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Synthesis and characterization of eco-friendly bioplastic

from low-cost plant resources
Akshaya Krishnamurthy, Pavithra Amritkumar
PG and  Research Department of Biotechnology, Women’s Christian College
Abstract
The alarming rate of environmental pollution caused by single-use plastics has necessitated
the search for cost-effective, sustainable alternatives. This study aimed to create bioplastic
films using jackfruit waste flour and sago as low-cost starch sources. Three composite
bioplastic films were created using a starch-lemon extract-water mixture but with different
cross-linkers: (1) PV (polylactic acid and crude palm oil), (2) AV (glycerol and crude palm
oil), (3) PAV (polylactic acid, glycerol, and crude palm oil). The formulated films physical,
chemical, mechanical, and biological parameters were characterized. PV film showed the best
tensile strength (TS) of 5.24 MPa and the least elongation at break (EAB) of 3.49%, while
PAV films had the least TS of 0.78 MPa with a maximum EAB (73.38%). FTIR analysis of
films showed peaks at 1736.3–1743.3 cm−1 indicating strong interaction of triglycerides
(C=O stretching). In thermogravimetric analysis (TGA), all the films displayed gradual
desorption occurring between 150 and 220 °C where the volatile compounds started to
evaporate, and around 300 °C the lower molecular weight compounds like plasticizer, cross-
linker, and other additives started to release out; pyrolysis of carbonated compounds occurred
above 500 °C. PAV films displayed the best thermal stability with half decomposition at
330 °C. The biodegradability of films was demonstrated using soil burial and culturing pure
cultures of microorganisms in minimal media with the film as a carbon source. Bioplastic
films developed in this study using low-cost plant starch sources demonstrated properties
with potential application in the food packaging industry.

1. Introduction
Plastics are widely used due to their versatility and excellent processability, thermal and
mechanical properties. Single-use plastic/disposable plastic (plastic carry bags, straws, cups,
cutlery, water packets, cling wraps, and bottles) is the most visible source of plastic pollution.
Approximately 380 million tonnes of plastic are produced and discarded annually. The
majority of this waste ends up in the environment, with only 10-13% being recycled. Despite
their widespread use, they are non-biodegradable due to their stable carbon-hydrogen bond
and very large complex polymeric structure, causing ocean and land pollution. They typically
disintegrate into tiny fragments over long periods, which are ingested by smaller eukaryotes,
which in turn are ingested by higher eukaryotes, affecting the entire food chain and putting
many species in jeopardy. Each year, an estimated 8 million tonnes of discarded plastic enter
the world's oceans through coastal regions. These plastics endanger coral reefs encased in
plastic bags; turtles, whales and sea birds with plastic stuffed in their bellies and nostrils
clogged with straws lead to painful deaths.
The study of obtaining starch sources from tropical agricultural waste is gaining
popularity. Jackfruit is a tropical fruit with 100 to 500 jackfruit seeds that weigh 8-15% of the
jackfruit and have a high starch content. According to Zawawi et al., sago starch is a natural
raw material that contains a high concentration of amylose, which can easily bond with other
compounds and gelatinizes when heated to 70 °C. Glycerol, as a plasticizer, can strengthen
bioplastics by improving chemical bonding, resulting in higher tensile strength. The current
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study aims to synthesize eco-friendly bioplastic from these renewable plant sources, develop
a cost-effective alternative to conventional petrochemical plastic, and evaluate its physical,
mechanical, and biodegradable properties systematically.
2. Methodology
Materials
Jackfruit wastes (seed and core) were gathered from a local fruit vendor, while sago (Tapioca
pearls), pearl corn, and crude palm oil were procured from local groceries. Hi-media was the
supplier of glycerol. For this investigation, only pure isolates of bacteria (Escherichia coli,
Pseudomonas aeruginosa, Staphylococcus aureus, Klebsiella pneumonia, Streptococcus spp.)
and fungi (Candida albicans, Aspergillus favus, and Penicillium chrysogenum) were utilized.
They were obtained from King's Institute in Chennai,
Preparation of starch source
Jack fruit wastes (seed and core) were gathered at a nearby fruit market after the interior,
pulpy fruit was removed. To get rid of any surface impurities, they were thoroughly cleansed
with warm water. The seed's outer covering was taken off. To speed up the drying process,
the core and seeds were broken into small pieces and dried in the sun for seven days. The
local flour mill used a dry milling procedure to turn the dried components into fine flour. To
reduce the moisture level, sago and pearl corn were dried in a hot air oven for five hours at 60
°C before being dry-milled into flour in a nearby flour mill (Mill Power Industries, India).
The resulting flours were finely sieved before being placed in airtight containers and kept in a
cool, dry location. Initially, the composition of the flours (sago, jackfruit seed, and core) was
characterized. According to accepted methods, the laboratory measurements of flours'
moisture, ash content, carbohydrate, protein, and starch content were made.
Synthesis of polylactic acid
The main starting point for the manufacture of polylactic acid is lactic acid (PLA). Lactic
acid was produced in the current investigation by fermenting pearl corn hydrolysate. For
hydrolysis, 95 ml of distilled water, 5% concentrated sulfuric acid, and 10 g of pearl corn
starch were combined. To obtain a pure hydrolysate, the contents were filtered through filter
paper and neutralized with NaOH. 850 ml of distilled water was combined with the standard
MRS broth ingredients, 50 ml of pure hydrolysate was added, the pH of the broth was raised
to 6.2, and it was sterilized. Through membrane filtration, 100 ml of a 4% glucose solution
was added to the flask. 84 hours were spent incubating Lactobacillus spores at 37 °C after
inoculation. Three copies of the procedure were completed. The traditional precipitation
process was used to remove the lactic acid from the fermented broth. First, the broth was
filtered to get rid of the Lactobacillus spp. cells. To balance the acid created in the broth,
excessive calcium carbonate was added. This caused calcium lactate salt to develop, which
crcrystacrystallized precipitate. To create calcium sulphate salt as precipitate and soluble
lactic acid into the filtrate, 5% concentrated sulfuric acid was added to the precipitate. To
extract the residual contaminants from the lactic acid, a little amount of activated carbon was
added to the filtrate and centrifuged for 10 minutes at 6000 rpm. The supernatant was then
put in storage to be used later. Ferric chloride was used in Kelling's test to detect the presence
of lactic acid. Using methylene red-bromophenol blue as an indicator and chloroform,
butanol, and water as the solvents, thin layer chromatography was used to measure the purity
level. Colorimetric analysis was used to determine the lactic acid concentration. By using the
direct polycondensation approach without a catalyst, PLA was synthesized in a lab [15]. The
lactic acid that had just been polymerized was used right away in the making of the film.
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Fabrication of composite bioplastic films

In this study, three different formulations were tested to create bioplastic films utilizing
starch, lemon extract, glycerol, palm oil, and PLA. All of the movies were made using
traditional casting techniques. 10 g of starch mix (sago, jackfruit seed, and core flours in a
ratio of 9:1:0.5) and 3 ml of lemon extract were added to 97 ml of sterile, distilled water, and
the mixture was then sonicated for five minutes to ensure perfect blending. Three copies of
this were created. 5% glycerol (A) and 5% crude palm oil (V) were added to formulation AV,
2.5% crude polylactic acid (P), 5% glycerol (A), and 5% crude palm oil (V) were added to
formulation PV, and all three formulations were well mixed. Each formulation was heated on
a hot plate until a thick, gelatinous consistency developed, at which point it was poured onto
aluminium foil and roasted in a hot air oven for two days at 45 °C. The films were removed
and prepared for additional analysis listing the three bioplastic films created in this
investigation and their composition.
3. Results and Discussion
Testing of lactic acid
The formation of iron lactate produced a canary yellow color in Kelling's test. Orange
coloration was observed in the water. The purity of lactic acid as determined by TLC was
half that of standard lactic acid (88%). The colorimetric concentration of lactic acid was
found to be 0.65 g/g of the product tested.
Bioplastic films and their properties
Properties PV film AV film PAV film
Brittleness High, when exposedModerate when Moderate when
to a temperature above
exposed to exposed to
50 °C temperatures above temperatures above
80–90 °C 70–80 °C
Ductility Low (when absorbs Moderate High
moisture)
Recasting Yes Yes Yes
ability
Texture Smooth surface and Slightly rough and Soft and flexible with
less flexible flexible an even surface

Thickness swelling percentage and water absorption

PV film absorbed three times as much water as AV film, and PAV had swollen twice as
much as AV. Polylactic acid-based starch film (PV) may have less cross-linking with starch;
PLA absorbs moisture easily, resulting in increased swelling. Glycerol and starch (AV) have
formed a very strong interaction, leaving little space for the film to absorb water while
swelling as little as possible. PLA starch containing glycerol (PAV) demonstrated
intermediate properties with moderate swelling.
Bioplastic film type Thickness before Thickness after Percentag
immersion (mm) immersion (mm) e
PV (PLA and crude palm oil) 0.28±1 0.39±1 39.3
AV (glycerol and crude palm oil) 0.34±1 0.35±1 2.94
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PAV (PLA, glycerol, and crude palm 0.27±1 0.35±1 29.6

oil)

Bioplastic film type Mass before Mass after Percentag

immersion (g) immersion (g) e
PV (PLA and crude palm oil) 0.28±1 1.08±1 285.7
AV (glycerol and crude palm oil) 0.30±1 0.40±1 3.33
PAV (PLA, glycerol, and crude palm 0.28±1 0.78±1 178.6
oil)

Film transparency
Bioplastic films were less transparent than synthetic polythene, which could be attributed to
the fillers used in bioplastic production as well as thickness. Despite this, PAV bioplastic was
more transparent than other studies.
Film type Absorbance Transmission Thickness Transparency
Polyethylene 0.398 39.99 0.12 13.34
PV 0.440 36.30 0.28 5.57
AV 0.450 35.48 0.34 4.56
PAV 0.420 38.30 0.27 5.86

Water solubility
The films' solubility indicates the presence of hydrophilic compounds in the film. Because of
the water-absorbing nature of PLA, PV film had a higher solubility. Glycerol films were less
soluble due to the high level of intermolecular attraction and crosslinking within the matrix,
resulting in a lower ability to interact with water. As a result, AV film had the lowest water
solubility percentage, whereas PAV had a moderate solubility percentage.
Bioplastic film type Initial dry weight Final dry weight Solubility
(g) (g) percentag
e
PV (PLA and crude palm oil) 0.20 0.06 70
AV (glycerol and crude palm oil) 0.25 0.22 12
PAV (PLA, glycerol, and crude palm 0.22 0.12 45.45
oil)

Biodegradation
Soil burial
When compared to other films, the PV film began to disintegrate more on day 30. Over the
AV film, fungal growth was observed. The PAV film was well mixed with the soil and began
to degrade. On day 45, PV film disintegrated into pieces, degrading half of the sample, 20%
of AV film, and 35% of PAV film. On day 60, the PV film had completely degraded, along
with 50% of the AV film and 80% of the PAV film. Throughout, no changes in synthetic
polythene were observed. This study discovered that starch-based bioplastics degrade faster
than synthetic plastics.
Laboratory culture-based microbial biodegradation
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On day 30, PV films showed the most degradation, followed by 15% AV film and 75% PAV
film. On day 45, there was 10% PV film, 45% AV film, and 20% PV film remaining. There
was no growth in synthetic polythene or the control. The metabolites/by-products released by
the microbes caused the change in colour of the media. A consortium of fungal cultures
biodegrades bioplastic films and synthetic polythene.
Discussion
Thus, the physical, chemical and biological properties of the three films synthesized (PV,
AV, and PAV) were extensively analyzed and compared in this study. The three bioplastic
formulations outperformed previous studies' jackfruit seed four-based biofilms in terms of
tensile strength, EAB, thermal stability, and biodegradability. The composite four,
crosslinkers, and plasticizers ratio used in this study significantly improved the properties of
the biofilms.
4. Conclusion
The goal of this study was to create affordable, eco-friendly bioplastic using only plant
materials. In this work, three bioplastic films were created utilizing the same starch supply,
water, and lemon extract, but with various cross-linkers: (1) PV (polylactic acid and starch in
crude palm oil); (2) AV (glycerol and crude palm oil with starch) (3) PAV (polylactic acid,
glycerol, and crude palm oil) (polylactic acid, glycerol, and crude palm oil). Regarding
hardness and tensile qualities, each film showed a range of characteristics. The physical,
chemical, mechanical, and biological characteristics of the formulated films were described.
While PAV film had the lowest tensile strength (TS) of 0.78 MPa and the highest EAB
(73.38%), PV film had the best TS of 5.24 MPa and the least elongation at break (EAB) of
3.49%. Films' spectrum closeness to synthetic polyethylene polymers was revealed by FTIR
investigation. All the films in the thermogravimetric analysis (TGA) showed gradual
desorption between 150 and 220 °C, where the volatile compounds began to evaporate, and
around 300 °C, where the lower molecular weight compounds, such as plasticizer, cross-
linker, and other additives, started to release out; pyrolysis of carbonated compounds
occurred above 500 °C. At 330 °C, PAV film showed the best thermal stability, with just
50% breakdown. The soil burial approach and the cultivation of pure cultures of
microorganisms in minimum media while using the film as a carbon source were used to
illustrate the biodegradability of films. Each of the three bioplastic films that were created
showed a variety of mechanical characteristics, making them suitable for use in various
contexts. Two products were tested in the lab for prospective applications based on the
characteristics revealed by the bioplastic films created in this study. As a safe and
environmentally friendly substitute, bioplastic straws were created from renewable starch
(PV formulation) and handmade paper covered with AV film, which was also tested for water
resistance. Paper without a coating quickly absorbed water, whereas paper coated with AV
bioplastic retained water even after two hours. The findings of this study demonstrated that
bioplastic may be produced using sago-jackfruit waste flour and polymer polylactic acid
(PLA) as a secure and affordable replacement for synthetic single-use polyethylene plastics.