Environment and Natural Resources Journal 2022; 20(6): 634-643

Selectivity of Malachite Green on Cationic Dye Mixtures Toward

Adsorption on Magnetite Humic Acid
Nur Ahmad1,3, Fitri Suryani Arsyad2, Idha Royani2, and Aldes Lesbani2,3*
1Magister Program in Environment Management, Sriwijaya University, Jl. Padang Salasa No. 524 Ilir Barat 1, Palembang 30139,
South Sumatera, Indonesia
2Graduate School, Faculty of Mathematics and Natural Sciences, Sriwijaya University, Jl. Palembang-Prabumulih, Km.90-32,

Ogan Ilir, South Sumatera, Indonesia

3Research Center of Inorganic Center of Inorganic Materials and Complexes, Faculty of Mathematics and Natural Sciences,

Sriwijaya University, Jl. Padang Salasa No. 524 Ilir Barat 1, Palembang 30139, South Sumatera, Indonesia

ARTICLE INFO ABSTRACT

Received: 29 Jun 2022 Magnetite humic acid (MHA) was successfully synthesized by the
Received in revised: 31 Jul 2022 coprecipitation method followed by hydrothermal process, as evidenced by the
Accepted: 8 Aug 2022
XRD, FTIR, VSM, and SEM analysis characterization results. XRD diffraction
Published online: 7 Sep 2022
shows diffraction peaks at 2θ=21.53º, 35.95º, and 57.93º. The FTIR spectra have
DOI: 10.32526/ennrj/20/202200142
a typical absorption at 3,410, 1,589, 1,396, 1,026, 910, 794, and 540 cm-1.
Keywords: Magnetite humic acid was paramagnetic with magnetization (Ms) 17.04 emu/g.
Magnetite/ Humic acid/ Selectivity/ Humic acid and magnetite humic acid have an irregular structure; the morphology
Malachite green/ Adsorption of magnetite humic acid is smoother than humic acid. Malachite green was more
selective than methylene blue and rhodamine B on magnetite humic acid. The
* Corresponding author: adsorption of malachite green on humic acid and magnetite humic acid was
E-mail: carried out at pH pzc 8.06 and 6.08. The adsorption capacity (Q max) of humic acid
aldeslesbani@pps.unsri.ac.id (77.519 mg/g) and magnetite humic acid (169.492 mg/g) were found with
pseudo-second-order kinetic and Langmuir isotherm models. After five
regeneration cycles, the adsorption percentages of malachite green with humic
acid and magnetite humic acid ranged from 94.67-61.37% and 62.03-21.11%,
respectively. Magnetite humic acid has high stability and reusability. The good
regeneration of MHA was supported by the XRD diffractogram. Magnetic
properties in the material simplify the adsorption process and minimize the
potential for damage to the surface of the material.

1. INTRODUCTION There are different technologies for removing

Textile wastewater is a severe problem for the dyes from textile wastewater, such as membrane
environment. Textile wastewater pollutes water, (Januário et al., 2022), electrocoagulation (Signorelli et
which is a basic human need. The industrial sector al., 2021), photocatalytic (You et al., 2022), and
uses 100,000 dyes to generate textile wastewater adsorption (Sachdev et al., 2022; Zhang et al., 2020).
(Fazal et al., 2018; Khalaf, 2008). However, only 8% The adsorption process is suitable for its simplicity,
of Textile wastewater is treated before being effectivness, efficiency, and low cost. Several
discharged into waters (Roohi et al., 2016). adsorbents have been reported, including kaolin
Wastewater is dangerous for the environment and (Angerasa et al., 2021), bentonite (Wang et al., 2021a),
human health because of the carcinogenic effects layer double hydroxide (Lesbani et al., 2020; Wijaya et
caused by these dyes. Malachite green (MG) dye is al., 2021), and humic acid (Yang and Antonietti, 2020).
used in textile and paper industries, and even in food Humic acid (HA) is extracted from peat soil
coloring additives (Srivastava et al., 2004). Malachite with -COOH and -OH groups (Stevenson, 1994).
green can cause disturbances in the immune and Humic acid is one of the fractions of humic
reproductive systems (Das and Dhar, 2020) and even compounds that are naturally occurring in soil organic
cause kidney failure (Eltaweil et al., 2020). matter. Humic acid (HA) has the potential for

Citation: Ahmad N, Arsyad FS, Royani I, Lesbani A. Selectivity of malachite green on cationic dye mixtures toward adsorption on magnetite humic
acid. Environ. Nat. Resour. J. 2022;20(6):634-643. (https://doi.org/10.32526/ennrj/20/202200142)

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adsorption because of its high adsorption capacity, and method followed by hydrothermal process (Taher et
use in organic and inorganic pollutants (Shao et al., al., 2021). FeCl3 (0.6488 g) and FeSO4·7H2O (0.5560
2021). However, the structure of humic acid is easily g) was added to 6 mL of distilled water, then stirred
damaged and difficult to separate from aqueous until dissolved. The mixture was added to 1 g of humic
solution. Magnetite (Fe3O4) is an iron oxide of the acid (HA) and stirred for 3 h at room temperature. NH3
spinel mineral group (She et al., 2021). Magnetite has (3 mL) was added to the mixture slowly, then stirred
been applied to adsorption for water treatment for 30 min at 75ºC. The obtained slurry was transferred
(Abdullah et al., 2022; Paz et al., 2022), catalysts (Liu to Teflon for hydrothermal treatment for 3 h at 150ºC.
et al., 2018), membrane processes (Vu et al., 2020), The slurry was washed and then dried at 100ºC.
and biodegradation (Shen et al., 2021). Magnetite, in
adsorption, imparts its magnetic properties to HA, and 2.3 Determination of functional group of HA and
it can separate the adsorbent from the solution using MHA
an external magnet (Lee and Kim, 2022). Composite 2.3.1 Total acidity
magnetite with humic acid (MHA) has been reported HA (0.1 g) or MHA (0.1 g) were added to
for removing phosphate (Rashid et al., 2017), gold ion Ba(OH)2 saturated solution (20 mL) under N2
adsorption (Santosa et al., 2021a), and removing atmosphere and stirred for 24 h at 25ºC. Afterward,
Pb(II) (Lu et al., 2019). Selectivity and adsorption of the HA or MHA treated was filtered using Whatman
MHA for malachite green has not been registered. paper and washed with distilled water. The filtrate
In this study, Magnetite Humic Acid (MHA) and wash water were combined and then titrated with
was synthesized by the conventional coprecipitation HCl (0.5 M) to pH 8.4 (Santosa et al., 2021a). The total
method followed by hydrothermal process as acidity of HA and MHA was then calculated by
evidenced by the characterization results using Equation (1):
XRD, FTIR, VSM, and SEM analysis. A selectivity
(V0 − Vs ) × M × 105
test was performed by mixing cationic dyes to Total acidity (cmol/kg) = (1)
W
determine the dye used for the adsorption process.
Adsorption processes such as kinetic, isotherm, and Where; V0 and Vs are the volume of HCl for
thermodynamic, and the stability of the adsorbent with titrated blank solution and sample, respectively; M is
regeneration were evaluated. the molarity of HCl; W is the mass of HA and MHA.

2. METHODOLOGY 2.3.2 Carboxyl content

2.1 Materials and instruments HA (0.1 g) or MHA (0.1 g) were added to the
Humic acid (HA) was extracted from the peat mixture of Mg(CH3COO)2 0.5 M (10 mL) and distilled
soil of South Sumatra, Indonesia. Chemicals water (40 mL) under N2 atmosphere and stirred for 24
(analytical-grade reagent) used in this study, FeCl3 h at 25ºC. Afterward, the treated HA or MHA was
(Merck, 162.2 g/mol), FeSO4·7H2O (Merck, 278.01 filtered using Whatman paper and washed with
g/mol), HCl (MallinckrodtAR®, 37%), NaOH (40 distilled water. The filtrate and wash water were
g/mol), and NH3 (25%) were purchased from combined then titrated with NaOH (0.1 M) to pH 9.8
EMSURE® ACS. Distilled water was purchased from (Santosa et al., 2021a). The carboxyl content was
PT. Bratachem Indonesia. Analytical instrumentals determined using Equation (2):
used included UV-Vis Spectrophotometer type
Biobase BK-UV 1800 PC (China), Fourier Transfer (V0 − Vs ) × M × 105
Carboxyl content (cmol/kg) = (2)
W
Infra-Red (FTIR, Japan) type Shimadzu Prestige-21,
X-Ray Diffractometer (XRD, Japan) type Rigaku
Miniflex-6000, Vibrating Sample Magnetometer Where; V0 and Vs are the volume of NaOH for
(VSM, England) type OXFORD VSM1.2H, and FEI titrated blank solution and sample, respectively; M is
Quanta 650 Scanning Electron Microscope (SEM, the molarity of NaOH; W is the mass of HA and MHA.
England) OXFORD.
2.3.3 Phenolic hydroxyl content
2.2 Synthesis of magnetite humic acid (MHA) Phenolic hydroxyl content is the difference
MHA was synthesized by coprecipitation between total acidity and carboxyl content. Phenolic
hydroxyl content was determined using Equation (3):

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Phenolic hydroxyl content (cmol/kg) (3) 343 K) in each beaker. After stirring at 100 rpm, MHA
= Total acidity − Carboxyl content was separated from the malachite green using an
external magnet. The adsorption isotherms were
2.4 Selectivity of cationic dye mixture analyzed by Langmuir and Freundlich isotherms
Selectivity was carried out to determine the most model with the following Equations 6 and 7,
adsorbed dye by the adsorbent. Selectivity was respectively.
performed using a mixture of 25 mg/L of rhodamine B,
Ce Ce 1
malachite green, and methylene blue. HA and MHA (20 = + (6)
Qe Qm Qm KL
mg) were added to 20 mL of the cationic dye mixture
and shaken for 15, 30, 60, 90, 120, and 150 min. The log Qe = log K F − 1⁄n log Ce (7)
absorbance was measured at the wavelength scan.
Where; Ce (mg/L) and Q e (mg/g) are the
2.5 Determination of pHpzc of MHA concentration of malachite green and adsorption
pHpzc of HA and MHA was determined by the capacity at equilibrium, respectively (mg/g); Q m
conventional pH-drift method. HA and MHA (20 mg) (mg/g) is the maximum adsorption capacity; K L and
were added to 20 mL of 1 M NaCl at various pH K F are the rate constant at Langmuir and Freundlich,
from 2 to 11 (Tombácz and Szekeres, 2004). HCl 0.1 respectively.
M or NaOH 0.1 M was added to adjust the initial pH The thermodynamic equation and the Gibbs
of the NaCl. Then, the mixture was shaken for 24 h. free energy were determined using Equations 8 and 9,
The final pH of each NaCl was measured. respectively.
Qe ∆S ∆H
2.6 Adsorption of malachite green ln = − (8)
Ce R RT
2.6.1 Adsorption kinetics
HA and MHA (20 mg) were added into 20 mL ∆G° = ∆H − T∆S (9)
of malachite green with 60 mg/L, which had been
adjusted at pHpzc. Stirring is done with time variations Where; Ce (mg/L) and Q e (mg/g) are the
of 10, 20, 30, 40, 50, 60, 70, 90, 120, 150, and 180 min concentration of malachite green and adsorption
in each beaker at 303 K. After stirring at 100 rpm, capacity at equilibrium, respectively (mg/g); ∆S
MHA was separated from the malachite green using (J/mol.K) is the entropy; ∆G° (kJ/mol) is the Gibbs
an external magnet. The dye solution has been free energy. ∆H (kJ/mol) is the enthalpy; R (J/mol/K)
separated is then measured its absorbance using a UV- is the gas constant; T (K) is the temperature.
Vis at 617 nm. The adsorption kinetics were analyzed
by pseudo-first-order (PFO) and pseudo-second-order 2.6.3 Regeneration of MHA
(PSO) with the following Equations 4 and 5, HA and MHA (20 mg) were added to 20 mL of
respectively. malachite green with a concentration of 80 mg/L
adjusted at pHpzc. Stirring was carried out for 2 h at
k1
log(Qe − Qt ) = log Qe − (
2.303
)t (4) 303 K. After the stirring process is complete, the
adsorbent is separated from the adsorbate. After that,
1 1 1
= + (5) the desorption process (distilled water medium) was
Qt k2 Qe 2 Qe
carried out to remove the dye from the adsorbent. HA
Where; Q e and Q t are adsorption capacity at and MHA were reused two to five times in the
equilibrium and t, respectively (mg/g); k1 (min-1) and adsorption and desorption processes.
k 2 (g/mg/min) are the rate constant at PFO and PSO,
respectively; t is the adsorption time of malachite 3. RESULTS AND DISCUSSION
green (min). 3.1 Characteristics of HA and MHA
XRD diffractogram of HA as shown in Figure
2.6.2 Adsorption isotherms 1(a) 21.53º, 25.03º, 35.75º, 55.08º, and 62.31º. XRD
HA and MHA (20 mg) were added into 20 mL diffraction of MHA shows diffraction peaks at
of malachite green with 50, 75, 100, 150, 175, and 200 2θ=21.53º, 35.95º, and 57.93º. The diffraction peaks
mg/L, which had been adjusted at pHpzc - stirring for that appear at 2θ=21.53º (002) indicate the presence of
2 h with various temperatures (303, 313, 323, 333, and high amounts of carbon contained in humic acid

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(Zhang et al., 2018). The diffraction peaks at O stretching in COO- (carboxyl content) (Anjum et al.,
2θ=35.75º (311) and 57.93º (511) are originally peaks 2019). The peak at 910 cm-1 is related to C=C bending
from Magnetite (Santosa et al., 2021b). and 540 cm-1 indicating the presence of metal ions in
The FT-IR spectra of HA and MHA are shown HA. After HA was modified with magnetite (MHA) at
in Figure 1(b). HA has a typical absorption at 3,410 540 cm-1, the absorption became sharper indicating the
cm-1 related to OH group stretching from phenolic presence of Fe-O. A new peak was observed at
hydroxyl content (Ahmad et al., 2022), 1,589 cm-1 as wavenumber 794 cm-1 due to the interaction between
C=C stretching, 1,396 and 1,026 cm-1 indicated as C- C-O and Fe-O.

Figure 1. XRD diffractogram (a) and IR spectra (b) of (1) HA, (2) MHA. The measured room temperature magnetization curve of MHA (c)

The magnetic curve of MHA was measured surface of MHA is smooth because it is synthesized by
using VSM. Figure 1(c) showed MHA was hydrothermal process.
paramagnetic with magnetization (Ms) 17.04 emu/g.
The magnetization (Ms) MHA was lower than Fe3O4 3.2 Determination of functional group of HA and
(66.3 emu/g) because Fe3O4 was classified as MHA
superparamagnetic (Santosa et al., 2021b). Figure 2 Total acidity and carboxylic content were
shows the surface morphology of HA and MHA by determined by titration using Ba(OH)2 saturated
SEM images. HA and MHA have irregular structures. solution and Mg(CH3COO)2, respectively (Stevenson,
The morphology of MHA is smoother than HA. The 1994). The total acidity, carboxyl content, and
Phenolic -OH of HA and MHA are displayed in Table

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1. MHA had a drastic decrease in the total acidity and then interact with positively charged Fe2+ and Fe3+
carboxyl content, respectively, from 670 cmol/kg to form Fe3O4 (Koesnarpadi et al., 2015). However, the
317.50 cmol/kg and 296 cmol/kg to 59.33 cmol/kg. carboxyl group more readily interacts with Fe3O4 than
This is due to the preparation of MHA carried out the phenolic -OH, so the carboxyl group’s reduction is
under alkaline conditions (addition of NH3). The very drastic.
carboxyl content and phenolic -OH are iodized and

(a) (b)

Figure 2. SEM images of HA (a) and MHA (b)

Table 1. Total acidity, carboxyl content, and phenolic -OH of HA and MHA

Functional group Stevenson (1994) Santosa et al. (2021a) (cmol/kg) This study (cmol/kg)
(cmol/kg) HA MHA HA MHA
Total acidity 570-890 710.66 320.44 670 317.50
Carboxyl content 150-570 315.79 87.43 296 59.33
Phenolic -OH 150-400 394.87 233.01 374 258.17

3.3 Selectivity adsorbent moves from the HA and MHA surface to the solution
Figure 3 shows a wavelength scan for and lowers pH of the solution.
selectivity of malachite green. MHA adsorbed
malachite green higher than rhodamine B and
methylene blue. The drastic decrease in malachite
green concentration indicated that the malachite green
structure was smaller than methylene blue and
rhodamine B (Mohadi et al., 2021; Palapa et al., 2021).
Therefore, malachite green is used for the adsorption
process.

3.4 pHpzc of HA and MHA

pHpzc of HA and MHA is the point neither
positively nor negatively charged (Derakhshani and
Naghizadeh, 2018). Through the movement of H+ ions
from the HA and MHA surface, the pHpzc can be easily
measured. Figure 4 shows the movement of H+ after
24 h in the shaker. At low pH, H+ moves from the
Figure 3. Wavelength scan of adsorption by MHA into a mixture
solution to the HA and MHA surface during shaking of MG, MB, and RhB
and increases pH of the solution. At high pH, H+

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The meeting point between the initial and final 3.5 Adsorption of malachite green
pH shows no movement of H+ ions, which means that Figure 5(a) shows that the adsorbed
this meeting point is that pHpzc. As shown in Figure 4, concentration of malachite green increased with time
pHpzc of HA and MHA were at pH 8.08 and 6.08, and was constant at 120 min. Pseudo-first-order and
respectively. In a solution with a pH less than pHpzc, pseudo-second-order kinetic adsorption parameters of
HA, and MHA are positively charged and at pH higher malachite green are shown in Table 2. The data in
than pHpzc, HA, and MHA are negatively charged. Table 2 shows that the value of the coefficient
correlation in the adsorption process of malachite
green using HA and MHA adsorbent tends to be a
pseudo-second-order. The coefficient correlation (R2)
for pseudo-second-order is higher than pseudo-first-
order. It means that the greater the concentration of the
malachite green, the more adsorbed. Therefore, the
adsorption process can be followed by chemisorption
(Liu et al., 2020; Siraorarnroj et al., 2022).
Based on Table 2 and Figures 5(b) and 5(c), the
coefficient correlation (R2) of HA and MHA for
Langmuir isotherm is higher than Freundlich isotherm
at temperature 303 K. The adsorption process tends
to follow the Langmuir isotherm. Therefore, the
adsorption process can be followed by monolayer
adsorption (Wang et al., 2021b). Adsorption capacity
(Qmax) of HA and MHA was 77.519 and 169.492 mg/g,
Figure 4. pHpzc of HA and MHA respectively. Adsorption of malachite green by several
adsorbents is shown in Table 3.

Table 2. Kinetic and isotherm model parameter of adsorption on MHA

Kinetic parameter Parameter Adsorbent

HA MHA
Pseudo-first-order Qeexp (mg/g) 41.981 56.075
Qecalc (mg/g) 52.918 78.289
k1 (min-1) 0.002 0.002
R2 0.980 0.966
Pseudo-second-order Qeexp (mg/g) 41.981 56.075
Qecalc (mg/g) 54.945 71.942
k2 (g/mg/min) 0.0004 0.0003
R2 0.990 0.990
Isotherm parameter Parameter Adsorbent
HA MHA
Langmuir Qmax 77.519 169.492
kL 0.047 0.042
R2 0.968 0.992
Freundlich N 1.294 2.396
kF 3.105 21.617
R2 0.866 0.935

Table 3. Comparison of HA and MHA with several adsorbents in terms of the adsorption capacity of malachite green

Adsorbent Qmax (mg/g) Reference

Date stones 98 Hijab et al. (2021)
CuCr-[𝛼-SiW12O40] 55.322 Palapa et al. (2020)
ZIF-8@Fe/Ni 151.520 Zhang et al. (2021)

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Table 3. Comparison of HA and MHA with several adsorbents in terms of the adsorption capacity of malachite green (cont.)

Adsorbent Qmax (mg/g) Reference

Chitosan-DES B 17.86 Sadiq et al. (2020)
EPS of Lysinibacillus sp. SS1 178.57 Miyar et al. (2021)
GALA 113.5 Chen et al. (2020)
Plasma-based biomass 15.55 Al-Yousef et al. (2021)
S@TP Biochar 30.18 Vigneshwaran et al. (2021)
Chinese fan palm seed biochar 21.4 Giri et al. (2022)
HA 77.519 This study
MHA 169.492 This study

(a) (b)

(c) (d)

Figure 5. Effect of contact time (a), effect of initial concentration and temperature (b) and (c), regeneration (d) of HA and MHA

Table 4 shows the thermodynamic data of HA regeneration cycles of HA and MHA, the adsorption
and MHA for adsorption of malachite green. The value percentages of malachite green decreased from 94.6-
of ∆G° is negative, meaning that the adsorption takes 61.37% and 62.03-21.11%, respectively. Magnetic
place spontaneously. ∆H is positive, meaning that the properties in the material simplify the adsorption
adsorption is endothermic and requires energy for the process and minimize the potential for damage to the
adsorption process. ∆S is positive, meaning that there material’s surface. MHA has high stability and
is an increase in irregularity on the surface of the reusability of adsorbent up to five times. The good
adsorbent. Based on Figure 5(d), during five regeneration of MHA indicates that MHA has good

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Table 4. Adsorption thermodynamic parameter

Adsorbent ∆H ∆S ∆G (kJ/mol) R2
(kJ/mol) (kJ/mol) 303 K 313 K 323 K 333 K 343 K
HA 8.189 0.029 -0.582 -0.871 -1.161 -1.450 -1.740 0.998
MHA 12.940 0.055 -3.764 -4.316 -4.867 -5.418 -5.969 0.988

stability, supported by the XRD diffractogram after ACKNOWLEDGEMENTS

adsorption with no significant changes as shown in Authors thank Research Center of Inorganic
Figure 6. The diffraction peaks at 2θ=21.53º (002), Materials and Complexes, Faculty of Mathematics and
35.95º (311), and 57.93º (511) can still be observed. Natural Sciences, Sriwijaya University for
The adsorption mechanism can be studied from instrumental analysis.
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