Journal of Environmental Treatment Techniques 2020, Volume 8, Issue 3, Pages: 1023-1028

1023

Sorption of Malachite Green from Aqueous Solution

using Typha australis Leaves as a Low Cost Sorbent

Abdoulaye Demba N’diaye

1,2 *

, Youssef Aoulad El Hadj Ali

, Ould El Moustapha Abdallahi

Mohamed Abdallahi Bollahi

, Mostafa Stitou

, Mohamed Kankou

and Driss Fahmi

Laboratoire de Chimie, Service de Toxicologie et de Contrôle de Qualité, Institut National de Recherches en Santé Publique,

Nouakchott, Mauritanie

Unité de Recherche Eau, Pollution et Environnement, Département de Chimie, Faculté des Sciences et Technique, Université de Nouakchott Al Aasriya,

Nouakchott, Mauritanie

Laboratoire de L’Eau, les Etudes et les Analyses Environnementales, Département de Chimie, Faculté des Sciences, Université Abdelmalek Essadi,

Tétouan, Maroc

Institut Supérieur d’Enseignement Technologique, Département des Sciences et Technologies des Aliments, Laboratoire de Biotechnologie Alimentaire,

Rosso, Mauritanie

Received: 12/06/2020 Accepted: 24/06/2020 Published: 20/09/2020

Abstract

Malachite Green (MG) is a carcinogenic and mutagenic dye which is harmful for human and animal cells; its discharge through

wastewater creates major environmental problems. For this reason, we have used Typha australis leaves, an abundant and available plant

along the Senegal River for removing MG from aqueous solution. The adsorption equilibrium isotherms of MG onto Typha australis leaves

as low cost sorbent were studied and modeled. In order to determine the best fit isotherm, the experimental data were fitted to the two-

parameter isotherms (Langmuir, Freundlich and Jovanovic) and three-parameter isotherms (Sips, Redlich – Peterson and Toth) by nonlinear

method. The best fitting isotherm was found to be the Langmuir isotherm. The monolayer adsorption capacities were found to be 85.21 and

56.88 mg g

-1

at 21.4 and 31.4 °C, respectively. This homogeneity was also confirmed by the constants of Sips and Redlich–Peterson isotherms.

The present study showed that the Typha australis leaves can be effectively used as low cost sorbent for the removal of the MG from its

aqueous solution.

Keywords: Malachite Green, Typha australis, Senegal River, Isotherms, Nonlinear

1 Introduction

Malachite Green (MG) is a cationic dye that has been used for

dyeing wool, silk, paper, leather and cotton as well as a biocide

and disinfectant [1-3]. It has become one of the most serious

environmental issues to treat MG dye-contaminated wastewater

because MG dye is toxic and create a serious hazard to the aquatic

system and human health [4].

Many treatment methods have been developed to remove MG

from aqueous solution. These include electrochemical

degradation [5], photo-degradation [6] and photocatalytic

degradation [7]. However, these processes are costly and cannot

effectively be used to treat the wide range of dye wastewater.

Adsorption is accepted as the most efficient technique for

removing pollutants from aqueous solution among many other

methods thanks to its characteristics such as simplicity of design,

high efficiency and economic feasibility [8]. However, the

adsorption of dyes onto activated carbons has attracted many

researchers, but its high cost inhibits its application on a large

Corresponding author: Abdoulaye Demba N’diaye, (a) Laboratoire de Chimie, Service de Toxicologie et de Contrôle de Qualité, Institut

National de Recherches en Santé Publique, Nouakchott, Mauritanie and (b) Unité de Recherche Eau, Pollution et Environnement,

Département de Chimie, Faculté des Sciences et Technique, Université de Nouakchott Al Aasriya, Nouakchott, Mauritanie. E-mail:

abdouldemba@yahoo.fr.

scale [9]. In this reason, researchers have concentrated on finding

alternative natural adsorbents to activated carbon. Natural

adsorbents are preferred for their biodegradable, non-toxic nature,

low commercial value and highly cost-effective nature. A number

of low cost adsorbents are reported in the literature. These include

Lignin [10], Humic acid [10], Prosopis cineraria [11],

organomineral sorbent-iron humate (Janos and Smıdova, 2005)

[12], de-oiled soya [13], citric acid modified rice straw [14], hen

feathers [15], palm ash [16], bottom ash [17], Rattan Sawdust

[18], natural zeolite [19], chlorella-based biomass [20], Sea Shell

powder [21], chemically modified rice husk [22], Castor bean

presscake [23], Cerastoderma lamarcki shell [24] and Annona

squmosa seed [25]. However, sorption potential of most of these

low cost sorbents is generally low.

The objective of our study were to investigate the potential of

using Typha australis leaves, an abundant and available plant

along the Senegal River as a low cost sorbent to remove MG from

aqueous solutions, to model the equilibrium of the process. The

Journal web link: http://www.jett.dormaj.com

J. Environ. Treat. Tech

ISSN: 2309-1185

Journal of Environmental Treatment Techniques 2020, Volume 8, Issue 3, Pages: 1023-1028

1024

retention capacity of MG onto the Typha australis leaves is

investigated with using the nonlinear two-parameter models

(Langmuir, Freundlich and Jovanovic) and three-parameter

models (Sips, Redlich-Peterson and Toth). So, the sorption

parameters obtained using the Typha australis leaves as low cost

sorbent will be compared with the ones presented in the literature.

2 Material and Methods

2.1 Preparation of adsorbate

The stock solution of MG was prepared by dissolving 1 g of

MG in 1 L of distilled water. All working solutions of desired

initial MG concentrations were prepared by diluting the stock

solution with distilled water. Other concentrations are prepared

by dilutions of the stock solution and used to develop the standard

curves using the Spectrophotometer UV1800 Ray Leigh.

2.2 Collection,

Preparation and Characterization of Typha

australis

Typha australis leaves were collected from the south of

Mauritania. The Typha australis leaves were washed thoroughly

with distilled water to remove dirt. The biomass was then air dried

for 3 days followed by drying in an oven at 105 °C for 24 h. The

dried biomass was ground, sieved to obtain particle sizes below

0.5 mm and stored in a dessicator before use [26]. The

physicochemical characteristics of the Typha australis leaf are

reported by [27]. The content of C, H, N, S and O of the Typha

Australis were measured by using an Element Analyzer CHNSO

Flash 2000 EA 1112.

The surface morphology of Typha australis

leaves

before and after adsorption of MG was observed using a

Scanning Electron Microscope (SEM).

2.3 Adsorption experiments

Batch adsorption studies were carried out by contacting 0.2 g

of Typha australis leaves with 100 mL of MG solution of known

initial dye concentration in flasks at a constant agitation speed of

150 rpm at two different solution temperatures 21.4 and 31.4 °C.

The contact was made for 24 h, which is more than sufficient time

to reach equilibrium [28]. After 24 h, the MG solutions were

separated from the adsorbent by centrifugation. The left out

concentration in the supernatant solution was analyzed using a

UV Spectrophotometer 1800 Ray Leigh. The adsorption uptake

at equilibrium time, q

, was expressed by equation (1):

 

VCC





(1)

where q

is the amount of MG adsorbed by Typha australis leaves

adsorbent (mg g

-1

), C

is the initial liquid-phase concentrations of

MG (mg L

-1

), C

is the liquid-phase concentration of MG (mg L

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

australis leaves adsorbent used (g). All batch experiments were

conducted in triplicate and the mean values are reported.

2.4 Equilibrium adsorption isotherms

Two parameter models (Langmuir, Freundlich and

Jovanovic) and three parameter models (Sips, Redlich-Peterson

and Toth) are used to analyze the experimental adsorption data.

Applicability of these models to fit the experimental in predicting

the mechanism of adsorption is accomplished using solver Excel.

The relative parameters of each equation are obtained using Sum

of the Squares of the Errors (SSE) and the coefficient of

determination (R

) between the calculated and the experimental

data by nonlinear method. The SSE and R

values, by using the

Solver Excel, are determined respectively by following equations

(2) and (3):

SSE=

 

modexp

qq 

(2)

exp mod

exp avr

q -q

R =100 1-

q -q







(3)

where q

exp

(mg g

-1

) is equilibrium capacity from the experimental

data, q

avr

(mg g

-1

) is equilibrium average capacity from the

experimental data and q

mod

(mg.g

-1

) is equilibrium from model.

So that R

≤ 100 – the closer the value is to 100, the more perfect

is the fit. Langmuir isotherm is valid for monolayer adsorption

onto a surface containing a finite number of identical sites [29].

The nonlinear Langmuir model can be expressed by non linear

equation (4):

eLm

CKq





(4)

where q

is the amount of MG adsorbed per unit mass of Typha

australis leaves (mg g

-1

), k

is the Langmuir constant related to

the adsorption capacity (L g

-1

), C

is the concentration of MG in

the solution at equilibrium (mg L

-1

), q

is the maximum uptake

per unit mass of Typha australis leaves (mg g

-1

). The factor of

separation of Langmuir, R

, which is an essential factor

characteristic of this isotherm is calculated by using the relation

(5):

)1(





(5)

where C

is the higher initial concentration of MG and k

is the

Langmuir constant related to the adsorption capacity (L g

-1

). The

parameters indicate the shape of the isotherm as follows: R

values indicate the type of isotherm. When R

= 1 adsorption is

linear; when 0 < R

< 1, it is favourable, when R

= 0, it is

irreversible, while to be unfavorable, while when R

> 1, it is

unfavorable. Freundlich model is commonly used to describe the

adsorption characteristics for a heterogeneous surface [29]. The

nonlinear representation of the Freundlich model is as in equation

(6):

eFe

CKq



(6)

where K

(mg g

-1

) (L mg

-1

)

and 1/n are the Freundlich constants

related to adsorption capacity and sorption intensity, respectively.

Jovanovic adsorption isotherm is similar to that the Langmuir

model with the approximation of monolayer localized adsorption

without lateral interactions. The assumptions in this model are

same in the Langmuir model in addition with the possibility of the

some mechanical contacts between the adsorption and desorbing

Journal of Environmental Treatment Techniques 2020, Volume 8, Issue 3, Pages: 1023-1028

1025

model [29]. The nonlinear Jovanovic model can be expressed by

equation (7):

 

eqq



 1

(7)

where q

(mg g

-1

) and K

(L mg

-1

) are Jovanovic constants related

to the adsorption capacity and the rate of adsorption, respectively.

Sips isotherm is a combination of the Langmuir and Freundlich

isotherms, which represent systems for which one adsorbed

molecule could occupy more than one adsorption site [30]. The

nonlinear representation of the Sips model is as in equation (8):

)1(





(8)

where q

the Sips maximum adsorption capacity (mg.g

-1

), K

the

Sips equilibrium constant (L mg

-1

) and n

the Sips model

exponent describing heterogeneity. Redlich–Peterson isotherm

model combines elements from both the Langmuir and

Freundlich equation and the mechanism of adsorption is a hybrid

one and does not follow ideal monolayer adsorption. It is used as

a compromise to improve the fit by Langmuir or Freundlich [30].

The nonlinear representation of the Redlich–Peterson model is as

in equation (9):

eRP







(9)

where K

(L g

-1

) and α

(L mol

-1

) are the Redlich-Peterson

isotherm constants, while n

is the exponent, which lies between

0 and 1. Toth adsorption model is developed to describe the

heterogeneous adsorption systems which satisfy both low and

high end boundary of adsorbate concentration. This model is the

modified form of Langmuir isotherm with the intension of

rectifying the error between the experimental and predicted data

[31]. The nonlinear representation of the Toth model is as in

equation (10):

 







(10)

where q

is the Toth maximum adsorption capacity (mg.g

-1

), α

is adsorptive potential constant (mg L

-1

) and n Toth’s

heterogeneity factor.

3 Results and Discussion

3.1 Characterization of Typha australis leaves

The outcome of the ultimate elemental analysis of Typha

australis leaves indicates that oxygen (49.04 %) and carbon

(43.93 %) are the major constituents of Typha australis leaves

along with the quantifiable amount of hydrogen (5.87 %),

nitrogen (0.88 %) and Sulfur (0.28 %). The surface morphology

of Typha australis leaves adsorbent was evaluated according to

the SEM images obtained in Figure 1. There is a change in surface

morphology of the Typha australis leaves before (Figure 1(a)) and

after the adsorption (Figure

1(b)) of MG.

(a)

(b)

Figure 1: Typical SEM micrograph of Typha australis leaves particle

(100 magnification): (a) before MG adsorption and (b) after MG

adsorption.

According to Figure 1(a), the Typha australis leaves before

MG adsorption possesses uneven and irregular surface with

considerable layers of rough heterogeneous pores which offers

high possibility for dye molecules to be adsorbed [32]. Thus, the

SEM image of Typha australis leaves after MG adsorption in

Figure 1(b) reveals smoother surface features with apparent

reduced pore structures, indicating the uptake and entrapment of

MG molecules by the accessible pore vicinities of the Typha

australis leaves surface. Figure 1(b) proves the engagement of

MG onto Typha australis leaves and this may be related to the

presence of carboxylic and hydroxyl groups within Typha

australis leaves, as evidenced by the FTIR spectral reported by

[27], which act as active sites for the adsorption of MG molecules.

3.2 Adsorption isotherm studies

The adsorption isotherm gives an idea of the equilibrium

behavior of an MG–Typha australis leaves system. Figures 2 and

3 shows the experimental equilibrium data and the predicted

theorical isotherms for the sorption of MG onto Typha australis

leaves. The isotherm parameters, obtained using nonlinear

method, are given in Table 1 for 21.4 and 31.4 °C. The values of

1/n, K

and R

are in between zero and one, indicating that the

sorption of MG onto Typha australis leaves sorbent is favorable.

The values of R

are compared, Langmuir isotherm are shown to

have higher values than Freundlich and Jovanovic isotherms.

Journal of Environmental Treatment Techniques 2020, Volume 8, Issue 3, Pages: 1023-1028

1026

0 2 4 6 8 10

(mg g

-1

)

(mg L

-1

)

Experimental data

Langmuir

Freundlich

Jovanovic

Figure 2: Langmuir, Freundlich and Jovanovic non linear for Typha

australis leaves at 21.4 °C

Figure 3: Langmuir, Freundlich and Jovanovic non linear for Typha

australis leaves at 31.4 °C

Table 1: Two- parameter isotherm models for MG retention on the

Typha australis leaves

Models

Parameters

21.4 °C

31.4 °C

Langmuir

85.21

56.88

0.12

0.38

0.077

0.026

SSE

2.34

3.71

(%)

99.85

99.76

Freundlich

1/n

0.67

0.48

10.58

15.77

SSE

9.57

(%)

99.39

98.41

Jovanovic

56.38

44.69

0.176

0.395

SSE

3.04

13.94

(%)

99.81

99.11

The lowest SSE values further confirmed the suitability of

Langmuir model in describing the equilibrium data, suggesting

the existence of monolayer adsorption of MG onto Typha

australis leaves. This result is consistent with the literature where

it is reported that the adsorption of MG using various adsorbents

is well represented by Langmuir isotherm model [33-38].

The parameters for Sips, Redlich–Peterson and Toth

isotherms, obtained using nonlinear method, at 21.4 and 31.4 °C

are given in Table 2. The resulting curves of Sips, Redlich–

Peterson and Toth parameters are compared to the experimental

data at Typha australis leaves sorbent for MG removal in Figures

4 and 5. According to table 2, the results show that the

experimental equilibrium data were best represented by the Sips,

isotherm (R

≥ 99.76). The maximum adsorption capacities

predicted by the Sips and Toth isotherms were lower than the

Langmuir isotherm. Worth mentioning the maximum adsorption

capacities obtained by Sips model, where q

was equal to 31.72

and 20.75 mg g

-1

at 21.4 and 31.4 °C, respectively. Values

attained for Typha australis leaves are inferior to that reported by

[38] for MG removal leaves of Typha angustifolia where q

equal

to 95.78, 83.53 and 83.07 mg g

-1

at 25, 35 and 45 °C, respectively.

0 2 4 6 8 10

(mg g

-1

)

(mg L

-1

)

Experimental data

Sips

Redlich-Peterson

Toth

Figure 4: Sips, Redlich– Peterson and Toth non linear for Typha

australis leaves at 21.4 °C

0 2 4 6 8 10

(mg g

-1

)

(mg L

-1

)

Experimental data

Sips

Redlich-Peterson

Toth

Figure 5: Sips, Redlich– Peterson and Toth non linear for Typha

australis leaves at 31.4 °C

Table 2: Three- parameter isotherm models for MG retention on the

Typha australis leaves

Models

Parameters

21.4 °C

31.4 °C

Sips

31.72

20.75

0.55

1.79

1.27

1.48

SSE

2.17

1.06

R )%(

99.87

99.94

Redlich-Peterson

10.88

25.27

0.14

0.59

0.96

0.89

SSE

2.32

2.36

R)%(

99.85

Toth

1.33

1.94

0.124

0.379

0.125

0.091

SSE

2.34

3.70

R)%(

99.85

99.76

The Sips and Redlich–Peterson isotherm constants (n

and

) is nearly 1, this means that the equilibrium isotherm behaves

as Langmuir, not as Freundlich isotherm. So, the application of

the Langmuir, Sips and Redlich- Peterson isotherms showed that

there was effective monolayer sorption and a homogeneous

distribution of active sites on the surface of the Typha australis

leaves sorbent. The monolayer adsorption capacities were found

to be 85.21 and 56.88 mg g

-1

at 21.4 and 31.4 °C, respectively.

These results are comparable with those reported in the literature

using other raw sorbents such as pineapple leaf powder [39],

0 2 4 6 8 10

(mg g

-1

)

(mg L

-1

)

Experimental data

Langmuir

Freundlich

Jovanovic

02 46 8 10

(mg g

-1

)

(mg L

-1

)

Experimental data

Sips

Redlich-Peterson

Journal of Environmental Treatment Techniques 2020, Volume 8, Issue 3, Pages: 1023-1028

1027

degreased coffee bean [40], Bivalve shell-Zea mays L husk leaf

[41], Chitosan beads [42] and dead leaves of plane tree [43]. A

comparison of q

for MG dye using different sorbents which are

previously reported, was performed and presented in Table 3. It

was noted that Typha australis leaves had better sorption capacity

in comparison to other sorbents listed here.

Table 3: Summary of previously published results for the removal of

MG dye from aqueous medium

Adsorbents

(mg g

-1

)

References

Lignin

31.2

[ 10]

Humic acid

6.4

Rattan sawdust

22.4

[ 18]

Zeolite at 25 °C

23.94

[19]

Zeolite at 35 °C

25.14

Chlorella biomass

18.4

[20]

Sea Shell powder

[21]

Activated Rice Husk

[ 22]

Castor bean presscake

[23]

Cerastoderma lamarcki shell

[24]

Annona squmosa seed

[25]

Diatomite at 25 °C

23.64

[37]

Diatomite at 35 °C

24.88

Diatomite at 45 °C

27.10

Typha australis at 21.4 °C

85.21

This study

Typha australis at 31.4 °C

56.88

This study

This, for instance, allows us to legitimately say that the Typha

australis leaves is a better sorbent for the removal of MG. Typha

australis leaves has a good sorption capacity and could be a

reliable sorbent for the removal of MG.

4 Conclusions

The removal of MG dye using Typha australis leaves as

sorbent was systematically investigated at 21.4 and 31.4 °C. The

best fitting isotherm was found to be the Langmuir isotherm. The

monolayer adsorption capacities were found to be 85.21 and

56.88 mg g

-1

at 21.4 and 31.4 °C, respectively. This homogeneity

was also confirmed by the constant of Sips isotherm. The findings

from this study demonstrated that the use of Typha australis

leaves as an alternative low cost sorbent for the removal MG from

colored effluents is feasible. For future studies, the usability of

Typha australis for dyes removal from real wastewater will be

tested and as comparison, a fixed bed column will be employed

to investigate the effect of reactor design.

Acknowledgment

The authors wish to thank Dr Med Abderrahmany Senhoury

from Materials Chemistry Research Unit, Department of

Chemistry, Faculté des Sciences et Technique, Université de

Nouakchott Al Aasriya, Mauritania, for SEM analysis.

Competing interests

The authors declare that there is no conflict of interest that

would prejudice the impartiality of this scientific work.

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