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CHAPTER 2

REVIEW OF RELATED LITERATURE AND STUDIES

This chapter presents the related literature and studies after thorough

and in-depth searching done by the researchers. The synthesis of the review of

related literature was also presented in this study.

RELATED LITERATURE

Foreign

Starch, according to International Institute of Tropical Agriculture (2015),

is boundless; everyone could get it from nature. It could be derived from root

crops and grains. It was generally used in food production. Also, it was useful

chemically, biologically, and physically. It was a raw material in food, adhesive,

textiles, beverages confectionary, building materials and pharmaceuticals.

Cassava starch had a lot of distinct characteristics including high viscosity, high

clarity and has a big-freeze thaw stability.

Moreover, according to Laird (2015), starch is one of the richest

biopolymers. It is inexpensive, renewable, and decomposable. Thus, using

cassava starch with some derivatives, modifiers and/or fillers in making a

bioplastic to be a substitute for petroleum – based ones was not surprising.

Based on the news article from American Chemical Society, the scientific

study of Rangari (2016) regarding the eggshell nanoparticles, they could lead to
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the expanded use of bioplastic in packaging materials. Rangari said that they

were breaking the eggshells down into their most tiny components and then the

developed special blend of bioplastics was infused with the eggshell. He added

that the eggshells’ nanoparticles added strength to the bioplastic and made it

more flexible. He believed that the kind of bioplastic they made could be an

ideal alternative packaging material and in addition to that, it was

biodegradable. On the enhancement of the bioplastic, his team exposed the

eggshells to ultrasonic waves that broke the eggshell fragments down into

nanoparticles. The result is that the mixture became 700% more flexible than

the other blends.

In accordance with the article written by Andrade (2019), the researchers

from Sao Paulo developed a bioplastic using cassava starch and ozone gas.

Carla Ivonne La Fuente Arias said, “Our tests indicate that this new technique is

able to generate a biodegradable plastic as strong as traditional ones made of

petroleum”. The new material, according to what Arias said, had a potential to

reduce the consumption of plastic due to improper waste disposal.

Furthermore, the bioplastic magazine (2016) presented results from the

study of using eggshells in bioplastic that could bend but did not easily break.

As stated by Vijaya K. Rangari, Ph., a professor in the Department of Materials

Science and Engineering, "We’re breaking eggshells down into their most

minute components and then infusing ranjarithem into a special blend of

bioplastics that we have developed". In addition, he said, "These nano-sized

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eggshell particles add strength to the material and make them far more flexible

than other bioplastics on the market. We believe that these traits — along with

its biodegradability in the soil — could make this eggshell bioplastic a very

attractive alternative packaging material”.

Additionally, according to Elkalla (2017), the eggshells were dried in the

sun before bonding them with organic and biodegradable polymers. If it weren’t

for the eggshells, the polymers would not have become stronger. The mixture

that had been made was then put through extrusion, pressing and injection

molding. It said in the article that the materials were 100% biodegradable, could

be drilled, sanded, or laser cut. Each batch that was made was different,

depending on the materials’ measurements. The product was a pebble hanger

designed with useful compartments for storing.

When using starch – based plastic, according to Green dot Bioplastic

(2020), starch reduced carbon footprint produced by the traditional petroleum-

based plastic because it was highly degradable.

In accordance with the data analyzed by Market Research Report, they

said that “starch blends are expected to account for the largest share in the

market” from year 2015 up to present. 2.05 million tons of bioplastics produced

in 2017 counting up to 18.8% worldwide (Green dot Bioplastic, 2020).

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Local

In the annual report year 2015 of Department of Science and

Technology, they developed cassava-starch based plastics with different local

nanomaterials. According to them, the promising solutions to the worsening

disposal problem of plastic waste were the starch-based plastics. Plastics made

from starch alone could face shortcomings because of the high product cost

and a weak gas barrier. In order to overcome the said shortcomings,

biodegradability and composability were improved by modifying the cassava

starch and other materials.

The news article written by Barrett (2019) stated that the Conglomerate

San Miguel Corporation certified that they were the first Filipino company who

used biodegradable plastic in packaging. The head of the company said, “We

are very serious when it comes to sustainability. We have stopped our plastic

bottled water business; we have taken on the challenge to reduce group-wide

nonproduct water use by 50 percent by 2025, and we’ve poured more

resources into major projects to clean up bodies of water, as well as into

research that supports plastic waste reduction."

Moreover, another Filipino national developed a bioplastic made from

mango and seaweeds. According to Montinola, the bioplastic is more flexible

and can simulate the conventional platic's mechanical strength. He used

mango peelings and seaweeds because they are both sustainable and
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abundant in the Philippines. Bioplastic is unique SINCE it can be dissolved in

water without releasing toxic chemicals (Barrett, 2019).

RELATED STUDIES

Foreign

According to Gadhave, Das, Mahanwar, & Gadekar (2018), plastics

made from petroleum dominated the packaging industry. Petroleum-based

plastics have brought convenience in food manufacturing; however, it also

brought problems related to the environment. Due to the concern of the

researchers for the environment towards the growing use of fossil fuels in the

production of plastic, the interest in developing a new and alternative plastic

that was biodegradable was established. In conclusion, they stated that to

improve the mechanical properties, and water obstruction, properties of the

bioplastic, blended with other polymers and/or fillers was recommended.

In developing bioplastic from starch, Tabil, Panigrahi, & Chang (2010),

concluded that the non-biodegradable plastics became the source of

environmental concerns. Due to the aforementioned reason, greener and more

environmental – friendly materials were the alternatives used. According to

them, the advantages of starch in production of plastic are; it is renewable,

good oxygen barrier in the dry state, abundant, low-cost, and degradable.

Based on the article of Sriroth, and Sangseethong (2010), cassava

starch could be a material for making different types of packaging products, it

was also based on some experimental studies. Cassava is a major source of

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starch according to them, which meant that areas that are rich in this kind of

root crop could benefit from it and be able to develop bioplastic. They

highlighted cassava in their research than other major types of starch-based

bioplastic.

In addition, the study of Ozdamar & Ates (2018) that focused on the

limits of the new materials that could be used to create a bioplastic, found

different results from different starches. They used corn, potato, wheat and

tapioca starch tested with natural fibers and aggregates and agricultural waste.

As the result they found out that the starch that gave the finest, smoothest, and

had the most tensile strength biopolymers among all is tapioca starch.

Starch could be used to make a bioplastic because it is renewable, low-

cost, abundant, and biodegradable. The researchers Fabunmi, Tabil, Panigrahi

and Chang (2009) have decided that for the purpose of achieving the desired

product, starch had been used as a filler in starch-filled polymers blends,

thermoplastic starch, in the production. However, according to them most

starch-based composites had poor material properties such as tensile strength

and poor moisture stability. So, the researchers were looking forward to future

inquiries.

To make the bioplastic more efficient, according to Schon & Schwartz

(2013), aside from using good quality starch in producing a bioplastic, using a

plasticizer which is the glycerin, a solvent (water), and an acid - a vinegar

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resulted in a flexible, and dense polymer that could be used for daily

applications.

In addition, the study of Wahyuningtiyas & Suryanto (2017) implied that

the use of cassava starch in making a bioplastic had a potential. They used

cassava as their main ingredient in doing the bioplastic. Their goal was to know

the effect of glycerol on the microbial degradation of plastic. They mixed

cassava starch with glycerol plasticizer at different concentrations. The

experiment aspects they studied were biodegradability, moisture absorption,

shelf life and morphological properties. The result showed that after 9 days, the

decomposition of the plastic was achieved. The result also revealed that adding

more concentrated glycerol would make the microbial degradation process

faster, increase its moisture, and extend the bioplastic's shelf life in a dry place.

Furthermore, the researchers Mulyono, Suhartono, & Stella (2015),

developed a bioplastic from cassava flour with its derivatives. The tapioca

starch was extracted into its nanoparticle. The biopolymers with glycerin as

plasticizer, cassava flour, and starch were used to produce the bioplastic. As

the result, bioplastic made from cassava starch and flour had a potential to be

used as soy sauce and oil packaging materials. On the other hand, it was not

suitable in water and chili sauce packaging. Additionally, the result revealed that

the bioplastic had a UV-A (absorption) that protects the product from

photooxidation degradation.
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Likewise, Oluwasina, Olaleye, Olusegun, Oluwasina, Mohallem (2019)

extracted native starch from cassava tuber, then it underwent oxidation process

to produced oxidized starch for making the bioplastic. The characteristic of the

oxidized starch, based on their observation was that it was coarse, brownish

with 15.68% carbonyl content; they also said that it was insoluble in cold water

and had a positive influence on bioplastic films. From the making of the

bioplastic, they noticed that the film thickness increased when adding more

oxidized starch from 0.21% to 0.23% .On the other hand, the moisture content

dropped from 7.93% to 5.36%, similarly to the water solubility that decreased

from 13.48% to 5.75%. They concluded that adding more oxidized starch will

lead to longer biodegradability and enduring water absorption kinetics. Also, the

mechanical property was improved by the addition of oxidized starch. The

researchers and their study have discovered that to improve the

physicomechanical properties of starch-based bioplastic film, oxidized starch

should be used.

Accordingly, Agustin, Ahmmad, Alonzo, & Patriana (2014), conducted a

study entitled Bioplastic based on starch and cellulose nanocrystals from rice

straw. In their study, they used starch as reinforcing filler in making rice straw.

They followed the steps of delignification, sulfuric acid, hydrolysis, and

sonication. Also, they cast and prepared an evaporation method with different

ratios of starch in bioplastic. In their study, they tested the tensile strength and

moisture resistance of the bioplastic, they also conducted a mechanical test and
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they found out that there was a significant increase in tensile strength.

However, cellulose nanocrystals’ moisture resistance decreased.

Burning plastic waste according to Wahyuningtiyas & Suryanto (2018),

may produce harmful gases that can harm people’s health. The use of synthetic

plastic that is made from fossil fuels and petroleum can be reduced by making

bioplastic. So, the researchers made a bioplastic from cassava starch. The

experimented cassava starch with glycerin as plasticizer and nano clay as

reinforcement, its aspects, the tensile strength, biodegradability, and moisture

absorption were tested in this study. The result revealed that the addition of

nano clay to cassava starch increased the bioplastic’s tensile strength. For the

degradation, the result showed that after 6 days, the cassava starch-based

bioplastic was completely decomposed.

The researchers namely Ahimbisibwe, Banadda, Seay, Nabuuma,

Atwijukire, Wembabazi, & Nuwamanya (2019), developed an alternative plastic

made from starch plasticized with glycerol due to the threat presented by

plastic. To deeply know the degradation process of the starch-based plastic, the

researchers buried the bioplastic in holes of loam sandy soil. They

photographed it weekly to see the effect of degradation. All the data they

needed were recorded and compared to the control set up. The test revealed

that what broke the bioplastic are the hydrophilic enzymes which caused an

increase of its weight – bioplastic absorbs moisture after saturation. Also,

because of the soil organisms like worms and termites, the degradation of
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bioplastic was further enhanced. The result also revealed that the faster the

bioplastic degrades, the higher potential it had to be a substitute to petroleum-

based plastic.

In terms of the softness of the bioplastic, according to the study of Ashok

& Rejeesh (2017), trihydroxy-propane (glycerin) as softening agent could give

stability and could improve the functional properties of starch since it could

replace the starch-starch bonds to starch-massive glycerin bonds. They found

out that the lower the amount of glycerin, the bioplastic could be more fragile

and brittle. On the other hand, when there was a large amount plasticizer, the

polymer may become coarser.

Bioplastic, according to Dianursanti, Gozan, & Noviasan (2018), is one of

the innovations to reduce plastic waste. They added glycerol to the mixture

they’ve made to create a flexible bioplastic. As a result, the bioplastic with the

content of 15, 20, 25, 30 wt% of glycerol varied in tensile strength and

elongation. The tensile strength of the bioplastic was close to the petroleum-

based plastic and the elongation property should be improved.

Likewise, in the study Yunos, and Rahman (2011), they used thermal

analysis to determine the degradation temperature of composite. Increasing the

amount of glycerol increases the tensile strength of composite. However,

increasing the amount of glycerol elongated the composition process of the

plastic. They concluded that increasing the amount of glycerol content will lead

to a decrease in degradation temperature of the composite.

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Accordingly, Sreekumar, Leblanc & Saiter (2012) studied the effect of

glycerin on the biodegradable wheat-based thermoplastic. They made bioplastic

with different amounts of glycerol – 20, 23, 25, 30 & 35%. The results showed

that when they increased the amount of glycerin, the hardness and tensile

properties of the bioplastic lowers. However, glycerin increased the melt flow

index.

According to Syaubari, Safwani, Riza (2018), one of the natural polymers

that could be used to produce a bioplastic is tapioca starch and chitosan. Their

aim was to study the synthesis of degradation of bioplastic from cassava starch

with chitosan and the bioplastic with glycerin that they’ve already produced. The

result showed that the bioplastic with the addition of NIPAm (N-

Isopropylacrylamide), an organic compound, and 1 ml of glycerin had the

highest tensile strength. The bioplastic with NIPAm and 4ml of glycerin had the

longest elongation, and lastly, the bioplastic with chitosan-graft poly (NIPAm)

and 1 ml of glycerol had the longest biodegradation because of the small mass-

loss.

Betancour & Cree (2017) conducted a study entitled Mechanical

Properties of Poly (lactic acid) Composites Reinforced with CaCO3 Eggshell

Based Fillers. They made a recyclable and thermoplastic bioplastic. They used

powdered eggshells of white chickens with ratios of 5 wt. %, 10 wt. % and 20

wt. They used ANOVA F-test to know the significant difference of the ratio that

they had used. As a result, they found out that the particle size of eggshells
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matters. They concluded that the smaller the particle of the eggshells the

stronger the bioplastic.

In line with the study of Kasmaru & Zait (2018), they developed the

already existing alternative bioplastic by utilizing eggshells and exoskeleton of

seafoods (chitosan) wastes instead of petroleum sources. They aimed to use

eggshells and chitosan as fillers in potato starch. The researchers of this study

showed that by adding eggshell into the potato starch-based bioplastic, its

tensile strength increased by 4.94%, also the reduction of water absorption by

10.95% was determined using eggshells as fillers. They also noticed that in

eggshells, the weight loss in biodegradability test was 21.06% within 20 days.

They concluded that eggshells as fillers performed much better than chitosan in

potato starch-based bio-plastic. Also, it could be inferred that adding fillers in

starch-based bioplastics could improve the bio-plastic performance.

Similarly, the study of Mohamad, Ramli, Norshahidatul, Shohaimi,

Zainuddin, & Lothfy (2018), the bioplastic made from plastic acid (poly) is a

thermoplastic that is biodegradable and recyclable. On the other hand, the

materials used in manufacturing the bioplastic lacked the strength and flexibility

required in order to be used in the packaging industry. So, in order to improve

the said bioplastic, they made a bioplastic from cornstarch with the addition of

eggshell as an enforcement material. The researchers mixed the cornstarch

and eggshell in a ratio of 1:1 with vinegar, water and glycerol while heating.

They buried the bioplastic in soil in 12 days for thermal degradation test and
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burial test. The results showed that the bioplastic made from starch with

eggshell degrades faster than the bioplastic without eggshell and the

commercial plastic. The eggshell from the bioplastic with eggshell remained in

soil after the degradation process. Thus, the revealed result suggests that the

eggshell could be used to increase the strength and stability of bioplastic with

characteristic of faster degradation.

Furthermore, in the study of Adhikari, Mukai, Kubota, Kai, Kaneko, Araki,

& Kubo (2016), they observed the degradation of bioplastics in soil and their

degradation effects on environmental microorganisms. In their study they

analyzed the effect of microbial biomass and microbial diversity to the

degradation of the different kind bioplastic that they had tested. As a result of

their analysis, the degradation rate of the bioplastic and its components had a

significant relationship. Also, starch showed the highest rate of degradability

after 28 days. Lastly, their study showed that the degradation of bioplastic does

not affect the microorganism in the soil.

Local

Girao, Inciong, Jacinto, Magbuhat, & Sayso (2013) aim to develop a

bioplastic from cassava starch as their main material. They mixed the cassava

starch with water,epoxidized soya bean oil (ESBO), glycerol, and polyvinyl

alcohol (PVA). To determine the best combination to use in making bioplastic,

they prepared 3 mixtures with different ratios of materials. They tested the

tensile strength, acid resistance, flammability, biodegradability, and solubility of

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the bioplastic. The researchers also had a controlled variable which they used

to compare the produced bioplastic, namely the polyethylene plastic. The result

showed that the quality of plastic was based on the number of additives used. It

also revealed that the acid had an effect to the bioplastic, it burned, there was a

decrease in size of the plastic when buried in soil, and it dissolved in water.

According to a study of Cataquis, Angeles, and Dancel (2019) entitled

“Utilization of Indigenous Plants as an Additive for the Manufacture of

Biodegradable Plastics”, the bioplastic made from cassava and other starches

were glossy and translucent. The researchers said that the density and

flexibility of the bioplastic were affected by the starch used. Furthermore, the

highest moisture content out of other starches was the cassava which has

70.800%. They added that the physical appearance of the bioplastics did not

seem to be affected after being exposed to open air and other atmospheric

temperatures. To prove the biodegradability of the bioplastics, they buried all of

them in soil and after 2 weeks, the bioplastic lost mass which lead to their

assumption of it being degraded.

SYNTHESIS

From the summarized related studies and literatures, the researchers

found out that creating a bioplastic from starch and eggshells with other

derivatives was feasible. Cassava starch was more efficient to use because it is

abundant, eco-friendly, and gives the best properties a starch should possess.

Eggshells, on the other hand, should be turned into nanoparticles because of

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the solute ability of the eggshell when it is made into nano size, making the

possibility of developing a better resulting bioplastic greater. Glycerin was one

of the given materials in making a bioplastic, but manipulating and increasing its

amount in the ratio of the bioplastic according to the literatures above would

result in a more flexible and fast degrading bioplastic. Furthermore, eggshells

had the ability to make the bioplastic more durable because they contain

calcium which affects the strength of a material. The addition of eggshells to the

development of bioplastic resulted in the faster degradation of the bioplastic

than the one without eggshells. The different compositions of the raw materials,

especially the starch, improved the tensile strength of the bioplastic, however, it

reduces the water absorption as well as the solubility of the bioplastic. To

summarize, the researchers were inspired to conduct the study using the raw

materials, namely the cassava starch and powdered eggshells. Because of the

good properties of the materials, it was not impossible to have the opportunity

of developing a good functional bioplastic.