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ORNL-TM-3718.txt
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MASTRR
OAK RIDGE NATIONAL LABORATORY-,
operated by -
» UNION CARBIDE CORPORATION w
. NUCLEAR DIVISION
| /‘} I( for the
3 U.S. ATOMIC ENERGY COMMISSION
ORNL- TM-3718
-z MASS TRANSFER BETWEEN SMALL BUBBLES AND LIQUIDS IN
. COCURRENT TURBULENT PIPELINE FLOW
.
(Thesis)
T. S. Kress
T CISTIEITTER OF T2 nefrp v i e
" Submitted as a dissertation to the Graduate Council of The University of Tennessee in partial fulfiliment of
the requirements for the degree Doctor of Philosophy .
This report was prepared as an account of work sponsored by the United
States Government. Neither the United States nor the United States Atomic
Energy Commission, nor any of their employees, nor any of their contractors,
subcontractors, or their employees, makes any warranty, express or implied, or
assumes any legal liability or responsibility for the accuracy, compileteness or
usefulness of any information, apparatus, product or process disclosed, or
represents that its use would not infringe privately owned rights,
Ny
)
ORNL~TM-3718
Contract No. W-T7L405-eng-26
MASS TRANSFER BETWEEN SMALL BUBBLES AND LIQUIDS IN
COCURRENT TURBULENT PIPELINE FLOW
T, 5. Kress
Submitted as a dissertation to the Graduate Council
of The University of Temnessee in partial fulfillment of
the requirements for the degree Doctor of Philosophy.
st e N O T | C E —
j‘-'i‘.ms port i , t of wor
“This t was -prepared as an accoun -
s ans;:ép?fby tigli United States Government. I::elther
'til',le"-Uni'téd States nor the United States Atomic nergg;
Commission, nogr any of their employ§e§, n?!:'p?;\ge:s
ir OF tors, or their e ees,
| their contractors, subcontractors, e sonues any
1 mskes any warranty, express or implied, s any
-Fability - bility for the accuracy,
legal -liability -or_responsi f 2 acy, com
' ness or usefulness of any information, app2 ,
‘ g}:?deuzt bf tm disclosed, or represents that its use
APRI L 1 972 woutd not infringe privately owned rights.
CAK RIDGE NATTONAL LABORATORY
Oak Ridge, Tennessee 37830
operated by
UNION CARBIDE CORPORATION
for the
U, 3. ATOMIC ENERGY COMMISSION
ACKNOWLEDGMENTS
This investigation was performed at the Oak Ridge National
Laboratory operated by the Union Carbide Corporation for the U. S.
Atomic Energy Commission. The author is particularly grateful for
the helpful discussions, guidance, and direction given the research
by the major advisor, Dr. J. J. Keyes, and the support of Dr.
H., W. Hoffman, Head of the Heat Transfer-Fluid Dynamics Department of
the Reactor Division.
Dunlap Scott of the Molten-Salt Reactor Program suggested the
problem and provided initial funding under the MSR Program. Dr. F. N.
Peebles, Dean of Engineering, The University of Tennessee, suggested
the use of the oxygen-glycerine-water system and carried out the original
analysis of the applicability to xenon-mclten salt systems.
The contributions of the following ORNL staff members are also
gratefully acknowledged: R. J. Kedl for his bubble generator develop-
ment work drawn upon herej; Dr. C. W. Nestor for computer solution of
the analytical model; and Frances Burkhalter for preparation of the
figures.
Special thanks are given to Margie Adair for her skillful and
cheerful preparation of the preliminary and final manuscripts, and, of
course, to my wife, Dee, for her forbearance.
ii
ABSTRACT
Liquid-phase-controlled mobile-interface mass-transfer coefficients
were measured for transfer of dissolved oxygen into small helium bubbles
in cocurrent turbulent pipeline flow for five different mixtures of
glycerine and water. These coefficients were determined by transient
response experiments in which the dissolved oxygen was measured at only
one position in a closed recirculating loop and recorded as a function
of time, Using an independent photographic determination of the inter-
facial areas, the mass-transfer coefficients were extracted from these
measured transients and determined as functions of pipe Reynolds number,
Schmidt number, bubble Sauter-mean diameter, and gravitational orienta-
tion of the flow,
Two general types of behavior were observed:
(1) Above pipe Reynolds numbers for which turbulent inertia forces
dominate over gravitational forces, horizontal and vertical flow mass-
transfer coefficients were identical and varied according to the regression
equation
Sh/Scl’ 2 = 0,34 Re®+9%¢ (dVS/D)l‘O )
The observed Reynolds number exponent agreed genefally'with other liter-
ature data for cocurrent pipeline flow but did not agree with expectation
based on equivalent power dissipation comparisons with agitated vessel
data,
(2) Below the Reynolds numbers that marked the equivalence of hor-
izontal and vertical flow coefficients, the horizontal-flow coefficients
continued to vary according to the above equation until, at low flows,
iii
iv
severe stratification of the bubbles made operation impractical. The
vertical-flow coefficients at these lower Reynolds numbers underwent a
transition to approach constant asymptotes characteristic of the bubbles
rising through the quiescent liquid. For small bubbles in the most
viscous mixture tested, both horizontal and vertical-flow coefficients
underwént this transition.,
An expression was developed for the relative importance of turbulent
inertial forces compared to gravitational forces, Fi/Fg' This ratio
served as a good criterion for establishing the pipe Reynolds numbers
above which horizontal and vertical-flow mass-transfer coefficients were
identical. In addition, it proved to be a useful linear scaling factor
for calculating the vertical-flow coefficients in the above mentioned
transition region.
A seemingly anomalous behavior was observed in data for water
(plus about 200 ppm N-butyl alcchol) which exhibited a significantly
smaller Reynolds number exponent than did data for the other fluid mix-
tures. To explain this behavior, a two-regime "turbulence interaction"
model was formulated by balancing turbulent inertial forces with drag
forces. The relationship of the drag forces toc the bubble relative-flow
Reynolds number gave rise to the two regimes with the division being at
Reb = 2, The resulting bubble mean velocities for each regime were then
substituted intb Frossling~type equations to determine the mass-transfer
behavior. The resulting Reynolds number exponent for one of the regimes
(Reb € 2) agreed well with the observed data but the predicted exponent
for the effect of the ratio of bubble mean diameter to conduit diameter,
dvs/D’ was less than that observed. The mass-transfer equations
v
v
b
particles in agitated vessels and alsc compared favorably with the
resulting from the other regime (Re, > 2) agreed well with data for
water data mentioned above,
For comparison, a second analytical model was developed based on
surface renewal concepts and an eddy diffusivity that varied with
Reynolds number, Schmidt number, bubble diameter, interfacial condi-
tion, and position away from an interface, Using a digital computer,
a tentative numerical solution was obtained which treated & dimension-
less renewal period, T,, as a parameter. This renewal period was
interpreted as being a measure of the rigidity of the interface, I, - 0
corresponding to fully mobile and T, » approximately 2.7 (in this case)
to fully rigid interfaces,
TABLE OF CONTENTS
CHAPTER
1. INTRODUCTION v & o o o o o o o o o o« o » o
II. LITERATURE REVIEW . . . . . . .
Experimental-Cocurrent Flow . . . . .
Experimental-Agitated Vessels .A. . e e
Discussion of Available Experimental Data .
Theoretical . + ¢ ¢« ¢ ¢ ¢ 4 ¢ ¢ « o o o
Surface Renewal Models . ¢« 4 o o & o &
Modeling of the Eddy Structure . .
Turbulence Interactions . . . . .7. .
Dimensional Analysis (Empiricism) . .
DisCUuSSion ¢« v v v o o « o o s o &
ITT. DESCRIPTION OF EXPERIMENT . . . ¢« « & » & &
Transient Response Technique
Apparatus . . + + . . o ; e e e e e e
Pump . . 0 0 0 0 0 0 e
Liquid Flow Measurement . . . . «
Temperature Stabilization . . . . .
Gas Flow Measurement . .
Dissolved Oxygen Measurement . . . . .
Bubble Generation . . « ¢« « o « «+ &
Bubble Separation . « « ¢ o « o « &
Test Section v v ¢« ¢« ¢ ¢« o « o o s &
vii
"PAGE
11
11
viii
CHAPTER PAGE
Bubble Surface Area Determination — Photographic
SYSTLEM + o o + « o o o « o o o o o s o o s o v o s . 38
ENG BEFECE 4 v o v o v o o o o o o o o o o w0 0w e . W7
Summary of Experimental Procedure . . . « « o o o« o o Lg
IV, EXPERIMENTAL RESULTS . & &« « ¢ 4 o o o o o s o s o o s o 55
Unadjusted Results . v ¢ ¢« ¢ o o o ¢ o o o o o o o s o 55
Equivalence of Horizontal and Vertical Flow
Mass Transfer . o o o & o o o o s o o o o o o o o o 56
Vertical Orientation Low-Flow Asymptotes . . . . . . . 60
Mass Transfer Coefficients . & o v ¢« ¢ v o o o o o & & 60
Calculating Vertical Flow Mass-Transfer Coefficients
forFi/FgLessThanl.5 C e e e e e e e e e e e . BT
Comparison with Agitated Vessels . ¢« ¢ « o ¢ o « o o & 69
Recommended Correlations . & ¢« o o+ o o o o o o o o o« o (1
V., THEORETICAL CONSIDERATIONS . . &+ ¢ v o 4 o o ¢ o « « o o« 6
Turbulence Interaction Model .+ v o o v o « o « « = o« &« 76
Surface Renewal Model . & v o« ¢ o 6 o o o o s o o s o 81
VI, SUMMARY AND CONCLUSIONS + & « v o o o o o o « o s o « o o 9h
VII. RECOMMENDATIONS FOR FURTHER STUDY . v v o « « & o o o o« o 100
Experimental . . v v & ¢ o ¢ o s s o s o o o o o s s 100
Theoretical v v v v o o « « o o o o+ o o o o o o « o o » 102
ILIST OF REFERENCES .+ 4 & &« o o o o s o s o = » s & o o o o o o o o« 105
APPENDICES s e » e 6 s s s s s s 8 s ® s e s e e e o s e s s « e ¢ 111
A PHYSICAL PROPERTIES OF AQUEOUS-GLYCEROL MIXTURES . . . . . 11l
ix
CHAPTER PAGE
B DERTIVATION OF EQUATIONS FOR CONCENTRATION CHANGES
ACROSS A GAS-LIQUID CONTACTOR . v & ¢« o o o o o » & o« o 117
C INSTRUMENT APPLICATION DRAWING . & & o ¢ o o o o « o o & » 121
D INS TRU-MEN-T CALIBRATI ONS L . * . . » . . * - . * - . . . . l 2 3
E EVALUATION OF EFFECT OF OXYGEN SENSOR RESPONSE SPEED ON
THE MEASURED TRANSIENT RESPONSE OF THE SYSTEM . . . . . 129
F MASS BALANCES FOR THE SURFACE RENEWAL MODEL ., . . +» « « « 131
G ESTIMATE CF ERROR DUE TO END-EFFECT ADJUSTMENTS . . . . . 13k
H MASS TRANSFER DATA . . . & & & ¢ o &« s o s o o o o o« o «» 137
LIST OF SYMBOLS 4 & « 4 o o o o « o o o o o « s o s o « o o o o o« 163
X
LIST OF TABLES
TABLE PAGE
1. Ranges of Independent Variables Covered . . « « ¢« + + o & 3
IT. Categories of Data Correlation for Mass Transfer from
a Turbulent Liquid to Gas Bubbles . . . « +. . + « + « & 12
ITT. Physical Properties of Aqueocus-Glycerol Mixtures (25°C)
Data of Jordan, Ackerman, and Berger®® ., . ... ... 20
IV. Experimental Conditions for Runs Used to Validate
Surface Area Determination Method for Vertical
F:LOWS . . . . . » . - . . . . . . * . . . . » . . - . s L}'L"
V. Experimental Conditions for Runs Shown on Horizontal
Flow Volume Fraction Correlation . . .« « « o« =« « o .« =« 45
VI. Conditions at Which Horizontal and Vertical Flow
Mass-Transfer Coefficients Become Equal
(Lamont ! S Data)ll . * . » . . » » - - - * - . . . - . L 5:,:}
10.
11.
LIST OF FIGURES
PAGE
Photograph of the Mass Transfer FPacility « o ¢ & o o o o & 2L
Schematic Diagram of the Main Circuit of the
Experimental Apparatus . . ¢ &« & & 4 ¢ o o o 0 e o s . 25
Diagram of the Bubble Generator . . .'. s e e e s e e e s 31
Comparison of Measured Bubble Sizes with the
Distribution Function « « « « ¢« « « o ¢ o & & o o « « o« 33
Diagram of the Bubble Separator . . « « o o « o « « « » « 30
Comparison of Interfacial Areas Per Unit Volume Measured
Directly from Photographs with Those Established
Through the Distribution Function. Vertical Flow . . . 43
Correlation of Horizontal Flow Volume Fraction . . . . . . 146
Comparison of Measured and Calculated Interfacial Areas
Per Unit Volume, Horizontal Flow . . . . « « « « « « & L8
Typical Experimental Concentration Transient Iliustrating
Straight-Line Behavior on Semi-Log Coordinants . . . . 53
Typical Examples of Bubble Photographs: a. Inlet b, Exit
Vertical Flow, 37.5% Glycerine-62,5% Water, @, = 20
gpm, Qg/QE = 0.3%, D = 2 inches, and dvs = 0,023
SNCHES &+ v o o b e e e e e e e e e e e e e e e e e 5L
Mass Transfer Coefficients Versus Pipe Reynolds Number
as a Function of Bubble Sauter-Mean Diameter. Water
Plus ~200 ppm N-Butyl Alcohol, Horizontal and
Vertical Flow in a 2-inch Diameter Conduit . . . . . . 62
X1
xii
FIGURE PAGE
12, Mass Transfer Coefficients Versus Pipe Reynolds Number
as a Function of Bubble Sauter-Mean Diameter. 12,5%
Glycerine-87.5% Water, Horizontal and Vertical Flow
in a 2-inch Diameter Conduit . . v v + &« ¢« « « « . « . 63
13. Mass Transfer Coefficients Versus Pipe Reynolds Number
as a Function of Eubble Sauter-Mean Diameter. 25%
Glycerine-75% Water. Horizontal and Vertical Flow
in a 2-inch Diameter Conduilt . . . . + ¢« ¢« ¢ ¢« & o o 6L
14, Mass Transfer Coefficients Versus Pipe Reynolds Number
as a Function of Bubble Sauter-Mean Diameter. 37.5%
Glycerine-62,5% Water, Horizontal and Vertical Flow
in a 2-inch Diameter Conduit . « & .« ¢ ¢ ¢ ¢ o ¢« « o . 65
15. Mass Transfer Coefficients Versus Pipe Reynolds Number
as a Function of Bubble Sauter-Mean Diameter. 50%
Glycerine-50% Water. Horizontal and Vertical Flow
in a 2-inch Diameter Conduilt . . ¢ ¢ o ¢ « o « o & o & 66
16, Observed Types of Horizontal Flow Behavior,
dVS = 0,02 inches and D = 2 inches . ¢ & ¢ o ¢ & & o = 68
17. Equivalent Power Dissipation Comparison of Results
with Agitated Vessel Data . & ¢ & ¢« ¢« ¢ ¢ ¢ o & o o o & 70
18, Equivalent Power Dissipation Comparison of Gravity
Dominated Results with Agitated Vessel Data . . . . . . 72
19. Correlation of Horizontal Flow Data . . . « . « . + « . . Th
20, Dimensionless Variation of Eddy Diffusivity with Distance
from an Interface, Effect of Surface Condition . . . . 88
FIGURE
21,
e,
23.
2k,
25,
26,
27
28.
29,
30,
31.
32,
33.
3k,
Variation of Eddy Diffusivity with Distance from an
Interface,
xiii
Data of Sleicher . ¢« « . ¢« ¢« ¢« o o o o o o o
Numerical Results of the Surface Rénewal Model.
of a, b,
and ¢ (Exponents on Re, Sc, and d/D,
Respectively) as Functions of the Dimensionless
Period, T* . » . - - . . . o o . . - ® - . ®
Schmidt Numbers of Glycerine-Water Mixtures . . .
Henry's Law
Constant for Oxygen Solubility in
Glycerine-Water Mixtures . « « « ¢ o o ¢ « o &
Molecular Diffusion Coefficients for Oxygen in
Glycerine-Water Mixtures.,
and Berger . & o & o o s o o ¢ o o o s s e s
Densities of Glycerine-Water Mixtures . . . « « &
Viscosities
of Glycerine-Water Mixtures . ., .
Instrument Application Drawing of the Experiment
Facility
Bubble Size
Calibration
Calibration
Calibration
Calibration
Calibration
. . » . - L ] ° . . - . - . . . .
Range Produced by the Bubble Generator
of Rotameter No, 1 (100 gpm) . . . . .
of Rotameter No. 2 (40 gpm) . . . . .
of Rotameter No. 3 (8 gpm) . . . . . .
of Gas-Flow Meter at 50 psig . . . « &
of Oxygen Sensors in two Mixtures of
Glycerine and Water . . « o« ¢ o o« ¢ ¢ o ¢ o o &
Comparison of Calculated Values with
Plots
Data of Jordan, Ackerman,
PAGE
92
112
113
114
115
116
121
123
124
125
126
127
128
FIGURE
35.
36,
37.
38.
L5,
Xxiv
Unadjusted Mass Transfer Data. Water Plus ~200 ppm
N-Butyl Alcohol. Vertical Flow . . . « « « « « « &
Unadjusted Mass Transfer Data. Water Plus ~200 ppm
N-Butyl Alcohol. Horizontal Flow . . « ¢« ¢ ¢ « o« &
Unadjusted Mass Transfer Data. 12.5% Glycerine-
87.5% Water, Vertical FIOW « v « o o o o« o « & o &
Unadjusted Mass Transfer Data. 12.5% Glycerine-
87.5% Water. Horizontal FIOW . . v « « ¢ « & o o
Unadjusted Mass Transfer Data., 25% Glycerine-75%
Water., Vertical FIOW . v & o o ¢ o o o o o o o & o
Unadjusted Mass Transfer Data. 25% Glycerine-T5%
| Water., Horizontal FIlOow ¢ o o v ¢« o o o &+ o o o & &
Unadjusted Mass Transfer Data. 37.5% Glycerine-
62.5% Water. Vertical FIOW v v v o o o o o« o o o« &
Unadjusted Mass Transfer Data, 37.5% Glycerine-
62,5% Water, Horizontal FIOW « v « v o o o o « o
Unadjusted Mass Transfer Data. 50% Glycerine-50%
Water., Vertical FIOW . . o & o« ¢« « ¢ o o o &
Unadjusted Mass Transfer Data. 50% Glycerine-50%
Water., Horizontal FIlOow . « ¢ « v v ¢ o o o o o o &
Unadjusted Mass Transfer Coefficients Versus Pipe
Reynolds Number as a Function of Bubble Sauter-Mean
Diameter. Water Plus ~200 ppm N-Butyl Alcohol.
Horizontal and Vertical FIOW .+ & o o o « o s o s »
PAGE
138
139
140
141
142
143
1hk
146
1h7
148
FIGURE
L6,
47.
L.
50.
51,
52.
53.
XV
Unadjusted Mass Transfer Coefficients Versus Pipe
Reynolds Number as a Function of Bubble Sauter-Mean
Diameter. 12.5% Glycerine 87,5% Water. Horizontal
and Vertical FI1ow . . ¢ o ¢ « « ¢ ¢ o« o o o o o o o
Unadjusted Mass Transfer Coefficients Versus Pipe
Reynolds Number as a Function of Bubble Sauter-Mean
Diameter, ?5% Glycerine-75% Water. Horizontal
and Vertical FIOW ., o o & ¢ ¢ ¢ o o o o s o o o
Unadjusted Mass Transfer Coefficients Versus Pipe
Reynolds Number as a Function of Bubble Sauter-Mean
Diameter. 37.5% Glycerine-62,5% Water. Horizontal
and Vertical Flow , . + o ¢ ¢« « « « &
Unadjusted Mass Transfer Coefficients Versus Pipe
Reynolds Number as a Function of Bubble Sauter-Mean
Diameter. 50% Glycerine-50% Water. Horizontal and
Vertical FI1ow . o ¢ v v ¢« &« o o o o o « &
Mass Transfer Data Adjusted for End-Effect. Water Plus
~200 ppm N-Butyl Alcohol., Vertical Flow . . . . .
Mass Transfer Data Adjusted for End-Effect. Water Plus
~200 ppm N-Butyl Alicohol, Horizontal Flow . .
Mass Transfer Data Adjusted for End-Effect. 12,5%
Glycerine-87.5% Water, Vertical Flow . . . . « . .
Mass Transfer Data Adjusted for End-Effect, 12,5%
Glycerine-87.5% Water. Horizontal Flow . . . . . .
PAGE
149
150
151
152
153
154
155
156
FIGURE
5k,
55,
56,
57
58.
Xvi
Mass Transfer Data Adjusted for End-Effect.
Glycerine-75% Water. Vertical Flow .
- Mass Transfer Data Adjusted for End-Effect.
Glycerine-75% Water. Horizontal Flow .
Mass Transfer Data Adjusted for End-Effect.
Glycerine-62,5% Water. Horizontal Flow .
Mass Transfer Data Adjusted for End-Effect,
Glycerine-50% Water, Vertical Flow .
Mass Transfer Data Adjusted for End-Effect.
Glycerine-50% Water. Horizontal Flow .
PAGE
25%
s e e e e . . 157
25%
e 516
37.5%
e o o . 159
50%
e e e e . . 160
50%
161
CHAPTER T
INTRODUCTICN
When gas bubbles are dispersed in a continuous liquid phase,
dissolved constituents of sufficient volatility will be exchanged between
the liquid and the bubbles, effectively redistributing any concentration
imbalances that exist. Common pradtices involve contacting gas bubbles
with an agitated liquid in such a manner that a relatively large inter-
facial area is available, Techniques such as passing gas bubbles up
through a liguid column or mechanically stirring a gas-ligquid mixture in
a tank have been studied extensively and the design technology for these
is relatively firm., However, one method, cocurrent turbulent flow in a
pipeline, has not been given a great deal of attention. A review of the
literature has shown that the availlable data are insufficient to‘allow
confident determination of the mass-transfer rates in such a system.
This research, then, was undertaken to provide additional information
that will aid in determining liquid phase controlled mass-transfer rates
for cocurrent turbulent flow of small bubbles and liquids in a pipeline.
The impetus for this work was provided by the Molten Salt Breeder
Reactor (MSBR) Program of the Oak Ridge National Laboratory where recent
remarkably successful operation of a molten salt fueled nuclear reactor!
has convincingly demonstrated the feasibility of this power system. The
economic éompetitiveness of an MSBR, however, depends to a significant
extent on the breeding ratio obtainable, The production within the
liquid fuel of fission-product poisons, principally xenon-135, exerts
2
a strong influence on the neutron economy of the reactor and consequently
on the breeding ratio itself,
One method proposed for removing the xenon would require injecting
small helium bubbles into the turbulently flowing regions of the fuel-
coolant stream and allowing them to circulate with the fuel. Since such
bubbles would be deficient in xenon compared to the nearby bulk stream,
the dissolved xenon would be transferred by turbulent diffusion across
the concentration potential gradient. By continuous injection and
removal of the helium bubbles the equilibrium xenon poisoning can be
significantly reduced. Since a large amount of gas in the fuel could
influence the reactivity of the core, this system would be limited to
low volume fractions.
Peebles® showed that removal of dissolved oxygen from a given mixture
of glycerine and water by small helium bubbles could closely match the
hydrodynamic and mass-transfer conditions in an MSBR and suggested using
such a system in a similitude experiment from which the actual MSBR
behavior might be inferred. Other desirable features of such a system
include: (1) convenient variation of the Schmidt number by using differ-
ent percentages of glycerine in water, (2) operation at room temperature
using glass hardware that allows photographic measurements through an
optically clear system, and (3) easy measurement of the dissolved oxygen
content by commercially available instruments. Therefore an oxygen-
glycerine-water system was chosen for this study.
The objective of the program was to measure liquid phase controlled
axially averaged mass-transfer coefficients, k, defined by
rL
k dx
X
L .
k =
3
The local mass-transfer coefficients, kx’ are defined by
J=k a [Cavg —-CS] s
where J is the mass transferred from the liquid to the bubbles per unit
time per unit volume of liquid, a is the interfacial area per unit volume
of liquid, Cavg is the bulk average concentration, and CS is the inter-
facial concentration,
These coefficients need to be established as a function of Schmidt
number, Reynolds number, bubble size, conduit diameter, gravitational
orientation of the flow (vertical or horizontal), interfacial condition
(absence or presence of a surface active agent), and the volume fraction
of the bubbles. The scope of this thesis is limited to the ranges of
variables listed in Table I, below, which for the most part represent
limits of the experimental apparatus. Extensions of this program, how-
ever, are projected to include different conduit diametersland different
interfacial conditions.
Table I. Ranges of Independent Variables Covered
Variable Range
Schmidt Number (weight percent of glycerine) 370 - 3446
(O, 12-5, 25, 3705) 50)
Pipe Reynolds Number 8 x 10® - 1.8 x 10°
Bubble Sauter Mean Diameter 0.01 to 0,05 inches
Gas to Liquid Volumetric Flow Ratio 0.3 and 0.5 percent
Gravitational Orientation of Flow Vertical and Horizontal
Conduit Diameter 2 inches
The mags~transfer coefficients were extracted from measurements of
the coefficient-area products, ka, and independent photographic measure-
ments of the interfacial areas per unit volume, a. The products, ka,
L
were established by means of a unique transient response technique in
which the changes in liquid phase concentration were measured as a func-
tion of time at only one position in a closed liquid recirculating system
while helium bubbles were injected at the test section entrance and
removed richer in oxygen at the exit. The apparatus for generating
these small bubbles (with an independent control of their mean sizej and
effectively separating a high percentage from the flowing mixture had to
be developed prior to the start of this research., These are described in
Chapter III along with the photographic equipment and technique for estab-
lishing the interfacial areas.
The fesults of this study are expected to be of immediate benefit
to the MSBR Program and should also prove useful to workers in the
general chemical industry. Application may extend to such diverse areas
as general extraction of radiocactive elements from reactor effluents,
bubble lifetimes in the coolant of liquid metal fast breeder reactors,
and oxygen treatment of sewage effluents, In addition, benefi%s of a
fundamental nature may be derived in that the research concerns transfer
of a scalar in a turbulent shear flow field in which the fluid velocity
field effectively seen by the bubbles is primarily due to the turbulent
fluctuations. The characteristics of mass transfer between dispersed
bubbles and a continuous liquid phase in turbulent flow are thus seen
to be of immediate scientific and practical importance,
CHAPTER IT
LITERATURE REVIEW
A comprehensive survey was made of literature related to mass
transfer between small bubbles and liquids in cocurrent turbulent flow.
An exhaustive review of all this literature would be lengthy and some-
what pointless. Consequently, only those works that are considered
representative of the field (not necessarily of most significance) are
included in this chapter and the author intends no derogation or slight-
ing by the omission of any work, No significance should be attached to
the order in which references appear. For a fairly complete documenta-
tion of work related to this subject, the reader is referred to several
excellent review articles.2 ®
Experimental-Cocurrent Flow
There have been very few direct measurements of mass-transfer
coefficients for cocurrent turbulent flow of small gas bubbles and
liquids, perhaps because substantial special apparatus seems to be
required for thesé measurements. Recently Jepsen® measured the liguid
phase controlled product of mass-transfer coefficient, k, and inter-
facial surface area per unit volume, a, for air/water flow in horizontal
pipes with and without spiral turbulence promoters. For straight tubes
fiithout turbulence promoters he correlated his data by the equation,
kas®l 2 gV 2 (008 po-68 _ 3 47 evo.4 .
As shown in Chapter IV, Page 58, the energy dissipation per unit
volume, ¢, can be represented as
v
(o 316) = B paire (1)
Therefore, Jepsen's correlation reveals that
Sh ~ Re'*l/§ 2a
Care must be taken in interpreting the influence of Reynolds number
on k when the product, ka, is reported because the interfacial area it-
self may depend on the Reynolds number. No attempt was made by Jepsen
to separate the area from the product.
Scott and Hayduk,'© in admittedly exploratory experiments, dissolved
carbon dioxide and helium into water, ethanol, and ethylene glycol in
horizontal flow pipelines. Thus they did vary the diffusivity but, like
Jepsen, did not separate the ka product.
Their results were correlated by the equation
ka = 0.0068 v 3074 S°-51 Mo.oia &30
Dl.SB 3
from which may be inferred
Sh ~ Re/&*%ta .,
Lamont!! and Lamont and Scott® dissolved, in single file fashion,
relatively large CO, bubbles into water under vertical and horizontal
flow conditions. They did not vary bubble diameter or Schmidt number.
At sufficiently large Reynolds_numbers their horizontal and vertical
results became identical. The data above these Reynolds numbers were
correlated as
k ~ Re©+B2
Heuss, King, and Wilke'® studied absorption into water of ammonia
and oxygen in horizontal froth flow, The liquid phase coefficients were
T
controlling only in the oxygen runs and consequently they did not vary
the Schmidt number and their results were also obtained as the product
of ka. However, using estimates of surface area in froth flow, their
data reveal
Sh ~ Re®*® .,
Hariott'? reported mass-transfer coefficients for particles of
boric acid and benzoic acid dissolving in water flowing cocurrently in
a two-inch pipeline, A data correlation was not given but a line tan-
gent to their data at the high flow end would indicate
Sh ~ Re®*93 |
Figueiredo and Charles® measured coefficients for dissolution of
NaCl particles carried along as a "settling" suspension in water in
horizontal flow., They correlated their data with mass-transfer coeffi-
cients previously measured for transfer between a liquid and the conduit
itself. However, a line tangent to the high flow end of their data
indicates
Sh ~ Ret*® .
Experimental-Agitated Vessels
Often the data for transfer to bubbles or particles in agitated
vessels are correlated in terms of the power dissipated. Using Equation
(1) we might relate these results to what would be expected for flow in
conduits,
Calderbank and Moo-Young'® correlated data for different particles
and small bubbles dispersed in different liquids in agitated vessels,
Their equation, determined partly through dimensional analysis, is
Using Equation (1) this would give for flow in conduits
Sh = 0,082 gel/ 3 Re®+52 (2)
They also indicate that in the range of mean bubble diameters, 0.025
< dvs’g 0.1 inches, the mass-transfer coefficients increase linearly,
undergoing a transition from "small" bubble behavior where Sh ~ Sc¥ 3 to
"large" bubble behavior where S8h ~ Sc¥ 2. They conclude that this tran-
sition corresponds to a change in interfacial condition from rigid to
mobile,
Sherwood and Brian'”’ used dimensional analysis to correlate data for
particles in different agitated liquids. Their correlation graphically
related Shb/801/3 to (emd4/v3)1/3. Using Equation (1) (with ev/p = em)
and drawing a line tangent to the high power dissipation end of their
correlating curve gives
Sh -~ SC1/3 ReC* 61 (d/D)-o.le . (3)
Barker and Treybal'® correlated mass-transfer coefficients for boric
acid and benzoic acid particles dissolving in water and 45% sucrose solu-
tions with a stirrer Reynolds number, ReT, proportional to the speed of
rotation., They reported
K ~ ReTC"88 Sct/ 2 g
If the power dissipation is assumed proporticnal to the cube of the
rotation speed, then
k ~ ReC*76 Scl/:a S .
The effect of Schmidt number is not as would be inferred from the zbove
because § was reported to be essentially proportional to Scfl/z in their
experiments.
9
The preceding are representative of data available that may have
direct applicability to cocurrent flow in conduits., Some other works
that may be of indirect interest include cocurrent turbulent flow of
19-22 mass transfer
dispersed liquid drops in a continuous liquid phase,
from a turbulent liquid to a free interface,®372® and innumerable studies
of the motions of, and mass transfer from, individual bubbles or parti-
cles under steady relative flow conditions (e.g., References 26-30).
For systems in which bubbles move steadily through a fluid, some
relevant findings include the fact that, depending on bubble size and
liquid properties, the bubble motion in a gravity field may vary from
creeping flow to flow characterized by a turbulent boundary layer.
Irrespective of this, the mass-transfer correlations usually take two
basic "Frossling" forms (neglecting the constant term) depending on
whether there is a rigid interface (no slip condition) or a completely
mobile interface with internal circulation of the fluid within the
bubble (or drop). In substantial agreement with theoretical treatments,
the former data are correlated with
Sh’b ~ Rebl/ 2 g01/ 3
and the latter
Sh, ~ Re, > ® 8¢/ % =pe V2 |
Good accounts of these relative flow equations and their derivations are
given by Lochiel and Calderbank®' and by Sideman. =%
Discussion of Available Experimental Data
It is seen that there have been very few direct measurements of
mass transfer to small cocirculating bubbles in a turbulent field and
10
none that are complete in terms of all the independent variables. The
product, ka, is often not separated, because of the difficulty in estab-
lishing the interfacial area, This makes some of the available data
difficult to interpret and of limited value for application at different
conditions.
Not enough experimental information is available to assess the
influence of Schmidt number on Sherwood number although the Schmidt