe of 1.25-in. diameter. They generate slugs by forcing
bard (1965) which was presented by Hubbard and Dukler the two-phase mixture through a riser before entering the
(1968) but unpublished. That version has been substantial- test section. If this riser had not been used it is doubtful if
ly revised to eliminate certain empirical aspects and certain they would have been able to observe slug flow, especially
simplifications made in the original work which have now a t the higher flow rates in their work. In this instance the
been found to be unnecessary. pressure measuring technique produced data that were
more meaningful. However, comparison with the earlier
Some Related Research Kordyban model leads the authors themselves to suggest
A number of early investigations (Govier and Omer, that the model is not adequate.
1962; Hoogendoorn, 1959; Martinelli and Nelson, 1948) The beginnings of an attempt to understand the details

Ind. Eng. Chem., Fundam., Vol. 14, No. 4, 1975 337


LEVEL DROPS

SLUG JUST PASSES OUT OF VIEW TO THE RIGHT LEVEL DROPS

LEVEL REBUILDS AND WAVE NEARLY BRIDGES PIPE

POSITION (OR TIME)

Figure 1. The physical model for slug flow.

BRIDGING OF PIPE BY LIQUID SLUG FORMATION

of slug flow can probably be found in the work of Nicklin et


al. (1962), who attempted to modify expressions for the
slug velocity which was developed theoretically for a verti- 0
cal system to the horizontal case. These ideas were general-
ized somewhat by Hughmark (1965), who was concerned SLUG SWEEPS UP LIOUID LEVEL DROPS
with the heat transfer problem and by Neal (1963), who ex- Figure 2. The process of slug formation.
amined some of the limited data of Richardson (1958) on
slug velocity. This was further examined by Marrucci
(1966).
Oliver and Wright (1964) reported on heat transfer dur- A Description of the Condition of Slug Flow, Its
ing slug flow in a test section of 0.25-in. diameter and 4 f t Initiation and Dissipation
long. They made no measurements of the detailed charac- The process of slug flow is a highly complex unsteady
teristics of the flow since their concern was the heat trans- phenomenon. An understanding of the flow mechanism has
fer process. Slug flow in these small sizes is a very special been developed from extensive visualization studies includ-
situation which is equivalent to bubble flow with Taylor ing short exposure time still photographs, motion picture
type bubbles having bullet shaped noses separated by liq- sequences at several speeds, and dye tracer work. The
uid plugs moving in laminar flow. There is little or no study was carried out in a 1.5-in. i.d. horizontal pipe, 65 f t
asymmetry and the similarity with slug flows in larger di- long. The mechanism proposed was substantiated by mea-
ameter tubes is small. surements of wall pressure using fast response pressure
Greskovich and Shrier (1972) applied the model present- transducers located flush with the wall. The results are
ed by Hubbard and Dukler (1968) to horizontal systems in summarized below.
pipes of 1.5 to 6.07-in. diameter but used independent rela- Visual Observations. Refer to Figure 1 for a sketch of
tionships for slug frequency and holdup. In general the re- an idealized slug which has been fully established and to
sults were shown to predict pressure drop with good reli- Figure 2 for a sketch of the process of slug formation in
ability. In a subsequent paper (Bonnecaze et al., 1971) they horizontal pipes. The picture of slug flow which emerges
modified the preliminary model to account for tube incli- from these observational studies is as follows.
nation. New relations for slug velocity were prepared based 1. Liquid and gas flow concurrently into a pipe. Near the
on a potential flow model but the relative importance of entrance the liquid flows as a stratified phase with the gas
gravity and friction forces was not clearly demonstrated. passing above. At gas and liquid velocities under which slug
Despite these untenable assumptions, agreement with flow takes place, the liquid layer decelerates as it moves
some field data taken by Esso on a 10,000-ft section of 6-in. along the pipe. As a result, its level increases, approaching
line was good. the top of the pipe. At the same time, waves appear on the
Vermeulen and Ryan (1971), following some aspects of liquid surface. Eventually the sum of the rising liquid level
Hubbard's model, compared their own data taken in a 0.5- plus the wave height is sufficient to bridge the pipe mo-
in. x 18-ft test section with their simplified form of the mentarily blocking the gas flow. (See Figure 2A, B, and C).
model. Their data included, in addition to the horizontal 2. As soon as the bridging occurs, the liquid in the bridge
flow configuration, some results at positive and negative in- is accelerated to the gas velocity. The liquid appears to be
clinations of 7'. Agreement was good but the model did not accelerated uniformly across its cross-section, thereby act-
account for film acceleration and the data itself was used to ing as a scoop, picking up all the slow moving liquid in the
estimate this quantity. Since such acceleration is over 50% film ahead of it and accelerating it to slug velocity. By this
of the whole, the compromise involved is clear. No compar- mechanism, the fast moving liquid builds its volume and
ison was presented between experiment and the simplified becomes a slug. (See Figure 2D.) A fully formed slug is
theory for many of the details of the flow. shown in Figure 1.
Application of two-phase flow in capillary tubing could 3. As the slug is formed and moves down the pipe, liquid
be of industrial importance in a few specialized instances. is shed uniformly from its back and forms a film with a free
Here the flow is laminar, the gas bubbles are almost sym- surface. This liquid in the film decelerates rapidly from the
metrically located in the pipe, liquid film exists at all slug velocity to a much lower velocity as controlled by the
points on the wall and the analysis is subject to a near rig- wall and interfacial shear. (See zone l f in Figure 1.)
orous development. The papers of interest are those by Cox 4. Once a slug is formed as it travels down the pipe it
(1964), Bretherton (1961), Goldsmith and Mason (1963), first sweeps up all the excess liquid which had entered the
Suo and Griffith (19641, and Suo (1968). Most of these pa- pipe since the last slug was formed. From that point on it
pers are directed toward determining the rate of propaga- picks up liquid film which has been shed from the preced-
tion of the gas bubble out of the tube but they also consider ing slug. Since the slug is now picking up liquid at the same
the velocity distribution and residence time of the gas rate that it is shed, its length stabilizes.
phase. 5 . The slug has a higher kinetic energy than that of the

338 Ind. Eng. Chem., Fundam., Vol. 14, No. 4, 1975


I 4 k O . l S /

Vs= 5.0 ft./sec.

Figure 3. Pressure-time trace for slug flow. Figure 4. Pressure-time trace for slug flow.

liquid film. Thus, the film penetrates a distance into the


slug before it is finally assimilated a t the slug velocity. This
over-running phenomenon creates an eddy at the front of
the slug which is essentially a mixing vortex. The distance
of penetration constitutes the length of the mixing eddy. In
r vs= 174 f t /sec

this mixing zone gas is entrapped due to the violent mixing


Figure 5. Pressure-time trace for slug flow.
operation. (See zone 1, in Figure 1.)
6. As the gas rate and consequently the slug velocity in-
crease, the degree of aeration of the slug increases. Ulti- of the entire system. In particular this is evident in Figure
mately the gas forms a continuous phase through the slug. 4 after the slug passes and these variations can be ex-
When this occurs the slug begins bypassing some of the gas. plained in terms of coupling between the slugs (Hubbard,
At this point the slug no longer maintains a competent 1965). Note that as the slug velocity increases there is a
bridge to block the gas flow so the character of the flow corresponding increase in the fraction of the total pressure
changes. This point is the beginning of “blow-through’’ and drop across a slug which is due to acceleration of the liquid
the start of the annular flow regime. film.
Qualitative Confirmation of the Model. Figure 1 In these experiments independent measurements were
shows an idealized pressure profile through a slug unit made of slug and film velocity as well as of film flow rate. It
viewed a t an instant in time and based on the mechanism was thus possible to calculate the pressure drop due to ac-
presented above. A sharp rise in pressure takes place across celeration and that due to friction. These were shown to
the mixing zone associated with the force necessary to ac- agree very well with the measurements made from several
celerate the slow moving liquid in the film ahead of the slug hundred traces of the type shown in these figures. Thus
to the velocity of the slug. There follows a linear change in there has been demonstrated the reasonableness of this
pressure due to gradient shear in the body of the slug and two-zone model which requires a pickup of the film in a
equivalent to that which would take place in full pipe flow mixing zone, the existence of a “full pipe flow” region be-
with no slip between the distributed gas and liquid. In the hind the mixing vortex and a process of shedding of the
film zone the pressure is essentially constant since the film behind the slug to form a film region.
pressure drop is small compared to that in the liquid slug. In the discussion which follows, the process of slug flow
Consider a wall pressure transducer located a t point, T , is treated as a fully deterministic one. In fact, experiments
along the test section. This point is selected so that there is make it evident that slug flow has certain random features.
never more than one slug between T and the discharge In particular, the time and space between slugs does vary
location. Then the pressure measured a t T is that due to and so does the pressure drop across slugs, the film veloci-
the pressure drop across one slug. When the slug passes out ty, and other features. There has been no satisfactory treat-
of the pipe so that vapor space exists between T and the ment of this randomness. However, the data show that the
exit (before another slug arrives) the pressure drops to es- probability distributions are narrow. In the work that fol-
sentially that at the exit. As a slug moves across the station lows each quantity can be interpreted as the mean of a set
a t T the profile of pressure through the slug can be record- of values which distribute about the mean.
ed.
Figures 3-5 are time traces obtained using air-water in a The Hydrodynamic Model
1.5-in. horizontal pipe with the pressure transducer located Pressure Drop across a Slug. Figure 1 shows that there
8.5 f t upstream of the discharge. Three different slug flow are two contributions to the pressure drop across a slug.
conditions appear. Figure 3 represents a low flow rate The first, APa, is the pressure drop that results from the
where the film and slug velocities approach each other and acceleration of the slow moving liquid film to slug velocity.
thus where film acceleration and its associated pressure
The second, APf, is the pressure drop required to overcome
drop are small. Figure 5 represents a very high slug velocity wall shear in the back section of the slug. The total pres-
and a low film velocity so that a large pressure drop is re-
sure drop across a slug is thus
quired to accelerate the film. In each trace the time during
which a slug passes over the measuring station is indicated AP, = A P , -k APi (1)
by a bar as determined from a separate conductivity probe. Pressure drop in the gas phase above the liquid film is neg-
These figures show the principal contributions to the pres- ligible.
sure pulse associated with a slug. The zone, labeled 1, is the Acceleration Contribution. A slug that ha5 stabilized
pressure rise due to the increase in hydrostatic pressure on in length can be considered as a body receiving and losing
the arrival of the slug over the measuring station. Zone 2 is mass a t equal rates. The velocity of the liquid in the film
an additional abrupt rise in pressure a t the front of the slug just before pickup is lower than that in the slug and a force
associated with the acceleration of the liquid film in front is therefore necessary to accelerate this liquid to slug veloc-
of the slug. Zone 3 is a gradual linear pressure rise due to ity. This force manifests itself as a pressure drop given by
the frictional pressure gradient across the back of the slug
behind the mixing zone. The pressure trace as measured a t
T also displays changes in pressure when the slug drops out
of the pipe and also reflects changes in the static pressure where x is the rate at which mass is picked up by the slug,

Ind. Eng. Chem., Fundam., Vol. 14, No. 4, 1975 339


-+ “fe-
I
AB C
t I

Figure 6. The pickup process at the front of a slug. Figure 7. The shedding process at the back of a slug.

V, is the mean velocity of fluid in the slug, and Vf, is the The translational velocity, Vt, must also satisfy the fol-
mean velocity of fluid in the film in front of a slug. This lowing relationship
pressure drop due to acceleration takes place over a mixing
translational mean fluid apparent velocity
eddy at the front of the slug which penetrates a distance,
l, into the body of the slug. velocity at = velocity in + gained by adding
Frictional Contribution. Behind the mixing eddy in the slug nose the slug fluid at the slug
the body of the slug pressure drop takes place due to wall nose
friction. For the calculation of this term, the similarity X
vt VS
analysis for two-phase frictional pressure drop developed P L ARS
by Dukler et al. (1964) is applied. Within this part of the Comparing this equation with eq 7 indicates that the cor-
slug the two phases are homogeneously mixed with negligi- rect definition of the mean slug velocity is
ble slip. Under this condition, the recommended pressure
drop equation becomes

Thus, V, can be calculated from a knowledge of the input


volumetric flow rates and the pipe area and is independent
The similarity analysis showed that for “non-slip” condi- of the distribution of liquid between the film and the slug.
tions f, could be correlated as a unique function of Re, Equation I can now be written as
when this parameter is defined in the following manner X
and that when the liquid holdup exceeded 0.7 ( R , > 0.7) v, = v, + ~

this correlation is identical to ones for single phase flow. PLARS


It is convenient to define a term C

In order to calculate pressure drop across a slug using eq


2, 3, and 4 the following quantities must be determined: which is the ratio of the rate of shedding to the rate of flow
liquid pickup and shedding rate, x ; film velocity, Vf,; aver- in the slug.
age fluid velocity in the slug, V,; slug holdup, R,; slug v, = (1 + C)V, (11)
length 1,; and length of acceleration section, 1.,
Slug Velocity. The scooping model requires that two In order to use eq 9 for calculating Vt it is necessary to de-
characteristic slug velocities be defined. V, represents the velop independent expressions for the pickup or shedding
mean velocity of the fluid in a slug relative to the pipe wall. rate, x , and liquid holdup in a slug, R,. The mechanism for
The observed rate of advance of the slug, Vt, is the sum of pickup and shedding are quite different. This provides for
V, and the rate of buildup a t the front due to film pickup. independent relationships between the variables.
As discussed above, the slug length remains constant be- The Pickup Process. Refer to Figure 6. Consider a slug
cause the amount of liquid shed from the rear is identically whose outline is designated by the solid line and whose
equal to the amount which adds to the front. front is located at the plant A-A a t a specified instant in
To develop a relationship between these two velocities, time. In the interval A t , the front of the slug shown dotted
consider the overall balance between liquid entering the moves to plane C-C. The film, formerly located at AA,
pipe and that which leaves with a slug unit of length, l,, as moves only to BB because of its lesser velocity. The
it passes out of the pipe. The mass of liquid in a slug unit is amount of film shown cross-hatched is picked up and
+
(lsRs IfRf)ApL and the time for the slug unit to pass out mixed into the slug. Thus the mass rate of pickup is
of the pipe is l / u s . However, as the slug unit passes out of x = p L A R f , ( V , - vfJ (12)
the pipe, the slug which follows overruns and captures part
The Shedding Process. Consider the region of the slug
of the liquid in the film. This liquid does not move out with
behind the mixing zone. According to the model the flow in
the slug unit as calculated above. The mass of liquid picked
this region is equivalent to fully established pipe flow and,
up by a second slug during the time the first slug unit pass-
as seen in eq 3, the pressure drop is calculated as if a pipe
es out of the pipe is xl,/Vt. Since u, = Vt/lu, the material
flow turbulent velocity distribution existed there. The
balance becomes
mechanism for shedding can now be understood by refer-
W X ence to Figure 7 . The average velocity of the liquid in the
= (Z,R, + IfRf)v, -- (5)
APL PLA slug is distributed radially from a value of zero at the wall
Similarly developed, the gas phase material balance is to a value above V, a t the center. There is one specific radi-
al location where the local velocity, u , equals the average
velocity, V,. Designate this radial position as r p . At values
of r < r p the fluid moves faster than V,. Thus it advances
Adding eq 5 and 6 and simplifying yields for the slug trans- in the direction of flow with respect to the motion of the
lational velocity slug. But in the region r > r p (see cross-hatched area) the
fluid moves slower than the average fluid in the slug. Thus
it eventually is shed from the rear of the slug. This rate of
shedding is the mass rate of flow in the slug across any

340 Ind. Eng. Chem.. Fundam., Vol. 14, No. 4, 1975


plane drawn normal to the pipe axis less that which flows
in the area r < rp. .30 n
x = R,pLV,A -s,” 2avpLudr (13)

There exist well established relationships for the velocity 20


50 100 500
distribution for turbulent pipe flow in terms of the dimen- ~ e ,iIO-?
sionless parameters, u f and y + where
Figure 8. Relationship between C and slug Reynolds number.
u+ = -U‘ Y + - ’*’
- - ( y = R - r) (14)
u* ’ U

(15)
*E.-
Written in terms of these variables the equation for C be-
-
comes dxt
1 2 3
Figure 9. Definition of control volume in the film.

where y is the value of y + a t the pipe centerline. the film velocity, Vf, and the film holdup, Rf, as a function
of position from the rear of the slug (or of time since slug
passage).
Refer to Figure 9 and consider the principle of momen-
A well accepted equation for the central region of the pipe, tum conservation as applied to the control volume of fluid
y + > 30, in terms of these variables is which exist between plane 1 and 2 separated by dxf. The
1 pressure in the vapor space is constant snd independent of
u+ = A + - In y +
K
(18) x f as shown by experiment. Thus a balance in the xf direc-
tion is
where K is the von Karman constant. There exist some dif-
ferences in the literature concerning the values to be as-
signed to A and K . For this work we use A = 5.75, K = 0.38.
Note that a t u = V,

(u+),, = In this equation the momentum associated with the gas


phase is neglected since the density is small compared to
the liquid and its change in velocity across the control vol-
ume is small. P represents the average hydrostatic pressure
acting on the liquid over the liquid area which exists in the
plane normal to xf. This, of course, depends on the value of
while the pressure in the gas phase, P,, and the distance from the
surface to the center of pressure in the liquid.
cy = K [ ~ - A ]
= P , i-
pLgL 50 (22)
gC
There is now sufficient information to perform the integra-
tion of eq 16. Using smooth friction factors for smooth where .$ is the ratio of the distance from the surface to the
pipes all terms in the equation can be calculated once Re is center of pressure in the liquid to the diameter. F , is the
specified. force a t the pipe wall due to friction and this force tends to
The integrations, which are straightforward, were carried retard the flow. F , is the force due to gravity acting in the
out over the range 30,000 IRe, I400,000 and the resulting xf direction. With /3 the angle between the horizontal and
values of C are presented in Figure 8. I t is seen that, in ac- the axis (for up flow this angle is positive), then
cord with experiment, the value of C varies only slightly
over a wide range of Reynolds numbers. The integration of F , = pLg4 AR, (sin p ) dx (23)
gc
eq 16 is cumbersome to carry out but the relation between
Re, and C can be approximated by observing the near log- The subscripts 1 and 2 designate the planes to which the
linear relationship shown in Figure 8. For purpose of com- bracketed term applies.
putation the following equation is recommended If plane 1 and 2 are allowed to approach each other then
in the limit the momentum equation becomes
C = 0.021 In (Re,) + 0.022 (21)
Hydrodynamics of the Film. In developing the equa-
tion for the pickup rate a new parameter was introduced,
Rf,,the fractional pipe area occupied by film just before
pickup by a slug. As seen from eq 2 it is also necessary to 7wpw - g L R f sin p (24)
find Vf,, the film velocity a t this same point. Both of these gc PLA
quantities depend on the process of deceleration in the film T, is the wall shear stress and P , is the perimeter wetted
behind the slug after shedding takes place. In order to ar- by liquid film. Note that Vf designates a film velocity aver-
rive a t these quantities, the momentum balance is applied aged over its cross-sectional area, (RfA). In order to inte-
to the film. By making the application to a differential grate this equation, it is necessary to develop expressions
length of film, it will be possible to derive expressions for for T,, P,, E and a relationship between Rf and Vf.

Ind. Eng. Chem., Fundam., Vol. 14. No. 4, 1975 341


The Wetted Perimeter, P,: Let b' be the angle which
subtends the liquid in the film as shown in Figure 11. Then
by definition
OD
3 Pw = - (33)
2
Figure 10. Flow relative to the stagnation point, S.
Thus
2nBR
Re, = -
0
Re, (34)

The Distance to Center of Pressure on the Liquid, 4.


The force due to pressure is obtained by an integration of
the pressure over the liquid crossectional area and this re-
sult is
8 + -
[ - R , 71~ 02 c o s - 2 ./2 sin3 -
Figure 11. Definition of the angle, 8.
2 3
But the force in terms of the distance to center of pressure
Relationship between Vf and Rf.The profile of the is
film behind a slug appears as shown by the solid curve in
Figure 9. The curvature a t the top of the pipe is due to sur-
face tension. If surface tension were zero, then the curve
would be as shown by the dotted extension to point S. In Equating these two expressions and solving for E gives
fact, the forces due to surface tension are easily shown to be
1 8 1
small compared to the other forces acting and the shape of 4 = -- cos -
2 2
+ - sin3
3nR,
the film at the back of the slug is assumed to end a t the
point designated as S. Since the slug moves without a Note that Rf and b' are uniquely related by
change in length, S must move along the pipe a t the same
B-sint,
velocity as the front of the slug, namely Vt. Define a veloci- R, = (36)
ty, w, measured relative to the velocity of propagation of 2n
this stagnation point, S. Then at any point Substituting the equation for Vf in terms of Rf (28), and
the equations for T, (30), P , (34), and E ( 3 5 ) into eq 24
Wf = Vf - vt (2 5) gives, after considerable transformation and simplification
Let the coordinate system translate to the right a t this ve-
locity, Vt. The point, S, is then stationary and flow then
takes place relative to S as shown in Figure 10. A material
balance between flow across plane 3 and any other plane
drawn normal to the film flow is
WfRiPLA = W ~ R ~ P L A (26)
From eq 11 and 25 In this equation, Fr is the Froude number
v, - v, = cv, = -w, (2 7)
(38)
Substituting (25) and (27) into (26) and recognizing from
+
(11)that Vt = (1 C)V, provides the needed relationship and $ is the dimensionless distance measured from the
between Vf and Rf. stagnation point, S.

V, = V, [1 - C R1)] = SVs (28)


$ =
1, -
D
Xf
(39)
Wall Shear Stress, T ~ In. the film region the wall shear The variables are separated and integrated to give
due to liquid flow is estimated by assuming pseudo parallel
flows.
(4 Oa)
(29)
where
Substituting for Vf from eq 28 gives

(30)
W(R,) =

C2Rs2 - -
Ri2 Fr
[: 8
R, s i n 5
1 - cos 8
+ 8
sin2 -
;
- - cos-
The friction factor for the film is evaluated from smooth
tube f(Re) data with the Reynolds number of the film f f B 2O- + R Sin P
based on the hydraulic diameter n Fr
(4Ob)
(31)
Note that W is a function of Rf as given by eq 40b and
varies along the film. At xf = 0, just before pickup of the
nDR B (32) next slug, J. = lf/D and R f = Rf,. At point S, x = lf, J. = 0,
Re, = Re,
P W and Rf = R,. The profile for Rf vs. xf can be obtained from

342 Ind. Eng. Chem.. Fundam., Vol. 14. No. 4, 1975


sRs Rf
W(Rf)dRf =
1, -
D
Xt
(41)
Velocity of the Gas Phase. Consider a coordinate sys-
tem moving with the velocity, Vt. Now examine velocities
of the gas phase relative to this moving coordinate system
as shown in Figure 10 for the liquid phase. In order to satis-
The integration of eq 40a must be accomplished numerical-
ly and requires a value of lf. The procedure starts by evalu- fy continuity requirements
ating W at the upper limit and adding increments of hRf
until a value of Rf is produced for which the integral equals
lf/D. This value of Rf = Rf,.
The Length of the Slug, I,, and the Film Region, If.
The length of a slug unit is

(42)

and that of the film region is With some rearranging this equation becomes

(43) (45)

The length of the slug can be calculated from a material Note that for liquid slugs that are free of entrained gas, R,
balance on the liquid. The rate of liquid flow into the pipe = 1.0. Then the gas velocity equals the velocity of propaga-
is WL. Consider a plane normal t o the flow a t some position tion of the slug, Vt, at all positions behind the slug. When
downstream where fully developed slug flow exists. We R, is not unity, then the gas velocity varies slightly with
proceed by calculating the mass of liquid crossing the plane location. At the point of pickup, where Rf = Rf,, the gas ve-
in (a) the time it takes for the slug to pass, T,, and (b) the locity is
time it takes for the film to pass, Tf. The sum of these two
quantities is then divided by the time for passage of one (46)
slug unit, 1/uS.
M , = mass c a r r i e d in the slug = While the gas phase velocity has no influence on the pres-
sure drop it is important to the modelling of heat and mass
JOT’ V$RspLdt = vfiRsp,Ts transfer operations for slug flow.
Length of the Mixing Eddy, I,. The depth of penetra-
tion of the liquid film into the slug appears to depend on
the relative velocity between slug and film. This observa-
1 tion derived on physical grounds is verified from studies of
;
II, V&RgL9 high speed films and still photographs. The relative veloci-
vt
ty is (V, - Vfe). A simple and effective estimate can be ob-
Similarly for the film tained using the “velocity head” concept. This velocity
head is defined as
,!A! = Jo VfARfpLdt
Tf

VH = PL(’S - ‘fJ2
2sLgc
where SL is the specific weight of the liquid. Resistance to
flow in unusual geometries has been shown to be related to
the velocity head as is the trajectory distance of h fluid re-
leased from a nozzle. A convenient measure of each of these
From eq 28, VfRf = V,[Rf - C(R, - Rf)] quantities is the “number of velocity heads.” From the ob-
servations mentioned above a simple correlation emerges
1, = 0.3VH
Solving for 1, and rearranging gives
(47)
_ _wL
__
[ R f e ( l + C) - CR,]Z A Summary of Equations, Variables, and Procedure
1“ = PLA v, for Solution. In Table I the equations are listed in se-
%{R, - [Rf,(l + C) - CR,]Z} quence and the new variables which are introduced in each
vt are identified. Note that the variables appearing in the
where equation set are 16 in number, namely: AP,,APa, APf, x,

.fo’ R f ( l + C) - CR Vs, Vfe, Rs, L, if, L, Res, WL, WG,Vt, Rfe, us. The physical
= R f e ( l + C) - CR: (7) , MG) and the tube size and orientation
properties ( p ~p, ~ ML,
(D, A, p) are, of course, known. As shown, the number of
The relationship between R f and xf can be calculated from independent equations is 12. Thus four variables must be
eq 41. Such calculations indicate the Z approaches 1.0 for specified to effect a solution. W Land WGare input data. It
all flow conditions. This confirms what is observed in ex- has been shown (see section on “Description of Slug Flow”)
periment, that the film drops quickly to near its value of that the slug frequency is controlled by conditions near the
Rf, a t a short distance behind the slug and then continues entrance and is not coupled to the behavior of a slug. At
to decrease only slightly. With Z set equal to 1.0 this time no independent relationship exists for R,. Thus
the independent variables which are required as input to
the model are WL, WG,us, R,.
Despite the complex appearance of the equation set the

Ind. Eng. Chem.. Fundam.. Vol. 14, No. 4. 1975 343


Table I. A Summary of Equations and Variables Table 11. Computational Sequence
SEOUENCE EPUATION
NUMBER EPUATION
NO. I N TEXT
P L . P O , PLI D w ~ WG,
t RS. vs
I I
CALCULITE

2 2 C4LCULATE Vs

3 3
C4LCUL4TE
R e s Ea 4

4 4

S 8
'L' 'G

8 10

T = 0.021 In Re. + 0.022 C 21 *NUMERICALLY


Ea
INTEGRATE
A F R O M R , TO A
P LRSAVS
V A L U E OF R t e WHICH M A K E S
1NTEGR4L 1 ,/ D
+ ClVS
2
8 v, = v, +*A' (I 9. I1

4-7
9 40A

C4LCULATE 1 NOTE V I L U E S OF R f . V f . V s .
X i , C4N BE OBTAINED
B Y STORING THE INTER-

408 M E D l 4 T E V b L U E S OF
THE lNTEGR4L 4S THE
C A L C U L I T I O N PROCEEDS.

8: I - C [ v ] 20

34

36
tions. Standard deviations associated with these measure-
IO 44 "s ments are as follows: Vt = 8%; V, = 5%; Vf, = 22%; 1, =

I1 PI'
".
2 -1, 43
35%; hp, = 20%. Part of this deviation is due to the ran-
domness of the slug formation process with the result that
each slug is somewhat different in length with different as-
I2 l.'o.lslvs-vf,,~~ 47 sociated film velocities. In part, the deviation is due to
'L
error in measurement. Measurement error is estimated to
be: V, and Vt = 5%;Vf, = 15%; 1, = 25%; AP, = 15%.
approach to solution is quite straightforward and is accom- As indicated above, test of the model requires as input
plished readily by computer, given the required four input data values of the frequency, us and slug holdup, R,. Exper-
variables. In fact, only one calculation loop is needed due to imentally measured frequencies as obtained from slug
the coupling between eq 40 and 49. The block diagram of count are shown in Figure 12. In a future paper the slug ini-
Table I1 details the calculational procedure. tiation phenomena will be explored and a model will be
presented for predicting these data. In the meantime, if the
Comparison of Model Prediction with Experiment model presented here is to be applied to other conditions,
An experimental study of slug flow for an air-water sys- the correlation of Grescovich and Shrier (1972) is recom-
tem has been carried out in a horizontal smooth glass tube mended.
1.5-in. i.d. and 65-ft total length. The test section length Values of the slug holdup, R,, were measured using an
was made up of 8.5-ft pipe lengths joined in Plexiglas impact probe especially designed to follow the transient as
blocks which were carefully machined to match the i.d. a slug passed. A water filled, Ih-in. tube formed in the shape
with no discontinuities. Fast response pressure transducers of the impact tube of a pitot was placed at the centerline
were located in each block and connected to the flow chan- with the opening facing upstream. This tube was connected
nel through small drill holes kept full of water. A tee type to a sealed water reservoir located outside of the test sec-
entrance section was used with water introduced on the run tion into which was fitted a pressure transducer. A second
and air on the tee. Extensive experimental studies with transducer was located at the wall of the test section a t the
various entrance sections demonstrated that slug frequency plane of the mouth of the impact tube. Stagnation and
and other fluid characteristics are independent of the con- static pressure were recorded continuously during slug
figuration. flow. When the slug passed across the tube a sharp rise of
The following variables were directly measured over a momentum flux and impact pressure was observed. Since
wide range of liquid and gas rates, V,, Vt, Vf,, U sl,,, l,, the fluid velocity could be calculated and the liquid and gas
R,, us. Tabulated data may be found in Hubbard (1965) moved without slip, it was a straightforward matter to de-
along with detailed discussion of experiment techniques. termine p , and R , using the pitot tube equations. Results of
The measurements clearly demonstrated the stochastic these experiments appear in Figure 13. It should be noted
nature of the slug flow phenomenon. All the quantities that the detector was positioned a t the axis and radial gra-
above except for frequency displayed a range of values. Be- dients in air concentration exists. In addition, considerable
cause of this fact, repeated measurements were made over fluctuation in impact pressure with time was observed
the passage of many slugs a t each gas-liquid rate pair. making it difficult to determine the impact pressure char-
Sample mean values were calculated from 25-100 observa- acteristic of that slug. For these reasons considerable scat-

344 Ind. Eng. Chem., Fundam., Vol. 14, No. 4, 1975


c I I I

20 L 4. 15
14-
13
.

-
I:! r

Y
L.C"

0 01 02 03 04
WG ilb/sec)
2 3 4 5 6 7 B 9 IO I1 12 13 14 15 16 17

Figure 12. Slug frequency data of Hubbard (1965) MEASURED Vr

Figure 14. Comparison of theory with experiment: V,.


10

i
R,

075

>
-
a FLOW RATE OF
20
a WATER IN A 1.5" Q
4
Y) HORIZONTAL TUBE
Y
05
0 10 20 30
v,

Figure 13. Hubhard data for slug holdup. CALCULATED Vt

Figure 15. Comparison of theory with experiment: VT.

ter was observed and this is clearly evident in the data.


Fortunately, the predicted results from the model are not
especially senSitive to the value of R, used as input.
Theory vs. Experiment: V,. Values of V, were mea-
sured by removing the end of the tube and allowing the
slugs to flow out the end and then undergo a free fall tra-
,--.
$19
jectory to the floor. Knowing the centerline height of the W
w
0
test section and measuring the horizontal distance from the 3
end of the test section to the point where floor contact was $ 0 4 FLOW RATE OF
Y
I WATER IN A 1 5 ' D
made, the velocity of the slug as it left the tube could be HORIZONTAL TUBE
calculated from well established trajectory equations. A 0 2 0 3 31 I b / $ e c

comparison of measured values of V, with values calculated


from the model, eq 8, appears in Figure 14 where agree- 0
ment is seen to be excellent. 0 0 2 0 4 06 OB 10

Theory vs. Experiment: Vt. Electrical contact probes CALCULATED (?)


were located 8.5 f t apart in the last two Plexiglas blocks of Figure 16. Comparison of theory with experiment: Vf,.
the test section. These probes were introduced into the top
of the block and penetrated only Y 4 - h into the test section.
The circuits were such that when the front of a slug passed,
the conducting water closed a circuit which started a timer. with time since the last slug passed and this is in accord
When the front of the same slug reached the next contact with the prediction of the model. This distance was record-
probe the timer was stopped. In this way the rate of ad- ed just before the next slug left the pipe and values of Vf,
vance of the front of the slug, or Vt, was measured. were calculated.
Equation 21 was used to calculate C as predicted from Values of VfJV, can be predicted from the model using
the model and Vt was then calculated from eq 15. A com- eq 28 with Rf, calculated from eq 40a. A comparison of cal-
parison of predictions of the model and experiment appear culated and measured values of this ratio appear in Figure
in Figure 15. Again agreement is seen to be excellent. 16. There appears to exist a small systematic error with
Theory vs. Experiment: Vfe.Experimental values of measured values being 10-15% lower than calculated ones.
Vf, were obtained by observing the trajectory of the film as In these measurements air resistance was not considered in
it flowed out of the end of the pipe in free fall in the man- the trajectory equation and as a result the values of Vf, will
ner similar to that described above for V,. It was observed be somewhat higher than those indicated here. Considering
that the horizontal distance reached by the film decreased the fact that there exists some controversy on correct rela-

Ind. Eng. Chem., Fundam., Vol. 14, No. 4, 1975 345


Conclusion
I SOLID LINES INDICATE PREDICTION
OF MODEL A model has been presented which can predict the de-
tailed structure of slug flow, given flow rates, fluid proper-
ties, tube geometry and inclinations, and measured or pre-
dicted values of slug frequency and slug liquid holdup. In a
future paper prediction of v, and R , will be discussed.
Notation
WATER IN A I 5 " D
HORIZONTAL TUBE A = cross-sectional area of the pipe
A f = cross-sectional area of the film
C = ratio of rate of mass pickup to rate of mass flow in the
0
0 5 IO IS 20 25 30 35
slug (see eq 10)
D = pipe diameter
", f s = friction factor for the slug
Figure 17. Comparison of theory with experiment:slug length. f f = friction factor for the film
F , = force acting on an element of film in the flow direction
due to gravity
F , = force at the pipe wall acting on an element of film in
the flow direction due to friction
g, = conversion factor
gL = acceleration of gravity
12 = Von Karman constant
1, = length of slug
n- l f = length of film
P 1, = length of slug unit
U
0 lm = length of mixing eddy
Y
a P = average hydrostatic pressure acting on film cross-sec-
VI
2 tional area
n P, = perimeter wetted by the film
m
J
AP, = pressure drop due to acceleration across slug
APf = pressure drop due to friction across slug
U s= pressure drop across slug
r = radial coordinate
0 10 20 30
Rf = fraction of pipe flow area occupied by film
", R f , = fraction of pipe flow area occupied by film just before
pickup
Figure 18. Comparison of theory with experiment: U s . R, = fraction liquid holdup in the slug
Ref = Reynolds number of film
Re, = Reynolds number of slug
SL = specific weight of the liquid
tionships to predict wall shear for open channel flow, this is Tf = time for passage of a film
very good agreement indeed. T , = time for passage of a slug
Theory vs. Experiment: Slug Length 1,. Slug length u = local velocity
was measured using a single electrical contact probe de- u* = friction velocity
scribed for the determination of Vt. In this case a counter u+ = dimensionless local velocity (See eq 14)
Vf = average velocity of fluid in the film
was started when the nose of the slug contacted the probe Vf, = average velocity of fluid in the film just prior to pick-
and was stopped when the contact was broken as the back up by the next slug
of the slug passed over the probe contact. Using this time V, = average velocity of fluid in the slug
interval and the measured value of Vt it was possible to cal- Vt = average translational velocity of the nose of the slug
culate an experimental value of l s . Because of the highly W , = gas mass flow rate
aereated nature of the front of the slug an accurate deter- WL = liquid mass flow rate
mination of arrival time was difficult. Furthermore, ran- W = grouping of variables (see eq 40b)
domness in the system is particularly evident in slug y = distance coordinate measured from the wall
length. y+ = dimensionless y (see eq 14)
1: = rate of mass pickup by slug
A comparison of predicted slug length from the model a = defined by eq 20
(solid lines) and the measurements (data points) appears in /3 = angle between pipe axis and the horizontal
Figure 17. Despite difficulties in measurement the agree- y = value of y c at y = R
ment is within experimental error and the correct trend is 0 = angle which subtends the liquid film (see Figure 11)
observed. p~ = viscosity of gas
Theory vs. Experiment: AP,. For each flow condition p~ = viscosity of liquid
pressure traces were recorded similar to those of Figures V, = slug frequency
4-6 and from these AP, was measured for 25-50 successive 5 = ratio of the distance from the film surface to the center
slugs and an average calculated. AP,,from the model is of pressure to the tube diameter
p~ = density of gas
predicted eq 1, 2, and 4 as indicated in Table 11. A compari-
p~ = density of liquid
son of experiment with the prediction of the model appears w = velocity measured relative to Vt (see eq 2 5 )
in Figure 18. There is a weak dependence of predicted
values on the liquid rate through the appearance of WL in Literature Cited
eq 42. For almost all conditions agreement between predic- Baker, O., OilGas J., 185 (July 1954).
tion and experience is within 20%. Considering that these Bonnecaze. R. H., Erskine, W., Grescovich, E. J., AlChEJ., 17, 1109 (1971).
Bretherton.F. P.. J. NuidMech.. 10. 166 (1961).
difficult transient measurements are within this accuracy Cox, B. G., J. FluidMech , 20, 13 (1964).
the agreement seems to be very good indeed. Dukler, A. E.,Wicks, M., Cleveland, R. G., AlChE J., 10, 44 (1964).

346 Ind. Eng. Chem., Fundam., Vol. 14, No. 4, 1975


Goldsmith, H. L., Mason, S.G.. J. ColbidSci., 18, 237 (1963). Kordyban, E. S., Trans. ASME, 83, 613 (1961).
Govier, G. W., Omer, M. M., Can. J. Chern. Eng., 40, 93 (1962). Kordyban, E. S..Ranov, R . R., "ASME Mukiphase Flow Symposium," p 1,
Greskovich. E. J.. Shrier, A. L., lnd. Eng. Chern.. Process Des. Dev., 11, 317 1963.
(1972). Marruci, G., Chern. Eng. Sci.. 21, 718 (1966).
Hewitt, G. F., Hall Taylor, N.S. "Annular Two Phase Flow" Pergamon Press, Martinelli, R. C., Nelson, B. D., Trans A S K , 70, (1948).
1970. Neal, L. G.. "An Analyses of Slip in Gas-Liquid Flow" Report of lnstitutt for
Hoogendoorn, C. J., Chern. Eng. Sci., 9, 205 (1959). Atomenergi, Kjeller Res. Est. (1963).
Hoogendoorn, C. J., Welling, W. A. "Symposium on Two Phase Flows," E x 6 Nicklin, D. J., Wilkes, J. O., Davidson, J. F., Trans. lnst. Chern. Eng., 40, 61
ter, 1965. ( 1962).
Hubbard, M. G.. Ph.D. Thesis, University of Houston, 1965. Oliver, D. R., Wright, S.I., Brit. Chern. Eng., 9, 540 (1964).
Hubbard. M. G., Dukler, A. E., "Proc. 1966 Heat Transfer 8 Fluid Mech. Richardson, B.,Argonne National Laboratory Report ANL-5949 (1958).
Inst.," M. A. Saad and J. A. Miller, Ed., Stanford University Press, 1966. Suo, M.. Trans. ASME, J. Basic Eng., 90, 140 (1968).
Hubbard, M. G., Dukler, A. E., paper presented at the AlChE National Meet- Suo, M., Griffith, P., Trans. ASME, J. BasicEng., 86, 576 (1964).
ing, Tampa, Fla.. 1968. Vermuellen, L. R., Ryan, J. T., Can. J. Chern. Eng., 49, 195 (1971).
Hughmark, G. A,, Chern. Eng. Sci., 20, 1007 (1965).
Johnson, H. A,, Trans. ASME, 77, 1257 (1955). Received for review February 5,1975
Kosterin. S. I., lzv. Ak. Nauk SSSR, Otd. Tekh. Nauk, No. 12, 24 (1949). Accepted June 5,1975

Nonideality of Binary Adsorbed Mixtures of Benzene and Freon-I 1 on


Highly Graphitized Carbon at 298.15 K

Earle D. Sloan, Jr. and J. C. Mullins'


Chemical Engineering Department, Clernson University, Clernson, Sooth Carolina 2963 1

Experimentaladsorption isotherms of binary gas mixtures of benzene and Freon-11 are presented for compari-
son with predictions by the ideal solution theory and by a two-dimensionalvan der Waals equation of state. The
homogeneous carbon black, Sterling MTFF-D-7 (310OOC) with a surface area of 9.6 m2/g, was the adsorbent.
A commercial electrobalance was used to measure both mixture isotherms at 298.15 K below 10 Torr and
pure component isotherms at 273.15 K and 298.15 K at pressures up to 125 Torr. A chromatographic tech-
nique was used to correct the mixing rule for the energy parameter crii The calculated isotherms, using the
corrected mixing parameter for the van der Waals equation, are shown to agree with the experimental iso-
therms. A small departure from the ideal adsorbed solution theory was found.

Introduction N
A
Many theories of adsorption such as the early BET theo- - -dd.rr
n
+ 2
i=l
xi dpia = 0 (constant T ) (1)
ry (Brunauer et al., 1938) and a more recent theory by Lee
and O'Connell (1972) assume sitewise homogeneity for the The chemical potential of species i in the ideal gas mixture
adsorbent. In spite of this basic assumption there is a pau- is given by
city of data for adsorption equilibria of mixtures on either
sitewise homogeneous adsorbents or adsorbents with a ho- pig(^, p , y i ) = G i o ( T ) + RT In P y l ( 2)
mogeneous field. The basic difficulty is that the composi- Since a t equilibrium the chemical potential of component i
tion of the adsorbed phase, which is frequently less than a is equal in the adsorbed and gas phases, the differential of
monomolecular layer on a relatively small (e.g., 10 m2/g) eq 2 may be substituted into eq 1 to obtain a useful rela-
surface area, must be determined. Friederich and Mullins tion.
(1972) obtained data for ideal mixtures of similar molecules
using an equilibrium calculation method suggested by Van --A d n + d l n P +
Ness (1969). The purpose of this paper is to present a dif- nRT
N
ferent method for determining homogeneous absorbent ( x i d In y i ) = 0 (constant T ) (3)
mixture equilibria and to extend the mixture data available i.1
to include components which exhibit nonideality in the
monomolecular layer region. If eq 3 is restricted to constant gas phase composition, a
means for calculating spreading pressure results
Adsorption Equilibrium Relations P
Two equilibrium relations have been used here in the = n d(ln P) (constant T and y i ) (4)
measurement of mixture equilibria on homogeneous adsor-
bents: a modification of the Gibbs-Duhem relation for the In eq 4 the number of moles adsorbed may be determined
adsorbed phase and a relation for determining infinite dilu- by the mass adsorbed and an average molecular mass
tion activity coefficients by a chromatographic technique.
Gibbs Adsorption Isotherm. The Gibbs-Duhem rela-
tion for a two dimensional adsorbed film, restricted to con-
stant temperature, is known as the Gibbs adsorption iso-
therm (Van Ness, 1969) i=1

Ind. Eng. Chem., Fundam., Vol. 14, No. 4, 1975 347

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