PROCESS DESI GN AND CONTROL

Rigorous Graphical Targeting for Resource Conservation via

Material Recycle/Reuse Networks
M. M. El-Halwagi,* F. Gabriel, and D. Harell
Department of Chemical Engineering, Texas A&M University, 3122 TAMU, CollegeStation, Texas 77843-3122
Materi al recycl e/reuse i s one of the key strategi es i n reduci ng the consumpti on of fresh resources
i n the process i ndustri es. Over the past decade, several techni ques have been devel oped to reduce
the consumpti on of speci fi c materi al uti l i ti es such as water and hydrogen. To date, none of the
publ i shed techni ques provi des a noni terati ve, systemati c, and graphi cal techni que for i denti fyi ng
a target for mi ni mum usage of the fresh resources ahead of detai l ed desi gn of the recycl e/reuse
network. I n thi s paper, we present a ri gorous graphi cal targeti ng approach to mi ni mi ze the use
of fresh resources by usi ng segregati on, mi xi ng, and di rect recycl e/reuse strategi es. Fi rst, the
probl em i s formul ated mathemati cal l y to provi de a systemati c basi s for i ts sol uti on. Then,
dynami c programmi ng techni ques are empl oyed to deri ve the mathemati cal condi ti ons and
characteri sti cs of an opti mal sol uti on strategy. These condi ti ons and characteri sti cs are
transformed i nto a graphi cal form that can be readi l y used to i denti fy ri gorous targets for
mi ni mum usage of fresh resources. The graphi cal techni que i s al so useful i n l ocati ng a materi al
recycl e/reuse pi nch poi nt, whi ch provi des i nsi ghtful i nformati on on the use of fresh resources,
the di scharge of unused materi al s, and the rel ati onshi ps between process streams (sources) and
uni ts (si nks). Several test probl ems are sol ved to i l l ustrate the ease, ri gor, and appl i cabi l i ty of
the devel oped targeti ng techni que.
Introduction
Processi ng faci l i ti es are characteri zed by the use of
enormous amounts of materi al resources. Such depl eti on
of natural resources poses many economi c, soci al , and
ecol ogi cal chal l enges. Consequentl y, the process i ndus-
tri es have pursued materi al conservati on as a key
approach toward market competi ti veness and sustai n-
abi l i ty. Several strategi es can l ead to materi al conserva-
ti on, i ncl udi ng materi al recycl e/reuse, materi al substi -
tuti on, reacti on al terati on, and process modi fi cati on.
Over the past decade, several desi gn techni ques have
been devel oped to mi ni mi ze the usage of fresh resources
usi ng network synthesi s and anal ysi s. I n 1989, El -
Hal wagi and Manousi outhaki s
1
i ntroduced the probl em
of synthesi zi ng mass exchange networks (MENs) that
seeks to transfer certai n speci es from a set of ri ch
streams to a set of l ean streams. They proposed sys-
temati c composi te representati ons to i denti fy targets for
the maxi mum extent of mass exchange among process
streams and mi ni mum usage of external l ean streams.
The synthesi s of MENs has been successful l y used i n
waste recovery/separati on appl i cati ons. An i mportant
vari ati on of MENs, wastewater mi ni mi zati on, was
i ntroduced i n 1994 by Wang and Smi th.
2
They proposed
a graphi cal approach to target the mi ni mum freshwater
consumpti on and wastewater di scharged by the transfer
of contami nants from process streams to water streams.
Both methods use the appl i cati on of process uni ts as
mass exchange appl i cati ons, and they rel y on the basi c
pri nci pl e of concentrati on dri vi ng force. Al though some
process uni ts are mass exchangers, there are many
water usage/wastewater di scharge probl ems that are
not i ncl uded i n the MEN-based wastewater mi ni mi za-
ti on approach of Wang and Smi th.
2
I n MEN-based
probl ems, the l ean stream (e.g., water) acqui res a
certai n l oad of mass and then proceeds to be potenti al l y
used i n other uni ts. There are several cases that are
not di rectl y covered by such scenari os. For i nstance, the
l ean streams mi ght not l eave the uni ts as di sti nct
streams (e.g., due to mi xi ng, reacti on, etc.). Another
exampl e i s when a stream moves i nto an unrecoverabl e
state. For i nstance, water mi ght l eave i n a product
stream or wet cake where i t wi l l not be recovered. A
thi rd case i s when the l ean stream (e.g., water, hydro-
gen, etc.) i s generated i n the process. I n thi s case, no
l ean stream enters the uni t, but a l ean stream does
l eave the uni t.
Dhol e et al .
3
and El -Hal wagi and Spri ggs
4
i ndepen-
dentl y observed the l i mi tati ons of mass exchange net-
works on the appl i cati on of wastewater and freshwater
mi ni mi zati on methods. Many i ndustri al processes usi ng
water and produci ng wastewater do not meet the
cri teri a of mass exchange uni ts. I nstead, they addressed
the probl em of water usage and di scharge through a
source (suppl y) si nk (demand) representati on. Thi s
probl em wi l l be referred to as the recycl e/reuse probl em
and i s the focus of thi s paper. The objecti ve of the
recycl e/reuse probl em i s to al l ocate vari ous process
sources (or streams) to si nks (uni ts that can empl oy the
sources) so as to mi ni mi ze the consumpti on of the fresh
resource (e.g., freshwater). Dhol e et al .
3
created a new
graphi cal techni que that represents concentrati on ver-
sus fl ow rate and creates a suppl y composi te and a
demand composi te. When the two composi tes touch, a
bottl eneck (water pi nch) i s i denti fi ed and can be el i mi -
* To whom correspondence shoul d be addressed. Tel .: (979)
845-3484. Fax: (979) 845-6446. E-mai l : El -Hal wagi @tamu.edu.
4319 I nd. Eng. Chem. Res. 2003, 42, 4319-4328
10.1021/i e030318a CCC: $25.00 2003 Ameri can Chemi cal Soci ety
Publ i shed on Web 08/14/2003
nated by mi xi ng of source streams. Even though the
methodol ogy had great i mpact on the concept for water
mi ni mi zati on, i t has i ts drawbacks. The key l i mi tati on
i s that Dhol e et al .
3
di d not provi de a systemati c method
for el i mi nati on of pi nch poi nts by mi xi ng. To overcome
thi s l i mi tati on, Pol l ey and Pol l ey
5
proposed a set of rul es
for sequenci ng mi xi ng and recycl e opti ons. Addi ti onal l y,
Sori n and Bedard
6
proposed an al gebrai c method, cal l ed
the evol uti onary tabl e, that i s based on l ocati ng the
gl obal pi nch based on mi xi ng source streams wi th cl oser
concentrati on di fferences fi rst, and then goi ng to the
stream wi th the next nearest concentrati on. However,
the evol uti onary tabl e al so has i ts negati ve aspects.
When the process has more than one gl obal pi nch, thi s
approach can have drawbacks for process modi fi cati ons
by not di scoveri ng the true gl obal pi nch, as i ndi cated
i n a study by Hal l al e.
7
To address thi s l i mi tati on,
Hal l al e
7
attempted to sol ve al l of the aforementi oned
l i mi tati ons by coupl i ng the water surpl us di agram wi th
a graphi cal representati on of puri ty versus fl ow rate
(si mi l ar to the Dhol e et al .
3
graphi cal representati on).
The i dea of surpl us was fi rst devel oped by Al ves
8
for
the appl i cati on of hydrogen recovery systems i n refi ner-
i es. Both methods rel y on extensi ve cal cul ati ons to
create the surpl us di agram to target mi ni mal consump-
ti on of resources (water i n the case of Hal l al e
7
and
hydrogen i n the case of Al ves and Towl er
9
). Al so, the
devel opment of thi s methodol ogy i s qui te tedi ous be-
cause many cal cul ati ons are requi red, and there i s a
dependence of two graphs to sati sfy fl ow rate and
composi ti on for the source-si nk structure.
Mathemati cal programmi ng techni ques have al so
been used to sol ve the recycl e/reuse probl ems (Savel ski
and Bagajewi cz
10,11
), i ncl udi ng mul ti component systems
(e.g., Al va-Argaez et al .,
12
Benko et al .,
13
and Dunn et
al .
14,15
). Addi ti onal l y, si mi l ar methods have been devel -
oped for unsteady-state and batch systems (e.g., Wang
and Smi th,
16
Al mato et al .,
17
and Zhou et al .
18
).
Notwi thstandi ng the useful ness of the aforementi oned
desi gn procedures for the recycl e/reuse probl em, none
of them presents a si ngl e-stage, systemati c, and graphi -
cal targeti ng procedure. I ndeed, these techni ques can
be broadl y cl assi fi ed i nto two categori es: i terati ve
targeti ng and detai l ed network desi gn. I terati ve target-
i ng i nvol ves the use of mul ti step graphi cal approaches
to evol ve the usage of fresh resource i nto a mi ni mum
target. On the other hand, detai l ed network desi gn
i nvol ves the matchi ng of sources and si nks and the
confi gurati on of a network that provi des mi ni mum
usage of the fresh resource. Mul ti pl e networks can be
confi gured to gi ve the same mi ni mum usage of fresh
resource. I n many cases, i t i s i mportant to i denti fy the
target for mi ni mum usage of fresh resources i n a
systemati c way, ahead of detai l ed desi gn and wi thout
commi tment to the fi nal network confi gurati ons.
The purpose of thi s paper i s to i ntroduce a systemati c,
si ngl e-stage, and graphi cal method for ri gorousl y tar-
geti ng mi ni mum usage of fresh resources through
materi al recycl e/reuse techni ques. Fi rst, we descri be the
probl em through an opti mi zati on formul ati on. Then, we
use dynami c programmi ng techni ques to determi ne the
mathemati cal condi ti ons and characteri sti cs of an op-
ti mal sol uti on strategy. These condi ti ons and charac-
teri sti cs are transformed i nto a graphi cal techni que that
can be readi l y used to i denti fy ri gorous targets for
mi ni mum usage of fresh resources. The devi sed vi su-
al i zati on tool i s a novel graph of l oad versus fl ow rate
constructed i n a way that yi el ds the ri gorous target
wi thout i terati ons. The graphi cal techni que i s al so
useful i n l ocati ng materi al recycl e/reuse pi nch poi nts,
whi ch provi des i nsi ghtful i nformati on on the use of fresh
resources, the di scharge of unused materi al s, and the
maxi mum extent of mass i ntegrati on among process
streams (sources) and uni ts (si nks). The broad ap-
pl i cabi l i ty and ease of i mpl ementati on of thi s new
method are shown and veri fi ed through the sol uti on of
several previ ous case studi es publ i shed i n earl i er l i t-
erature.
ProblemStatement
Consi der a process that consi sts of a set of process
si nks and a set of process sources descri bed as fol l ows:
The set of process si nks (uni ts) i s desi gnated SI NKS
) {j ) 1, 2, ..., N
si nks
}. Each si nk requi res a feed wi th a
gi ven fl ow rate, G
j
, and a composi ti on of a si ngl e
targeted speci es, z
j
i n
, that sati sfi es the fol l owi ng con-
strai nt
where z
j
mi n
and z
j
max
are gi ven l ower and upper bounds,
respecti vel y, on admi ssi bl e composi ti ons to uni t j.
The set of process sources, desi gnated SOURCES )
{i ) 1, 2, ..., N
sources
}, can be recycl ed/reused i n process
si nks. Each source has a gi ven fl ow rate, W
i
, and a gi ven
composi ti on, y
i
.
Al so avai l abl e for servi ce i s a fresh (external ) resource
that can be purchased to suppl ement the use of process
sources i n si nks.
Gi ven the above-descri bed process, the objecti ve i s to
devel op a noni terati ve graphi cal procedure that deter-
mi nes the target for mi ni mum usage of the fresh
resource.
ProblemRepresentation
The fi rst step i n the anal ysi s i s to represent the
probl em through a source-si nk representati on, as
shown i n Fi gure 1 (e.g., El -Hal wagi
19
). Each source i s
spl i t i nto fracti ons (of unknown fl ow rate) that are
al l ocated to the vari ous si nks. An addi ti onal si nk i s
pl aced to account for unrecycl ed/unreused materi al . Thi s
si nk i s referred to as the waste si nk. The fresh
resource i s al so al l owed to spl i t and i s al l ocated to al l
si nks but the waste si nk.
Figure 1. Source/si nk al l ocati on.
z
j
mi n
e z
j
i n
e z
j
max
for j ) 1, 2, ..., N
si nks
(1)
4320 I nd. Eng. Chem. Res., Vol . 42, No. 19, 2003
Opmization Formulation
The opti mi zati on probl em i s formul ated as fol l ows
subject to the fol l owi ng constrai nts
where F
j
i s the amount of fresh resource fed to the jth
si nk. Consi deri ng a fresh source, whi ch has no i mpuri -
ti es, we obtai n the fol l owi ng component materi al bal -
ance around the mi xi ng poi nt of the feed to the si nk
As an asi de, note that the same equati on can be appl i ed
even when the fresh source has a nonzero content, y
fresh
,
of the pol l utant by defi ni ng composi ti ons as di fferences
based on the fresh composi ti on, i .e.
Nonnegati vi ty of each fracti on of source al l ocated to a
si nk and of fl ow of fresh resources
The foregoi ng formul ati on i s a l i near program that
can be sol ved gl obal l y to i denti fy the opti mal target and
source-si nk matches. However, as menti oned earl i er,
our objecti ve i s to devel op a graphi cal techni que that
can provi de val uabl e i nsi ghts i nto the key characteri s-
ti cs of the probl em and not just i ts sol uti on. These
i nsi ghts can gui de many desi gn and operati ng deci si ons
that extend beyond fi ndi ng a speci fi c sol uti on.
Derivation of Optimality Conditions via
Dynamic Programming
Dynami c programmi ng i s an opti mi zati on techni que
that i s parti cul arl y useful for handl i ng mul ti stage
operati ons. I t i s based on Bel l mans pri nci pl e of opti -
mal i ty,
20
whi ch states that an opti mal pol i cy has the
property that, whatever the i ni ti al state and the i ni ti al
deci si on are, the remai ni ng deci si ons must consti tute
an opti mal pol i cy wi th regard to the state resul ti ng from
the fi rst deci si on. I n dynami c programmi ng, three
el ements must be defi ned:
(1) The fi rst el ement i s the stage (j), whi ch represents
the porti on of the probl em for whi ch a deci si on i s to be
made. Hence, we choose each si nk as a stage (Fi gure
4). We rank the si nks i n ascendi ng order of maxi mum
al l owabl e composi ti on (i .e., z
1
max
e z
2
max
e z
j
max
e
z
N
si nks
max
).
(2) The second el ement i s the return functi on for each
stage, whi ch represents the objecti ve functi on associ ated
wi th that stage. For our case, thi s corresponds to the
fl ow rate of the fresh source used i n that stage (i .e., F
j
).
(3) The fi nal el ement i s the state of each stage (R
j
),
whi ch represents the connecti on between succeedi ng
stages such that, when each stage s i s opti mi zed
separatel y, the resul ti ng deci si on i s automati cal l y fea-
si bl e for the rest of the stages. Here, we defi ne the state
of the jth stage as the remai ni ng (unused) fl ows of the
sources up to that stage. Therefore
where
Let us start by deri vi ng the opti mal i ty condi ti ons for
the fi rst subprobl em correspondi ng to stage j ) N
si nks
subject to
Nonnegati vi ty of each fracti on of source al l ocated to
a si nk and of fl ow of fresh resources i mpl i es
Figure 2. Spl i tti ng of sources.
Figure 3. Mi xi ng of sources at i nl ets of si nks.
mi ni mi ze consumpti on of fresh resource )

j)1
N
si nks
F
j
(2)
Spl i tti ng of the sources (Fi gure 2)
W
i
)

j)1
N
si nks
w
i,j
+ w
i,waste
for i ) 1, 2, ..., N
sources
(3)
Mi xi ng of the jth si nk (Fi gure 3)
G
j
) F
j
+

i)1
N
sources
w
i,j
for j ) 1, 2, ..., N
si nks
(4)
G
j
z
j
i n
)

i)1
N
sources
w
i,j
y
i
for j ) 1, 2, ..., N
si nks
(5)
z
j
mi n
e z
j
i n
e z
j
max
for j ) 1, 2, ..., N
si nks
(1)
z
j
i n
e z
j
i n,actual
- y
fresh
and y
i
) y
i
actual
- y
fresh
w
i,j
g 0 for i ) 1, 2, ..., N
sources
and
j ) 1, 2, ..., N
si nks
(6)
F
j
g 0 j ) 1, 2, ..., N
si nks
(7)
R
j
) [R
1,j
, R
2,j
, ..., R
i,j
, ..., R
N
sources
,j
] (8)
R
i,j
) W
i
-

j)1
j-1
w
i,j
for i ) 1, 2, ..., N
sources
(9)
mi n F
N
si nks
(10)
G
N
si nks
) F
N
si nks
+

i ) 1
N
sources
w
i,N
si nks
(11)
G
N
si nks
z
N
si nks
i n
)

i)1
N
sources
w
i,N
si nks
y
i
(12)
z
N
si nks
mi n
e z
N
si nks
i n
e z
N
si nks
max
(13)
R
i,N
si nks
) W
i
-

j)1
N
si nks
-1
w
i,j
for i ) 1, 2, ..., N
sources
(14)
I nd. Eng. Chem. Res., Vol . 42, No. 19, 2003 4321
To deri ve the opti mal i ty condi ti ons for F
Nsi nks
, we need
to i denti fy opti mal parametri c val ues for z
N
sources
i n
and
w
i,Nsi nks
. Let us start wi th the case of a si ngl e process
source, i, mi xed wi th a fresh stream. The program then
becomes
subject to
By combi ni ng constrai nts 19 and 20, we obtai n
Hence, we can state the fol l owi ng si nk-composi ti on
rul e: To mi ni mi ze F
Nsi nks
, the val ue of z
N
si nks
i n
shoul d be
maxi mi zed whi l e sati sfyi ng the nonnegati vi ty con-
strai nts for the fresh resource and for the ith source
and
Therefore, when these two nonnegati vi ty constrai nts
are sati sfi ed, we can al so state more speci fi cal l y the
fol l owi ng opti mal i ty condi ti ons
(i mpl yi ng usage of fresh resource, F
Nsi nks
> 0) and
(i mpl yi ng no usage of fresh resource, F
Nsi nks
) 0). These
two condi ti ons can be summari zed by the fol l owi ng
speci fi c si nk-composi ti on rul e: The opti mum i nl et com-
posi ti on of the si nk shoul d be set to i ts maxi mum l i mi t
unl ess no fresh resource i s to be used i n thi s si nk (i n
whi ch case, the i nl et composi ti on of the si nk i s that of
the recycl ed/reused sources).
I t i s worth poi nti ng out that, i f the recycl abl e source,
i, has been compl etel y recycl ed (i .e., R
i,Nsi nks
- w
i,Nsi nks
)
0), then the mi ni mum amount of fresh resource i s gi ven
by a si mpl e materi al bal ance
Consequentl y
Havi ng i denti fi ed the opti mal val ue of the i nl et
composi ti on to the si nk, we now turn our attenti on to
the opti mi zati on of w
i,Nsi nks
. Let us start wi th two sources
(i ) 1 and 2), where, accordi ng to our termi nol ogy, y
1
<
y
2
. Constrai nts 11 and 12 can be wri tten as
Combi ni ng these two equati ons, we obtai n
Because
then
Therefore, before consi deri ng the use of source i ) 2,
the use of source i ) 1 shoul d be maxi mi zed subject to
the avai l abi l i ty constrai nt of source i (nonnegati ve state
vari abl e)
Figure 4. Stage representati on.
w
i,N
si nks
g 0 for i ) 1, 2, ..., N
sources
(15)
F
j
g 0 for j ) 1, 2, ..., N
si nks
(16)
R
i,N
si nks
g 0 for i ) 1, 2, ..., N
sources
(17)
mi n F
N
si nks
(18)
G
N
si nks
) F
N
si nks
+ w
i,N
si nks
(19)
G
N
si nks
z
N
si nks
i n
) w
i,N
si nks
y
i
(20)
z
N
si nks
mi n
e z
N
si nks
i n
e z
N
si nks
max
(21)
R
i,N
si nks
) W
i
-

j)1
N
si nks
-1
w
i,j
for i ) 1, 2, ..., N
sources
(22)
F
N
si nks
) G
N
si nks
-
G
N
si nks
y
i
z
N
si nks
i n
(23)
F
N
si nks
g 0
R
i,N
si nks
- w
i,N
si nks
g 0
z
N
si nks
i n,opti mum
) z
N
si nks
max
for y
i
> z
N
si nks
max
(24a)
z
N
si nks
i n,opti mum
) y
i
for y
i
e z
N
si nks
max
(24b)
F
N
si nks
mi n
) G
N
si nks
- R
i,N
si nks
(25)
z
N
si nks
i n
)
R
i,N
si nks
y
i
G
N
si nks
(26)
G
N
si nks
) F
N
si nks
+ w
1,N
si nks
+ w
2,N
si nks
(27)
G
N
si nks
z
N
si nks
max
) w
1,N
si nks
y
1
+ w
2,N
si nks
y
2
(28)
F
N
si nks
) w
1,N
si nks
(
y
1
y
2
- 1
)
- G
N
si nks
(
z
N
si nks
max
y
2
- 1
)
(29)
(
y
1
y
2
- 1
)
< 0
F
N
si nks
opti mum
corresponds to w
1,N
si nks
) w
1,N
si nks
max
(30)
R
1,N
si nks
) W
1
-

j)1
N
si nks
-1
w
1,j
g0 (31)
4322 I nd. Eng. Chem. Res., Vol . 42, No. 19, 2003
I f thi s constrai nt becomes acti ve (i .e., R
1,Nsi nks
) 0), then
we move to maxi mi zi ng the usage of source i ) 2. By
i nducti on, one can reach the same resul t when more
than two process sources are consi dered.
We now proceed to the use of dynami c programmi ng
for the subsequent subprobl em (j ) N
si nks
- 1). Hence,
the fol l owi ng source pri ori ti zati on rul e can be stated:
For a gi ven si nk wi th several remai ni ng sources (unused
i n previ ous si nks), recycl e/reuse of sources i s pri ori ti zed
on the basi s of composi ti on, i n ascendi ng order. A source
i + 1 whose composi ti on i s hi gher than that of source i
shoul d not be used unti l source i i s ful l y recycl ed/reused.
The next subprobl em can be formul ated as fol l ows:
The objecti ve functi on i s
subject to
Because F
N
sources
opti mum
has al ready been i denti fi ed by sol v-
i ng the fi rst subprobl em, the sol uti on of the second
subprobl em yi el ds the same source pri ori ti zati on rul es
for opti mal i ty condi ti ons. Hence, for a si nk j and
avai l abl e process sources (wi th source i bei ng the stream
wi th the l owest composi ti on that has not been ful l y
consumed by previ ous si nks), we can state the fol l owi ng
two fundamental opti mi zati on rul es for mi ni mi zi ng the
use of fresh source:
Rule 1a. I f a si nk requi res the use of fresh source,
the i nl et composi ti on to the si nk shoul d be maxi mi zed,
i .e.
unl ess no fresh resource i s to be used i n thi s si nk (i n
whi ch case, the i nl et composi ti on of the si nk i s that of
the recycl ed/reused sources).
Mul ti pl y the above condi ti on by the fl ow rate of the
si nk, G
j
, and recal l that the pol l utant l oad enteri ng the
si nk, M
j
si nk
, i s defi ned as
Then, the foregoi ng rul e can be restated as fol l ows:
Rule 1b. I f a si nk requi res the use of fresh source,
the i nl et pol l utant l oad to the si nk shoul d be maxi mi zed,
i .e.
unl ess no fresh resource i s to be used i n thi s si nk (i n
whi ch case, the i nl et l oad of the si nk i s that of the
recycl ed/reused sources).
Rule 2. Maxi mi ze the recycl e/reuse of the avai l abl e
amount of source (i) unti l i t i s ful l y consumed; then
maxi mi ze the recycl e/reuse of the next source i n ascend-
i ng order of composi ti on (i + 1), and so on.
These rul es consti tute the basi s for the fol l owi ng
graphi cal procedure:
(1) Rank the si nks i n ascendi ng order of maxi mum
admi ssi bl e composi ti on
(2) Rank sources i n ascendi ng order of pol l utant
composi ti on, i .e.
(3) Start wi th the fi rst si nk, j ) 1. Recycl e/reuse the
fi rst source, i ) 1, unti l i t i s ful l y consumed or unti l the
maxi mum i nl et l oad to the si nk i s met. I f the fi rst source
i s ful l y consumed, recycl e/reuse the second source, i )
2, unti l i t i s ful l y consumed or unti l the maxi mum i nl et
l oad to the si nk i s met (whi chever comes fi rst), and so
on.
(4) Move on to the second si nk, j ) 2. Repeat the same
procedure as i n step 3, starti ng wi th the remai ni ng
source that has the l owest composi ti on. The same
procedure i s subsequentl y repeated for the rest of the
si nks i n ascendi ng order.
Fi gure 5 i l l ustrates the graphi cal procedure. The
graphi cal representati on i s a pl ot of pol l utant l oad
versus fl ow rate. For each si nk, the maxi mum pol l utant
l oad, whi ch i s cal cul ated through
i s pl otted versus the fl ow rate requi red by the si nk, G
j
.
Thi s gi ves a strai ght l i ne whose sl ope i s z
j
max
.
Si mi l arl y, the l oad of each source i s gi ven by
Hence, the source l oad i s pl otted versus i ts fl ow rate to
gi ve a strai ght l i ne whose sl ope i s the composi ti on of
the pol l utant, y
i
.
Let us start wi th the fi rst si nk and consi der a case
where the pol l utant l oad for the fi rst source exceeds the
maxi mum i nl et l oad to the fi rst si nk. Therefore, we
move the source arrow unti l i t touches the si nk arrow
wi th the source compl etel y bel ow the si nk i n the
overl apped regi on, as shown i n Fi gure 5.
F
N
sources
opti mum
+ mi n F
N
si nks
-1
(32)
G
N
si nks
-1
) F
N
si nks
-1
+

i)1
N
sources
w
i,N
si nks
-1
(33)
G
N
si nks
-1
z
N
si nks
-1
i n
)

i)1
N
sources
w
i,N
si nks
-1
y
i
(34)
z
N
si nks
-1
mi n
e z
N
si nks
-1
i n
e z
N
si nks
-1
max
(35)
R
i,N
si nks
-1
) W
i
-

j)1
N
si nks
-2
w
i,j
for i ) 1, 2, ..., N
sources
(36)
z
j
i n,opti mum
) z
j
max
for j ) 1, 2, ..., N
si nks
(37)
M
j
si nk
) G
j
z
j
i n
(38)
M
j
i n,opti mum
) M
j
max
for j ) 1, 2, ..., N
si nks
(39)
Figure 5. Load versus fl ow rate graph for one source and one
si nk.
z
1
max
e z
2
max
e e z
j
max
e e z
N
si nks
max
(40)
y
1
< y
2
< < y
i
< < y
N
sources
(41)
M
j
si nk,max
) G
j
z
j
max
(42)
M
i
source
) W
i
y
i
(43)
I nd. Eng. Chem. Res., Vol . 42, No. 19, 2003 4323
The overl apped fl ow rate represents the extent of
recycl e/reuse from the fi rst source to the fi rst si nk. The
unful fi l l ed fl ow rate of the si nk must now be provi ded
by a fresh resource. The remai ni ng fl ow rate of the fi rst
source i s consi dered for recycl e/reuse i n the second si nk
and i s suppl emented wi th fresh source as needed
(Fi gure 6).
The feed requi rements for the thi rd si nk can be
sati sfi ed by a mi xture of the remai nder of the second
source and a fracti on of the thi rd source. No fresh source
i s requi red i n the thi rd si nk. Wi th no more si nks i n the
probl em, the rest of the thi rd source i s di scharged
(Fi gure 7).
By addi ng the fresh fl ow rates requi red i n si nk
1
and
si nk
2
, we obtai n the total amount of fresh usage. Thi s
total amount of fresh usage (F
1
+ F
2
) i s pl otted al ong
wi th source
1
, source
2
, and source
3
i n ascendi ng order
(l owest to hi ghest concentrati on) just as for si nk
1
, si nk
2
,
and si nk
3
(Fi gure 8), wi th the poi nt of contact between
the sources and si nks bei ng the materi al recycl e pi nch
poi nt. Subsequentl y, by pl otti ng the sources and si nks
i n the above-descri bed method, composi te curves are
generated wi th the source composi te bei ng shi fted to the
ri ght unti l i t l i es compl etel y bel ow the si nk composi te
(Fi gure 9).
Targeting Procedure
Thus far, we have sol ved the recycl e/reuse probl em
by i denti fyi ng opti mal recycl e/reuse strategi es. None-
thel ess, the objecti ve i s to determi ne a targeti ng pro-
cedure that provi des a val ue for mi ni mum usage of fresh
resource pri or to desi gn and wi thout detai l i ng the
al l ocati on strategi es. Furthermore, whereas there i s a
si ngl e target for fresh resource consumpti on, there are
many (someti mes i nfi ni te) al ternati ve source-si nk
matches that can yi el d the target. Therefore, i t i s
necessary to extract a targeti ng procedure from the
previ ous resul ts.
A key i nsi ght can be obtai ned from the precedi ng
graph. There i s a poi nt on the graph that di sti ngui shes
two zones. Bel ow that poi nt, fresh resource i s used i n
the si nks, and above that poi nt, unused process sources
are di scharged. Thi s poi nt wi l l be referred to as the
materi al recycl e/reuse pi nch poi nt. The key charac-
teri sti c of thi s poi nt i s based on the fol l owi ng observa-
ti on: the pi nch poi nt i s the poi nt where the l oad of
recycl ed/reused sources matches that of the si nk. There-
fore, i t can be graphi cal l y determi ned through the
fol l owi ng procedure:
(1) Rank the si nks i n ascendi ng order of maxi mum
admi ssi bl e composi ti on
(2) Rank the sources i n ascendi ng order of pol l utant
composi ti on, i .e.
(3) Pl ot the maxi mum l oad of each si nk (M
j
si nk,max
)
G
j
z
j
max
) versus i ts fl ow rate. Create a si nk composi te
curve by superi mposi ng the si nk arrows i n ascendi ng
order.
Figure 6. Load versus fl ow rate graph for two sources and two
si nks.
Figure7. Load versus fl ow rate graph for three sources and three
si nks.
Figure 8. Revi sed l oad versus fl ow rate graph for three sources
and three si nks.
Figure 9. Source/si nk composi te.
z
1
max
e z
2
max
e e z
j
max
e e z
N
si nks
max
y
1
< y
2
< < y
i
< < y
N
sources
4324 I nd. Eng. Chem. Res., Vol . 42, No. 19, 2003
(4) Pl ot the l oad of each source (M
i
source
) W
i
y
i
) versus
i ts fl ow rate. Create a source composi te curve by
superi mposi ng the sources i n ascendi ng order.
(5) Move the source composi te stream unti l i t touches
the si nk composi te stream, wi th the source composi te
bel ow the si nk composi te i n the overl apped regi on. The
poi nt where they touch i s the materi al recycl e/reuse
pi nch poi nt. The fl ow rate of si nks bel ow whi ch there
are no sources i s the target for mi ni mum fresh di s-
charge. On the other hand, the fl ow rate of the sources
above whi ch there are no si nks i s the target for waste
di scharge.
I t i s worth noti ng that the above procedure i s geared
toward si ngl e-component systems. I t can al so appl y to
mul ti component systems where there i s a l i mi ti ng
component and the sol uti on strategi es for the other
components are consi stent wi th that of the l i mi ti ng
component. For other mul ti component probl ems, a more
general approach shoul d be devel oped.
Case Studies
To i l l ustrate the appl i cabi l i ty of the devi sed proce-
dure, we sol ve four case studi es that were publ i shed
recentl y wi th sol uti ons through i terati ve procedures or
detai l ed anal yses encompassi ng the structure of the
recycl e/reuse networks.
Example1. Thi s case study i s taken from Sori n and
Bedard.
6
Tabl e 1 shows si x processes contai ni ng a si ngl e
contami nant. Each process has an i nl et and outl et water
fl ow rate and contami nant concentrati on, wi th the
excepti on of process 3, whi ch consumes i ts enti re fl ow
rate and therefore has no outl et. Addi ti onal l y, the
process i nl et and outl et fl ow rates have been fi xed for
al l si x operati ons.
To begi n the targeti ng procedure, fi rst the si nks and
sources are i denti fi ed and ranked i n terms of ascendi ng
concentrati on l evel s. I n thi s system, each process i nl et
i s i denti fi ed as a si nk. Addi ti onal l y, the outl ets of
processes 1, 2, 4, 5, and 6 are i denti fi ed as sources.
Fol l owi ng the procedure outl i ned i n the Targeti ng
Procedure secti on, the si nks are cumul ati vel y pl otted
on a l oad versus fl ow rate di agram starti ng wi th those
wi th the l owest concentrati on. Then, the sources are
pl otted cumul ati vel y on the same graph, al so i n ascend-
i ng order of concentrati on. Fi nal l y, the source composi te
l i ne i s shi fted to the ri ght by addi ng freshwater unti l
the enti re composi te source l i ne l i es to the ri ght and
bel ow the composi te si nk l i ne. The resul ti ng pl ot can
be seen bel ow i n Fi gure 10. As shown i n Fi gure 10, the
mi ni mum freshwater requi red i s 200 tonnes/h, and the
mi ni mum wastewater di scharge i s 120 tonnes/h. These
val ues agree exactl y wi th those found by Sori n and
Bedard
6
usi ng thei r al gebrai c evol uti onary tabl e method.
Addi ti onal l y, the graph i denti fi es two poi nts where the
source composi te touches the si nk composi te.
By exami ni ng the graph, two water recycl e/reuse
pi nch poi nts are i denti fi ed correspondi ng to composi -
ti ons of 100 and 180 ppm. Through the evol uti onary
tabl e method, Sori n and Bedard
13
l ocated a l i mi ti ng
source concentrati on of 180 ppm that they deemed the
gl obal pi nch source. The exi stence of mul ti pl e pi nch
poi nts at 100 and 180 ppm i n thi s case study was
di scovered by Hal l al e
14
through an i terati ve water
surpl us di agram. Hal l al e
14
al so veri fi ed the targets
found for freshwater and wastewater by Sori n and
Bedard.
13
Example 2. The second case study i s taken from
Pol l ey and Pol l ey.
5
Thi s probl em i nvol ves four sources
and four si nks, and rel evant i nformati on about them i s
provi ded i n Tabl e 2:
Constructi ng the cumul ati ve composi te curves and
shi fti ng the source composi te to the ri ght as i n the
previ ous exampl e, the shi fted source/si nk composi te
graph can be created and i s shown bel ow i n Fi gure 11.
Fi gure 11 shows that the mi ni mum freshwater re-
qui red by the si nks i s 70 tonnes/h, and the mi ni mum
wastewater di scharged from the process i s 50 tonnes/
h. Addi ti onal l y, the pi nch concentrati on i s shown to
correspond to source 3 (150 ppm). The mi ni mum fresh-
water and wastewater targets found above are i denti cal
to those found by Pol l ey and Pol l ey
5
usi ng thei r method.
Pol l ey and Pol l ey di d not l ocate a pi nch poi nt; however,
Hal l al e,
7
usi ng a water surpl us di agram, determi ned the
pi nch l ocati on to be 150 ppm, whi ch i s i n agreement
wi th the val ue obtai ned here.
Table 1. Process Information for Example 1
si nk
fl ow
(tonne/h)
maxi mum i nl et
concentrati on (ppm)
l oad
(kg/h)
1 120 0 0
2 80 50 4
3 80 50 4
4 140 140 19.6
5 80 170 13.6
6 195 240 46.8
source
fl ow
(tonne/h)
concentrati on
(ppm)
l oad
(kg/h)
1 120 100 12
2 80 140 11.2
3 140 180 25.2
4 80 230 18.4
5 195 250 48.75
Figure 10. Shi fted source/si nk composi te curves for exampl e 1.
Table 2. Process Information for Example 2
si nk
fl ow
(tonne/h)
maxi mum i nl et
concentrati on (ppm)
l oad
(kg/h)
1 50 20 1
2 100 50 5
3 80 100 8
4 70 200 14
source
fl ow
(tonne/h)
concentrati on
(ppm)
l oad
(kg/h)
1 50 50 2.5
2 100 100 10
3 70 150 10.5
4 60 250 15
I nd. Eng. Chem. Res., Vol . 42, No. 19, 2003 4325
Example3. To show the appl i cabi l i ty of the approach
to a l arge process, the thi rd case study i s taken from
Jacob et al .
20
The study i s of a thermomechani cal pul p
and newspri nt mi l l consi sti ng of 54 si nks and 10
sources. The source and si nk data are presented i n
Tabl es 3 and 4.
Upon exami nati on of the si nks, i t i s cl ear that there
are onl y four concentrati on l evel s of i nterest. Therefore,
the si nks can be l umped i nto four si nks wi th fi nes
concentrati ons of 0, 0.018, 0.02, and 1. The resul ti ng
l umped si nks can be seen i n Tabl e 5.
Usi ng the i nformati on from Tabl es 3 and 5, the shi fted
source/si nk composi te can be constructed and i s shown
i n Fi gure 12.
From Fi gure 12, the mi ni mum wastewater di scharge
can be determi ned as 34 292 L/mi n; however, to deter-
mi ne the mi ni mum freshwater requi rements and pi nch
l ocati on, the regi on cl ose to the ori gi n must be exami ned.
I n Fi gure 13, a magni fi ed pl ot of the area of i nterest i n
Fi gure 12 can be seen.
Anal yzi ng Fi gure 13, the mi ni mum freshwater re-
qui red for the process can be found as 1342 L/mi n, wi th
a pi nch l ocated at 0.07% fi nes. Accordi ng to Jacob et
al .,
21
the mi ni mum freshwater requi red for thi s system
i s 1380 L/mi n, whi ch i s sl i ghtl y hi gher than the target
we i denti fi ed.
Example 4. To show the broad appl i cabi l i ty of the
proposed method, the fi nal case study to be sol ved
i nvol ves the recycl e and reuse of hydrogen rather than
water. The fourth case study i s taken from Al ves and
Figure 11. Shi fted source/si nk composi te curves for exampl e 2.
Table 3. Process Source Information for Example 3
source
fl ow
(L/mi n)
fi nes
concentrati on (%)
l oad
(L/mi n)
TMP cl ear water 25 000 0.07 17.5
TMP cl oudy water 39 000 0.13 50.7
i ncl i ned screen water 5980 0.5 29.9
press header water 2840 0.49 13.9
save-al l cl ear water 6840 0.08 5.5
save-al l cl ear water 3720 0.1 3.7
si l o water 73 000 0.39 284.7
machi ne chest whi tewater 8585 0.34 29.2
vacuum pump overfl ow 2570 0 0.0
resi dual showers 1940 0.13 2.5
Figure 12. Shi fted source/si nk composi te curves for exampl e 3.
Table 4. Process Sink Information for Example 3
si nk
fl ow
(L/mi n)
maxi mum al l owabl e
fi nes concentrati on (%)
l oad
(L/mi n)
1 200 1 2.0
2 400 1 4.0
3 355 0.02 0.1
4 150 1 1.5
5 13 000 1 130.0
6 4250 1 42.5
7 2800 1 28.0
8 4580 1 45.8
9 1950 1 19.5
10 500 1 5.0
11 1000 1 10.0
12 3000 1 30.0
13 435 1 4.4
14 310 1 3.1
15 60 1 0.6
16 1880 1 18.8
17 4290 1 42.9
18 9470 1 94.7
19 6500 1 65.0
20 620 1 6.2
21 55 1 0.6
22 70 1 0.7
23 320 1 3.2
24 1050 1 10.5
25 73 000 1 730.0
26 1765 1 17.7
27 235 1 2.4
28 95 1 1.0
29 20 1 0.2
30 180 0 0.0
31 160 0.018 0.03
32 30 0.018 0.005
33 20 0.018 0.004
34 315 0 0.0
35 315 0 0.0
36 930 0.018 0.2
37 460 0.018 0.1
38 30 0.018 0.005
39 30 0.018 0.005
40 315 0 0.0
41 315 0 0.0
42 110 0.018 0.02
43 110 0.018 0.02
44 190 0 0.0
45 190 0 0.0
46 100 0 0.0
47 20 0 0.0
48 15 0 0.0
49 60 0.018 0.01
50 30 0.018 0.005
51 100 0 0.0
52 20 0 0.0
53 100 0 0.0
54 20 0 0.0
Table 5. Consolidated Process Sink Information for
Example 3
si nk
fl ow
(L/mi n)
maxi mum al l owabl e
fi nes concentrati on (%)
l oad
(L/mi n)
1 2195 0 0.0
2 1970 0.018 0.4
3 355 0.02 0.1
4 132 005 1 1320.1
4326 I nd. Eng. Chem. Res., Vol . 42, No. 19, 2003
Towl er.
9
Thi s case study i nvol ves the opti mi zati on of a
hydrogen di stri buti on system wi thi n a refi nery, and i t
compri ses four si nks and si x sources. The perti nent
i nformati on regardi ng these si nks and sources i s gi ven
i n Tabl e 6.
Addi ti onal l y, i n thi s case study, the fresh resource
contai ns a smal l quanti ty of i mpuri ty, i .e., the fresh
hydrogen has a 5% i mpuri ty l evel . Usi ng the i nforma-
ti on i n Tabl e 6, the shi fted source/si nk composi te curves
can be constructed, as shown i n Fi gure 14.
From Fi gure 14, one can determi ne that the mi ni mum
hydrogen requi red and waste hydrogen to be di scharged
are 268.8 and 102.5 mol /s, respecti vel y. Addi ti onal l y, the
pi nch poi nt occurs at the l ast source, whi ch corresponds
to a hydrogen i mpuri ty of 30%. These val ues are i n
agreement wi th those found by Al ves and Towl er
9
usi ng
the i terati ve hydrogen surpl us di agram approach.
Conclusions
We have devel oped a si ngl e-stage, systemati c, and
graphi cal method for i denti fyi ng ri gorous targets for the
recycl e/reuse probl em. The opti mal i ty condi ti ons were
fi rst deri ved usi ng a dynami c programmi ng formul ati on
and an anal yti cal sol uti on for parametri c opti mi zati on.
The resul ts of the mathemati cal anal ysi s were next
i nvoked i n devel opi ng a new pi nch-based graphi cal
representati on of composi te l oad versus fl ow i n a way
that ensures opti mal i ty. The devi sed vi sual i zati on tool s
accuratel y determi ne the mi ni mum usage of fresh
resources, the mi ni mum di scharge of waste, and the
maxi mum recycl e/reuse of process streams. Several
publ i shed case studi es were used to i l l ustrate the ease
and appl i cabi l i ty of thi s novel graphi cal techni que.
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Figure 13. Magni fi ed shi fted source/si nk composi te curves for
exampl e 3.
Table 6. Process Information for Example 4
si nk
fl ow
(mol /s)
maxi mum i nl et i mpuri ty
concentrati on (mol %)
l oad
(mol /s)
1 2495 19.39 483.8
2 180.2 21.15 38.1
3 554.4 22.43 124.4
4 720.7 24.86 179.2
source
fl ow
(mol /s)
i mpuri ty concentrati on
(mol %)
l oad
(mol /s)
1 623.8 7 43.7
2 415.8 20 83.2
3 1801.9 25 450.5
4 138.6 25 34.7
5 346.5 27 93.6
6 457.4 30 137.2
Figure 14. Shi fted source/si nk composi te curves for exampl e 4.
I nd. Eng. Chem. Res., Vol . 42, No. 19, 2003 4327
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Received for review Apri l 16, 2003
Revised manuscript received June 24, 2003
Accepted June 24, 2003
I E030318A
4328 I nd. Eng. Chem. Res., Vol . 42, No. 19, 2003