I L. D. SMOOT, 6. W. MAR,' and A. L.
BABB
Department of Chemical Engineering, University of Washington, Seattle, Wash.
Flooding Characteristics and
Separation Efficiencies of Pulsed
Sieve-Plate Extraction Columns
Experimental Data Applied to Design of Extraction Columns
This article details equations and gives nomographs for calculating
flooding velocities and over-all transfer unit heights
P U L S E D sieve-plate solvent extraction
columns are widely used in radiochemical
separation processes. Although invented
by Van Dijck (27) in 1935> the pulsed
column was not used in the chemical
industry until its application to solvent
extraction separations in the radio-
chemical field in the late 1940's. Be-
cause size and space are important
economical factors in the nuclear indus-
try, the greater efficiency and smaller
size of the pulsed columns greatly reduce
the over-all cost of radiochemical separa-
tions compared to conventional columns.
Other advantages are mechanical sim-
plicity: ease of operation, and flexibility
( 2 3 ) . Wiegandt and Von Berg (29),
reviewed the functions and performance
of the apparatus.
For experimental studies, pulsed
columns are constructed of either pre-
cision-bore tubing with an inserted sieve-
plate cartridge or short lengths of glass
stacked between sieve plates and held in
compression. A cartridge normally con-
sists of a central rod on which the sieve
plates and spacers are alternately strung
and positioned by nuts on both ends of
the rod. Phase disengaging sections,
located at both ends of the column, are
approximately 30% larger in diameter
than the column proper. Pulsation is
provided by metal or Teflon bellows
driven by variable-speed drive units or
reciprocating metering pumps. A typi-
cal laboratory column is described by
Stephenson (22).
A great many experimental studies
have been conducted using pulsed sieve-
plate extraction columns. Table I sum-
l Present address, Boeing Airplane Co.,
Seattle: Wash.
marizes flooding and mass transfer
experimental data, including the range
of pulsed column variables and systems
studied, and the number of experiments
utilized in this study. Flooding correla-
tions have been presented by Beyer and
Edwards ( 2 ) : Sege and Woodfield (79):
Swift ( 2 3 ) , Pike and others (76), Crico
(6), and Thornton (26). The most com-
prehensive study of flooding was made
by Thornton (25: 26) and Logsdail and
Thornton (75), who developed an em-
pirical correlation based on experimental
flooding data for six liquid systems
(Table I). Correlating equations for
mass transfer data have been presented
by Swisher ( 2 4 ) ,Rubin and Lehman (78),
Crico (6): and Thornton (26). Thornton
has also produced the most complete mass
transfer correlation available in the
literature.
This work correlates the experimental
flooding and mass transfer data in the
literature for sieve-plate pulsed columns
using dimensional analysis and multiple
regression techniques.
A Generalized Flooding Correlation
Flooding in pulsed columns may be
defined as the flow condition when the
fluid of one phase entering a t one end of
the column cannot leave a t the opposite
end and must exit through the effluent
line intended for the second phase (79).
I t can occur both above and below a
region of stable operation. Flooding
owing to inadequate pulsation will
occur when insufficient mechanical agita-
tion is supplied to force the liquids
through the perforated holes of the
column plates. Thus, the plates act as a
VOL. 5 1 , NO. 9
physical barrier in prohibiting counter-
current flow of the two immiscible
phases. As pulsation is increased, a
region of stable operation is reached,
followed by flooding at an upper limit
of pulsation where mechanical agitation
becomes excessive and "emulsion" flood-
ing occurs. This is characterized by
mixtures of fine and coarse dispersed
phase drops, the formation of large
globs of dispersed phase by coalescence,
and periodic reversals of the continuous
phase in short sections of the column.
Geier (8) describes five regions of opera-
tion. This study and the majority of
previous flooding studies are concerned
with flooding in the upper region of
operation. Flooding is frequently ex-
pressed in terms of the volume flow rate
of the continuous phase, Vc,plus the dis-
persed phase, V,. based on the cross
section of the empty column-Le., V, +
Vd:cubic feet per hour per square foot.
Selection of Variables. The vari-
ables considered to affect the total flood-
ing velocity in sieve-plate pulsed columns
are: f, pulse frequency; a, pulse ampli-
tude; VC, superficial velocity of con-
tinuous phase; V,, superficial velocity of
dispersed phase; d, sieve hole diameter;
D,column diameter; 1, plate spacing;
E , fractional free space per plate; y,
interfacial tension; pc, p d 3 viscosities
of the continuous and dispersed phases,
respectively; pe, p d : densities of con-
tinuous and dispersed phases, respec-
tively; and g, acceleration due to
gravity. Other variables are: pulse
wave form, plate material, clearance
between plates and column wall, and
temperature. Data obtained from col-
umns with plates of materials other than
SEPTEMBER 1959 1005
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1 006 INDUSTRIAL AND ENGINEERING CHEMISTRY

 E X T R A C T I O N COLUMNS

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VOL. 51, NO. 9 SEPTEMBER 1959 1007

 brass or steel were not included in the
correlation. Only data obtained with Table II. Maximum and Minimum Values of Variables Used in Obtaining
sinusoidal pulse wave forms were used. Correlating Equations
Moreover, as runs were generally made Flooding
a t room temperature, the effect of tem- Variable Min. Max.
perature was neglected. It has been
a, ft./cycle 0.009 0.0416
demonstrated experimentally (23) that D,feet 0.167
the effect of plate thickness can be d, feet 0.00167 0.0155
ignored. D,,sq. ft./hr. ...
Several variables can be related by a f, cycles/hr. 870 18,000
theoretical equation defining the power
(HTU),,,feet ...
...
I , feet 0.0416
input to the column. Jealous and V,,ft./hr. 8 195
Johnson (10) first introduced a method v d , ft./hr. 4 255
for computing power requirements for a E 0.081
-1, lb./hr.* 0.288 x 106 1.20 x 106
pulsed column and this approach was wC, lbJ(ft.1(hr.) 2.42
recently applied to pulsed column p d , lb./(ft.) (hr.) 1.41
correlations by Thornton (261, who p0 lb./cu. ft. 62.4
p d , Ib./cu. ft. 46.9
relates the frequency, amplitude, column
height, number of plates, and fractional
free area per plate in terms of one
variable, I/,,,the maximum power
found to be independent of the column
absorbed per unit mass of fluid. For a
diameter. Equation 2 with the recom-
sine wave pulse:
mended constants represents the 665
experimental points with an average
deviation of 19.6%. This result can be
made more useful by combining common
where C, is the orifice coefficient. factors and supplying numerical values
for p c , pe, and g, which were constant:
By combining the remaining variables,
D,d, V C ,Vdj +/, g, AP: p d ,
P C , P C , and 7 V, + V d = 3.20 X
into significant dimensionless groups A n
105 P’_-.
63 d0.m vcn0 1 1
. ~-
(77, 27), the following exponential func- y o . i u #,o.zn7 Pdo ao vdo.oic (3)
~~~
tion is obtained :
The accuracy of this equation has not
been reduced by this manipulation.
This equation best illustrates the de-
pendence of the total flooding velocity
on the principal variables.
For rapid calculation of flooding veloc-
where the majority of groups are identical
ities in experimental pulsed columns
to those derived by Thornton (26). where water is the continuous phase, a
While this function need not be exponen-
nomograph based on Equation 3 is pre-
tial in nature, it often represents experi-
sented in Figure 1. The flooding veloc-
mental data very closely. ities determined from the nomograph
Analysis of Experimental Data. A
are within 20% on the average of the
total of 751 flooding experiments from experimental values. Table I1 sum-
five investigators were available in the
marizes the range of pulsed column
literature, from which 665 experiments
variables to which this equation applies.
of four investigators were utilized in the Application to D e s i g n . Once the
flooding correlation. In many instances
total flooding velocity has been predicted
the experimental data were not amen- for a given set of conditions using Equa-
able to correlation because physical
tions l and 2 or the flooding nomograph
properties of complex systems (7, 9, 72, in Figure 1, the required column diam-
73, 78, 79) were not available, or the eter can be calculated from the relation-
column was operated in a region other
ship :
than emulsion flooding (2) or had un-
usual constructional or operational char-
acteristics such as Teflon plates (72),
packed columns ( 3 ) ,or pulse wave forms
where F is the fraction of the flooding
other than sinusoidal (26).
Equation 2 was transformed logarith- velocity at which the column is to operate
mically, and multiple regression tech- and W is the design capacity of the
niques were applied to obtain the co- column in cubic feet per hour.
efficient and exponents from the data
with the aid of an IBM 650 digital Generalized Mass
computer. T h e recommended values Transfer Correlation
for use with Equation 2 are : When mass transfer of the solute from
the feed stream to the solvent occurs,
bo = 0.527 ba -0.207 ba = 0.81
bi = -0.014 bi 0.458 bi = -0.20 it is generally assumed that diffusion is
bz = 0.63 b5 = 0 so rapid that equilibrium exists a t the
interface between the two phases and
Total flooding velocity, V , + V , was that all resistance to diffusion can be
1 008 INDUSTRIAL AND ENGINEERING CHEMISTRY
Mass Transfer
.Min. Max.
0.018 0.098
1.00 0.1667 1.0
0.0052 0.0104
... 6.92 X lo-& 9.86 Y 10-5
7,200 30,600
... 0.71 7.10
0.25 0.0417 0.1667
9.9 104.5
12.5 94.9
0.62 0.085 0.62
4.06 X 105 9.72 X 10’
2.42 2.55 2.55
3.19 1.36 1.81
62.4 62.4 62.4
55.0 53.5 55.0
represented by two hypothetical stagnant
liquid ‘:films,” one on either side of the
interface. This “two-film concept” was
first postulated by Whitman (28) in
1923. Concentration gradients are said
to exist within the films which represent
the driving force for mass transfer be-
tween the interface and the bulk streams.
As it is very difficult to determine the
interfacial concentration, the entire po-
tential for mass transfer is combined in
a n over-all driving force to be used in
conjunction with over-all mass transfer
coefficients. The coefficients are as-
sumed to remain constant throughout the
column, and all the resistance is assumed
to be concentrated in one phase or
another, which is often the case
I t would be difficult to correlate
HTU’s on an ”over-all” basis unless the
resistance to mass transfer was concen-
trated principally in one phase, in which
case the resistance in the second phase
could be neglected. For the systems
utilized in this study, it is assumed
that the major resistance to m a s transfer
lies in the dispersed phase “film” with
negligible resistance in the continuous
phase. This assumption was verified
by analyzing the distribution of solute
between the two immiscible phases for
each system.
Selection of Variables. Thc variables
thought to affect the ratr of mass rransfer
of the solute through the dispersed phase
film are VO,LTc, V d , D,d, I , P d , AP. Y, pd,
and P d , where b’o = fa/€,a term which is
assumed to be proportional to the mean
velocity of the dispersed phase bubbles
through the sieve plate perforations ( 7J).
T h e relationship among the selected
dimensionless groups can be expressed as:
The Reynolds number, Schmidt number,
and density group are based on the dis-
persed phase properties where the major
resistance is assumed to exist. C; and
 E X T R A C T I O N COLUMNS

3
t-
I
v

VOL. 51, NO. 9 0 SEPTEMBER 1959 1009

pc are not considered to have an appreci-
able effect on mass transfer in the dis-
persed phase.
Analysis of Experimental Data. Of
the 696 data points which were available
in the unclassified literature, 285 were
applied to the mass transfer correlation.
T h e remainder of the data were excluded
for the reasons cited in analysis of the
flooding data. I n addition, only the data
for which mass was transferred from the
dispersed phase to the continuous phase
were utilized in obtaining the mass
transfer correlation.
Evaluating the coefficient and ex-
ponents for the mass transfer relation-
ship in a manner identical to that used in
the flooding analysis, the following con-
stants, when applied to Equation 5, were
found to represent the mass transfer
data with an average deviation of 16.4% :
C( = 0.20 C3 = 0.865 C6
CI = - 0 . 4 3 4 C( 0.096 CI
C? 1.04 CL = -0.636
This equation is strictly valid only for
extraction in pulsed columns, where mass
transfer occurs from the dispersed phase
to the aqueous continuous phase and
where the major resistance to mass
transfer is in the dispersed phase. I t is
possible that similar correlaiions could
be applied to transfer of mass from the
continuous phase to the dispersed phase
or to the case where the major resistance
is in the continuous phase. However,
certain exponents would be expected to
be different for these cases.
Analysis of the range of variables for
the terms of Equation 5 shows that the
physical properties of the liquid systems
were very nearly constant as outlined in
Table 11. Thus, the exponents of
(A ’ P (PU’P~DJ, ( A P / P ~ , and (Y ’
~ T
V C p J are not to be considered too
accurate. However, a qualitative anal-
ysis of these exponents reveals certain
trends which are thought to be correct.
For instance, the HTU is proportional
to the density difference of the immiscible
phases, inversely proportional to the
diffusion coefficient of the solute in the
dispersed phase, and nearly independent
of the interfacial tension. T h e exponent
for the ratio of viscosities is thought to
be unduly large and possibly represents
only a constant in the equation. Equa-
tion 5 with the recommended constants
can be simplified without reducing the
accuracy to give :
(HTU),, =
Such a n equation best illustrates the
dependence of H T U on the major vari-
ables.
T o provide a means of rapid calcula-
tion of HTU values for sieve-plate
pulsed columns, a nomograph based on
Equation 5 is presented in Figure 2 .
The optimum values for the exponents,
1 01 0 INDUSTRIAL AND ENGINEERING CHEMISTRY
in part, are still uncertain. Thus, the
nomograph is most useful when systems
with properties similar to the data
analyzed in this study are to be investi-
gated. However, Equation 5 should
account for a wide range of systems,
if the exponents were verified or altered
by more extensive data. T h e H T U
values predicted using the nomograph
are within 20% of the experimental
values on the average.
Application to Design. (HTU),,.
the over-all height of a transfer unit
based on the continuous phase. can be
calculated from Equation 5, or hy using
the nomograph cf Figure 2, for any
given set of conditions. Sincc A’,,,,,
the number of over-all transfer units
based on the ccntinuous phase, can be
determined from equilibrium data (20)
and a knoL51edge of the desired extraction
of the solute, the height of the column
= 0.317
for a given set of conditions can be
= 4.57
calculated ( 4 ) from the equation:
h = (HTU)dL.Vto c
Alternatively, design Equation 6 can
be used to investigate effects of important
independent variables on the height of a
transfer unit.
Acknowledgment
T h e authors thank IVayne Van Meter
and Satoru Tashiro for assistance with
the calculations.
Nomenclature
a = pulse amplitude, feet,’cycle
bo-bi constants
= 49, 340 (1953).
GO-c, =constants
CO = orifice coefficient = 0.60
D = column diameter, feet
d = diameter of plate hole, feet
D, = diffusivity of solute in dis-
persed phase, sq. ft./hr.
f
= (Vc +
Vd)operaiin&/(vc + y d ) f l o o d i n g
= pulse frequency, cyclesihr.
g = acceleration of gravity, ft.lhr.2
k = column height, feet
(HTU),,, = overall height of a transfer
unit based on continuous
phase, feet
I = plate spacing, feet
N , = number of transfer units
V = superficial velocity, ft./hr.
Vo = fa/^, ft./hr.
W = total column design capacity,
cu. ft./hr.
t = plate thickness, ft.
SUBSCRIPTS
c = continuous phase
d = dispersed phase
GREEKLETTERS
e = fractional free space per plate
$, = power function, sq. ft./hr.3
y = interfacial tension, lb./hr.2
p = viscosity, lb./(ft.)(hr.)
p = density, lb./cu. ft.
Ap = density difference between con-
tinuous and dispersed phases,
lb./cu. ft.
Literature Cited
(1) Belaga, M. W.,Bigelow, J. E., U. S.
Atomic Energy Comm., Rept. KT-133
(1952).
(2) Beyer, H. G., Edwards, R. B., Ibzd.,
ISC-553 (1954).
(3) Chantry, W. A., Von Berg, R. I..,
Wiegandt, H. F., IND.ENG.CHEM.47,
1153 (1955).
(4) Chilton, T. H., Colburn, A. P., Ibid.,
27, 255 (1935).
(5) Cohen, R. M., Beyer, G. H., U. S.
.4tomic Enrrgy Comm., Rept. ISC-294
(1953).
(6) Crico, 4 . , Genie chim. 73, 57 (1955).
!7) Ellison, C. V., U. S. Atomic Energy
Comm., Rept. ORNL-912 (1956).
( 8 , Geier, R . G., Ibid.. HW-49542-A
11957).
(9) Griffith, W. L., Jasny, G. R., Tupper,
H. T., Ihid., KT-114 (19521.
(10) Jealous, A. C., Johnson, H. F.,
IND. E N G . CHEM. 47, 1159 (1955).
(11) Klinkenberg, A., Mooy, H. H.,
Chem. Enp. P r q r . 44, 19 11948).
(12) Lane, A. F., U. S. Atomic Energy
Comm., Rept. UCRL-2983 (1955).
(13) Lehman, H . R., Zbid., UCRL-1558
(1956).
(14) Li, W. H., Newton, W.li.,A.1.Ch.E.
(7) Journal 3. 56 11957).
(15) Logsdail, D. H., Thornton, J. D.,
Trans. Inst. Chem. Engrs. (London) 35,
331 (1957’1.
(16) Pike, F. P., Nelli, J. R., Erickson,
F. E., Arnold, D. S., Box, G. E. P.;
Hunter. S. J.. U . S. Atomic Enerw
V I
Comm.; Rept. ORO-140 (1954).
117) Ibid.. ORO-141 11954).
i18j Rubin, B., Lehman, H. R., Thio‘.,
UCRG718 (1950).
(19) Sege, G., Woodfield, F. I\’,, Zbid.,
HW-31259 (1954).
(20) Sherwood. T. K., Pipford. R. L.,
’ “Absorption ‘and Extractyon,“ ’ 5th ed.,
McGraw-Hill, New York, 1952.
(21) Smoot, L. D., M.S. thesis, University
of Washington, Seattle, Wash., 1958,
(22) Stephenson, R., Chern. Eng. P r o y .
(23) Swift, W. H., U. S. Atomic Enerpv
Comm., Rept. HW-33953 119541.
(24) Swisher, G. F., Dissertalion Abstr. 16,
1421 (1956).
125) Thornton. J. D.. Brit. Chem. Ener.
\-
3,247 11958j. ’
(26) Thornton, J. D., T r a n s . Inst. Chem.
Engrs. (London) 35, 316 (1953).
(27) Van Dijck, W. J. O., U. S. Patent
2,011,186 (1 935).
(28’1 Whitman. W. G.. Chem. ‘Met. Ener. 29,
Y .
127 (1925).
(29) Wiegandt, H. F., Von Berg, R. L.,
Chem. Eng.61, No. 7, 149 (1954).
RECEIVED
for review July 23, 1958
ACCEPTED April 15, 1959
Based on work performed at the Univer-
sity of Washington for Atomic Energy Com-
mission, Contract No. AT(45-1 t1053.
Synthetic Lubricant-
Correction
In the I/EC Special Feature on syn-
thetic lubricants [IND. EKG.CHEM.51,
49A-63A (May 1959)] the illustrations
on pages 50 A and 51 A should have been
placed with the article by J. S. McClure
on page 57A.