Ind. Eng. Chem. Res.

1989, 28, 793-803 793

de Sedimentation des Suspensions dans les Recipients Inclines.
Keijo J . Med. 1937, 8, 256-296.
Ponder, E. On Sedimentation and Rouleaux Formation. Q. J . Exp.
Physiol. 1925, 15, 235-252.
Schaflinger, U. Influence of Nonuniform Particle Size on Settling
Beneath Downward-Facing Walls. Int. J. Multiphase Flow 1985,
1 1 , 783-796.
Zhang, X. Particle Classification for Dilute Suspensions Using In-
clined Settlers. M.S. Thesis, University of Colorado, Boulder,
1988.
Received for review August 9, 1988
Revised manuscript received January 30, 1989
Accepted February 17, 1989

Analysis and Algorithms for Multistage Separation Processes

Lakshmi N. Sridhar and Angelo Lucia*
Department of Chemical Engineering, Clarkson University, Potsdam, New York 13676

Multistage equilibrium separation processes involving binary homogeneous mixtures are analyzed.
For several sets of specifications, it is shown that these process models admit a unique steady-state
solution without the need for a constant molar overflow assumption or other energy balance or phase
equilibria simplifications. The steady-state model equations are analyzed directly, and the role of
homogeneity in determining solution uniqueness is clearly identified. The analysis is constructive
and gives insight into the behavior and development of algorithms for solving multistage separation
process model equations in both the binary and multicomponent cases. To illustrate this, convergence
results are established for direct substitution and certain Newton-like accelerated direct substitution
methods. Also, a new generalized Broyden acceleration technique is developed and used in the context
of a sum-rates algorithm to solve several example problems. Numerical results show that the proposed
acceleration method is comparable t o Newton acceleration and clearly outperforms traditional
Broyden acceleration. Other properties predicted by the analysis are also illustrated.

1. Introduction process involving binary homogeneous mixtures is ana-

In a recent paper, Doherty and Perkins (1982) provide
a very comprehensive review of research concerned with
the mathematical analysis of homogeneous distillation
processes. By homogeneous distillation, we mean one in
which both the liquid and vapor on any stage of the column
are stable with respect to phase splitting (see Van Dongen
et al. (1983) and Lucia (1986)). The paper by Doherty and
Perkins focuses on the issues of uniqueness and asymptotic
stability of steady-state solutions to a variety of distilla-
tions. Although many dynamic models are discussed, it
is the constant molar overflow (CMO) process that forms
the basis for most of the useful qualitative results in this
area, including those of Lapidus and Amundson (1950),
Acrivos and Amundson (1955), Rosenbrock (1960, 1962),
and Doherty and Perkins (1982). In particular, Doherty
and Perkins consider CMO multistage columns involving
binary homogenous mixtures and use both a simplified
dynamic model (without energy balances) and classical
linear stability analysis to prove that any distillation of
this type has a unique and stable steady-state solution.
Unfortunately, in many practical applications, the as-
sumption of constant molar overflow can be a poor one.
Furthermore, analysis of a dynamic model provides little
knowledge of the convergence behavior of algorithms used
for the steady-state simulation of multistage separators.
Therefore, in this work, the steady-state model is analyzed
directly and no simplifying assumptions are made with
regard to energy balance effects. Constructive proofs are
presented, and algorithms based on these proofs are im-
plemented and compared with existing methods.
This manuscript is organized in the following way.
Useful perturbation and eigenvalue-eigenvector results for
feed and temperature perturbations to a single-stage,
isobaric flash process are presented in section 2. In section
3, a multistage analogue of the isothermal, isobaric (T,P)
* Author to whom all correspondence should be addressed.
0888-588518912628-0793$01.50/0
lyzed. Here the column temperature and pressure profiles
are specified, and the stages of the separator are decoupled.
By use of the single-stage results, the separation process
model is put back together in the form of a classical fix-
ed-point iteration, which is shown to be globally convergent
to a unique solution in the two-phase region using the
contraction mapping principle. Other, more practical
specifications are analyzed in section 4. These specifica-
tions, which include fixing the reboiler and condenser
duties or specifying the reflux ratio and total bottoms flow
rate, are analyzed by constructing nonlinear maps using
the implicit function theorem and subsequently showing
that these maps are one-to-one and onto. In section 5,
insights provided by the analysis are used to construct
Newton-like accelerated direct substitution techniques for
solving separation process model equations. Convergence
and rates of convergence of these algorithms are also es-
tablished. Many numerical examples are presented in
section 6.
The main conclusions of this research are that 1. binary
separation processes involving homogeneous mixtures
admit unique steady-state solutions under a variety of
specifications; 2. for the specifications that were studied,
the assumptions of constant molar overflow and simplified
phase equilibrium are unnecessary, and solution unique-
ness is solely determined by the homogeneous nature of
the mixture; and 3. direct analysis of steady-state sepa-
ration process models gives useful insights concerning the
construction of reliable and efficient computer algorithms
for solving these model equations.
2. Useful Single-Stage Results
In this section, useful perturbation results for single-
stage, isobaric flash processes involving homogeneous
mixtures are collected because they are needed to analyze
the multistage separation process models that appear
throughout the remainder of the paper.
0 1989 American Chemical Society
794 Ind. Eng. Chem. Res., Vol. 28, No. 6, 1989
-- . "I
t
Figure 1. Flash process.
Consider the single-stage flash process shown in Figure
1. Assuming equilibrium stage behavior, one set of model
equations for this process is given by
/J- - gv = 0 (phase equilibrium)
f-I - v = 0 (conservation of mass)
FHF- L H L - VHv + Q = 0 (energy balance)
where pL and pv are vectors of component chemical po-
tentials in the liquid and vapor phases, respectively, and
f , 1 , and v are vectors of feed, liquid, and vapor phase
component molar flow rates. Furthermore, F , L , and V
are the total molar flow rates of the feed, liquid outlet, and
vapor outlet streams, respectively, and HF, HL,and H V
are the corresponding stream molar enthalpies. Finally,
Q is the heat duty to the flash drum. T and p are the
equilibrium temperature and pressure, respectively, and
n, is the number of components in the mixture. Note that
the quantities pL, pv, f , I , and v are vectors of length n,.
At constant temperature and pressure, the energy bal-
ance can be removed from the analysis. Differentiation
of the phase equilibrium equations gives the condition
V2G LAl - V2G 'Av = 0
where V2GL and V2GV are the Hessian matrices of the
Gibbs free-energy function for the liquid and vapor phases,
respectively.
For feed perturbations, say A f , conservation of mass
implies the simple relationship
AI = h f - Av
Substitution of eq 5 in eq 4 and some algebra give
Av = (V2GL + V2GV)-lV2GLAf
Furthermore, the matrix V2GL + V2GV is guaranteed to
be invertible at any nonazeotropic equilibrium point if the
mixture is homogeneous (see Lucia (1986)). Finally, the
definition M = (V2GL + V2GV)-'V2GL and eq 5 imply that
AV = MAf A I = (I - M ) h f
which gives the changes in vapor and liquid component
molar flow rates as a function of the feed perturbation at
the given temperature and pressure. Equation 7 is one of
the results that we will use many times in the subsequent
sections of this paper.
Straightforward application of the Gibbs-Duhem
equation for the liquid and vapor phases shows that the
matrices M and I - M both have eigenvalues of 0 and 1
in the binary case. To see this, note that the Gibbs-Duhem
equation for the liquid phase implies that M x = 0, which
in turn implies that (I - M ) x = x , where x is the equi-
librium liquid-phase composition. Similarly the Gibbs-
Duhem equation for the vapor phase and the fact that
1 - M = 1 - (V2G L + V2G V)-1V2G L =
(V2G + V2G V)-1V2G
give the conditions My = y and (I - M)y = 0 , where y is
the equilibrium vapor-phase composition. Thus, both
matrices M and I - M, which are 2 X 2 in the binary case,
have eigenvalues of 0 and 1 and share the same two ei-
genvectors; those eigenvectors are the equilibrium liquid-
and vapor-phase compositions x and y , respectively.
These relationships, which can be expressed compactly in
the form
Mx=O My=y
(I - M)x = x (I - M)Y = 0 (9)
will also be used frequently in subsequent sections of this
paper.
In order to include energy balance effects in the analysis
(1) of the multistage process, the changes in equilibrium phase
(2) molar flow rates as a function of arbitrary changes in
equilibrium temperature for a single-stage are also needed.
(3) These results, which are given in Lemma 4 in Lucia (1986,
p 1766), are simply restated here for convenient reference.
For an arbitrary scalar perturbation in equilibrium tem-
perature, say AT, the changes in equilibrium vapor and
liquid molar flows at constant pressure are given by
AV = (AT/T)(v~G~ + V2GV)-lAH
AI = - ( A T / T ) ( V 2 G L + V2GV)-'AR (10)
where A H = Hv - HL and HLand Hv are vectors of
component partial molar enthalpies for the liquid and
vapor phases, respectively. Equation 10 will be used re-
peatedly in analyzing multistage processes involving con-
denser and reboiler duty specifications.
Finally, we note that the results in this section carry over
to the multicomponent case with little or no modification.
In particular, eq 7,9, and 10 apply to the multicomponent
(4)
case with no modification. Furthermore, it is possible to
establish that all of the eigenvalues of M and I - M must
lie in the closed interval [0,1] for multicomponent homo-
geneous mixtures. This fact can be proved by using a
simple similarity transformation.
3. Multistage Binary Separation Processes
(5)
In this section, we show that any binary homogeneous
separation process, in which the temperature and pressure
profiles are specified, has a unique steady-state solution.
(6) As highlighted in section 1, to establish the result, we 1.
decouple the stages of the separator, 2. use the single-stage
results from the previous section to reassemble the mul-
tistage model in the form of a fixed-point iteration, and
3. show that this fixed-point iteration is globally con-
vergent to a unique solution in the two-phase region using
(7) the contraction mapping principle (Ortega and Rheinboldt,
1970, p 120).
Consider then the multistage separation process shown
in Figure 2, in which the temperature and pressure at each
stage are specified. The stages are numbered from top to
bottom, and although only one feed is shown in the figure,
the results that are established remain valid for any num-
ber of feeds and/or separator equipped with a total or
partial condenser.
The stages of the separator can be decoupled by
"tearing" the vapor input stream to each stage, 1 through
ns - 1. Application of the straightforward perturbation
analysis in section 2 (i.e., eq 7 ) to each stage in the sepa-
rator gives the equations
Avj = Mj[Avj+l + AI,-J j = 1, ..., ns (11)
(8) Alj = (I - Mj)[Avj+l + AIjJ j = 1, ..., ns (12)
 Ind. Eng. Chem. Res., Vol. 28, No. 6, 1989 795

Chart I
0
M3
0 ... 0
0 ... 0 1

x, Y
Figure 3. Tzy diagram for homogeneous binary mixture.

(see Figure 3). For binary, heterogeneous mixtures, ai-’

and Pj+’ need not be unique at stage temperatures below

v T8 *Pa

Figure 2. Multistage separation process.

18 Q8
the heterogeneous azeotropic temperature (see Figures 11
and 17 in Van Dongen et al. (1983)),and this observation
clearly indicates that homogeneity is a necessary condition
for guaranteeing solution uniqueness.
Define the transformation P by
-y z 0 ... 0 wp 0 ... 0
with appropriate modification for the end stages (Le., AZO 0 y3 ... 0 0 w3 ... 0
= 0 and Avns+l = 0 ) . 0 0 0
Elimination of AZ,, j = 1, ..., (ns - 1)by using eq 12 in P=
eq 11shows that the following fixed-point iteration, in the
variables vi, j = 2, ..., ns, can be constructed
-
Xk+’ = G(Xk) (13)
where wj = yj-’ - ( yj-lTyj/yjTyj )yj,j = 2, ..., ns and y j
where X = (vZT,vST,..., vWqTand where G’, the Jacobian denotes the vector of vapor-phase compositions on stage
matrix of the fixed-point iteration, is defined in Chart I. j in the separator. Note that P is invertible, and this gives
Each of the block matrices Mj and I - M j is n, X n, or 2 the similarity transformation
X 2 in the binary case. Note that eq 13 is a linear equation
in the case of binary mixture and a nonlinear equation in
the multicomponent case.
P-IG’P = [ A
0
@
0
]
To show that the fixed-point iteration defined by eq 13
converges to a unique solution, we apply the contraction where the matrix A is given by
mapping principle (Ortega and Rheinboldt, 1970, p 120).
One way to do this is to show that the spectral radius of
the Jacobian matrix, p(G’), satisfies
p(G’) = maxl,isn lAi(G’)l 1 (15)
To establish this bound, first note that, under the as-
sumption that a solution exists, the compositions on any
J
stage of the separator must satisfy where aj, Oj E (0,l) for each j as before and where each
block of the matrix P-lG’P is (ns - 1) X (ns - 1). Note
yj = aj-’xj-’+ (1 - aj-l)y,-l j = 2, ..., ns (16) that A is a nonnegative matrix.
xj = + (1 - fij+l)Yj+l I’= 1, (ns - 1) (17) Equation 19 shows that the eigenvalues of G‘ are the
Oj+lXj+l .*a,

same as the eigenvalues of the two (ns 1) X (ns - 1) -

where ajw1, fij+l E (0,l). For binary, homogeneous mix- diagonal blocks of P-’G’P. Thus, one-half of the eigen-
tures, the values of aj-l and fij+l in eq 16 and 17 are unique values of G’ are zero and p(G’) = p ( A ) . Application of
796 Ind. Eng. Chem. Res., Vol. 28, No. 6, 1989

Lemma 2.5 in Varga (1962, p 31), energy balance equations

gives the desired upper bound on p(A) because eq 20 shows

that each column of the nonnegative matrix A has a sum

/ )
that is strictly less than one for cyI, bj E (0,l). Conse- (0,P)solutions
quently,
d G ' ) = p(A) < 1 (22)
We are now in a position to use the contraction mapping
theorem, which is stated here for reference.
Contraction Mapping Theorem (Ortega and Rhe-
inboldt, 1970, p 120). A mapping G:D C R" Rn is -
contractive on a set Do C D if there is a k < 1 such that
Figure 4. Nonlinear energy balance mapping.

be shown to be invertible throughout the domain of in-

terest.
IlG(x) - G(y)II Ikllx- yII for all x, y E Do. Suppose G Consider the binary separation process shown in Figure
is contractive on a closed set Do C D and GDo C Do. 2 . The energy balance for the j t h stage in the process is
Then G has a unique fixed point. given by
To apply this theorem to the fixed-point iteration de-
fined by eq 13, let Do be the set intersection of the two- Ej(lj-1, vj+l,l j , vj, TI, 7 ' 2 ,
*a*,TnJ =
phase regions for each stage in the column and set k = F j H r + Lj-lHkl + Vj+1Hy+1- LjHiL - V,H.'
I 1 + Qj = 0
p(G'). If a two-phase solution to the column model exists, (23)
then Do must be a closed set. Furthermore, the condition
p(G') < 1 and Lemma 2.2.8 (Ortega and Rheinboldt, 1970, where Lj = ciljj,
V, = Civij,and all other quantities are
p 44) establish that G is contractive on Do. Consequently, defined as before. Application of the implicit function
the iteration defined by eq 13 converges to a unique fixed theorem to eq 23 gives
point in Do, and any separator involving a binary homo- AQj = -Lj-l(dH~-l/dTj-l)ATj_l-
geneous mixture and fixed temperature and pressure ns
profiles has a unique solution, provided those specified Hk1[ E (bLj-l/aTk)ATk]- Vj+l(dHy+l/dTj+l)AT,+l
-
temperature and pressure profiles admit any solution. k=l
Hy+1 [ (d v;+l/d Tk)A Tk] + Lj(dHjL/a Tj)AT; -t
4. Other Specifications k
Specifying the column temperature and pressure profiles
k
+ Vj(aHj"/dTj)ATj +
H;L[c(dLj/dTk)ATk]
has both analytical and computational value. As shown
in the previous section, it provides a useful way of ana- HjV[C(dvj/aTk)ATk](24)
k
lyzing the number of solutions to binary separation pro-
cesses using classical fixed-point theory. Furthermore, the Note that the term dLj/dTkand dVj/dTkappear in eq 24
analysis is constructive, and as we show in subsequent because of the material balance interlinking between ad-
sections, this is important in understanding the conver- jacent stages in the separator and that a change in any
gence behavior of certain equation-tearing algorithms for stage temperature affects the total liquid and vapor flow
multistage separation calculations (e.g., the Sujata sum- rates throughout the separator.
rates algorithm (Sujata, 1961)). However, specifying the From eq 24, it is readily apparent that in order to de-
temperature and pressure profiles is neither the usual way termining the quantity AQj, it is necessary to determine
nor the only way to fix the operation of a multistage sep- dLj/dTkand dVj/dTk. Using the single-stage results (i.e.,
arator. It is more common to specify the adiabatic oper- eq 7 and 10) in section 2, the Neumann lemma (Ortega and
ation of all intermediate stages in the separator and to fix Rheinboldt, 1970, p 45), the inverse nonnegativity of the
two additional end conditions such as the reboiler and matrix V2GL+ V2GV (Lucia, 1986, p 1768), and certain
condenser duties or the reflux ratio and total bottoms flow continuity properties, it is possible to establish the fol-
rate. Other end specifications are possible. lowing conditions
In this section, we study the steady-state behavior of
binary multistage separators involving the specifications aLj eo j l k aVj >O j 5 k
described above (i.e., adiabatic intermediate stages with -aT,
=( >O j > k -dTk
= ( <O j > k (25)
fixed reboiler and condenser duties or fixed reflux ratio
and total bottoms flow rate). To do this, nonlinear maps provided there are no retrograde effects or supercritical
from a set of specifications for which the solution is unique components throughout the separator. A derivation of the
to the set of specifications of interest are analyzed by using conditions given by eq 25 and all of the associated as-
the implicit function theorem. Uniqueness is preserved sumptions are presented in detail in Appendix A; however
if the nonlinear map is one-to-one or, equivalently, if the it is important to note that the property of inverse non-
Jacobian matrix of the map is invertible throughout the negativity can only be guaranteed for homogeneous mix-
domain of interest. We begin with the specifications of tures and, again, illustrates the pivotal role of homogeneity
reboiler and condenser duties. in determining solution uniqueness in the binary case.
4a. Reboiler and Condenser Duties. Define the set We are now in a position to show that the nonlinear map
of solutions in which the temperature and pressure profiles from the set of (2'9)solutions to the set of (QQ) solutions
in the separator are fixed as the set of ( T Q ) solutions and preserves uniqueness. Let Q = E ( T ) denote the set of
the set in which the heat duty to each stage and pressure stage energy balance equations for the separator. Appli-
profile are fixed as the set of (Q,P)solutions. Note that cation of the implicit function theorem gives
the stage energy balance equations define a nonlinear map A Q = JAT (26)
from the set of ( T Q )solutions to the set of ( 8 9 )solutions
(see Figure 4). It is this map whose Jacobian matrix must where A Q T = (AQ1,AQ2, ..., AQnS),ATT = (AT1,AT2, ...,

ATn ), and the elements of the Jacobian matrix, Jjk =
dQ.JbTk,are defined through eq 24 for j = 1, 2, ..., ns.
rfo establish that the Jacobian matrix in eq 26 is in-
vertible, note that
aQj/dTk = -sj-l,k[Lj-l(aHfil/aTk)] - Hfil(aLj-i/aTk) -
s j + l , k [ vj+l(aHT+l/ a Tk)1 - Hy+l(dVj+l/aTk) +
bjk[Lj(dHjL/dTk)+ vj(aHjV/dTk)]+ HjL(aLj/aTk)+
Hjv(a vj/dTk) (27)
where 6jk is the Kronecker delta defined by
1 j = k
,a, = (28)
0 j # k
Choose a reference state such that
HjL < 0 Hjv > 0 j = 1, 2, ..., ns
Use of eq 24 and 29 in eq 27 with j = k and the fact that
dH/aT > 0 shows that
aQk/aTk = -Hk-l(aLk-l/aTk) - Hx+i(avk+i/aTk)+
Lk(dHkL/dTk)+ vk(aHkV/aTk)+ HkL(dLk/dTk)
HkV(dvk/aTk)> 0 (30)
Note that each term in eq 30 is positive. Furthermore, it
is possible to show that
dQk+l/dTk -Lk(aHkL/dTk)- HkL(aLk/aTk)-
Hx+z(avk+z/aTk)+ Hk+,(aLk+l/aTk)
Hx+l(aVk+l/aTk)< 0 (31)
and
dQk-l/dTk = -Hk-z(aLk-,/aTk) -
vk(aHkV/dTk)- HkV(dVk/dTk)+ Hk-l(aLk-,/aTk) +
Hx-,(aVk-l/dTk) < 0 (32)
A detailed derivation of the conditions given by eq 31
and 32 can be found in Appendix B. Finally, using argu-
ments similar to those in Appendix B, it can be shown that
for j # k - 1, 12, and k + 1,
are relatively small quantities in comparison to the tri-
diagonal terms of the Jacobian matrix, even though they
can be either positive or negative.
Therefore, the Jacobian matrix in eq 26 can be written
in the form
J = S + T = S(I + S-lT) (34)
where S is an invertible tridiagonal M matrix and p(S-lT)
< 1. The matrix S is invertible because it is diagonally
column dominant. To see this, consider the energy balance
around the envelop enclosing stages k - 1, k, and k + 1,
which is given by
Lk-2Hk-2 - vk-1Hx-1 - Lk+lHk+l + vk+2Hx+2 + Qk-i
Qk + Qk+i = 0 (35)
Straightforward differentiation of eq 35 with respect to Tk
shows that
a(Qk-1 + Qk + Qk+l)/dTk = -Hk-z(aLk-,/aTk)
Hl-i(avk-i/aTk) Hk+i(aLk+i/aTk)-
Hx+2(aVk+z/aTk)> 0 (36)
Ind. Eng. Chem. Res., Vol. 28, No. 6, 1989 797
by application of eq 24 and 29. This, together with eq 30,
31, and 32, implies the condition
aQk/aTk > I(&!k-i/aTk)+ (aQk+i/aTk)l (37)
which shows that the matrix S is diagonally column dom-
inant and therefore invertible. Moreover, because the
quantities aQj/dTkfor j # k - 1, k , k + 1 are relatively
small with respect to the elements in the kth column of
S, it follows that p(S-'T) < 1 and that I + S-'T is inver-
tible. Therefore,
J-1 = (I + S-'T)-'S-' (38)
and this implies that the map from the set of (TQ) solu-
tions to the set of ( Q , P )solutions perserves uniqueness.
4b. Reflux Ratio and Total Bottoms Flow Rate
Specification. For separation processes like distillation,
(29) it is common to define the operation of the column by
fixing the pressure on all stages, by fixing the heat duty
to all intermediate stages (usually Qj = 0 for j = 2, ..., (ns
- 1)but this is not necessary), and by specifying the reflux
ratio and total bottoms (or distillate) flow rate denoted by
R and B, respectively. In fact, this set of specifications is
+ often referred to as the standard set of specifications. In
this section, it is shown that this standard set of specifi-
cations gives a unique solution. Uniqueness is established
by defining a nonlinear map from the set of (8s) solutions
to the set of solutions for which the reflux ratio, bottoms
flow rate, and heat duty to all intermediate stages are fiied
and by producing a contradiction if the Jacobian matrix
of that map exhibits singularity.
Define the latter set of solutions as the set of ( R , B )
solutions. Let AQj = 0, j = 2, ..., (ns - 1). Also let AR =
0 and AB = 0. Since AB = 0, the total mass balance
around the separator gives
AVl = 0 (39)
because the feed to the separator is fixed. Straightforward
differentiation of the defining equation for the reflux ratio
R = Ll/Vl (40)
implies the condition
A R / R = AL1/L1 - AVl/Vl (41)
which together with eq 39 and the fact that AR = 0 gives
AL1=0 (42)
Moreover, the mass and energy balance around stage 1
implies that both
AV2 = 0 (43)
and
AQ1 = 0 (44)
If AQns = 0, then we are done because this means that the
Jacobian matrix of the nonlinear map from the set of (QQ)
solutions to the set of (R,B) solutions is nonsingular.
Therefore, suppose AQ,, # 0. Equations 39 and 42-44
together with the fact that AB = 0 and the energy balance
equation for the envelop enclosing stages 2 through ns
imply the condition
AQ, # 0 for a t least one j = 2, ..., (ns- 1) (45)
However, this is a contradiction since the specifications
demand that all intermediate stage heat duties remain
fixed. Consequently, AQ, = 0, the map from the set of
( Q P )solutions to the set of (R$) solutions is nonsingular,
and the standard set of specifications admits a unique
solution.
798 Ind. Eng. Chem. Res., Vol. 28, No. 6, 1989
5. Algorithms
In this section, we show that the preceding analysis can
be used to help understand the behavior of certain existing
algorithms for steady-state multistage separation process
calculations. It can also be used to construct new algor-
ithms. In particular, we show that the multistage TP
analysis in section 3 gives insight into the convergence of
the inner loop of sum-rates methods for absorbers, strip-
pers, and distillations of wide boiling mixtures (see Sujata
(1961)). Furthermore, it can be used to construct new
reliable and efficient Newton-like acceleration methods for
sum-rates algorithms. The analysis in section 4, on the
other hand, can be used to understand the convergence
behavior of the outer (temperature) loop in the sum-rates
method (see Sujata (19611, Friday and Smith (1964), and
King (1971)).
5a. Sum-Rates Algorithms. The sum-rates method
for absorber, stripper, and wide boiling distillation calcu-
lations was originally proposed by Sujata in 1961 and is
certainly well-known by now. The reader is referred to the
paper by Sujata (1961) as well as the book by King (1971,
p 529) for a description of the algorithm. For the purposes
of our discussion, it suffices to state that these algorithms
use fixed temperature and pressure profiles in an inner
loop and solve the phase equilibrium and mass balance
equations for the column (in any number of ways and to
a variety of desired accuracies). The outer loop consists
of using the energy balance equations and stage heat duty
specifications to adjust the temperature profile in the inner
loop. Several choices of inner loop tear stream variables
are possible, but certainly one set of variables is the vapor
component molar flow rates for each stage j = 2 , ..., ns.
Thus, the inner loop of the sum-rates method can be
written in the form of the fixed-point iteration given by
eq 13, where the associated Jacobian matrix, G ’ ( X ) ,is
given by eq 14. The outer loop can be handled by using
eq 26 and 34.
It is convenient to interpret direct substitution and
accelerated direct substitution methods in the context of
solving the system of equations
F ( X ) = X - G ( X )= 0 (46)
The values of Xk+l are defined by the iteration
Xk+’= Xk - Jk -‘F(Xk) (47)
where the Jacobian matrix J k is given by
Jk = 1 - G ’ ( X k ) (48)
Approximation of the matrix Jk by the identity matrix (by
assuming G’ = 0 ) at each iteration corresponds to direct
substitution, which is usually characterized as extremely
reliable but slow. Evaluation of the Jacobian matrix Jk
at each iteration defines Newton acceleration and gives a
local quadratic rate of convergence; however, in this con-
text, Jacobian evaluations can be expensive because de-
rivative information is most commonly available in implicit
form. Other acceleration techniques such as Wegstein
(1958) acceleration, dominant eigenvalue methods (Orbach
and Crowe, 1971; Crowe and Nishio, 1975), and traditional
Broyden acceleration (Boston and Britt, 1978) can also be
used to speed convergence.
5b. Direct Substitution. The analysis in section 3
shows that direct substitution of the inner loop is globally
convergent to a unique solution for any well-defined, bi-
nary homogeneous multistage separation process in which
the temperature and pressure profiles are specified. The
analysis is not restricted to stripper and absorber calcu-
lations but does show that, when applied to binary mix-
tures, the sum-rates method is globally convergent.
Furthermore, the Linear Convergence Theorem shows that
the rate of convergence is R linear with a convergence
factor equal to p(G’(X*)),where X * denotes the fixed
point. Proof of this theorem can be found in Ortega and
Rheinboldt (1970, p 301) and requires no modifications for
this application.
Unfortunately, the convergence results for direct sub-
stitution do not carry over to the multicomponent homo-
geneous case. Simple examples can be constructed for
which p ( G ( X * ) )> 1and thus show that direct substitution
cannot be guaranteed to converge in the multicomponent
case without additional restrictions.
5c. Newton Acceleration. The analysis in section 3
can be easily extended to show that Newton-accelerated
direct substitution is convergent to a unique solution by
applying Lemma 10.1.7 in Ortega and Rheinboldt (1970,
p 304) to the Newton fixed-point iteration defined by eq
47. In this case, we define GN(X)as the right-hand side
of eq 47, and straightforward differentiation of eq 47 shows
that
G’N(X) = I - ( I - G’)-’[I- G ’ ] = 0 (49)
because G’ is a constant matrix in the binary case. In
practice, this means that Newton’s method converges in
one acceleration step in the absence of rounding error.
5d. Quasi-Newton Acceleration Methods. Because
of the fact that p(G’(X*))> 1 for direct substitution can
occur, we have also considered a variety of Newton-like
acceleration methods for sum-rates algorithms. In this
section, it is shown that the analyses in sections 2 and 3
suggest quasi-Newton acceleration methods that have
outstanding convergence characteristics in the binary and
ternary cases.
In order to approximate J - l , we build approximations
to the blocks M,, j = 1, 2, ..., ns by using a generalized
Broyden updating strategy and by constructing G’ ac-
cording to eq 14. Each block M, is subject to the Gibbs-
Duhem and secant constraints given by eq 9 and 11, re-
spectively. Thus, the following least change secant up-
dating problem (see Dennis and Schnabel (1979)) can be
defined
min //AJ- A,IIF:A,Z, = R, (50)
where A, and A, are successive approximations to M, =
(V2GIL + V2Glv)-’V2GJL and where Z, and R, are n, x 3
matrices defined by
Z, = [ v I k +I,k+’,
l, sik] R, = [vik+l, 0, y I k ] (51)
where s,k = (Av,k-l + AIJ-lk)and ylk= AvJk. The solution
to this problem is given by
A, = A, + (R, - A,Z,)(ZJTZ,)-’ZJT (52)
Those familiar with quasi-Newton updating will recognize
the update defined by eq 52 as a generalized Broyden
formula. It is a least change rank p correction to A, and
reduces to the usual Broyden update for p = 1. In our
applications, p = 2 or 3 in the binary or multicomponent
case, respectively.
For binary mixtures, Newton and generalized Broyden
accelerations are identical. This is true because each block
of G ’ ( X )is constant and uniquely determined by its as-
sociated pair of Gibbs-Duhem equations, and thus the
Jacobian matrix produced by the generalized Broyden
update is the true Jacobian matrix. For ternary mixtures,
it is possible to show that the generalized Broyden ac-
celeration technique is quadratically convergent. In this
case, each block of G ’ ( X ) ,while not constant, is uniquely
determined by its associated pair of Gibbs-Duhem equa-
tions and secant condition. Consequentlv, the matrix
 Ind. Eng. Chem. Res., Vol. 28, No. 6, 1989 799

Table I. Example Problem: Wide Boiling Binary Mixture Table 11. Example Problem: Narrow Boiling Binary
Problem Definition Mixture
vapor ideal condenser partial Problem Definition
liquid ideal feed sat liq, stage 2 vapor nonideal condenser partial
no. of 4 (1) n-butane, 40 kmol h-' liquid nonideal feed sat liq, stage 4
stages (2) n-decane, 30 kmol h-' no. of 8 (1)methanol, 40 kmol h-'
Dressure 4.013 X 10' Pa stages (2) water, 60 kmol h-'
starting values and solution pressure 1.013 X lo5 Pa
vo, kmol starting values and solution
stage T,K h-' v*, kmol h-' stage T,K y o , kmol h-' v *, kmol h-'
1 334 25 10 35.68 0.0494 1 339.05 3.28 0.91 37.86 0.91
2 370 25 10 36.84 0.0545 2 339.71 211.93 10.14 217.92 10.24
3 400 25 10 11.48 0.6215 3 340.98 211.50 17.50 214.49 19.50
4 430 25 10 3.53 0.5695 4 343.61 190.17 32.54 194.16 35.53
5 344.68 180.62 40.93 184.62 40.93
produced by the generalized Broyden update converges to 6 347.98 164.96 57.79 164.96 57.79
the true Jacobian matrix in the limit, and the asymptotic 7 356.77 113.27 99.95 113.27 99.95
rate of convergence is quadratic. 8 367.75 40.90 160.98 40.90 160.98

6. Preliminary Numerical Results Table 111. Example Problem: Wide Boiling Ternary
Mixture
In this section, some preliminary numerical results are Problem Definition
presented that compare direct substitution and a variety vapor ideal feed sat liq, stage 2
of Newton-like acceleration techniques on several example liquid ideal (1) propane, 40 kmol h-'
problems. Also, some of the properties predicted by the no. of stages 8 (2) n-butane, 30 kmol h-'
analysis are illustrated. pressure 4.013 X lo5 Pa (3) n-decane, 30 kmol h-'
6a. Problem-Solving Results. For the purpose of condenser Dartial
illustration, the convergence methods are compared in the starting values and solution
context of an inner loop of a sum-rates method, in which stage .'7 K y o , kmol h-' v*, kmol h-'
the temperature and pressure profiles in the separator are
specified. Thus, the corresponding iteration is defined by 1 310 25 20 10 39.98 29.24 0.02
2 350 25 20 10 40.38 30.22 0.46
eq 47. The acceleration techniques studied include New- 3 370 25 20 10 4.96 8.78 0.22
ton and traditional Broyden accelerations, as well as the 4 390 25 20 10 2.20 8.30 0.39
new generalized Broyden acceleration technique developed 5 420 25 20 10 0.93 6.72 0.87
in this work. These convergence methods are defined as 6 440 25 20 10 0.33 3.93 0.97
follows: 7 470 25 20 10 0.15 2.73 1.91
1. Direct Substitution (DS). Jk = I for each iteration 8 495 25 20 10 0.04 1.15 2.52
k in eq 48. Table IV. Example Problem: Narrow Boiling Ternary
2. Broyden Acceleration (BA). The matrix Jk-l is Mixture
approximated directly using the inverse Broyden update
Problem Definition
and traditional secant information. vapor non idea 1 feed sat liq, stage 1
3. Newton Acceleration (NA). Each block of the liquid nonideal (1)methanol, 25 kmol h-'
matrix G'(X) in eq 14 is evaluated using analytical de- no. of stages 6 (2) benzene, 40 kmol h-'
rivative information. The Jacobian matrix is computed Dressure 1.00 x io5 Pa (3) n-hexane, 35 kmol h-'
by using eq 48. starting values and solution
4. Tridiagonal Newton Acceleration (TNA). Only stage T,K vo,kmol h-' v*, kmol h-'
the tridiagonal blocks of G'(X) in eq 14 are evaluated.
5. Generalized Broyden Acceleration (GBA). Each 2 330.0 15.0 10.0 12.5 2.83 2.20 2.46
block of G'(X) is approximated by using eq 52. 3 332.0 7.5 7.5 7.5 1.22 1.17 1.28
6. Tridiagonal Generalized Broyden Acceleration 4 334.0 2.0 2.5 2.5 0.67 0.82 0.88
5 336.5 0.5 1.0 1.0 0.37 0.65 0.69
(TGBA). Only the tridiagonal blocks of G'(X) are ap- 6 339.0 0.1 0.5 0.5 0.15 0.41 0.43
proximated by using eq 52.
Note that, for methods NA, TNA, GBA, and TGBA, the (see Crowe and Nishio (1975),Westerberg et al(1979), and
matrix G'(X) or its tridiagonal approximation must be Michelsen (1982)) because the corrections in the unknown
constructed and the corresponding Jacobian matrix must variables have a natural tendency to align with the ei-
be inverted, whereas for traditional Broyden acceleration genvector associated with the dominant eigenvalue of the
the inverse Jacobian matrix is approximated directly. Jacobian matrix. This causes near collinearity of the steps
There is also a provision in our computer program that and usually results in secant information that is of little
allows any specified number of direct substitution steps use. For Newton and generalized Broyden accelerations,
to be used prior to acceleration or between successive ac- on the other hand, acceleration was used on every iteration.
celeration steps. Finally, the convergence tolerance for the loop was IlVk"
The foregoing convergence methods were tested on a set - vkl12 < and all calculations were performed in
of separation problems involving both wide boiling and double-precision arithmetic on an IBM 4341 computer.
narrow boiling binary and multicomponent mixtures. A summary of the results for five separation problems
Problem definitions and solutions can be found in Tables is given in Table VI. The results in Table VI show that
I-V. All physical properties were calculated using the data the proposed generalized Broyden acceleration technique
and models given in Prausnitz et al. (1980). For Broyden is competitive with Newton acceleration. It usually re-
acceleration, two initial direct substitution steps were used, quires the same or only a few iterations more than Newton
and subsequent acceleration was used every fifth iteration. acceleration and clearly outperforms traditional Broyden
This strategy of delaying has been recommended by others acceleration.
800 Ind. Eng. Chem. Res., Vol. 28, No. 6, 1989

Table V. ExamDle Problem: Wide Boiling Four-ComDonent Mixture

Problem Definition
vapor ideal pressure 4.013 X lo5 Pa feed (1) propane, 25 kmol hW1
liquid ideal condensor partial (2) n-butane, 25 kmol h-'
no. of stages 10 feed sat liq, stage 2 (3) isobutane, 25 kmol h-l
(4) n-decane. 25 kmol h-l
starting values and solution
vo, kmol h-' v*, kmol h-I
stage T,K
1 330 20 30 20 24 24.99 24.56 24.78 0.13
2 350 20 30 20 24 25.09 24.74 24.92 0.46
3 370 25 20 10 24 2.57 6.07 5.03 0.22
4 385 25 20 10 24 0.97 4.86 3.46 0.28
5 400 25 20 10 24 0.42 4.08 2.55 0.39
6 420 25 20 10 24 0.18 3.28 1.85 0.61
7 440 25 20 10 24 0.08 2.30 1.20 0.82
8 460 25 20 10 24 0.03 1.54 0.76 1.07
9 480 25 20 10 24 0.02 0.92 0.44 1.37
10 495 25 20 10 24 0.01 0.37 0.18 1.18

Table VI. Comparison of Various Convergence Methods

iterations
mixture no. of stages DS -
BA NA TNA GBA TGBA
c4, G o 4 9 9 2 4 2 4
MeOH, H,O 8 50" 29 3 8 3 8
cs, c4, ClO 8 35 26 4 6 7 7
MeOH, C6H6, n-C6Hl, 6 13 13 4 5 5 5
cs,n-C,, i-C4, c,o 10 44 28 4 9 13 14
a Failed to reach convergence tolerance in 50 iterations.

Table VII. Coefficients of Convex Combinations perturbations AT, = 0.01 K for k = 1-4, the Jacobian
P matrix in eq 26 is given by
stage CY
- -
1 0.0444 69.75 -75.44 0.005 -4.56
2 0.0570 0.4401
3 0.1176 0.8170 J = lo2 -29.02 306.36 -32.25 -4.56
(54)
-0.824 -230.91 197.91 -26.73
4 0.8931
-
-0.739 0.0045 -165.65 158.37-
In order to reduce the storage requirements associated From this, it is easy to verify that the tridiagonal part (S)
with both Newton and generalized Broyden accelerations, of the Jacobian matrix is a diagonally column dominant
we studied the effect of approximating G ' ( X ) ,and there- M matrix and is invertible. Furthermore, for J = S + T,
fore J(X), by its block tridiagonal part. The results in the eigenvalues of S-'T are (-0.0589,0.0183, -1.849 X
Table VI show that this is, in general, a useful trade-off, 9.368 X lo*). Consequently, p(S-'T) = 0.0589, and the
especially for problems involving wide boiling mixtures. Jacobian matrix given by eq 54 is invertible.
Usually only a few additional iterations are required to
reach reasonable accuracy. Acknowledgment
6b. Illustration of Properties Predicted by Analy-
sis. Here we show that the bounds on the spectral radius This work was supported by the Office of Basic Energy
given by eq 21 are easily satisfied by separation process Science, U.S. Department of Energy, under Grant DE-
problems involving binary mixtures. The first example FG02-86ER13552.
problem in Table VI is used for illustrative purposes. For
this problem, the coefficients of the convex combinations Nomenclature
given by eq 16 and 17 are shown in Table VII. The A = quasi-Newton matrix approximation
corresponding matrix A (see eq 20) is given by E = energy balance function

A =

1
0.0249
0.0036
0.0017
0.9430
0.0104
0.0050
0
0.8824
0.0126
] (53)
f = vector of feed component molar flow rates
F = total feed flow rate
G L, G v, G = total Gibbs free energy of liquid phase, of vapor
phase, of fixed-point function
H , H = molar enthalpy, partial molar enthalpy
J = Jacobian matrix
The eigenvalues of A are (0.1570, 0.5144 + 0.0761i, 0.5144 I = vector of liquid component molar flow rates
- 0.0761i) and thus p ( h ) = 0.5905. Note that two of the L = total liquid flow rate
eigenvalues of A are complex. It is easily verified that M = operator
P = pressure
0.0302 = minlSJSn (Chi,)< p(A) < Q = heat duty
1=1 R = real vector space, right-hand side of matrix constraint
n
equation
maxlSJSn(CA,) = 0.9584 T = temperature
1=1
v = vector of vapor component molar flow rates
Finally, it is illustrated that the Jacobian matrix in eq V = total vapor flow rate
26 can be written in the form given by eq 34 and that x = vector of liquid mole fractions
p(S-'T) < 1. For problem 1 (see Table I) and temperature X = unknown variables
 Ind. Eng. Chem. Res., Vol. 28, No. 6, 1989 801

y = vector of vapor mole fractions or right hand side of secant tk = Apflk + VkGk - Yk) (A6)
condition
Z = left-hand side of matrix constraint equation
-tk = - A v k X k + Lk(& - xk) (A7)

Greek Letters where AT, > o implies AVk > 0.

Equations A6 and A7 complicate the analysis because
a,fl = coefficients of convex combination
A = nonnegative matrix of the presence of the quantities and 4 . However,
6 = Kronecker delta because, for example, t k is a positive vector, the approxi-
A = eigenvalue mation
p = vector of chemical potentials tk A p f l k (A8) .
Subscripts must be qualitatively correct; otherwise, a contradiction
i = component index that t k is not a positive vector would occur. The same is
j = stage index true for
?.

Superscripts -tk -AvkXk (A9)

F = feed Consequently, the second term in eq A6 and A7 can be
k = iteration counter
L = liquid dropped, simplifying the analysis without affecting its
V = vapor qualitative outcome. However, while eq A8 and A9 can
be used for qualitative purposes, they will in general give
Appendix A: Effect of Temperature on the Total poor quantitative approximations.
Vapor and Liquid Flow Rates in a Multistage Let ATk > 0 and ATj = 0 for j # k. From eq 9,17, A2,
Separator A8, and A9, it follows that

I
In this appendix, we show that the conditions given by 0
eq 25 are satisfied in the absence of any retrograde effects
throughout the separator.
Application of eq 7 and 10 to each stage in the separator
and some algebra give the equation 0
r= Yh
A v = (I - G')-lr (AI) -(1 - @k+l)Yk+l
-(1 - @k+l)@k+lYk+Z
..., A v , ~ ) ~where
where A v = ( A v , ~ AvQT,
, , G' is defined
by eq 14, where r is the vector

Because p(G') < 1, the Neumann lemma (p 45 in Ortega

and Rheinboldt (1970)) gives
r=
(I - G')-' = I + G' + (G'), + (G')3+ ...
(All)
Application of the transformation P-l, where P is defined
J by eq 18, together with the use of eq A10 and A l l gives
the equation
and where
A V = [I + A + Az + ...I R (AW
t k = (V2GkL+ V2Gk")-'(&" - nkL)-
Tk
(A3) where AV = (AV,, AV,, ...,AV,,JT,A is defined by eq 20,
and the vector R is given by
and the subscript k denotes a stage index. Thus, eq A1
accounts for the change in vapor component molar flows
throughout the separator for perturbation in any stage
temperature through eq A2 and A3.
For any binary homogeneous mixture, the matrix V2GkL
+ V2GkVis inverse nonnegative (see p 1768 in Lucia
(1986)). Furthermore, in the absence of retrograde effects
and supercritical components in the separator, the vector
nk" - BkLis a positive vector. Consequently for AT, >
0, the vector tk, which represents the change in the vapor
component molar flow rates for stage k,is a positive vector.
Also note that the corresponding change in liquid molar Approximation of each element of the matrix-vector
flow rates for stage k is - t k , which is a negative vector (see product in eq A12 by the first nonzero term, which is also
p 1766 in Lucia (1986)). the dominant term, shows that
It is more convenient to express the vectors tk and - t k

!
in the form
tk = p&k - vflk (-44)
(1 - a k - Z ) ( l - ak-1)
-tk = i k 2 k - LkXk (A5)
AV = Apk 1 + ak-1(1 - @k) - (1 - ak)(l - @ k + l ) (A141
where p k , i k , j j k , and are the total vapor flow rate, liquid - ak-l@k)(l- @ k + l ) - ak(1 - @ k + d 2 -
flow rate, vapor composition, and liquid composition as- (1 - ak+l)bk+l(l - @k+2)
sociated with stage k that result from the temperature
perturbation AT,. For sufficiently small AT,, it follows
that
802 Ind. Eng. Chem. Res., Vol. 28, No. 6, 1989

Observe that for j = 2, 3, ..., ( k - 1) Similar application of eq 11 and 12 to stage ns - 2 and use
k-1 of eq B5 and B6 gives
avj/aTk = A v k ( n , ( l - ai))> 0 (A151 G s - 2 = [I - (1- Mns-~)M,B-iBns-i,ns-21-1(I
-
I =I

M”s-2)A1n,-3 = Ans-2,ns-3(I - Mns-2)Alns-3 039)

because all aiE (0,l). Furthermore,
and
avk/aTk = A V k ( a k - i ( l - Pk) + a k + P k + l ( l - a h ) ) > 0
(-416) Avns-2 = MnS-2[1 + Mns-lBns-l,ns-~Ans-~,ns-31 X
(1 - Mns-2)AIns-3 = MnS-2Bns-2,ns-3Alns-3
since (Yk-1, a k , P k E (0,l). Finally, for j > k
Continuing in this manner, we obtain the expression
Avk+2 = Mk+2Bk+2,k+lAlk+l
= Mk+PBk+P,k+lAk+l,k(I - Mk+l)Alk (B11)
However, Taylor series expansion of Alk in eq B11 shows
that
A l k = ( t k - L k ) X k + J!/k(kk - x k ) = h L k X k + L k ( k k - x k )
(BW
since all a, /3 E (0,l). Consequently, eq A15-Al7 show that
where the quantities t k and k k are the total liquid flow rate
and composition associated with stage k at Tk ATk. Use +
of eq 17 and subsequent substitution of eq B12 in eq B11
gives
The partial derivatives d L j / d T k can be analyzed in a sim-
ilar manner and show that Avk+?Yk+2 = [GkPk+l +
Lk(bk+l - Pk+l)lMk+2Bk+2,k+lAk+l,kXk+l
where the quantity in brackets is a scalar quantity.
The results in hppendix A show that for small pertur-
bations ATk > 0, L k < L k . Moreover, it can be shown that
which establishes the condition given by eq 25. P k + l > P k + l and that

Appendix B: Structure of the Jacobian Matrix tkPk+l LkPk+l (B14

for the ( T , P ) to ( Q ,P ) Mapping This follows from the fact that L k a 1 / T k and @k+l 0: T k
In this appendix, we show that for small ATk Consequently, the scalar quantity in eq B13
satisfies
UkPk+l + Lk(Pk+l - Pk+l) ;z 0 (B15)
and
aVk+z/aTk 0 (B16)
Taking partial derivatives of the energy balance equation
for stage k + 1 with respect to Tk gives
Application of eq 11 to stage k + 1 and the results in
Appendix A show that
aQk+i/dTk = [Hl+l(aVk+l/aTk) - Hl+2(aVk+2/dTk)l + Avk+lYk+l = AVk+i = Mk+l[Alk 4- A v k + , l
[-HkL(aLk/aTk) + Hk+i(aLk+i/ VTk)] - Lk(aHkL/aTk) = Mk+l[ukXk + LkAXkI
(B3) =
k‘ [ - (‘_kPk+l +
Lk(Pk+l - Pk+l))lYk+l
The last term in eq B3 is negative. We show that the terms
in brackets are also negative.
Consider then the first term in brackets and begin by
comparing the quantities aVk+l/aTkand dVk+z/dTk. To
-
Since the term in parentheses in eq B17 goes to zero faster
than u k as ATk 0, it follows that
l a v k +1/ a Tk I >> l a v k + 2 / a Tk I 0318)
do this, we use eq 11 and 12 recursively and traverse the
column from stage ns to stage k + 1. For stage ns,we have Moreover, if Hi+l and Hi+2are of the same magnitude,
then eq B18 implies
Avns = MnsAlns-1 (B4)
IH’a;1(8v k + 1/ Tk) I > I H 1 + 2 (av k + 2 / d T k ) I (B19)
For stage ns - 1 application of eq 11and 12, use of eq B4
and some algebra give the relationships This together with eq 25 and 29 shows that the first term
in brackets in eq B3 is negative. Similar arguments can
Alns-1 = Ans-l,ns-dI - Mns-JAlnS-2 035) be used to show that the second term in eq B3 is also
negative and consequently that the inequality given in by
and eq B1 is valid. Finally, the inequality given by eq B2 can
Avns-1 = Mns-1Bns-l,ns-2ALns-2 (B6) be established in exactly the same manner.

where Literature Cited

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1533-1541.
and Boston, J. F.; Britt, H. I A Radically Different Formulation and
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Magnetic Filter for Solids: Theory and Experiment
Shoichi Kimura and Octave Levenspiel*
Chemical Engineering Department, Oregon State University, Corvallis, Oregon 97331
This paper introduces a new type of filter for removing ferromagnetic solids from a flow stream,
one that freezes the particles to the tube wall by magnetic forces alone. Basic theory is developed
t o tell how to find the parameters of any given system, and experiments are run to verify the theory.
This is a report on a new type of filter that is designed
to remove ferromagnetic solids from a slurry flowing in a
tube or pipe. It acts by creating a strong magnetic field
in the flow channel so as to freeze the solids to one side
of the flow channel. Solids build up there, and eventually
the flow channel becomes so restricted that no more solids
can be captured. It is then time to turn off the magnetic
field, which releases the captured solids to a collection
chamber. The whole operation is then repeated.
Asema (1988) presently offers such filters for removing
suspended magnetic fines from industrial wastewaters.
Another use for this device is for recovering ferromagnetic
catalyst particles or catalyst particles having ferromagnetic
cores from fluid streams leaving slurry reactors. At the
beginning and close to the end of an operating cycle, a
small fraction of the flowing solids may escape the mag-
netic filter. Hence, if all the solids are to be recovered, the
magnetic filter will have to be followed with an ordinary
filter. Nevertheless, with this magnetic filter, the duty of
the mechanical filter will be greatly reduced because the
magnetic filter can hold a large amount of solid with only
a relatively small increase in pressure drop. In general,
low pressure drop is a special advantage of the magnetic
filter over its mechanic61 counterpart. This follows from
the fact that it has no mechanical obstruction in its flow
channel.
Theory
Consider a pair of activated electromagnetic pole pieces
snugly fitted to a paramagnetic tube through which is
flowing a slurry containing ferromagnetic particles, as
shown in Figure 1. With a high enough field intensity,
0888-5885/89/2628-0S03$01.50/0
803
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Received for review July 29, 1988
Revised manuscript received February 11, 1989
Accepted February 17, 1989
particles can be arrested at the pole pieces, and since the
magnetic flux density between the pole pieces is highest
when the air gap is smallest, particles collect there first.
Once a layer of particles is formed, the magnetic flux
density increases because of the increased permeability of
this solid layer.
The solid layer grows progressively while reducing the
cross-sectional area of the flow channel. This process
continues until the magnetic forces just balance the net
frictional and gravitational forces on the particles. This
progression is shown in Figure 2.
This section develops the basic theory which relates the
capture current and the quantity of solids captured with
the pole piece geometry, particle size, system geometry,
and operating conditions.
Balance of Forces. The pertinent forces influencing
the action of a magnetic filter are the magnetic force,
gravity, and hydrodynamic drag.
Let us focus attention on a spherical particle that is
touching a layer of already frozen particles. The net force
tending to sweep the particle downstream is the result of
gravity and drag, given by
where Cd is the drag coefficient and u is the mean velocity
of the slurry. In eq 1,j = +1 for upflow of slurry, and j
= -1 for downflow of slurry.
Opposed to this is the vertical component of the mag-
netic force, F,, acting on the particle, or
FZ = CfF, (2)
62 1989 American Chemical Society