How to cite:
Iswandi, Dwi Puryanti, Elvaswer. (2022). Remediation of Heavy
Metals in the Leachate of the Final Waste Processing Site Using
Magnetite Nanoparticles. Journal Eduvest. Vol 2(5): 930-937
E-ISSN:
2775-3727
Published by:
https://greenpublisher.id/
Eduvest Journal of Universal Studies
Volume 2 Number 5, May, 2022
p- ISSN 2775-3735- e-ISSN 2775-3727
REMEDIATION OF HEAVY METALS IN THE LEACHATE OF
THE FINAL WASTE PROCESSING SITE USING MAGNETITE
NANOPARTICLES
Iswandi
1
, Dwi Puryanti
2
, Elvaswer
3
Andalas University, Indonesia
Email: [email protected], dwipuryanti@sci.unand.ac.id,
ARTICLE INFO ABSTRACT
Received:
April, 26
th
2022
Revised:
May, 14
th
2022
Approved:
May, 16
th
2022
Nanoparticles are iron oxides that are used in various fields of
life, one of which is to absorb heavy metals. In this study,
magnetite (Fe
3
O
4
) nanoparticles were synthesized using the
correspirate method and magnetite nanoparticle templates
with PEG-6000. Synthesis of magnetite nanoparticles was
carried out to obtain magnetite nanoparticles to be used to
remediate heavy metals Cu, Ni and Mn in waste leachate. The
susceptibility analysis of the leachate sample type showed that
the type of magnetic material. The calculation results from the
XRD diffractogram obtained that the crystal size of Fe
3
O
4
nanoparticles is 56.35 nm. By varying the mass of 0.4 grams of
Fe
3
O
4
, 0.8 grams of Fe3O4 and coating Fe
3
O
4
using PEG 6000,
it is known that the reduction in the concentration of heavy
metal Cu is 7.71%, 23.09% and 42.31%, respectively. The
percentage reduction in the concentration of heavy metal Ni
was 6.29%, 9.45% and 7.09%, respectively.The percentage
reduction in the concentration of heavy metal Mn was
25.369%, 19.98% and 4.05%, respectively. This indicates that
Fe
3
O
4
and PEG-6000 nanoparticles are able to reduce the
concentration of heavy metals in waste leachate contained in
the leachate sample.
KEYWORDS
Synthesis, Nanoparticles, Fe3O4, heavy metal, Remediation,
PEG-6000
This work is licensed under a Creative Commons
Attribution-ShareAlike 4.0 International
Iswandi, Dwi Puryanti, Elvaswer
Remediation of Heavy Metals in the Leachate of the Final Waste Processing Site Using
Magnetite Nanoparticles 931
INTRODUCTION
Human activities using nature always leave residues that are considered no longer
useful so that they are treated as discarded goods, namely garbage and waste (Widyatmoko
dan Sintorini, 2002). This waste and waste if not managed properly will have a negative
impact on the environment and human health. To accommodate garbage and waste
resulting from the daily activities of residents, this waste and waste is accommodated in the
final waste processing site (TPA). In Padang Panjang City, the location of the final waste
processing site is in the Andok River area. The Andok River TPA is close to residential
areas and the river that empties into the Andok River, Manggis Village Village. The Andok
River TPA applies the open dumping method in waste management. The open dumping
method is a management method by leaving the waste open without a cover, only
compacted using heavy equipment, so that when it rains the garbage will be exposed to
rainwater and dissolve the elements contained in the waste that produce leachate.
Leachate is water that is the result of degradation from waste and can cause
pollution if it is not treated before being discharged into the environment. This leachate is
generally toxic because it contains high amounts of microorganisms, contains heavy metals
that are dangerous when exposed to the environment, and others. The quantity and quality
of leachate can also be affected by climate. Rainwater infiltration can carry contaminants
from waste piles and provide the moisture needed for biological decomposition processes
in the formation of leachate. The main source of the formation of this leachate is the
infiltration of rainwater. The high amount of rain and the non-solid nature of the
embankment will accelerate the formation and increase the quantity of leachate produced
(Pohland dan Harper. 1985).
The leachate that comes from new landfills is usually characterized by high fatty
acid content and a high ratio of BOD and COD. Meanwhile, leachate from old landfills will
contain lower BOD, COD and pollutant concentrations. This is because in new landfills,
biodegradation generally takes place rapidly, which is characterized by an increase in acid
production and a decrease in the pH of the leachate which results in the high dissolving
ability of the materials in the waste by water. Comparison of BOD with COD in new
landfills will range from 0.4% to 0.8%, the value will be greater in the methanogenesis
phase. The degradation of waste material in the landfill is caused by biological processes
(Munawar, 2011) Figure 1 is the process of entering the leachate into the TPA.
Figure 1. Leachate Entry Process to TPA (Source: Damanhuri, 2008).
Eduvest Journal of Universal Studies
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932 http://eduvest.greenvest.co.id
The content of heavy metals in leachate from waste include Vanadium (V), Titan
(Ti), Chromium (Cr), Iron (Fe), Cobalt (Co), Zinc (Zn), Rhodium (Rh), Neodinium (Nd),
Manganese (Mn), Europium (Eu), Ytterbium (Yb), Indium (In) and Sircon (Zr) (Iswandi
dkk., 2015). Heavy metals are a group of metal elements with a density greater than 5
g/cm3, at certain levels become toxic and dangerous materials. Heavy metals are one of the
important problems that must be addressed because the effects of heavy metals that enter
the environment can pollute the environment and threaten human health. Heavy metals are
still a metal group with the same criteria as other metals. The difference lies in the effect
produced when these heavy metals enter or are given into the body of living organisms
(Heryanto dan Polar, 2004). One of the effects of heavy metals when they enter the human
body is nervous system and organ system disorders.
One solution that can be done to reduce pollution in the environment, especially in
waters is remediation. Remediation is a way to restore the environment, both water, soil
and air that have been polluted by organic and inorganic pollutants so that pollution is
reduced, especially pollution caused by heavy metals. Advances in technology and
communication today encourage scientists and researchers to make the latest breakthroughs
in an effort to overcome environmental pollution from this heavy metal. Several methods
used to reduce heavy metal levels in the environment are membrane filtration, chemical
precipitation flotation, chitosan, solgel, magnetic adsorption and others. Adsorption
technique is one of the effective techniques applied in reducing heavy metal content in
waters because the magnetic adsorption method is very economical. The adsorption
technique uses an adsorbent to absorb heavy metal content in water or waste. Heavy metals
will be separated from the waste and will unite with the adsorbent. To remediate heavy
metals in waters and waste, an adsorbent is needed that is able to absorb part.
RESEARCH METHOD
Tools and materials
The tools used in this study were measuring cups, beakers, sample boxes, magnetic
strirer C-MAG HS 7, Bartington Susceptibility Meter type MS2, dropper, spatula, digital
scale PGW 2502i, permanent magnet, wathman 40 filter paper, X- Ray Difractometer
(XRD), Atomic Absorption, Spectroscopy (AAS), PH meter, aluminum foil. The materials
used in this study were waste leachate, Polyethylene Glycol 6000 (PEG 6000), Fe3O4
nanoparticles, distilled water, NH4OH solution, 12 M HCL solution, 96% alcohol. The
leachate samples were obtained from the Andok River TPA, Padang Panjang City.
Leachate samples were taken from the landfill leachate reservoir.
Testing the Magnetic Susceptibility Value of Leachate Samples
The process of measuring the magnetic susceptibility value of leachate samples using
a Bartington Susceptibility Meter type MS2. Sample test in 15 directions was performed
on LF (Low Frequency) and HF (High Frequency). Magnetic susceptibility test with dual
frequency is to determine the value of FD (%) (Frequency dependent susceptibility) so that
the presence of superparamagnetic particles in the sample can be known.
Fe3O4. nanoparticle synthesis process
The Fe3O4 nanoparticle synthesis process was carried out by washing Fe3O4 using
distilled water. Then add 20 ml of HCL solution at a temperature of 900C, then dissolved
and stirred for about 60 minutes using a magnetic stirrer. Filter the solution using filter
paper. Add 25 ml of solution with ammonia, let stand for 30 minutes until precipitation
Iswandi, Dwi Puryanti, Elvaswer
Remediation of Heavy Metals in the Leachate of the Final Waste Processing Site Using
Magnetite Nanoparticles 933
occurs. Wash the precipitate with distilled water until it is clean and the ammonia smell is
gone. then the samples were dried using a furnace at a temperature of 900C for 2 hours.
Furthermore, the results of the dry deposition were carried out by XRD test to see the
structure and crystal size of the sample. To calculate the crystal size of the sample we use
the Scherrer equation, as in equation 1 below:
(Equation 1)
The process of absorption of Cu, Ni and Mn. metals
The metal uptake process in leachate was carried out by dissolving 0.4 grams of
Fe3O4 into 80 ml of leachate, then stirred using a magnetic stirrer. At the beginning of the
stirring process, the solution was given NH4OH with levels adjusted to the pH conditions
for each sample. The resulting solution was then stirred using a magnetic stirrer with a
stirring time of 3 hours and room temperature conditions. After the stirring process is
complete, the solution is placed on a permanent magnet for one hour. Furthermore, the
solution that has been separated from the precipitate is filtered with filter paper, then the
AAS test is carried out.
Furthermore, the samples were used for the absorption of Cu, Ni and Mn metals with
Fe3O4 variations of 0.8 grams. Samples were adsorbed on Cu, Ni and Mn metals with
Fe3O4 coating using PEG 6000 with a mass ratio of 1:1. The percentage decrease in metal
content is calculated by equation 2 below:
% Decrease =
𝒊𝒏𝒊𝒕𝒊𝒂𝒍 𝒎𝒆𝒕𝒂𝒍 𝒄𝒐𝒏𝒕𝒆𝒏𝒕−𝒇𝒊𝒏𝒂𝒍 𝒎𝒆𝒕𝒂𝒍 𝒄𝒐𝒏𝒕𝒆𝒏𝒕
𝒊𝒏𝒊𝒕𝒊𝒂𝒍 𝒎𝒆𝒕𝒂𝒍 𝒄𝒐𝒏𝒕𝒆𝒏𝒕
X 100 ( Equation 2 ).
RESULT AND DISCUSSION
1. Characterization of Fe3O4 . Magnetic Nanoparticles
The characterization of magnetite nanoparticles using XRD is shown in Figure 2.
XRD results in Fig. 2 shows that the Fe3O4 phase has formed in the synthesized sample,
this is indicated by the presence of Fe3O4 peaks that appear. The highest Fe3O4 intensity
appeared at 2 of 35.6322. This high intensity indicates that the crystal has good crystal
order or the more atoms are arranged in an orderly and neat manner. Based on the
identification of data matching, the diffraction peaks at an angle of 2 for the Fe3O4 phase
formed were 30.158, 35.522, 43.2202, 53.8947, 57.3404, 62.8457, 90.1376. While the
Miller index of the Fe3O4 phase formed is (220), (311), (400), (422), (511), (440), (731).
Figure 2 X-ray diffraction pattern of Fe3O4. nanoparticles
Eduvest Journal of Universal Studies
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934 http://eduvest.greenvest.co.id
The results of this diffraction indicate that the synthesis process has succeeded in
obtaining Fe3O4 material. The result of the calculation of the crystal size calculated using
the Scherrer equation shows that the crystal size of Fe3O4 is 56.35 nm. The results of the
X-ray diffractogram show that in addition to the Fe3O4 phase, there are also other phases
related to impurities in the tested sample. The impurity phase that appears is the -Fe2O3
(hematite) phase. Fe2O3 is an antiferromagnetic material with a hexagonal structure and is
formed in the sample which is predicted as a result of the Fe3O4 oxidation process. The
sample obtained from this synthesis process is dominated by a dark black color which
indicates the characteristics of Fe3O4 material, while Fe2O3 has a physical appearance
which is characterized by a brown color.
2. Magnetic Susceptibility Analysis of Leachate Samples
The results of measuring the magnetic susceptibility values of the Andok River
TPA leachate samples using the Bartington Susceptibility Meter type MS2 ranged from
326.4 x 10-8 m3/kg to 329.3 x 10-8m3/kg at high frequencies while at low frequencies the
leachate susceptibility values ranged from 300.2 x 10- 8 m3/kg to 333.1 x 10-8 m3/kg. This
value range indicates that the leachate sample belongs to the hematite material. The results
of the calculation of the value of FD (%) (Frequency dependent susceptibility) of the
leachate sample is 0.79%, this indicates that the sample contains less than 10%
superparamagnetic grains.
3. Initial Content of Heavy Metals Cu, Ni and Mn
Testing the levels of heavy metals in leachate using Atomic Absorption
Spectrophotometry (AAS). The results of testing the levels of heavy metals Cu, Ni Mn in
leachate without the addition of Fe3O4 were 0.1711 ppm, 0.3144 ppm and 0.1656 ppm, as
shown in Table 1 below:
Table 1 Heavy metal content in leachate without the addition of Fe3O4
No
Concentration (ppm)
1
0.1711
2
0.3144
3
0.1656
4. Heavy Metal Cu Uptake in Leachate
In the heavy metal absorption process, Cu was absorbed three times with variations
in the addition of Fe3O4 magnetic nanoparticles as shown in Table 2 with an initial
concentration of 0.1711 ppm Cu heavy metal.
Table 2 Results of absorption of heavy metal Cu with the addition of absorbent
No
Variation of Absorbent
Concentration (ppm)
% Decrease
1
Sample lindi (Fe
3
O
4
+ PEG 6000)
0.0987
42.31
2
Sample lindi (0.8 gr Fe
3
O
4
)
0.1316
23.09
3
Sample lindi (0.4 gr Fe
3
O
4
)
0.1579
7.71
The absorption of Cu heavy metal by varying the mass of the adsorbent shows that the
heavy metal is adsorbed by Fe3O4 magnetic nanoparticles. This absorption occurs because
there is an active site on the Fe3O4 adsorbent. The biggest absorption occurred when the
addition of Fe3O4 magnetic nanoparticles with PEG 6000 with a percentage decrease of
42.31%. PEG 6000 functions as a template, which wraps the particles so that no further
aggregates are formed, because PEG 6000 sticks to the particle surface and covers the
positive ions in question to hang and enlarge, so that in the end you will get particles with
Iswandi, Dwi Puryanti, Elvaswer
Remediation of Heavy Metals in the Leachate of the Final Waste Processing Site Using
Magnetite Nanoparticles 935
a uniform spherical shape. Therefore, Fe3O4 coated with PEG 6000 adsorbed metal ions
better.
a. Ni Heavy Metal Uptake in Leachate
In the Ni heavy metal absorption process, three absorptions were carried out with
variations in the addition of Fe3O4 magnetic nanoparticles as shown in Table 3 with an
initial concentration of 0.3144 ppm Ni heavy metal.
Table 3. The results of the absorption of heavy metal Ni with the addition of absorbent
The absorption of heavy metal Ni by varying the mass of the adsorbent was found
that the heavy metal was adsorbed by Fe3O4 magnetic nanoparticles. This absorption
occurs because there is an active site on the Fe3O4 adsorbent. The greatest absorption
occurred when the addition of magnetic nanoparticles Fe3O4 0.8 g with an absorption of
9.45%. The absorption with the PEG 6000 template was lower than the absorption using
0.8 g 0.8 g Fe3O4 . This can happen because in the synthesis process, hematite (Fe2O3)
remains.
b. Mn Heavy Metal Uptake in Leachate
In the heavy metal absorption process, Mn was absorbed three times with variations
in the addition of Fe3O4 magnetic nanoparticles as shown in Table 4 with an initial
concentration of 0.1656 ppm Mn heavy metal.
Table 4. Results of absorption of heavy metal Mn with the addition of absorbent
No
Variation of Absorbent
Concentration (ppm)
% Decrease
1
Sample lindi (Fe
3
O
4
+ PEG 6000)
0.1589
4.05
2
Sample lindi (0.8 gr Fe
3
O
4
)
0.1325
19.98
3
Sample lindi (0.4 gr Fe
3
O
4
)
0.1236
25.36
The absorption of heavy metal Mn by varying the mass of the adsorbent showed
that the heavy metal was adsorbed by Fe3O4 magnetic nanoparticles. This absorption
occurs because there is an active site on the Fe3O4 adsorbent. The biggest absorption
occurred when the addition of magnetic nanoparticles Fe3O4 0.4 g with an absorbent of
25.36%. The measurement results show that Fe3O4 and PEG 6000 nanoparticles can be
used as adsorbents in heavy metal remediation in waste leachate.
CONCLUSION
Based on the results of research that has been carried out in heavy metal remediation
in landfill waste leachate, it can be concluded as follows:
1. Based on the magnetic susceptibility value of the leachate sample measured using the
Bartington susceptibility meter, it shows that the leachate sample belongs to the
hematite material, while the results of the calculation of the FD (%) (Frequency
No
Variation of Absorbent
Concentration (ppm)
% Decrease
1
Sample lindi (Fe
3
O
4
+ PEG
6000)
0.2921
7.09
2
Sample lindi (0.8 gr Fe
3
O
4
)
0.2847
9.45
3
Sample lindi (0.4 gr Fe
3
O
4
)
0.2946
6.29
Eduvest Journal of Universal Studies
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936 http://eduvest.greenvest.co.id
dependent susceptibility) value of the leachate sample are 0.79%, this indicates that the
sample contains less of 10% superparamagnetic grains.
2. The measurement results using XRD showed that the synthesized Fe3O4 crystal size
was 56.35 nm.
3. Fe3O4 nanoparticles can be used as adsorbent for remediation of heavy metal levels of
Cu, Ni and Mn in waste leachate.
4. Coating Fe3O4 nanoparticles with PEG 6000 can be used as an adsorbent in
remediating heavy metal levels in waste leachate.
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