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The authors are indebted to Professor = signal frequency, radians/hr.

Hans Kramers for several valuable sug- M = a matrix 6J

Subscripts

these papers on control while he was Minne- reactors in a chain or reaction

sota Mining and Manufacturing-Visiting order 0, 1 = C.S.T.R. feed and product

Professor of Chemical Engineering a t the Q = modified heat of reaction, (OK.) streams

University of Minnesota. (mole)/liter of A D = derivative controller

R = general reaction rate I = integral controller

NOTATION t = time, hr. n = reactor number in a chain

T = temperature, OK., or controller P = proportional controller

A = a chemical compound or its time constant S = steady state

concentration (mole/liter) V = reactor volume, liters or varia-

B = same tion vector LITERATURE CITED

C = specific heat of the reacting 2 = concentration of feed com-

mixture, calories/g. 1. Acton, F. S., and Leon Lapidus, Znd.

ponent, mole/liter Eng. Chem., 47, 706 (1955).

C = concentration, mole/liter X = variation in concentration of 2. Bilous, Olegh, and E. L. Piret, Chem.

e = volumetric C.S.T.R. (continu- feed component, mole/liter Eng. Progr. (to be published).

ously stirred tank reactor) to Y = concentration of product com- 3. Devyat,ov, B. N., and G. N. Bogashev,

batch efficiency ratio ponent, mole/liter Zhuy. Priklad. Khirn., 24, 807 (1951).

F = flow rate, liters/hr. Y = variation in concentration of 4. Eldridge, J. W., and E. L. Piret, Chem.

h = reactor heat input, "K./hr. product component, mole/liter Eng. Progr., 46, 290 (1950).

H = reactor heat input, OK./hr. 2 = variation in reactor tempera- 5. James, H. M., N. B. Nichols, and R. S.

A H R = heat of reaction, calories/mole ture, OK. Phillips, "Theory of Servomechanisms,"

of A McGraw-Hill Book Company, Inc.,

a,p, y = stoichiometric coefficients New York (1947).

I = control quality A = fractional control quality 6. Kramers, Hans, and G. Alberda, Chem.

i = pure imaginary, d 7 e = C.S.T.R. holding time, hr. Eng. Sci., 2, 173 (1953)

k = reaction-rate constant, differ- P = density of reacting mixture, 7. Mason, D. R., and E. L. Piret, Znd. Eng.

ent units. g./liter Chem., 42, 817 (1950); 43, 1210 (1951).

Reactors, and Unit Reactor Control Loops

The results which were obtained in tions X o and Y o

vi-l = M,Vi (3)

Part I for a single reactor can be used to

calculate step by step the response of a (1+ aOR,' + jcoO)X Xo =

(') with

chain of reactors. Interest in these calcu- -OR,'X + (1 + jUe)y= yo (2)

lations is twofold. First the safe operation

of the whole chain may put upon a These may be written in matrix form, the

reactor in the chain more stringent control variation vector V i representing the

requirements than would individual oper- variations in the composition of the feed

ation, especially in the case of reactions

highly sensitive to temperature. Second,

to reactor i + 1:

Therefore, the relation between product

and feed variations in composition is

these calculations can be used to deter-

mine simpler modes of control for the

v.= X; V,=(M,M, . . . M i. . * M n ) - l v o (5)

whole chain. In some cases, for instance, iyil

the feed Row is controlled by inlet This formula gives the desired result,

sampling and the whole heating system and the matrix M , of the variation CO- namely that the product composition

by a sampling of the final product, the efficients being introduced. varies as a function of feed-composition

individual heat-control loop on each I n matrix notation Equations (1) and variations.

reactor thus being eliminated. The calcu- (2) may be written

lations arc straightforward and the theory

is easily devcloped with the introduction

of matrices. It will be developed here

on the basis of the example used pre-

viously, of a reaction involving com-

ponents A and B, with a rate R(x, T). and for the reactor i in a chain

1 + aOiRzi' + j d , , 0 Xi-1

Equations (17) and (18) of Part I are - OiR,i', 1 + jwO, Yi-1

Illustration 4 INPUT OUTPUT feed- and product-composition variations

The foregoing formula will be applied to for a chain of n stirred-ffow reactors. It

the case of a first-order reaction m a y be interesting t o examine what

happens when t h e number of reactors

A-+B FINAL increases indefinitely, the total holding

CONTROL COMROLLER INSTRUMENT

performed isothermally in a chain of ELEMENT time remaining constant. This limiting

reactors of equal size. The rate of the case is represented b y a tubular reactor

reaction is Fig. 4. Block diagmm of a control system. with uniform conditions i n a cross section.

R(x) = dB dA

- = -- = kx with a 9570 conversion of compound A . Limiting Case of the Tubular Reactor

at dt The inlet and outlet concentrations are

All holding times are assumed equal

Therefore R,'(z) = 12 and the quantity compound A and r = no is the tubular-reactor holding

OR,' = Ok is constant for all reactors. All 20= 1.00 mole/liter, X, = 0.05 mole/liter time. Therefore

the matrices M , are therefore the same, and product B

Formula (5) may be written as v n = M-"vO yo = 0.00 mole/liter, yn = 0.95 mole/liter

nr

"1

where the increment AT is thus defined.

Then Expression (4) of t h e matrix Mi

- ek:, may be written .

Matrix multiplication and division yields

I + ek + j w e , The operation is isothermal, with a rate

1

constant

1 + jwe lc = 19.0 hr.-'

Ari

1 The holding time, 0, for a reactor of the -RZi', jw

-1 + elc + j w e y

- (I

0 chain is found from a mass balance over

the system, given by Neglecting second-order terms in AT;

gives

X=n-1 at vanishing frequency. I t s value, calculated

Q = elc C (1 + elc + jwe)A-n from Formula (9) for w = 0, is

the relation between variations in concen- = 1- Xn

- = 0.95

tration of A in the feed and product streams Xn

to be Passing t o t h e limit gives

It is therefore a constant, independent of

the number of reactors.

While vanishing frequency results are the

easiest to calculate, more information about

and the variation in the conoentration of B system behavior may be derived from the

i n the product stream Y,, caused by con- values of the phase angle and amplitude

centration variations X,, IToin the feed ratio of the concentration variations a t a

stream, frequency physically related to system (11)

Y, = 9x0 + (I+jw8)"

1 yo

properties, that is, for instance, such as

w n 8 = 1. Such results, calculated by means The exponential form of the transfer func-

of Equation ( Q ) , are presented in the accom- tions characterizing t h e behavior of

Usually Y o = 0, no product being present panying table.

i n the feed stream, and thus

Y, = QXO, POLAR-PLOT

DATAFOR A REACTOR

CHAIN,FOR wnO = I

or Amplitude ratio

X=n-1

Number of Unit holding Total holding I Yn/XoI Phase angle

Y, = elc CX=O

+ ek: + jwe)"-"

(I

reactors, n time, O time, nO for wn8 = 1 for wnO = 1, deg.

1 1,000 hours 1.000 hours 0.671 -48

(I + jwe)-'-'x0 (9) 2

3

0.183

0.090

0.366

0.271

0.763

0.813

-56

-57

or, summing the geometric series, 5 0.043 0.216 0.861 -58

10 0.018 0.184 0,904 -58

Yn

- = (1

xo +j d - " - (I + jwe + ek)-" m 0.000 0.158 0,950 -57.3

These values give an indication of t h e

This is an interesting result, as it relates transformation of t h e shape of t h e systems with dead time may be recog-

the variation8 in product composition to Nyquist plot with reactor number. From nized. The matrices

those in feed composition for a reactor chain. a nearly circular plot touching t h e imagi-

To illustrate this relationship bether, a nary axis a t t h e origin for a single reactor,

numerical example is presented. A chain t h e plots evolve toward a circle centered

of n equal-sized reactors operates on the

fir&-order reaction at t h e origin for the limiting case of t h e

tubular reactor.

A-B Formula ( 5 ) gives t h e relation between

CONVERSION, I - *e

1.0 , I I I I I

CONVERSION. I- +e CONVERSION, I- %

Fig. 6. Fractional control quality against Fig. 7. Fractional control quality against

conversion for proportional control of a first- conversion for derivative control of a first-

order reaction in a C.S.T.R. order reaction in a C.S.T.R.

conversion for integral control of a first-

order reaction in a C.S.T.R.

-aQ8R,’X + (1 + jw8 is obtained, which must be satisficd in

the case of a highly exothermic reaction

- aQ8ET’)Z = Z, (Q > Rzt’/RTc‘)in order to have stable

operation. This is again an example of

commute; therefore Expression (11) niay obtained from the basic expressions (17), the restrictions which control require-

be written (18), (19) of Part I. ments may impose on reactor design.

The matrix M , similar to (4) is now

I 1

variations for a chain of n reactors is as

before REACTOR CONTROL

or

In the preceding page only the calcu-

lation of the frequency response of

continuously stirred tank reactors has

8, = exp { - j w ~ } been considered. This section will com-

bine for illustrative purposes, the fre-

quency-response functions thus obtained

with different controller-response func-

Developing this matrix expression one tions to find the quality of the control

finds the formula for a tubular reactor V,=(M,M,. . . M ; . .Mn)-‘V, (15) circuit formed by reactor and controller.

(with any order reaction) whirh cor- The control system considered may be

responds to Expression (9) for a reactor where the vectors Ti, are defined now as represented by Figure 4.

chain : A variable in the reactor outlet stream,

V “= I x,,y , , z,I for instance product concentration, is

Numerical calculations on Formula (15) measured and is compared with the

are best carried out step by step. desired value in the controller which

.exp { - j u ~ ] X , , (13) The determinant of Matrix (14) is sends out a signal acting on the controlled

variable in the reactor inlet stream, for

The Nyquist diagram, which represents D, = (I + jw8,)’[1 + a8,(R,,’ instance feed concentration, through a

final control element. Detailed informa-

I’,/Xo, is a circle centered a t the origin

of the complex plane. - QRz.,’) + jw8,I tion about such diagrams and control

theory in general may be found in

The factor

references 1 and 2.

Second Case: Variation in Concentration and

Temperature with a Steady Heat Input 1 + ae,(R,,’ - +

Q R ~ , ’ ) jwe, A negligible lag is assumed in measure-

ment and in the final control element, in

The treatment for this case is similar is recognized as one that appeared in order to isolate the effect of controller-

to that above, the equations to be con- Expression (24) of Part I. response characteristics on the system.

sidered being The stability of the reactor chain is For present purposes the three usual

obtained when all units of the chain are idealized types of controllers arc ex-

(1+ a8R,’ + jw8)X + oc8Rz.’Z = X, stable. Following the discussion in Part I

the condition on the holding times

amined ( 1 ) . Actual controllers often

approach combinations of these and can

- 8R,’X + (1 + j w 8 ) Y be treated in the same manner; such a

case will be illustrated in the analogue

- 8RT’Z = Y,, example.

0 006 G,(jw) is the frequency-response function

for the reactor chain without control.

For the controlled system (Figure 4)

the input to the rcactor is equal to the

input to the system Xuminus the output

of the final controller. The input to the

controller is the output of the reactor

Y,. Hence if G(ju) represents the fre-

quency-response function for the con-

troller, thp output of the controller is

G(jw)Y,; the input to the reactor is

Xu - G(jw)Y,; and the output of the

reactor is Y , = G,(jw)[Xa - G(ju)Y,].

Fig. 8. R.E.A.C. circuit for Sol\Ting this for Y , yields

temperature control in a

C.S.T.R. Data of I ,.

illustration 3.

system with control is therefore

0.020 TIME from formula (IS), where Y(jw) is

0 replaced by its expression (20).

-100 The case of a single reactor will be

examined in more detail. The expression

of control quality for a single reactor

with different controllers or no control are,

Frequency response from the foregoing development,

Controller G(+)

integral control

Integral -P/E = l/jwTl

Proportional -P/E = K

Derivative -P/E = jwrl;

I n t h e preceding expressions of con-

troller response to a cyclic disturbance of proportional control

frequency w , E designates the error

signal and P the controller output. The

quantities T I , K , T z are constants char-

acteristic of controller operation.

Control quality may be expressed by

the quantity derivative control

unit impulse applied to systcm input a t These expressions are valid only for When there is no control, that is to say,

time zero. The choice of this criterion stable systems. The value of I would be

takes into consideration the importance infinite for an unstable system, as in -1= K = T - 0

of the deviation amplitude caused by the this case response W ( t ) is undamped or 2 -

perturbation and also the length in time TI

ever increasing in amplitude.

of the deviation. This expression will be these integrals reduce to

used in the study of control quality.

Example

The integral 1 may be evaluated in

terms of the frequency-response function A control loop will be considered on the

of the controlled system Y ( j w ) . From basis of measurement of product con-

reference 2 centration in the outlet stream and -

- ek2

control of feed concentration in the inlet 2(1+ ek)~)(2+*

W(t)= -

1

1

2a.

/ "+m

-m

dwe'"'Y(jw) (17) stream. Reactor operation is assumed to

be isothermal and data of Illustration 4 The integrals expressed above are

are used. Thus the frequency-response calculated by integration in the complex

Therefore function for a chain of n equal-sized plane or use of tables in the appendix of

reactors is given by Expression (9) : reference 9. The results have been

I ='S,- 1 W ( t ) l a dt cl(jw)= --

Y, = ek C

X=n-1

(1 + ek

expressed here in terms of the system with

no control in fractional form:

X0 X-0

= /m Y ( j w ) Y ( - j w ) du (18)

a G O

which better shows the gain in control These equations, written for an appro- dY

quality due to the controller. The value priate control loop, may be associated e- - e R L f X+ Y

dt

of A when the control loop is broken is with the linearized equations describing

zero and reaches unity for perfect control. - BRTfZ = Y o (22)

reactor behavior: [Equations (12), (13),

The expressions for the respective frac-

tional control qualities are for integral

control

(14) of Part I]. dZ

e- - aQOR,fX

dt

+ (1 - a&enTf)z

e dt + (1 + aewx

dX = eAH + Zo (23)

The system thus obtained may be solved

+ a % R T f Z= X , (21) to obtain the response of the controlled

c_ I TIME , MINUTES QOI 1 Y, MOLE /LITER

p -001 -0.01

X . MOLE/LITER TIME , MINUTES

for derivative control

TIME , MINUTES

T,lc 1 2 , *K 0 10 20

AD =

2 + + rF2%

elc

.K 1.0 0 7

represented for the different modes of

control A,, Ap, A, against conversion in 0.0 -2.0 H, .K/MINUTE

Figures 5, 6, and 7. Curves are given for 0

different values of the characteristic CONTROLLER SETTINGS = K = I , T = 1/10 MIN.

control parameters T I , K , and TO.

Conversion in this case is V

I--=-----

X ek Fig. 9. Example of C.S.T.R. temperature control (underdamped case).

z0 1 + ek

where z,,,J: are the concentrations of

reactant A in the feed and the product.

The plots of Figures 5, 6, and 7 show W

0.01 1 TIME, MINUTES 0.01 I Y, M O L E l L l T E R

same instrument when the conversion W

:.

-0.01

decreases, which is evident a priori, X . MOLE/LITER TIME ,MINUTES

the feed will have only a small effect on 10 20

K

.

outlet product concentration. The plots

are characteristic of the three simplified

modes of control examined. Idealized

components have been used in this loop

analysis and the results in practice must TIME ,MINUTES

be tempered with a knowledge of the 00 -20 I H I 'K/MINUTE

performance of the components and

system actually available. CONTROLLER SETTINGS : K 14 , T, = 114MIN.

ANALOGUE SIMULATION OF

CONTROLLED SYSTEMS

of the three types of controllers which

have becn considered in this study are 0.01 I TIME , MINUTES QOll I Y, MOLElLlTER

Integral control

d -aoi

X, MOLElLlTER TIME, MINUTES

TIME, MINWES

*K 1.0 , r\ 2 , .K O

0r 10 20

Proportional control

1

E = --p 0.5 I/ \

K

Differential control " \- g-2.01

TIME, MINUTES

10 20

H, .K / MINUTE

p = -T -

dt Fig. 11. Example of C.S.T.R. temperature control (overdamped case).

reactor to a given disturbance. The CYCLING IN SYSTEMS WITH DEAD TIME

1

analytical solution will, however, in If the number of stirred flow reactors

- In K(1 - e-kr) <o

many cases be cumbersome and in in a chain is increased indefinitely, the

practice, especially when more complex or

over-all holding time remaining constant, K(l - e+) < 1

performance functions are needed, the at the limit the case of a tubular reactor

use of an analogue computer is of great is obtained. The frequency-response func-

advantage. An example will be solved Thus a limitation exists on the values of

tions for the isothermal tubular reactor the proportional factor K which may be

with the analogue technique. without volume change have been ob-

Considered here is the case of a tem- used. If controller action is too powerful

tained in Expression (12). For the case (high K ) , cycling may develop.

perature-control loop with a controller of a first-order reaction the expression of

combining the proportional and integral the frequency-response function relating

control modes. A constant feed compo- product-concentration variations Y , to COMMENT

sition is assumed, that is to say Xo = feed concentration variations Xo has

Y o = 0, and a disturbance caused by a been found:

It should be realized that in the prac-

change in feed temperature, Zo. The tice of automatic control the results of

equations which describe this system are frequency-response analyses can today

(21), (22), (23) and the controller equlttion be used to advantage principally for

for the temperature-control loop becomes The presence of the imaginary expo- guidance rather than for the exact pre-

nential in the expression of the frequency- diction of the performance to be expected

response function is characteristic of of a practical control system. I n the

systems with dead time. Thus a measuring first place the disturbances occurring in

instrument placed a t the reactor outlet an industrial operation will not usually be

With the values of Illustration 2 for a will perceive feed perturbations only a regular or periodic, although of course the

second-order exothermic reaction time after they happen and any corrective typically random disturbance will excite

action will be delayed by that much. This all frequencies. Furthermore, the differ-

2A-+B+D dead time in the reactor system increases ences found between theory and practice

are often the result of deviations from the

with A H R = -50,000 cal./mole of A with the number of reactors in the chain simplified characteristicswhich are usually

these equations take the following form: and approaches a maximum time in a assumed for the sensing and the control

tubular reactor, and so in the latter

design control may be more difficult than elements. Furthermore largely indeter-

dX

+ +

0.33 - 16.50X 0.12452 = 0

dt in a continuously stirred tank reactor minate lags often occur in industrial

(C.S.T.R.). Also control by stages may installations. Nevertheless the equations

more readily be applied to the selected obtained as a result of the application of

dY

0.33 - - 7.750X

dt

+ Y elements of a chain. frequency response theory offer real ad-

Dead time may easily lead to cycling vantages in simplicity of treatment and

- 0.06222 = 0 of the controlled system if the control is

clarity of exposition, have proved ex-

improperly designed. Only an example tremely helpful in understanding the

dZ of such a case will be given, for propor- control process itself, and have guided the

0.33 - - 775.X - 5.2242 tional control applied to a tubular engineer to practical solutions to auto-

dt

reactor by measurement of product matic-control problems. As more precise

= 0.33AH + 2, concentration a t the outlet and control characterizations of modern commercial

instruments and of lag systems become

of inlet-feed concentration.

dH clZ 0.33 If A ( t ) designates the disturbance on available, better predictions are to be

0.33 - = -0.33K - - __ Z expected.

dt dt T, the feed concentration a t the reactor inlet,

the disturbance on product concentration Numerical examples have been worked

The analogue circuit which represents out in this paper and especially in Part I

a t the outlet is (1 - e-kr)A(t - T ) and

these equations with a time scale changed the equation of the proportional-control in order to demonstrate clearly the

from hours to minutes is given as an loop is method of application of frequency-

illustration on Figure 8. The symbols of response analysis to continuous-flow

be found in reference 3.

+

the circuit diagram are standard and may A(t) K ( 1 - e-k‘)A(t - T ) = 0 (25) reactions. These should also serve to

clarify the characteristics of the chemical

This circuit was used to determine the where K is the characteristic constant of reactor control process itself. It was

response of the controlled reactor to a the proportional controller. Equation (25) shown for example that such important

change in feed temperature is of the difference type, and methods of factors as temperature-sensitive rates of

solution are well known. Thus introducing reaction can be readily analyzed by these

2, = 1°C. a solution methods.

for three different settings of the con-

troller characteristics K and T I . The A ( t ) = e*‘

NOTATION

results are given on Figures 9, 10, and 11. into Equation (25) results in a charac-

Figure 9 represents a case with low teristic equation which gives the values See page 256.

damping ( K = 1, T I = 1/10 min.). The of s for which e * t is a solution of (25):

system oscillates around the steady state. LITERATURE CITED

Figure 10 represents a more damped case

( K = 4, T I = K min.), which would be

+

1 K ( l - e-kT)e-sT= O 1. Eckman, D. P., “Principles of Industrial

acceptable in practice. The system It is found that Control,” John Wiley and Sons, Inc.,

represented in Figure 11 is overdamped New York (1948).

2. James, H. M., N. B. Nichols, and R. 8.

( K = 5, T I = M min.) but may still be Phillips, “Theory of Servomechanisms,”

acceptable in practice. Such examples McGraw-Hill Book Company, Inc.,

could be multiplied for various combina- New York (1947).

tions of controller types. Discussion of where X may take any integer value. The 3. Korn, G. A., and T. M. Korn, “Elec-

them is easy, and they will not be system is stable if the exponential e” is tronic Analog Computers,” McGraw-Hill

developed further here. damped : Book Company, Inc., New York (1952)

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