Desalination, 58 ( 1 9 8 6 ) 2 2 7 - - 2 4 1 227

Elsevier Science P u b l i s h e r s B.V., A m s t e r d a m - - P r i n t e d in T h e N e t h e r l a n d s

PRETREATMENT OF SEAWATER BY FLOCCULATION AND

SETTLING FOR PARTICULATES REMOVAL

A. A D I N a n d C. K L E I N - B A N A Y
Human Environmental Sciences, Graduate School o f Applied Science and Technology,
The Hebrew University o f Jerusalem, Jerusalem (Israel) Tel. (02) 221281
(Received O c t o b e r 25, 1 9 8 5 ; in revised f o r m D e c e m b e r 29, 1 9 8 5 )

SUMMARY

Seawater flocculation was studied in this investigation as an aid in preventing

fouling of reverse osmosis (RO) membranes by particulates. The behavior of
clays in seawater and their possible use in the pretreatment process was also
investigated. Mediterranean seawater samples were f o u n d to have a salinity
of about 36%0, pH of 7.9--8.2 and turbidity of 1.0--17.5 NTU (Nephelo-
metric Turbidity Units). After 1--3 h of quiescent settling, 30--50% of the
turbidity remained and then stabilized, pointing to a possible advantage
of lagooning prior to further treatment.
Tests carried o u t with artificial seawater, as well as natural seawater, were
carried out to study particle removal in general, and algae and clay in
particular. Different conventional and polyelectrolytic flocculants were
used in the experiments. The best clarification was f o u n d using alum and an
anionic polymer in combination, resulting in 2 0 - 1 0 0 particles per ml and a
turbidity of less than 1 NTU. It was also f o u n d t h a t particle size distribution
measurements m a y provide a better picture of the quality and mechanism
of treatment.

INTRODUC~ON

It has long been established that particulate matter can cause mechanical
fouling in reverse osmosis membrane units by being caught in the membrane
fibers or on its surface. As the water passes through, these substances are
concentrated and a process similar to coagulation--flocculation takes place.
Neutralization of the particles' charge and coagulation of additional matter
m a y occur, while the trapped m a t t e r acts as a nucleus for polymerization or
flocculation. As the rate of flow increases so does the rate of fouling since
more nuclei are created and, thus, the rate of growth increases [1, 2].

0011-9164/86/$03.50 © 1 9 8 6 Elsevier Science Publishers B.V.

228

Despite the high salt c o n t e n t of seawater, particles of colloidal nature do

n o t tend to coagulate and settle on their own. The main c o m p o n e n t s of
particulate matter that m a y be f o u n d in coastal water are microorganisms,
detritus, quartz and clay minerals. Numerous studies have proven that there
is enough surface-active organic matter to be adsorbed on the surface of the
particles, thus affecting the predictions of the double-layer theory and
allowing particles to remain discrete [ 3--7 ].
Usually filtration is used as a pretreatment for the removal of particulate
matter from seawater. Different case reports of pilot plants and full scale
plants in operation have been published [8--11], and most of them utilize
either in-line (contact) coagulation or conventional clarification as a
destabilization means prior to the filtration step. For either m e t h o d
preliminary testing of flocculants is highly r e c o m m e n d e d due to similar
attachment mechanisms [12, 1 3 ] .
The above articles point o u t the important role of flocculants in the
pretreatment of seawater and, together with the existing need for the
improvement of the design and economics of the systems involved, call for
more systematic research in this area.
Our research was aimed at studying seawater flocculation by: (a) chemical,
physical and biological characterization of seawater (in this case Mediterranean
water) and particulates in relation to flocculation mechanisms; (b) study of
clays and algal behaviour in a seawater chemical environment; and (c) study
of seawater flocculation as a m e t h o d for the removal of particulates or as
a preparatory destabilizing step before filtration.

EXPERIMENTAL

The flocculation o f algae and clays was first studied in artificial seawater.
Water was prepared according to the analysis of salt c o n t e n t of real sea-
water made by L y m a n and Fleming [21]. Clay (bentonite and kaolinite)
suspensions were prepared b y dissolving 2.5 g clay in 500 ml distilled water
and then mixed at 2 5 r p m for 2 0 m i n , at 2 5 0 r p m for l min and 3 0 s
sonication. The alga chosen was Nannochlorus, a non-flagellate spherical
cell f o u n d free-floating in the water. The tested flocculants were aluminum
sulphate (alum) and various polyelectrolytes. The tests were carried o u t in
a jar test apparatus consisting of six paddles with 11 beakers of sample. Each
"jar" contained a different concentration of coagulant tested. The standard
test involved 1 min, 1 0 0 r p m rapid mixing and 2 0 m i n , 25 rpm slow mixing,
followed b y quiescent settling. After 30' of settling, turbidity and pH were
measured and for certain tests particle size distribution was determined.
Such main characteristics of seawater and of particles as salinity, pH,
alkalinity, total dissolved solids, suspended solids, turbidity, particle size
distribution, algal c o u n t and identification were determined. Samples were
taken from different beaches on the Mediterranean coastline. Analytical
 229

methods were those of Strickland and Parsons [14] and Standard Methods
[15]. A H I A C / R O Y C O particle size analyzer, model PC-320, was used to
measure particle size distribution in the 4 - - 3 0 0 p m range. This instrument
was f o u n d to be very useful for this t y p e of work [ 1 6 ] . In addition, scanning
electron micrographs were made of the residuals of various samples filtrated
through a 0 . 4 5 p m MiUipore filter. Turbidity measurements t o o k place
using a HACH nephelometer.
The last stage o f experimental work consisted of flocculation tests in the
jar test apparatus with Mediterranean seawater using alum, ferric chloride
and various polyelectrolytes.

RESULTS

Artificial seawater
Clays were tested with a double purpose: (1) to represent the inorganic
(mineral) suspended solids c o m p o n e n t of seawater, and (2) to examine the
possibility of using clay as a flocculant aid b y increasing the number of
particles present or as material for absorption, improving flocculation.
In the first stage, settling tests were carried o u t with different concen-
trations of clay in artificial seawater. Within a few hours most of the clay
had settled and after 24 h the residual turbidity was less than 1 NTU for all
concentrations of clay, pointing at very unstable conditions.
Flocculation tests with three concentrations of bentonite (10, 50 and 200
mg/1) were performed with different flocculants such as alum, cationic and
anionic polymers and combinations of these. Fig. 1 shows flocculation
curves for tests with alum alone. At a b o u t 25--35 mg/1 of alum the turbidity
removal reaches a maximum (60--85% removal, 0.75--1.75 NTU residual).
A sharp peak, as is usually f o u n d for polyelectrolytes b u t n o t for alum in
surface water, appears at the o p t i m u m alum dose, presenting a quick over-
dose phenomenon. Flocculation curves for similar tests performed with a
combination of o p t i m u m alum doses and polyelectrolyte (Magnafloc LT 25)
are presented in Fig. 2. Maximum turbidity removal was 77--95% with the
typical p h e n o m e n o n of a single peak for optimal polymer dosage. It can also
be observed from the graphs that particle counts followed the turbidity
results pretty closely.
The range of algae concentrations in seawater is usually 1.2--2.6 × 103
cells/ml [17, 18]. As mentioned above, Nannochlorus was used as the
representative alga in these experiments. Concentrations of this alga of less
than 103 cells/ml did n o t affect turbidity.
Fig. 3 shows the results of flocculation tests of artificial seawater containing
705--2 X l 0 s algal cells/ml with alum. The o p t i m u m alum concentration was
similar (20 mg/1) over most of the algal concentration. The flocs were usually
small and light. Overdosing occurred at slightly higher doses. Turbidity and
particle size distribution were measured. Turbidity removal was relatively
 230

low (45--75%). Since there was n o direct way to measure removal o f algae it
is hard to say what percentage o f algae was removed. The use o f 0.05 mg/l
anionic polyelectrolyte (superfloc A l l 0 ) with alum improved the turbidity
removal (84%) and gave larger flocs.

200m~/lclay
ooL /
50 mg/lclay
4c-

~ 2(-
i0 mg/lclay

o v
I I I I
16~

lO 1

[.-i

I " ~ ---~/~200mgll
~ ..~4~"- ''~
2 %% 50 mg/l
"- 4-- _ ......... • 1o mgll
I J I I I (Alumdose,mg/l)
0 20 40 60 80 I00

Fig. I. Flocculation curves for tests with alum in artificialseawater containing varying
concentrations of Kao|inite R a m o n .
 231

100 ~ ......._..-.-.-...~

~ 200 mg/l clay

80
.~....O.

60 -- I0 mg/l clay

40 --

~ mg/l clay

20 I I I I r
2400
Q 20o ,.~/1
/
4.0 __ /
/,,-
2000

//
// 1600
- //
1200 ou

2.0 50 mg/l

800 c.

i0 mg/l
1.0 ~ ~
400

_ _F_O__i----
o
0.2 0.4 0.6 0.8 1.0
Ma~nafloc "LT 25 dose, mg/l

Fig. 2. Flocculation curves for tests with alum and Magnafloc LT 25 in artifical seawater
containing Bentonite R a m o n , o, turbidity; o, particle count.

Fig. 4 shows the flocculation curves when both algae and clay were added
to artificial seawater. A larger plateau of good removal was obtained here as
compared to algae alone. The optimum dose was 25--35 mg/1 alum. The
lowest final turbidities were for 10mg/1 clay, but they were higher for no
232

I:

J //
'i 0

......._........-.---"'"

v v
>
• ° ° °

~N 'E~TPTqan~ lenpTse~

C
0

,-4
u

,-4 \
,-d
,-4 o \
\ x x

~.. mL •

,,~ ~ ..'"
0 c

'* \~" -- ~-'-L"~. o

I i °" ... I I'~.-..~ i 1 ~Q --/'" I
o

leAOm~= ~TpTqan~ ~u~D1~ d ALN ~ T I J T q ~ n ~

 233

clay addition (0.36 and 0.40 NTU as compared to 0.45 and 0.42 NTU for
10 a and l 0 s cells/ml respectively).

Mediterranean seawater characteristics

Eleven samples o f seawater were taken from a number of beaches. Table
I shows the date and location of sampling and some of the quality parameters
measured for each sample. As can be seen, salinity, as measured by titration
with silver nitrate, ranged from 30.06--38.88%0, total suspended solids
were 7.6--35.4 mg/1 and turbidity 1.0--17.5 NTU. High turbidity was due to
the presence of sand. pH was in the normal range for seawater (7.9--8.2)
as was the number of algae, 62--2650 cells/ml. Total particle counts for
4--300 pm ranged from 1072--5292 particles/ml.
Algae identified included Nannochlorous, Asterionella, Nitzchia and
Chlamydomonaa All these algae are also f o u n d in polluted estuaries and
were present in most o f the samples examined.
In addition, to characterize the particles in seawater in the range of less
than 4 #m, electron micrographs were made using a scanning electron micro-
scope (SEM). Particles in the colloidal size range of less than 1 pm and even
as small as 0.1/zm were measured. These were usually crystallites, although
some particles were of undefined shape. Matsumura et al. [19] indicated
that the crystallites are likely aluminum silicate clay particles and perhaps
algae.
A settling test was carried out for each sample in order to determine the
a m o u n t of settleable solids. Fig. 5 shows tests for several samples of seawater.
Turbidity was measured at varying intervals during a 48 h period. The
samples started with a large range of turbidities: 1--12 NTU. After 1--3 h
the turbidity dropped sharply (30--50%) and after 48 h only 12--50% of the
initial turbidity remained (0.5--1.5 NTU). The significance of these results
in planning pretreatment is that it may be useful to have a primary settling
basin with 1--3 h residence time before flocculation or direct filtration.
Fig. 6 shows results for the settling of sample G (see Table I) to which
several concentrations of clay were added (10, 150, and 200 mg/1) w i t h o u t
any chemical addition. After 2 3 h of settling, the appropriate turbidities
approached each other (1.7--2.4 NTU) and after 47 h t h e y ranged from 1.0
to 1.5 NTU, while the sample that contained no clay had the lowest final
turbidity. These results indicate that the addition of clay considerably
improves the percentage sedimentation, as could be expected from
flocculation kinetics, b u t does n o t improve the clarification o f seawater by
settling in absolute numbers.

Flocculation o f natural seawater

Flocculation tests were carried o u t with alum and ferric chloride. Comstock
[11] considered the latter more effective but the results f o u n d in this work
do n o t indicate it clearly (one m a y bear in mind that iron itself is considered
234

TABLE I

SUMMARY OF RESULTS OF CHARACTERIZATION OF SEAWATER

Sample Date Location Salinity Salinity TDS pH Turbidity

of of °/oo by °/~o by mg/l NTU
sampling sampling titration density 180°C

A 14/12/82 Tel Aviv near 37.49 ND+ ND 8.2 11.5--17.!

the opera (21.31)*
B 15/1/83 Jaffa Port 35.59 ND ND 7.9 4.9
(20.20)
C 23/2/83 Ashelon 34.39 ND 27 760 8.2 8.0
desalination (19.5)
plant
D 10/3/83 Jaffa Port 30.06 ND 28 860 8.1 5.7
(16.99)
E** 4/6/83 Rishon L e - 35.04 ND 38 160 8.0 2.0
Zion Beach (19.88)
F** 18/6/83 Gordon 37.87 37.1 36 870 ND 1.9
Beach -- (21.53)
Tel Aviv
G 5/7/83 Ashkelon 36.76 41.4 41 960 7.96 2.4--3.0
desalination (20.88)
plant
H** 9/7/83 Rishon Le -- 34.28 41.0 43 810 8.26 1.0
Zion Beach (19.40)
I 21/8/83 Nof Yam 36.14 39.4 27 590 8.2 2.1
Beach (20.52)
J** 18/10/83 Rishon Le -- 38.88 41.4 42 130 8.15 1.2
Zion Beach (21.33)

* Chlorinity by titration.
+ N D - - Not Done.
** Temperature taken at time of sampling for samples E, F, H and J was 27, 28, 28 and 25°C,
respectively.

t o b e a f o u l i n g a g e n t ) . F e r r i c c h l o r i d e gave s l i g h t l y l a r g e r f l o c s t h a n a l u m
b u t i n b o t h cases ( w h e n u s e d as sole f l o c c u l a n t s ) t h e f l o c s w e r e s m a l l , l i g h t
a n d s l o w t o s e t t l e . Fig. 7 s h o w s , f o r e x a m p l e , f l o c c u l a t i o n c u r v e s f o r t w o
seawater samples flocculated with a l u m i n u m sulfate a n d ferric chloride.
S u m m a r i z i n g all t h e t e s t s p e r f o r m e d , t h e m a x i m u m t u r b i d i t y r e m o v a l w a s
4 0 - - 8 0 % d e p e n d i n g o n i n i t i a l t u r b i d i t y as w e l l as c l a r i f i c a t i o n . F o r all s a m p l e s
t h e o p t i m u m a l u m d o s a g e r a n g e w a s 3 0 - - 5 0 m g / 1 a n d t h e FeC1 s d o s a g e
 235

Total Volatile Particle Total Algae Phosphorus Optimal

suspended suspended count alkalinity cells rag/1 alum dose
solids solids per ml per ml per mg/1
mg/1 mg/1 (4--300 p m ) as CaCO3 ml

9 4.4 ND 135 ND ND 40

18.4 -- ND 133 ND ND 30

41.5 6.8 4373 148 ND ND 30

9.8 5.2 5292 145 ND ND 40

7.6 2.9 2964 145 625 0.008 30

10.8 5.6 2677 ND 2650 0.029 30

9.6 4.6 2580 145 460 ND 35

ND ND 1072, 147 63 ND 30--35

35.4 8.7 1824 143 2000 ND 50

30.4 24.2 1420/1855 158 1100 ND 30

r a n g e 2 0 - - 5 0 mg/1. O v e r d o s i n g o c c u r r e d r a t h e r c l o s e t o t h e o p t i m u m d o s e ,
g i v i n g a s m a l l p l a t e a u , w h i l e c o n v e n t i o n a l c o a g u l a n t s in s u r f a c e w a t e r u s u a l l y
give a w i d e r r a n g e o f o p t i m u m t u r b i d i t y r e m o v a l . T h e l o w e s t p a r t i c l e c o u n t s
for treatment with alum were 42--237 particles/ml (up to 95% removal).
pH decreased linearly with increasing coagulant doses (little more than 1
u n i t f o r 1 0 0 mg/1 o f c o a g u l a n t ) . F e r r i c c h l o r i d e w a s s l i g h t l y m o r e i n f l u e n t i a l
in this respect.
2,36

12

6t.. , D
"O-,

A_
54
0 4 8 Iz 16 2~ 24
Time~ hrs

3.0

1.5 dl~ "~..E. . . . . . . . . . . . :.?

o.~_ ~ ~ ~ ~o
I I 2o 24 28
-- 4 B 12 16
Time, hrs

Fig. 5a. Settling tests for seawater samples A--D. A is represented by two curves: A for
after mixing of sample and A' for mixing and 15 rain settling of sample before txansfex
to settling test.
Fig. 5b. ,qettling tests for seawater samples E--J.
 237

80

i.'i["-.-.....
6O _
II~ ~ "..
~ --f ~"~--~ " ~ ~ i 0 mg/l clay

~- o m~ll ~V--~'0
L/~..
-- "~ "e
~' 20

\ .!oo ~I~ ///>'7-

o l I I f ~-----I •

24

~ 12 --
2oo ~g/z

6 "'0 ..... ....... 50 mgll

. . . . . . . .

lO ~g/l 1-16" " "j

. . . . . . . . . . o_~I L__ _ ---.a

o
I I ] • - " "

6 12 18 24
Time, hrs
Fig. 6. Settling tests in seawater sample G, containing various concentrations o f Bentonite
Ramon.
238

loo

,J 40 -- \_
~= ~ Sample C

20

I I I I I
4.5 --

~ 3.o

~ Sample C

~,~. "I~ ~ / _Ib 4-- Sample G

0
20 40 60 SO i00
Coagulant dose, mg/l
Fig. 7. C o m p a r i s o n o f f l o c c u l a t i o n c u r v e s o f M e d i t e r r a n e a n s e a w a t e r w i t h c o n v e n t i o n a l
f l o c c u l a n t s : a l u m i n i u m s u l f a t e a n d f e r r i c c h l o r i d e , o, a l u m ; o, FeC13.

The best results for particle removal by flocculation were f o u n d when

alum was used with an anionic polyelectrolyte. The flocs formed were larger,
settled more quickly and formed a more compact precipitate than alum
alone. The most effective polymers (out of 16 tested) were Magnafloc LT25
(0.05--0.1mg/1) and Superfloc A1839 (0.01--0.05 mg/l). Superfloc A-110
(0.025--0.05 mg/1) was also effective (e.g. Fig. 8). All three flocculants are
 239

p e r m i t t e d for use in drinking water by the U.S. Health authorities. The

presented experimental findings indicate a clear case for optimal p o l y m e r
dosage, in accordance with previous works done with polyelectrolytes [ 1 2 ] .
Although the i m p r o v e m e n t in t ur bi di t y due to addition o f polyelectrolytes
is small, c o m p a r e d to t r e a t m e n t with alum alone t he i m p r o v e m e n t in the
flocs properties is significant, and can be o f great effect in actual plants.
Clay, in concentrations o f up to 400 mg/1, was f u r t h e r tested f o r use as an
aid in flocculation with alum. It was f o u n d t hat it did n o t significantly
improve turbidity removal whereas a m u c h larger precipitate was f o r m e d .
According to work d o n e on sewage t r e a t m e n t by Narkis et al. [20] higher
clay co n cen tr at i ons m a y be needed in order to obtain improved treatment.
However, this creates t he problem o f massive sludge removal or storage.

1.2 Turbidity 600

z q
.~ O. 8

0.4
S I
Particles
- ---O
400

q s 200
i
o-
~0 S
I I I I I
0 0.2 0.4 0.6 0.8 i .0

Dose o f Superfloc All0, rag/l

Fig. 8. Flocculation curve for seawater sample E after flocculation with 30 mg/1 alum and
various doses of Superfloc All0.

DISCUSSION

Th e best clarification by flocculation o f seawater at different clay concen-

trations was f o u n d with alum and an anionic polymer. This c o m b i n a t i o n
gave larger, m o r e stable flocs than those with aluminum alone. This suggests
t h a t the anionic p o l y e l e c t r o l y t e is likely to act as a flocculating agent via
chemical interaction and bridging.
Algae do n o t significantly c ont r i but e t o the t urbi di t y o f seawater at usual
concentrations n o r are algae always c o u n t e d one to one by a particle counter.
This depends on t he size o f t he algae and the det ect i on limits o f the particle
counter. Percent t ur bi di t y removals o f algae-containing seawater were lower
than for clays. However, this m a y or m a y n o t reflect similar removal of
algae. Since no simple and reliable m e t h o d could be f o u n d t o m o n i t o r
240

algal concentrations, none was used. The addition of clay did n o t seem to
improve the removal of algae. Alum with an anionic polyelectrolyte gave
better t r e a t m e n t than alum alone.
Settling tests indicate that an initial clarifier in the pretreatment of sea-
water could help if it allowed for 1--3 h settling. Settling with the addition
of clay in seawater was similar to t h a t in artificial seawater but did n o t
actually contribute to turbidity removal.
A l u m i n u m sulfate as a coagulant gave better turbidity removal than ferric
chloride. The flocculation of seawater does n o t seem to differ from that of
fresh water except that overdosing occurs in a very close range to the point
o f m a x i m u m turbidity removal by conventional coagulants. Therefore
frequent monitoring o f coagulant dosing is necessary.
Flocculation tests were carried out both to test the use of flocculation as
a pretreatment process and as preparatory work for contact flocculation--
filtration tests. Although these processes differ, a similarity in the relation
between removal efficiency, dose and strength of flocs formed was f o u n d
by other investigators, showing that there are some c o m m o n mechanisms in
the two processes.
The use of polyelectrolytes as primary coagulants did n o t give good
clarification. This may be due to the relatively low particle concentration,
thus making collisions less frequent. However, alum with an anionic polymer
gave the best treatment in the case of clays. Although turbidity removal
values were n o t always higher than for alum alone, the flocs were larger
and settled three times as quickly. The addition of clay as a settling aid
did n o t improve t r e a t m e n t and merely increased the a m o u n t of precipitate
(making it uneconomical as well).

CONCLUSIONS

1. Setting tests in seawater indicate that a sedimentation tank with 1--3 h

residence time could give 50--70% turbidity removal. The use of clays as
settling aids gives practically no advantage.
2. The best treatment by flocculation in the seawater tested was by
aluminum sulfate dosages of 20--30mg/1 with an anionic polyelectrolyte
flocculant aid at concentrations of 0.025--0.1 mg/l.
3, A combination of alum and an anionic polyelectrolyte gives the best
clarification in artifical seawater containing clay -- about 70--98% turbidity
removal.
4. Algae do n o t affect the turbidity level at the concentrations most
c o m m o n l y f o u n d in seawater, i.e. less than 103 cells/ml. It is possible to
remove them by 45--75% with flocculation using alum or alum and an
anionic polymer.
5. A particle counter is useful for the evaluation of the flocculation process
and shows t h a t the percent removal of particles is greater than the turbidity
removal in the range tested.
 241

ACKNOWLEDGEMENT

This work was supported by a grant from Mekorot Water Company Ltd.
and by a scholarship from the Environmental Protection Service, Ministry
of the Interior, Israel.

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