EPA-R2-72-023
May 1972
            CYCLIC OPERATION OF PLATE COLUMNS

               FOR GAS-LIQUID  CONTACTING
                           by

                    James D. Dearth

                   Lawrence B.  Evans

                   Edwin R. Gilliland
           Department of  Chemical Engineering

          Massachusetts Institute of  Technology

                Cambridge, Massachusetts



                      May 1,  1972
  This  report describes work  carried out  from  October,  1971

  through May,  1972  under  Task  Order No.  2  of  EPA Contract

  68-02-0018.

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                          PREFACE






     This report describes the results of work carried out un-



der Task Order No. 2 of EPA Contract 68-02-0018. during the



period October, 1970 through May, 1972.  This work comprises



doctoral thesis investigation of Mr. Dearth being carried



out under the supervision of Professors Gilliland and Evans.



When it is completed the results will be described in full



in Mr. Dearth's doctoral thesis.



     A decision has been made to seek continued support for



completion of the work by means of an EPA grant rather than



through extension of the current contract.  This report,



therefore, serves as an interim report to document the pro-



gress achieved to date under the contract and to support the



proposal for a grant.

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                         ABSTRACT





     Previous experimental and theoretical work has indicat-



ed that the efficiency and capacity of gas-liquid contact-



ing equipment may be improved by controlled-cycling of gas



and liquid flows.  However, difficulties encountered in the



design of large-scale systems, where hydraulic instabilities



and axial liquid mixing effects have been found to be severe,



has prevented wide-scale application of such systems to in-



dustrial separations.  This report describes a proposed pro-



gram for obtaining needed information on tray hydraulics



and liquid mixing, and summarizes some initial data and ten-



tative conclusions for both steady-state and cyclic flows



of an air-water system in a three-tray section of a cyclic



absorber.  Fluctuations in liquid-heads and interstage pres-



sure differences; entrainment of small air bubbles in the



downflowing liquid; and weepage of liquid due to liquid



"sloshing" in the gas flow period have been found to have



a pronounced effect upon column hydraulics.

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                          CONTENTS
                                                                 Page

I.  Introduction

     A.  General Description and Motivation                        1

     B.  Literature Review                                         2

     C.  Current Problem Areas                                     5

II.  Objectives

     A.  Short-range                                               7

          1.  Experimental                                         7

          2.  Computational                                        8

     B.  Long-range                                                8

III.  Apparatus                                                   10

IV.  Experimental Approach

     A.  Hydraulics                                               12

     B.  Liquid Mixing                                            15

V.  Results and Tentative Conclusions

     A.  Hydraulics                                               16

          1.  Steady-state Air Flow                               16

          2.  Steady-state Liquid Flow                            19

          3.  Variable-Venting Experiments                        26

          4.  Vented Cyclic Results                               30

          5.  Sealed Steady-State and Cyclic Operation            34

     B.  Liquid Mixing                                            36

     C.  Mathematical Simulation Models                           37

          1.  Hydraulics                                          37

          2.  Mass-transfer Model with Mixing                     40

VI.  Direction of Current and Future Work                         40

VII.  Summary                                                     42

VIII.  Appendix                                                   43

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A.  Models for Axial Liquid Mixing in Cyclic Operation       . ^3

     1.  Liauid-Phase Mixing from Evolution of Vertical       ^3
         Concentration-Distance Profile.

     2.  Overall Mixing Parameter from Measurements of        ^5
         Well-Mixed VFP Composition

B.  Model for Gas and Liquid Flows Through a Perforated       ^7
    Plate.

C.  Mathematical Model for Mass-Transfer and Licruid Mixing    51
    in a Cyclic Absorber.

     1.  Gas Flow Period                                      51

     2.  Plug-Flow Conditions                                 52

     3.  Mixing-Model Equations                               52

     4.  Periodicity Conditions                               53

     5.  Average Exit-Gas Composition                         53

     6.  Overall Column Efficiency                           -5^

     7.  Dimensionless Form                                   5^

D. Sample Calculations                                        59

     1.  Comparison of Experimental Slope of Liquid-head      59
         vs. Flow Rate with Hagen-Poiseuille Law.

     2.  Calculation of Flowrate for Critical Weber Number.   60

     3.  Effect of Licruid Aeration on Velocity-Head           60

     4.  Initial Rate of Pressure Rise Due to Air Flow        6l
         into a Sealed Column Section

     5.  Estimate of Liquid Residence-Time and Ratio of       6l
         Flow-Period Lengths.

E.  Nomenclature.                                             63

F.  Literature Cited.                                         69

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                            -1-




I.  Introduction



     A.  General Description and Motivation



     Increased process efficiency and equipment capacity are



among the benefits which can result from controlled cycling



of many traditionally steady-state chemical engineering oper-



ations.  Sufficient studies, both experimental and theoreti-



cal, have been conducted to demonstrate that benefits can



accrue from imposing a repetitive discontinuity upon an oth-



erwise continuous operation.  Because of the widespread use



of gas-liquid contacting equipment in industry for distilla-



tion or gas absorption applications, it is felt that the intro-



duction of controlled cycling into this area may have a sub-



stantial impact upon the economics of any process which uti-



lizes these unit operations for purification or product re-



covery.  In particular, the perfection of a high-capacity,



high-efficiency tail-gas scrubber design might help to re-



duce the economic  burden imposed on many industries by the



advent of stricter state and federal pollutant emissions stan-



dards .



     This investigation is concerned with the design of



staged gas-liquid contacting equipment for cycled operation.



The configuration currently under consideration resembles a



conventional sieve-tray column, but lacks the weirs and down-



comers associated with normal crossflow operation.  Each oper-



ating cycle consists of two distinct phase-flow periods.  Dur-



ing the vapor flow period gas is allowed to flow upward for



a short period of time, at a rate sufficient to maintain a

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                            -2-

pool of liquid on each tray without leakage through the per-
forations.  Mass transfer occurs across the interface between
the rising gas bubbles and the vigorously agitated liquid.
During the liquid flow period the gas flow is interrupted
and liquid is allowed to drain through the trays by a weep-
age mechanism, while fresh liquid is fed into the column.
Before proceeding to outline the objectives of the current
study and the organization of the research program, it would
be appropriate to review the historical development of con-
trolled-cycling and to summarize some of the important con-
clusions of previous investigators.

     B.  Literature Review
     The concept of cycled operation was originated by Cannon
(!_) in 1952.  At that time it was suggested that many exist-
ing mass-transfer operations might be substantially improved
by changing the method of contacting the flowing phases.  The
first mention of an operating cycle was made four years later
in connection with a proposed liquid-extraction process which
employed alternate upflow and downflow of the light and heavy
phases (2).  Cycled or "rmlsed" columns of this type were
found to have high separation efficiencies and capacities,
and many have since found their way into industrial use.  Oth-
er cycled systems have been employed on a laboratory scale for
particle-size segregation, crystallization, and ion exchange
(1§.' ii' 12.) •
     The first data on cycled gas-liquid systems were reported
by Gaska and Cannon (5) and McWhirter and Cannon (13) for the

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                            -3-





rectification of benzene-toluene and methylcyclohexane-n-



heptane mixtures in a 2-inch ID glass column.  It was conclud-



ed from these early investigations that cycled distillation



columns could be operated for either high efficiency or high



capacity, depending upon the relative lengths of the gas and



liquid flow periods.  The highest column efficiencies observed



were in the range 130 to 150%, indicating that each tray of a



cycled column had a separating ability superior to that of a



single "theoretical plate."  In a subsequent investigation



McWhirter and Lloyd (14) confirmed the earlier results using



a 6-inch ID column containing five 3-inch "packed plates."



For operating cycles of 3 to 9 seconds' duration overall ef-



ficiencies were in the range 160 to 200%.  The observed sepa-



rating ability was rationalized in terns of the greater aver-



age mass-transfer driving forces present in a cycled column.



A simple mathematical model of a cycled column confirmed this



hypothesis and predicted efficiences similar to those observed.



     Theoretical analyses by Robinson and Engel (17) and



Sommerfeld, et al.  (1_9_) established an exact analogy between



the time-axis concentration profiles in a cycled column and



the crossflow concentration gradients in conventional columns.



The latter case had been analyzed by Lewis (9) who concluded



that such gradients could produce substantial improvements in



the efficiency of bubble-cap trays.  Analytical transient solu-



tions to McWhirter's model were developed by Chien, et al.  (3)



for the simplest case of a linear equilibrium relation, and



iterative procedures were developed to handle more general non-

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                             -4-


linear expressions.  An extensive simulation study was carried

out to determine the effects of local point efficiency, slopes

of the operating and equilibrium lines, amount of liquid dropped

during the liquid flow period, and other parameters, on both

overall column and individual plate efficiencies.  The most

important conclusions may be summarized  as follows:

     1)  For controlled cycling operation at total reflux
     with negligible liquid mixing during the liquid flow
     period, the overall column efficiency attains its max-
     imum value when the contents of one tray are dropped
     per cycle.

     2)  Liquid mixing during the liquid flow period tends
     to degrade the efficiency improvement obtained by cy-
     cling.  In the limit of perfect mixing there is no im-
     provement.

     3)  The fractional increase of column efficiency be-
     tween noncycled and cycled operation is greatest when
     the individual point efficiencies are high.

     4)  The overall column efficiency increases to an
     asymptotic limit as the total number of stages is in-
     creased.  This limiting behavior of overall efficiency
     was noted by Horn  (8) , who developed an asymptotic
     solution using z-transform techniques.

     Schrodt, et al. (18) carried out a series of experiments

using a 12-inch ID cycled column containing 15 perforated

trays without downcomers.  It was concluded that the cyclic

unit was superior in flexibility and throughput character-

istics to the same unit in conventional dual-flow operation;

however, the cycled column efficiencies were, at best, slightly

lower than for conventional-flow.  One reason for this was

that the column operation was hydrodynamically unstable.  It

was noted that the existence of dynamic flow lags often caused

the lower trays to drain completely before the liquid had be-

gun to flow from the upper trays.  Gerster and Scull  (6\, in

studying the cyclic desorption of ammonia from aqueous solu-

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                            -5-


tion into an air stream, observed a different type of insta-

bility in the form of excessive liquid accumulations on the

lower trays.  Despite unimpeded liquid mixing, efficiencies

as much as 40 percent higher than those obtainable in conven-

tional service were reported.  A model for liquid mixing was

proposed and incorporated into the existing model for mass

transfer.  The data were found to be in good agreement with

the model predictions, and values of a single "mixing param-

eter" were estimated.

     To gain insight into the nature of the hydraulics of a

cycled column Wade, et al. (21) formulated a reasonably de-

tailed mathematical model of a cycled distillation column.

Using several empirical relations for gas and liquid flow

rates, they found that it was possible to alleviate the prob-

lem of liquid-flow lags by strategic manipulation of isola-

tion valves in the lines to the condenser and reboiler.  The

shortcomings of the model and of the method of solution were

as follows:

     1)  The hydraulic relations used were completely
     empirical, with no experimental justification.

     2)  The solutions obtained were for single cycles
     or small numbers of cycles.  No attempt was made
     to select initial conditions to satisfy the perio-
     dicity conditions of pseudo-steady cycled operation.

     3)  For convenience in the solution of the model
     equations, perfect mixing of the liquid phase was
     assumed at all times.


     C.  Current Problem Areas

     Thus far, a general lack of understanding of the tray

hydraulics and liquid-mixing phenomena which occur in full

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                             = 6-





scale cyclic equipment has made it virtually impossible to



apply the results obtained from simulation studies to the



design of multistage cyclic cascades.  In the first place, the



existing models for cyclic mass-transfer presuppose a knowl-



edge of the liquid holdup on each tray.  This quantity is de-



termined by the liquid head needed to drive a specified flow



rate of liquid down through the tray perforations against an



opposing  gas-phase pressure difference.  This flow configura-



tion has received little attention in previous literature,



since in a conventional crossflow tray weepage of liquid through



the holes is undesirable: in fact, much effort has been di-



rected  towards the prediction of the minimum gas velocities



needed to prevent liquid flow through the holes.  Existing



theories are unable to predict the magnitudes of liquid heads



and gas-ohase pressure differences, and the phenomenon of free



liquid drainage with no gas-phase pressure difference appears



not to be adequately described by simple orifice equations.



Yet liquid holdup is a predominant factor in determining



point contacting efficiency and cycle time.



     There is additional experimental evidence which indicates



that hydraulic coupling among successive stages may result in



undesirable drainage-rate and holdup characteristics.  Trays



near the top end of the column may run dry while excessive



amounts of liquid may accumulate on the lower trays.  Quali-



tative explanations for these phenomena have been suggested,



but no quantitative techniques have been developed to predict



the occurrence of hydraulic instabilities and to indicate

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                             -7-





methods for alleviating their undesirable effects upon col-



umn performance by proper design.



     The results of a ground-breaking study of axial liquid



mixing have suggested an effective one-parameter mixing model



which can be easily incorporated into the existing overall



simulation scheme for cyclic absorption.  It remains to cor-



relate the extent of mixing against flowrates, liquid heads,



and geometric parameters in order to indicate column design



configurations for minimizing the undesirable effects of liq-



uid mixing during the LFP.






II.  Objectives



     A.  Short-Range.



     The purpose of the current research program is to pro-



vide information necessary to the formulation of rational



criteria for the design of cyclic absorbers.  The immediate



objectives of such a study are summarized below.



          1.  Experimental.



              The goal of the experimental ohase of the



          work is to provide information on the physical



          processes which influence the hydraulic opera-



          tion of cyclic columns.  Once the important phe-



          nomena are understood, the data obtained can be



          used to test mathematical models and evaluate



          parameters in the proposed correlations.  The



          specific objectives are as follows:



               a.  To develop correlations for predicting



               gas and liquid flows as functions of liquid

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                        -8-





          head and interstage pressure difference, for



          various tray geometries.



          b.  To evaluate alternative column configura-



          tions and modes of operation to gain an appre-



          ciation of their relative advantages and limi-



          tations .



          c.  To evaluate mixing parameters and correlate



          them to hydraulic and geometric variables.



     2.   Computational.



         The shortcomings of previous attmpts to simulate



     hydraulics and mass-transfer under controlled-cyclic



     conditions were due primarily to the lack of experi-



     mental hydraulic data.  It is anticipated that this



     need will be adequately filled by the correlations



     derived from the experimental phase of the work, and



     that the following simulation studies may then be



     carried out:



          a.  To simulate the hydraulic behavior of a



          long cyclic cascade, noting any non-uniformi-



          ties of flow or liquid-head distribution pre-



          dicted.



          b.  To simulate the overall mass-transfer be-



          havior of a cyclic absorber, to obtain values



          of overall column efficiency as functions of



          a set of column parameters specified by the



          designer.




B.   Long—range.



     The ultimate objective of the research program is to

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                       -9-





answer the following set of design questions:



     1.  Is cyclic operation of absorption and distil-



     lation systems technically feasible?



     2.  What are the optimal choices for the  design



     and operating parameters?



     3.  Is the "best" cyclic system economically com-



     petitive with existing equipment?



The studies carried out to date seem already to have an-



swered the first question in the affirmative.   It remains



to solve the optimal design problem and to interpret the



results in the light of similar experience for convention-



al columns.



     The design model formulated in the initial stages of



the research program should be tested against  experimental



results to assess its reliability.  A reasonable method



for carrying out such tests is to select a gas-liquid sys-



tem and to conduct a series of small-scale experiments



to develop correlations for point efficiency.   The effi-



ciency correlations, together with equilibrium data and



specifications of inlet and outlet gas concentrations and



gas flow rate, are fed into the mathematical model, and



an optimum set of design-variable values is generated.



The actual performance of this "optimal" column once con-



structed may then be compared with that predicted by the



model.  The results of such a study would yield informa-



tion on both the shortcomings of the model and the actual



separations obtainable in a well-designed cyclic absorber.

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                            -10-





III.  Apparatus.





     The experimental apparatus shown in Figure 1 consists of



a three tray section of a 6-inch diameter Lucite column, with



associated gas and liquid supply systems.  The trays are fabri-



cated from 1/4-inch thick plexiglas sheet with holes drilled



on a triangular pitch.  A sightglass is provided on each of



the bottom two trays for measurement of the average clear liq-



uid head, and a manometer is provided for measurement of the



interstage pressure difference across each of the test trays.



The tray inserts  currently in use contain 1/8-inch holes, with



a fractional perforated area of 10%.  In order to insure uni-



form drainage, the bottom of each tray is sprayed with a fluo-



rinated hydrocarbon coating to make it non-wettable.



     The gas used is air, supplied from a 125 psig oil-free



compressed air line, passed through a reducing pressure regu-



lator, humidified to 95% of saturation, and delivered to the



base of the column through 1-inch supply lines containing ori-



fice plates for flow metering.  The liquid phases consist of



water and a dilute sodium chloride tracer solution pumped



from two identical 150-gallon polyethylene tanks through a set



of rotameters to the top of the column.



     Cyclic control of flows is imposed by placing 3-way so-



lenoid valves in the lines, in close proximity to the column.



During their respective "off-cycles the air will be vented,



while water and tracer solution will be returned to their



storage tanks.  This arrangement permits continuous metering



of flows even under conditions of cyclic operation.  The sole-

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                                                    "Sliding Box" for Step Tracer Inputs
 Rotameters
   AT
                       Return
           1  i
                                                     Rotameters
                                                    	A
          r
             Bypass
                  }
Pneumatic cylinder
                                  ,
                                         Water I (Tracer
                                          Side
                   S1de
                            Return
       1%-HP
     Centrifugal
        Pump
 125 psig
Compressed
   Air
                                Leads
                              to conduc-
                              tivity
                              bridge
                              and re
                              corder
Vent -e-
 Orifice
  Plate
                                     Bypass
                                  Sightglasses,     1%-HP
                                  Manometers,     Centrifugal
                                  and flanifold       Pump
                              4-kw. Heating
                                Element
                 Saturator
                   Drum
                         Straightening
                            Vanes
                                      FIGURE  1
                                                 Drain
                                SKETCH OF PROPOSED APPARATUS
                                Column Scale:  2 mm = 1  inch
                                Gas and Liquid Supplies  Not
                                  to Scale.
                                        Cxi
                                    -  Flow-Control  Valve

                                    - Pressure-Reducing Valve

                                    - Solenoid Valve
                                                                      (ODD 11/15/70)

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                            -12-






noid valves are operated by electrical signals from a cycle-



timer-relay control box, which permits independent variation



of the gas and liquid flow period lengths.



     To permit optional venting of the column sections to at-



mospheric pressure, a set of solenoid valves is mounted at the



rear of the frame.  Each valve is connected to a venting port



in a particular column section, and may be  closed or opened



by manual switching or by cyclic relay control.  A float valve



has been installed in the bottom of the column to seal the liq-



uid drain line and prevent the oscillations in the overflow



leg during the gas flow period.



     A rather uniaue feature of the apparatus is the "sliding



box" arrangement provided for the alternate introduction of



water and salt solution during liquid-mixing experiments.  The



box has two chambers, one containing water and the other, tra-



cer solution.  The position of the box relative to the perfor-



ations in the top plate is controlled by the piston of a pneu-



matic cylinder, so situated that either chamber may be located



above the column.  Salt concentrations in the liquid on a par-



ticular tray may be monitored by inserting 5 mm. glass conduc-



tivity probes through the side wall of the  column.  Fittings



allow the probes to be traversed radially in order to check



for concentration gradients in the radial direction.






IV.  Experimental Approach.




     A*  Hydraulics.



          In dealing with the complex phenomena associated with



     the hydraulics of a sealed cyclic column, it has been



     found advantageous to decompose the more difficult general

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                       -13-






problem into a sequence of individual sub-problems more



amenable to measurement and interpretation.  The piece-



wise - steady nature of cyclic operation suggests that



one might reasonably group the phenomena of interest into



three main subdivisions as follows:



     1.  Steady-state gas flow through a non-flowing mass



     of aerated liquid supported on a sieve tray.



     2.  Steady-state liquid drainage through the perfor-



     ations of a sieve tray against an opposing gas-phase



     pressure difference.



     3.  Departures from steady-state gas flow and liquid



     drainage, resulting from on-off flow cycling.



Each of these sub-areas can, in turn, be broken down into



their component phenomena, as illustrated by the diagram



in Figure 2.  Pressure drops for gas flow are, in general,



represented as the sum of a dry-plate component and a liq-



uid-head contribution.  In an analogous fashion, steady-



state liquid heads can be thought of as being composed of



a liquid head for free drainage with no gas-phase pressure



difference, and an additional level difference to overcome



the effect of pressure buildup in the gas phase.  Simi-



larly, the departures from steady-state hydraulics may



result both from phenomena which arise when the column



sections are vented during the liquid flow period, and



from other effects due exclusively to the decay of the



pressure gradient set up during the vapor flow period.



     The independent variables and their approximate



ranges of variation may be summarized as follows:

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                        -15-
     1.  Gas Flow Rate:        0.5 - 1.5 ft3/sec (1 atm, 70°F)



     2.  Liquid Flow Rate:     1   - 30 gal/min.



     3.  Gas Flow Period:      0.5 - 10 sec.



     4.  Liquid Flow Period:   0.5 - 10 sec.



     5.  Tray Hole Diameter:   1/8 - 1/2 inch



     6.  Tray Free Area:       5   - 20 %



B.  Liquid Mixing.



     The values of liquid mixing parameters reported in



the literature have been deduced from mass-transfer ex-



periments by comparing the experimental results with



those obtained from the mathematical simulations modi-



fied to include a simple mixing model.  The excellent



agreement reported between theory and experiment for a



constant mixing parameter value ic an encouraging sign



that the model selected may give a good representation



of the actual column behavior.



     What is now needed is a correlation of mixing-param-



eter values as functions of liauid flow rate, liquid hold-



up, plate spacing, and tray geometry.  For this purpose,



mass-transfer experiments would be both expensive and



time-consuming, and the results might contain errors and



uncertainties due to imperfect modelling of mass-transfer



phenomena and inaccurate values of input parameters such



as point efficiency.  As an alternative it has been found



desirable to devise a means to test the mixing model in



the absence of mass-transfer, thus taking advantage of



the fact that mixing of liquid on the trays results only



from hydraulic phenomena.

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                             -16-
          The experimental technique involves the introduction



     into the test column of water and a dilute sodium chloride



     tracer solution during alternate liquid flow periods of



     cyclic operation.  This alternating step-function concen-



     tration input gives rise to salt-concentration gradients



     in the vertical direction on each of the lower two test



     trays during the liquid flow period, as well as to up-



     and-down fluctuations in average tray licruid composition



     in alternate cycles. The distance-gradients and time-vary-



     ing fluctuations in average concentration can be monitored



     by inserting conductivity probes into the tray liquid and



     recording the changes in the voltage imbalance of a bridge



     circuit which result from changes in the resistance of



     the solution.  The distance-gradient results can be used



     to provide information on the detailed mixing process,'



     while  the average-concentration measurements permit the



     straightforward evaluation of an overall parameter.  The



     interpretation of the results is discussed in Appendix



     VIII.A.






V.  Results and Tentative Conclusions.



     A.  Hydraulics.



         In the following sections, the results for  gas and



     liquid flows through a 1/8-inch hole size, 10% free area



     tray insert have been summarized.  Tentative conclusions,



     based on the existing information, have been formulated,



     and suggestions for further study in each of several areas



     have been made.



          1.  Steady-State Air Flow.

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                   -17-
    One of the first experiments performed on the



completed column assembly was the measurement of



dry-plate pressure drops for the first set of tray



inserts.  A large quantity of experimental data in



this area is available in the literature and a gen-



eral correlation of the data has been suggested by



McAllister et al.(ll).  The usual approach is to ex-



press the pressure drop as a multiple of the velocity-



head of the gas flowing through the holes.  The pro-



portionality constant which will be referred to as



a "discharge-loss coefficient," is assumed to be



equal to the product of a term representing the sum



of sudden contraction losses, sudden expansion losses,



and friction losses,multiplied by a function of the



plate thickness to hole diameter ratio.  A comparison



of the data with this calculation is shown in Figure



3.  The results have been plotted as discharge-loss



coefficient vs. Reynolds number.  The calculated val-



ue of the coefficient, neglecting the friction term,



is 1.15. This is in excellent agreement with the



data at the high-Reynolds number asymptote.  At Rey-



nolds' numbers below about 3000 the omitted friction-



loss term seems to become important, resulting in an



increase in the experimental coefficient.  The scatter



in the data at the low Reynolds' number  end is due



to the fact that in this region both gas flowrates



and pressure-drops were extremely small, resulting



in large percentage errors.

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                   -19-
    All experimental observations of cyclic opera-



tion to date suggest that, with one possible excep-



tion, transients at the beginning of the gas flow



period are very fast.  A fraction of a second after



resumption of gas flow, the column is hydraulically



at steady-state, and this steady-state is, for all



practical purposes identical to that which one finds



in a cross flow tray in the limit of zero liquid rate.



Hence, one may make use of all available correlations



for calculating wet-plate pressure drops from liquid



heads and dry-plate pressure drops.  If the liquid



holdup on every plate is known at the end of the liq-



uid flow period, the pressure gradient through the



column during the gas flow period may be simply and



efficiently computed.  The modelling difficulties



are associated almost entirely with liquid flow.






2.  Steady-sJ:ate Liquid Flow.



    Two limiting modes of operation are of particu-



lar interest, when one considers the relationships



governing liquid flow in a cyclic column.  In the



first case, henceforth referred to as "vented" oper-



ation, the intertray spaces are connected via elec-



tric or pneumatic valves to a common manifold.  At



the beginning of the liquid flow period these valves



are opened, permitting essentially instantaneous



equalization of gas-phase pressure across every tray.



As a result, liquid flow is influenced only by the



tray liquid head; no pressure buildups or fluctuations

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                   -20-


may occur in the gas phase.  The opposite extreme

of "unvented" operation dispenses with the addition-

al valves and manifold and allows interstage pressure

differences to "seek their own levels."  Pressures

remain at non-zero values even after the inflow of

air at the bottom is interrupted, and oscillations

in the gas phase may have a significant effect upon

liquid drainage.  All stages are coupled together

through the gas phase, and a disturbance in liquid

head will be communicated up and down the column by

resulting pressure disturbances.

    A mathematical representation of either of

these cases must make use of the fundamental steady-

state discharge relationship for liquid flow through

a perforated plate.  This relationship is determined

by means of the following experiment:

    With the pressure in all column sections main-
tained at one atmosphere, water is introduced through
a distributor pipe at the top of the column at a
specific volume flowrate.  The liquid drains through
the perforations of each plate and falls through the
intertray space onto the tray below.  Liquid heads
are established on the various stages and are meas-
ured, with respect to some horizontal datum plane,
on sightglasses.

The results are plotted as clear liquid head above

datum in inches of 1^0 vs. liquid volume flowrate

in gallons per minute.  Such a plot is shown in Fig-

ure 4 for the 1/8-inch hole size, 10% free area tray

insert.

    Although the data could be easily replotted as

discharge-loss coefficient vs. Reynolds number, in

analogy with the air-flow results, we will be content

-------
                     -21-
    /.&
     /.o
    0.8
I  0.6

2
    o.z
       o
  \      T


 '/Q - /*/€/•/

 /O % P/2EE AKEA
            STEADY ~
  Z     4     6     8
    0
L/qa/D  FLOW #AT£  ( GALLONS
                                                       /&
                                 4  .

-------
                   -22-
for the moment with this simple representation.



Note that at low flowrates the dependence is essen-



tially linear and that at flowrates above about 10



gallons per minute the curve becomes concave upwards.



    All flowrates in the range of experimental meas-



urements correspond to Reynolds' numbers less than



2100, but because the entrance length required for



complete development of a parabolic velocity profile



is from one to two orders of magnitude larger than



the length of each short tube, the discharge charac-



teristics are dominated by entrance effects.  A sim-



ple calculation  (Appendix VIII.D.I) illustrates that



the slope of the linear portion of the experimental



curve is about 20 times what one would predict using



Poiseuille's law.  The predominant effects are the



contraction of the entering jet and the shear of



the tube wall.  A discharge-loss coefficient defined



for this case would be expected to have a value in



the range 1.5 to 2.7, with a weak inverse power-de-



pendence on Reynolds' number.  This agrees well with



the data at the high-flowrate end of the curve.



    If there is no wetting of the bottom of the tray,



liquid will drain as single drops until the inertia



of the liquid flowing  through the holes is sufficient



to distort the drop shape and produce an elongated



jet.  The critical Weber number for this drop to jet



transition is about 6.8. For the tray insert under



consideration, this critical value corresponds to a

-------
                   -23-
volume flowrate of 11.3 gallons/minute.CAppendix
VIII.D.2.)
    Above this flowrate jets have been observed to
form at all holes; however, intermittent jetting has
also been observed at flowrates considerably below
this critical value.  This seems to imply that local
hole velocities may be large enough to give rise to
jet formation, even though the average velocity, based
on the entire perforated area, is not.  In effect,
we are saying that at any given time, only a frac-
tion of the available holes  is  passing liquid.  The
data seem to indicate that this effective fraction
increases as flowrate is increased, thus tending
to moderate changes in the velocity head, and yield-
ing the nearly-linear dependence observed at low
flowrates.  The sealing and unsealing of holes is
believed to be brought about by the fluctuations
of liquid head at various locations on the tray, with
liquid flow occurring at those perforations where
the instantaneous local liquid head is sufficient to
overcome surface tension.
    A further complication results from the fact
that liquid drops or streams falling onto a free
liquid surface entrain air bubbles into the bulk
liquid phase.  Some of these pass on through the
perforations with the downflowing liquid and enter
the gas space below.  This phenomenon produces a
small steady flow of the gas phase down the column

-------
                   -24-
during the liquid flow period.



    If there is good disengagement of gas from liq-



uid in the bottom of the column, then in the complete-



ly vented mode all air that passes down through the



bottom stage by this entrainment mechanism must



exit through the bottom venting port.  Hence, to



measure the rate of air entrainment one needs to meas-



ure only the flow rate of air through the vent.



Since rotameters and soap-film meters were found to



be unsatisfactory flow-measuring devices due to ex-



cessive pressure drops, a scheme was devised for



mixing a small metered flowrate of CC>2 with the



main vent air stream.  The air flowrate was calcu-



lated from the known CC>2 rate and the mole fraction



of C02 in the mixture, determined chromatographically.



The results are shown in Figure 5.



    This plot shows air entrainment rate in cc./



sec. as a function of liquid flowrate in both gallons/



minute and cc./sec.  The curve is seen to be "s"-



shaped, with an apparent point of inflection in the



vicinity of 8 gallons/minute.  The interpretation of




such data is quite complicated, since at least two



competing processes are at work.  Increasing the



liquid flowrate by itself probably tends to increase



the entrainment rate by increasing the total volume



of air bubbles in the liquid phase, as well as by in-



creasing the size of the largest bubble whose terminal



rise velocity will be exceeded.  On the other hand,



the accompanying increase in liquid holdup makes it

-------
                     -25-
                 FLOW &ATE (c.c./sec.)
      o   /oo  zoo
   300
   ^so
lg  ZOO


K.

§  /so


!
£  /OO
    so
    o
               i     i
                                 I    I     I    I
                              Sr£AD/ - Sr/t re
                       I	I	I	J	I
      O
         L/Q U/D

-------
                   -26-
more difficult for bubbles to penetrate to the tray



surface.  The latter effect is more important at



high flowrates and probably accounts for the de-



creasing slope at the upper end of the curve.  These



data indicate a 20 to 30 percent aeration  of the



liquid flowing down through the holes.  If the mix-



ture of air and water is a uniform froth of small



bubbles in the liquid it can be shown  (Appendix VIII.



D.3.) that the pressure drop for flow through the



perforations is from 30 to 40 percent larger than



for the same volume rate of non-aerated liauid.



3.  Variable-venting Experiments.



    Another simple calculation  (Appendix VIII.D.4)



shows that pumping air at a rate of 200 cc./sec. in-



to a sealed volume of 5.5 liters maintained at room



temperature results in an initial rate of pressure



change of 1 inch of water every 0.07 second.  Thus,



the hydraulic conseauences of air entrainment can



be quite significant in an unvented column.  One can



imagine an experiment in which the bottom vent line



is gradually closed.  If air is carried down by the



liquid into this closed gas space the pressure in-



creases, the liquid head builds up, and as a result,



the rate of influx of air is diminished.  At steady-



state the flowrate of air into the sealed section



must be balanced by an equivalent outflow, either by



entrainment of small bubbles in the exit stream or by



air bubbling up through the perforations.



    Such variable-venting experiments have been car-

-------
                   -27-






ried out by adjusting a valve in the vent line from



the bottom section.  Figures 6 and 7 show the effect



upon tray liquid head and interstage pressure differ-



ence of decreasing the air venting rate from its



maximum value to zero.  Pressure difference and



clear liquid head in inches of water have been



plotted against air venting rate in cc./sec., for a



range of different liquid flow rates.  When the vent



valve is fully-open the pressure difference is zero



and the liquid-head lies on an envelope corresponding



to the "s" shaped entrainment  curve discussed pre-



viously.  As the venting rate is reduced to zero the



pressure difference and liquid head increase, gradu-



ally at first, with a final sharp rise as the vent-



ing rate is decreased below about 15 cc./sec.



    The difference between the clear liquid head



and the differential pressure constitutes a nei: pres-



sure difference favoring liquid flow.  In Figure  8



values of this quantity are plotted against air vent-



ing rate.  These data indicated that at a fixed liq-



uid flowrate the net difference decreases as the vent



is closed, even though the individual values of liq-



uid head and gas-phase pressure difference are in-



creasing.  In effect, this says that it is "easier"



to force a given flowrate of liquid down through a



tray into a sealed vapor space than into a vented space,



whereas one would intuitively expect that the net



difference of head should be about the same in both

-------
2.2
o.z -
S^/f£oi
V
O
A""
O
a "
•
A
i.'fu'C/ Put' (tjpm)
4 .36
' S-5
7 . Z5
...... ..8.73. ...
/O.Z
// ,6S
/•3. /
                /OO
        A /x?
 /so
&Are
 2.00

(c.c.,
                                                                                                               I
                                                                                                              10
                                                                                                              00
                                                                                                               I

-------
                -29-
OJ -
Syrneo i>
V
O
A
O
D
«
A
Liquid Rote. Cop?»)
4.36
S-.B.
7.2S
8 .73
/0 .2,
/ / .63-
/ 3 . /
O
/CO
ZOO
                                               3 CO
                                         ./sic.)
                            8

-------
                   -30-
cases.



    Two factors seem to be at work here.  First, as



the vent valve is closed and liquid head is allowed



to build up, the fraction of air bubbles in the liquid



draining through the holes is cut down dramatically.



As pointed out earlier, decreasing air entrainment



decreases the velocity-head of the flowing gas-in-



liquid dispersion, so that one might expect to ob-



serve a drop in the required pressure difference.



Second, when the column section is sealed, pressure



fluctuations in the gas phase increase in magnitude.



It can be shown that such fluctuations act to over-



come the stabilizing influence of surface tension,



and allow larger flow rates of liquid with the same



average net pressure difference.  More air-entrain-



ment data are needed at different flowrates and liq-



uid heads in order to draw quantitative conclusions



about the relative importance of these factors  (Ap-



pendix VIII.B.).  It is anticipated that experiments



with different tray inserts will provide the necessary



information.



4.  Vented Cyclic Results.



    One of the reasons for investigating the clear



liquid head vs. liquid flow relationship at steady-



state was that the results were expected to be appli-



cable to a vented cyclic column.  It was hoped that



the removal of gas-phase pressure differences would




stabilize liquid flow, so that liquid holdups would

-------
                   -31-
be about the same on all stages and eaual to the



values predicted from steady-state data.  In fact,



although the expected stabilization of flow was



achieved, clear liquid heads measured in controlled-



cyclic operation were found to be consistently lower



than those measured at steady-state.  A comparison



of results for the two cases is shown in Figure 9.



The plot shows clear liquid head in inches of water



as a function of liquid flow rate in gallons per min-



ute.  The solid circles denote steady-state results,



while the open symbols represent cyclic data at var-



ious liquid flow period lengths, ranging from



1.2 to 9.6 seconds.  The gas flow period and air flow



rate were held constant at 5-4 seconds and .9 ft /sec.,



respectively.



    The clear liquid heads measured for the cyclic



case are observed to be always less than the corres-



ponding values at steady-state, regardless of liquid



flow rate or length of liauid flow period.  The effect



of liquid flow period length is most pronounced at



the high liquid rates where the shorter liquid flow



periods give rise to smaller clear liauid heads. The



near-coincidence of the curves for liquid flow periods



of 5.4,7.8, and 9.6 seconds seems to indicate that



as LFP length is increased indefinitely an asymptotic



upper limiting liauid head is approached at a given



flowrate.



    There is good evidence to support the contention



that weepage during the vapor flow period may be part-

-------
-32-

-------
                   -33-
ly responsible for the observed discrepancies.  Grad-



ual shifts in the sightglass levels have been noted



during the course of a cycle, indicating a decrease



of liquid level during the vapor flow period.  At



large holdups or gas flowrates a side to side oscil-



lation of the froth has been found to produce brief



spurts of liquid flow near the side walls.  If liq-



uid flow occurs during part of the VFP,  the actual



flowrate per unit time will be reduced from the value



obtained by assuming flow only in the LFP, and this



reduction in average flowrate will be reflected in



a smaller value of clear liquid head.  Since the



total liquid weepage per cycle is equal to the aver-



age weep rate multiplied by the gas flow period



length, the correction for weepage is largest when



the VFP/LFP ratio is large, and it is under these



conditions that the maximum discrepancies in liquid



holdup are observed.  However, the weepage hypothesis



does not seem to account for the differences between



the cyclic and steady-state results at low flowrates.



    At present time experiments are being undertaken



to measure the effect of varying LFP time, VFP time,



and the VFP/LFP ratio, in order to determine the ex-



tent of their interactions.  It would also be instruc-



tive to eliminate liquid oscillations by appropriate



baffling and to observe the effect upon the clear



liquid head results.  It is believed that physically

-------
                   -34-






meaningful corrections can be applied to the



steady-state results to predict the hydraulic be-



havior in vented cyclic operation.



5.  Sealed Steady-State and Cyclic Operation



    Although no reliable quantitative studies have



been made either at steady-state or in the controlled-



cyclic mode with all column sections sealed, some



qualitative observations are available.  It has been



noted that although the liquid holdups and interstage



pressure differences on the lower trays were similar



in magnitude, those on the top plate were always found



to be much larger, sometimes by factors of three or



four.  In the cyclic mode, this problem became extreme-



ly serious, and holdups of as much as 6 inches of



clear liauid have been observed on the top stage at



liquid flow rates around 2 gallons per minute.



    It is feared that many of the problems encountered



are the result of liquid-flow end effects.  At the



top of the column the liquid phase is introduced on-



to the highest tray through a perforated-pipe distri-



butor.  The .liquid streams leaving the distributor



have velocities much higher than the drainage veloc-



ity from a tray insert, and this may result in a



greater entrainment of air bubbles into the gas space



below the top plate.  It has already been mentioned



that column operation may be sensitive to the amount



of air entrained in the drain-line liquid.  This is



undesirable, since drain-line configurations may dif-

-------
                  -35-





fer considerably from one unit to the next, yet it



is desired to make the hydraulic performance as uni-



form as possible.  A solution suggested by Gerster



and Scull  (6) was to vent the bottom section through



a valve.  Clearly, if the rate of air flow through



the  partly-opened valve is considerably larger than



that through the drain line, the buildup of pressure



is under the control of the operator and not at the



mercy of spurious effects due to column drain config-



uration.  In an actual column the vent line would



probably be connected from the bottom section of the



column to the top.



    Considerations of good column design seem also



to favor some sort of variable-venting scheme to



increase the liquid residence-time on a tray.  Cal-



culations  (Appendix VIII.C.5) show that for a com-



pletely-vented tray with 1/8-inch holes and 10%



free area the mean liquid residence time is around



0.6 second.  Liquid flow period lengths of this or-



der are too small to be of much commercial interest,



so it is desirable to find some means to increase the



liquid holdup at a given liquid flow rate.  This can



be accomplished by reducing the fractional perforated



area, but a reduction in free area will also increase



the pressure droo of the gas during the VFP.  One



solution to this problem is to allow the pressure-



difference in the gas phase to oppose the drainage



of liquid through the holes; moreover, it may be

-------
                        -36-
     possible to control tray liquid holdups throughout



     the column by manipulation of the venting valve in



     the bottom section.



         Another problem with vented cyclic operation is



     that to obtain a ratio of molal gas flow rate to molal



     liquid flow rate of order unity, the gas flow period



     must be twenty to fifty times as long as the liquid



     flow period.  With such large "£/^ ratios, it is



     feared that weepage of liquid during the vapor flow



     neriod would become prohibitive.  This problem would



     be made much less serious by partial venting to de-



     crease the allowable LFP liquid rate.




B.  Liquid Mixing.



     Although no in-rig experiments on axial liquid mix-



ing have been conducted, the probes, bridge circuits,



and recorder have been tested by performing a simple..



stirred-tank residence-time study and observing the decay



of solution conductivity with time.  The value of mean



residence-time determined from the recorded exponential



curve was found to be in excellent agreement with that



calculated from the known flowrate and tank volume.



     Another experiment was conducted to assess the effect



of noise due to bubbles in the liquid phase upon the meas-



ured voltage signal.  It was found that severe.high fre-



cruency fluctuations in voltage signal made measurements



quite difficult, so that filtering of the response was



considered necessary  for accurate measurements.  Accord-



ingly, a filter box was constructed, containing two iden-

-------
                        -37-
tical 2nd-order, low-pass, operational amplifier circuits




designed to attenuate the noise frequencies by a factor



of 100 with no appreciable influence upon the form of the



measurement signals.  It was found that this arrangement



successfully eliminated bubble-noise, but that the time-



average electrical conductivity of the aerated liquid was



lower than that for clear liquid having the same salt con-



centration.



     This dependence of solution conductivity upon degree



of aeration of the liquid phase is unfortunate in that it



necessitates careful calibration of the probes under the



same hydraulic conditions to be used in a particular run.



The voltage signals corresponding to the maximum and mini-



mum salt concentrations in the aerated licruid must be known



accurately in order to normalize the response signals



properly.  On the other hand, the measurement of depar-



tures from non-aerated behavior gives an estimate of void-



age fractions which are difficult to measure accurately



by comparing froth height with clear liquid height.






C.  Mathematical Simulation Models:



     1-  Hydraulics.



         In order to facilitate the correlation of data



     for liquid flow with an opposing gas-phase pressure



     difference and non-negligible surface tension effects



     a semi-empirical flow model has been developed.  Pre-



     vious investigators have suggested that the behavior



     of a particular perforation on a sieve plate is deter-

-------
                  -38-






rained by the instantaneous net pressure difference



across it, and that fluctuations in gas-phase pres-



sures and liquid heads may result in bubbling of gas,



draining of liquid, or bridging at any instant of



time and any location.   Prince and Chan (15) attempt-



ed to cast this quantitative picture into a very



simple mathematical representation, which assumed



that superimposed upon the mean pressure difference



was a small fluctuating pressure having the value



+ Afy at holes which were bubbling gas and - A.Pp at



holes which were draining liquid.  The possibility



of bridging with no flow of either phase was neglect-



ed.  The fraction of holes bubbling was then select-



ed to minimize the pressure-fluctuation,^^.



    The principal shortcoming in this approach was



that it failed to include any information on the



physical processes causing the fluctuation.  As a



result, it is found that an additional equation



must be supplied in order to predict gas and liquid



flow rates from the mean pressure difference.  Also,



since bridging of holes is commonly observed in the



case of trays with perforation-diameters of 1/4-inch



or smaller, the neglect of this effect could intro-



duce serious errors.



    These difficulties can be overcome by substitu-



ting for the minimization-of-pressure-fluctuation



condition, the physically realistic assumption that



pressure-fluctuation amplitudes are random quantities

-------
                   -39-






having some distribution of values about a zero mean.



If the spread of the distribution is sufficiently



large, it is possible to have finite probabilities



for each 6f the three possible states.   From momen-



tum-balances for gas and liquid flow, one may deduce



"expectation values" for the flowrates  if the param-



eters of the distribution are known, or, for a given



distribution shape, the parameters of the distribu-



tion may be deduced from data.  The details of .the



model equations and their use are discussed in Appen-



dix VIII.B.



    Thus far it has been virtually impossible to use



the model for data interpretation, not  because of any



inherent shortcoming in the mathematical representa-



tion, but because the data obtained from the single



tray insert used have not been sufficiently conclusive



to permit evaluation of all necessary input quantities



As mentioned in the discussion of hydraulic results,



the actual discharge relationship has been obscured



by surface-tension effects at the low-flowrate end



and by air entrainment at all flowrates.  For inter-



pretation of the variable-venting results, the depen-



dence of air entrainment rate upon both liquid flow-



rate and clear liquid head must be specified.  For



a single tray insert these two variables are strong-



ly coupled and the individual dependences are prac-



tically impossible to determine unless  the exact form



of the desired correlation is known.

-------
                             -40-
          2.  Mass-transfer Model with Mixing.



              The complete mass-transfer simulation model of



          Gerster and Scull ( 6 ) has been programmed for use



          on an IBM 1130 computer.  The program can handle



          short (less than 6 stages) columns with computation



          times on the order of 30 seconds; conversion for use



          on larger,.faster machines, such as the IBM 371 sys-



          tem, is straightforward and will essentially remove



          all limitations on total core storage and solution



          time.



              The dimensionless differential and algebraic



          equations are summarized in Appendix VIII.C., together



          with some typical simulation results.  The differen-



          tial equations are integrated numerically using a 4-



          th order Runge-Kutta algorithm, and stable cyclic sol-



          utions are obtained by simulating the startup of a



          column from an assumed set of initial conditions until



          the periodicity conditions are satisfied within a cer-



          tain tolerance.  Much of the programming and all of



          the simulation experiments were carried out by Miss



          D. Jarmoluk, a graduate assistant working on the pro-



          ject.



              The program is prepared to generate results, once



          correlations for hydraulic variables and mixing param-



          eters have been developed.



VI.  Direction of Current and Future Work.




     As suggested in the discussion of results, it is anticipated



that repetitions of some of the experimental studies using trays



of different free area fraction will provide the needed infor-

-------
                             -41-
mation on the intrinsic head-vs.-liquid flowrate and air en-



trainment rate vs. liquid flow rate and head relations.  Once



such information is available, the flow model can be brought



into play to assess the relative effects of liquid aeration



and pressure fluctuations upon the liquid heads and pressures



measured in partially-vented steady-state experiments.



     Currently, a series of experiments is being conducted



to measure the quantitative effects of changing flow-period



lengths in vented cyclic operation.  It is hoped that the weep-



age mechanism postulated to explain some of the observed de-



partures from steady-state hydraulics can be made more quanti-



tative, and that other contributing phenomena can be postulated



and verified by examination of the data.



     The electronic circuits developed for the salt-tracer



mixing studies and the associated hardware for two-supply



cyclic operation await their first in-rig test.  It will prob-



ably be found desirable to adjust the rates of air venting



from the various sections, in order to increase the liquid



residence time to around 2 seconds for experimental conven-



ience.  It may be found that tracer experiments also give in-



formation on weepage rates and other hydraulic phenomena which



will be useful in interpreting the previous hydraulic data.



     Once a model for column operation is formulated, it should



be tested by carrying out absorption experiments in a well-



designed cyclic column as suggested in the section on long-



term objectives.  The results of such a study should be helpful



in suggesting alternate design configurations and modes of oper-



ation.

-------
                             -42-






VII.  Summary.




     Hydraulic experiments carried out in a 3-tray cyclic col-



umn, using air and water as the counterflowing phases, have



indicated the form of the gas- and liquid-phase discharge re-



lationships , the importance of air-bubble entrainment in the



liquid phase, and the effect of flow-period lengths in produc-



ing departures from steady-state liquid heads in vented cyclic



operation.  Equipment for measurement of mixing parameters



has been assembled and tested and computer programs and sim-



ulation models have been developed for interpretation of ex-



perimental data and prediction of cyclic column performance.



It remains to complete the cyclic hydraulics and liquid mix-



ing studies, and  to use different tray inserts to finalize



the steady-state hydraulic relationships.

-------
                             -43-



VIII.  Appendix




     A.  Models for Axial Liquid Mixing in Cyclic^ Operation.



          1.  Liquid-phase Mixing from Evolution  of  Vertical



          Concentration-Distance Profile.



              If the mixing in the liquid phase  (excluding the



          falling liquid streams) is assumed  to be described



          by a "dispersion coefficient", then in  analogy with



          Pick's law,



                                                            (A.1-1)
          in normalized coordinates.  The boundary  conditions



          suggested by Danckwcrts apply:




             1 •      c - O  a.£  & " O _>  -£0*- a// J" .
             3.        =  O
          The infinite-series solution  to  this  problem has the



          form,

where,



           •"• / -^  X" ^//.  * ~~9 ~\~ I

                                                    ,.1-4)





             "^~~" ^  ~PC..
                        r
                     - / /fe

-------

/
= 777
      /O
                                     ^ /
                                     /
                                        s^'

                                F/GURE   //

-------
                   -45-
    y  is the n-th eigenvalue solving,
                       -
        art,   <-^-  ~   ?*- /    '          (A. 1-5)


    and       »  ta-KT'      .                    (A. 1-6)
    The predicted  functional  form can  be  fitted,  in


a least-squares sense, to  data on concentration vs.


distance and time, by choice  of  the  Peclet number,


Pe.


2.  Overall Mixing Parameter  from Measurements  of


Well-Mixed VFP Liquid Composition.
Let,       ( ZCeJ-          =    (&  .          (A. 2-1)
           (  ^  -

Then, for cycle fl,
                          \  =

                          J
                                  Ct)  ,           (A. 2-2)
                 —^	~y   J       }  =  /'(/)  .           (A.2-3)
            V %  j?  — x  /



For periodicity,

                                      :  X/o       (A. 2-4)

                    s
                                                  (A. 2-7)
Hence,          fft , _ _^^_                  (A. 2-8)
                      ~

-------
                   -46-
The mixing-model equations are,



                                                      (A.2-9)
                     = O
                                                      (A.2-10)


                                                    /
                            O
 Hence,
                                                      (A. 2-11)

 The solution is,
                                  *
           f°}=  ]  ,   >,  -C-&J   r    /-^/   (A.2-12)
          J         /- ]Te.             Sor --~ < /
                                                      (A.2-13)
from which ^" can be determined if   r > /   °


The case  £*- /-"^  means that the mixing situation


cannot be distinguished from plug flow.

-------
                        -47-
B.  Model for Gas and Liquid_Flows Through a Perforated
Plate.
     It has been suggested that "simultaneous" flows of
gas and liquid through a perforated plate at steady-state
may result from pressure and liquid-head fluctuations
which bias the holes positively or negatively.  Thus, at
any given hole any one of three possible conditions may
exist at any given time :
     1.  Bubbling of gas up through the hole.
     2.  Draining of liquid down through the
         hole .
     3.  Bridging, with no flow of either phase.
     If we may assume for simplicity that the pressure
drop of a continuous medium flowing through a perforation
is a constant multiple of the velocity-head based on the
cross-sectional area of the hole, the following approxi-
mate steady-state momentum balances may be written:
     1.  For the gas phase,
                ,    (AP6 -^ JL} + Aty  >
     2.  For the liquid phase,
     3.  For bridging,
                                                       .   (B-3)

-------
                        -48-

     The basic assumption upon which the flow model
rests can be stated as follows :
     The pressure-fluctuation,^)/^, is a random variable,
in the probabalistic sense, whose density function,
        0~) will be assumed to have the following properties
     1.  A mean of zero.
     2.  An index of deviation from the mean, 0~.
     3.  Symmetry about the mean; i.e.,
     Before proceeding to derive the relationshios for
average gas and liquid f lowrates , it is advantageous to
cast the preceeding momentum balances into a more symmetri-
cal form.  Thus ,
                                                          (B-5)
Now, define,

                                 7~P) + Afy  J           (B.6)

                                       *                   (B-7)

and       =-                                      (B_8)
Clearly, then,
     1.  For gas bubbling,    £ > }
     2.  For liquid draining,    £ <"
     3.  For bridging,  - y £ / ^

                                     '         *-*       (B-9)

-------
                        -49-
     From the basic assumption it is easily shown that the


density function for the "net pressure difference,"  o   ,


has a mean of  a0 , an index of deviation of C~ , and sym-


metry about the new mean.  It may be represented as
     The probability of each of the three types of  flow


behavior may now be calculated.


     1.  Probability of gas bubbling   =  ^3 '/
               r °
               /  /e> Ccf- **  J  (^1-^)^/9(2-2.^ /J  <2 ;       (B-17)



 and,

-------
                        -50-
Now, introduce the new variables,

             = JL - Z0  .
                        "                                  (B-19)
                    >    3-  ~  P — do •
                    -*-"   J
Then,
                  .^
              - J
for gas flow.  For liquid flow,  let


                -  3 -  7
              ~"    Xv   xO. x)
                   ,*>-  7                                   (B-21)
             =  —  f —  A. £>    *


whence it can be shown that
                                                           (fi-22)

If we let,

                                        '                   (B-23)
                                                           (B-24)
      \U&/  =  T (. F ~ xC0y j
                   u
and,

                                                           (B-25)
One point of hydraulic data consists  of  experimental val-

ues for the quantities ,
Since we have two relations to  determine <3~ ,  the "spread"

of the pressure fluctuation, we may  select a 
-------
                        -51-




Since S0 is a difficult quantity to measure experimentally,


however,  the recommended procedure is to solve the two equa-


tions exactly for  O~ and  o0 , knowing  \ && / and  \t4^/-


The agreement of measured and calculated oa-values consti-


tutes a test of the predictive power of the model  (using


the chosen density-function) while 0~is a single empirical


parameter which can be correlated.


     The "flowrate correlation" is completely specified


by,


     1.  A probability density function, i& .


     2.  An empirical correlation for  O~, the deviation


     from the mean pressure-difference.




C.   Mathematical Model for Mass-Transfer and Liquid Mixing


in a Cyclic Absorber.


     The mathematical model equations originally suggested


by McWhirter and Lloyd (14) and modified by Gerster and


Scull  (6) to account for the effects of axial liquid mix-


ing are summarized for a general stage as follows:


     1.  Gas Flow Period.


         Assuming constant and equal liquid holdups, H,


     and equal Murphree point efficiencies, -M , on  all


     stages; a constant molal gas flowrate, G* ; and a. di-


     lute gas phase with Henry's law constant, m;  an un-


     steady state component material balance on the i-th


     stage  (see Figure 10) gives,



                   -  J^/Vz/.  - */ • ~)
                      //  r«-'     ^                     (c-i)

-------
                   -52-

The composition of the gas stream leaving the stage
is related to the composition of the gas stream enter-
ing the stage and to the tray liquid composition by
the Murphree efficiency,
                           -/                        (C-2)
           *,=
           7    x, x; -  *ss-s    '
2.  Plug-Flow Conditions .
    If during the liquid flow period a fraction 
-------
                    -53-




a nd an overall balance on the entire tray holdup


gives for the average tray liquid composition,
                                                     (C-5)
The composition of liauid leaving the plug-flow


section at any time is,
                    ,   X+ <"?& J     ^  ^ •
where           ,   _  (/- irj ^
A.  =
                               ^.
4.  Periodicity^ Conditions.


    Compositions at the end of the LFP are related


to initial VFP compositions by,



              %*o  ~  X+ C ^1 )  .                    (C-7)


5 .  Average Exit-Gas Composition.


    In order to calculate the number of theoretical


stages to accomplish the given separation, it is


necessary to compute the average exit-gas composition.


    For the plug-flow case, an overall solute mater-


ial balance for all flows during one cycle gives,
                                                     (C-9)

-------
                    -54-



and k and 1 are previously-defined integers,


    For the generalized mixing model case,
where, -^ C7!) is defined by,
                                                    (C-ll)
6.  Overall Column Efficiency.


    Colburn ' s analytical solution for the number of


theoretical plates required to accomplish a given


separation is,                                      (C-12)
    The overall efficiency of the cyclic column is,

then,

                   =
7.  Dimensionless Form.


    The foregoing equations may be cast into dimen


sionless form by means of the following transforma


tions :
    /<
    0 =
          /  £•/  &  s



                                                    (C-15)

-------
                    -55-
For gas flow:
           -*1 -
           J



           >'



For plug flow:
                 =/
                       &r  -
For generalized mixing
                                            >•   -
                                                   /  .
                                                      (C-17)
                                                      (018)

-------
                  -56-



For average exit gas composition

    in plug flow,
where,
or, for generalized mixing,                         (C-19)
where               -                               (c"20)
with
              >


For overall column efficiency
and
                                                     (C-22)

The overall column efficiency,
is a function of 5 dimensionless parameters. It has

become customary to illustrate this relationship for

plug-flow by plotting  £0 as a function of  & , yield-

ing a curve with cusp-like maxima at the first N posi-

tive integral values of y .  Such a plot is shown

in Figure 12 , for  /^= O .  For values of the mix-

ing parameter f> O , the solution curves break off

-------
                          -57-
^oo
/90\-
/80 - ~
                          -n~ /.o
                          A * /.O

-------
.OOO/

-------
                        -59-


     from the plug-flow solution at fi = f/ — fj and show

     flatter and less well-defined maxima at lower values

     of overall efficiency.

         Colburn's equation is normally plotted as log

     normalized 'exit-gas composition vs. log( 1+ number

     of theoretical trays)  , with absorption factor as a

     parameter.  A similar plot for the cyclic case illus

     trates the improvement in separation.  (Figure 13.)

D.  Sample Calculations .

     1.  Comparison of Experimental Slope of Liquid-Head

     vs. Flow Rate with Hagen-Poiseuille Law:
              _
              Q  =

     D - 1/8 inch = 1/96 ft.

     L = 1/4 inch = 1/48 ft.

     AH = Ah (inches) /12 ft.

     pL- 62.4 lbs/ft.2

     g = 32.2 ft/sec2

     ^L= 6.72 x 10~4 lb/(ft.sec)

     Q = q  (gallons/min.) x 2.228 x 10~3  ft3/sec


     Therefore ,
                                                      0}



                   ^       '        0   
-------
                    -60-




2.  Calculation of Flowrate for Critical Weber Number
    ThUS'
    NOW,
    N = 230 holes


    D = 1/96 ft.


    g = 32.2 ft/sec2


    0~= .00495 Ib/ft,


    jO± =62.4 Ib/ft3




So that,  C
          Scr/'t  -  I*. 3J-&  tSe cw£


The reported value of  >4^ cr/£ =  ^.8   ; hence,
                         
-------
                   -61-
                        /            2-                (D.3-5)
or, a 33% increase in pressure drop over  that  for

clear licruid.

4.  Initial Rate of Pressure Rise Due  to  Air Flow

Into a Sealed Column Section.

Assuming isothermal pressure increase,
                                                      (D.4-1)


                                      '      .          (D.4-2)



If the gas enters at the same conditions,


                                                      (D.4-3)


                               2.  )                    (D.4-4)
For a given small ^/^
P  = 1 atm. = 407.0 inches of H->O
AP = 1 inch of H20
V0 = 5500 cm3
vin =200 cm3/sec.
           /     /   /
     .'.   A -6  =  (  yoj-(  200

Initial  pressure  increase  is  1  inch  of 1^0 in .068

sec.

5.   Estimate  of Liquid  Residence-Time  and Ratio of

-------
                    -62-
Flow-Period Lengths .

    a.  The residence-time of liquid on a tray may

    be estimated from the measured values of  liquid

    flow rate and clear liquid height as follows :

                                   A 7-rcy  .         (D . 5-1 )


                                       ^               (D.5-2)
                              s
    Test case: AH » 1 inch H20 = 1/12 ft H,0
               Qlia " 13 9Pm - .0290 ft3/sec
               ATray " 0.196 ft2
    b.  To estimate the order of magnitude of  the

    '7G/'?2.   ratio for vented cyclic operation, we

    make the following assumptions:

        (1) Dry-plate pressure drop ^clear  liquid

        head ^liquid velocity head.

            .-.  f& U& * ~ ^ ^.^  .            (D.5-3)

        (2) Ratio of average molal gas  and liquid

        flowrates of unity.

                           /"        X^L £>£*  *^2j
                                    /    ^  	 -   (D.5-4)
        From which,


                   ~-  ^ ^~ (^  ^)          (D'5-5)

        But,                             ''
                                                      (D.5-6)



                                                      (D.5-7)
        With   „        i i_/,t_   ,
                    29  Ib/lb-mole
               ML * 18  Ib/lb-mole
               PL - 62.4  lb/ft3
               PG « .075  Ib/ft3
                 -72

-------
                          -63-
E.  Nomenclature:

    1.  Appendix:  A.I.

        A  = n-th coefficient term of series expansion, Eqn.
         *"  (A.1-3)

        C  = tracer concentration normalized on [0,1].

        n,  - subscript for terms in infinite-series solution

        Pe = Peclet number

        4^ = n-th eigenvalue, solution of Eqn. (.1-5)

        $Z>  = phase angle for n-th eigenvalue, defined by
             Eqn.  (A.1-6)

        0  - dimensionsless time variable

       J>  = dimensionless length variable

    2.  Appendix:

        R = reduced concentration ratio, defined by Eqn.  (A.2-7)

        % - average tracer concentration at any time

        Z/f - tracer concentration in LFP#1 feed.

        ytif = tracer concentration in LFP#2 feed.

        •%j0 = tracer concentration at start of LFP#1

        Kza = tracer concentration at start of LFP#2

        ft"'= well-mixed fraction

        & = fractional tray holdup dropped per cycle

        & = dimensionless time

          = reduced average tracer concentration

          f = reduced tracer concentration in well-mixed cell.

         p - reduced tracer concentration in stream leaving
             plug-flow section.

-------
                   -64-
3.   Appendix:   B.

    C/g = gas-phase discharge-loss coefficient

    C^ = liquid-phase discharge-loss coefficient

    h  = clear liquid head on tray

   A Pj = randomly-distributed pressure-fluctuation

   APg = gas-phase pressure difference across tray

   •A Ps = oressure difference due to surface-tension
           required to form a drop or bubble.

    T p = tray thickness

    U^ = instantaneous gas velocity through hole

    U^ = instantaneous liquid velocity through hole

         = average gas velocity through holes

         = average liquid velocity through holes

       y   = reduced average gas velocity

           = reduced average liquid velocity

      = dimensionless dummy intearation variable,
         defined by Eq'n (B-19) and Eq'n (B-21)

     / = probability that a hole will bubble gas

     £ = probability that a hole will drain liquid

       = probability that a hole will bridge

      = modified surface-tension term, defined by
         Eq'n (B-8) .

     = modified randomly-distributed net pressure
         difference defined by Eq'n. (B-6) .

       = modified  average net pressure-difference,
          defined  by eq'n (B-7)

    ^ = reduced  net randomly-distributed pressure-
         difference

    A0 = reduced average net pressure difference

       = gas density

       = liquid  density
    CT=  index of deviation  of random fluctuating
         pressure from the  mean

-------
p
               -65-
= integration limit defined by  Eq ' n  (B-19)  and
   Eq'n  (B-21)

  = reduced surface-tension term
Appendix: C.

A = absorption  factor  defined  by  Eq'n  (C-   )

E0 = overall column efficiency

G = average molal  gas  flowrate for  entire  cycle

G  = actual molal  gas  flowrate during  the  VFP

H = molal tray  liquid  holdup

k = lower-bounding integer  for

1 = upner-bounding integer  for

*• = average molal  liquid  flow  rate  for entire
     cycle

m = Henry's law constant  in mole -fraction  units

N = number of stages in cyclic colujn

NC = number of  theoretical  stages in a conventional
      column for same  separation.

t = time variable

t/e= residence-time in plug-flow  section

,2£g = average bottom liquid  composition variable

-2%c = average tray  composition  in  LFP on stage i

•^fc = tray liquid composition in VFP on stage  i

s£*'o-= initial VFP  liquid  composition on stage i
  /5**= composition of well-stirred  cell  in  LFP on
       stage i

 2^/5^= composition of liquid  stream from plug-flow
       section in LFP on stage  i

%.-r= entering liquid composition

&k = gas composition in entering stream

3f^ = gas composition in stream  leaving  stage  i

& o
-------
                   -66-
      = fraction of tray holdup assumed well-mixed
         in LFP

      = fraction of a tray holdup dropped per cycle

     "^ =VFP length

     1 = LFP length

     '  = reduced time variable

     .= reduced bottom liquid-composition variable

    j^j = reduced VFP tray liquid composition on stage i

     j= reduced LFP average liquid composition on
          stage i

    ff/^ = reduced LFP well-mixed liquid composition
   ^        on stage i

      ^^ = reduced composition on liquid from plug-
            flow section during LFP on stage i

       = reduced entering liquid composition

    & & = reduced gas compos: tion in entering stream

    c^  = reduced gas composition in stream leaving
   <-/      stage i

    a"0(jf-  - reduced average exit-gas composition
              variable.
    ^1 = Murphree point vapor efficiency


5.   Appendix:  D.I.

    D = hole diameter

    g = gravitational acceleration

    Ah = clear liquid head, in. of 1^0

    
-------
                   -67-



    Appendix:   D.2.

    D = hole diameter

    g = gravitational acceleration

    N = number of perforations

        /£= critical liquid rate for drop to jet
             transition, gallons/min.

          = critical liquid rate, ft-Vsec.

          = critical liquid velocity

      er/'A = critical Weber number

       = liquid density

    O~' = air-water surface tension

    Appendix:   D.3.

       /r = flowrate of air through perforations by
            entrainment in the liquid phase.

      s^o^ liquid flow rate

       = velocity of aerated liquid through holes

      .= velocity of clear liquid through holes

      = volume fraction of gas in gas-liquid mixture

       = density of aerated liquid

         = density of gas phase

       = density of clear liquid


8.   Appendix:   D.4.

    n = number of moles of gas in closed volume

    P = absolute pressure of gas in closed volume

    P 0 = initial absolute gas pressure

    AP  = small pressure increment

    R = ideal-gas law constant

    t = time-variable

-------
                    -68-


   -At = small time -increment
      't* = rate of gas inflow
       =5 volume of gas space
    Appendix:  D.5.
  ^Tray = column cross-sectional area
   A H = clear liquid head
     ' G - molecular weight of gas
       = molecular weight of liquid
       .  = licruid flow rate
       ^
       = gas velocity through holes
       =liquid velocity through holes
       = density of gas
       = density of liquid
    <% = gas flow period length
    ?Z = liquid flow period length
    ^e. = approximate mean liquid residence time
10.   Special Abbreviations:
    VFP - vapor (gas) flow period
    LFP - liquid flow period.
&

-------
                        -69-
 F.   Literature  Cited.
 (1)   Cannon,  M.  R. ,  "A New Type of Distillation,
      Absorption  and  Extraction Column," Oil Gas J.,
      51_,  268  (1952).

 (2)   Cannon,  M.  R.,  "Here's a New Liquid Extractor,"
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 (3)   Chien, H. H., J.  T.  Sommerfeld, V. N. Schrodt,  and
      P. E.  Parisot,  "Study of Controlled Cyclic Distilla-
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      (1966)

 (4)   Garcia,  A., and A. R. Bayne, "Gas Flow Through Sub-
      merged Orifices," S.  B.  Thesis, Massachusetts Insti-
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 (5)   Gaska, R. A., and M.  R.  Cannon, "Controlled Cycling
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 (6)   Gerster, J. A.,  and H. M. Scull, "Performance of Tray
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 (7)   Holland, C. D. ,  "Multicomponent Distillation,"
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 (8)   Horn,  F. J. M.,  "Periodic Countercurrent Processes,"
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 (9)   Lewis, W. K., Jr., "Rectification of Binary Mixtures,"
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(10)   Lin, R.  C., "Periodic Processes in Chemical Engineer-
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(11)   McAllister, R.  A., P. H. McGinnis, and C. A. Plank,
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(12)   McKay, D. L., and H.  W.  Goard, "Crystal Purification
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(13)   McWhirter,  J. R., and M. R. Cannon, "Controlled
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-------
                        -70-
      Eng.  Progr.,  59,  58  (1963).

(15)   Prince,  R.  G.  H.,  and B.  K.  C.  Chan,  "The Seal
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(16)   Robertson,  D. C.,  and A.  J.  Engel, "Particle Separation
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(17)   Robinson, R.G.,  and  A. J. Engel, "An Analysis of
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           4
(18)   Schrodt, V. N.,  J. T. Sommerfeld, 0.  R. Martin,
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(19)   Sommerfeld, J. T., V. N.  Schrodt, P.  E. Parisot, and
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(20)   Tan,  K.  S., "A Study of the Dynamics of Cyclic
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-------