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Enhancement of Bio-plastic using Eggshells and Chitosan on Potato Starch

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 International Journal of Engineering & Technology, 7 (3.32) (2018) 110-115

International Journal of Engineering & Technology

Website: www.sciencepubco.com/index.php/IJET

Research paper

Enhancement of Bio-plastic using Eggshells and Chitosan on

Potato Starch Based
Norhafezah Kasmuri1*and Muhammad Safwan Abu Zait2
1,2
Faculty of Civil Engineering, Universiti Teknologi MARA, Shah Alam 40450, Selangor, Malaysia
*Corresponding author E-mail:norhafezahkasmuri@salam.uitm.edu.my

Abstract

The extensive production of polymer plastics and their use in different commercial applications had burdened the municipal in cost and
operation of the waste management system. This unwanted waste had also posed a significant threat to the environmental surroundings
which destroyed biota. Hence, alternatives called bio-plastic evolved as the development of renewable resource by utilizing agricultural,
eggshells and exo-skeleton seafood (chitosan) wastes instead of petroleum sources. The aim of this research is to use the eggshells and
chitosan as fillers in potato starch to overcome the inherent drawbacks of bio-plastic. The experimental study was done on tensile
strength, water absorption and biodegradability for potato starch-based bio-plastic with eggshells or chitosan. The results showed that by
adding the eggshells into the potato starch-based bio-plastic had increased the tensile strength by 4.94% compared with chitosan only
1.28%. The reduction of water absorption by 10.95% was determined using eggshells as fillers. Meanwhile, the used of chitosan resulted
in 27.59% reduction in water absorption. In eggshells, the weight loss in biodegradability test was 21.06% compared to chitosan of 7.9%
within 20 days. It can be concluded that eggshells as fillers performed much better that chitosan in potato starch-based bio-plastic. It also
can be deduced that adding fillers in starch-based bio-plastics can improve the bio-plastic performance.

Keywords: biodegradability; bio-plastic; chitosan; eggshells; potato starch; shrimp shells; tensile strength; water absorption.

Polymer-plastics are commonly used in daily life as it is low cost,

1. Introduction versatile and durable. According to the Statistics of Plastic Usage,
shoppers worldwide are currently using an approximate rate of
In early age, the first plastics were made by using plant through 500 billion plastic bags per year. Most were predominantly from
the internal chemical synthesis. One of the first synthetic plastics petroleum and natural gas [4]. The plastic waste problem is in-
was made from cellulose which is a substance come from plants creasing until today. Regarding on the environmental issue, plastic
and trees. Plastics are the most widely used polymer in daily life, waste is responsible in polluting the ocean which can affect not
since plastic offers a lot of benefits, in a variety of shapes, for only marine and aquatic organisms but also human beings.
example, film, panels, sheets, or can be flexible for any applica- The major significance drawback of plastic is that this material is
tions which requires packaging [1]. Every year, the productions of not biodegradable [2]. The degradation time depends on different
petroleum-based plastic surpass 300 million tons in 2015 [2]. types of plastic, for example, the plastic bottle takes 450 – 1000
The polymers basically are produced from non-biodegradable years to decompose completely. The petroleum-based plastic such
petrochemical-based products over the decades ago. Moreover, as polyethylene terephthalate (PET) basically does not decompose
those polymers take a very long time to decompose, which can the same way as the organic material. Furthermore, the bottles
create a serious problem caused by the long life of plastic waste, made from PET will never biodegrade [5]. Hence, nature itself
for example, the volume of industrial and commercial dumps in chooses another alternative in holding together large molecules of
the landfills increased [3]. this material since the carbon-carbon bonds in polypropylene re-
Bioplastics are biodegradable plastics which are made from bio- quire too much energy. In this case, it is hard for organisms to
mass. Based on the definition, biodegradable plastic is capable to synthesize carbon-carbon bonds compare to peptide bonds which
break down or decomposed through actions by bacteria or others can be found in the proteins or any other organic materials which
living organisms. There are two types of bioplastics, which are link carbon to nitrogen. Since the plastic is unable to be degraded
plastics that made from renewable raw materials such as poly-3- by nature, the people tend to incinerate the plastic. In fact, poison-
hydroxybutyrate (PHB) and polyhydroxyvalerate (PHV) and plas- ous gases such as dioxins, furans, and mercury will be produced
tics that contain additives to enhance biodegradation. and released to the air. These toxic substances are very harmful to
Bioplastic or biodegradable plastic could be obtained from starch. the ecosystem and surrounding environment.
In the basic knowledge, by using the pure starch, it is able to ab- Nowadays, in spite of accumulation of plastic waste due to the
sorb humidity. Thus, it is a suitable material for production in growth of population, food waste also becomes a significant prob-
pharmaceutical sector in the making of drug capsules. To produce lem to the environment. In fact, 70% of the municipal solid waste
bioplastic from starch glycerol should be added in the heating (MSW) in Malaysia comes from food waste. Generally, 90% of
process. The elasticity characteristic of bioplastic can be fabricat- food waste is biodegradable. Thus, the rate to reuse and recycle
ed by adding glycerol as plasticizer. Hence, the flexibility of the the food waste is still low. In addition, there is no specific method
plastic is provided. to dispose the food waste in Malaysia [6].
Copyright © 2018 Authors. This is an open access article distributed under the Creative Commons Attribution License, which permits unrestricted
use, distribution, and reproduction in any medium, provided the original work is properly cited.
International Journal of Engineering & Technology 111

The new innovative technique in the production of bioplastic can The procedures for producing potato starch based bioplastic have
promote a sustainable solution to reduce plastic waste together been repeated by adding 2.5 g of eggshells powder or/and chitosan
with food waste in long term. Bioplastic shows a great sign to powder into the mixture. In order to prepare the eggshells powder,
overcome the pollution since it is biodegradable. Prolong to that, first, the eggshells were crushed into smaller pieces and placed in
bioplastic is potentially suitable to replace the plastic materials a beaker. Next, sodium hypochlorite was poured into the beaker
from petroleum based. Therefore, bioplastic is the best alternative with eggshells and stirred using glass rod until the mixture be-
to minimize the cost of solid waste management in Malaysia. comes hot and releases bubbles.
The beaker was closed using aluminium foil and left for 24 hours.
2. Materials and Methods After 24 hours, the sodium hypochlorite was removed and the
eggshells were washed using water. At the same time, the oven
was turned on and set to 50˚C. The eggshells were placed in a
Sodium hypochlorite, glycerol, and acetic acid were purchased ceramic bowl. After the oven has reached the required temperature,
from Merck KGaA, Darmstadt, Germany. The chitosan (shrimp the ceramic bowl with eggshells was placed in the preheated oven
shells) filler was purchased from Sigma Aldrich brand under and left for 24 hours.
Merck KGaA, Darmstadt, Germany. The eggshells have been After 24 hours, the oven was turned off. The ceramic bowl with
collected from the food stalls at Dataran Cendekia (UiTM Shah eggshells was taken out and left to cool to room temperature (see
Alam) meanwhile potato starch was purchased from a grocery Figure 3a). Then, the eggshells were ground using grinder until it
shop in Shah Alam, Selangor, Malaysia. Deionized water (Merck becomes powder (see Figure 3b). After that, the eggshell powder
Millipore) has been used in this experiment in the Environmental was sieved using sieve size 63μm to get a constant size. Lastly, the
Laboratory, Faculty of Civil Engineering, Universiti Teknologi eggshells powder was stored in a container.
MARA, Shah Alam, Selangor, Malaysia. The procedure of bio-
plastic production has been done in the laboratory based on the
method from [7]. Meanwhile, eggshells filler have been prepared
according to [8].
In this research, bioplastic from potato starch without fillers, bio-
plastic from potato starch with the additives of filler from egg-
shells, bioplastic from potato starch with additives of fillers from
chitosan, and bioplastic from potato starch with both eggshells and
chitosan as additives have been produced. A B
Fig. 3: A) Eggshells after crushed, B) Eggshells after grinded
2.1. Preparation of Bio-Plastic
2.2. Tensile Test
An amount of sixty (60) ml of distilled water was measured using
100 ml measuring cylinder and poured into the 100 ml beaker. After the production of bioplastic, the tensile test was conducted
Secondly, ten (10) g of potato starch was measured using weight in the laboratory as shown in Figure 4. This test is conducted to
balance and placed in the beaker with distilled water. The mixture determine the mechanical properties of bioplastic on Tensile
was stirred and mixed together using glass rod. After that, five (5) Strength (TS) and Young’s Modulus (YM). In this test, ASTM-
ml of glycerol and 5 ml of acetic acid were measured using 10 ml D638-77 will be used as the standard method to determine the
measuring cylinder and poured into the beaker with the mixture. mechanical properties of bioplastic [9]. However, the required
The mixture was stirred again. At the same time, the hot plate was dimensions of bioplastic are 100mm x 30mm [3].
turned on and set at 70˚C. When the mixture was well mixed, the In the beginning, five (5) samples with dimensions of 100mm x
beaker was placed on the preheated hot plate. The mixture was 30mm from four types of bioplastic were prepared. Next, the sam-
stirred continuously. Then, a milky white liquid appeared in the ple was hung using thread to a ring with attached hook at the bot-
beaker. When it becomes sticky and almost transparent, the hot tom part of the sample to place the loads (see Figure 4). Then, the
plate was turned off and the mixture was spread on aluminium foil. load was applied until the sample failed. The total loads were rec-
Lastly, the mixture was left for four (4) days to cool to room tem- orded and the total length of the failure sample was measured and
perature (refer to Figure 1 and Figure 2). recorded. Young’s Modulus will be calculated. The following
equation is to calculate Young’s Modulus (YM);

Young’s Modulus (N/mm2) = (F/A) / [(L1-Lo)/Lo] (1)

Where F is the total applied load (N), A is the area of bioplastic

(mm2), L1 is the total length of bioplastic after breaking (mm) and
Lo is the initial length of bioplastic (mm). The steps will be re-
peated for the next sample of bioplastic. Finally, all data were
calculated and averaged. The graph was plotted to compare the
results of the different type of bioplastics.

A B
Fig. 1: A) The mixture is stirred, B) The mixture becomes sticky

Fig. 4: Illustration of Tensile Test on the bioplastic

Fig. 2: The mixture is laid on aluminium foil and cooled
112 International Journal of Engineering & Technology

2.3. Water Adsorption Test the results of the different type of bioplastics in a different type of
soils.
The water absorption test was conducted in Environment Labora-
tory, Faculty of Civil Engineering, Universiti Teknologi MARA,
Shah Alam. This test is to determine the water absorption behav-
iour on bioplastic. In this test, ASTM D570-63 was used as the
standard method in order to determine the water absorption of
bioplastic [10]. Thus, to test the bioplastic, 100mm x 100mm di-
mensions are required [3]. Hence, to conduct the overall test a
maximum period of 50 days is required.
In an early step, a sample of bioplastic with dimensions of 100mm
x 100mm from four types of bioplastic was prepared. An oven was
turned on and set at 80˚C. Once the oven reached to the required
temperature, the samples were placed in the oven and left for 24 Fig. 6: Bioplastics buried under compost soil
hours to be dried. Next, after 24 hours of drying, the oven was
turned off and the samples were taken out. The samples were
cooled to a room temperature by using desiccator for one (1) mi-
3. Result and Discussion
nute. Next, the samples were weighted using weight balance and
the data was recorded as an initial data. Then, all the samples were The result has been evaluated based on the experiment carried out
immersed in distilled water at room temperature for 50 days (see for the preparation of bioplastic and the test run for this material.
Figure 5). Within ten (10) days interval, the samples were re-
moved and were wiped using tissue paper in removing the remain- 3.1. Bio-plastic Trial Result
ing water from the surface of the samples. The sample was
weighted and data was recorded. The following equation was used Generally, first (1st) trial to third (3rd) trial, the production of bio-
to calculate water absorption; plastic had failed. However, on the fourth (4th) trial, the bioplastic
had been successfully produced with the dimensions of 100mm x
Water Absorption (%) = [(Wt -Wo) / Wo] × 100 (2) 100mm. The failure of the early bioplastic was affected by several
factors. Basically, the first (1st) trial to the fourth (4th) trial was
Where Wt (g) is the weight of bioplastic at the time being and Wo based on the method from [7].
(g) is the initial weight of bioplastic before being immersed in On the first (1st) trial, the production of bioplastic had failed due to
distilled water. The steps were repeated for the next sample of the incorrect ratio used. After the process of making the bioplastic
bioplastic. Finally, all data were calculated and averaged. The and four (4) days period for hardening process, the sample was
graphs were plotted to compare the results of the different type of still in a wet condition. Therefore, the wet condition indicated that
bioplastics. the failure result of bioplastic production in first (1st) trial.
On the second (2nd) trial, the glycerol was measured in 1 ml in-
stead of 5 ml. The used of glycerol is to act as a plasticizer to hold
the bond of molecules in the bioplastic. As for the incorrect meas-
urement of glycerol in the first place, it leads to the brittleness of
bioplastic. Hence, the sample was cracked right before its rigid
state.
On the third (3rd) trial, the production had failed due to the process
of heating the mixture. The moisture content of the mixture was
lost due to the excessive time of heating process. The mixture
became over-sticky and hard or unable to be stirred. Furthermore,
the mixture was merely hardened in the beaker before it is laid on
Fig. 5: The bioplastic is being immersed in the distilled water to the aluminium foil.
On the fourth (4th) trial, the procedure requirements fully fulfilled
the precise measurement; hence the production of bioplastic was
2.4. Biodegradability Test successfully produced with dimension 100 mm x 100 mm (see
Table 1).
The biodegradability behaviour test is to determine the biodegra-
dability of bioplastics using compost soil. In this test, ASTM Table 1: Formulation Proportion Materials of Bioplastic
D6003-96 was used as the standard method to determine the Proportions
weight loss of bioplastics [10]. Hence, the limitation of this test Potato Potato Potato Potato
was limited to 20 days to observe the behaviour of biodegradabil- Starch Starch Starch Starch
ity. Materials Based Based Based Based
In the beginning, sample of every four (4) types of bioplastic were Bioplastic Bioplastic Bioplastic Bioplastic
prepared. All the samples were weighted using weight balance. Without with with with
Filler Egg Shells Chitosan Egg Shells
The weight data was recorded as an initial data. Next, the samples
as Filler as Filler and Chi-
were buried for 64 days in natural soil and compost soil (refer to tosan as
Figure 6). With seven (7) days interval, the sample was removed Filler
from the soils. The sample was washed with distilled water and Distilled water 60 ml 60 ml 60 ml 60 ml
dried in an oven of 60˚C for 24 hours. After 24 hours, the sample Potato Starch 10 g 10 g 10 g 10 g
was weighted and the data was recorded. The following equation Glycerol 5 ml 5 ml 5 ml 5 ml
was used to calculate weight loss; Acetic acid 5 ml 5 ml 5 ml 5 ml
Egg shells 0g 2.5 g 0g 2.5 g
Weight Loss (%) = [(Wo – Wt) / Wo] × 100 (3) Chitosan 0g 0g 2.5 g 2.5 g
Dimension
Where Wo (g) is the initial weight of bioplastic before buried in Length 140 mm 160 mm 170 mm 170 mm
soil while Wt (g) is the weight of bioplastic at the time. The steps Breadth 140 mm 140mm 150 mm 160 mm
were repeated for the next sample of bioplastic. Finally, all data
was calculated and averaged. The graphs were plotted to compare
International Journal of Engineering & Technology 113

egg [12]. The membrane of the eggshells holds the bond between
the molecules exists in the bioplastic. Therefore, the theory of the
eggshells membrane able to enhance the bioplastic is accepted in
this research.
Meanwhile, based on Figure 9 and Figure 10, potato starch-based
bioplastic with the addition of eggshells and chitosan filler indi-
cate the lowest value in Young Modulus and tensile strength. The
proportion of the production of this bioplastic is the main cause of
reducing the strength of bioplastic. The amount of plasticizer such
as glycerol is lacking and lead to the brittleness of the bioplastic.
Basically, plasticizer like glycerol or water has a low molecular
A B weight and volatility which can facilitate the process of hardening
by decreasing the intermolecular force’s chain and hence increas-
ing their mobility [13]. Therefore, to increase the strength of bio-
plastic, the consideration amount of glycerol should be reconsid-
ered again in order to accommodate the amount of filler such as
potato starch, eggshells, and chitosan.

C D
Fig. 7: A) 1st trial – Wet condition, B) 3rd trial – Early hardening, C) 2nd
trial – Cracking before its rigid state, D) 2nd trial – Cracking after its rigid
state

Fig. 9: Young Modulus bar chart

A B

C D
Fig. 8: A) 50x magnifier, B) 100x magnifier, C) 400x magnifier, D)1000x
magnifier of bioplastic in microscope

Figure 8 shows the potato starch-based bioplastic with different Fig. 10: Maximum load applied bar chart
size dimension under the microscope. The image shows the inner
details of bioplastic sample. The bioplastic was light and flexible
3.3. Water Adsorption Test Result
to be bent. There was some bubbles trap in the bioplastic due to it
is not properly compressed during the laying process. However, Figure 11 shows that the optimum reading of potato starch-based
the bubbles did not affect the flexibility of the sample.
bioplastic of 16.71 g with the maximum rate of water absorption
55.88% on day 50. Specifically, behavioral of potato starch-based
3.2. Mechanical Properties bioplastic until day 20 presented a rapid increased of water ab-
sorption level. Further demonstrated a gradually increase of water
Based on Figure 9, the graph indicates that potato starch-based uptake and finally reached to an equilibrium point. This graph also
with the addition of eggshells filler has the highest Young Modu- has a similar trend to the previous study from [3].
lus value with 0.0333 N/mm2. The higher the Young Modulus Nevertheless, as for potato starch-based bioplastic with eggshells
value, the stronger and stiffer the bioplastic would be. It indicated as filler, the optimum reading is 14.29 g with the maximum rate of
that the filler of eggshells able to hold the particle bond, hence the water absorption 44.93% on day 50. However, the bioplastic start-
bioplastic become more rigid. ed to show the optimum reading on day 30 which is 14.20 g with
In Figure 10, the graph also indicates that potato starch with the the rate of 44.02%. This indicated that by adding eggshells filler
addition of eggshells filler able to cater greater load compared to into potato starch-based bioplastic was able to reduce the water
others. This is because every eggshell has a membrane layer and it absorption content in the bioplastic. This is because the filler ca-
is divided by two types of the layer which lie beneath the shell, pable to cover up the pores contained in the bioplastic. Hence, it
outer and inner shell membranes [11]. Both of the membranes are reduced the rate of water absorption.
made up of protein fibres; exactly lie parallel to the surface of the
114 International Journal of Engineering & Technology

In the same way, potato starch-based bioplastic with chitosan as 3.4. Biodegradation Behaviour Test
filler, the graph of Figure 12 indicates the optimum reading of
12.97% with the maximum rate of water absorption (28.89%). Up The biodegradability test of bioplastic was determined after 20
to day 10, it shows the rapid increase of water absorption level and days. This test carried the result of bioplastic mass reduction in
on day 10 up to day 50 in water uptake demonstrated a gradually natural soil and compost soil. Based on Figure 14, it indicates the
increase until it finally reached to an equilibrium point. Chitosan biodegradability behaviour in reducing the mass of bioplastics.
is known as a non-starch organic material, thus has the same struc- The initial mass of potato starch-based bioplastic was 7.77 g on
ture to cellulose [14], therefore, this research finding agreed with day 0 and reduced to 1.05 g on day 20 with the optimum rate of
the previous research result from [3]. Hence, by comparing the weight loss of 86.49%. Therefore, in Figure 15 the value of
two types of bioplastic above, the addition of chitosan was far 86.49% is the optimum rate of weight loss which indicated that
better due to the lowest rate of water absorption and minimum the potato starch-based bioplastic had a good ability to biodegrade
water content absorbed. The chitosan filler has a film-forming under the compost soil. Hence, the result obtained is similar with
based which able to absorb lesser water [15]. the previous research which mentioned that bioplastic is able to be
decomposed completely within 24 days [16].
Figure 15 shows the addition of eggshells filler into potato starch-
based bioplastic has slowed down the rate of biodegradability of
bioplastic with the optimum rate of weight loss of 65.43%. Based
on Figure 14, the initial mass of the sample is 5.41 g and reduced
to 1.87 g on day 20. Eggshell is largely made up of calcium car-
bonate which has the major content up to 95% following with
3.5% minor amount of organic matrix in the eggshell [17]. There-
fore, the microorganisms degrade the bioplastic but the calcium
carbonate remains. Since it has an average rate of biodegradability,
this would deduced that by adding the eggshells filler, it takes
more time for microorganisms to break the bond chains between
nutrients in bioplastic.

Fig. 11: Weight (g) against days for water adsorption test

Fig. 14: Weight (g) against days for biodegradability behaviour test

Fig. 12: Rate of water absorption (%) against days for water adsorption On top of that, by referring to Figure 15, the addition of chitosan
test into potato starch-based bioplastic also has a good ability to bio-
degrade under the compost soil with the optimum rate of 78.59%.
Based on Figure 13, the sample was taken out after 10 days un- Based on Figure 14, the initial mass of the sample is 6.26 g and
dergone the process of water absorption test. Fungus started to able to reduce to 1.34 g on day 20. It is capable to assume that the
grow on the sample due to the damp condition on the bioplastics sample can completely decompose within 25 days. However, in
surface. This happened due to air voids produced during the order to accelerate the biodegradation time of potato starch-based
heating process of bioplastic in which the deionized water in the bioplastic with chitosan filler, the enzymes known as chitinase and
content of the mixture was heated up and evaporated. This cause chitosanase are needed [18].
bubbles in the end of bioplastic production. During the immersion During the biodegradability behaviour test, some observation was
of bioplastic in deionized water, the air voids become a space for made. In the beginning, on day 5, the compost soil began to grow
the water to penetrate it. Since the fillers were added into the mix- fungus on the surface area of the soil. This indicates that more
ture, the fillers replacing the void of the bioplastic. Therefore, the fungus grew in the compost soil, the higher the mass reduction of
rate of water absorption was reduced since the water was unable to bioplastic. Hence, the higher rate of weight loss of bioplastics to
penetrate and filled the void of the bioplastic. be decomposed. There are at least 90 species of microorganisms
that responsible for biodegradation of bioplastics such as aerobes,
anaerobes, photosynthetic bacteria, archae-bacteria and lower
eukaryotic [2].

Fig. 13: A sample of bioplastic after ten (10) days undergo water
absorption test
 International Journal of Engineering & Technology 115

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Acknowledgement
The authors gratefully acknowledged Universiti Teknologi MA-
RA, Shah Alam and Bestari Perdana Grant (600-IRMI/DANA
5/3/BESTARI (063/2018), provided by RMI for financially sup-
porting this study and providing the resources.

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