Pergamon

Computers chem. Engng Vol. 20, No. 4, pp. 427-435, 1996 Copyright 1996ElsevierScienceLtd Printed in Great Britain. All rights reserved 0098-1354(95)00032-1 0098-1354/96$15.00+ 0.00

DESIGN ISSUES RELATED TO THE CONTROL OF CONTINUOUS CRYSTALLIZERS

R. A. EEK,:~ A. J. HOOGENBOEZEM and O. H. BOSGRAt Mechanical Engineering Systems and Control Group, Mekeiweg 2, 2628 CD Delft, Delft University of Technology, The Netherlands

Abstract--This paper addresses design and control issues related to a continuous crystallization process. Design addresses the configuration of actuators for this process. Results from both model studies and from experimental analysis show how different operation and design choices, related to the actuators, influence the process behaviour. The main conclusion is that classifiedremoval of small crystals (fines) and large product crystals improves the shape of the crystal size distribution (CSD) at steady-state, however, at the expense of open-loop cyclingof the CSD. A simple SISO feedback control strategy that acts on the fines removal rate can be used to stabilize these cycleseffectively. Fine particles are classified with an annular zone. The size of the annular zone can be decreased without affecting the dynamic controllability, significantly.Classified removal of product crystals from the crystallizer is achieved with a vibrating screen. The aperture size of the screen and the flow feeding the screen are considered important design parameters. Good product quality is obtained with a low feed flow and a large aperture size. Controllability analysis further reveals that for both designs only two degrees of freedom exist, i.e. a quantity related to the small particles in the CSD and the total mass production rate per unit of time can be controlled independently.

1. INTRODUCTION Crystallization from solution is a well-established and important industrial separation and purification process. The product of a crystallization process is mainly characterized by a spectrum of differently sized particles, called the crystal size distribution (CSD). The economic importance of crystallization is enormous. World-wide production of basic materials, such as adipic-acid, sucrose, ammonium sulphate and sodium chloride exceed 106 T/yr. The quality and quantity of crystals produced with continuous crystallizers is often limited due to instabilities or oscillatory behaviour of the CSD. In addition to this, the shape of the size distribution of crystals often does not meet requirements for optimal separation of the solid crystal phase from the product slurry in the crystallizer downstream.Improvement of the process performance can be achieved with feedback control, proper selection of the operation conditions and finally with design changes, like the implementation of additional actuation mechanisms. For a large class of crystallizers, a good design including a feedback controller will stabilize oscillatory behaviour, suppress disturbances and produce coarse product particles, which enhances t To whom all correspondence should be addressed. ~tCurrently with Bayer AG. ZF-TST. Leverkusen, Germany.

solid-liquid separation in the crystallizer downstream. The median crystal size can be used as an indicator for the presence of coarse particles. In general the design of a crystallization process involves decisions on several micro- and macro-scale process conditions, of which the most important are: 1. The effective crystallizer volume; 2. Suspension mixing, to ensure good micro and macro transport characteristics; 3. The supersaturation of mother liquor, as the main driving force for crystallization; 4. The effective nucleation (birth) or seeding rate; 5. And the residence time of crystals. Aspects concerning mixing are reviewed by Tavare (1986). In Hallas and Hannan (1990) a first attempt is described for modelling of flow patterns for a certain (idealized) crystallizer geometry. Nyvilt (1992) and Mersmann (1988) present several basic rules for the design and the selection of optimal operation conditions. In Bennet (1992), heuristic design rules for the selection of a crystallizer type, the process scale, and for nominal process conditions like the pressure in the boiling zone, the slurry residence time and the heat input are provided. In Randolph (1965), the mixed suspension mixed product removal (MSMPR) concept for crystallizer design is introduced. A main assumption for this design is that all particles have the same

427

428

R. A. EEK et al.

probability to be removed from the volume. More realistic models describe this probability as a function of the crystal size. In Randolph and Larson (1988), idealized models are used to study the effect of the residence time of fine and large particles on the stationary and dynamic performance of crystallizers. A review on modelling and control of crystallizers is provided by Rawlings et al. (1993). Decisive answers, however, as to which design achieves the best stationary product quality (e.g. shape of the CSD) and the best ability to suppress disturbances, are not provided in literature due to the lack of good models and reliable experimental facilities necessary for the evaluation of these models. This contribution will be limited to a single stage suspension crystallizer and the design aspects will be focused primarily on the selection of actuation mechanisms for the crystal nucleation rate and the residence time. In particular, fines removal will be studied as an actuation mechanism for the number of small particles, to improve the stationary CSD, to achieve stability and to reject disturbances in the effective nucleation rate. Secondly, product classification will be studied for its ability to enhance the steady-state product quality, e.g. a large relative number of coarse particles, and its ability to reject process distrubances. With respect to the other three aforementioned design issues, we assume that a well-mixed 1 m 3 constant effective volume is present, in which a supersaturation is maintained by evaporation of solvent. A first principles model for the CSD dynamics including a model for the CSD sensor, as described by Eek et al. (1995), is used as a tool for process simulation and analysis. Experimental evaluation of plant dynamics and controller performance is done with a 9701 pilot evaporative continuous crystallizer, which is equipped with an on-line CSD sensor. The effect of the two actuation mechanisms on the closed-loop performance will be evaluated and the influence of some design parameters will be discussed.
2. PROCESS DESCRIPTION

vessel

QP' p

..ll
"" P,~

l q , ....
Qi,T,

Fig. 1. Schematic drawing of an evaporative crystallizer, equipped with a fines and product removal system. with N ( x , t ) the cumulative number function describing the number of crystals per unit of volume, with a size equal or lower than x. The substance system we used is ammonium sulphate.
2.1. Actuators

As process actuators, the fines removal rate Qf, the total heat input defined by: P,ot=P~,+Pex, and the product removal rate Qof, are considered. Selective removal of fine and large product particles influences the residence times of small and large particles in the crystallizer volume. The heat input will mainly affect the steady-state mass production rate. In Fig. 2, the experimental fines and product classification system are described. Fines are removed selectively with an annular settling zone, in which a slow upward slurry velocity is maintained. Fines are assumed to be dissolved totally by heating (Pex) the fines flow up a further 10C, in an external heat exchanger. The volume of the annular zone is approx. 6001, which is large in comparison to the crystallizer volume. The cross sectional area of the annulus is 0.7461 m 2. Below we will investigate how the size of the annular zone affects the closed-loop dynamics. The fines removal flow rate can be varied in the range of 0.3-3.5 l/s. Product classification is achieved with a vibrating screen (Fig. 2). The feed Qv

Qf P e x ~ Pin

A schematic drawing of the single stage suspension crystallizer is given in Fig. 1. A detailed description is given in Eek et al. (1995). The process is assumed to be isothermal with a constant volume of 970 I. The CSD is described by a population density function, defined by: n (x, t) =lima, s0
A A N ( x , t)

CSD sensor

oi

Ax

Fig. 2. Schematic drawing of pilot crystallizer equipped with fines and product classifiers.

Design issues related to the control of continuous crystallizers

429

:~ 0.81t~

'

'hf

............

!]

"f__.2. 0 xt 200

0.2

Y
400

600 xp 800 size in microns

"'

'
1000 1200

Fig. 3. Removal efficiency functions.

flow to the screen can be varied in the range of 0.5-2.0 l/s. When product is removed wihout classification Qpf will equal Qp. Both classified fines and product removal are described by efficiency functions hf(x,t) and hp(x, t), respectively, which describe the probability that a particle with size x is removed from the main crystallizer volume. The function hf is given by:
1

hf(x,t)

[ x Ira2"

(1)

Because the solid concentration is low ( < 1%), the cut-size xf(t), defined as the crystal length where the probability of withdrawal from the crystallizer volume is 50%, can be derived from Stokes' relation for calculating settling velocities:

x, (t) = ~ 6 ) P , , / A

(2)

where Pn is a constant factor determined by the physical properties of the substance system and A the cross sectional area of the annular zone. The function hp is given by: / x \,p2

Pp3+ (1-- 2pp3) ~ Z ) hp(x) 1 + (1 - 2pp3) ( x / p ~ 2 (3)

models (Hecht, 1987), which relate an observed light diffraction pattern to the distribution where it originates from. A scatter matrix is developed based on Fraunhofer diffraction theory. Discretization of this model results in the following linear output model: L = Gn, with G the sensor model matrix, L the scattered light energy vector measured on 31 concentricai detector rings, and n a discrete population density. Meaningful quantities, like the median crystal size (denoted as Xs0), and the spread of the distribution, can be estimated from the diffraction pattern (Boxman et al., 1991) with the inverse diffraction model. These quantities are advantageous as they have a direct physical interpretation. However, the inverse diffraction model is ill-conditioned (see also Rawlings et al., 1993), and it is not sure whether the best information present in the outputs is used. Therefore, in addition to this method, we decomposed the scattered light energy vector to its principal components. The principal components are estimated from an eigenvalue decomposition of the correlation matrix estimated from a large set of samples of the scattered light energy vectors recorded from the sensor over a large time span. For details of this method we refer to Fukunage (1972). The eigenvectors corresponding to the largest eigenvalues are orthogonal vectors. Projection of the 31 measured energy values onto these signal directions, results in a reduced set of output signals, which are denoted as Ya, Y,2, In Fig. 4, the three principal eigenvectors of six different correlation matrices, which were calculated from six independent historical data sets, are given. The corresponding eigenvalues reveal that more than 95% of the total signal energy is captured by these three components. The
0.51

\PpI/
This function contains three parameters: the cut-size Xp, parametrized by an unknown factor Ppl, the imperfection Pp2 and an offset Pp3. The latter has a large influence on the void fraction of the product. In Fig. 3, an example of these S-shaped curves is given. A distinction is made between classified and unclassified removal of product slurry. In the latter case hp(x)= 1, O<x~xe, with x, the largest particle size accounted for in the model.

olU'-'
_0.5 L 0.51 _ ,~. i

2.2. Sensors
On-line measurement of the CSD is not straightforward. In this work, forward laser light scattering is applied. The scattering of an incident laser beam by a population of differently sized particles, suspended in a liquor flowing through an optical cell, can be described by several so-called diffraction
CkCE ZO:4-1

10

15 20 ring number

25

30

Fig. 4. Principal components of output vector estimated from eight different data sets.

430

R. A. EEl< et al.

signal Yr, is correlated strongly to the number of fine particles. As will be illustrated below, this signal has excellent properties to serve as an input to a stabilizing fines controller. In addition to the CSD sensor, an independent sensor is used to measure the solids fraction in the product flow. The solids flow in (kg/s) is calculated from the third moment of the CSD and the product flow:

removal AC CSD

M,=kvpcQpf]nx3dx,
where kv is a shape factor, and Pc the density of crystals.
3. PROCESS DYNAMICS

Fig. 5. Interconnection diagram for a single stage continuous crystallizer (from Randolph and Larson, 1988).

Crystallization processes are in principle distributed parameter processes in which the dynamics are mainly influenced by crystal growth, birth and crystal removal. The crystallizer considered here is described by a supersaturation balance, for the supersaturation of mother liquor and a population balance for the dynamics of the CSD. The supersaturation is a nonlinear ODE described by: dAC(t)

d ~ -~fac(U, n, t),

(4)

with the process inputs: u = {Qf, Qp, etot}. The supersaturation mainly determines the growth rate of particles. However, supersaturation may also affect the purity of crystals, their mechanical properties, and their morphology (Mersmann, 1988). Therefore the level of supersaturation at which the crystallizer operates is taken as an important design parameter for which often an upper limit exists. Below the relative supersaturation in percentage of the saturation concentration is used. The evolution in time of the CSD is described by the population balance:

On(x,t) --dOt

OG~(x,t)n(x,t) Ox I-Qf(t)yf + [~hf(x,

x n (x, t) = 0, Qpf(t)

t)+

V hp(x, t)]
(5)

growth rate of crystals suspended in the slurry and the birth rate of new crystals. The birth rate mainly determines the boundary condition of the crystal population. The growth rate, together with the removal rate of particles, determines the slope of the population density function n(x, t). For a stationary crystallizer, operated with a constant growth rate Ge = g , with hf = 0 and hp = 1, the population density vs size describes a straight line with slope -Qp/gV on a semilogy plot. For a nonstationary crystallizer cycling of the CSD occurs due to the physical feedback loops (see Fig. 5) between the CSD and the birth rate, and between the CSD and the supersaturation, via the total surface area of particles (SA) available for consumption of the supersaturation. For simulation and analysis purposes, the population balance model is lumped with a finite difference scheme and linearized analytically by applying a first-order Taylor approximation (de Wolf, 1990). To perform an analytic linearization is laborious, however, this approach was necessary to avoid numerical problems that clearly exist with numerical linearization schemes. The resulting model used for process analysis is chosen as a 100-order linear statespace model {A, B, C, D}. The state vector contains 99 elements for the discrete population density and one element for the supersaturation. A nonlinear lumped population balance model, including 199 discrete elements for the CSD, is used for plant simulation. We found that the linearized model accurately predicts the stability of the process, and gives a sufficiently accurate description of the process input-output behaviour in the frequency domain.
4. FINES REMOVAL

with the initial condition ns(x, to), the boundary condition: n(xo, t) = B(t)/Gk(t) and ),f a mass separation efficiency factor. The birth and growth rate of crystals are both described by empirical relations (Eek et al., 1995). In Fig. 5, the process dynamics are further explained. The supersaturation, determined from mass and heat balances, affects both the

The first design considered here, is a crystallizer equipped with a fines removal system, and an unclassified product removal system. As the main design parameters, the cross sectional area of the fines classifier (Fig. 2) and the removal flow are

Design issues related to the control of continuous crystallizers considered. Equation (2) relates the product flow and the cross sectional area to the cut-size xf.
40

431

4.1. Open-loop plant behaviour

In Fig. 6, the open-loop start-up response of the process is given for three different fines flows and in Fig. 7 the slurry density corresponding to the startup with 1.01/s fines removal, is given. Also the retention time of fine particles defined as:
r(f = V / Q f ,

~ 2o
0 5 10 15 20 25 time [hours] 30 35 40

Fig. 7. Experimental response of mass production rate corresponding to start-up experiment with 1.01/s fines removal.

is given. Because product is removed unclassified from a well-mixed vessel with a constant rate, and the heat input is constant, the repsonse of the slurry density follows a first-order exponential response, that reaches a stationary value after six residence times, which is 8 h (see Fig. 7). The experimental results reveal that increasing the fines removal rate strongly promotes cycling of the CSD.

4.2. Model results

Model studies performed with the nonlinear process model [which is fitted to these experimental data as described in Eek et al. (1995)[, reveal that the product quality of the stationary crystallizer increases with increasing fines flows. In Table 1, the median crystal size, the relative number of fines: defined as:

R,=flfndx/findx
and the level of supersaturation in percenage of the saturation concentration, for three different fines flows are given. As can be seen, fines removal increases the median crystal size, however, also increases the relative amount of fines and the level

800

Qf=l.0 l/s

4O0 200

1000~ '~ 800[ t/~

600

Qf=2.2l/s rtf=7.3min

200t
8O0 6OO 4OO 2OO 5 10

/~

iJ

of supersaturation. This is further explained in Fig. 8 where we plotted three normalized stationary distributions after positive step changes in the fines flow, the product flow and the heat input. These distributions are normalized by subdividing a nominal distribution, representing a crystallizer operated with a fines flow of 1.0 l/s, a product flow of 0.215 l/s and a heat input of 120 kW. Clearly, fines removal counteracts itself by increasing the number of fines in the region of very small particles (x ~<50 ~tm), for an increased removal rate. This is explained by additional nucleation which is caused mainly by the increase in supersaturation and the increase in the number of large mother crystals. Figure 8 further shows that the main effects of fines and product removal and heat input variation is a rotation and translation of the stationary CSD. Hence, only two independent effects are observed. Application of a singular value decomposition to the dynamic linearized plant model with the inputs u = {Qf, Qp, Ptot} and the outputs y={yrl, gso, Mt} shows that the condition number (i.e. the ratio of the largest to the smallest singular value) is larger than 100 over the whole frequency domain. This points at a large directionality of the plant [see Skogestad and Morari (1988) for details on the use of the singular value decomposition for controllability analysis]. A simplified plant is obtained by omitting the median Xs0 as output and the unclassified product flow as actuator, which is desired as this input has a large interaction with the up- and down-stream processes, present in the same cascade. A two-input-two-output plant is thus obtained, which has a limited interaction and a condition number lower than 5 over the whole frequency domain of interest. Hence, a multiloop PI control configuration is assumed to be sufficient. The first loop, that controls yf~, is expected to
Table 1. Stationary C S D values at different fines flows Qf (l/s) Xso (~m) 517 611 735 811 Rf ( - - ) 0.64 0.66 0.73 0.80 AC (%) 0.30 0.37 0.49 0.64

/)

A34,~s /~
30

/47rain// t

1
!
40

15

20 25 time [hours]

35

Fig. 6. Experimental start-up responses of median crystal size for three different fines flows (from Eek et al., 1995).

0.00 0.75 1.50 2.25

432
3[
. . . .

R.A. EEK et al.

1.5*Ptot t 0 -1 -2 -3 80(3-crystal size [microns] ,...y

Fig. 8. Simulated effect of 50% positive changes in process input parameter values on normalized stationary crystal size distributions.

g 70c ~ 6~

stabilize the CSD as disturbances or cycling behaviour is initiated as disturbances to the CSD in the small particle size range that grow to the region of large particles. The experimental evaluation of this scheme is described in the next section. In Fig. 9, a Gain plot of the linear model, with fines removal Qf as input and the first reduced output of the diffraction model as output, is calculated for different values for the cross sectional area A of the fines classifier, and for different removal flows. From these plots, it can be concluded that lowering the cross sectional area of the settling zone slightly increases the bandwidth of the open-loop process, which is desired, also a small effect on the phase plot was observed. However, from the simulations we also found that the solids concentration in the fines loop corresponding to the decreasing values for A were 52, 130 and 300g/m 3, respectively. Consequently, the minimum value for A, should be based on the maximum capacity of the fines dissolving system, rather than on the basis of process dynamics. Increasing the removal flow mainly enlarges the bandwidth of the process, as shown in the lower plot of Fig. 9. The solids fraction in the fines loop will, however, also increases for an increasing flow. The respective values for the solids concentration where 61, 130 and 189 g/m 3. Hence, the nominal fines flow should be selected on the basis of both the desired fastest speed of response

I340 ~'~320 ~1300 5 10 15 Time [hrs] 20 25 30

Fig. 10. Experimental open-loop response on a blocked product removal flow at A and C; a controller is used between B and C and after D to stabilize the open-loop response. and the maximum capacity of the fines dissolving system. 4.3. Experimental controller evaluation To stabilize the CSD and to reject CSD disturbances, a single-loop PI controller using Yr~ as input parameter and Qf as output parameter is evaluated with simulation. The results revealed that stability can be achieved easily with this controller. The controller is tested for its ability to reject a disturbance caused by blockage of the product discharge system for I h. During this disturbance the process is operated batchwise. In Fig. 10, the open-loop respsonse of the process is given for two repeated disturbances. As can be seen the slurry density increases

80()

~10" 10-3 lOI '~ 10"1~ 11~: ~ 10"~

..

A=0.375 m^2 .-

3 600

'I

. . . . . . . . .

.....

..... qf=2.0 l/s - - qf=l.0 I/s .:.:i. qf=0.5 I,s 10-4

" ' ~ .... ~ . . ----,---. ~ 10-3

1340 ~1320 [ 0 , 2

10-2

, 4

frequency ]l/s]

8 10 Time ]hrs]

12

14

16

18

Fig. 9. Bode plots for different cross sectional areas of the annulus (upper), and different values of the stationary fines removal flow (lower).

Fig. 11. Experimental closed-loop process response on blocked product flow for 1 h at A and B. Yr~is controlled on a setpoint (dashed) of -0.5.

Design issues related to the control of continuous crystallizers

433

~70o
b

soot
400[ Time [hrs] -800 [ .

::~oor_-07 ~ , ~
.......... . . . .

~__Y ....
. .

".
--

5t
j

9pf=0.50 I/s
. Opf=].50 l/s

Fig. 12. Experimental manipulated variable response (fines flow) on a blocked product flow during 1 h at A and B; dashed-clotted line is constraint. linearly after closing the product discharge and a badly dampened cycle of the CSD occurs. For control a SISO MPC controller is used (Eek, 1995). The results of a closed-loop experiment with this controller are described in Figs 11 and 12. Analysis performed after the experiment revealed that the performance of the SISO MPC controller is strongly comparable to the SISO PI controller. Therefore the latter is recommended for industrial application. As can be concluded from this result a crystallizer equipped with a fines removal system, operated in a closed-loop, improves both the stationary and dynamic process behaviour.
5. C L A S S I F I E D P R O D U C T R E M O V A L

,oot
4 o 5

b-'
o 10
15 20 25 Time [hours]

~
30

35

! J

Fig. 14. Experimental response of median crystal size of crystals in the crystallizer vessel for two experiments at different feed flows Qpf ( - - - ) ; small feed flows (upper) large feed flows (lower); the screen is switched on at T=8h. microns. In a first experiment the feed flow (Qpf) was varied step-wise. To stabilize the open-loop start-up response, the crystallizer is started without product classification in closed-loop with the SISO PI controller that is described in the previous section. After reaching sufficient stability of the CSD (8 h in the plots), the controller is switched off and the product classifier is started with a feed flow of 0.75 l/s. After 12 h the feed flow is changed stepwise from 0.75 to 0.50 l/s. The fines flow is kept constant at 1.41/s, Figure 13 also shows that the mass flow of product and the density in the crystallizer vessel, corresponding to this first experiment, exhibit oscillatory behaviour with similar dynamics. Thus product classification introduces additional interaction between CSD dynamics and the mass production rate, which was not the case with nonclassified product removal (cf. Fig. 7). A second experiment is performed with the same start-up procedure, now the screen is switched on with a feed flow of i l/s. After 17 h a step change to 1.5 l/s is made, and after 8 h the flow is switched back to 1.0 i/s (see Fig. 14). During this experiment the fines

The second design includes both a fines removal and a classified product removal system. The crystals leaving the deck of the vibrating screen (see Fig. 2) are now considered as product crystals. The product is a viscous cake which does not disperse. The solids fraction in this cake is approx. 55% (measured by hand), and fairly constant over time. The crystals and the mother liquor passing the screen apertures are returned to the crystallizer.

5.1. Open-loop plant behaviour

Two series of open-loop experiments are performed, using a screeen with an aperture size of 800

200f g,oo I i7 ....

800

Median crystal size in vessel r

400[ ':

Qpf=0.75 I/

......

Op['--0:50 i/s ....... Qpf=l.50 l/s ........

700 600 0 5 10 15 20 25 time in [hours] 30 35 5001 4001 ...................

....

. 10

15

Fig. 13. Experimental response of product mass flow (upper) and the density of slurry in the crystallizer (lower), corresponding to the first experiment with product classification.

Opf=l.00 l/s . . . . 20 25 Time [hours]

30

35

Fig. 15. Simulated behaviour of open-loop process behaviour using product classification with vibrating screen, corresponding to the two open-loop experiments.

434

R. A. EEK et al. stationary simulated values related to the product CSD, and the level of supersaturation in the crystallizer as a percentage of the saturation concentration are given for different feed flows to the screen and a constant fines flow of 1.01/s. As can be seen a further improvement of the product quality at stationary conditions is obtained in comparison with fines classification. The relative number of fines is lowered, the median is increased and the supersaturation in the crystallizer is lowered. In the first instance, it is desirable to choose the aperture size of the screen as large as possible, to produce a coarse product. However, we found that increasing Xp by 100 ~tm, roughly increases the solids fraction in the crystallizer by 10%. Therefore, the upper limit for Xp should be determined from the maximum allowed solids fraction in the crystallizer. Finally the steady-state and dynamic controllability were studied using a model with u = {Qf, Q p f , Ptot} as inputs and y = {Yrb Xs0, Mr} as outputs. Also for this case we found that varying the process input values only two main effects are observed in the size distribution: a rotation and a translation. The condition number of the three-input-three-output system is larger than 100 over the whole frequency domain. Therefore, we propose to operate the system with Qpf o n a constant and low value and to use a multiloop controller with the fines flow coupled to Yr~ and the heat input to m3. The condition number of this system is found to be lower than 10 over the whole frequency domain, indicating easy controllability. The interaction between the separate control loops is found to be small. 5.3. Experimental controller evaluation Model simulation studies reveal that for this case also, the crystallizer can be stabilized with the simple SISO PI controller, which was also used to achieve stability in the case of unclassified product removal. In Fig. 16, the results of an experiment are given where we applied this controller after switching on the screen, 6 h after a start-up without product classification. The results show that stability is achieved. Because the density in the crystallizer, and thereby the mass production rate, still shows some deviations, a multiloop controller is expected to further enhance the process behaviour.
6. CONCLUSIONS 1'0 15 2'0 Time [hours1 25 3'0 35

Table2. Stationaryproduct CSD valuesat differentclassifierfeed flows Qpf (J/s) 0.50 1.00 1.50 xso (gm) 672 620 597 Rf (--) 0.45 0.42 0.41 AC (%) 0.20 0.26 0.32

flow is kept constant at 0.8 i/s. As can be concluded, a lower feed flow Qpf, in conjunction with a larger fines flow, promote cycling of both the CSD and the mass production. Increasing the feed flow, gives a response that dampens after approx. 3 cycles. Besides, step-wise changes in the feed flow seem to have a limited effect on the CSD in both experiments. However, proper judgement is difficult in this case, due to the strong cycling behaviour. 5.2. Model results The empirical parameters in the process model related to crystallization kinetics and fines removal [equation (1)] were estimated on the basis of a series of start-up experiments, the results of which are presented by Eek et al. (1995). The parameters pp~ and Pp3 related to the product classification efficiency [equation (3)] could be determined a priori from the aperture size of the screen and the measured solids fraction of the product ( = 5 5 % ) . The efficiency factor Po2 was used as a tuning factor to match the simulation results to the experimental results. The product classification parameters thus obtained were pp~=800~tm, pp2=5.0 and pp3 = 0.029. In Fig. 15, the model output related to the screen experiments is given. As can be seen, the model gives a reasonable description. In Table 2,

1 0.5 0 -

-0.5

1320[ t310~
~ 1 2 9 0 ~ 1280 I 0 5

Fig. 16. Comparison of experimental open-loop and closed-loop response of y., the median crystal size and the density in the crystallizer vessel after switching on the screen at T= 8 h (A).

Both classified fines and product removal enhance the stationary performance of a crystallizer, however, at the expense of open-loop cycling of the CSD. With product classification additional interaction between the CSD and the mass production rate

Design issues related to the control of continuous crystallizers and the density in the crystallizer is observed. Closed-loop stability is obtained for both cases, with a simple closed-loop feedback controller which uses fines removal as its actuator and a linear combination of diffracted light energy values observed on a CSD detector as its input. For both configurations only a translation and rotation of the CSD could be achieved with changes in the process inputs. This observation is confirmed by dynamic controllability analysis which shows that only a two-input-two-output system is easily controllable. For both configurations, therefore, a multiloop control structure is proposed using the fines flow and the heat input as actuators and using the weighted number of fines and the slurry density as outputs. It is found that the feed flow to the screen can be operated at a low value, while the maximum aperture size of the screen should be determined from the maximum allowable solids fraction in the crystallizer. Large fines flows are preferable; however, they also increase the supersaturation level, which might be undesired. The size of the annular zone does not affect strongly the dynamics of the controlled process, however this parameter determines strongly the amount of solids to be dissolved.

435

Acknowledgements--The authors are indebted to Hans Gerla, Sven Rusticus and Jaap Both, who carried out part of the experimental work and to the Dutch Foundation of Technology (STW), AKZO, ICI, DOW Chemicals, DSM, E.I. Dupont de Nemours, and Eastman Chemical Company for their financial support of the UNIAK project.
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