Applied Clay Science 146 (2017) 343–349

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Applied Clay Science

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

Research paper

Drinking water treatment sludge as an efficient adsorbent for heavy metals MARK
removal
S.A. Abo-El-Eneina, Ahmed Shebla,⁎, S.A. Abo El-Dahabb
a
Chemistry Department, Faculty of Science, Ain Shams University, Abbassia 11566, Cairo, Egypt
b
Holding Company for Water and Wastewater, Egypt

A R T I C L E I N F O A B S T R A C T

Keywords: Green chemists paid much more attention towards the alternative ways to reutilize waste materials instead of its
Drinking water treatment sludge disposal in a non-ecofriendly manner. In this study, drinking-water treatment sludge (DWTS), which is a by-
Lead cadmium nickel removals product resulted from drinking water treatment plants, was successfully applied as an adsorbent for Pb(II), Cd(II)
Adsorption and Ni(II) removal from wastewater. The physicochemical characteristics of DWTS were investigated using X-ray
Quartz
diffraction (XRD), X-ray fluorescence (XRF), scanning electron microscopy (SEM) and N2 adsorption-desorption
Illite
isotherms.
Albite
The XRD analysis revealed that the DWTS under study consists of quartz and illite phases which had been
reported for their adsorption efficiency. Firing of DWTS at 500 °C causes the appearance of albite phase in
addition to previous ones which enhances the adsorption capacity of these materials. The influence of different
parameters such as firing temperature of DWTS, contact time, pH, DWTS dose and initial metal ions con-
centration on the adsorption of heavy metal ions and, consequently, on their removal were investigated. DWTS
exhibit an adsorption efficiency towards Pb(II) > Cd(II) > Ni(II). The extremely high efficiency of DWTS
towards Pb(II) adsorption can nominate it as a specific low-cost adsorbent for Pb ions.

1. Introduction
Drinking-water treatment sludge (DWTS) is a by-product from the
coagulation-flocculation process using aluminum or iron based salts to
precipitate clay, colloidal particles, algae and humic substances from
water resources. Due to its high production rate and its environmentally
unfavored disposal to landfill, several researchers paid a considerable
attention for using this waste material in different applications espe-
cially those of low cost. The chemical composition of DWTS varies
depending on the source of water under treatment as well as the type of
coagulant used. These applications include utilization of DWTS for
ceramic products (Zamora et al., 2008; Kizinievic et al., 2013; Mymrin
et al., 2017), cement and concrete production (Rodríguez et al., 2010;
Sales et al., 2011; Hwang et al., 2017) as well as wastewater treatment
as an adsorbent for the removal of phenolic compounds (Fragoso and
Duarte, 2012), phosphates (Razali et al., 2007; Piaskowski, 2013), dyes
from textile industry discharge (Chu, 1999) and heavy metals (Ippolito
et al., 2011; Siswoyo et al., 2014).
Pollution of water resources by heavy metals such as lead, cadmium
and nickel which are continuously discharged in huge amounts from
different growing industrial activities has been recognized (Ribeiro
et al., 2012; Yang and Cui, 2013; Keränen et al., 2015). These heavy
metals are considered as hazardous materials where their toxicity to
living organisms comes from their tendency to accumulate in living
tissues since they are not biodegradable causing several health hazards
like kidney problems, anemia, lung cancer and dyspnoea
(Ahmaruzzaman, 2011; Visa et al., 2012). Therefore, a tremendous
number of researches deals with the removal of such heavy metals
especially via adsorption process (Bailey et al., 1999; Babel and
Kurniawan, 2003; Ngah and Hanafiah, 2008; Tofighy and Mohammadi,
2015; Castaldi et al., 2015; Isaac et al., 2015; Dobrowolski et al., 2017;
Azimi et al., 2017).
The aim of this study is to get a beneficial use of DWTS as a low cost
adsorbent for the removal of lead, cadmium and nickel metal ions from
wastewater.
2. Experimental
2.1. Starting materials
The material used in this investigation is DWTS waste produced
during 4 months from El-Fustat drinking water treatment plant (Egypt).

⁎
Corresponding author.
E-mail address: a_ahmed@sci.asu.edu.eg (A. Shebl).

http://dx.doi.org/10.1016/j.clay.2017.06.027
Received 1 May 2017; Received in revised form 13 June 2017; Accepted 23 June 2017
Available online 27 June 2017
0169-1317/ © 2017 Elsevier B.V. All rights reserved.
S.A. Abo-El-Enein et al.
Table 1
Chemical oxide composition of DWTS.
Oxide Weight, %
SiO2 36.51
Al2O3 22.21
Fe2O3 5.65
CaO 2.66
Na2O 1.35
MgO 1.34
K2O 0.49
Sulphate as SO3 0.08
Loss on ignition (L.O.I) 28.1
Its chemical composition is given in Table 1.
2.2. Preparation and firing of DWTS
DWTS was dried at 110 °C for 48 h, and then crushed. The crushed
DWTS was fired at different temperatures of 100, 400, 500, 600 and
700 °C for a period of 2 h and then quenched in air.
2.3. Chemicals
The synthetic solutions used in this study were prepared from Pb
(NO3)2 99% produced by LOBA Chemie, Cd(NO3)2·4H2O 99% produced
by LOBA Chemie and Ni(NO3)2·6H2O 98% produced by Oxford la-
boratory reagent. Solutions of 0.1 M nitric acid and ammonium hy-
droxide were used to adjust pH.
2.4. Batch adsorption experiments
Batch adsorption experiments including the effects of firing tem-
perature, contact time, adsorbent dosage, initial metals concentration
and initial solution pH were studied. Batch experiments were carried
out at room temperature by addition of known weight of burnt DWTS
into a number of 100 mL glass stoppered conical flasks on a rotary
shaker at 200 rpm containing individual 50 mL of nitrate solutions of
Pb(II), Cd(II) or Ni(II) (100 mg/L) in distilled water.
The effect of firing temperature was conducted to DWTS by shaking
0.5 g of DWTS, after burning at different temperatures (100, 400, 500,
600 and 700 °C), with 50 mL of the individual nitrate solutions of Pb
(II), Cd(II) or Ni(II) (100 mg/L) in distilled water for 24 h. The effect of
contact time was conducted by shaking 0.5 g of burnt DWTS at op-
timum firing temperature and individual nitrate solutions of Pb, Cd or
Ni (100 mg/L) in distilled water for different time intervals of 2, 4, 6, 8,
12 and 24 h. The effect of initial pH was performed by shaking 0.5 g of
burnt DWTS at optimum conditions of firing temperature and contact
time and individual nitrate solutions of Pb, Cd or Ni (100 mg/L) at
different initial pH values of 3, 4, 5, 6, 6.5, 7, 7.5, 8 in addition to
original pH value of metal nitrate solution.
The effect of adsorbent dosage was conducted by adding desired
amounts of burnt DWTS (0.5, 1, 1.5 and 2 g) at the optimum conditions
with 50 mL of the individual nitrate solutions of Pb(II), Cd(II) or Ni(II)
(100 mg/L) in distilled water. The effect of initial metals concentration
was conducted by adding 2 g of burnt DWTS to 50 mL of the individual
nitrate solutions of Pb(II), Cd(II) or Ni(II) having different concentra-
tions of 100, 200, 300, 450 and 650 mg/L in distilled water. Effect of
competitive adsorption at the optimum conditions was also carried out
by mixing groups of Pb(II)-Cd(II), Pb(II)-Ni(II) and Pb(II)-Cd(II)-Ni(II)
at different initial concentrations of 200 and 450 ppm.
2.5. Methods for physicochemical characterization
DWTS was characterized by X-ray fluorescence (XRF) technique
using Pnanalytical Axios advanced XRF; as well as X-ray diffraction
344
Applied Clay Science 146 (2017) 343–349
(XRD) analysis using a stabilized X-ray generator fitted with a copper
target X-ray tube, (Geiger Muller tube). The settings used were tube run
at 30 kV, 15 mA divergence, receiving and scatter solids, 1, 1, cm and 1
respectively and chart speed 100 C.P.S.
Adsorption–desorption isotherm of purified N2 at 77K was carried
out using Nova 2000, Quanta Chrome (commercial BET unit). The ex-
ternal morphology of DWTS was observed using scanning electron
microscope (SEM) FEI Quanta 250 FEG. The heavy metals analysis was
examined using Inductive Coupled Plasma (ICP) instrument Perkin
Elmer Model: ICP – OES Optima 7300 DV; in which an ICP source
consists of a flowing stream of argon gas ionized by an applied radio
frequency field typically oscillating at 40 MHz; this generates about
6000 to 8000 K which called plasma. The high temperature of the
plasma excites atomic emission efficiently. Ionization of a high per-
centage of atoms produces ionic emission spectra.
3. Results and discussion
3.1. Physicochemical characteristics of DWTS
3.1.1. Chemical composition
The results of chemical analysis of DWTS are given in Table 1 in
terms of oxide composition. It is obvious that DWTS composed mainly
of silica and alumina as a result of precipitated clay as well as coagulant
used in the treatment.
3.1.2. X-ray diffraction analysis
The mineral composition of DWTS, fired at different temperatures,
was identified by means of XRD analysis as shown in Fig. 1. The results
indicate the presence of quartz and illite phases in all samples while
albite phase appears additionally at 500 °C. It had been recorded in
previous researches the potential application of quartz- silicon oxide-
(Tikhomolova et al., 2001; Reich et al., 2010; Al-Anber, 2010; Bellucci
et al., 2015) and illite (Ozdes et al., 2011; Benedicto et al., 2014a,
2014b; Cui et al., 2015) in heavy metal removal as adsorbents. Illite is a
clay mineral of the layer type 2:1. It has the general formula of
KyAl4(Si8−y, Aly)O20(OH)4, usually with 1 < y < 1.5, and composed
of two silica tetrahedral sheets that sandwich an alumina octahedral
sheet (Alvarez-Puebla et al., 2005; Hongxia et al., 2016). The efficiency
of illite as an adsorbent for heavy metal ions is ascribed to ion exchange
reaction with its potassium ions that are trapped in its interlayer spaces;
as well as inner-sphere complexes formation through ^SieO− and
^AleO− groups are located at the edges (McBride, 1994; Sheng et al.,
1999; Celis et al., 2000; Gu and Evans, 2007).
Q+I
I
Q I I I 700 C
o
o
600 C
Intensity
A Q+A
500 C
o
400 C
o
o
100 C
10 20 30 40 50 60
2 θ (deg.)
Fig. 1. XRD analysis of the DWTS fired at different temperatures. (Q = quartz, I = illite
and A = albite).
S.A. Abo-El-Enein et al. Applied Clay Science 146 (2017) 343–349

Table 2
Surface area and pore structure characteristics of DWTS after thermal treatment at 100, 500 and 700 °C.

Temperature (°C) SBET C constant Vp (mL/g) Mean pore radius (Å) St (m2/g) Most probable radius (Å)

100 22.61 30.66 0.0655 57.95 22.00 18.90

500 61.92 58.2 0.1550 50.01 83.10 18.66
700 50.27 65.32 0.1738 69.15 68.27 18.91

The presence of albite mineral, which is an alumino silicate of the 50

formula NaAlSi3O8 (sodium feldspar), in addition to quartz and illite in (a)
DWTS fired at 500 °C can enhance the adsorption capacity as it will be
clearly evidenced later in this study that albite is already examined for 40

Volume adsorbed (cc/g)

its efficiency as an adsorbent for both organic and inorganic materials
(Chernyshova et al., 2001; Vidyadhar et al., 2002; Feng et al., 2013; Liu
et al., 2015). 30

3.1.3. Surface area and pore structure characteristics

20
The main surface and pore structure characteristics of the DWTS,
after thermal treatment at 100, 500 and 700 °C, were studied using
nitrogen gas adsorption at liquid nitrogen temperature (77.2 K) and the 10
results are summarized in Table 2. The adsorption-desorption isotherms
are shown in Fig. 2a–c for the DWTS samples after heat treatment at
100, 500 and 700 °C, respectively. 0
Evidently, the adsorption-desorption isotherm obtained for the 0.0 0.2 0.4 0.6 0.8 1.0
DWTS heated at 100 °C shows that the adsorption process is irreversible o
P/P
indicated the presence of the type of constricted “ink bottle” pores. The
ink bottle type of pores is hinted by Kraemer (1931), developed by 120
McBain (1935) and others (Rao, 1941; Katz, 1949). It consists of a (b)
wider body with a narrow entrance as shown from the hysteresis loop 100
which is closed at a relative pressure (p/po) of 0.45 from which the
Volume adsorbed (cc/g)

radius of narrow pores can be calculated (Fig. 2a); meanwhile, the ra-
dius of wider pores can be calculated from the relative vapor pressure of 80
0.70 where capillary condensation takes place where the radii of
narrow entrance and wider body could be calculated by using Kelvin 60
equation (Abo-El-Enein et al., 1974).
However, thermal treatment of the DWTS at 500 °C resulted in a sort
40
of pore opening as indicated by the wider hysteresis loop which is
closed at a relative vapor pressure of 0.35 just after the formation of the
first adsorbed layer (monolayer capacity), (Fig. 2b), with a consequent 20
increase in the specific surface area of the DWTS heated at 500 °C,
(Table 2).Therefore, a large number of pores become accessible for the
0
removal of a larger fraction of pollutants as reported later in this study 0.0 0.2 0.4 0.6 0.8 1.0
(Fig. 4).
Moreover, thermal treatment of the DWTS at 700 °C resulted in a P/Po
sort of sintering with a consequent decrease in the specific surface area 140
where mesopores become more dominant; mesopores possess lower (c)
surface areas and larger pore volumes as compared with micropores 120
(Fig. 2c). This could be clearly distinguished from the results of Table 2.
Therefore, the percentage removal of pollutants by the DWTS after
Volume adsorbed (cc/g)

100
thermal treatment at 700 °C decreases as reported later in this study
(Fig. 4). 80

3.1.4. Scanning electron microscopy analysis 60

Fig. 3a–c represents the SEM micrographs of DWTS heated at
100 °C, 500 °C and 700 °C, respectively. The microstructure of DWTS 40
heated at 100 °C displayed a more porous structure with the appearance
of large and rod-like particles as representing a more open structure 20
consisting mainly of mesoporous (Fig. 3a); the results of XRD analysis
indicated that as well the presence of the only phases indentified are
0
quarts and illite as well as the presence of algae and diatoms are coated 0.0 0.2 0.4 0.6 0.8 1.0
by amorphous layers of hydration products. o
The SEM micrograph of DWTS fired at 500 °C shown in Fig. 3b P/P
displayed the formation of albite particles which appeared as small fi- Fig. 2. N2 adsorption-desorption isotherms of DWTS after thermal treatment at (a)
bers and wrinkled foils together with nearly amorphous and micro- 100 °C, (b) 500 °C and (c) 700 °C.
crystalline particles; which appeared as coatings around the grains;

345
S.A. Abo-El-Enein et al. Applied Clay Science 146 (2017) 343–349

100

90

80

70

Removal (%)
60

50

40

30

20 Pb
Cd
10 Ni
0
100 200 300 400 500 600 700 800
Firing Temperature (oC)

Fig. 4. Effect of firing temperature of DWTS on the removal percent of metal ions (metal
ion conc. = 100 ppm; adsorbent dose = 0.5 g; solution volume = 50 ml; contact
time = 24 h; temperature = 25 ± 2 °C; agitation speed = 200 rpm; pH = 5.5).

3.2. Factors affecting the efficiency of metal ions removal

3.2.1. Effect of firing temperature

Fig. 4 shows the effect of firing temperature of DWTS on the re-
moval percent of Pb(II), Cd(II) and Ni(II) from their aqueous solutions
of original pH value = 5.5 (DWTS dose = 0.5 g and contact
time = 24 h). Evidently, firing of DWTS has no considerable effect on
its adsorptive capacity towards Pb(II) where its removal percent is
nearly 100% at all firing temperatures; whereas for Cd(II) its removal
percent increases with the increasing of firing temperature up to 500 °C
then decreases. The removal percentage of Ni(II) increases up to 600 °C,
then decreases. From the aforementioned observations, for economic
consideration 500 °C was chosen as an optimum firing temperature of
DWTS for the removal of metal ions under investigation since the re-
moval percent of Ni(II) does not change appreciably from 500 to
600 °C.

3.2.2. Effect of contact time

Fig. 5 shows the effect of contact time on the removal percent of Pb
(II), Cd(II) and Ni(II) from their aqueous solutions of original pH
value = 5.5 using 0.5 g of DWTS fired at the optimum firing tempera-
ture of 500 °C. It was observed that the removal percent increases with
increasing contact time, and then gradually reaches to an almost

100

Fig. 3. SEM images of DWTS heated at a) 100 °C, b) 500 °C and c) 700 °C.
80
such a structure leads to an increase in the surface area available for
adsorption of larger amounts of metal ions from their aqueous solution.
Removal (%)

60
These SEM micrographs are also confirmed by the increase in surface
area available for the removal of metal ions; the contents of pore size
distribution proved that the pore system is composed mainly of meso-
40
pores which are accessible for adsorption of larger amounts of metal
ions.
Thermal treatment of DWTS at 700 °C, however, the results of SEM Pb
20
micrograph displayed the presence of quartz and illite phases in addi- Cd
tion to algae and diatoms with the disappearance of albite phases Ni
within a noticeable decrease in surface area available to the removal of
0
small fraction of metal ions as confirmed by the results of pore structure 0 5 10 15 20 25
which indicated assort of pore narrowing with consequent decrease in
Time (Hours)
the fraction of mesopores which are accessible to the removal of metal
ions, Fig. 3c. Fig. 5. Effect of contact time on the removal percent of metal ions (metal ion
conc. = 100 ppm; adsorbent dose = 0.5 g; adsorbent firing temperature = 500 °C; solu-
tion volume = 50 ml; temperature = 25 ± 2 °C; agitation speed = 200 rpm; pH = 5.5).

346
S.A. Abo-El-Enein et al. Applied Clay Science 146 (2017) 343–349

100 100

90

80 80
70
Removal (%)

60

Removal (%)
60
50

40
40
30
Pb
20
Cd Pb
10 Ni 20
Cd
0 Ni
3 4 5 6 7 8 9
0
pH 0.5 1.0 1.5 2.0
Fig. 6. Effect of initial solution pH on the removal percent of metal ions (metal ion Dose (g)
conc. = 100 ppm; adsorbent dose = 0.5 g; adsorbent firing temperature = 500 °C; so-
lution volume = 50 ml; contact time = 4 h; temperature = 25 ± 2 °C; agitation Fig. 7. Effect of burnt DWTS dose on the removal percent of metal ions (metal ion
speed = 200 rpm). conc. = 100 ppm; adsorbent firing temperature = 500 °C; solution volume = 50 ml;
contact time = 4 h; temperature = 25 ± 2 °C; agitation speed = 200 rpm; pH = 5.5).

equilibrium value in 4 h. The fast metals removal in the initial stages of

contact time is attributed to the large amount of available active sites 100
especially for Pb(II) adsorption which shows removal percent closing to
90
100% even before 4 h. Evidently, the progressive removal of Cd(II) and
Ni(II) ions takes place in a slower rate. According to these results, the 80
optimum contact time was fixed at 4 h for Cd(II) and Ni(II) where the 70
removal percents are 91 and 78%, respectively.
Removal (%)

60

3.2.3. Effect of pH 50
Fig. 6 shows the effect of solution pH on the removal percent of 40
metal ions using 0.5 g of DWTS fired at the optimum firing temperature
30
of 500 °C and contact time of 4 h. The metal ions removal percent in-
Pb
creases by increasing the pH value of the solution. This could be ex- 20
Cd
plained as follows: at lower pH the protonation takes place on the Ni
10
DWTS surface blocking the active sites available for positive metals ions
adsorption while as pH value increases the protonation will be de- 0
100 200 300 400 500 600 700
creased and the negative charges on DWTS surface will be more ex-
posed resulting in electrostic attraction towards positive metal ions in Concentration (ppm)
solution. Fig. 8. Effect of initial metal ions concentration on the removal percent of metal ions
(adsorbent dose = 2 g; adsorbent firing temperature = 500 °C; solution volume = 50 ml;
3.2.4. Effect of burnt DWTS dose contact time = 4 h; temperature = 25 ± 2 °C; agitation speed = 200 rpm; pH = 5.5).

The effect of burnt DWTS dosage on heavy metal removal, at the

optimum firing temperature (500 °C) of DWTS optimum contact time
(4 h) and optimum initial pH (5.5), was studied by varying the dosage
of burnt DWTS and the results are shown in Fig. 7. Evidently, an almost
complete removal of Pb(II) as obtained by using the different dosages of
burnt DWTS where the removal efficiency reached 99% with varying
the dose from 0.5 up to 2 g. For Cd(II) and Ni(II) the removal percents
increase with increasing burnt DWTS dose till 2 g, where the removal
efficiency reached almost 99%. This is mainly due to the increase of the
adsorbent sites by increasing dosage level up to 2 g. Thus, it can be
concluded that the optimum dose for heavy metals removal is 2 g with
the removal efficiency of 99%.
3.2.5. Effect of initial metal ions concentration
Fig. 8 shows that the effect of initial metal ions concentration on
efficiency of their removal, at optimum firing temperature of DWTS
(500 °C), optimum contact time (4 h), optimum initial pH (5.5) and
optimum fired DWTS dose (2 g). The Pb(II) removal does not affected
by the increase of the initial metal ion concentration where an almost
complete removal is obtained at all initial concentrations. For Cd(II)
and Ni(II) the removal percent is almost 100% at initial concentration
of 100 ppm. Afterwards the removal percent decreases considerably.
Therefore initial concentration of 100 ppm was chosen as the optimum
one.
3.2.6. Competitive metal ions adsorption
The competitive adsorption of metals under study was investigated
by applying two binary mixtures of Cd(II) and Ni(II) individually with
Pb(II) in addition to a tertiary mixture of all of them together. The
experiment was carried out using DWTS fired at optimum temperature
of 500 °C, optimum contact time (4 h), optimum initial pH (5.5) and
optimum fired DWTS dose (2 g). Two initial concentrations of metal
ions of 200 ppm and 450 ppm were utilized. The results of the removal
percent of each metal ion are shown in Table 3.
The high affinity of DWTS towards Pb(II) adsorption almost does
not change whatever the metal ion present in the mixture as well as the
initial concentration applied. For Cd(II) and Ni(II) in the binary and
tertiary mixtures with Pb(II), increasing the initial concentration causes
a decrease in their removal percents but the decrease in that of Ni(II) is
twice that of Cd(II)in the binary mixtures and is five times that of Cd(II)
in the tertiary mixture.
Generally, the removal percent of metals is found to be in the order
Pb(II) > Cd(II) > Ni(II) in the tertiary mixtures. This trend matches
with the order of ionic radius of metals and hydration energy but
doesn't match with other characteristics listed in Table 4.

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S.A. Abo-El-Enein et al. Applied Clay Science 146 (2017) 343–349

Table 3
Removal percent of Pb(II), Cd(II) and Ni(II) in binary and tertiary mixtures.

Pb-Cd mixture Pb-Ni mixture Pb-Cd-Ni mixture

At 200 ppm At 450 ppm At 200 ppm At 450 ppm At 200 ppm At 450 ppm

Pb(II) removal % 99.9% 97.6% 99.2% 97.8 99.3% 98.5%

Cd(II) removal % 85% 72% – – 74% 70.2%
Ni(II) removal % – – 80% 54% 66% 45%

Table 4 carbon. J. Chem. Eng. Process Technol. 4, 158. http://dx.doi.org/10.4172/2157-

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