POLYMER APPLICATION EXAMPLES IN INDUSTRIAL WASTEWATER TREATMENT

A. TURKMAN
Dokuz EylUI University
Dept. of Environmental Engineering
Izmir-TURKEY

ABSTRACT. Polymer application in industrial wastewater treatment has

b'ecome very important in recent years due to the increased pollutant
removal efficiencies, easier sludge disposal, economy in chemicals
consumption, etc. Polymers may either be used as coagulants or as coagu-
lant aids for the aggregation of colloidal particles.
In this study, various industrial wastewater samples were treated
with and without polymers in order to determine the effectiveness of
polymers as coagulant aids. They were found to increase turbidity remo-
val efficiency by 69 % and COD removal efficiency by a maximum of 46 %.

1. POLYMERS IN INDUSTRIAL WASTEWATER TREATMENT

A polymer is a large molecule built up by the repetition of small,

simple chemical units. In some cases the repetition is linear, much as a
chain is built up from its links. In other cases the chains are branched
or interconnected to form three dimensional networks. The repeat unit of
the polymer is usually equivalent or nearly equivalent to the monomer,
or starting material from which the polymer is formed (Billmeyer, 1984).
Polymers with ionizable groups along the chain, termed polyelec-
trolytes, normally exhibit properties in solution that are quite
different from those with nonionizable structures.
When a polyelectrolyte is dispersed in water it dissociates into
disymmetric ions. The large ion is called the polyion. Its molecular
weight, m" is of the same order of magnitude as the molecular weight of
the macromolecule; the number of ionizable sites (~ ) is greater than
unity. The IIZII number determines the surface charge; z, e. The smaller
ion is called the counter ion with molecular weight, ~~m1' it has
usually a single ionizable site (z2=1).
As an example, consider the polysalt derived from sulfonated poly-
styrene

93
A. Tiirkman and O. Uslu (eds.). New Developments in Industrial Wastewater Treatment. 93-109.
© 1991 Kluwer Academic Publishers.
94

where n is the degree of polymerization. The number ~ of ionizable

sites here is equal to n (Jannink, 1986). Polyelectrolytes are linear or
branched chains of small identical subunits, sometimes two or three
different kinds of subunits. These subunits contain ionizable -COOH,
-OH, -P0P.312 -Nf2 or Ht NI2 groups (Fair et aI, 1968). These kinds of
polymers are soluble in water, conduct electricity and are affected by
the electrostatic forces between their charges. Some natural polyelec-
trolytes, i.e., polymers of biological origin are important in the orga-
nization of the biological ~ructure. Long chain molecules of this kind
contain from 2-3 to nearly 1& subunits. Polymers dissociating to form
negatively charged polymeric ions are called anionic polymers, and the
ones forming positively charged ions are called cationic polymers. Poly-
mers dissociating to give both large positive ions and large negative
ions are called ampholitic polymers. Cationic, anionic, nonionic and
ampholytic polymers can be prepared by choosing a suitable monomer.
Examples follow (Faust, 1983):
Nonionic Polymers:
Polyethylene oxide (-CH 2-CH2 -O-)n
Polyacrylamide (PAM) (-CR 2 -CR-)n
C=o
NH2

Anionic Polyelectrolytes:

Polyacrylic acid (PAA) -CH2 - ~H - ] n-

c=o
6 n

Hydrolyzed polyacrylamide (HPAM)

[
_CH, -
t::
~H-l
c=o
I
NH2 m

Cationic Polyelectrolytes:
Polydiallyldimethylammonium (PDADMA)

n
 95

Polyvinylpyridinium salt

2. EFFECT OF POLYMERS IN COAGULATION

It is a necessity to define the terms coagulation, flocculation, coagu-

lant and coagulant aid because of the complication created in relation
to their meanings by different researchers. In this study, the term
coagulation is used to indicate destabilization of colloids, but as a
unit operation it comprises coagulation in the above sense as well as
flocculation and sedimentation. Flocculation is the growing of destabi-
lized colloids (microflocs) by velocity gradients to large, settleable
floes. The coagulant is the chemical substance used in order to destabi-
lize colloids and to cause them to settle. A coagulant aid is the chemi-
cal substance added in order to improve the settling characteristics of
flocs by mechanisms explained in this section. In some studies, inor-
ganic salts are called coagulants and polymeric substances, flocculants,
therefore, aggregation of colloids is called coagulation if inorganic
salts are used, and flocculation if polymers are used. There are other
definitions also, but in this study, the first group of terms have been
adopted.
Coagulants most often used in wastewater treatment include alum
(Al2(S04)3.14H20), ferric chloride (FeCI 3.6H 20), ferrous sulphate
(FeS04.7H20) and some polyelectrolytes. The materials that find utili-
zation as 'coagulant aids' are for the most part polyelectrolytes. By
applying these substances higher density flocs may be obtained.
The polyelectrolytes, when serving as coagulant aids act to reduce
the stability of colloidal systems and facilitate their coagulation.
Their effectiveness in water and wastewater treatment has been shown in
many applications (Correl, 1979, TUrkman et ale 1987, Kavuk~uogullar1,
1988, Toroz, 1988, Karada§, 1988).
In coagulation, chemicals are added to the wastewater (or water)
to reduce the forces that keep the colloidal particles apart. Floccu-
lation of a polymer-sol system of like charges results only if an
appropriate concentration of a salt is present in the solution. However,
floculation usually occurs at electrolyte concentrations much smaller
than those necessary in the absence of polymers (stumm, 1976).
Destabilization in most of the wastewater treatment processes is
accomplished by polymers. These polymers can be added to the process or
they may be produced within the process. Undoubtedly the processes in-
volved in flocculation are highly complex, but a simplified mechanism
will help explain the behaviour of polymers in the flocculation process.
The flocculation of colloidal dispersions with polymers takes
place by (1) adsorption of the polymer on the colloid (2) by cross lin-
kage of the segments of polyelectrolytes to form bridges between the
96

REACTION 1
Initial adsorption (Optimum polymer dosage)
A
7
I
r + 0 , ~
Polymer Colloidal particle Destabilized
particle
~

~
REACTION 2

+~
Formation
~

Destabilized particles Floc

REACTION 3

~
Second~dsorptlon

~ ..stabiUZ'd
partIcle

\i
REACTION 4
Initi al adsorption I E x cess POIYme~
~ + 0 ~
Excess

~
polymers
REACTION 5
Rupture }of floc
By high 5h~
7' 4;
Colloidal particle Stable particle

Floc Floc fragments

IZ
REACTION 6

tf
Secondary adsorption
~

Floc fragment Res1abilized particle

Figure 1. Schematic representation of the phenomena which can

occur in the coagulation of colloids uSing polymers.
 97

dispersed colloidal particles, and (3) by the resulting formation of a

loose, three dimensional structure.
It has been found experimentally that the behaviour of polymer-
solid adsorption systems can be approximated by a simple adsorption
isotherm of the Langmuir type as shown by equation (1), where 0 is the
fraction of the adsorption sites on the surface of the solid particles
covered by adsorbed polymer, P is the equilibrium concentration of
polymer in solution and b is an adsorption constant depending on the
properties of the polymer and of the particle.

6 = bPf(1+bP) (1)

P is related to the initial concentration of polymer, Po, by the

expression given in equation (2)

P= Po-kwe (2)

where k is a constant depending upon the specific surface area of the

solid and the number of adsorption sites per unit area, and w is the
content of the solids in suspension. Combination of equation (1) and (2)
gives equation (3), showing the increase of 0 with increasing polymer
content, Po, and with decreasing concentration of suspended solids, w.

9= b(p -kwS)/(1+b (P -kw9» (3)

o
The principal theories of flocculation assume that polymer mole-
cules attached to solid particles still have free active centers that
can be adsorbed on the remaining free surfaces of other particles. This
process results in "bridging" between solid particles and in the
consequent formation of large flocs having a three dimensional network
structure. The bridging mechanism involves a bimolecular process, the
rate of which is dependent upon the concentration of both of the par-
ticles carrying floculant, no9 (where n is the number of solid particles
per unit volume), and of particles with free surface able to adsorb
flocculant, no(1-6). Thus, the rate of floc formation may be given
by equation (4) where k1 is a constant.

-dn /dt = k n~ 6(1-9) (4)

The floes break down at a rate which is directly proportional to
the volume of floc and inversely proportional to the surface area and to
a bridging factor, 9(1-9) (Boke,' 1983) •
Figure 1 shows the reactions taking place in the coagulation of
colloids with the help of polymers. When a polymer comes into contact
with a colloidal particle, some of these groups adsorb at the particle
surface", leaving the remainder of the molecule extending out into the
solution (reaction 1). If a second particle with some vacant adsorption
sites contacts these extended segments, attachment can occur (reaction
2). A particle-polymer-particle complex is thus formed, in which the
polymer serves as a bridge. If a second particle is not available, in
time the extended segments may eventually adsorb on other sites on the
98

original particle, so that it is no longer capable or serving as a

bridge (reaction 3). Many mechanisms ror the interaction between a
polymer group and a site on the particle have been proposed. In many of
the industrial wastewater treatment applications toilet, kitchen etc.
wastes are collected with process wastes and treated together. Thus,
industrial wastewater contains microorganisms also. When coagulation is
applied they are removed from wastewaters together with other colloids.
Although the size of bacteria range between 0.3 micron and 50
micron, they are mostly 0.5-3 micron size. Viruses range between
0.02-0.2 micron (Mara, 1980). They are hydrophilic biocolloids that
carry a net negative charge within the pH range that is generally app-
lied in coagulation. Their agglomoration is not brought about merely
by reduction in the charge density in electrostatic repulsion. Instead,
agglomeration may be looked upon as an interaction of polyelectrolytes
of natural origin. Polymers, polysaccharide and polyacids, for instance
are excreted at the surface of microorganisms. This seems to happen
under all physiological conditions (Fair et aI, 1968).
When organisms grow prolirically, for example, new surfaces are
created faster than they become covered with polymers. This brings about
an improvement in biorlocculation during the declining growth phase and
becomes optimal in the endogenous phase. Essential components of bio-
masses in conjunction with aerobic generation are (1) creation of dis-
persed microbic populations and their utilization of substrate ror
energy and cell growth (2) chemical coagulation of the dispersed growths
by multivalent metal ions and synthetic organic polyelectrolytes, and
(3) phase separation of coagulated biomasses.

3. USE OF POLYMERS IN INDUSTRIAL WASTEWATER TREATMENT

3.1. Experimental Method

Wastewater samples were collected from various industries in the Izmir

area and coagulation tests were applied in order to determine the effect
of polymer addition on treatment. The coagulation experiments were
carried out in a jar test apparatus conSisting of a set of six beakers
each with a capacity of 1 liter and with a mixing device. In all the
experiments 3 minutes of rapid m~x1ng, 140 rpm, 30 minutes of slow
mixing, 12 rpm; and one hour of sedimentation were applied. Four types
of industrial wastewater samples were used in conducting the jar test
experiments.

1st series: Textile Industry

2nd series: Dye Industry
3rd series: Milk Industry
4th series: Licorice (Radix Liquiera) Root Industry

The polyelectrolytes that were used in the laboratory study as coa-

gulant aids were commercially available anionic, cationic and nonionic
type polymers. The removal efficiencies were measured in terms of
turbidity or chemical oxygen demand (COD). In conducting jar tests,
 99

first pH optimization was conducted and then the optimum dosage of

chemical is determined at that pH level. Turbidity, pH and chemical
oxygen demand were determined using procedures outlined in Standard
Methods (1981).
The removal efficiencies obtained by coagulating various industrial
wastewaters are given in Tables 1 to 5.

3~2; Data and Findings

Experimental results are given in Table 1 for textile industry wastewa-

ters, Table 2 for dye industry wastewaters, Table 3 for biologically
treated dye industry wastewaters, Table 4 for milk industry wastewaters
and Table 5 for licorice root industry wastewaters. The experimental
data is also summarized graphically in order to observe the effect of
polymers as coagulant aid.

Table 1. Jar test results for textile industry wastewaters at

pH= 7.34 (Initial COD=418 mg/l).
Chemical Subs. Added,mg/l COD, mg/l COD Removal Eff.%

A~ (S~ ~ 125 280 33

250 180 57
375 164 61
500 148 64
625 108 74
875 104 75
1000 108 74
1125 120 71
Aia, (S~ )3 (875 mgll)
+ E 0.1 52 88
0.5 36 91
1.0 56 87
2.0 64 85
3.0 65 84
Fec~
100 160 62
200 140 66
300 120 71
400 96 77
500 116 72
600 200 52
Fec~ (400 mg/l)
+KP 0.1 156 63
0.5 100 76
1.0 104 75
2.0 76 82
3.0 146 65
100

Table 2. Best removal efficiencies obtained for water samples

taken from effluent of a dye industry.

Coagulant and coag. aid: Clay

+KPE
pH 6.25 6.25 7.50 7.50
Dose mg/l+ml/l 500 300+1 300 600+2.5
Turbidity of raw ww,JTU 700 700 700 700
Turbidity of treated ww,JTU 12 15 650 165
Turbidity removal % 98.3 97.9 7.1 76.4
F.~oliform in raw ww,
10 /100 ml 10000 5000 10000 5000
F.~oliform in treated ww,
10 /100 ml 0.4 0.3 150 7
F.Coliform removal % 99.9 99.9 98.5 99.9
Table 3. Best removal efficiencies obtained for water samples
taken from effluent of dye industry biological water treat-
ment plant
Coagulant and coag; aid: A~ (s'h)3 A~ (50.')3 Clay Clay
+KP~ +KPE

pH 6.25 6.25 7.50 7.50

Dose mg/l+ml/l 75 25+1 100 75+1
Turbidity of raw ww,JTU 9 9 9 9
Turbidity of treated ww,JTU 2 2 14 6
Turbidity removal % 77.8 77.8 55.6 33.3
F.~oliform in raw ww,
10 /100 ml 200 150 150 150
F.~oliform in treated ww,
10 /100 ml 4 1 20 20
F.Coliform removal % 98.0 99.3 86.7 86.7
Table 4: Best removal efficiencies of obtained for water
samples taken from effluent of a milk industry
Coagulant and coag. aid: Clay
+APE
pH 6.25 6.25 7.50 7.50
Dose mg/l+ml/l 300 150+1.5 350 200+2
Turbidity of raw ww,JTU 650 650 650 650
Turbidity of treated ww,JTU 37 13 440 390
Turbidity removal % 94.3 98.0 32.3 40.0
F.~oliform in raw ww,
10 /100 ml 7000 4000 4000 4000
F.~oliform in treated ww,
10 /100 ml 40 30 300 30
F.Coliform removal % 99.4 99.3 92.5 99.3
 101

Table 5 .. Jar test results for licorice root industry waste-

waters at pH=7 (Initial COD:845 mgtl).

Chemical Subs.' Added,mgtl COD,mgtl COD Removal Eff.%

A~ (S04)3 800 632 25

825 624 27
850 616 27
875 610 28
900 598 30
925 616 28
A3:2 (S~)3 (900 mgtl)
+APE
10 228 73
33 200 76
70 342 60
90 264 69
110 278 67
FeC~
150 392 54
240 372 56
330 368 57
420 464 45
510 496 42
600 512 40
Fec~ (330 mgtl)
+AP
10 113 87
30 85 90
50 128 85
70 171 80
90 270 68

4.' DISCUSSION

Some experimental results were not presented because of the lack of

space. The experimental results that were unsuccessful with respect to
turbidity or COD removal were omitted and pH optimization data was not
given,; Only optimum pH value results were indicated~

1. Although destabilization of colloids by aluminium and iron (III)

salts can be accomplished by hydroxo-metal-polymers, addition of
synthetic polymers were very effective in coagulation,- owing to the
bridging mechanism created by these substances. Thus, addition of
cationic polyelectrolytes as coagulant aids caused a maximum COD removal
efficiency increase of 16 % and a maximum turbidity removal efficiency
increase of 69 %. Comparative figures for anionic polymers were 46 % for
COD and 8 % for turbidity. But the only creteria for polyelectrolyte
application is not their contribution to the removal efficiency. The
cost of coagulant aid is generally offset by a combination of factors
like savings in the cost of primary coagulant and effluent water quality
102

requirements. As an example, 1 milliliter of polyelectrolyte addition

causes a saving of 200 mg/l of A12 (SO) for about the same
efficiency for dye industry wastewaters (¥a~le 2). In such a case the
application of polyelectrolyte may be preferred considering the costs of
alum and polymer.
2. Destabilization by polymers is more effective at high colloid con-
centrations. This may be because of insufficient contact opportunities
between the colloids in dilute solutions. For example, comparing Tables
4 and 5, using the same coagulant and coagulant aid 98 % efficiency was
obtained at a turbidity of 700 and 78 % efficiency was obtained at 9;
3; Considering the figures given above, 78 % efficiency at a turbidity
of 9 is a relatively high figure compared to the 98 % efficiency at a
turbidity of 700~ This phenomenon may be explained by bioflocs formed
during the biological treatment of wastewaters. Because the
microorganisms are in the endogenous phase after the biological
treatment, this results in improvement in coagulation as a result of the
polymers excreted by the microorganims.
4. Application of polyelectrolytes also affects the removal of coliform
bacteria.' This may be interpreted in terms of microorganism-coagulant
-polymer interactions. Many bacteria and algae have a tendency to adhere
to interfaces and to each other (bioflocculation). Coliform removal was
found to be very efficient both in the presence of anionic and cationic
polyelectrolytes. Because of the hydrophilic surface of the microorga-
nisms, bioflocculation should have been affected by polymers more than
the reduction of surface potential.
5. Compared with other coagulants, clay is not a very effective coa-
gulant. But when it is used in combination with coagulant aids, the
efficiency increases to comparable levels with other chemicals (Figures
5,7 and 9). The efficiency of clay in the presence of coagulant aid may
be explained by the bridging mechanism.
Clay particules are negatively charged at the surface and at the
edges the charge may be positive or negative depending on the pH of the
medium (Demiralp, 1987). At the pH value studied (pH= 7.50) clay par-
ticles are negatively charged. This explains the high removal efficiency
obtained by USing a cationic polyelectrolyte (Figure 5). Also it is
possible to mention a sweep floc effect of clay-polymer flocs. When clay
is used alone, it may even cause an increase in turbidity (Figure 7).
6. Almost all the Figures indicated the effect of restabilization when
the coagulants or coagulant aids were used in excess. This observation
indicates the importance of sensitivity of jar tests~ The chemicals used
in excess results in a loss of chemicals and a reduction in water
quality~'

7. Figure 2 indicates that in coagulating the textile industry waste-

water the application of polymer is more important than the determi-
nation of exact dose to be applied~ In order to obtain 90 % efficiency',
 103

aluminium sulphate should be used in combination with a cationic poly-

electrolyte. Lower efficiencies were obtained with the same polyelec-
trolyte when used in combination with iron chloride (Figure 3). When
treating dye industry wastewaters, it is possible to save aluminium
sulphate by applying small amounts of cationic polyelectrolyte (Figure
4). Figure 6 indicates that pollutant removal efficiency increase by
applying polymer to biologically treated dye industry wastewater.
Figures 8, 10 and 11 indicate both the efficiency increases and the
chemicals savings.
In developing countries like Turkey, an economical industrial
wastewater treatment is very important in order to achieve both indust-
rialization and environmental pollution control. In spite of theoretical
aspects of coagulation, it is still as much of an art as a science.
Research studies on the subject by applying different kinds of chemi-
cals as coagulants and coagulant aids to diverse industrial wastewaters
will add a lot to our knowledge in this field.

ACKNOWLEDGEMENT

The author acknowledges Muammer Karada~ and Nevin Eroglu for their labo-
ratory help.
Alum (875 mg/l) + KPE ,mgll
1.2 1.6 2.0 2.4 2.8
100
90 o Alum + KPE

-
0 b o o
• 80
~

• Alum
;: 70
w
CJ 60
>
0
E 50
I»
Ix:

Q
40
0
u 30

20

0 200 400 600 800 1000 1200 1400

AI2 (5°4 )3 I mgll

Figure 2. Graphical representation of the data obtained for textile

industry wastewater using alum.
104

FeCI 3 (400 mg/ll + KPE, mg/l

90 0.4 0.8 1.2 1.6 2.0 2.4 2.8

--
400 mg/l FeCI + J<PE
~80
•
•
...:
w 70
ti
g>
0
0
~ 60

50 •
0 100 200 300 400 500 600 700
Fe C1 3 • mg/l

Figure 3. Graphical representation of the data obtained for

textile industry wastewater using iron chloride.

100
Aluminium sulphate +KPE (lmllll

~ sulphate

•...!!
c>
0
E 90
~
>-
.!:
"C
:c...
:J
t-

OOO~--~1=OO~~2~O~O--~30~O--~4~OO~~S~OO~--6~O-O--~
Aluminium sulphate (mg II)

Figure 4. Graphical representation of the data obtained for dye

industry wastewater using alum.
 105

100

.-
90
•..: 80
-0 70
0
>
E 60
...
CII

:-
>-
SO
c '0
:c...
....
::J
30
20
10 Cia

0 100 300 '00 500 600

Clay (mgll)

Figure 5. Graphical representation of the data obtained for dye

industry wastewater using clay.

100
...:
• 90
c 80 Aluminium sulphate + KPE !1mlll)
>
0
E 70
...
CII

>- 60
.~

"... SO
:s
::J
l-
'D
30
20
0 25 SO 75 100 125 ISO
Aluminium sulphate (mg/l)

Figure 6. Graphical representation of the data obtained for

biologically treated dye industry wastewater using alum.
106

40
0 0 0 0 0 0
30
Clay and KPE IIml/!)
~

~
20
•
a
10
>
0
E a
...
1\1

-
>-
"0
:0
-10
-20
::; -30
~

-40
-50
0
- 60
Clay
-70
75 100 125 150 175 200
Clay ( mgll)

Figure 7. Graphical representation of the data obtained for

biologically treated dye industry wastewater using clay.

100
~
•
a>
0
E 95
...
-...
1\1

>-
.-6
.0 90 0

:::I
~

85
100 150 200 250 300 350 400
Aluminium sulphate (mg/l)

Figure 8. Graphical representation of the data obtained for milk

industry wastewater using alum.
 107

_40 o o D D
•
£: Clay and APE (2 mill)
a
~
~... 35

"Q
:0.
:; 30
....

25L---~----~--~----~----~---L----~-
100 150 200 250 300 350 400
Clay (mg/ll

JFigure 9. Graphical representation of the data obtained for milk

industry wastewater using clay

Figure 10. Graphical representation of the data obtained for licorice

root industry wastewater using alum.
108

Anionic polyelectrolyte, mgll

10 20 30 40 SO 60 70 80 90 100 110 120 130 140

90
88

86
330 mg/l FeCI 3 + APE
84
82

-
...:
~
80

78
:>.
~ 76
.!!
u
:: 74
w
g 72
o
~ 70
iii:

g 68
u

Iron (lI1l chloride

so
48

46
o

"
42 o

40 o

ISO 200 250 300 350 400 450 500 550 600 650 700 750 800
FeCIJ,mg/l

Figure 11. Graphical representation of the data obtained for licorice root
industry wastewater using iron(III) chloride.
 IW

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Jannink, G. (1986) 'Experiments on polyelectrolyte solutions',
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Tor5z, I.(1988) 'Yapag~ y~kama at~ksular~n~n alum ve polielektro-
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Turkman, A., $engul, F. (1987) 'Application of polyelectrolytes in
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