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Preprints of the 8th IFAC Symposium on Advanced Control of Chemical Processes

The International Federation of Automatic Control


Furama Riverfront, Singapore, July 10-13, 2012

Time-optimal batch diafiltration


Radoslav Paulen Miroslav Fikar Greg Foley
Zolt
an Kovacs Peter Czermak ,

Faculty of Chemical and Food Technology, Slovak University of
Technology in Bratislava, Radlinskeho 9, Bratislava, Slovakia, (e-mail:
{radoslav.paulen,miroslav.fikar}@stuba.sk)

School of Biotechnology, Dublin City University, Dublin, Ireland
(e-mail: greg.foley@dcu.ie)

Institute of Bioprocess Engineering and Pharmaceutical Technology,
University of Applied Sciences Mittelhessen, Wiesenstrasse 14, 35390
Giessen, Germany (e-mail: {kovacs.zoltan,
peter.czermak}@kmub.th-mittelhessen.de)

Department of Chemical Engineering, Kansas State University,
Manhattan, Kansas

Abstract: This study concentrates on time-optimal operation of a general batch diafiltration


process. The process model consists of a set of input affine differential equations. We apply
Pontryagins minimum principle to formulate necessary conditions of optimality. These are then
used to identify the shape of optimal control as well as singular surface in concentration space.
Comparison is made between traditional control techniques and obtained minimum time control.
It is shown that traditionally used operations are suboptimal for selected case studies.

Keywords: Optimal control; Singular control; Pontryagins minimum principle; Diafiltration;


Membrane filtration.

1. INTRODUCTION tem. To achieve given separation goal we may dynamically


influence the concentrations by adding solute-free solvent
Diafiltration is known as an effective membrane process (diluant) to the feed tank. By the good choice of diluant
for separation of two or more solutes from a solution. adding strategy, we can further enhance the economics of
Currently, it is well established in chemical, biochemical, the process and achieve time-optimal production.
food and pharmaceutical industry (Lipnizki et al., 2002). Several diluant utilization schemes have been proposed
Its aim is the increase of concentration of a desired product to efficiently control the diafiltration process (Jaffrin and
together with the simultaneous decrease of concentration Charrier, 1994, Foley, 2006). These considered various
of impurities in solution. This goal is achieved by employ- combinations of three operational modes: concentration
ing selective separation membrane. mode (C), constant volume diafiltration (CVD) mode and
This process may be implemented as continuous or batch variable volume diafiltration (VVD) mode.
while the current setup is case-by-case dependent on the Pioneering work in optimization of diluant adding during
scale, system properties (e.g. solution viscosity and stabil- diafiltration process is attributed to Ng et al. (1976). They
ity), and overall economics. Once decided whether con- used concentration polarization model of transmembrane
tinuous or discontinuous regime of the process will be flow and derived optimal concentration to start CVD step.
exploited, the control strategy is picked. Control strate- Up to now, many attempts appeared in the literature
gies such as constant flux, constant pressure, or constant to treat the problem of time-optimal diafiltration. These
(membrane) wall concentration (van Reis et al., 1997) are either optimize switching times between arbitrarily prede-
usual choice. fined operational modes (Asbi and Cheryan, 1992, Foley,
In this study, we consider batch process under constant 1999, Yazdanshenas et al., 2005) or find approximations
pressure operation. This means that pressure, tempera- to optimal control (Takaci et al., 2009, Fikar et al., 2010).
ture, and internal liquid circulation flowrate between feed The present study builds upon our previous work (Paulen
tank and membrane module are kept constant in the sys- et al., 2011) where time-optimal control was proposed
This research is a cooperative effort. The first and the second using Pontryagins minimum principle approach for con-
author acknowledge the contribution of the Scientific Grant Agency centration polarization model. We generalize it for a gen-
of the Slovak Republic under the grant 1/0095/11 and the Slovak eral batch membrane process and show that the resulting
Research and Development Agency under the project APVV-0551- control strategy can be applied with a large set of known
11. The fourth author would like to thank the Hessen State Ministry membranes. Following sections give generalized process
of Higher Education, Research and the Arts for the financial support model, derivation, and interpretation of optimality condi-
within the Hessen initiative for scientific and economic excellence
(LOEWE-Program).

IFAC, 2012. All rights reserved. 804


8th IFAC Symposium on Advanced Control of Chemical Processes
Furama Riverfront, Singapore, July 10-13, 2012

diluant retentate permeate


1
q q
C-CVD-C
membrane
module


C-VVD

feed tank VVD

0
time
Fig. 2. Representation of traditional control strategies in
terms of the function.

Fig. 1. Schematic representation of a generalized UF/DF V = ( 1)q, V (0) = V0 . (2)


process.
3. PROCESS OPTIMIZATION
tions. Finally, time-optimal control is compared with tra-
ditionally used control approaches on selected case studies.
The objective of this optimization task is to find the time
2. PROCESS DESCRIPTION dependent function (t) which uses minimum time to
drive the process from the initial state to the prescribed
A schematic diagram of a generalized diafiltration pro- terminal state. Mathematical formulation of this dynamic
cess is shown in Fig. 1. Solution containing diluant (sol- optimization problem is as follows
vent), micro-solute (low molecular weight component) and J = min tf , (3a)
(t)[0,)
macro-solute (high molecular weight component) is taken
from the feed tank to the membrane module. Installed s.t.
membrane is designed (prepared) in a way to let pass c1 q
c1 = (R1 ), c1 (0) = c1,0 , c1 (tf ) = c1,f , (3b)
micro-solute and retain macro-solute. Permeate stream V
then leaves the system with the flowrate q which is specific c2 q
c2 = (R2 ), c2 (0) = c2,0 , c2 (tf ) = c2,f , (3c)
for given membrane, operating conditions and is often V
a function of actual concentrations of separated species. V = ( 1)q, V (0) = V0 . (3d)
Retentate stream is then introduced back to the feed tank. The value of = represents, physically, a pure dilution
Hence this setup can be used both for recovery of low step, i.e. pouring certain amount of diluant into the feed
molecular weight components as well as for concentration tank in one time instant. We will make use of Pontryagins
of high molecular weight components in solution. The minimum principle (Pontryagin et al., 1962, Bryson, Jr.
process control is achieved by adjusting the flowrate of and Ho, 1975) to this problem. The process differential
solute-free diluant (usually water) to the feed tank. Con- equations are affine in control
trol variable is traditionally defined as a ratio between
the inflow of diluant to the feed tank and the outflow of x = f (x) + g(x), (4)
permeate q. where x = (c1 , c2 , V )T . Due to this, Hamiltonian function
takes control-affine form as well
We consider a process where a macro-solute is to be
increased in concentration from c1,0 to c1,f and a micro- H(x, , ) = H0 (x, ) + H (x, ). (5)
solute reduced in concentration from c2,0 to c2,f . The stan- with vector of adjoint variables = (1 , 2 , 3 )T . Neces-
dard three-step operation is to pre-concentrate, diafiltrate sary conditions of optimality as derived in Pontryagins
with constant volume, and optionally post-concentrate (C- principle of minimum are then defined as
CVD-C), defined in Fig. 2. Pre-concentration with variable = arg min H(x, , ) (6a)
volume diafiltration (C-VVD) has been shown to have [0,)
some advantages in terms of water saving and its potential
   
H c1 (tf ) c
time-optimality has to be investigated. As VVD strategy x = , x(0) = x0 , = 1,f , (6b)
c 2 (t f ) c 2,f
possesses only 2 degrees of freedom (constant value and
H
proces duration) and these are used to fulfill given separa- = , 3 (tf ) = 0. (6c)
tion goal, its possible time-optimality is questionable. x
Since Hamiltonian is linear in its minimum will be
We assume a solution with two species with concentrations attained with on its boundaries as
c1 and c2 . The balance of each solute can be written as 
0 if H > 0,
ci q = (7)
ci = (Ri ), ci (0) = ci0 , i = 1, 2 (1) if H < 0.
V
where V is the retentate volume at time t. The rejection If H = 0 the Hamiltonian is singular and does not depend
coefficient Ri (c1 , c2 ) is assumed to be a function of both on . In this case it may be possible to construct optimal
concentrations. The same holds for the permeate flowrate surface S(x) = 0 corresponding to singular control that
q(c1 , c2 ). The volume balance can be written as depends on state variables only (Johnson and Gibson,

805
8th IFAC Symposium on Advanced Control of Chemical Processes
Furama Riverfront, Singapore, July 10-13, 2012

1963, Srinivasan et al., 2003). We use the fact that the determinant we find the expression for optimal control on
condition H = 0 implies that its derivatives with respect so-called singular arc, if such exists.
to time are equal to zero as well. We will make use of the
The overall control strategy will not change from the
following equations
previously mentioned one. In this case however, switches
H (c1 , c2 , V, 1 , 2 , 3 ) = 0, (8a) between constrained and singular control trajectories have

H (c1 , c2 , V, 1 , 2 , 3 ) = 0, (8b) to be found by other means. In our study we find them
(c1 , c2 , V, , 1 , 2 , 3 ) = 0. numerically by formulating a simple optimization problem.
H (8c)
to eliminate the adjoint variables . Hence that first
4. RESULTS
two conditions are control variable free. Further it can
be shown that conditions (8) form a system of linear
homogeneous equations in variables 1 , 2 , 3 (Bryson, Jr. The optimality conditions (8a) and (8b) give after some
and Ho, 1975). manipulations condition for singular surface
S = 1 c1 S1 + 2 c2 S2 = 0, (11)
3.1 Optimal control in special cases where Si (for i = 1, 2) is given as
Si = (Ri 1)(q + c1 q1 + c2 q2 ) + q(c1 Ri1 + c2 Ri2 ), (12)
As it will be shown later, the optimal state surface will
be in special cases a function of concentrations only, and
q Ri
S(c1 , c2 ) = 0. Thus, it will be a curve in the concentration qj = Rij = i, j = 1, 2. (13)
space. Once it is found, the corresponding singular control cj cj
can be obtained by considering its derivative with respect Although the singular surface (11) depends on unknown
to time trajectories of adjoint variables, we can eliminate them in
1 , c2 ) = S c1 + S c2 = 0.
S(c (9) some special cases as follows
c1 c2
R1 = 1 (R11 = R12 = 0). This represents a common
Using process differential equations (1) then yields for situation for a macro-solute that does not get through
S S
c1 c1 R1 + c2 c2 R2 the membrane and micro-solute can have arbitrary
(t) = S S
. (10) properties. The optimal curve S(c1 , c2 ) is given as
c1 c1 + c2 c2
(R2 1)(q + c1q1 + c2 q2 ) + q(c1 R21 + c2 R22 ) = 0 (14)
To summarize the results, once the optimal concentration
surface S(c1 , c2 ) is found the optimal operation can be both R1 , R2 are constant (Rij = 0). If both retention
stated as follows: coefficients R1 and R2 are constant and do not depend
on concentrations (for example a perfect membrane
(1) The first step is either pure dilution ( = ) or with R1 = 1, R2 = 0) the optimal curve is given as
pure filtration ( = 0) until state variables arrive at
optimal curve S(c1 , c2 ) = 0. q + c1 q1 + c2 q2 = 0 (15)
(2) The second step is diafiltration with time dependent In both these special cases we can proceed to find expres-
(t) given by (10) maintaining optimal concentration sions for optimal control (10) and use directly the optimal
values. control procedure as stated in Section 3.1.
(3) Finally, the third step is again either pure dilution
( = ) or pure filtration ( = 0) until final The expression for singular control in general case can be
concentrations of both components are obtained. derived by calculating the determinant of the homogeneous
system (8). This gives
Any of these three steps can be missing at a particular
(S1 S2 )b3 + S1 b2 S2 b1
problem, depending on process initial and final conditions = , (16)
as well as actual functions Ri (c1 , c2 ), q(c1 , c2 ). S2 a 1 S1 a 2
where expressions ai and bi for i = 1, 2 are given as follows
This result establishes that all traditionally used opera-
tions (C-CVD-C, C-VVD, VVD) are potentially optimal Si Si
ai = c1 q c2 q , (17)
for some special types of problems. However, neither one  c 1 c2 
of these can be concluded as generally time-optimal. Si
bi = c1 qR1 (qRi1 + Ri q1 )S1 (18)
c1
3.2 Optimal control in general case
 
Si
+ c2 qR2 (qRi2 + Ri q2 )S2 , (19)
c2
In general it might be not possible to end up with closed
form representation of singular surface without using ad- and
joint variables . However, it is possible to find an expres- b3 = c1 q1 S1 + c2 q2 S2 . (20)
sion for optimal control as a function of concentrations Therefore, optimality conditions provide only control (16)
only. along singular arc but not the state arc itself.
This argument is based on a fact that optimality condi-
tions (8) represent the system of homogeneous equations 5. CASE STUDIES
linear in adjoint variables. This system has a non-trivial
solution only if the determinant of its coefficient matrix In this section we concentrate on selected case studies from
is zero (Srinivasan et al., 2003). Thus by computing the literature on the optimal control of diafiltration processes.

806
8th IFAC Symposium on Advanced Control of Chemical Processes
Furama Riverfront, Singapore, July 10-13, 2012

5.1 Separation of lactose from proteins


6
S(c ,c )=0
1 2
We consider a process described in Rajagopalan and
Cheryan (1991) where lactose is separated from milk 5 min. time
proteins. Both retention coefficients are constant R1 = 1, CCVD
R2 = 0. Permeate flow was determined experimentally as 4
q(c1 , c2 ) = b0 + b1 ln c1 + b2 ln c2 , (21a)

c2 [g/dL]
= 63.42 12.439 ln c1 7.836 ln c2 (21b) 3
where c1 is concentration of proteins and c2 denotes
concentration of lactose. 2
The optimum concentration curve depends on both con-
centrations and is given by (15) as 1
S(c1 , c2 ) = b0 + b1 + b2 + b1 ln c1 + b2 ln c2 = 0. (22)
Once these optimal concentrations are obtained the con- 0
0 5 10 15 20 25
trol is calculated from (10) c1 [g/dL]
b1
(t) = = 0.61. (23)
b1 + b2
1
We consider to drive concentrations from initial point
[c1,0 , c2,0 ] = [3.3, 5.5] to final point [c1,f , c2.f ] = [9.04, 0.64]. 0.8
To perform this task in minimum time we use a three step
strategy (see state diagram in Fig. 3):
0.6
(1) Start at green circle, horizontal line: concentrate with

= 0 until optimal surface S(c1 , c2 ) is attained,


0.4
(2) Stay on this surface using constant control (23),
(3) Follow the line towards origin: pure dilution step to
arrive at the final point (red cross). 0.2

The resulting final time in this case is 4.49 hours. This can
min. time
be compared to the operation described in Rajagopalan 0
CCVD
and Cheryan (1991) where two step process (C-CVD) was
0 0.5 1 1.5 2 2.5 3 3.5 4 4.5
used. This traditional operation takes for the same initial time [h]
and final conditions 4.74 hours, an increase of 5.3%. As
we can see from the lower diagram in Fig. 3, traditional
CVD step ( = 1) starts earlier but it takes more time Fig. 3. Separation of lactose from proteins: comparison of
to reach the final point as the VVD step ( = 0.61) in minimum time and C-CVD control strategy in con-
minimum time control. There, it is assumed that the last centration diagram (upper plot) and corresponding
step (upward arrow) takes no time. Although this is not control (lower plot).
true in reality, we can simply move the dilution step out
the batch to further processing. restriction implies that optimal pure dilution step will be
actually replaced by CVD step.
5.2 Sucrose sodium chloride separation It is desired to concentrate sucrose and dilute sodium
chloride in solution from their initial concentrations given
This case study is taken from our previous study (Fikar by point [c1,0 , c2,0 ] = [10, 250] to final concentrations
et al., 2010) where we concentrated on utilization of represented by the point [c1,f , c2,f ] = [50, 50].
numerical methods of dynamic optimization to derive the The optimum concentration curve depends on both con-
optimal control of diafiltration process using an economic centrations and is given by (14). This curve was found
cost function. using numerical nonlinear equation solver. Fig. 4 shows for
This case study represents diafiltration system with one comparison of the minimum time and C-CVD-C control
variable retention coefficient (R1 is almost constant and strategy. Results show that minimum time approach takes
equal to one) and the empirical relations for q and R2 as 10.2 hours. This is visualized in lower plot in Fig. 4 as a
functions of feed composition are as follows: dashed line for the purpose of lucidity of actual comparison
of two control approaches.
q = U1 (c2 )eU2 (c2 )c1 , (24a) In contrast to that, a traditional solution with C-CVD-C
V2 (c2 )c1 strategy lasts 14.5 hours, which yields 42% optimality loss.
R2 = V1 (c2 )e , (24b)
Although that two-step approach (C-CVD) would result in
where U1 , U2 , V1 , V2 are second order polynomials which faster process it yields unacceptably high concentrations
coefficients were determined from laboratory experiments of salt (during the process run) out of the range studied
with the process solution in Kovacs et al. (2009). For in Kovacs et al. (2009). This can be observed from upper
operational reasons, it is assumed that [0, 1]. This plot in Fig. 4. For C-CVD approach, it would be neces-

807
8th IFAC Symposium on Advanced Control of Chemical Processes
Furama Riverfront, Singapore, July 10-13, 2012

550

500
0.5
450

400
0.4
350
c2 [mol dm3 ]

300

c2 [g/dL]
0.3 min.time
250 CCVDC

200 0.2

150
S(c ,c )=0 0.1
100 1 2

50 min. time
CCVDC 0
0
0 10 20 30 40 50 60
10 15 20 25 30 35 40 45
c1 [mol dm3 ] c1 [g/dL]

1
1 min.time
0.9 CCVDC
0.9
0.8
0.8
0.7
0.7
0.6
0.6

0.5
0.5

0.4
0.4
0.3
0.3
0.2
0.2
0.1
min. time min tf 0.1
0 CCVDC min tf
0
0 2 4 6 8 10 12 14
0 0.1 0.2 0.3 0.4 0.5
time [h] time [h]

Fig. 4. Comparison of minimum time and C-CVD-C con- Fig. 5. Comparison of minimum time and C-CVD-C con-
trol strategy for sucrosesodium chloride separation. trol strategy for radiopaque ethylene glycol separa-
Upper plot concentrations diagram, lower plot (t) tion. Upper plot concentrations diagram, lower plot
trajectory. (t) trajectory.
sary to follow the first part of the red trajectory until
c1 = 50 mol dm3 . This would result in inadmissibly high This example represents a situation when we are not able
concentration c2 . VVD approach is clearly sub-optimal to obtain expression for optimal concentration surface ana-
since it takes 22.8 hours (124% optimality loss). lytically. We proceed as suggested previously and derive an
expression for singular optimal control from (16). Then we
use numerical optimization to find corresponding lengths
5.3 Radiopaque ethylene glycol separation of intervals for boundary values of control as well as for
singular one. Results indicate that the optimal control
In this case study we treat modified case study taken trajectory consists of three parts: pre-concentration, singu-
from Lutz (1997) where filtration using reverse osmo- lar arc, and post-concentration step. Numerical procedure
sis membrane was studied to treat a solution containing determines lengths of all these parts. Once the structure
12 g/dL of radiopaque component (c1 ) and 0.5 g/dL of and lengths of respective intervals are fixed, we can operate
ethylene glycol (c2 ) to end up with the product with the process optimally with singular control (16) in the
concentrations: 40 g/dL of radiopaque and 0.01 d/dL of middle part.
ethylene glycol. Experimentally obtained membrane char- Fig. 5 shows optimal evolution of concentrations under
acteristics are as follows minimum time control , sketched as well. When com-
q = 29.19 ln c1 + 118.1 (25) pared with traditional control strategies, minimum time
R1 = 1 (0.01c1 + 0.25c2 + 0.1) (26) strategy saves 4.5% of process time in comparison with C-
CVD-C and 18% of process time when compared to VVD
R2 = 1 (0.0073c1 + 0.813) (27) control strategy. C-CVD-C is graphically compared to the
For the purpose of this example constants which character- minimum time one in Fig. 5. Dashed line is used, for lower
ize rejection of radiopaque were slightly changed to reflect plot, to clearly distinguish the end-point of minimum time
the situation where rejection R1 is not close to one. strategy.

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8th IFAC Symposium on Advanced Control of Chemical Processes
Furama Riverfront, Singapore, July 10-13, 2012

6. CONCLUSIONS P. Ng, J. Lundblad, and G. Mitra. Optimization of


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