Republic of the Philippines

BATANGAS STATE UNIVERSITY

Chemical and Food Engineering Department

SYNTHESIS OF MAGNETIC GRAPHENE OXIDE FROM OIL

PALM LEAVES FOR REMOVAL OF LEAD (II) IONS FROM

WATER

Bool, Reaner Jacqueline

A. Luwalhati, Ghia C.

Tan, Nicole

Elizabeth ChE-3101
 I. RATIONALE

Water is an essential substance needed for life in this world. With the advancement of

society, however, the quality of water sources is becoming progressively worse. The age of

industrialization, along with the increase of human population, has brought dramatic increase in

pollution levels. Because of this, access to clean water has become increasingly difficult in

various parts of the world. Toxic pollutants which include organic pollutants, radioactive

substances, and heavy metals have been affecting water quality. Devising ways of purifying

water is therefore essential in combatting this growing problem. Several researches on removing

toxic heavy metal ions have emerged in hopes of addressing one of the biggest environmental

concern that endangers human health.

Removal of pollutants in water is considered to be one of the principal challenges in

today's time. In fact, there are various techniques proposed in order to purify water resources,

such as coagulation, chemical precipitation, photocatalysis oxidation and adsorption. However,

adsorption is studied to be one of the most efficient methods of removing pollutants present in

water due to its low cost and much higher removal efficiency of pollutants. Furthermore,

different materials were experimented for the potential of this method, such as clay minerals,

polymers, zeolites, and mesoporous materials. Yet, these materials possess low adsorption

capacity and are unstable at low or high pH values (Liu et al., 2019).

Graphene is prominently known for its wide applications in different fields of research

and engineering. Out of these applications, graphene is deemed to be one of those notably used

material in water purification because of its remarkable nature. One striking derivative of

graphene is the graphene oxide, which turned out to be a potential material for the pre-

concentration of the heavy metal ions based on its relatively large specific area, abundant

functional groups, and extraordinary

merit in removing heavy metal ions from aqueous solutions, such as lead (Pb(II)), copper

(Cu(II)), cobalt (Co(II)), cadmium (Cd(II)), chromium (Cr(VI)). In spite of these merits, a strong

inter- functional bond between graphene sheets exists, leading to inactive surface chemical

properties, decreased surface area, and low dispersion and agglomeration in aqueous solutions.

These drawbacks limit the performance of its adsorption ability and further applications in

wastewater treatment. Several GO-based materials including chemical modification of GO,

fabrication of GO/metal oxide composites, GO/organic compound composites,

GO/photocatalytic composites, have been methodically synthesized as remarkable adsorbents

having high efficiency to enhance and eliminate various heavy metal ions from wastewater to set

right the mentioned drawbacks (Liu et al., 2019).

With superior magnetic properties and great biocompatibility, iron oxide nanoparticles

can be utilized in the magnetic separation of heavy metals in water resources. Other features of

iron oxide nanomaterials that would aid in the magnetic separation are the high surface-area-to-

volume ratio, the surface modifiability, and their extremely small size. With an appropriate

magnetic field, a convenient and low cost way for the separation through magnetic nanoparticles

are possible without slow and tedious filtration or centrifugation (Ain et al., 2020). Synthesizing

a magnetic adsorbent will, therefore, be helpful in improving heavy metal removal in water.

The aim of this study is to synthesize magnetic graphene oxide (MGO). Graphene oxide

can be prepared in a number of ways. The bottom-up method can be utilized in synthesizing this

material. In this method, the raw material from which graphene oxide will be made is glucose

(Tang et al., 2012). This technique was found to be safe, simple, easy to control, and more

environmental-friendly in comparison with other methods which utilize strong oxidizers.

Through
the catalytic spray method, graphene oxide can be synthesized from the cellulose of a natural

material (Fathy et al., 2019). Oil palm leaves were chosen to be the source of the needed

cellulose. The synthesized graphene oxide will then be combined with magnetic nanoparticles to

improve its performance in adsorbing heavy metals, particularly lead (II) ions. Lead (Pb) can

lead to severe problems in health, specifically in the nervous system, for both animals and

humans. This study therefore seeks to test the efficiency of MGO as an adsorbent for the removal

of lead (II) ions from water.

II. OBJECTIVES

General Objective

- To produce magnetic graphene oxide for the removal of Lead (II) ions from water.

Specific Objective/s:

- To synthesize graphene oxide from palm oil leaves through a green route.

- To prepare magnetic graphene oxide by using co-precipitation method.

- To test the efficiency of the synthesized magnetic graphene oxide in adsorbing lead (II)

ions.

III. MATERIALS AND METHODS

Graphene oxide will be combined with magnetic nanoparticles in this study. The following

methods will be used in the bottom-up synthesis of graphene oxide from palm leaves.

Synthesis of graphene oxide (GO) from Oil palm leaves

1. The microcrystalline cellulose fraction present in oil palm leaves will be hydrolyzed with

1% w/t sulfuric acid at 120 °C for one hour to get into hydrolysate fraction as monomeric

sugars.
 2. Using 1.5% wt/wt NaOH and 0.5% wt/wt H 2O2 mixture, the amorphous microcrystalline

cellulose will undergo delignification process at 120 °C for one hour.

3. During the delignification process, the lignin and silica present in the pretreated rice

straw will be mixed with the black liquor.

4. In order to prepare graphene oxide sheets, 0.1 grams of silica will be placed in a 100-mL

round-bottom flask, and 5 grams of amorphous microcrystalline cellulose dosed with 5

ml concentrated H2SO4 and will be left for 10 minutes.

5. Afterward, it will be filtered and washed with boiling water (pH 7) and will be kept in an

oven at 40 °C for 6 hours.

6. The carbon material will then be decanted in a flask containing 0.01 g cobalt silicate

nanoparticle and will be heated to 40 °C for 30 minutes to obtain an agglomerated

graphene oxide sheet. This sheet will be cooled for 1 hour and is dehydrated at 50 to 70

°C for 24 hours to obtain an exfoliated single layer.

7. Graphene oxide will be dispersed in water with a concentration of 0.3 mg per mL and

will be sonicated for 1 hour in a bath sonicator to attain homogenous suspension.

8. For graphene oxide nanoparticles, GO water suspension (0.3 mg per mL) will

additionally be sonicated with a horn sonicator for 4 and a half hours (Fathy et. al, 2019).

Synthesis of magnetic graphene oxide (MGO)

The synthesized graphene oxide will then undergo co-precipitation method to produce

magnetic graphene oxide. The following methods will be used.

1. In order to prepare magnetic graphene oxide (MGO) using co-precipitation method, 0.15

grams of graphene oxide will be dispersed in a beaker containing 150 ml of deionized

water.
 2. Afterwards, it will be sonicated for 2 hours. This will show a clear suspension of the GO

films.

3. FeCl3.6H2O and FeCl2.4H2O will be prepared as an aqueous solution with a 2:1 mole

ratio (respectively) in a beaker with 100 ml of distilled water.

4. At room temperature, the mixed solution will be added gently to the GO suspension for

20 minutes under rapid agitation. Next, a drop wise addition of 30% ammonia solution

will be used in order to obtain a pH level of 10. This will show a black color suspension.

5. The black suspension obtain will be stirred continuously for 20 minutes under a

temperature of 85 deg C. This will be followed by cooling at a room temperture.

6. The product will be washed using a deionized water and will dried in a vacuum at 69 deg

C. This process will obtain the magentic graphene oxide (GO/Fe3O4) (Ain et al., 2020).

Characterization Techniques

Characterization of the synthesized magnetic graphene oxide was performed using UV-

VIS Spectrometer, Fourier-transform infrared spectroscopy, Scanning Electron Microscope, X-

ray diffraction, Vibrating Sample Magnetometer, and Atomic Absorption Spectrophotometer

(Ain et al., 2020).

Adsorption Experiments

Lead (II) ions are chosen as the heavy metal that will be removed by the synthesized

magnetic graphene oxide. Water containing Pb2+ will be simulated. The adsorption tests will be

performed. These tests will also be performed in a range of conditions. The water samples will

be analyzed before and after the tests to find out the removal efficiency of the synthesized

materials.
 IV. REFERENCES

Ain, Q.-U.-, Farooq, M. U., & Jalees, M. I. (2020). Application of Magnetic Graphene Oxide for

Water Purification: Heavy Metals Removal and Disinfection. Journal of Water Process

Engineering, 33, 101044. doi:10.1016/j.jwpe.2019.101044

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based materials for efficient removal of heavy metal ions from aqueous solution: A

review. Environmental Pollution. doi:10.1016/j.envpol.2019.05.050

Fathy, M., Hosny, R., Keshawy, M., & Gaffer, A. (2019). Green synthesis of graphene oxide

from oil palm leaves as novel adsorbent for removal of Cu(II) ions from synthetic

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large- scale graphene oxide nanosheets. Journal of Materials Chemistry, 22(12), 5676.

Fathy, M., Moghny, T. A., & Mousa, M. A. (2018). Fast and Fully Scalable Synthesis of

Graphene Oxide from Cellulose by Catalytic Acid Spray Method (CAS). Arabian Journal

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