Karabelas - Liquid - Liquid Droplet Size Distribution PDF
Karabelas - Liquid - Liquid Droplet Size Distribution PDF
Karabelas - Liquid - Liquid Droplet Size Distribution PDF
Savino, “An Analysis of the Transient , “Die asyrnptotischen Losungen fur Vorgange
Solidification of a Flowing Warm Liquid on a Convectively des Erstarrens,” Intern. I. Heat Mess Transfer, 19, 597
Cooled Wall,” Proc. 3rd Intern. Heat Transfer Conf., Vol. 4, (1976).
pp. 141-151, Chicago, 111. ( 1966). Tao, L. C., “Generalized Numerical Solutions of Freezing a
Stephan, K., “Influence of Heat Transfer on Melting and Solid- Saturated Liquid in Cylinders and Spheres,” AIChE J., 13,
ification in Forced Flow,” Intern. J. Heat Mass Transfer, 12, 165 ( 1967).
199 (1969).
-, and B. Holzknecht, “Warmeleitung heim Erstarren
geometrisch einfacher Korper,” Wurme-und StofFiibertragung, Manuscript received December 6, 1976; revision received September
7,200 ( 1974 ). 27, and accepted October 12, 1977.
Reliable estimates of the distribution of droplet sizes Sleicher (1962) predict maximum droplet sizes d,,, in
in flowing liquid/liquid dispersions are required in many turbulent pipe flow, which differ almost by an order of
areas of chemical engineering practice, for example, in the magnitude for flow conditions and liquid properties of
design of chemical reactors and of physical separation practical interest. Moreover, according to the Hinze model,
processes. At present, it is impossible to make such a priori d, is approximately inversely proportional to the mean
estimates even in common problems, including pipe flow velocity whereas in the Sleicher correlation, d,, varies
of dilute dispersions, owing to insufficient information with u - 2 . 5 . It is clear, therefore, that in the problem con-
about the effect of flow conditions on the size spectrum. sidered here, the literature provides very little guidance of
Collins and Knudsen (1970) have published the only questionable reliability.
available drop size distribution data, obtained in well-
The need to describe dispersions of water in flowing
defined turbulent pipe flow with water as the continuous
hydrocarbons provided the motivation for this work. The
phase. These authors reached a rather disturbing conclu-
main objective was to make accurate measurements of
sion, namely, that their data did not conform to any of
droplet size spectra generated in turbulent pipe flow. In
the presently available distribution functions, such as the
lognormal, upper limit log-normal, etc. In order to in- the absence of a satisfactory theory, such measurements
terpret the measured size spectra, Collins and Knudsen are necessary in order to select the most representative dis-
developed a computer aided stochastic model by postu- tribution function and to study the influence of flow con-
lating a breakup mechanism in which the maximum stable ditions and liquid properties on some physically significant
drop size d,, is a basic input parameter. However, the parameters of the size spectrum, for example, the Sauter
presently available correlations due to Hinze (1955) and mean a2 or the maximum droplet diameter d,,.
PREVIOUS WORK tively short test section of 3.81 cm ID which were not
in agreement with predictions based on Equation ( 5 ) . A
Basic studies of droplet breakup in homogeneous and transient type of technique was employed in these tests;
isotropic turbulent flow were first presented by Kolmo- that is, large drops of equal size were first introduced into
gorov (1949) and Hinze (1955). The main assumption in the pipe when the flow rate was very small, and then the
these studies is that drop fragmentation is caused by flow was accelerated, very fast, to the desired higher
dynamic pressure forces, due to rapid turbulent fluctua- level. It was considered that the maximum stable diame-
tions in the vicinity of the drops, which overcome inter- ter d,,, had been obtained when less than 20% of the
facial tension forces. The mean square of velocity fluctua- photographed drops had diameters smaller than the
tions z, over a distance equal to the drop diameter d, original size. Data obtained by Collins (1967) suggest
provides a measure of the dynamic pressure forces. There- that the line length used in this study may have been
fore, an estimate of the maximum stable drop diameter insufficient (6.7m or l'i6 pipe diameters of fully devel-
dma,can be obtained from the condition oped flow) for the large drops to reach a stable maximum
size.
Pr 3 4u
-=c'- (1) Sleicher took into account viscous forces and correlated
2 &ax his data by the following expression
For an isotropic and homogeneous flow field, it has been
shown that z i s proportional to ( ~ d ) 2 / if3 the length d
is much greater than the Kolmogorov microscale TJ =
(6)
( v3/6) lI4. It follows that
which is very different from Equation ( 5 ) . For instance,
it suggests that d,,, is independent of pipe diameter,
which is in sharp contrast to the dependence of
Equation ( 5 ) . Paul and Sleicher (1965) published later
where the constant C must be determined from experi- a few data points taken in a 1.27 cm ID pipe, which
mental data. Hinze (1955) interpreted data taken by showed only a slight diameter effect (d,,, cc D-".'). The
Clay (1940) in a Couette flow field and obtained the constant C = 43 in Equation ( 6 ) gave a better fit of these
value C = 0.725 corresponding to dg5.The main assump- data than C = 38. In subsequent calculations with this
tions made in the derivation of Equation ( 2 ) are, of equation, the value C = 40 will be used.
course, open to criticism. For instance, turbulent shear Levich (1962) provides an interesting discussion of
fields of practical interest are far from isotropic and homo- drop fragmentation mechanisms in his book and reviews
geneous. Nevertheless, Equation ( 2 ) has been found to related Russian work. He points out that the Kolmogorov
describe quite satisfactorily experimental data obtained model can give good estimates of stable drop diameters
in agitated vessels; see, for example, Mlynek and Resnick in the core of turbulent pipe flow but not in the region
(19i2), Shinnar (1961), and Sprow (1967). close to the wall, In this region of large velocity changes,
In order to estimate d,,, or dg5 in pipe flow, the mean much smaller drops will develop, with the smallest drop
rate of energy dissipation per unit mass of fluid Tmay be size to be found at the edge of the sublayer where
used
(7)
(3)
Obviously, during the transient period of dispersion for-
with the friction factor calculated from the Blasius equa- mation in a pipe, the drop diameter will vary between a
tion for smooth Ltmes
L maximum, possibly given by the Kolmogorov-Hinze model
0.0791 for the core, and a minimum resulting from fragmentation
f=- (4)
Re114 at the wall, as suggested by Levich. At present, it is im-
possible to predict the equilibrium drop size distribution
and the constant C = 0.725 obtained in Couette flow. The as a function of flow conditions and liquid physical prop-
result is erties, and accurate experiments are necessary to gain
some insight into this problem.
Collins and Knudsen (1970) have published the only
available drop size distribution data,' obtained in a 11.3
where We = ( DpeT2)/ ( U ) is a dimensionless Weber num-
0 AAer this paper was submitted for publication, a similar study
ber based on the pipe diameter D and mean velocity was published by Kubie and Gardner (1977). These authors, using a
Equations ( 2 ) and ( 5 ) will be reexamined in this paper photographic technique, measured drop size spectra but mede no at-
tempt to correlate them. They did conclude, however, that the mea-
and compared with data obtained in our study. sured maximum drop sizes were in good agreement with the Hinze
Sleicher (1962) made measurements of dmax in a rela- correlation [Equation (5)l.
DESCRIPTION OF EXPERIMENTS
Fig. 1. Schematic of flow system.
Flow Loop
A schematic of the flow system is shown in Figure 1. The test A sampling vessel (No. 8, Figure 1) was made out of a
section was made of acrylic pipe sections, with very smooth transparent acrylic pipe section, -1.15 m long, with an inside
joints, and had a total length of -32.3 m. The true inner di-
ameter was 5.04 cm. Fluid was circulated by a rotary type of
pump (manufacturer Bowie Company, 500 series). A Schroeder
diameter of 13.9 cm. This vessel was equipped with a gau e
and a regulator (11) in order to adjust the pressure and wit a-
draw fluid from the pipe under nearly isokinetic conditions. It
LF-1 in-line filter (No. 2, Figure 1) was installed at the dis- was filled up to about 7'0% of its capacity with kerosene con-
charge end of the pump to remove small particles or droplets. taining 0.2% wt dissolved terephthaloyl chloride. This com-
A pressure relief diaphragm ( 3 ) and a pulsation dampener ( 4 ) pound was first dissolved in 300 to 400 cm3 of carbon tetra-
were necessary to protect the pipe against pressure surges and chloride and then mixed with an appropriate amount of kero-
to eliminate flow pulsations, respectively. A calming section ( 5 ) , sene. The short sampling tube had a conical end ( 9 ) , immersed
made of a 15 cm I D pipe, served the dual purpose of dis- approximately 2 em into the fluid, in order to reduce the dis-
engaging gas bubbles from the fluid and providing a uniform charge velocity of the droplets into the vessel, thus increasing
stream into the main line. their settlin time. Upon contact of the droplets with the
A special water injection facility ( 6 ) was used. Water was sampler fluii, the piperazine dissolved in the water reacted
released at a steady rate ( 5 to 12 cm3/s) into the main stream, with the terephthaloyl chloride forming a protective coating.
through a 6 mm steel tube, Under these conditions, that is, low The bottom of the vessel was covered with a layer of viscous
relative jet velocity and fairly large jet diameter, it is expected silicone oil ( Dow Corning 200, 10100 centistokes) approximately
that the jet breakup is controlled almost entirely by the tur- 7 mm thick. The function of this layer was twofold: to terminate
bulence in the main stream. Moreover, it is reasonable to the reaction between droplets and the continuous phase which,
expect that the largest droplets developing upon disintegration beyond a certain time, tends to produce rough coatings on the
of this jet are greater than the ultimate maximum stable droplet surfaces and to result, occasionally, in agglomerates; to
diameter generated by the pipe flow; that is, the process of prevent water wetting of, and droplet sticking onto, the bottom
breakup continues downstream of the injection tube. Experi- plate and to preserve the spherical shape of the settled drops.
ments by Collins (1967) with similar injection tubes, and The density of the silicone oil was between that of kerosene
larger main flow velocities than those of our experiments, show and water. The bottom of the vessel on which droplets de-
exactly this trend. posited was made of optical quality, thick glass plate. As
Pictures of the flowing dispersion were taken at a special indicated in Figure 1, the lower section of the sampling vessel
test section ( 7 ) , and samples were withdrawn simultaneously ( 1 0 ) could be disengaged by using a Victaulic connector.
through a short 1.14 cm ID tube, located approximately 29 This short section was transferred to a stand without disturbing
and 30 m, respectively, downstream of the injection point. the already settIed drops, and pictures were taken from the
The center line of the sampling tube was approximately bottom.
1.45 cm below the pipe center line. This technique was in general very satisfactory. Sampling
A IIalliburton turbine meter ( 1 2 ) was used to monitor the over a period of 3 to 5 s provided a sufficiently large number
flow rate. TWO: a l p steel tanks were employed. One of them of droplets which were distributed on the bottom plate without
(14) was connected to the suction side of the pump and con- excessive crowding and overlapping. Pictures with total magni-
tained clean fluid; the other (13) was used only to collect the fication five to twenty-three times the real object were used to
contaminated fluid while water was injected into the system. measure droplet size distributions under various pipeline flow
This arrangement prevented reentrainment of water droplets conditions. Usually all the droplets in a picture were measured
into the test section. with an accurate ruler under additional magnification. In most
Droplet Size Measurement Techniques cases more than one picture was used to obtain a total count
Droplet Encapsulation. With this method it is possible to of more than 300 drops.
prevent droplet coalescence and preserve the size distribution, Photographic Technique. During the tests with kerosene,
in a properly taken sample, as follows. A protective coating is photographs of the dispersions were taken, concurrently with
formed quite fast on the surface of each droplet, when a small the droplet encapsulation data, in order to compare the two
quantity of a certain monomer, present in the dispersed phase, techniques. A test section very similar to that used by Collins
comes in contact with another monomer dissolved in the con- (1967) was located approximately 0.8 m upstream of the
tinuous phase. Recently, Mlynek and Resnick (1972) suc- sampling tube. Two diametrically opposite holes were drilled
cessfully employed this technique to measure drop size dis- with their centers on the vertical axis of the pipe. Optical
tributions in an agitated vessel. The reacting compounds in quality glass disks were mounted essentially flush with the
their experiments were 0.05% wt piperazine in the aqueous, pipe surface and held in place by a Plexiglas collar.
continuous phase and 0.05% wt terephthalic acid chloride in The camera was focused at a distance of 6.4 mm from the
the dispersed phase, which was a mixture of carbon tetrachlo- inner pipe surface. The viewing ports and camera were aligned
ride and iso-octane. The same additives were used in our study. on an axis approximately 15 deg from the vertical pipe diameter.
A concentration 0.75% wt anhydrous piperazine dissolved in A General Radio Strobotac, type 153-AB light source was
deirnized water gave the best results. Indigo-caramine dye was located diametrically opposite to the camera, 23 cm from the
added to the water to obtain a deep blue color before injection pipe. The flash duration was -0.5 +s. A Nikon F camera was
into the line. Two different liquids, that is, kerosene and used with 1.4 Nikon lens and a specially made 43 cm extension
viscous ti-ansformer oil, were used as the continuous phase. between camera body and lens to obtain the desired magnifica-
tion. The camera setting was F-4 at 1/30 with F X synchroniza- quired for droplet encapsulation. Interfacial tension measure-
tion. Panatomic X film was used and developed in HC-110 ments with a DuNouy tensiometer gave the following results:
mixture B. The negatives were enlarged six times and prints
were made on Polycontrast F pa er. Kerosene/water u = 33.1 mN/m at 22.8%
The same type of camera an{ film were used to photograph 31.7 mN/m at 24.4"C
the samples of encapsulated droplets. Nikon bellows and a Trans. oil/water u = 35.0 mN/m at 17.8"C
Nikon F-2 lens were employed. A camera setting of F-4 gave 33.7 mN/m at 23.3"C-
the best depth of field and sharpness in this case. In order to 32.7 mN/m at 26.7"C
light the sample tray, a photo-flood was mounted 0.6 m above Experimental conditions are summarized in Table 1. Mean
the sample. The light was filtered through a sheet of diffusion velocities varied between -1.2 and 3.0 m/s. After a pipeline
paper located 30 cm above the sample. flow rate was selected, the water injection system was adjusted
Experimental Conditions to provide a steady injection rate of 0.20% by volume. Only
Experiments were carried out with kerosene (Dispersol by in runs No. 12 and 15 the water volume concentration was
Shell Oil Company) and a more viscous transformer oil 0.26% and 0.16%, respectively.
(Texaco Transformer Oil No, 55) as continuous phases. The Samples and line photographs were taken simultaneously.
dispersed phase was deionized water with the additive re- The raw data obtained from direct droplet size measurements
were digitized and processed in the computer. In order to
obtain size distributions and-&2, size intervals of 100 pm
( u p to 1000 pm) and 200 pm (above 1OW pm) were
selected.
-
- 001
- 005
- 010
- 0 20
- 030
- 040 >
- 0 50 z.
- 060 0
;
0
- 010 2
LL
- 080 UJ
I
- 085 3
- 090 2
0
1
c
- 0 9 5 43
2
3
0
01 02 05 1 2 5 10
v = exp [- (;)n] 0 05
0 10
070
to any other characteristic diameter to specify the distri- L'
3
bution. If do5 is used, Equation (8) becomes +-4 080
3
0 95
An equally good, and in many cases better, fit of the
data presented here is obtained by the upper limit log- 0 98
probability function, suggested by Mugele and Evans 0 99
(1951). The volume distribution function in this case is 0 995
given as
d(1-VV)
--6 exp(-
- S2z2) (10) 01
1 1
02
I 1
04
I
06
I I I l l
1
1
2
1
4
1 1
6
dz G d/(d,,,-dl
and upon integration Fig. 4. Drop size distribution of water in kerosene, represented by an
1 upper limit log-probability function. u=
2.98 and 2.22 m/s.
exp( - x2)dx = - [I - erf(Sz)]
2 the data. Drop size distribution parameters for all the
(11) runs made with water-in-kerosene dispersions are sum-
where
z=~n[ ad dl marized in Table 2. This table also includes &, calcu-
lated directly from the raw data, as well as the diameter
of the largest drop in a sample.
dmax -
and
a=
&ax - d50
d50
Three parameters are required to specify this distribution,
that is, dmaX,
a, and S, and can be obtained from the data R U N 45
as
&ax - d50(d90 + dl0) - 2d90dlo 0 05
-- (14)
d50 d502 - dgodio > 010
and 2
S=
0.394 ; 020
[ ""1
0
2 030
log10 LL
050 Lu 040
I
3 050
where ui = di/(d,,, - di) . Given the three parameters,
9 060
the Sauter mean diameter 2 3 2 , and dy5 are calculated as Lu
2 070
F
&,X 5 080
T2 = (16) 3
I
2 090
and 0 95
0 98
a
d95 = 0 99
Rosin-Rammler
Run number
-U , m/s
Velocity
a
Upper limit log-normal distribution
6 &ax, pm
distribution Data
3s 2.98 1.174 0.915 1074 808 416 2.90 820 407 756
5s 2.57 1.339 0.827 1404 1057 479 2.53 1075 455 1111
6s 2.22 1.163 0.965 2087 1547 828 3.07 1550 794 1547
7s 1.84 1.535 0.809 3600 2638 1108 2.31 2650 1066 2603
lso 1.52 0.938 0.953 4767 3733 2133 3.30 3800 2083 4242
2s 1.52 1.495 0.881 5338 3814 1743 2.52 3850 1887 4310
4s 1.18 1.269 0.845 5491 4 158 1960 2.58 4250 1942 5172
Arithmetic average 1.329 0.874 2.65
/
- 005
0 05
-0 10
- 020
-030 ,
-040 .
z
-050 0
- 0 6 0 I-v
Q
-070 E
UI
-000 5
-085 6>
- 090 2
-
+
I:
-095 2
3
V
- 098
O '
0.005 O F /" I I I 1 1 1 1 1 I I
1
I
0'99
0.995
01 02 05
d/(d,,, di
1 2
TABLE
4. DROPSIZE DISTRIBUTION
PARAMETERS FROM DATA WITH VISCOUSCONTINUOUS
PHASE (TRANSFORMEROIL). DATAOBTAINED FROM SAMPLES
Rosin-Rammler
Run number
Velocity
-
U, m/s a
Upper limit log-normal distribution
6 dmax,pm d95, clm
-
d32, ~m
Data
&z, fim dmaxt, pm n
distribution
d95, pm
11s 3.00 1.369 0.818 1030 775 345 347 730 2.42 790
17s 2.60 1.286 0.888 1 097 814 397 401 951 2.73 825
10s 2.24 1.231 0.914 1383 1 028 520 512 1110 2.82 1045
18.5 2.08 1.819 0.792 1 579 1113 426 428 1217 2.13 1130
15s 1.86 1.283 0.839 2 009 1521 710 700 1381 2.54 1540
14s 1.52 1.230 0.858 2 498 1896 916 840 1805 2.63 1935
12s 1.19 1.573 0.828 2 625 1 894 804 844 1987 2.34 1925
ArithMetic average 1.399" 0.848 2.51
.I
-
----
dgS/D = 4.0
HINZE. EQUATION 15)
SLEICHER, EQUATION ( 6 ) I
sured d95 from Equation (5), at velocities smaller than
2.4 m/s. As shown elsewhere (Karabelas, 1977), if the
carrier liquid viscosity is small, the largest droplets tend
to concentrate at the bottom of a horizontal pipe at low
velocities. This tendency may have affected our data as
follows:
1. Since the sampling tube was located below the pipe
center line, the samples became less representative of the
average distribution with decreasing flow rate. The con-
sistently greater deviation of d95 from the predictions of
Equation (5) with decreasing flow rate, shown in Figure
10, is indicative of this effect.
2. The increasing mean concentration at the pipe bot-
tom, with decreasing flow rate, coupled with a possible
velocity lag of the largest droplets, may have promoted
coalescence and formation of drops somewhat larger than
01 110 12 14 16 18 20 22 24 26 28 30 those encountered in dilute, homogeneous dispersions.
At this point we must conclude that the Hinze/Kol-
MEAN VELOCITY, G, mls
mogorov model is more reliable than the Sleicher correla-
Fig. 9. Effect of velocity on maximum drop diameter. W a t e r dispersed tion because it has a more solid theoretical basis and it is
in transformer oil (uC = 14.2 to 20.5 mm2/s). generally in better agreement than Equation (6) with the
data presented here. Next, we shall briefly review the con-
ditions under which this model [Equation ( 2 )] applies to
pipe flow. In particular, we shall examine whether the
mean rate of energy dissipation; substituted into Equa-
tion ( 2 ) , provides satisfactory estimates of d, or d95.
The mam assumption involved in the development of
Equation ( 2 ) is that the flow is homogeneous and iso-
tropic. In such a case, most of the kinetic energy of turbu-
lent fluctuations is contained in the range of wave numbers
(inertial subrange) where the Kolmogorov distribution
law is valid. As is well known (see, for example, Tennekes
and Lumley, 1972), the same law describes energy distri-
bution in the inertial sublayer of pipe flow, that is, at y+
greater than 30 to 35 where Equation ( 2 ) is expected to
be valid. If the Blasius Equation (4)is employed to esti-
mate ti*, y + = 35 corresponds to a distance from the wall
PIPELINE
---- dg$3 = 4 0 We-'
--- SLEICHER, EQUATION ( 6 ) where R is the pipe radius. Figure 11 shows that, for a
given pipe diameter, the thickness of the buffer layer is
greatly reduced at high Reynolds numbers; that is, the
lower boundary of the inertial sublayer is very close to the
wall. For example, in a 25.4 cm ID pipe at Re = lo6,
Fig. 10. Effect of velocity on maximum drop diameter. W a t e r dispersed the inertial .sublayer (3' N 35) is within 250 p from the
i n kerosene (vC = 2.2 to 2.3 mm2/s). pipe wall.
-
Reynolds numbers, the largest droplets, of relative size
d,,,/D, that can survive at a distance from the wall
y/Rbmay be comparable in size or larger than the thick-
Collins' data, plotted in terms of cumulative volume
fractions, can indeed be fitted with a Rosin-Rammler or
101
ness of the buffer layer, but they are small compared to
y/RI, These droplets can move deeper into the inertial
sublayer, that is, closer to the wall, where the local energy 5
= 35 have a common point of intersection. Fig. 11. Effect of Reynolds number on wall layer thickness and on
-
Substituting Equation (22) into (21), we obtain of €local = E.
IOCUS