Journal of Water Process Engineering 27 (2019) 193–204

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Journal of Water Process Engineering

journal homepage: www.elsevier.com/locate/jwpe

Revisiting of coagulation-flocculation processes in the production of potable T

water
F.K. Katrivesisa, A.D. Karelab, V.G. Papadakisa, C.A. Paraskevab,c,
⁎

a
Department of Environmental & Natural Resources Management, University of Patras, GR30100, Greece
b
Department of Chemical Engineering, University of Patras, GR26504, Greece
c
Institute of Chemical Engineering Sciences, FORTH/ICEHT, GR26504, Greece

ARTICLE INFO ABSTRACT

Keywords: Water Treatment Plants treat "flushy" raw waters and the majority use electrolytes and polyelectrolytes for the
Water treatment removal of the solid and organic impurities included in surface waters. The dose of the used reagents depend
Coagulant strongly on the nature of the incoming surface water and its turbidity. Turbidity is due to the suspended particles
Flocculant in the source water and up to date is main criterion for the appropriate choice of the electrolyte and poly-
Chitosan
electrolyte nature and dosage. One of the main findings of the present work is that the selection of the appro-
CMInulin
PDADMAC
priate dose of coagulants and flocculants as a linear function of turbidity is not right, especially for the large
values of turbidity. The most common electrolytes Aluminum sulfate and PolyAluminiumChloride together with
the polyelectrolyte PolyAcrylaMide, are tested for their effectiveness in the removal of suspended particles and
their results discussed based on the particle’s ζ-potential and size distribution. These common reagents have
raised public health concerns due to the residual aluminium and acrylamide which remain in treated water and
at produced sludge. Thus, the present work examined and suggests the use of polymers as the natural Chitosan
and CMInulin and the synthetic PolyDiallylDiMethylAmmoniumChloride, as alternative, environmentally
friendly coagulants, for their performance on the treatment of potable water. The new reagents proved to reduce
the turbidity of the surface water up to 96%.

1. Introduction
Drinking water must be safe for the health of the consumers and
contain all the elements that make it drinkable, e.g. the correct pH, the
correct mineral concentration and the absence of any kind of micro-
organisms. Its quality shall be ensured by the authorities of municipal
treatment plant, since it is an indicator of the health and well-being of a
local society. Drinking water from any source (lakes, rivers, under-
ground water, and sea) should be carefully and thoroughly processing
before consumption. Removal of turbidity from river water is a problem
faced by water treatment plants for producing potable water. The
properties of the raw water depend on the amounts of dissolved in-
organic, organic materials and gases and the presence of any microbial
content. The most noticeable properties in the raw and treated water
are: inorganic and organic matter concentration, pH, temperature,
turbidity, color, conductivity, hardness and the presence of pathogenic
or non-pathogenic microorganisms. The selection of the appropriate
treatment method for the raw water depends mainly on the nature and
the origin of the water and the demands set by the end user [1]. Usually
groundwater is clean enough and only reagents for disinfection are
added for the protection from pathogenic bacteria. Sea water treatment
is performed with Reverse Osmosis or Nanofiltration processes to re-
duce the high salinity concentrations. Surface waters (lakes or rivers)
are the most common sources for the production of drinking water and
their effective treatment, usually, involves a combined scheme of
physicochemical processes, such as coagulation, flocculation, filtration
in gravity or pressure filters and disinfection.
Coagulation and flocculation occur in successive steps aimed to
overcome the forces stabilizing the suspended particles in the aqueous
solution. In coagulation, which is the most important physicochemical
operation in potable water treatment, coagulants are added in order to
reduce the electrical charge among the suspended particles and re-
spectively in flocculation, flocculants are added to enhance the collision
and the growth of flocs. In this regard it should be pointed out that
dosage of destabilisation reagent is a very important factor influencing
the overall quality of the purified water as well as the economy of the
purification process [2]. In most cases the particles in natural waters
have a strong negative charge on their surfaces that forces particle to

⁎
Corresponding author at: Department of Chemical Engineering, University of Patras, GR26504, Greece.
E-mail address: takisp@chemeng.upatras.gr (C.A. Paraskeva).

https://doi.org/10.1016/j.jwpe.2018.12.007
Received 14 September 2018; Received in revised form 4 December 2018; Accepted 15 December 2018
2214-7144/ © 2018 Elsevier Ltd. All rights reserved.
F.K. Katrivesis et al. Journal of Water Process Engineering 27 (2019) 193–204

remain far from each, forming stable solutions with suspended particles polymers will be needed for the treatment of raw waters with high
means. Coagulants destabilize the colloidal particles allowing the initial turbidity values and possible content of natural organic matter.
creation of micro-flocs. Extra addition of flocculant reagents helps the Since Alum and PAC are still in practice in many municipal treat-
aggregation of microflocs to form larger and denser flocs that can be ment plants, the present work revisited the coagulation flocculation
easier precipitated in sedimentation tanks [3]. Electrolytes such as alum processes with Alum and PAC and evaluated the process for the selec-
(aluminum sulfate, Al2SO4) and PAC (polyaluminium chloride, AlnCl(3n- tion of the proper concentration of electrolytes, which is based so far,
m)(OH)m) are widely used as coagulants while PAM (polyacrylamide, on the turbidity value of the raw water.
(C3H5NO)n), is used as a flocculant of the formed microflocs by the
electrolytes [4,5]. Despite the fact that Alum, PAC and PAM are quite
effective in the removal of suspended particles, there is a great debate 2. Experiment methods and materials
on the problems caused on public health due to the amount of alumi-
nium ions that are remained after the treatment with Alum and PAC The target of the experiments in the coagulation process is to create
and are associated with the Alzheimer’s disease [6–8] and the presence a small flock that will consist of both the hydrophobic solids and the
of acrylamide which also has been accused as a threat for human health hydrophilic organic suspended solids. The choice of the optimum dose
because it causes neurological disorders [9–11]. However, Alum and of each flocculant was made by a combination of observations and
PAC are still in use in many municipal and industrial plants because the measurements, particularly based on the measurements of the ζ-po-
cost of these electrolytes is quite low and affordable for industrial ap- tential, the suspended and dissolved solids particle size distribution and
plications. Beyond the problems for human health the use of Alum the UV254 absorption. It was observed that the suspended solids in the
creates technical problems. Renault et al [12], reported that Alum test samples are characterized by a negative charge (negative values of
produces abundant sludge that is difficult to dehydrate and treated ζ-potential). The cationic character of the electrolytes was of vital im-
further, the formed flocs are not very well resistant to external me- portance in neutralizing the ζ-potential so as to produce the desired
chanical distortions, and the removal efficiency depends strongly on the effects in reducing turbidity. The decrease in pH and the COD values are
pH. Moreover, the use of Polyaluminum Chloride and Polyacrylamide key factors for the selection and dose of the flocculant.
in this process has more drawbacks such as the fact that it reduces water
alkalinity, it is strongly pH dependent and it can cause secondary pol-
lution through the disposal of the produced sludge. 2.1. Methods
Therefore, the present work focuses on the investigation of new
reagents based on natural material as the chitosan and inulin and a new 2.1.1. Experimental arrangement - jar test
synthetic polymer, the PolyDiallylDiMethylAmmonium Chloride The experimental procedure must be representative of the water
(PDADMAC), that could form complexes and would harm human’s treatment unit so as to provide useful results. There are several critical
health. PDADMAC has found to work effectively for the removal of parameters to consider, such as the intensity and duration of the mixing
suspended particles and part of the organic heavy load of agroindustrial process as well as the settling time. The Jar test procedure (Fig. 1) was
wastewaters [13,14]. followed in order to carry out the experimental series in this work, so as
Chitosan is reported as an eco-friendly approach [12,15] for the to select and quantify an appropriate treatment schedule to remove the
treatment of water in different application in fields such as engineering, suspended solids from raw water. The tests are carried out on the FLOC-
biotechnology, pharmaceuticals, etc. Chitosan is a biodegradable 6 Device from Raypa Company, where six beakers of 600 ml each were
polymer, nontoxic with high molecular weight linear cationic chain used. Initially, a coagulant is added with fast stirring (1min@250rpm)
[16]. Ran Yang et al [15], reported the use of Chitosan based floccu- taking place, followed by flocculation of the system with or without the
lants for the removal of different pollutants as inorganic suspended addition of flocculant with gentle stirring (10min@50rpm) taking
solids, heavy metals, humic acid, microorganism, raw natural water, place. Afterwards, the system is allowed to precipitate for 90 min and
textile and paper production effluents, etc. According to the report of finally, samples were taken from the supernatant formed. Subsequently,
Zeng et al [17], where the effectiveness of Chitosan with traditional measurements of turbidity, pH, TS, TSS, TDS, zeta potential, UV254,
chemical flocculants was compared, the required dosage of Chitosan is conductivity, hardness, alkalinity, particle size, etc. were carried out for
less, the process shows a faster depositing velocity, a higher efficiency further analysis and processing.
in the removal of COD, SS and metal ions and the obtained sludge can
be treated more easily compared with sludge received with classic
flocculants (e.g. PAM). Chitosan was also reported as a reagent that is
used in hybrid material which is composed of two or more different
components in one polymeric matrix. A second natural compound
known for its extra flocculant properties is the carboxymethyl inulin
(CMI or CMInulin). The efficiency of CMI has been studied in different
aqueous suspensions and is considered also as a novel flocculant for
wastewater treatment [18]. The potential of using biopolymers chitosan
and inulin, in the coagulation process has received limited attention so
far [16,19], while many studies have focused on their use for industrial
waste treatment.
Apart from the natural coagulants, the organic polyelectrolyte
PDADMAC has been studied as well for its effectiveness in the removal
of suspended particles. PDADMAC is a high charge density polyelec-
trolyte which has been effective in the removal of hydrophobic natural
organic matter (NOM) [20,21]. An important advantage of PDADMAC
is the fact that during the coagulation/flocculation process smaller
amounts of sludge is produced which is easier to dewater. In Bauer et al
[22], results for flocculation and stabilization of colloidal particles are
presented at very low concentrations of PDAMAC or other copolymers
of DADMAC (0.1-0.3 mg/L). This is a promising result that fewer Fig. 1. Snapshots from the visual experiment observation.

194
F.K. Katrivesis et al.
2.1.2. Turbidity measurement method
Turbidity is a measure of purity and, therefore, of the quality of
water. It is formed by insoluble and suspended particles -organic or
inorganic- contained in water. It was measured on the device SMART3
Colorimeter of LaMotte Company, which compares the radiation scat-
tered by the particles contained in the sample with that scattered by a
reference standard sample.
2.1.3. ζ or z-potential measurement method
The ζ-potential is a measure of the electrical potential of the parti-
cles and indicates the repulsive interaction among them. The charge of
the particles is determined by measuring their speed as they move due
to electrophoresis. ζ-potential with a zero value or a value near zero
means that the conditions for the aggregation of particles are optimum
[23]. Zeta potential is an indirect evaluation of particle surface charge,
evaluating electrokinetic properties as related to coagulant dose
[24–26]. So, zeta analyzers represent the best available analytical
technology for optimizing the coagulation of difficult to treat waters
[27]. Therefore, by monitoring the zeta potential, the use of flocculants
can be adjusted to determine optimal doses for the coagulation/floc-
culation process [28]. Studies in the laboratory have shown that when
operating in a ζ-potential range between −10 mV and + 5 mV, the
removal of particles and colloids in raw water is maximized [29]. ζ-
potential and conductivity were measured at the Zetasizer NanoS de-
vice of Malvern Company.
2.1.4. Total solids (TS) measurement method
Total solids are the solid residue in a sample of water after eva-
poration at 105 °C and weighing. They are a measure of the suspended
solids (TSS) and dissolved solids (TDS), present in water. High values of
total solids reduce the purity of water. The total solids contained in the
samples were measured by Standard Methods method 2540B. The MLW
oven and the Shimadzu AUW220 analytical balance were used.
2.2. Materials
Aluminum sulfate, [Al2(SO4)3·16H2O, alum] is an inorganic elec-
trolyte prepared by adding aluminum hydroxide to sulfuric acid or by
heating aluminum metal in sulfuric acid solution, it has a density of
1.34 g/ml and a solids content of 48.5%. 60.62 g of aluminum sulfate
powder was dissolved in 1000 ml of water in the laboratory with a
density measured at 1.03 g/ml.
PolyAluminiumChloride, [AlnCl(3n-m)(OH)m, PAC] is an inorganic
polyelectrolyte produced by the reaction of aluminum with hydro-
chloric acid, having an Al2O3 content of > 17% and a relative density of
1.35gr/ml.
PolyDiallylDiMethylAmmoniumChloride, [(C8H16NCl)n, PDADMAC]
is a synthetic, biodegradable and non toxic polyelectrolyte with very low
molecular weight and medium charge density (Sigma-Aldrich
522376.1 L), produced by the reaction of allylchloride (propylene
chloride) with dimethylamine and polymerization with a quaternized
ammonium salt. PDADMAC 35% w/w was used with a density of
1.09gr/ml.
Chitosan, [(C6H11O4N.HCl)n, CH], is a natural, antibacterial and
environmentally friendly biocompatible polymer with medium mole-
cular weight and charge density, purchased from Sigma-Aldrich-
448877.50 G, and consists of 1:4 random copolymerization of D-gluco-
samine and N-acetyl-D-glucosamine. Made by treating chitin shells from
shrimps and other crustaceans with an alkaline substance that causes
75˜85% deacetylation of chitin. In order to make a 1:1000 chitosan
solution, 1 g of chitosan was dissolved in 997 ml of deionized water and
2 g of HCl. This solution had a density of 0.997 g/ml.
CarboxyMethyl Inulin, [(C6nH10n+2O5n+1), CMI] is a natural, linear
polysaccharide, natural carboxymethylated biopolymer polyelectrolyte,
produced from Cosun Biobased Products by reacting 25% carbox-
ymethyl groups (CMI-25) to the natural polysaccharide inulin extracted
195
Journal of Water Process Engineering 27 (2019) 193–204
from chicory roots. To prepare the solution, 1 ml of a 15% w/w solution
with a density of 1.14 g/ml is obtained and 19 g of H2O is added. The
density of the solution was measured 1 g/ml and its concentration was
0.75% w/w.
PolyAcrylamide, [(C3H5NO)n, PAM] is an anionic polyelectrolyte of
high molecular weight produced by copolymerization of weak car-
boxylic acid and acrylamide or polymerization of the acrylamide fol-
lowed by partial hydrolysis. To prepare the solution, 10 ml of a 15% w/
w solution with a density of 0.956 g/ml was dissolved in 90 ml of water.
The density of the solution was measured 0.989 g/ml and its con-
centration was 1.5% w/w.
3. Results and discussion
The present paper focuses on the understanding and optimization of
the various factors that govern the coagulation process by natural and
synthetic polymers in the treatment of surface water of the Glafkos
River, in Patras drinking water treatment plant in Achaia region.
Therefore, in the present study the effect of the doses of the already
used electrolytes, Alum and PAC and the effect of new polymers, one
synthetic (PDADMAC) and two natural (CH and CMI) on the removal of
solid content were studied, with the help of parameters such as zeta-
potential and pH, conductivity and suspended solids concentration
(TS).
Today, water from Glafkos River is processed in the local treatment
plant with PolyAluminium Chloride as a coagulant and polyacrylamide
as a flocculant. Few years ago, aluminium sulfate was used as coagulant
but it was abandoned because of the quality and the quantity of the
precipitated sludge. PAC reduces the amount of the precipitated sludge
but the concentration of aluminium anions in water has not improved.
Aluminium anion concentration in water, according to STASH
3904:1997 (ICS 130600-water quality) [30], and European standard
EC80/778/EEC (quality of water intended for human consumption)
[31], must be near the value 0.05 mg/L and with the maximum allowed
peak of 0.2 mg/L [32,33]. Polyacrylamide has already reported as re-
agent which causes problems and its limits has been set to 0.2 ppb in
drinking waters [34]. Because of the link between aluminium anion
exposure and Alzheimer's disease development [35–38], and of the link
of acrylamide with health risks such as neurological disorders and male
reproductive organs [39,40], it is necessary that the process of coagu-
lation-flocculation is optimized and dosages of aluminium ions (Al3+)
and of polyacrylamide in treated water are kept below the above va-
lues. Moreover, the use of PolyAluminium Chloride and Polyacrylamide
in this process has additional drawbacks such as the fact that it reduces
water alkalinity, it is strongly pH dependent and it can cause secondary
pollution through the disposal of the produced sludge. Furthermore, the
non-optimal chemical dosing of electrolytes and/or polyelectrolytes
may cause more problems than the initial water turbidity.
3.1. Turbidity of the raw water
Fig. 2 shows the seasonal variation of the turbidity of the raw water
for the year 2017 that fed the local treatment plant in Patras, Greece,
with 1000 to 2500 m3 per hour. As Fig. 1 shows, in the first quarter of
the year and particularly for the months January and February, the raw
water that entered the treatment plant had turbidity values above 10
NTU and for some weeks the turbidity values exceeded the value of 100
NTU and in few cases reached the huge value of 1000 NTU. In the
second quarter of 2017, the raw water had turbidity values in the range
up to 10 NTU and few peaks were appeared according to rainfalls for
May and some days in June. The third quarter of 2017, which includes
summer months, shows that the water that was coming from Glafkos
river had very low concentrations of particles apart from a week in July
and a week in August due to storms occurred in the local area those
days. The most troubled period with high particle concentrations was
the fourth quarter of the year due to prolonged rainfall, where values
F.K. Katrivesis et al.
Fig. 2. Seasonal variation of the turbidity of the raw water that fed the local water treatment plant on 2017.
for turbidity above 100 NTU were observed, which in many cases
reached 1000 NTU.
The aforementioned discussion on the turbidity of the raw water is
related to the process of coagulation that is used in local (and many
others) drinking water treatment plants. The treatment of the raw water
starts with the injection of electrolyte upon it arrives in the treatment
station and the injection polyelectrolyte in the primary sedimentation
tank. The selection of the appropriate doses of both electrolyte and
polyelectrolyte were based on empirical equations, which linearly
correlate added amount of electrolyte or polyelectrolyte with the tur-
bidity of the raw water. So, for many days or even many weeks a year,
large concentrations of reagents were used to enhance the coagulation/
flocculation of the suspended particles, concentrations that may not
needed and probably caused problems since overact doses of aluminum
remained in the residual sludge and in treated water. The choice of
concentration of electrolyte and polyelectrolyte were based on em-
pirical formulas that calculates the electrolyte (Eq. 1) and polyelec-
trolyte (Eq. 2), as a function of the turbidity
Celectrolyte = 0.103113 x Turbidity Values + 8.433543
Eq. 1 is used for the evaluation of the appropriate dose of alum only
when the turbidity was above 8.5 NTU. Polyelectrolyte was added only
when the turbidity value was exceeded the value of 9.5 NTU, in order
microflocs from coagulation process to be gathered in larger flocs and
the sedimentation to be enhanced. For turbidity values less than 8.5
NTU the choice of the appropriate dose is done on the experience of the
trained personnel of the treatment unit. The estimation of the appro-
priate PAM dose was done using Eq. 2
CPolyelectrolyte = 0.0013 x Turbidity Values – 0.012
Journal of Water Process Engineering 27 (2019) 193–204
Thus for the case of low turbidity values, small or non doses of alum
and PAM were used. In these cases the duty for the removal of the
suspended particles was transferred to the sand bed filtration process
which is effective for the treatment of water with relatively low con-
centrations of suspended particles.
However, the problems with the use of alum, PAC and PAM ap-
peared for the case of high turbidity values which was typical case in
days with storms or high raining days, in areas that feed Glafkos river
(Fig. 1). At those days treatment plant calculates high doses of alum,
PAC and PAM according to Eqs. 1 and 2. For example, for turbidity
values in the range of 100–1000 NTU the concentration of alum fluc-
tuated in the range of 20–100 mg/L which are considered as extremely
high concentrations, if aluminium ions are not been consumed during
the coagulation process. Eq. 1 was also used (incorrectly) for the eva-
luation of the appropriate doses of PAC. Alum and PAC are useful only
for the destabilization of small charged colloidal particles and not for
non colloidal particles (e.g. particles with mean size larger than 10 μm).
Fig. 3 shows the estimated values of coagulant and of the combi-
nation of coagulant plus the flocculant PAM concentrations based on
(1)
the empirical correlations (Eqs. 1 and 2), illustrated as straight lines and
the used doses of coagulants (square symbols) or combination of coa-
gulant and PAM (triangular symbols) that were used in the experi-
mental study and resulted in the reduction of the 98% of suspended
particles. It is obvious that the procedure that was followed up to day
and was based on the linear correlation of electrolytes (and/or poly-
electrolyte) doses with turbidity were not correct.
The results included in the present work showed that the high
quantities of electrolytes added in solutions with turbidity values higher
50 NTU did not affect the precipitation and rather caused problems to
(2) coagulation since they re-stabilized the suspended particles. In all
196
F.K. Katrivesis et al.
Fig. 3. Turbidity values of the raw water as a function of the electrolyte and
polyelectrolyte predicted concentrations by Eqs. 1 and 2 (Alum and PAC, red
solid line and Alum + PAM and PAC + PAM, blue solid line).Symbols and
dashed line, referred to the coagulant and flocculant doses used in the experi-
mental study that have reduced turbidity up to 98% (For interpretation of the
references to colour in this figure legend, the reader is referred to the web
version of this article).
experiments with initial measured turbidity value larger than 50 NTU,
it was found that main part of turbidity was due to large solid particles,
larger than 10 μm, up to 100 μm. These particles are not colloidal
particles which need destabilization of their surface electrical charge,
and most of them would precipitate alone in the sedimentation tank.
The extravagant dose of electrolyte will change the negative charge of
the suspended particles to positive, far from the isoelectric point where
zeta potential becomes equal to zero. Another negative effect of the
overdosing procedure is that the extra quantity of the added electrolyte
will remain in the treated water and goes to the consumption chain.
Thus the undesired contamination of the treated water with aluminium
ions is not avoided.
The experimental study showed that small concentrations of elec-
trolytes and polyelectrolytes can act properly for the removal of the
suspended particles from raw waters with high turbidity values since
the major part of the turbidity was due to the large particles that can be
precipitated alone thanks to their own gravity. More results are given in
the next section where the effects of other parameters related to the
destabilization of the colloidal particles are taken also into the discus-
sion.
Fig. 4. Turbidity reduction rates (%) as a function of the doses of (a) Alum and (b) PAC, for the treatment of raw water with different initial turbidity values.
197
Journal of Water Process Engineering 27 (2019) 193–204
4. Effect of used coagulants in raw water treatment
In the first parametric series, experiments were carried out with raw
waters with initial turbidity values of ranging from 50 NTU to 250 NTU.
The calculation of the appropriate doses of coagulant and/or flocculant
was done according to the data of the process followed until today,
using the linear equations 1 & 2 with an account of the initial turbidity
value. The use of aluminum sulfate and polyaluminium chloride give
good results in terms of the removal of initial turbidity at the predicted
values, but the used doses were quite large. Thus, high concentrations
of aluminium ions remained in the treated water and among other
things, a very big drop in the pH value was observed, followed by a
significant hardness increase, especially in the case of PAC. The 1st
experimental series was repeated with much less concentration of
coagulants and flocculants where again high removal rates of the initial
turbidity were observed. Therefore, experiments with low concentra-
tions of alum (< 15 mg/L) and PAC (< 20 mg/L) were designed and
the effect of PAM polyelectrolyte as flocculant was examined.
4.1. Alum and PAC dosing and performance
In the 1st series of experiments, the effect of the concentration of
aluminum sulfate Al2(SO4)3.16H2O] on the reduction of raw water in-
itial turbidity was investigated. Doses of 3 to 65 mg/L of alum were
used, for turbidity values of 50 to 250 NTU, as Fig. 4a shows. It is clear
that doses of alum from 10 mg/L to 30 mg/L removed more than 97% of
the suspended particles. What is interesting in Fig. 4a is the fact that for
the raw water with initial turbidity of 227 NTU the removal efficiency
was higher than in those with lower initial turbidity values 110 and 55
NTU. This remark confirms the previous discussion where it was con-
cluded that the ‘real’ turbidity value is not the one that arrives at the
inlet of treatment station but the turbidity that reflects the concentra-
tion of the colloidal particles, which remained in the suspension and
cannot be precipitated alone because of their gravity. Fig. 4b shows the
reduction of the turbidity as a function of the dose of the second elec-
trolyte that is discussed in the present work, the PAC. PAC found to
behave as a good coagulant like Alum since the reduction of the initial
turbidity was up to 99% for the same range of doses of electrolyte.
Again here it is clear that a dose of electrolyte in the range of 5–20 mg/
L reached turbidity reduction values up to 98%. The remaining tur-
bidity is due to some colloidal particles which readily will be removed
in the next processing step in the gravity filter system. In the afore-
mentioned series of experiments with alum turbidity reduction values
up to 98% were obtained without the use of flocculant earning the cost
of PAM and avoiding the neurological problems caused by the presence
F.K. Katrivesis et al. Journal of Water Process Engineering 27 (2019) 193–204

Table 1 For the case of Alum, Fig. 5e shows that for the cases of raw water with
Initial and final turbidity of raw water after 2 h sedimentation without any turbidity values of 55 and 110 NTU there was a reduction on solids
coagulants or flocculants. concentration whereas for the case of experiment with 227 NTU a re-
Initial Turbidity Final Turbidity Turbidity Reduction stabilization of the suspended particles was observed, probably of the
(NTU) (NTU @ 2 h) (%) change of the negative electrical charge to positive electrical charge
that maintains the charged particles suspended in the solution.
53 30.5 42%
The effect of the doses of Alum and PAC on the electrical charge of
54 32.0 41%
57 36.5 36% the suspended particles can be better explained by the investigation of
62 39.0 37% particle’s ζ-potential as shown in the experiments in the second series.
95 47.0 51% ζ-potential is a measure of the electrical surface charge of the particles
102 45.0 56%
and is the main index of the destabilization or the stabilization of sus-
113 61.5 46%
115 42.0 63%
pended material of the solutions. Fig. 6a and b shows that ζ-potential
120 55.0 54% values are very sensible on the concentration of electrolytes. Again here
123 63.0 49% is obvious that electrolyte doses larger than 10 mg/L resulted in the
130 60.0 54% reduction of ζ-potential to more negative values. It is known the sta-
132 51.0 61%
bilization of suspended particles occurs at high negative (< −20 mV)
133 33.0 75%
200 31.0 85% or high positive values (> + 20 mV). If destabilization is intended, one
205 34.0 83% shall choose doses of electrolytes which limit ζ-potential in the range of
209 61.0 71% −2 mV to + 8 mV [42]. Depending on the nature of the suspended
212 20.0 91%
particles a large variation of electrolyte may lead to the change of ζ-
215 37.0 83%
240 52.0 78%
potential from positive values to negative values (case of initial tur-
bidity of 227 NTU in Fig. 6a), or to inverse the negative charge to
positive values (case of initial value of 106 NTU in Fig. 6b). Un-
fortunately Fig. 6a and b didn’t show a range of electrolyte dose that
of the polyacrylamide substances. will limit ζ-potential to the range of -5 and + 5 mV. However, values
As Table 1 shows the major part of the turbidity reflects the particles close to −10 mV or even close to −20 mV suggest that the solutions
that are quite heavy and can precipitate alone without the use of a can be destabilized and particles will reach each other and form mi-
coagulant or a flocculant. Sand grains or silt or clay particles and sus- croflocs that subsequently will be gathered by a flocculant to form large
pended organic matter present in turbid water have specific gravity and heavy flocs and precipitate seasonal (April through May) changes
between 1.04 and 2.65. The particles having specific gravity more than that occur naturally to the raw incoming water supply at this location.
1.2 can precipitate more easily while the lighter particles do not settle Zeta potential measurements can be used as indicators of optimal do-
readily and their removal becomes difficult. The velocity of flow sage for flocculating agents: zeta potential as an indicator of particle
transporting a particle horizontally, the viscosity of liquid offering stability and charge, and turbidity as an indicator of optical clarity and
frictional resistance and the size and shape of particles oppose the particle presence. Together they are good tools for determining the
settlement of particles. The process of plain sedimentation may remove effectiveness of agents as well as optimizing the efficiency and economy
about 60% of the suspended matter and 75% of bacteria. Thus, plain of the operation of a water treatment facility. Frequent measurements
sedimentation can reduce high loads on sandbed filters. The high of zeta potential have replaced the need to conduct jar tests to de-
temperature, correct pH value, proper inlet and outlet flows, large re- termine alum dose [43].
tention periods and appropriate dimensions are the favorable condi-
tions for an effective sedimentation. 5. Study on the performance of synthetic polymer and
Measurements in the jar test experiments indicated that with a pre- biocoagulants on the removal of river water turbidity
treatment time equal to the clarification (=coagulation/flocculation/
sedimentation) treatment time, the values of turbidity reduction ranged Polymeric flocculants were mainly selected as alternative agents for
from 40 to 80 percent (Table 1). The smaller percentages correspond to coagulation and flocculation and for the reduction of the problems that
smaller turbidity initial values (50–110 NTU), while the larger ones in are caused using the inorganic electrolytes, (pH, reduction, con-
great initial turbidity (210–260 NTU). Having thus, raw water with ductivity and TSS increase and harmful effects to human health.
initial turbidity 55 NTU, the user shall calculate coagulant dose for 32 However, the flocculation mechanisms are not the same in polymeric
NTU initial turbidity from the pre-sedimentation output, while re- and inorganic flocculants and shall be taken into accounts when a water
spectively for turbidity of 265 NTU, the user will need coagulant for just treatment process is to be designed.
55 NTU turbidity. As reported in Stechemesser et al [44] and Bratby [11], inorganic
Fig. 5 shows the effect of Alum and PAC on some of the major electrolytes can form multi-charged polynuclear complexes with en-
parameters that influence the quality of the treated water, such as the hanced adsorption properties when are added in colloidal aqueous
pH, the conductivity and the concentration of Total Solids, TS. Fig. 5a suspensions. These metal inorganic coagulants can rapidly be hydro-
and b show that doses of Alum and PAC over 10 mg/L resulted in the lyzed and result in direct colloidal destabilization since they neutralize
substantial reduction of the pH of the treated water. Thus, despite the the negative charge of the colloids and allow forming of aggregates and
fact that high turbidity reduction rates could be obtained at high con- consequently enhance the sedimentation. However, this rapid hydro-
centrations (> 10 mg/L) of coagulants, these doses shall be avoided lysis is carried out in an unsustainable manner and the destabilization
because reduction of pH below 6.5 in drinking water is not re- performance depends on the effectiveness of rapid mixing, dosage,
commended by the international institutions (Environmental Protection change in pH, temperature and nature of the solution, which determine
Agency, World Health Organization) [41,32]. Fluctuations on the which type of hydrolysis is effective. This is referred to as a major
conductivity of the treated water as a function of electrolyte doses are disadvantage because there is inability to control the nature of the
illustrated in Fig. 5c and d. Conductivity in most of potable water shall hydrolysis species formed when the coagulant is introduced into the
be closed to 0.6 mS/cm and reduction up to 0.2 mS/cm which was solution.
observed in Fig. 5c and d shall be avoided. Fig. 5e and f shows the Total On the other hand, the polymeric flocculants of the various struc-
Solids concentration as a function of electrolyte doses for Alum and tures can act either by polymer bridging or by load neutralization or by
PAC. Again here fluctuations of TS values are observed in Fig. 5e and f. applying both mechanisms at the same time. According to Elimelech

198
F.K. Katrivesis et al.
Fig. 5. Effect of Alum and PAC doses on the final pH of the treated water, 5a and 5b, on the conductivity of the treated water, 5c and 5d and on TS concentration, 5e
and 5f.
[45], flocculation is a very complex process involving 5 stages: a)
mixing the polymer with the colloidal particles, b) the polymer mole-
cules adhere to the surface of the colloids, c) reassembling the polymer
molecules on the surface of the particle, (d) coagulation of the particles,
and (e) the degradation of the agglomerates due to the shear during the
rotary mixing of the suspension. All of this can be both concurrent and
competitive and often compete.
The present study involves study of the ζ-potential and polymer
adsorption of the flocculated particles as a function of polymer dosage
for better understanding of the flocculation mechanism operating for
each charged polymer. Polymer charge density influences the
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Journal of Water Process Engineering 27 (2019) 193–204
configuration in solution since for a given molecular weight, the charge
density increases and stretches the polymer chains through increasing
electrostatic repulsion between charged units, thereby increasing the
viscosity of the polymer solution.
5.1. PDADMAC dosing and performance
In the 3rd experimental series, the effect of the concentration of the
inorganic, synthetic polymer PolyDiallylDimethylAmmonium Chloride,
[(C8H16NCl)n], on the main physicochemical properties of the raw
water, was studied. Doses of 0.5 to 80 mg/L were tested for initial
F.K. Katrivesis et al.
Fig. 6. Variation of Zeta potential values for different doses of (a) alum and (b) PAC in experiments with raw water of different initial values.
Fig. 7. Performance of PDADMAC doses on turbidity reduction rate for the
treatment of raw water with different initial turbidity values.
turbidity values of 50 to 350 NTU. The reduction of turbidity for all
electrolyte doses was over 70%, while best results are obtained at tur-
bidities over 200 NTU with small coagulant doses 0.8–8 mg/L. As Fig. 7
shows, PDADMAC doses over 10 mg/L resulted in the deterioration of
the removal of initial turbidity as it happened in the case of Alum and
PAC. Values of PDADMAC dose close to 0.1 mg/L didn’t help the re-
moval of particles and the best performance took place at PDADMAC
doses close to 1 mg/L while in the case of ALUM and PAC the corre-
sponding best performance (in terms of all parameters under con-
sideration) was from 10 to 30 mg/L.
As for the physicochemical parameters are concerned, Fig. 8a to 8d
showed that values of PDADMAC close to 1 mg/L do not alter drama-
tically the values of those parameters. Fig. 8a shows that the variation
of the pH of the treated water was close to 7 for the entire and wide
range of the tested doses of PDADMAC. Similar conclusions can be
derived from Fig. 8b where the conductivity of the treated water was
plotted against the doses of PDADMAC. In all cases the conductivity
remained close to 0.5 mS/cm (acceptable value for drinking waters)
apart for the case where the concentration of the polyelectrolyte
reached the 100 mg/L. Fig. 8c shows the effect of PDADMAC dose on
the concentration of Total Solids that remained suspended in the
treated water. Again the best performance in terms the lowest con-
centration of suspended particles was observed for low doses of
PDADMAC, and the treatment of any kind of raw water with initial
turbidity values in the range of 50 to 300 NTU shall not exceed the
10 mg/L. For values above 10 mg/L the TS concentration increased,
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Journal of Water Process Engineering 27 (2019) 193–204
leading to the conclusion that the destabilized particles at low con-
centrations were re-stabilized again at high concentrations and the
particles repelled each other. This is also shown and explained in
Fig. 8d, where the zeta potential was plotted again the doses of
PDADMAC. Fig. 8d shows that at very low concentrations close to
0.1 mg/L or far from the optimum value which seemed to be the 1 mg/
L, the electrical charge of the particles remained high (positive or ne-
gative) and in some cases there is inversion on mean value of the zeta
potential of the suspended particles from negative values to positive
high values.
5.2. Chitosan dosing and performance
In experiments of 4th series, the effect of the natural polymer chit-
osan was examined. Doses from 0.1 to 110 mg/L were used for initial
turbidity values of 50 to 250 NTU. Although the decrease in initial
turbidity did not approach the values of alum and PAC, it was over 75%
for almost all electrolyte doses and was higher at lower doses. The re-
commended doses of Chitosan are among 1 and 10 mg/L for all type of
raw waters that are arrived at different initial turbidity values. The
remaining turbidity in terms of suspended particles can be further
treated in the system of sand bed filters where no chemicals are needed.
As for the other physicochemical parameters, Fig. 10a–d shows that
values of the natural polymer Chitosan among 1 and 10 mg/L illu-
strated the best performance, after two hours sedimentation. Fig. 10a
shows the pH variation on the dose of Chitosan and showed that pH
ranged from 6.5 to 8.0 which is according to the environmental stan-
dards. The same behavior is illustrated in Fig. 10b where conductivity
of the treated water was plotted against the dose of Chitosan and few
fluctuations from the initial values of conductivity were observed for all
tested values of Chitosan and for all type of raw waters with different
initial turbidity. Fig. 10c shows the TS concentration as a function of
Chitosan dose and that non important distortion in TS values were
observed. Fig. 10d where ζ-potential values is plotted against Chitosan
doses, showed that the charge of the suspended particles showed better
behavior for small coagulant doses, especially close to 10 mg/L
5.3. CM inulin dosing and performance
In 5th series experiments, the effect of the natural polymer
CarboxyMethyl Inulin was examined. Doses of 10–120 mg/L were used
for initial turbidity values of 50–250 NTU. As far as the decrease in
turbidity is concerned (Fig. 11), CM Inulin worked better at large initial
turbidity values and at higher electrolyte doses, but is not so effective as
the other tested natural polymer, the Chitosan.
F.K. Katrivesis et al.
Fig. 8. Effect of the PDADMAC doses on the (a) final pH, (b) conductivity, (c) Total Solids concentration and (d) ζ-potential values of the treated water.
Fig. 9. Performance of Chitosan doses on turbidity reduction rate for the
treatment of raw water with different initial turbidity values.
As for the other physicochemical parameters are concerned,
Fig. 12a–d showed that values of the CMI among 10 and 100 mg/L gave
the best performance. Fig. 12a shows the pH variation with CMInulin
doses and for all tested waters at different initial turbidity values. It is
clear that the pH in the treated water never moved away from the range
6.5–8.0 set by the rules for drinking water. Fig. 12b, where the changes
of the conductivity are shown as function of CMI doses, suggested not to
exceed inulin doses more than 20 mg/L because the conductivity in-
creased more than 800 μS/cm which is far from the mean conductivity
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Journal of Water Process Engineering 27 (2019) 193–204
values in tap water [46]. As for the Total Solids, Fig. 12c shows that
doses of inulin close to 10–20 mg/L kept reasonable concentrations of
solids within the treated water but for very large doses the concentra-
tion of particles increased significantly. Finally, Fig. 12d, where the ζ-
potential of the suspended particles is shown, suggests that none of the
tested values of inulin resulted in the reduction of the zeta potential and
all values were in the range of -10 to −20 mV for all types of raw water
at different initial turbidity values. Any action of inulin shall be ad-
dressed to the formation of clusters of particles with the polymeric
chains and not due to the destabilization of the suspended particles.
5.4. Comparisons among the suggested polyelectrolytes and the old
inorganic electrolytes
As Figs. 4,7,9 and 11 show the turbidity reductions of polymeric
flocculants were general lower than those of the case of inorganic
electrolytes. However, the main target of the present work was not to
reach a 100% reduction of the turbidity but to suggest new coagulants
in order to eliminate the disadvantages of the used of the inorganic
electrolyte. As pointed above aluminum-based electrolytes were found
to cause reduction of the pH at high concentrations, increase the con-
ductivity and solids concentration and what is more important, these
electrolytes have accused to cause harm effects to human health. As the
laboratory experiments show, the doses of polymeric flocculants were
optimized and show that turbidity reduction values up to 90–94%. The
remaining turbidity could readily be removed in the sand filtration
process that follows the coagulation/ flocculation process.
Experiments in jar-tests were implemented using PDADMAC,
F.K. Katrivesis et al.
Fig. 10. Effect of Chitosan dose on the (a) final pH, (b) conductivity, (c) Total Solids concentration and (d) ζ-potential of the treated water.
Fig. 11. Performance of CMInulin doses on turbidity reduction rate for the
treatment of raw water with different initial turbidity values.
Chitosan and CMInulin showed that the biopolymers have the potential
and the performance to substitute prior used coagulants/flocculants in
water treatment which were accused to harm human health (Alzheimer,
neurological problems). Experiments showed, as we can see in
Fig. 13a,b, that their use as coagulant/flocculant in potable water has
proven to be beneficial, because they are effective in small doses, allow
reduction of quantity and increase the quality of the sludge produced
and at the same time their impact on pH and alkalinity is insignificant,
as reported also in literature. Concerning PDADMAC, it was found to be
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Journal of Water Process Engineering 27 (2019) 193–204
effective as both coagulant and flocculant and its best performance was
obtained at very low concentrations close to 1 mg/L.
All tests also determine that it is necessary to include ζ-potential in
the equitation of reagents dose evaluation. Since optimum coagulation
chemistry is generally known as “the lowest dosage of all chemicals that
results in the desired removal of contaminants with the lowest total
operating costs”, ζ-potential will make the dose estimation more ac-
curate while it evaluate the interfusion of lower coagulant/flocculant
doses.
Another remarkable conclusion derived from the present study is
the fact that the polymeric flocculants show more evident re-stabiliza-
tion at overdose than inorganic coagulants that suggest controlled in-
jection of the polyelectrolytes into water stream and frequent mea-
surements of the tested parameters (ζ potential, pH, TSS, conductivity,
etc.). This re-stabilization effect is different among the tested polymers.
The synthetic polymer (PDADMAC) has high charge density than the
charge of the tested water particles, which may lead to increase of the
factorial growth of ζ-potential, resulting in particle re-stabilization and
decrease of sedimentation performance. In the case of the natural
polymers Chitosan and CMInoulin, the increase of the dose acted gentle
to the value of ζ- potential, with re-stabilization to occur mainly be-
cause of weakly coherence of flocs.
6. Conclusions
The first scope of this study was the investigation of the effective-
ness of the known electrolytes, Alum and PAC and polyelectrolyte, PAM
on the removal of suspended particles in raw water. We found out that
F.K. Katrivesis et al. Journal of Water Process Engineering 27 (2019) 193–204

Fig. 12. Effect of CMInulin doses on the (a) final pH, (b) conductivity, (c) Total Solids concentration and (d) ζ-potential for raw waters with different initial turbidity
values.

although they have a very good turbidity reduction response, the choice
of the appropriate dose, based on a linear correlation of turbidity and
dose of electrolyte, is wrong since the most part of the high turbidity
values is due to large particles that can precipitate alone because of
their gravity. Therefore, it is suggested a natural pre-sedimentation
process for up 1 h to take place in order large particles to be removed
and then to add doses of electrolytes calculated on the ‘real’ turbidity
values due to the suspended colloidal particles. The process of plain
sedimentation may remove about 60% suspended matter and 75%
bacteria. Measurements in the jar test experiments indicated that with a
pre-treatment time equal to the time needed for the coagulation, floc-
culation and sedimentation treatment, the values of turbidity reduction
ranged from 41% (for initial turbidity in the range of 50–100 NTU) up
to 83% (for turbidity values 210–260 NTU).

Fig. 13. Effect of coagulant dose on the (a) Turbidity reduction rate and (b) ζ-potential value for the three suggested new coagulants/flocculants.

203
F.K. Katrivesis et al.
As second target of the present work, new natural polymers were
tested for the coagulation and flocculation of suspended particles con-
tained in river raw water with different initial turbidity values and the
already applied coagulation/flocculation process was revisited and
evaluated for its effectiveness. Experiments using PDADMAC Chitosan
and CMInulin showed that the biopolymers have the potential and the
performance to substitute prior used coagulants/flocculants in water
treatment which were accused to harm human health (Alzheimer,
neurological problems). Also experiments show that ζ- potential mea-
surements are key parameters to monitoring and maintaining optimal
conditions in water treatment facilities. This can be especially im-
portant during upsets or naturally occurring seasonal changes in water
production.
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