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Modeling, simulation and control of liquid-liquid extraction columns

Article  in  Chemical Engineering Science · January 1998

DOI: 10.1016/S0009-2509(97)00310-2

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 Pergamon Chemical Engineering Science, Vol. 53, No. 2, pp. 325-339, 1998
~c~,1997 Elsevier Science Ltd. All rights reserved
Printed in Great Britain
PII: S0009-2509(97)00310-2 ooo9 2509/98 $19.00 + o.oo

Modeling, simulation and control of

liquid-liquid extraction columns
O. Weinstein, R. Semiat and D. R. Lewin*
Department of Chemical Engineering, Technion I.I.T., Haifa 32000, Israel

(First received 21 May 1997; accepted 12 June 1997)

Abstract A model describing the hydrodynamics and mass transfer of countercurrent liquid-
liquid extraction columns is developed and solved. The hydrodynamic model assumes that the
dispersed-phase drops behave as spheres of uniform diameter. The model has been found to be
qualitatively in agreement with experimental results published in the literature. It is shown that
conventional dispersion interface level control using the continuous-phase effluent flow rate as
the manipulated variable causes unavoidable overshoots and oscillations in the mean holdup
and outlet concentrations, while an alternative scheme using the continuous-phase feed flow
rate leads to a significant improvement in the dynamic response. A model-based decentralized
M I M O control scheme is designed and tested by simulation, and is shown to provide excellent
servo and regulatory performance. © 1997 Elsevier Science Ltd

Keywords: Liquid-liquid extraction column; mathematical models; dynamic simulation and

control.

l. INTRODUCTION coalescence models, on which the approach relies,

Solvent extraction in continuous columns is one of the
most important separation processes in chemical en-
gineering. However, the control of these units can
often be problematic, partially due to their multiphase
nature, and partially due to the difficulty of on-line
measurement of output variables. Thus, the reliable
simulation of the transient behavior of these columns
is extremely valuable. A review of the progress on the
dynamic modeling and simulation of extraction col-
umns was published by Steiner and Hartland (1983).
Most previous studies have dealt with mass-transfer
transients while assuming hydrodynamic steady state.
In contrast, the detailed experimental results pub-
lished by Hufnagl et al. (1991) imply that the dynamic
response of outlets, holdup and concentrations are
determined largely by the dynamic behavior of disper-
sed phase.
Recently, several papers (e.g. Casamatta and Von-
derpohl, 1985; Dimitrova A1 Khani et al., 1989; Tsoris
et al., 1994) have developed models relying on a drop
population. These models have the potential of ex-
plaining the nonuniformity of holdup profiles along
the contactor, and thus they allow a more realistic
description of flooding conditions. On the other hand,
this approach leads to complicated mathematical
formulations. Aside from this, drop breakage and
*Corresponding author. E-mail: dlewin@techunix.tech-
nion.ac.il.
325
have not yet been developed for all types of columns.
Perhaps for these reasons, this approach has not been
used for control purposes. For example, the holdup
overshoot and oscillations in response to input dis-
turbances shown analytically by Brownstein and
Schegolev (1988), and demonstrated experimentally
by Hufnagl et al. (1991), is an important characteristic
of extraction column dynamical behavior. Neverthe-
less, this phenomenon has not been studied in the
works dealing with drop population models.
This paper will show that important aspects of
extraction-column dynamics may be investigated with
sufficient accuracy using a simpler approach, based on
a hydrodynamic model relying on the Sauter mean
diameter, which is an accepted measure of the average
diameter of a dispersed-phase drop. This has been
widely used in relationships for parameters of extrac-
tion processes and for the estimation of flooding con-
ditions (Bair and Lane, 1973; Baird and Shen, 1984).
The model assumes a uniform drop diameter and
thus, the number of equations that need to be solved is
much smaller than that for drop population models.
The model for mass-transfer developed accounts for
changes in the continuous and dispersed flow rates
caused by the holdup profile transient. The model
is intended to be used for control purposes, and is
used to simulate conditions both for a Karr column
(Karr et al., 1987), in which the dispersion layer
is supported on a stack of perforated, vibrating plates,
and for a Kuhni column, in which it is supported on
rotating plates (Hufnagl et al., 1991). The novel
326 O. Weinstein et al.
dispersion-level control scheme suggested by Hufnagl liquid-liquid extraction equipment is discussed by
et al. (1991) is simulated using the proposed model, Godfrey and Slater (1991). The relationships for
and compared to the conventional control commonly Vs and other parameters used in the model are dis-
adopted. Finally, a multivariable controller for a Karr cussed below.
column is developed, relying on a linear model ap- Since the cross-sectional area is constant, it is pos-
proximating the dynamics of the column. This is sible to introduce new variables Ue = Qe/S, Uc =
tested by simulation on the detailed nonlinear model Qjs, Ue.in = Qe.~./S, Uc.,n = 9_c.,#S, Ue .... = Qe.out/S
developed in this study. and U.... t = Q .... t/S. Thus, eqs (1) to (3) can be
rewritten as
2. M A T H E M A T I C A L MODELING
Oe(h)
Ua(h) = e(h) Ve(h) - De(h) - - (5)
2.1. Assumptions Oh
The mathematical model for a liquid-liquid extrac-
U c - - U d = U c , in - Ud,ou t = U .... t -- U d . in = A U
tion column relies on the following main assumptions:
(6)
(1) The radial variations of the mean velocity and
U~
the concentrations of each phase are negligible.
Vc = 1 - e" (7)
(2) The phase volume flow rates are independent of
mass-transfer and solute concentration. A balance of dispersed phase in an elementary volume
(3) The dispersed-phase drops behave as spheres of of the column leads to the following dynamic equa-
a uniform diameter. tion:
(4) The model describes the processes occurring in
the dispersion layer of an extraction column. O~_ dUe_ O(Va~) O/ &\
The length of this dispersion layer is fixed.
(8)

2.2. Modeling of fluid dynamics Substituting eq. (5) in eq. (6) gives
Since the dispersed phase is assumed to consist of O~
spherical drops of uniform diameter, the mean drop U,. = AU + Ua = AU + e V e - De ~ (9)
size in a dispersion is expressed as the Sauter mean
diameter: d32 = Z n f l ~ / Z n i d 2 where di is the indi- and by using eqs (4), (7) and (9), Ve is obtained as:
vidual drop diameter and n~ is the number of drops
with this diameter.
Va = (1 - e)V,(e) - AU + De -~. (10)
The direction of movement of the dispersed phase
coincides with the positive vertical direction. The flow
rate of the dispersed phase, Qa, through the cross- The boundary conditions are
section S is expressed by: &
h=0; Ua, i n = r ~ V a - D e ~ (11)
0~(h)
Qe(h) = St(h)Ve(h) - SDa(h) - - (1)
Oh Oe
h=l; T~=0. (12)
where De(h) is dispersion coefficient, Vd(h) is velocity
of dispersed phase, e(h) is the volume fraction holdup
These boundary conditions arise from material
of dispersed phase at the height h of the dispersion
balances across the system's boundary planes, with
layer in the column. The flow rate of continuous
the assumption that the column is a "closed system",
phase, Q~, can be obtained by assuming incompress-
i.e. dispersion occurs only between h = 0 + and
ible flow in the material balance between cross-
h = l - . The significance of these conditions is dis-
sections h = 0 and h = h
cussed by Wehner and Willem (1956). Miyauchi and
Q c - - Q~d = Q c , in - - Q a , o u t = Qc,out -- Qa.i, = AQ (2) Vermeulen (1963) applied similar boundary condi-
tions in their steady-state solutions of an axial disper-
where Q~,in and Qa, in are continuous- and dispersed- sion model.
phase feed flow rates, Q.... t and Qa, o,t are continuous The outlet flow, Ue,out, is expressed by
and dispersed phase effluent flow rates, and Vc is the
velocity of the continuous phase:
h=l, Ue,o~t=eVe=e(V~- V~)=~ V~- 1-~]"
Qc
V~ S(1 - e)' (3) (13t
For Vn and V~ the relationship The variation of the input parameter U~,i~ will cause
an immediate change to the flow of the continuous
ve + v~ = v~(~) (4)
phase on the whole column height. This follows from
is valid. An appropriate expression relating the slip physical properties of the system. The variation of the
velocity, V~, and the dispersed phase holdup, E, in input parameter Ud, i. induces the flow change that
 Liquidqiquid extraction columns 327
spreads with limited velocity, so that U .... t is obtained tions. The column is considered as a series of
from material balance: n perfectly mixed stages with countercurrent flows.
Subscripts 0 and n + 1 refer to the disengagement
g .... t = Uc, in "~ Ud, in - - Ud. out" (14) sections h = 0 and h = l, respectively, as shown in
Fig. 1. In order to simplify matters, it has been
2.3. Modelin9 of mass transfer assumed that the axial dispersion coefficients are inde-
The following flow rates of solute passes through pendent of height.
the cross-section S of the column:
3.1. Holdup dynamics
for the continuous phase:
Applying eq. (8) to an interior point i using a finite
8[(I - e)Y] difference approximation gives
Qy = S V c Y (1 - `g) + SDc (15)
Oh
~'`gi Ere,V e i l -- [F,V d ] i - 1 el-1 - 2`gi + ei+ l
-- + De
for the dispersed phase: & Ah Ah 2
(22)
a[ex]
Qx = SVdX`g + SDa O~ (16) The boundary conditions (11) and (12) in discretized
form are
where Y = Y(h) and X = X(h) are the concentrations el - ,go
in the continuous phase and in the dispersed phase, `g,+x - e, = 0; Uda. = [eVd]o--Dd A--'--~ (23)
respectively. The mass transfer in an arbitrary volume
element of column can be expressed as
[ V J i : [-(1 - e)Vs(`g)]i - AU + Dd `gi+l - `gl (24)
Ah
S A h a K x (X* - X)
or Substituting the discretized boundary conditions (23) at
S A h a K y ( Y - Y*) (17) i = 0 into eq. (22) for i = 1 gives

where X * is the solute concentration in equilibrium 0el ( (e2- 81)Ua.m)~ (25)

0t-= [eVe]x-De A ~
with Y and Y* is the solute concentration in equilib-
rium with X. The interfacial area per unit volume, a, is The equation for section i = n accounts for the bound-
calculated by a = 6e/d32 , where d32 is the Sauter ary condition at i = n + 1:
mean diameter. Using eqs (15~(17), a mass balance
for the continuous and dispersed phase around an 0`g. [eVa]. - [eVa].- ~ `g.- ~ - `g.
(;t Ah t- De Ah 2 (26)
arbitrary volume element of column in the interval
0 < h < l leads to the following differential equations:

Ud,out U c, in
+ aKx(X* - X) (18)
n+l
OE(1 - `g)r] O

I
at Oh [V=(1 - `g)Y] n

O/ O[(1 n-I
+~tD< ~E)Y])-aKx(X*-X) (19)
. . . . . . ...........
Z ..........
with boundary conditions D ispersion
laver
O(ex)
h = O, X i n U d , in = `gVaX - De - -
Oh

O[(1 -`g)Y]
-0 (20)
Oh

8[(1 -e)Y]
h=l, YinUc,in = (1 - e)V~Y + D~
Oh '

O[ex]
- - = 0. (21)
Oh
Ud, in I IUc,out
3. SOLUTION OF THE DYNAMIC EQUATIONS
The dynamic equations derived in Section 2 are
spatially discretized using finite-difference approxima- Fig. l. The discrete grid scheme.
328 O. Weinstein et al.
Finally, eq. (13) in discretized form is expressed by 0[(1 - DY]a [(1 - e) Y V ~ ] z - [(1 -- e) YVc]I
& Ah
gd .... =[~gd],,+a = e V~ 1--e/J,,+1
[ ( i - e) Y ] 2 - - [(1 - e) Y ] t
+ De Ah2 -- N1 (35)
3.2. Mass transfer
Finite-difference approximation of eqs (18) and (19)
8[(1 -- 0 Y-]. (
for an interior grid point i gives c3t Uc, i.gi. - [(1 -- e) YVc].
~[~S]i [eXVd]i -- [~XVd]i_ 1
8t Ah [(1 - E ) Y ] . - [(1 - e ) Y ] . - l ~ l
I

D~ / - -

ah / ah
[eX],_, - 2 1 8 X ] , - [eX],+~
+ Da Ah 2 + Ni -- N . . (36)
(28)
These equations are solved using a Runge-Kutta
3[(1 - e)Y], [(1 - c)YVJi+x - [(1 - ~)YV~]i integrator. The solution method has been implemented
& Ah using MATLAB/SIMULINK. This flexible platform
also allows for the testing of alternative control schemes
D[(1 - e)Y]i+ a - 2[(1 - e)Y]i + [(1 - e)Y]i-1
+ (see Section 6).
Ah 2

-- N i (29) 4. OPEN-LOOPSIMULATIONS
where
4.1. Model parameters
Ni = [aKx(X* - X ) ] , = [aKr(Y - Y*)],. (30) The developed model can describe any common type
The boundary conditions (20) and (21) in discretized of liquid-liquid extraction column. The only additional
form are requirements are relationships for parameters such as
the Sauter drop diameter, the slip velocity, axial mixing
DX]o = D x ] I , Ud, oo,Xou, = DXVd]. (31) coefficients and mass-transfer coefficients. In the follow-
ing, calculations of model parameters are based on data
[(1 - e ) Y ] . = [(1 - e ) Y ] . + b
from Hufnagl et al. (1991): the simulations results will
U ..... You, = [(1 - e) YVc]I. (32) therefore be compared to the experimental results which
appear there. The experiments were performed using
The equations for sections i = 1 and i = n must include a Kuhni column: a liquid-liquid extraction column in
the effect of the boundary conditions at i = 0 and which the dispersion layer is supported on rotating
i=n+l: perforated plates. The liquid system was the EFCE-test
system (toluene-acetone-water), for which physical data
8[eX]~ _ ([eXVd]l - Dd [eX]z -- [eX]l is available (Misek et al., 1984). The data for this column
8t \ Ah and physical properties of the employed system are
)1 given in Table. 1.
- Ud,inXi. --~ + N1 (33) The Sauter mean drop diameter is calculated from an
equation of Fisher as reported by Hufnagel et al. (1991)
8 Dx]. [eXVd]. - [ ~ x v A . _ 1
& Ah
da2 = 0.19W~R0"61dR 1 + nzL22 / ~ R (1 + 2.8e).
[~x].-1 - [Ex].
+ Dd Ah 2 + N. (34)
(37)

Table 1. Physical properties and column data for the Kuhni column

Parameter Value Units Description

Pc 998.2 (kg/m 3) Continuous-phase density (water)

Pd 866.7 (kg/m 3) Dispersed-phase density (toluene)
rlc 1.003 x l 0- 3 (kg/(m s)) Continuous-phase viscosity
qd 0.586 X 10- 3 (kg/(m s)) Dispersed-phase viscosity
I 2.52 (m) Column height
dr 0.15 (m) Column diameter
dR 0.085 (m) Rotor diameter
hz 0.07 (m) Section height
(o 0.27 -- Free fractional area of plate
 Liquid-liquid extraction columns 329
The slip velocity, V~, is given by the empirical equation Mass-transfer outside the drops is determined using
of Kumar (1986) the film coefficient equation of Heertjes et al. (1954)

V, = 1.18 x 10 - 3 q00"g (38) k~ = 0.83 ~ (43)

~lcdRn2 "

Equation (38) is valid for holdups of less than 0.3. For where Dm.~ is the continuous phase molecular diffus-
higher values, this equation can be extended by a (1 - e) ivity coefficient. Mass-transfer inside the drops is de-
tenn. The dispersion coefficients for the continuous and termined by an equation of Handlos and Baron, as
the dispersed phase are computed using expressions suggested by Blab et al. (1986)
which appear in Bibaud and Treybal (1966)
kd = 0.00375 V.~ r/----L--~. (44)
rl~ + qd
D,. = ~Vchz I - 0.171 + 0.02 dRn(1--
~
e)] (39)
The distribution coefficient, m, which depends on the
I / \4.18 -1 1
effluent solute concentration, is calculated from an
Dd=a2n 1.3x10-~We1'5~( P--d~ ~ Re°6~ I . empirical expression presented by Misek et al. (1984):
k,G -- Pay d 3
In(m) = ~ bi(XAc- Xp) i (45)
(40) i: o

The interfacial tension can be computed as a function where xp = 0.6367, bo = - 5.0, b~ = - 2.711, be =
of the acetone concentration, XA¢ (mass fraction), - 9.356 and b3 = - 7.225.
using an empirical correlation presented by Misek A grid size of n = 30 has been used in the simula-
et al. (1984) tions.

10-3 2
4.2. Simulation results
O" m
1 + 5XA~ ~ ai(XA~ --Xp) i+l (41)
i=1 Figure 2 shows the simulated column dynamics
resulting from an increase of 40% in the dispersed-
with xp = 0.6367, al = 135.405, a2 = 79.72012. phase inlet flow. In the plots, the dispersed-phase
The overall mass-transfer coefficients Kx and variables, y(t), have been normalized with respect to
Ky are calculated from the phase mass-transfer coeffi- their initial values: Kv = (y(t) - y(O))/y(O). Other sym-
cients k~ and kd, and the distribution coefficient, m: bols in the plot are Vca, the continuous-phase effluent
flow rate; ed, the dispersed-phase mean holdup; and
1 1 1 1 m 1 (42) d32, the Sauter mean drop diameter. The simulations
KG=k~ +~ and KG=k~ +~" are based on the assumption of fixed interface level

I
w 0.1
~3
0.2

/..'"
/~'" ~

-.......
Ccl
Cc2

d0 ~....=~ r." - - -

......
Cc3

Cc4
I
-0.l I i I I i / i i
500 1000 1500 2000 2500 3000 3500 4000 4500 5000
t [sl

0.8 / , ,
/ A
g o.6
"~ 1 _ / \ C r~ Holdup
.o 04. '~" ".. _ ~ ~ v

-n ,21 , "~." . . . . . . ,
v'-0 500 1000 1500 2000 2500 3000 3500 4000 4500 5000
t lS]

Fig. 2. Simulated transient behavior in response to a step change of 40% in dispersed-phase feed flow rate.
The initial values of the input variables at steady state just before the onset of the disturbance are
Ud = Uc = 0.0024 m3/m z s, f = 2.9 l/s, y~, = 1 1 kmol/m 3 (Kuhni column). Co,, Col, Cc2, Cc3 and Cc4
represent concentrations in positions l, 6, 12, 18 and 24, for n = 30.
330 O. Weinstein et al.
between the two liquid phases in the upper separation
chamber (i.e. perfect level control). This explains the
slight difference between the simulated and experi-
mental behavior of the continuous-phase effluent
flow. The concentrations are presented as perturba-
tions from the initial concentrations just before the
onset of the disturbance. The simulated concentra-
tions in Sections 1, 6, 12, 18 and 24 for n = 30 (see
Fig. 1.) are denoted as Co,, C~1, Cc2, Cc3 and C~4,
respectively. These positions approximately corres-
pond to the locations of the concentration measure-
ment detectors in the experimental system of Hufnagl
et al. (1991). The simulated continuous-phase effluent
concentration value (Cc, in Fig. 2), is related to the
bottom cross-section of the dispersed layer, not to the
bottom settler outlet pipe as in the experiments. Thus,
the simulation does not account for the dispersion
and time delay associated with the column settler. The
simulation results compare well with the experimental
transient values in response to a step of 40% in the
dispersed-phase inlet flow, as shown in Fig. 3.
In order to explain the resonance observed in the
mean holdup in both the experimental and simulated
transients, additional simulation results showing
holdup profiles at various times are shown in Fig. 4.
At the onset of the disturbance, the continuous-phase
outlet flow increases as a result of the displacement of
the continuous phase by the dispersed-phase (segment
OE in Fig, 2). As a result of the propagation of the
local holdup to the top of the column (profiles from
t = 149 276s in Fig. 4), the dispersed-phase outlet
flow rate undergoes an incremental increase from
about t = 250 s. As a result, there is a reduction in the
effluent flow rate of the continuous phase at h/l = 0
due to mass balance (segment F G in Fig. 2). This in
turn causes a reduction in the local holdup in the
bottom cross-section (h/l = 0) due to the relationship
between holdup and the flow rates [eqs (4), (7) and
(10)], which then propagates up the column (see pro-
files t = 392-613 s in Fig. 4). This causes a decrease in
the total holdup (segment AB in Fig. 2). When this
holdup reduction disturbance arrives at the top of the
column, the dispersed phase outlet flow decreases.
Thus, the outlet of the continuous phase at h/l = 0
increases (segment GH in Fig. 2). This causes an
increase in the local holdup in this section (see profiles
t = 716-927 s in Fig. 4) and the described process is
repeated with a lower amplitude (segments BCD and
HIJ in Fig. 2). Thus, we see that the changes in the
flows at h/l = 1 implies changes at h/1 = 0, with
decaying oscillations in holdup. This phenomena has
been demonstrated by Brownstein and Schegolev

0.4

0.3
E cc2
O 1
E 0.2
,x
o (3
0 0.1 - ~ ~'' " X,.r~

"9 O

--O. 1
o looo 2ooo sooo 400o 5000
t Is]
1.O

(?.8

0.6

.9
=~ o . 4

._E 0.2

.~ o

--0.2 Vca
looo 2000 50o0 4oo0 5ooo
t [sJ

Fig. 3. Experimental transient behavior in response to a step change of 40% in dispersed-phase feed flow
rate (Kuhni column data from Hufnagl et al., 1991).
 Liquid liquid extraction columns 331

0.38 w

0.3~ °

0.34 t = 276 s
t=392s . "
~ t= ~ s t = 613s . ~ . . .
0.32
~ 6 S
0.3

~ 0.28

0.26

0.24

0.22

0.2

0.l~
0'.1 0'.2 0:3 0:4 01s 0'.6 017 018 019
Igl [dimensionless]

Fig. 4. Simulated transient behavior of the holdup profiles at various times in response to a step change of
40% in dispersed-phasefeed flow rate. The initial values of the input variables at steady state just before the
onset of the disturbance are as in Fig. 2 (Kuhni column).

(1988) by an analytical solution of a system of equa-
tions describing the holdup dynamics in an extraction
column using the method of small perturbations.
This phenomenon is also observed in response to
disturbances in continuous-phase flows and in rotor
speed. Unfortunately, Hufnagl et al. (1991) did not
report the actual values they used for parameters such
as continuous- and dispersed-phase feed flow rates
and rotor speed. Thus, the experimental and
simulated results can only be compared qualitatively.
Nevertheless, the model appears to accurately predict
the main experimentally observed phenomena.
5. IMPROVING DISPERSION INTERFACE
LEVEL CONTROL
The control of the dispersion interface level is
crucial for the reliable operation of liquid-liquid ex-
traction columns. If this level is not adequately stabil-
ized, the dispersion layer could entrain out of
the column, leading to loss of solvent and product.
The resonance effects observed in the open-loop
simulations are detrimental to good dispersion inter-
face level control. Hufnagl et al. (1991) have
suggested a novel method to solve this problem by
manipulating the continuous-phase feed flow rather
than the effluent flow, which is the industrially accep-
ted practice. In this scheme, the continuous-phase
effluent flow is left free to control the throughput.
Applying these conditions to the model gives new
relationships for the dispersed-phase effluent flow rate
and the continuous- phase feed flow rate. Thus, the
continuous-phase feed flow rate, Uc,in, is obtained
from material balance
Uc, in = U . . . . t -~- U d , o u t - Ud, in"
From eqs (13) and (46), the effluent flow, Ua..... is
expressed by
h= h
( Uc.out + Ua out - Ud.in)
Vd,ou t = ~. V s - - ~'~
= e[Vs(1 - e) - U..... t Jr- Ud,in]' (47)
The simulated dynamic responses of the Kuhni
column to step changes in the manipulated variables:
dispersed-phase feed flow rate, continuous-phase
feed/effluent flow rate and rotor speed, are plotted in
Figs 5-7. These are the manipulated variables usually
used to control the holdup and outlet concentrations.
In the plots, the responses of the conventional level-
control scheme are shown by solid lines, while those of
the improved scheme by dashed lines. The open-loop
responses for the case of the improved level-control
scheme exhibit monotonic behavior, while those for
the conventional level-control show overshoots, oscil-
latory behavior and even inverse response (e.g. the
effluent concentration plotted in Fig. 7). Clearly, the
control of the column will be much easier if the im-
proved level-control scheme is adopted.
6. DESIGN AND SIMULATION OF MULTIVARIABLE
CONTROL
For the case of the conventional interface level
controller, the manipulated variables available for
control are the plate-stack oscillation frequency, the
dispersed- and continuous-phase feed flow rates.
When the modified interface level controller is used,
the continuous effluent flow rate may be employed as
(46) the control variable instead of the continuous-phase
 332 O. Weinstein et al.

0.4

~ 0.3

0.2
6
0.1
lobo '
2000 3o;o '
4000 5000
t [s]

~0.4

e~

~-o.3

~o.2 2o o 30;0 40;0 5000

t [s]

Fig. 5. Comparison of the transient behavior in response to a step change of 40% in dispersed-phase inlet
flow for the two level-control schemes: (- ) conventional scheme; (---) novel scheme. The initial values
of the input variables before the onset of the disturbance are Ud = Uc = 0.0024 m3/m 2 s , f = 2.9 l/s, y~. = 1
1 kmol/m 3 (Kuhni column).

0.5

~ 0.4

~0.3
6
0.2
1000 2000 3000 4000 5000
t [s]

-~
c-
0.3
O

"~ 0.28
.e
~0.26

~0.24

0.22
Z~ 10;0 20;0 30b0 40;0 5000
t [sl

Fig. 6. Comparison of the transient behavior in response to a step change of 40% in continuous-phase inlet
flow for the two level-control schemes: ( ) conventional scheme; (---) novel scheme. The initial values
of the input variables before the onset of the disturbance are Ud = Uc = 0.0024 m3/m 2 s , f = 2.9 l/s, Yi, = 1
1 kmol/m 3 (Kuhni column).

feed flow rate. Both types of level controller were
discussed in the previous section. The system outputs
are effluent c o n c e n t r a t i o n s a n d dispersed-phase hold-
up. Multivariable control for a K a r r column will now
be designed a n d tested by simulation. F o r this system,
p h o s p h o r i c acid is fed in the c o n t i n u o u s phase (pen-
tanol) a n d extracted in the dispersed phase (water).
Physical d a t a for the w a t e r - p e n t a n o l - p h o s p h o r i c
acid system appears in D a u b e r t a n d D a n n e r (1985).
D a t a for the c o l u m n a n d physical properties are given
in Table 2.
6.1. Generatin9 an empirical model
The responses of h o l d u p a n d b o t h phase outlet
c o n c e n t r a t i o n s to 10% step changes in the control
variables are plotted in Fig. 8 for the case of the
c o n v e n t i o n a l level controller, a n d in Fig. 9 for the case
 Liquid-liquid extraction columns 333

0.4

~ 0.35

¢* 0.3

0"250 1000 2000 3000 4000 5000

t [sl
~o.3
g~
Q

~-o.2

0.1~
10bo 20b0 40b0 50o0
t Is]

Fig. 7. Comparison of the transient behavior in response to a step change of 31% in rotor speed for the two
level-control schemes: ( ) conventional scheme; (---) novel scheme. The initial values of the input
variables before the onset of the disturbance are Ud = Uc = 0.0015 m3/m 2 s,f = 2.8 l/s, Yin = 1 1 kmol/m 3
(Kuhni column).

Table 2. Physical properties and column data for the Karr column

Parameter Value Units Description

pc 814.4 (kg/m 3) Continuous-phase density (pentanol)

Pa 998.2 (kg/m 3) Dispersed-phase density (water)
r/c 0.4045 x 10-3 (kg/(m s)) Continuous-phase viscosity
qa 1.003 x 10 3 (kg/(m s)) Dispersed-phase viscosity
m 12.25 Distribution coefficient
l 2.5 (m) Column height
dr 0.05 (m) Column diameter
ho 0.027 (m) Rotor diameter
Co 0.9 -- Orifice coefficient
So 0.6 -- Fractional open area

of the modified level controller. In both figures, level-controller case in the vicinity of the operating
the process outputs are simulated for positive (solid point
line) and negative (dashed line) step changes in

].E,
inputs. For the case of negative inputs, changes in
the responses have been plotted with opposite sign. Y=P'U~ = P21 (48)
As with the K u h n i column, the Karr column re- P22 P23] Uc
sponses for the case of the conventional level-
Pij =
control scheme (Fig. 8) show overshoots and oscil-
lations in the holdup in response to disturbances in
Ii (K + AK) [(zt + Azl)s + 1]
all control variables as well as an inverse response
272 + A~2)2S 2 + 2(z 2 + Az2)(~ + A~)s + l J i j '
and overshoot in outlet dispersed-phase concentra-
tion. The modified level-control scheme shows i = 1,2; j = 1,2,3. (49)
significant improvement of the system's dynamic re-
sponse (Fig. 9), which should permit more effective In the above, ~ is the change in holdup, )( is the
control. change in the outlet dispersed phase concentration,
An empirical uncertain linear model has been iden- f is the change in the plate stack oscillation frequency,
tified by fitting low-order transfer functions model Ua is the change in the dispersed-phase feed flow rate,
using simulated step response data for the modified Uc is the change in the continuous effluent flow rate.
334 O. Weinstein et al.

f [l/s] Ud [m/s] x 10 "a Uc [m/s]

- 0.04 i

0.02
~::O0~l 10~:)0 o,~t
2000 0 1000 2000
X 103 x 103

:°]A
x 10~

. . . . .

0 IOO0 2000 0 1000 2000 2000

xlO 3 x 10~ x 104

O:

~'-2
-2 ~
,olaf
0 IOO0 2000 0 1000 2000 0 1000 2000
t[sl t [s] t (sl

Fig. 8. Simulated transient behavior in response to positive ( ) and negative (---) 10% step change in
the control variables for the case of conventional level control. The initial values of the input variables at
steady state just before the onset of disturbance are Ud = 0.006 m3/(m 2 s), Uc = 0.003 m3/m z s , f = 1.2 l/s,
Y~n = 0.2 kmol/m 3 (Karr column).

f [l/s] Ud Ira/s] x 10 3 UC [m/s]

IY
! - o.~i
4i
~:~0.01 0.02i

o ~ .,~ 20o0 o0 1000 2000 2000

,!y
x 10"3

]
x 10~ xlo -3

X 2 ....

0u , J
0 1000 2000 0 1000 2000 2000
x l o -~ xlO ~ x l O "4

O:

~'-2

0 1000
t [s]
2000 0 1000
t [s]
2000
i/o t [s]
2000

Fig. 9. Simulated transient behavior in response to positive ( ) and negative (---) 10% step change in
the control variables for the case of modified level control. The initial values of the input variables at steady
state just before the onset of disturbance are U~=O.OO6m3/m2s, Uc=0.003 m3/m2s, f = 1.2 l/s,
Yio = 0.2 kmol/m 3 (Karr column).
 Liquid liquid extraction columns 335
Table 3. Process transfer function coefficients

Element K AK Z1 A'r I 1:2 A~C2 ~ A~

Pit (eft) 0.264 0.018 16.1 2.7 84.9 3.2 0.85 0.03
P12 ('g/Ud) 0.439 0.082 23.3 6.6 93.2 18.2 0.86 0.07
P13 (,g/Uc) 0.055 0.003 16.5 0.03 83.9 3.9 0.84 0.01
P21 (X/f) 0.016 0.003 773 261 65.9 16.9 1.53 0.46
P22 (X/Ua) -- 0.077 0.005 123 123 98.3 52.2 0.76 0.15
P23 (X/U~) 0.091 0.001 42.2 2.4 109.9 3.6 0.98 0.05

Equations (48) and (49) describe the response of the
two-process output variables to the three-process in-
puts as a matrix of uncertain linear transfer functions.
The transfer functions parameters are given in Table
3. The uncertainties AK, Art, At2 and A~ reflect the
variation in model parameters required to enable
a reasonable fit to the process trajectories in response
to positive and negative step changes in the inputs in
the vicinity of the operating point. The simple transfer
functions (49) are not able to capture all the observed
nonlinear features shown in Fig. 9, especially for the
response of the dispersed-phase effluent concentra-
tion. This leads to additional unquantified high-
frequency uncertainty in the parameters associated
with this output.
6.2. Control system design
Decentralized (i.e. diagonal) control has been
chosen. From RGA analysis (Bristol, 1966), it is ap-
parent that the most promising pairing is to control
the outlet dispersed-phase concentration using the
continuous feed flow rate and the holdup using the
plate-stack oscillation frequency. The IMC synthesis
procedure described by Morari and Zafiriou (1989)
has been used for control system design. As a result,
the two single-loop IMC controllers are determined
as
[ z2s2+2r2~s+l l designed in order to compensate for the effect
q'(i/)?) = LK(77s +~+- lj],1
[ r2~s= + 2 r d s + I ]
q2(g/CL) = L.K(G7s + 1)i;,e3s + 1) 23
The RIM provides a sufficient stability condition for
decentralized diagonal control. Clearly, if the off-
diagonal elements of the MIMO system are small
relative to the diagonal elements, then it will be rela-
tively easy to satisfy eq. (51), since the complimentary
sensitivity functions are of the order of unity.
Frequency ranges where diagonal dominance does
not hold will result in RIM values under unity and
will limit achievable bandwidth. The RIM parameter
therefore represents constraints on achievable perfor-
mance caused by the interactions in the process. Thus,
plotting RIM as a function of frequency indicates the
bandwidth over which stabilizing control is guaran-
teed. The limiting time constant value, 2~s, of filter, f,
can be determined by eq. (51). This procedure is illus-
trated in Fig. 10. for 2 = 15s. The filter time constant
values, 211 and 223 used in closed-loop simulations
have been chosen as 100s, providing responses free of
oscillations. The increased filter time constant values
reflect a desire for increased gain margin in the face of
unmodeled uncertainty (especially in the response of X).
The dispersed-phase holdup is an important system
output variable because its overshoot may lead to
flooding, aside from its effect on the concentration
dynamics. For this reason, a dynamic decoupler and
feedforward controller have been designed to stabilize
the holdup. A block diagram for the control system is
shown in Fig. 11. A dynamic decoupler has been
of continuous-phase feed on holdup magnitude. The
(50) parameters of the decoupler are calculated using
the nominal process model (indicated by the super-
script ~)

--/D13 [K(rls -[- 1)]13[-r2s 2 -1- 2Zz(S + 1111

The tuning of the IMC controllers was carried out
using the Rijnsdorp Interaction Measure (RIM,
Rijnsdorp, 1965): nominal stability is guaranteed in
the face of process interaction, if
f P2.ico)p13(i~)"]-1
~/[P11(ko)P23(io)) // > Ihis(i~)lV~
where the left-hand-side-term is the RIM, and his is
the nominal complementary sensitivity function relat-
ing process output i to set-point change j. According
to IMC design procedure, his = Paisfq. Since in our
case PA~S= 1 (the process has no N M P components),
his(s) =f~(s) = (2iss + 1)- 1.
DIs) = /311 = - [K(rlS + 1)]11[z22s2 + 2"c2~s + 1113"
(53)
A feedforward controller has been introduced in order
to compensate for the effect of dispersed-phase feed
(51) flow on holdup. The IMC design procedure has been
used for the feedforward controller
-- /~12
qf(g/Oa)-- Plx
[K(rls + 1)]12[r2s 2 --k 2%~s + 1111
[K(rxs + l)]11['T22s 2 + 2%¢s + 1112'
(52) (54)
336 O. Weinstein et al.

101 ........ , ........ , ....... , ....... , ........ , ........ , ........

Z
10°

........ , ........ i ........ , .... ":...., ........ , .......

10~10-5 i , ,,....i
104 t O "3 10 -2 1 0 -1 10 ° 101 10 2

Frequency [rad/s]

Fig. 10. RIM test for tuning the IMC controller.

] +

• {
£
~p

ql
I

Fig. 11. The block diagram of the control scheme.

The designed control scheme was implemented using shown for the IMC scheme in Fig. 13(a) and for the
MATLAB/SIMULINK. decoupled IMC scheme in Fig. 13(b). The level is
maintained perfectly by the decoupled scheme. The
6.3. Closed-loop simulation results dynamic decoupler eliminates interaction between the
Closed-loop simulations were carried out both for continuous-phase feed flow rate and the holdup al-
decentralized IMC control alone and for an IMC most perfectly due to relatively low uncertainties in
controller augmented by a decoupler and a feedfor- the linear approximation and the relatively low sensi-
ward controller. Figure 12 shows the simulated con- tivity of holdup to the continuous-phase feed flow
trol system performance for a 10% set-point change in rate.
outlet dispersed-phase concentration: the decoupled Finally, the regulatory performance of the de-
scheme [-Fig. 12(b)] performs significantly better than coupled IMC scheme augmented by feedforward con-
the scheme without the decoupler [Fig, 12(a)]. trol [-Fig. 14(b)] can be compared to that of the simple
The regulatory closed-loop response to a 10% dis- decentralized IMC scheme [Fig. 14(a)], for a dis-
turbance in continuous-phase feed concentration is turbance in the dispersed-phase feed flow rate. Here,
 Liquid-liquid extraction columns 337

(a) Decenla-allzedIMC

0.1 ...... .........................................................................

~. 0.05
"7..
f
0
I I I I I I I I I
100 200 300 400 500 600 700 800 900 1000
time [s]
Co) D c c o u p l e d I M C + F F

0.1 .."" ..............................................................................

Z ..'"

~
,--?
0.05

I I I I I I I I
0 100 200 300 400 500 600 700 800 903 1000
time [sl

Fig. 12. Simulated closed-loop response to a set-point 10% step change in outlet dispersed-phase concen-
tration: (a) decentralized IMC scheme; (b) decoupled IMC [ ( - - ) g/e(t = 0), (---) X / X ( t = 0)].

(a) DecentralizedIMC
0 . 0 3 [ ~ . . . .

Z ore- .."
+ •
0.01 :" '"' ............
: ""',,,..,..
~ O: ..................

-001 ~ ' ~ ~ ' I

• 0 100 200 300 400 500 600 700 800 9OO 1000
time [sl
(b) DecoupledIMC + FF
0.03[ ,
,,, . . . . . , . . .
,

°.°'t. .............
~.ooi: • 0 100 200 300 400 500
..............................
600 700 800 900 1000
time Is]

Fig. 13. Simulated closed-loop response to a 10% step change in feed continuous-phase concentration: (a)
decentralized IMC scheme; (b) decoupled IMC [( ) g/~(t = 0), (---) X / X ( t = 0)].

the impact of augmenting feedforward and decoupler conclusions based only on simulation results. It would
components for the holdup alone can be seen; the be advisable to compare closed-loop performance for
holdup level is almost perfectly stabilized in face of both level-control systems experimentally•
a - 5% step change in Ue, at the price of a slight
deterioration in the response of the outlet dispersed-
phase concentration. 7. CONCLUSIONS
A similar procedure was adopted to design decen- A theoretical dynamic model has been developed
tralized control for the conventional level control for a countercurrent liquid-liquid extraction column
configuration. The resulting performance is slightly based on the average dispersed-phase drop diameter.
worse than that obtained with the proposed modified The dynamic simulations relying on this model have
level control strategy. It should be noted that this been found to be in agreement with experimental data
 338 O. Weinstein et al.

(a) Dccentrallz~IMC

".....

N -0.04
i i i
-0.% 100
' 200
' 300
' 4 0' 0 O0 700 800 900 1000
time [sl
fo) DecoupledIMC + FF

Z 0.04
~. o.oz "'.....
o
'-741.02
-0.04
-0.06 . . . . .

100 200 300 400 500 600 7 8 1(300

time [s]

Fig. 14. Simulated closed-loop response to a - 5% step change in feed dispersed-phase flow rate: (a)
decentralized IMC scheme, (b) decoupled IMC augmented with feedforward action [( ) k/e(t = 0),
(---) 2/x(t = 0)].

and some published theoretical results. Thus, the S cross-section's area, dimensionless
model can be reliably applied to the control of an U loading (Uc -- Qc/S and Ud = Qd/S),
extraction column and for the study of the extraction m3/m 2 s
process. Two control schemes for dispersion interface Q flow rate, m3/s
level have been investigated: conventional level con- V velocity [V~ = U c / ( 1 - e) and Vd =
trol using the continuous-phase effluent flow rate as Ud/E)], m/s
the manipulated variable, and level-control using the V~a continuous phase effluent flow rate,
continuous-phase feed flow rate. It has been shown m3/s
that the conventional level-control scheme leads to Xac acetone mass fraction, dimensionless
unavoidable overshoots and oscillations in the output X solute concentration in the dispersed
variables, while the proposed alternative scheme leads phase, kmol/m 3
to smoother, overshoot-free response. It has also been Y solute concentration in the continu-
demonstrated by simulation that a model-based I M C ous phase, kmol/m 3
controller, augmented by a dynamic decoupler and
feedforward control, provides excellent servo and Greek symbols
regulatory response for a Karr column. volume fraction holdup of dispersed
phase, dimensionless
I M C controller filter time constant, s
NOTATION viscosity, kg/m s
a specific interfacial area, m 1 P density, kg/m 3
d32 Sauter mean drop diameter, m a interracial tension, N/m
dK column diameter, m z time constant, s
dR rotor diameter, m co frequency, rad/s
D axial dispersion coefficient, m2/s ~o free fractional area of plate, dimen-
D,, molecular diffusivity coefficient, mZ/s sionless
f IMC controller filter, dimensionless
h level, m Subscripts
hz section height, m c continuous phase
K overall mass transfer coefficient, m/s d dispersed phase
l column height, m
n grid, dimensionless Dimensions numbers
nz rotor speed, 1/s nzd~pc .
q I M C controller transfer function, di- ReR = - - impeller Reynolds n u m b e r
qc
mensionless
2 3
t time, s nzdRpc .
WeR - - impeller Weber n u m b e r
s Laplace operator, i/s (7
 Liquid-liquid extraction columns
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