Available online at http://ijcpe.uobaghdad.edu.iq and www.iasj.net

Iraqi Journal of Chemical and Petroleum
Engineering

Vol.21 No.2 (June 2020) 15 – 23
EISSN: 2618-0707, PISSN: 1997-4884

Corresponding Authors: Name: Teba H. Mhawesh

, Email: eng.teba94@yahoo.com , Name: Ziad T. Abd Ali, Email: z.teach2000@yahoo.com

IJCPE is licensed under a Creative Commons Attribution-NonCommercial 4.0 International License.

Reuse of Brick Waste as a Cheap-Sorbent for the Removal of

Nickel Ions from Aqueous Solutions

Teba H. Mhawesh

and Ziad T. Abd Ali

University of Baghdad/ College of Engineering/ Environmental Engineering, Baghdad Iraq

Abstract

The potential application of granules of brick waste (GBW) as a low-cost sorbent for removal of Ni

+2
ions from aqueous solutions

has been studied. The properties of GBW were determined through several tests such as X-Ray diffraction (XRD), Energy dispersive

X-ray (EDX), Scanning electron microscopy (SEM), and BET surface area. In batch tests, the influence of several operating

parameters including contact time, initial concentration, agitation speed, and the dose of GBW was investigated. The best values of

these parameters that provided maximum removal efficiency of nickel (39.4%) were 1.5 hr, 50 mg/L, 250 rpm, and 1.8 g/100mL,

respectively. The adsorption data obtained by batch experiments subjected to the Three isotherm models called Langmuir, Freundlich

and Elovich, The results showed that the Freundlich isotherm model described well the sorption data (R
2
=0.9176) in comparison with

other models. The kinetic data were analyzed using two kinetic models called pseudo-first-order and pseudo-second-order. The

pseudo-first-order kinetic model was found to agree well with the experimental data.

Keywords: Sorption, Ni

+2
, brick waste, Isotherms, Kinetics, Wastewater

Received on 13/10/2019, Accepted on 18/02/2020, published on 30/06/2020

https://doi.org/10.31699/IJCPE.2020.2.3

1- Introduction

Many branches of industry nowadays generate large

quantities of wastewater containing toxic and

carcinogenic organic and inorganic compounds. Heavy

metals are considered inorganic pollutants such as

mercury, cadmium, lead, cobalt, zinc, nickel, manganese

etc. It’s not decomposed so their metal concentrations

should be at minimum to reasonable levels before drain

into their environment, [1].

Nickel metals are danger and toxic to humans, it's

represent a serious environmental issue, [2]. Nickel exists

in the effluents of storage battery industries; desalinate

plants, gas turbines, coinage, and costume jewelry, [3].

The US Environmental Protection Agency )EPA)

requires nickel metals not to exceed 0.015 mg/L in

drinking water ,[4].

Above the permissible limit may cause

adverse health impacts such as anemia, diarrhea

, hepatitis, the damages of lungs and kidney and

pulmonary fibrosis,[5];[2].

Accordingly, many methods have been studied to

remove toxic metal ions from industrial wastewater

include, chemical-precipitation, ion-exchange, bio-

sorption , reverse-osmosis, floatation, and sorption etc.

[2], [6].

Several sorbents can be utilized for removal of toxic

metals from wastewater but porous carbons sorbent are

utilized extensively in contrast with other methods

because these sorbents have a large specific, high sorption

capacity, and easily regenerated, but is considered an

expensive sorbent material.

For that reason, different cheap materials like: zeolites,

[7], metal oxides, [8], iron oxide-coated sand, [9], and

clay minerals, [10], had recently been examined with the

purpose to demonstrate their capacity for heavy metal

removal from pollutants wastewater. But, the solution of

specific water issues encountered in communities of

developing countries had required the elaboration of

proven and locally more suitable water - handling

procedures at low costs, [11].

In the recent years, the ability of brick waste utilized

as a cheap sorbent to remove soluble heavy metal

pollutants from wastewaters had been studied, [12, [13].

The nature of brick material, surface area, and surface

charge influence the extent of interaction with metal ions.

As brick granules are negatively charged, therefore

cations will be strongly attached to brick granules [14].

Based on the above mentioned concepts, the purpose of

this study is to use brick waste as a cheap and abundant

material to remove nickel ions from aqueous solutions.

The influence of contact time, initial concentration of

Ni
+2

, agitation speed, and sorbent mass on the removal

percent of nickel ions were studied.

http://ijcpe.uobaghdad.edu.iq/
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https://doi.org/10.31699/IJCPE.2020.2.3

T. H. Mhawesh

and Z. T. Abd Ali / Iraqi Journal of Chemical and Petroleum Engineering 21,2 (2020) 15 - 23

2- Experimental work

2.1. Granules of Brick Waste (GBW) Preparation

Pieces of brick waste, which are left unused after

construction, were used as sorbent in this study. It were

crushed and sieved with size ranging from (1.18) mm to

(1.7) mm.

The obtained granules of GBW were washed several

times with distilled water then dried as shows in Fig. 1.

Fig. 1. Granules of brick waste (GBW)

2.2. Characterization of GBW

a. Surface Area

Surface area is an important factor in determining the

active sites that will be occupied with the contaminants.

Therefore, increasing the surface area of the material

increases its susceptibility to adsorb more quantity of

pollutants. The BET surface area was measured using

(Quanta chrome, USA), at the Petroleum Research and

Development Center/ Ministry of Oil / Baghdad - Iraq.

b. X-Ray Diffraction (XRD) Analysis

The surface qualitative analysis was carried out to

characterize and confirm the existence of the major

components; samples were analyzed before uptake of

nickel. This analysis was accomplished using (BRUKER,

D2 PHASER, Germany).

c. Energy Dispersive X-ray (EDX) Analysis

EDX analysis is a chemical microanalysis technique

utilized in conjunction with scanning electron microscopy

(SEM).It’s used to recognize the elemental composition

of materials. This test carried out using ( TESCAN,Vega

III , Czech Republic).

d. Scanning Electron Microscopy (SEM)

Scanning Electron Microscope (TESCAN, Vega III, and

Czech Republic) was utilized for the surface studies of

GBW. Using the optimized conditions for the sorption of

nickel ions, the loaded mass was filtered, washes and

dried at 105
o
C for 30 min. Unloaded mass was also

subject to the same circumstances and both the loaded and

unloaded mass was subjected to SEM to identify the

changes on the surface of the GBW before and after

loading by the nickel ions molecules.

2.3 Preparation of Synthetic Wastewater

The synthetic solution of nickel with a concentration of

1000 mg/L was prepared by dissolving a 4.95 g of of

nickel nitrate (Ni(NO3).6H20) in 1 L of distilled water

and this synthetic solution was pH adjusted using 0.1 M

of ( HNO3 ) and/or (NaOH ) as required.

2.4 Sorption Experiments

These experiments were carried out to identify the

better conditions of contact time, , initial concentration of

contaminant, agitation speed and dosage of sorbent. A

number of flasks of (250 ml) are employed and each one

is filled with 100 ml of Ni
2+

ions solution which has initial

concentration of (50 mg/l ), initial pH= 4 and about

(1g/100ml) of sorbent(GBW) was added into each flask

.The flasks were preserved stirred in (200 rpm) speed

orbital shaker at ambient temperature. Then the GBW was

separated from the pollutant solution by filtration.

These tests were conducted at different time

(10,20,30,50,70,90,150,180,240 min.), initial

concentrations (50, 100,150,200,250 mg/l ) , agitation-

speeds (0, 50, 100, 150, 200 and 250 rpm),and sorbent

dosages (0.2, 0.4, 0.6, 0.8,1,1.1,1.2,1.3,1.5,1.8 and 2

g/100ml).

The metal ion concentration at saturation was calculated

by atomic absorption spectrometry (Shimadzu, Japan).

The concentration of metal ion sorbed by GBW was

calculated from the difference between the initial and ,the

final concentration of metal ions solution obtained before

and after contact between the GBW and the synthetic Ni
+2

solution. The sorption capacities were determined using

Eq. (1) [15]:

𝑞𝑒 =
(𝐶𝑜−𝐶𝑒)𝑉

𝑚
(1)

Where: qe is the amount of sorbed nickel ion, per unit

mass of GBW (mg/g), Co and Ce are the initial and

equilibrium concentrations of nickel in the solution

(mg/L), V is the volume of solution (L), and m is the mass

of the sorbent GBW (g).The removal efficiency (R%) of

the Ni
+2

was calculated using Eq. (2), [15]:

𝑅% =
𝐶𝑜−𝐶𝑒

𝐶𝑜
𝑥100 (2)

T. H. Mhawesh

and Z. T. Abd Ali / Iraqi Journal of Chemical and Petroleum Engineering 21,2 (2020) 15 - 23

3- Isotherm Models

In the current study, three isotherm models is used to

simulate the performance of GBW in removing nickel

ions from wastewater. A summary of these models is

presented below:

 Langmuir model: assumes a surface with
homogeneous binding sites, equivalent sorption

energies, and no interactions between sorbed species,

[16] . The linear form of this model can be written as

follows:

𝐶𝑒

𝑞𝑒
=

𝐶𝑒

𝑞𝑚𝑎𝑥
+

𝑞𝑚𝑎𝑥 𝐾L
(3)

Where:

qmax ,is the maximum sorption capacity (mg/g).

KL, is the Langmuir sorption constant (L/mg).

Ce , is the concentration (mg/L) of Ni
+2

in solution at

equilibrium.

The plot of (Ce/qe) against (Ce) gives a straight line

with a slope and intercept of (1/qmax) and (1/qmax KL)

respectively.

 Freundlich model: It’s an empirical model not limited
to monolayer coverage alone but also describe

multilayer adsorption, [16]. It is expressed linearly as

in Eq.4:

ln qe =
1

n
ln Ce + ln KF (4)

Where: KF, is the Freundlich sorption constant.

Ce, is the concentration (mg/L) of Ni
+2

in solution at

equilibruim.

n, is an empirical constant indicative of the intensity of

the sorption.

The Plots of (log qe) against, (log Ce), gives a linear

graph with slope 1/n and intercept log KF from which n

and KF can be determined respectively.

 Elovich model: is based on a kinetic principle
assuming that the sorption effective sites increase

exponentially with sorption, which implies a

multilayer sorption, [17], [18]. It can be expressed as:

𝑙𝑛
𝑞𝑒

𝐶𝑒
= 𝑙𝑛𝐾𝐸 𝑞𝑚 −

𝑞𝑒

𝑞𝑚
(5)

Where: KE is the Elovich equilibrium constant (L/mg)

and qm is the Elovich maximum adsorption capacity

(mg/g).

4- Kinetic Models

Kinetic sorption models are helpful to understand the

mechanism of the sorption process of nickel onto GBW.

These models include pseudo first order and pseudo-

second order, [19].

 The pseudo-first order kinetic rate equation is :

𝑙𝑛(𝑞𝑒 − 𝑞𝑡) = 𝑙𝑛(𝑞𝑒) − 𝐾1𝑡 (6)

Where: qe and qt, represent the amounts of metal ion

(Ni
+2

) sorbed per unit mass of GBW at equilibrium (mg/g)

, and time t (min), respectively.

K1, is the rate constant of pseudo_ first _ order sorption

(1/min). The pseudo_second_order kinetics rate equation

is:

𝑡

𝑞𝑡
=

𝐾2 𝑞𝑒
2

+
𝑡

𝑞𝑒
(7)

Where: K2, is the rate constant of pseudo_second_order

sorption (g / mg. min).

5- Results and Discussion

5.1. Characterization of GBW

a. XRD Analysis

The XRD measurement was performed to identify the

mineralogical composition of GBW. Fig. 2 illustrates that

GBW was composed mainly of Diopside (29.9%), Quartz

(22.4%), wollastonit (22.2%), akermente (20.5%) and

Mellite (5%). Diopside Originating from dolomite

(CaO, MgO, 2CO2), also explain that (quartz) and

(calcite) are the most popular compounds, with the

addition of clays and clay minerals. However, due to the

application of high temperature handling through the

manufacturing process, the decomposition of clay

minerals forming ( SiO2 ) compound, which followed by

the loss of their crystal structure. CaCO3 compound

decompose and resulting CaO compound that may react

with the clay resulting calcium-silicate called wollastonite

[20].

Fig. 2. XRD of GBW

T. H. Mhawesh

and Z. T. Abd Ali / Iraqi Journal of Chemical and Petroleum Engineering 21,2 (2020) 15 - 23

b. EDX Analysis

The EDX analysis was carried out and the spectra are

given in Fig. 3. This figure indicates that the GBW

composed of oxygen, calcium ,Silicon , aluminium , iron

, magnesium, sodium, potassium and sulfur, with

percentage of 44.2%, 21.7%, 18.1%, 5.7%,5%, 2.8%,

1.4%, 0.6% and 0.6% , respectively.

The analysis for GBW showed the presence of oxygen ,

calcium, silicon , and other small percentages of metals

.The existence of these oxides and hydroxides in GBW

because its having a various (higher) sorption capacity ,

[21] .

Fig. 3. EDX spectra of GBW

c. SEM Analysis

The SEM analysis images at 50 Mm gained before/after

sorption to identify the surface morphology. Fig. 4 (a)

represents the SEM spectra of the GBW before nickel

loading, its shows irregular structure having small pores,

which simplify the process of sorption.

The SEM analysis after nickel sorption indicates that

these pores become filled with nickel ions as shown in

Fig. 4 (b) [21].

(a)

(b)

Fig. 4. SEM spectra of the of GBW (a) before and (b)

after nickel ions loading

d. Surface Area

The results of this test clarify that the GBW

sample show a low BET surface area of (1m
2
/

g).this results in a good agreement with previous

study of Kooli [22].

5.2. Influence of Batch Operating Parameters

a. Effect of Contact Time

The impact of the contact time on sorption of Ni
+2

using

GBW was studied by using contaminated aqueous

solution with initial nickel concentration 50(mg/L) at

pH=4. The relation between the contact time and removal

efficiency of nickel ions is shown in Fig.5,the best

removal efficiency (28%) was reached within about

90(min). The sorption of Ni
+2

ions occurred in two phase,

an initial rapid sorption followed by subsequent slow

sorption. The sorption process appeared to proceed

rapidly when the numbers of active sites are much higher

than the number of metal species to be sorbed, [23].

The increase of solution pH during the contact with

GBW can be attributed to the dissolution of some of their

components, [20].

Fig. 5. Effect of contact time on Ni

+2
removal percent (Co

= 50 mg/L, pH= 4, agitation speed = 200 rpm, and mass

of GBW = 1g /100ml)

T. H. Mhawesh

and Z. T. Abd Ali / Iraqi Journal of Chemical and Petroleum Engineering 21,2 (2020) 15 - 23

b. Effect of Initial Concentration

The initial metal ions concentration is a very important

factor to be investigated in sorption studies as most

contaminated wastewaters usually present different

concentrations of metal ions, so determination of its effect

is necessary for an elaborate sorption study, [24].

The effect of initial metal ion concentration on the

percentage removal of Ni
+2

ions using GBW is shown in

Fig. 6. The percentage removal of metal ions decreased

with increase in the initial metal concentration from 50 to

250 mg/L. A decrease from 28% to 9 % of Ni
+2

ions was

obtained. This decrease is due to the fact that the sorbent

material (GBW) has a fixed number of active sites and at

higher concentrations, the active sites become saturated,

[25]
The simple hydrolysis of generality divalent metal ions

can be written as follows:

M
+2

+H2O⇌M(OH)
+
+H

+ (8)

Where: M
+2

is Ni
+2

or any metal ions. The final pH

increase when the concentration of the solution decreases.

This happens when GBW is being occupied by Ni
+2

ions, the reaction above shifts to the left, leading to the

depletion of protons and hence rise in pH, [26]

Fig. 6. Effect of initial concentration on Ni

+2
removal

percent (Time= 90 min., pH= 4, agitation speed = 200

rpm, and mass of GBW = 1g /100ml)

c. Effect of Agitation Speed

The effect of agitation speed of the sorbent/sorbate

system was monitored at (0, 50, 100, 150, 200, and 250

rpm) as shown in Fig.7.The significant increase in

sorption is primarily due to the fact that agitation speed

facilitates proper contact between Ni
+2

ions in solution

and the GBW effective sites and consequently promoting

better transfer of sorbate ions (Ni
+2

) to the sorbent sites,

[27].In addition, the increase of the pH of the solution

during the contact with GBW can be attributed to the

dissolution of some GBW components as reported by

Jelić ,[20].

Fig. 7. Effect of agitation speed on Ni

+2
removal percent

(Co = 50 mg/L, Time=150 min, pH=4, and mass of GBW

= 1g /100ml)

d. Effect of the Dose of GBW

The study of the mass of GBW that utilized for the

removal of Ni
+2

ions, was carried out using the various

dosage of GBW range from (0.2 - 2) g. The effect of

sorbent dose on the sorption of nickel by GBW was

presented in Fig. 8. As illustrated in Fig.8, the nickel

removal percent increased with increase of sorbent dose.

The increase in the GBW dosage improved the

availability of more effective sites for the sorption, thus

making easier penetration of nickel ions to the sorption

sites, [23]. Moreover, the final pH increase due to release

the amounts of dissolved Ca
+2

and other light metal

alkalis in solution during the reaction between GBW and

Ni
+2

ions, [20].

Fig. 8. Effect of sorbent dose on Ni
+2

removal percent (Co

= 50 mg/L, pH= 4, Time= 90 min, and mass of GBW =

1g /100ml)

5.3. Sorption Isotherms

The sorption data for nickel is fitted with linearized

equations of three isotherm models namely; Langmuir,

Freundlich and Elovich.

-1

100

0 0.5 1 1.5 2

F
in

a
l

p
H

R
e

m
o

va
l

mass of sorbent (g)

Ni…

T. H. Mhawesh

and Z. T. Abd Ali / Iraqi Journal of Chemical and Petroleum Engineering 21,2 (2020) 15 - 23

Accordingly, the empirical coefficients for each model

were determined from the slope and intercept of linear

plot using Microsoft Excel 2013 software. The isotherm

graphical representations of these three models are shown

in Fig. 9. All constants are presented in Table 1.

The value of R
2
close to 1 denotes that the respective

equation a good fits the experimental data, [27]. So, the

Freundlich isotherm model was concluded to be preferred

isotherms models for the experimental data.

(a)

(b)

(c)

Fig. 9. Isotherm models plot: a. Langmuir isotherm

model, b. Freundlich isotherm model, c. Elevich isotherm

model

Table 1. Sorption isotherm constants with coefficients of

determination for Ni
+2

onto GBW
Isotherm model Parameters GBW

Langmuir

qm (mg/g) -1.69

b (l/mg) -0.014
R

2
0.5784

Freundlich

KF (l/mg) 0.00247

n 0.547
R

2
0.9176

Elovich

qm (mg/g) -3.07

KE (l/mg) -0.00874
R

2
0.8437

5.4. Kinetic Study

To identify the type of sorption mechanism occurs, the

kinetic equations namely pseudo-first -order and pseudo-

second - order were utilized. It is clear from Fig. 10 and

Table 2 that the reaction for GBW is pseudo-first -order

because the value of the experimental qe was the closest

to the qe calculated from the pseudo-first -order in

compared with the pseudo-second - order model,

irrespective to the amount of the correlation coefficient

(R
2
), so that the mechanisms will be physical sorption

[29].

(a)

(b)

Fig. 10. The kinetic models for sorption Ni
+2

onto GBW:

a. Pseudo-first order reaction model, b. Pseudo-second-

order reaction model

T. H. Mhawesh

and Z. T. Abd Ali / Iraqi Journal of Chemical and Petroleum Engineering 21,2 (2020) 15 - 23

Table 2. The kinetic constants for the sorption of Ni
+2

onto

qe (exp)
(mg/g)

pseudo- first-
order

pseudo- second –
order

1.153

K1(1/min)

qe (calc.)

(mg/g)

R
2

0.0323

1.11

0.9886

K2 (g/mg*min)

qe(calc.)

(mg/g)

R
2

0.024

1.42

0.9926

6- Conclusions

Based on the results obtained from the experimental

work, the following conclusions can be drawn:

 The granules of brick waste (GBW) material proved
low effectiveness in removing nickel ions from

aqueous solutions with removal percent of 39.4% at

dose value of 1.8 sorbent according to the

experimental conditions .

 The batch results indicated that several parameters
including contact time, initial concentration, agitation

speed, and granular brick waste dose affect the

sorption process. The optimum values of these factors

which provided maximum removal percent ( 39.4%)

of nickel with initial pH of 4 were 90 min, 50 mg/l,

250rpm, and 1.8/100ml, respectively. The maximum

sorption capacity for GBW (1.153mg/g (

 The isotherm study refers that the sorption data
correlated well with Freundlich isotherm model

which showed the highest value of the correlation

coefficient (R
2
= 0.9176)

 The kinetic study showed that the pseudo-first -order
kinetic model was conform better than pseudo-second

- order model kinetic model. This result clarify that

physical sorption have been predominant in the

sorption of Ni
+2

ions using GBW.

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T. H. Mhawesh

and Z. T. Abd Ali / Iraqi Journal of Chemical and Petroleum Engineering 21,2 (2020) 15 - 23

يونات النيكل من المحاليل المائيةاإعادة استخدام نفايات الطابوق كمادة رخيصة إلزالة

طيبه مهاوش و زياد عبد علي

جامعة بغداد, كلية الهندسة, قسم الهندسة البيئية

الخالصة

Ni +2( كمواد منخفضة التكلفة إلزالة أيونات GBWتمت دراسة امكانية تطبيق حبيبات مخلفات الطوب )

من خالل العديد من الفحوصات مثل حيود األشعة السينية GBWمن المحاليل المائية. تم تحديد خصائص
(XRD( األشعة السينية المشتتة للطاقة ، )EDX( المجهر اإللكتروني المسح الضوئي ، )SEM والمساحة ، )

بما في ذلك وقت االتصال السطحية. في اختبارات الُدفعات ، تم فحص تأثير العديد من العوامل
. كانت أفضل قيم المعامالت التي وفرت أقصى كفاءة إزالة GBWوالتركيزاالبتدائي وسرعة الرج وجرعة

، على التوالي. بيانات g/100ml 1.8، و 1.5hr ،50mg/l ،250rpm%( : 39.4للرصاص )
الثالثة isothermضعت لنماذج االمتصاص التي تم الحصول عليها من خالل تجارب الُدفعات التي خ

وصف بشكل Freundlich. أظهرت النتائج أن نموذج Elovich)،و Langmuir ،Freundlichالمسماة )
( بالمقارنة مع النماذج األخرى. وقد تم تحليل البيانات الحركية R2 0.9176جيد بيانات االمتصاص )=

-pseudo(. تم ايجاد ان pseudo-second-orderو pseudo-first-orderباستخدام نموذجين :
first-order .يمثل جيدا البيانات التجريبية

مياه الصرف الصحي ,نفايات القرميد , Ni + 2الكلمات الدالة: االمتصاص,